National Library of Energy BETA

Sample records for aerosol chemical speciation

  1. Long-term Measurements of Submicrometer Aerosol Chemistry at the Southern Great Plains (SGP) Using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect (OSTI)

    Parworth, Caroline; Fast, Jerome D.; Mei, Fan; Shippert, Timothy R.; Sivaraman, Chitra; Tilp, Alison; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the U.S. Department of Energy’s Southern Great Plains (SGP) site are discussed. Over the period of 19 months (Nov. 20, 2010 – June 2012) highly time resolved (~30 min.) NR-PM1 data was recorded. Using this dataset the value-added product (VAP) of deriving organic aerosol components (OACOMP) is introduced. With this VAP, multivariate analysis of the measured organic mass spectral matrix can be performed on long term data to return organic aerosol (OA) factors that are associated with distinct sources, evolution processes, and physiochemical properties. Three factors were obtained from this VAP including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when nitrate increased due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations showed little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increased and were mainly associated with local fires. Isoprene and carbon monoxide emission rates were computed by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) to represent the spatial distribution of biogenic and anthropogenic sources, respectively. From this model there is evidence to support that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  2. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations ofmore » the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.« less

  3. Long-term measurements of submicrometer aerosol chemistry at the Southern Great Plains (SGP) using an Aerosol Chemical Speciation Monitor (ACSM)

    SciTech Connect (OSTI)

    Parworth, Caroline; Tilp, Alison; Fast, Jerome; Mei, Fan; Shippert, Tim; Sivaraman, Chitra; Watson, Thomas; Zhang, Qi

    2015-04-01

    In this study the long-term trends of non-refractory submicrometer aerosol (NR-PM1) composition and mass concentration measured by an Aerosol Chemical Speciation Monitor (ACSM) at the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site are discussed. NR-PM1 data was recorded at ~30 min intervals over a period of 19 months between November 2010 and June 2012. Positive Matrix Factorization (PMF) was performed on the measured organic mass spectral matrix using a rolling window technique to derive factors associated with distinct sources, evolution processes, and physiochemical properties. The rolling window approach also allows us to capture the dynamic variations of the chemical properties in the organic aerosol (OA) factors over time. Three OA factors were obtained including two oxygenated OA (OOA) factors, differing in degrees of oxidation, and a biomass burning OA (BBOA) factor. Back trajectory analyses were performed to investigate possible sources of major NR-PM1 species at the SGP site. Organics dominated NR-PM1 mass concentration for the majority of the study with the exception of winter, when ammonium nitrate increases due to transport of precursor species from surrounding urban and agricultural areas and also due to cooler temperatures. Sulfate mass concentrations have little seasonal variation with mixed regional and local sources. In the spring BBOA emissions increase and are mainly associated with local fires. Isoprene and carbon monoxide emission rates were obtained by the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and the 2011 U.S. National Emissions Inventory to represent the spatial distribution of biogenic and anthropogenic sources, respectively. The combined spatial distribution of isoprene emissions and air mass trajectories suggest that biogenic emissions from the southeast contribute to SOA formation at the SGP site during the summer.

  4. Overview of Detailed Chemical Speciation and Particle Sizing...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Diesel Exhaust, Both Real Time and Filter Based Measurements Overview of Detailed Chemical Speciation and Particle Sizing for Diesel Exhaust, Both Real Time and Filter Based ...

  5. Overview of Detailed Chemical Speciation and Particle Sizing for Diesel

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Exhaust, Both Real Time and Filter Based Measurements | Department of Energy Detailed Chemical Speciation and Particle Sizing for Diesel Exhaust, Both Real Time and Filter Based Measurements Overview of Detailed Chemical Speciation and Particle Sizing for Diesel Exhaust, Both Real Time and Filter Based Measurements 2002 DEER Conference Presentation: University of Wisconsin - Madison PDF icon 2002_deer_foster.pdf More Documents & Publications The Impact of Oil Consumption Mechanisms on

  6. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOE Patents [OSTI]

    Lee, Yin-Nan E. (East Setauket, NY); Weber, Rodney J. (Atlanta, GA)

    2003-01-01

    An apparatus and method for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution are provided. The apparatus includes a modified particle size magnifier for producing activated aerosol particles and a collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical methods. The method provided for on-line measurement of chemical composition of aerosol particles includes exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

  7. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOE Patents [OSTI]

    Lee, Yin-Nan E.; Weber, Rodney J.; Orsini, Douglas

    2006-04-18

    An apparatus for continuous on-line measurement of chemical composition of aerosol particles with a fast time resolution is provided. The apparatus includes an enhanced particle size magnifier for producing activated aerosol particles and an enhanced collection device which collects the activated aerosol particles into a liquid stream for quantitative analysis by analytical means. Methods for on-line measurement of chemical composition of aerosol particles are also provided, the method including exposing aerosol carrying sample air to hot saturated steam thereby forming activated aerosol particles; collecting the activated aerosol particles by a collection device for delivery as a jet stream onto an impaction surface; and flushing off the activated aerosol particles from the impaction surface into a liquid stream for delivery of the collected liquid stream to an analytical instrument for quantitative measurement.

  8. Chemical and Physical Characteristics of Diesel Aerosol | Department of

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Energy and Physical Characteristics of Diesel Aerosol Chemical and Physical Characteristics of Diesel Aerosol 2002 DEER Conference Presentation: University of Minnesota PDF icon 2002_deer_kittelson1.pdf More Documents & Publications Mass Correlation of Engine Emissions with Spectral Instruments The Impact of Oil Consumption Mechanisms on Diesel Exhaust Particle Size Distributions and Detailed Exhaust Chemical Composition Nanoparticle Emissions from Internal Combustion Engines

  9. Chemical distribution in high-solids paint overspray aerosols

    SciTech Connect (OSTI)

    D'Arcy, J.B.; Chan, T.L. )

    1990-03-01

    The chemical composition of high-solids basecoat paint overspray aerosols was determined as a function of particle size. Detailed information on the chemical composition of the overspray aerosols is important in health hazard evaluation since the composition and distribution within the airborne particles may differ significantly from the bulk paint material. This study was conducted in a typical down-draft paint booth equipped with air-atomized spray painting equipment. A fixed paint target was used to simulate typical overspray generation conditions and the aerosols were collected isokinetically with a seven-stage cascade impactor for size-fractionated analysis. The overspray aerosol from six paints consisted of organic paint binders with varying amounts of inorganic species as pigments or luster enhancers. These overspray aerosols had mass median aerodynamic diameters (MMAD) ranging from 2.9 to 9.7 microns. The size-fractionated paint samples collected on the impaction stages were analyzed by energy dispersive X-ray spectrometry on a scanning electron microscope (SEM-EDXRS) to identify the metallic elements. Atomic absorption spectrometry was used to determine the mass distribution of aluminum and iron as indicators of nonuniform distribution. Three of the aerosols containing aluminum were found to have bimodal distributions with most aluminum distributions having cumulative MMADs larger than the total aerosol. Iron in the aerosols was bimodal for three of the paints with all samples having an overall iron MMAD less than or equal to the overspray aerosol MMAD. Analysis using ultraviolet spectrometry revealed that the organic compounds present in the size-fractionated particulate samples consisted of a single, polydispersed mode with an MMAD similar to that of the total overspray aerosol.

  10. Characterization of Chemical Speciation in Ultra Thin Uranium Oxide Films by Neutron Reflectometry

    SciTech Connect (OSTI)

    Wang, Peng

    2012-06-20

    Motivation for this project is due to more than 17 kg of HEU and 400 g of Pu have been interdicted through an international effort to control nuclear smuggling. Nuclear forensics - Detection and analysis of nuclear materials recovered from either the capture of unused materials or from the radioactive debris following a nuclear explosion or activities, which can contribute significantly for national security. Develop new nuclear forensic methods can be applied to: (a) Environmental swipes, (b) Small particulates, and (c) Thin films. Conclusions of the project are: (1) A unique approach: Neutron Reflectometry + Surface Enhanced Raman Spectroscopy; and (2) Detection of chemical speciation with {angstrom}-level resolution.

  11. Frontiers in Assessing the Role of Chemical Speciation And Natural Attenuation on the Bioavailability of Contaminants in the Terrestrial Environment

    SciTech Connect (OSTI)

    Gerson, A.R.; Anastasio, C.; Crowe, S.; Fowle, D.; Guo, B.; Kennedy, I.; Lombi, E.; Nico, P.S.; Marcus, M.A.; Martin, R.R.; Naftel, S.J.; Nelson, A.J.; Paktunc, D.; Roberts, J.A.; Weisener, C.G.; Werner, M.L.

    2009-05-28

    It has long been recognized that contaminants interact with the solid soil phase via a series of sorption-desorption (all chemicals) and precipitation-dissolution (polar and ionic compounds) reactions including physical migration into micropores and diffusion into the solid phase (see Chapter 2). Until recently the extent of such interactions and the binding with different solid pools was established via a series of chemical extractions (see Chapter 20) and a combination of instrumental techniques. However, none of these techniques provide a true indication of the speciation of contaminants on or in solid minerals and organics. The last decade has witnessed the emergence of tools that provide an assessment of the speciation and attenuation of chemicals at molecular level. In this chapter we provide an overview of the current state-of-the-art for assessing speciation and attenuation of contaminants in the terrestrial environment. Given that speciation and attenuation influence chemical bioavailability, we devote part of this chapter to the application of isotopic dilution techniques to bioavailability assessment. We have not attempted to be exhaustive but rather to highlight a number of studies in sufficient detail so that the reader will be provided with an insight as to whether such approaches are applicable to their field of endeavor and what the realistic outcomes might be.

  12. Direct Measurement and Chemical Speciation of Top Ring Zone Liquid During Engine Operation

    SciTech Connect (OSTI)

    Splitter, Derek A; Burrows, Barry Clay; Lewis Sr, Samuel Arthur

    2015-01-01

    The present manuscript consists of proof of concept experiments involving direct measurements and detailed chemical speciation from the top ring zone of a running engine. The work uses a naturally aspirated single cylinder utility engine that has been modified to allow direct liquid sample acquisition from behind the top ring. Samples were analyzed and spectated using gas chromatographic techniques. Results show that the liquid mixture in the top ring zone is neither neat lubricant nor fuel but a combination of the two with unique chemical properties. At the tested steady state no-load operating condition, the chemical species of the top ring zone liquid were found to be highly dependent on boiling point, where both low reactivity higher boiling point fuel species and lubricant are observed to be the dominant constituents. The results show that at least for the tested condition, approximately 25% of the top ring zone is comprised of gasoline fuel like molecules, which are dominated by high octane number aromatic species, while the remainder of the liquid is comprised of lubricant like species.

  13. Aerosol chemical vapor deposition of metal oxide films

    DOE Patents [OSTI]

    Ott, Kevin C. (4745 Trinity Dr., Los Alamos, NM 87544); Kodas, Toivo T. (5200 Noreen Dr. NE., Albuquerque, NM 87111)

    1994-01-01

    A process of preparing a film of a multicomponent metal oxide including: forming an aerosol from a solution comprised of a suitable solvent and at least two precursor compounds capable of volatilizing at temperatures lower than the decomposition temperature of said precursor compounds; passing said aerosol in combination with a suitable oxygen-containing carrier gas into a heated zone, said heated zone having a temperature sufficient to evaporate the solvent and volatilize said precursor compounds; and passing said volatilized precursor compounds against the surface of a substrate, said substrate having a sufficient temperature to decompose said volatilized precursor compounds whereby metal atoms contained within said volatilized precursor compounds are deposited as a metal oxide film upon the substrate is disclosed. In addition, a coated article comprising a multicomponent metal oxide film conforming to the surface of a substrate selected from the group consisting of silicon, magnesium oxide, yttrium-stabilized zirconium oxide, sapphire, or lanthanum gallate, said multicomponent metal oxide film characterized as having a substantially uniform thickness upon said FIELD OF THE INVENTION The present invention relates to the field of film coating deposition techniques, and more particularly to the deposition of multicomponent metal oxide films by aerosol chemical vapor deposition. This invention is the result of a contract with the Department of Energy (Contract No. W-7405-ENG-36).

  14. RETENTION AND CHEMICAL SPECIATION OF URANIUM IN A WETLAND ON THE SAVANNAH RIVER SITE

    SciTech Connect (OSTI)

    Li, D.; CHANG, H.: SEAMAN, J.; Jaffe, P.; Groos, P.; Jiang, D.; Chen, N.; Lin, J.; Arthur, Z.; Scheckel, K.; Kaplan, D.

    2013-06-17

    Uranium speciation and retention mechanism onto Savannah River Site (SRS) wetland sediments was studied using batch (ad)sorption experiments, sequential extraction desorption tests and U L{sub 3}-edge X-ray absorption near-edge structure (XANES) spectroscopy of contaminated wetland sediments. U was highly retained by the SRS wetland sediments. In contrast to other similar but much lower natural organic matter (NOM) sediments, significant sorption of U onto the SRS sediments was observed at pH <4 and pH >8. Sequential extraction tests indicated that the U(VI) species were primarily associated with the acid soluble fraction (weak acetic acid extractable) and NOM fraction (Na-pyrophosphate extractable). Uranium L3- edge XANES spectra of the U-retained sediments were nearly identical to that of uranyl acetate. The primary oxidation state of U in these sediments was as U(VI), and there was little evidence that the high sorptive capacity of the sediments could be ascribed to abiotic or biotic reduction to the less soluble U(IV) species. The molecular mechanism responsible for the high U retention in the SRS wetland sediments is likely related to the chemical bonding of U to organic carbon.

  15. Chapter 7: Frontiers in assessing the role of chemical speciation and natural attenuation on the bioavailability of contaminants in the terrestrial environment

    SciTech Connect (OSTI)

    Gerson, A.R.; Anastasio, C.; Crowe, S.; Fowle, D.; Guo, G.; Kennedy, I.; Lombi, E.; Nico, P.S.; Marcus, M.A.; Martin, R.R.; Naftel, S.J.; Nelson, A.J.; Paktunc, D.; Roberts, J.A.; Weisener, C.G.; Werner, M.L.

    2008-07-18

    It has long been recognised that contaminants interact with the solid soil phase via a series of sorption-desorption (all chemicals) and precipitation-dissolution (polar and ionic compounds) reactions including physical migration into micropores and diffusion into the solid phase (see Chapter 2). Until recently the extent of such interactions and the binding with different solid pools was established via a series of chemical extractions (see Chapter 20) and a combination of instrumental techniques. However, none of these techniques provide a true indication of the speciation of contaminants on or in solid minerals and organics. The last decade has witnessed the emergence of tools that provide an assessment of the speciation and attenuation of chemicals at molecular level. In this chapter we provide an overview of the current state-of-the-art for assessing speciation and attenuation of contaminants in the terrestrial environment. Given that speciation and attenuation influence chemical bioavailability, we devote part of this chapter to the application of isotopic dilution techniques to bioavailability assessment. We have not attempted to be exhaustive but rather to highlight a number of studies in sufficient detail so that the reader will be provided with an insight as to whether such approaches are applicable to their field of endeavour and what the realistic outcomes might be.

  16. Limitations and requirements of using the chemical speciation code, MINTEQA2, to predict water quality impacts at fossil plants

    SciTech Connect (OSTI)

    Danzig, A.J.; McEntyre, C.L.

    1995-10-01

    The chemical speciation model, MINTEQA2, was used to simulate the effects of proposed waste process changes on the final waste water effluent at coal-fired power plants. The chemistry of the waste water system at the plants was extremely complex, involving factors such as temperature, redox couples, ionic strength, adsorption, and gas phase equilibria. MINTEQA2 is capable of computing equilibria among the dissolved, adsorbed, solid, and gas phases in an environmental setting. This paper focuses on the limitations and requirements of using the model for these purposes. Specifics include sampling protocols, biological factors, and knowledge of how MINTEQA2 works. This approach could be used to aid in modeling treatment systems for a variety of power generated wastes.

  17. Lidar techniques for chemical and aerosol air pollution studies

    SciTech Connect (OSTI)

    Hardesty, R.M.

    1993-12-31

    At the Wave Propagation Laboratory (WPL), lidar methods are being applied in several areas of air pollution research. Differential absorption lidar (DIAL) systems for measuring ozone, ethylene, and other pollutants have been recently developed. The ozone instrument profiles ozone concentration in the boundary layer and lower troposphere to study sources, sinks, and transport of ozone. A goal is to combine DIAL and Doppler lidar techniques for measurement of the vertical fluxes of ozone and other pollutants. Doppler lidars have been also used at WPL to study visibility reduction caused by aerosol pollutants at the Grand Canyon, and to investigate dispersion of hazardous emissions near the Rocky Flats nuclear plant.

  18. Chemical Composition and Sources of Coastal Marine Aerosol Particles during the 2008 VOCALS-REx Campaign

    SciTech Connect (OSTI)

    Lee, Y.- N.; Springston, S.; Jayne, John T.; Wang, Jian; Hubbe, John M.; Senum, Gunnar I.; Kleinman, Lawrence I.; Daum, Peter H.

    2014-05-23

    The chemical composition of aerosol particles (Dp 1.5 ?m) was measured over the southeast Pacific Ocean during the VAMOS (Variability of the American Monsoon Systems) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) between 16 October and 15 November 2008 using the US Department of Energy (DOE) G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and of how they interact with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL) aerosol mass was dominated by non-sea-salt SO2?4, followed by Na+, Cl?, Org (total organics), NH+4 , and NO?3 , in decreasing order of importance; CH3SO?3 (MSA), Ca2+, and K+ rarely exceeded their limits of detection. Aerosols were strongly acidic with a NH+4 to SO2?4 equivalents ratio typically < 0.3. Sea-salt aerosol (SSA) particles, represented by NaCl, exhibited Cl? deficits caused by both HNO3 and H2SO4, but for the most part were externally mixed with particles, mainly SO2?4. SSA contributed only a small fraction of the total accumulation mode particle number concentration. It was inferred that all aerosol species (except SSA) were of predominantly continental origin because of their strong land-to-sea concentration gradient. Comparison of relative changes in median values suggests that (1) an oceanic source of NH3 is present between 72 W and 76 W, (2) additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31 S, with possible cloud processing, and (3) free tropospheric (FT) contributions to MBL gas and aerosol concentrations were negligible. The very low levels of CH3SO?3 observed as well as the correlation between SO2?4 and NO?3 (which is thought primarily anthropogenic) suggest a limited contribution of DMS to SO2?4 aerosol production during VOCALS.

  19. Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K. M.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2015-07-24

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased duringmore » photo-oxidation, and the final OA OSc ranged from -0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  20. Morphological and chemical changes of aerosolized E. coli treated with a dielectric barrier discharge

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Romero-Mangado, Jaione; Nordlund, Dennis; Soberon, Felipe; Deane, Graham; Maughan, Kevin; Sainio, Sami; Singh, Gurusharan; Daniels, Stephen; Saunders, Ian T.; Loftus, David; et al

    2016-02-12

    This paper presents the morphological and chemical modification of the cell structure of aerosolized Escherichia coli treated with a dielectric barrier discharge (DBD). Exposure to DBD results in severe oxidation of the bacteria, leading to the formation of hydroxyl groups and carbonyl groups and a significant reduction in amine functionalities and phosphate groups. Near edge x-ray absorption fine structure(NEXAFS) measurements confirm the presence of additional oxide bonds upon DBD treatment, suggesting oxidation of the outer layer of the cell wall. Electron microscopy images show that the bacteria undergo physical distortion to varying degrees, resulting in deformation of the bacterial structure.more » The electromagnetic field around the DBD coil causes severe damage to the cell structure, possibly resulting in leakage of vital cellular materials. The oxidation and chemical modification of the bacterial components are evident from the Fourier transform infrared spectroscopy and NEXAFS results. The bacterial reculture experiments confirm inactivation of airborne E. coli upon treating with DBD.« less

  1. Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-09-14

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed tomore » OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient number of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and is not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide range of solubilities.« less

  2. Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Slade, J. H.; Thalman, R.; Wang, J.; Knopf, D. A.

    2015-03-06

    Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH andmore » O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.« less

  3. The Statistical Evolution of Multiple Generations of Oxidation Products in the Photochemical Aging of Chemically Reduced Organic Aerosol

    SciTech Connect (OSTI)

    Wilson, Kevin R.; Smith, Jared D.; Kessler, Sean; Kroll, Jesse H.

    2011-10-03

    The heterogeneous reaction of hydroxyl radicals (OH) with squalane and bis(2-ethylhexyl) sebacate (BES) particles are used as model systems to examine how distributions of reactionproducts evolve during the oxidation of chemically reduced organic aerosol. A kinetic model of multigenerational chemistry, which is compared to previously measured (squalane) and new(BES) experimental data, reveals that it is the statistical mixtures of different generations of oxidation products that control the average particle mass and elemental composition during thereaction. The model suggests that more highly oxidized reaction products, although initially formed with low probability, play a large role in the production of gas phase reaction products.In general, these results highlight the importance of considering atmospheric oxidation as a statistical process, further suggesting that the underlying distribution of molecules could playimportant roles in aerosol formation as well as in the evolution of key physicochemical properties such as volatility and hygroscopicity.

  4. The darkening of zinc yellow: XANES speciation of chromium in artist;s paints after light and chemical exposures

    SciTech Connect (OSTI)

    Zanella, Luciana; Casadio, Francesca; Gray, Kimberly A.; Warta, Richard; Ma, Qing; Gaillard, Jean-Franois

    2012-03-14

    The color darkening of selected brushstrokes of the masterpiece A Sunday on La Grande Jatte - 1884 (by Georges Seurat) has been attributed to the alteration of the chromate pigment zinc yellow. The pigment originally displays a bright greenish-yellow color but may undergo, after aging, darkening to a dull, ocher tone. We used XANES to probe the oxidation state of Cr on paint reconstructions, and show that color changes are associated with the reduction of Cr(VI) to Cr(III). Paint mixtures containing the pigment and linseed oil to mimic mixtures used in La Grande Jatte were subjected to artificial aging in the presence of light, SO{sub 2}, and variable air humidity - 50 and 90% relative humidity. High relative humidity led to the largest degree of Cr(VI) reduction whereas low relative humidity promoted light-induced alterations. These results are corroborated by visible reflectance measurements on the same laboratory samples and contribute to a better understanding of the chemical reactivity of chromate pigments, which are present in many historical works of art.

  5. Methyl Formate Oxidation: Speciation Data, Laminar Burning Velocities, Ignition Delay Times and a Validated Chemical Kinetic Model

    SciTech Connect (OSTI)

    Dooley, S.; Burke, M. P.; Chaos, M.; Stein, Y.; Dryer, F. L.; Zhukov, V. P.; Finch, O.; Simmie, J. M.; Curran, H. J.

    2010-07-16

    The oxidation of methyl formate (CH{sub 3}OCHO) has been studied in three experimental environments over a range of applied combustion relevant conditions: 1. A variable-pressure flow reactor has been used to quantify reactant, major intermediate and product species as a function of residence time at 3 atm and 0.5% fuel concentration for oxygen/fuel stoichiometries of 0.5, 1.0, and 1.5 at 900 K, and for pyrolysis at 975 K. 2. Shock tube ignition delays have been determined for CH{sub 3}OCHO/O{sub 2}/Ar mixtures at pressures of ? 2.7, 5.4, and 9.2 atm and temperatures of 12751935 K for mixture compositions of 0.5% fuel (at equivalence ratios of 1.0, 2.0, and 0.5) and 2.5% fuel (at an equivalence ratio of 1.0). 3. Laminar burning velocities of outwardly propagating spherical CH{sub 3}OCHO/air flames have been determined for stoichiometries ranging from 0.81.6, at atmospheric pressure using a pressure-release-type high-pressure chamber. A detailed chemical kinetic model has been constructed, validated against, and used to interpret these experimental data. The kinetic model shows that methyl formate oxidation proceeds through concerted elimination reactions, principally forming methanol and carbon monoxide as well as through bimolecular hydrogen abstraction reactions. The relative importance of elimination versus abstraction was found to depend on the particular environment. In general, methyl formate is consumed exclusively through molecular decomposition in shock tube environments, while at flow reactor and freely propagating premixed flame conditions, there is significant competition between hydrogen abstraction and concerted elimination channels. It is suspected that in diffusion flame configurations the elimination channels contribute more significantly than in premixed environments.

  6. Aging of secondary organic aerosol from small aromatic VOCs. Changes in chemical composition, mass yield, volatility and hygroscopicity

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Hildebrandt Ruiz, L.; Paciga, A. L.; Cerully, K.; Nenes, A.; Donahue, N. M.; Pandis, S. N.

    2014-12-12

    Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form and transform SOA from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx. The effects of chemical aging on organic aerosol (OA) composition, mass yield, volatility and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state OSC) and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSmore » C ranged from -0.29 to 0.45 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.« less

  7. Experimental determination of the speciation, partitioning, and release of perrhenate as a chemical surrogate for pertechnetate from a sodalite-bearing multiphase ceramic waste form

    SciTech Connect (OSTI)

    Pierce, Eric M.; Lukens, Wayne W.; Fitts, Jeff. P.; Jantzen, Carol. M.; Tang, G.

    2013-12-01

    A key component to closing the nuclear fuel cycle is the storage and disposition of nuclear waste in geologic systems. Multiphase ceramic waste forms have been studied extensively as a potential host matrix for nuclear waste. Understanding the speciation, partitioning, and release behavior of radionuclides immobilized in multiphase ceramic waste forms is a critical aspect of developing the scientific and technical basis for nuclear waste management. In this study, we evaluated a sodalite-bearing multiphase ceramic waste form (i.e., fluidized-bed steam reform sodium aluminosilicate [FBSR NAS] product) as a potential host matrix for long-lived radionuclides, such as technetium (99Tc). The FBSR NAS material consists primarily of nepheline (ideally NaAlSiO4), anion-bearing sodalites (ideally M8[Al6Si6O24]X2, where M refers to alkali and alkaline earth cations and X refers to monovalent anions), and nosean (ideally Na8[AlSiO4]6SO4). Bulk X-ray absorption fine structure analysis of the multiphase ceramic waste form, suggest rhenium (Re) is in the Re(VII) oxidation state and has partitioned to a Re-bearing sodalite phase (most likely a perrhenate sodalite Na8[Al6Si6O24](ReO4)2). Rhenium was added as a chemical surrogate for 99Tc during the FBSR NAS synthesis process. The weathering behavior of the FBSR NAS material was evaluated under hydraulically unsaturated conditions with deionized water at 90 ?C. The steady-state Al, Na, and Si concentrations suggests the weathering mechanisms are consistent with what has been observed for other aluminosilicate minerals and include a combination of ion exchange, network hydrolysis, and the formation of an enriched-silica surface layer or phase. The steady-state S and Re concentrations are within an order of magnitude of the nosean and perrhenate sodalite solubility, respectively. The order of magnitude difference between the observed and predicted concentration for Re and S may be associated with the fact that the anion-bearing sodalites contained in the multiphase ceramic matrix are present as mixed-anion sodalite phases. These results suggest the multiphase FBSR NAS material may be a viable host matrix for long-lived, highly mobilie radionuclides which is a critical aspect in the management of nuclear waste.

  8. Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

    SciTech Connect (OSTI)

    Thornton, Joel

    2015-01-26

    The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

  9. Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Xu, L.; Williams, L. R.; Young, D. E.; Allan, J. D.; Coe, H.; Massoli, P.; Fortner, E.; Chhabra, P.; Herndon, S.; Brooks, W. A.; et al

    2015-08-28

    The composition of PM1 (particulate matter with diameter less than 1 ?m) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two High-Resolution Time-of-Flight Aerosol Mass Spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the sources of OA are distinctly different. The concentration ofmoresolid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC, measured by a soot-particle aerosol mass spectrometer) only accounts for less

  10. Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; Brune, W. H.; Hunter, J. F.; Kroll, J. H.; Cummings, M. J.; Brogan, J. F.; Parmar, Y.; Worsnop, D. R.; et al

    2015-03-18

    We performed a systematic intercomparison study of the chemistry and yields of secondary organic aerosol (SOA) generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0 × 108 to 2.2 × 1010 molec cm-3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2 × 106 to 2 × 107 molec cm-3 over exposure times of several hours. The OH concentration in themore » chamber experiments is close to that found in the atmosphere, but the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. In most cases, for a specific SOA type the most-oxidized chamber SOA and the least-oxidized flow reactor SOA have similar mass spectra, oxygen-to-carbon and hydrogen-to-carbon ratios, and carbon oxidation states at integrated OH exposures between approximately 1 × 1011 and 2 × 1011 molec cm-3 s, or about 1–2 days of equivalent atmospheric oxidation. This observation suggests that in the range of available OH exposure overlap for the flow reactor and chambers, SOA elemental composition as measured by an aerosol mass spectrometer is similar whether the precursor is exposed to low OH concentrations over long exposure times or high OH concentrations over short exposure times. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of sulfate seed particles on isoprene SOA yield measurements was examined in the flow reactor. The studies show that seed particles increase the yield of SOA produced in flow reactors by a factor of 3 to 5 and may also account in part for higher SOA yields obtained in the chambers, where seed particles are routinely used.« less

  11. THE APPLICATION OF SINGLE PARTICLE AEROSOL MASS SPECTROMETRY FOR THE DETECTION AND IDENTIFICATION OF HIGH EXPLOSIVES AND CHEMICAL WARFARE AGENTS

    SciTech Connect (OSTI)

    Martin, A

    2006-10-23

    Single Particle Aerosol Mass Spectrometry (SPAMS) was evaluated as a real-time detection technique for single particles of high explosives. Dual-polarity time-of-flight mass spectra were obtained for samples of 2,4,6-trinitrotoluene (TNT), 1,3,5-trinitro-1,3,5-triazinane (RDX), and pentaerythritol tetranitrate (PETN); peaks indicative of each compound were identified. Composite explosives, Comp B, Semtex 1A, and Semtex 1H were also analyzed, and peaks due to the explosive components of each sample were present in each spectrum. Mass spectral variability with laser fluence is discussed. The ability of the SPAMS system to identify explosive components in a single complex explosive particle ({approx}1 pg) without the need for consumables is demonstrated. SPAMS was also applied to the detection of Chemical Warfare Agent (CWA) simulants in the liquid and vapor phases. Liquid simulants for sarin, cyclosarin, tabun, and VX were analyzed; peaks indicative of each simulant were identified. Vapor phase CWA simulants were adsorbed onto alumina, silica, Zeolite, activated carbon, and metal powders which were directly analyzed using SPAMS. The use of metal powders as adsorbent materials was especially useful in the analysis of triethyl phosphate (TEP), a VX stimulant, which was undetectable using SPAMS in the liquid phase. The capability of SPAMS to detect high explosives and CWA simulants using one set of operational conditions is established.

  12. DEVELOPMENT OF FINE PARTICULATE EMISSION FACTORS AND SPECIATION PROFILES FOR OIL AND GAS-FIRED COMBUSTION SYSTEMS

    SciTech Connect (OSTI)

    Glenn C. England

    2004-10-20

    In 1997, the United States Environmental Protection Agency (EPA) promulgated new National Ambient Air Quality Standards (NAAQS) for particulate matter, including for the first time particles with aerodynamic diameter smaller than 2.5 micrometers ({micro}m) referred to as PM2.5. PM2.5 in the atmosphere also contributes to reduced atmospheric visibility, which is the subject of existing rules for siting emission sources near Class 1 areas and new Regional Haze rules. There are few existing data regarding emissions and characteristics of fine aerosols from oil, gas and power generation industry combustion sources, and the information that is available is generally outdated and incomplete. Traditional stationary source air emission sampling methods tend to underestimate or overestimate the contribution of the source to ambient aerosols because they do not properly account for primary aerosol formation, which occurs after the gases leave the stack. Primary aerosol includes both filterable particles that are solid or liquid aerosols at stack temperature plus those that form as the stack gases cool through mixing and dilution processes in the plume downwind of the source. These deficiencies in the current methods can have significant impacts on regulatory decision-making. PM2.5 measurement issues were extensively reviewed by the American Petroleum Institute (API) (England et al., 1998), and it was concluded that dilution sampling techniques are more appropriate for obtaining a representative particulate matter sample from combustion systems for determining PM2.5 emission rate and chemical speciation. Dilution sampling is intended to collect aerosols including those that condense and/or react to form solid or liquid aerosols as the exhaust plume mixes and cools to near-ambient temperature immediately after the stack discharge. These techniques have been widely used in recent research studies. For example, Hildemann et al. (1994) and McDonald et al. (1998) used filtered ambient air to dilute the stack gas sample followed by 80-90 seconds residence time to allow aerosol formation and growth to stabilize prior to sample collection and analysis. More accurate and complete emissions data generated using the methods developed in this program will enable more accurate source-receptor and source apportionment analysis for PM2.5 National Ambient Air Quality Standards (NAAQS) implementation and streamline the environmental assessment of oil, gas and power production facilities. The overall goals of this program were to: (1) Develop improved dilution sampling technology and test methods for PM2.5 mass emissions and speciation measurements, and compare results obtained with dilution and traditional stationary source sampling methods. (2) Develop emission factors and speciation profiles for emissions of fine particulate matter, especially organic aerosols, for use in source-receptor and source apportionment analyses. (3) Identify and characterize PM2.5 precursor compound emissions that can be used in source-receptor and source apportionment analyses.

  13. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Mikhailov, E. F.; Mironov, G. N.; Pöhlker, C.; Chi, X.; Krüger, M. L.; Shiraiwa, M.; Förster, J. -D.; Pöschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; et al

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water solublemore » fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κv, ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv ≈ 0.15) and a Colorado boreal forest (κv ≈ 0.16). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv, p. The obtained κv, p values overestimate the experimental FDHA-KIM-derived κv, ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be partly explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (>300 nm) and supermicron aerosol particles possess core-shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.« less

  14. Chemical composition, microstructure, and hygroscopic properties of aerosol particles at the Zotino Tall Tower Observatory (ZOTTO), Siberia, during a summer campaign

    SciTech Connect (OSTI)

    Mikhailov, E. F.; Mironov, G. N.; Phlker, C.; Chi, X.; Krger, M. L.; Shiraiwa, M.; Frster, J. -D.; Pschl, U.; Vlasenko, S. S.; Ryshkevich, T. I.; Weigand, M.; Kilcoyne, A. L. D.; Andreae, M. O.

    2015-03-16

    In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61 N; 89 E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical composition of aerosol particles were analyzed by X-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38% of PM in the accumulation mode and coarse mode, respectively. The water soluble fraction of organic matter was estimated to be 52 and 8% of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34% in the accumulation vs. ~ 47% in the coarse mode.

    The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 599.4% RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same RH, starting at ~ 70%, while efflorescence occurred at different humidities, i.e., at ~ 35% RH for submicron particles vs. ~ 50% RH for supermicron particles. This ~ 15% RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments.

    The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 599.4% RH range. Based on KIM, the volume-based hygroscopicity parameter, ?v, was calculated. The ?v, ws value related to the water soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained ?v, ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (?v ≈ 0.15) and a Colorado boreal forest (?v ≈ 0.16).

    We used the ZdanovskiiStokesRobinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, ?v, p. The obtained ?v, p values overestimate the experimental FDHA-KIM-derived ?v, ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be partly explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (>300 nm) and supermicron aerosol particles possess core-shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10?12 cm2 s?1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second time scales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer

  15. Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Faiola, C. L.; Wen, M.; VanReken, T. M.

    2015-04-01

    The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- andmore » post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.« less

  16. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused particle growth while...

  17. Comparison of secondary organic aerosol formed with an aerosol flow reactor and environmental reaction chambers: effect of oxidant concentration, exposure time and seed particles on chemical composition and yield

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; Brune, W. H.; Hunter, J. F.; Kroll, J. H.; Cummings, M. J.; Brogan, J. F.; Parmar, Y.; Worsnop, D. R.; et al

    2014-12-02

    We performed a systematic intercomparison study of the chemistry and yields of SOA generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0×108 to 2.2×1010 molec cm-3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2×106 to 2×107 molec cm-3 over exposure times of several hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, butmore » the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. A linear correlation analysis of the mass spectra (m=0.91–0.92, r2=0.93–0.94) and carbon oxidation state (m=1.1, r2=0.58) of SOA produced in the flow reactor and environmental chambers for OH exposures of approximately 1011 molec cm-3 s suggests that the composition of SOA produced in the flow reactor and chambers is the same within experimental accuracy as measured with an aerosol mass spectrometer. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors, rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of sulfate seed particles on isoprene SOA yield measurements was examined in the flow reactor. The studies show that seed particles increase the yield of SOA produced in flow reactors by a factor of 3 to 5 and may also account in part for higher SOA yields obtained in the chambers, where seed particles are routinely used.« less

  18. Aerosol Oxidation Speeds Up in Smoggy Air

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Oxidation Speeds Up in Smoggy Air Aerosol Oxidation Speeds Up in Smoggy Air Print Wednesday, 17 February 2016 11:37 Organic aerosols (nanometer-sized liquid or solid particles suspended in air) are important constituents of the troposphere, and their chemistry has large-scale impacts on climate, pollution, and health. Accurate predictions of these aerosol impacts require a robust microphysical understanding of all relevant chemical reaction mechanisms and time scales, including those

  19. Speciation of Uranium in Biologically Reduced Sediments in the Old Rifle

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aquifer | Stanford Synchrotron Radiation Lightsource Speciation of Uranium in Biologically Reduced Sediments in the Old Rifle Aquifer Wednesday, May 16, 2012 - 1:30pm SSRL Conference Room 137-322 Juan S. Lezama Pacheco The speciation and dynamics of Uranium(IV) in naturally and artificially bioreduced sediments, as well as its local nanometer-to-millimeter scale physical and chemical environment, controls its stability, susceptibility to oxidation, and subsequent transport behavior in

  20. Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge

    SciTech Connect (OSTI)

    Moffet, Ryan C.; Henn, Tobias R.; Laskin, Alexander; Gilles, Marry K.

    2010-10-01

    We have developed an automated data analysis method for atmospheric particles using scanning transmission X-ray microscopy coupled with near edge X-ray fine structure spectroscopy (STXM/NEXAFS). This method is applied to complex internally mixed submicron particles containing organic and inorganic material. Several algorithms were developed to exploit NEXAFS spectral features in the energy range from 278-320 eV for quantitative mapping of the spatial distribution of elemental carbon, organic carbon, potassium, and non-carbonaceous elements in particles of mixed composition. This energy range encompasses the carbon K-edge and potassium L2 and L3 edges. STXM/NEXAFS maps of different chemical components were complemented with a subsequent analysis using elemental maps obtained by scanning electron microscopy coupled with energy dispersive X-ray analysis (SEM/EDX). We demonstrate application of the automated mapping algorithms for data analysis and the statistical classification of particles.

  1. Chemistry of α-pinene and naphthalene oxidation products generated in a Potential Aerosol Mass (PAM) chamber as measured by acetate chemical ionization mass spectrometry

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Chhabra, P. S.; Lambe, A. T.; Canagaratna, M. R.; Stark, H.; Jayne, J. T.; Onasch, T. B.; Davidovits, P.; Kimmel, J. R.; Worsnop, D. R.

    2014-07-01

    Recent developments in high resolution, time-of-flight chemical ionization mass spectrometry (HR-ToF-CIMS) have made possible the direct detection of atmospheric organic compounds in real-time with high sensitivity and with little or no fragmentation, including low volatility, highly oxygenated organic vapors that are precursors to secondary organic aerosol formation. Here, for the first time, we examine gas-phase O3 and OH oxidation products of α-pinene and naphthalene formed in the PAM flow reactor with an HR-ToF-CIMS using acetate reagent ion chemistry. Integrated OH exposures ranged from 1.2 × 1011 to 9.7 × 1011 molec cm−3 s, corresponding to approximately 1.0 to 7.5 daysmore » of equivalent atmospheric oxidation. Measured gas-phase organic acids are similar to those previously observed in environmental chamber studies. For both precursors, we find that acetate-CIMS spectra capture both functionalization (oxygen addition) and fragmentation (carbon loss) as a function of OH exposure. The level of fragmentation is observed to increase with increased oxidation. We present a method that estimates vapor pressures of organic molecules using the measured O/C ratio, H/C ratio, and carbon number for each compound detected by the CIMS. The predicted condensed-phase SOA average acid yields and O/C and H/C ratios agree within uncertainties with previous AMS measurements and ambient CIMS results. While acetate reagent ion chemistry is used to selectively measure organic acids, in principle this method can be applied to additional reagent ion chemistries depending on the application.« less

  2. Aerosol Oxidation Speeds Up in Smoggy Air

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Oxidation Speeds Up in Smoggy Air Print Organic aerosols (nanometer-sized liquid or solid particles suspended in air) are important constituents of the troposphere, and their chemistry has large-scale impacts on climate, pollution, and health. Accurate predictions of these aerosol impacts require a robust microphysical understanding of all relevant chemical reaction mechanisms and time scales, including those involving highly reactive free-radical molecules. However, detailed modeling is

  3. Aerosol Oxidation Speeds Up in Smoggy Air

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Oxidation Speeds Up in Smoggy Air Print Organic aerosols (nanometer-sized liquid or solid particles suspended in air) are important constituents of the troposphere, and their chemistry has large-scale impacts on climate, pollution, and health. Accurate predictions of these aerosol impacts require a robust microphysical understanding of all relevant chemical reaction mechanisms and time scales, including those involving highly reactive free-radical molecules. However, detailed modeling is

  4. Aerosol Oxidation Speeds Up in Smoggy Air

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Oxidation Speeds Up in Smoggy Air Print Organic aerosols (nanometer-sized liquid or solid particles suspended in air) are important constituents of the troposphere, and their chemistry has large-scale impacts on climate, pollution, and health. Accurate predictions of these aerosol impacts require a robust microphysical understanding of all relevant chemical reaction mechanisms and time scales, including those involving highly reactive free-radical molecules. However, detailed modeling is

  5. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused

  6. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused

  7. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused

  8. Aerosol Oxidation Speeds Up in Smoggy Air

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Oxidation Speeds Up in Smoggy Air Print Organic aerosols (nanometer-sized liquid or solid particles suspended in air) are important constituents of the troposphere, and their chemistry has large-scale impacts on climate, pollution, and health. Accurate predictions of these aerosol impacts require a robust microphysical understanding of all relevant chemical reaction mechanisms and time scales, including those involving highly reactive free-radical molecules. However, detailed modeling is

  9. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused

  10. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the ALS have revealed chemical reactions on and in atmospheric aerosol particles that caused

  11. Geochemical Speciation Mass Transfer

    Energy Science and Technology Software Center (OSTI)

    1985-12-01

    PHREEQC is designed to model geochemical reactions. Based on an ion association aqueous model, PHREEQC can calculate pH, redox potential, and mass transfer as a function of reaction progress. It can be used to describe geochemical processes for both far-field and near-field performance assessment and to evaluate data acquisition needs and test data. It can also calculate the composition of solutions in equilibrium with multiple phases. The data base, including elements, aqueous species, and mineralmore » phases, is independent of the program and is completely user-definable. PHREEQC requires thermodynamic data for each solid, gaseous, or dissolved chemical species being modeled. The two data bases, PREPHR and DEQPAK7, supplied with PHREEQC are for testing purposes only and should not be applied to real problems without first being carefully examined. The conceptual model embodied in PHREEQC is the ion-association model of Pearson and Noronha. In this model a set of mass action equations are established for each ion pair (and controlling solid phases when making mass transfer calculations) along with a set of mass balance equations for each element considered. These sets of equations are coupled using activity coefficient values for each aqueous species and solved using a continued fraction approach for the mass balances combined with a modified Newton-Raphson technique for all other equations. The activity coefficient expressions in PHREEQC include the extended Debye-Huckel, WATEQ Debye-Huckel, and Davies equations from the original United States Geological Survey version of the program. The auxiliary preprocessor program PHTL, which is derived from EQTL, converts EQ3/6 thermodynamic data to PHREEQC format so that the two programs can be compared. PHREEQC can be used to determine solubility limits on the radionuclides present in the waste form. These solubility constraints may be input to the WAPPA leach model.« less

  12. Parameterizing the Mixing State of Complex Submicron Aerosols...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    DA Knopf, MK Gilles, and RC Moffet. 2015. "Chemical imaging of ambient aerosol particles: Observational constraints on mixing state parameterization." Journal of Geophysical...

  13. ARM - Data Announcements Article

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    matrix data collected by the aerosol chemical speciation monitor (ACSM) and multivariate analysis to obtain an estimate of the types of organic aerosols. Currently, time...

  14. ARM - Measurement - Aerosol concentration

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    CSPHOT : Cimel Sunphotometer CPC : Condensation Particle Counter HTDMA : Humidified Tandem Differential Mobility Analyzer IAP : In-situ Aerosol Profiles (Cessna Aerosol Flights)...

  15. Aerosol Characterization Data from the Asian Pacific Regional Aerosol Characterization Project (ACE-Asia)

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    The Aerosol Characterization Experiments (ACE) were designed to increase understanding of how atmospheric aerosol particles affect the Earth's climate system. These experiments integrated in-situ measurements, satellite observations, and models to reduce the uncertainty in calculations of the climate forcing due to aerosol particles and improve the ability of models to predict the influences of aerosols on the Earth's radiation balance. ACE-Asia was the fourth in a series of experiments organized by the International Global Atmospheric Chemistry (IGAC) Program (A Core Project of the International Geosphere Biosphere Program). The Intensive Field Phase for ACE-Asia took place during the spring of 2001 (mid-March through early May) off the coast of China, Japan and Korea. ACE-Asia pursued three specific objectives: 1) Determine the physical, chemical, and radiative properties of the major aerosol types in the Eastern Asia and Northwest Pacific region and investigate the relationships among these properties. 2) Quantify the physical and chemical processes controlling the evolution of the major aerosol types and in particular their physical, chemical, and radiative properties. 3) Develop procedures to extrapolate aerosol properties and processes from local to regional and global scales, and assess the regional direct and indirect radiative forcing by aerosols in the Eastern Asia and Northwest Pacific region [Edited and shortened version of summary at http://data.eol.ucar.edu/codiac/projs?ACE-ASIA]. The Ace-Asia collection contains 174 datasets.

  16. Selenium Speciation and Management in Wet FGD Systems

    SciTech Connect (OSTI)

    Searcy, K; Richardson, M; Blythe, G; Wallschlaeger, D; Chu, P; Dene, C

    2012-02-29

    This report discusses results from bench- and pilot-scale simulation tests conducted to determine the factors that impact selenium speciation and phase partitioning in wet FGD systems. The selenium chemistry in wet FGD systems is highly complex and not completely understood, thus extrapolation and scale-up of these results may be uncertain. Control of operating parameters and application of scrubber additives have successfully demonstrated the avoidance or decrease of selenite oxidation at the bench and pilot scale. Ongoing efforts to improve sample handling methods for selenium speciation measurements are also discussed. Bench-scale scrubber tests explored the impacts of oxidation air rate, trace metals, scrubber additives, and natural limestone on selenium speciation in synthetic and field-generated full-scale FGD liquors. The presence and concentration of redox-active chemical species as well as the oxidation air rate contribute to the oxidation-reduction potential (ORP) conditions in FGD scrubbers. Selenite oxidation to the undesirable selenate form increases with increasing ORP conditions, and decreases with decreasing ORP conditions. Solid-phase manganese [Mn(IV)] appeared to be the significant metal impacting the oxidation of selenite to selenate. Scrubber additives were tested for their ability to inhibit selenite oxidation. Although dibasic acid and other scrubber additives showed promise in early clear liquor (sodium based and without calcium solids) bench-scale tests, these additives did not show strong inhibition of selenite oxidation in tests with higher manganese concentrations and with slurries from full-scale wet FGD systems. In bench-tests with field liquors, addition of ferric chloride at a 250:1 iron-to-selenium mass ratio sorbed all incoming selenite to the solid phase, although addition of ferric salts had no impact on native selenate that already existed in the field slurry liquor sample. As ORP increases, selenite may oxidize to selenate more rapidly than it sorbs to ferric solids. Though it was not possible to demonstrate a decrease in selenium concentrations to levels below the project?¢????s target of 50 ???µg/L during pilot testing, some trends observed in bench-scale testing were evident at the pilot scale. Specifically, reducing oxidation air rate and ORP tends to either retain selenium as selenite in the liquor or shift selenium phase partitioning to the solid phase. Oxidation air flow rate control may be one option for managing selenium behavior in FGD scrubbers. Units that cycle load widely may find it more difficult to impact ORP conditions with oxidation air flow rate control alone. Because decreasing oxidation air rates to the reaction tank showed that all ?¢????new?¢??? selenium reported to the solids, the addition of ferric chloride to the pilot scrubber could not show further improvements in selenium behavior. Ferric chloride addition did shift mercury to the slurry solids, specifically to the fine particles. Several competing pathways may govern the reporting of selenium to the slurry solids: co-precipitation with gypsum into the bulk solids and sorption or co-precipitation with iron into the fine particles. Simultaneous measurement of selenium and mercury behavior suggests a holistic management strategy is best to optimize the fate of both of these elements in FGD waters. Work conducted under this project evaluated sample handling and analytical methods for selenium speciation in FGD waters. Three analytical techniques and several preservation methods were employed. Measurements of selenium speciation over time indicated that for accurate selenium speciation, it is best to conduct measurements on unpreserved, filtered samples as soon after sampling as possible. The capital and operating costs for two selenium management strategies were considered: ferric chloride addition and oxidation air flow rate control. For ferric chloride addition, as migh

  17. Aerosol mobility size spectrometer

    DOE Patents [OSTI]

    Wang, Jian (Port Jefferson, NY); Kulkarni, Pramod (Port Jefferson Station, NY)

    2007-11-20

    A device for measuring aerosol size distribution within a sample containing aerosol particles. The device generally includes a spectrometer housing defining an interior chamber and a camera for recording aerosol size streams exiting the chamber. The housing includes an inlet for introducing a flow medium into the chamber in a flow direction, an aerosol injection port adjacent the inlet for introducing a charged aerosol sample into the chamber, a separation section for applying an electric field to the aerosol sample across the flow direction and an outlet opposite the inlet. In the separation section, the aerosol sample becomes entrained in the flow medium and the aerosol particles within the aerosol sample are separated by size into a plurality of aerosol flow streams under the influence of the electric field. The camera is disposed adjacent the housing outlet for optically detecting a relative position of at least one aerosol flow stream exiting the outlet and for optically detecting the number of aerosol particles within the at least one aerosol flow stream.

  18. Biosensor for metal analysis and speciation

    DOE Patents [OSTI]

    Aiken, Abigail M.; Peyton, Brent M.; Apel, William A.; Petersen, James N.

    2007-01-30

    A biosensor for metal analysis and speciation is disclosed. The biosensor comprises an electron carrier immobilized to a surface of an electrode and a layer of an immobilized enzyme adjacent to the electrode. The immobilized enzyme comprises an enzyme having biological activity inhibited by a metal to be detected by the biosensor.

  19. Characterization of Technetium Speciation in Cast Stone

    SciTech Connect (OSTI)

    Um, Wooyong; Jung, Hun Bok; Wang, Guohui; Westsik, Joseph H.; Peterson, Reid A.

    2013-11-11

    This report describes the results from laboratory tests performed at Pacific Northwest National Laboratory (PNNL) for the U.S. Department of Energy (DOE) EM-31 Support Program (EMSP) subtask, Production and Long-Term Performance of Low Temperature Waste Forms to provide additional information on technetium (Tc) speciation characterization in the Cast Stone waste form. To support the use of Cast Stone as an alternative to vitrification for solidifying low-activity waste (LAW) and as the current baseline waste form for secondary waste streams at the Hanford Site, additional understanding of Tc speciation in Cast Stone is needed to predict the long-term Tc leachability from Cast Stone and to meet the regulatory disposal-facility performance requirements for the Integrated Disposal Facility (IDF). Characterizations of the Tc speciation within the Cast Stone after leaching under various conditions provide insights into how the Tc is retained and released. The data generated by the laboratory tests described in this report provide both empirical and more scientific information to increase our understanding of Tc speciation in Cast Stone and its release mechanism under relevant leaching processes for the purpose of filling data gaps and to support the long-term risk and performance assessments of Cast Stone in the IDF at the Hanford Site.

  20. Speciation of Energetic Materials on a Microcantilever Using Surface Reduction

    SciTech Connect (OSTI)

    Yi, Dechang; Senesac, Larry R; Thundat, Thomas George

    2008-01-01

    Although microcantilevers have been used to detect explosives with extremely high sensitivity using variations in adsorption-induced bending and resonance frequency, obtaining selectivity remains a challenge. Reversible chemoselectivity at ambient temperatures based on receptor-based detection provides only limited selectivity due to the generality of chemical interactions. The oxygen imbalance in secondary explosives presents a means to achieve receptor-free speciation of explosives using surface reduction of adsorbed molecules. We demonstrate highly selective and real-time detection of Trinitrotoluene (TNT) using a copper oxide-coated cantilever with a surface reduction approach. Not only can this technique exclusively differentiate explosives from nonexplosives, but also it has the potential to specify individual explosives such as TNT, pentaerythritol tetranitrate (PETN), and RDX. This technique together with receptor-based detection techniques provides a multimodal approach for achieving very high selectivity.

  1. Aerosol Extinction Profiles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and Thermodynamic Responses to Uncertainty in Aerosol Extinction Profiles For original submission and image(s), see ARM Research Highlights http://www.arm.gov/science/highlights/ Research Highlight Aerosol radiative effects are of great importance for climate simulations over South Asia. For quantifying aerosol direct radiative effect, aerosol optical depth (AOD) and single scattering albedo (SSA) are often compared with observations. These comparisons have revealed large AOD underestimation and

  2. ARM - Measurement - Aerosol scattering

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    : Nephelometer PASS : Photoacoustic Soot Spectrometer RL : Raman Lidar TDMA : Tandem Differential Mobility Analyzer Field Campaign Instruments AMT : Aerosol Modeling...

  3. Solid aerosol generator

    DOE Patents [OSTI]

    Prescott, D.S.; Schober, R.K.; Beller, J.

    1992-03-17

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration is disclosed. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates. 2 figs.

  4. Solid aerosol generator

    DOE Patents [OSTI]

    Prescott, Donald S. (Shelley, ID); Schober, Robert K. (Midwest City, OK); Beller, John (Idaho Falls, ID)

    1992-01-01

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates.

  5. Improved solid aerosol generator

    DOE Patents [OSTI]

    Prescott, D.S.; Schober, R.K.; Beller, J.

    1988-07-19

    An improved solid aerosol generator used to produce a gas borne stream of dry, solid particles of predetermined size and concentration. The improved solid aerosol generator nebulizes a feed solution of known concentration with a flow of preheated gas and dries the resultant wet heated aerosol in a grounded, conical heating chamber, achieving high recovery and flow rates. 2 figs.

  6. DOE/SC-ARM-10-018 CARES: Carbonaceous Aerosol and Radiative

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    chemical environments via an integrated approach to field, laboratory, and modeling studies. Field observations show that tropospheric aerosol particles can be composed of a...

  7. ARM - Measurement - Inorganic chemical composition

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govMeasurementsInorganic chemical composition ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Inorganic chemical composition The chemical composition of an aerosol, with the exception of those with hydrocarbons, and usually including carbides, oxides of carbon, metallic carbonates, carbon sulfur compounds, and carbon nitrogen compounds. Categories Aerosols Instruments The above measurement is

  8. ARM - AOS Aerosol Properties Plots

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ViewersAOS Aerosol Properties Plots XDC Data Viewers Aerosol Properties Plots SGP AMF NSA (BRW) AOS Aerosol Properties Plots These plots are designed to provide a quick look at the measured aerosol properties or review current station operations. Be aware that they are raw unedited data. Do not quote and cite. Aerosol Properties Plots SGP AMF NSA (BRW)

  9. Thermally Speciated Mercury in Mineral Exploration | Open Energy...

    Open Energy Info (EERE)

    Speciated Mercury in Mineral Exploration Abstract Abstract unavailable. Author S.C. Smith Conference IGES; Dublin, CA; 20030901 Published IGES, 2003 DOI Not Provided Check...

  10. Laboratory Product Speciation Studies of the LNT + in situ SCR...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Laboratory Product Speciation Studies of the LNT + in situ SCR NOx Emission Control Concept Understanding the detailed chemistry of Nox Reduction across the combined LNT+SCR ...

  11. Chemical Imaging Analysis of Environmental Particles Using the Focused Ion Beam/Scanning Electron Microscopy Technique: Microanalysis Insights into Atmospheric Chemistry of Fly Ash

    SciTech Connect (OSTI)

    Chen, Haihan; Grassian, Vicki H.; Saraf, Laxmikant V.; Laskin, Alexander

    2013-01-21

    Airborne fly ash from coal combustion may represent a source of bioavailable iron (Fe) in the open ocean. However, few studies have been made focusing on Fe speciation and distribution in coal fly ash. In this study, chemical imaging of fly ash has been performed using a dual-beam FIB/SEM (focused ion beam/scanning electron microscope) system for a better understanding of how simulated atmospheric processing modify the morphology, chemical compositions and element distributions of individual particles. A novel approach has been applied for cross-sectioning of fly ash specimen with a FIB in order to explore element distribution within the interior of individual particles. Our results indicate that simulated atmospheric processing causes disintegration of aluminosilicate glass, a dominant material in fly ash particles. Aluminosilicate-phase Fe in the inner core of fly ash particles is more easily mobilized compared with oxide-phase Fe present as surface aggregates on fly ash spheres. Fe release behavior depends strongly on Fe speciation in aerosol particles. The approach for preparation of cross-sectioned specimen described here opens new opportunities for particle microanalysis, particular with respect to inorganic refractive materials like fly ash and mineral dust.

  12. ARM - Measurement - Aerosol extinction

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    extinction ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Aerosol extinction The removal of radiant energy from an incident beam by the process of aerosol absorption and/or scattering. Categories Aerosols Instruments The above measurement is considered scientifically relevant for the following instruments. Refer to the datastream (netcdf) file headers of each instrument for a list of all available

  13. ARM - Measurement - Aerosol image

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    image ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Aerosol image Images of aerosols from which one can derive characteristics such as size and shape. Categories Aerosols Instruments The above measurement is considered scientifically relevant for the following instruments. Refer to the datastream (netcdf) file headers of each instrument for a list of all available measurements, including those

  14. Two-Column Aerosol Project

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Column Aerosol Project Tiny particles in the sky known as "aerosols" come in many forms-dust, soot, and sea salt, for example. Depending on the type of aerosol, it can either...

  15. Aerosol remote sensing in polar regions

    SciTech Connect (OSTI)

    Tomasi, Claudio; Kokhanovsky, Alexander A.; Lupi, Angelo; Ritter, Christoph; Smirnov, Alexander; O'Neill, Norman T.; Stone, Robert S.; Holben, Brent N.; Nyeki, Stephan; Mazzola, Mauro; Lanconelli, Christian; Vitale, Vito; Stebel, Kerstin; Aaltonen, Veijo; de Leeuw, Gerrit; Rodriguez, Edith; Herber, Andreas B.; Radionov, Vladimir F.; Zielinski, Tymon; Petelski, Tomasz; Sakerin, Sergey M.; Kabanov, Dmitry M.; Xue, Yong; Mei, Linlu; Istomina, Larysa; Wagener, Richard; McArthur, Bruce; Sobolewski, Piotr S.; Kivi, Rigel; Courcoux, Yann; Larouche, Pierre; Broccardo, Stephen; Piketh, Stuart J.

    2015-01-01

    Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness ?(?) at visible and near-infrared wavelengths, from which best-fit values of ngstrm's exponent ? were calculated. Analysing these data, the monthly mean values of ?(0.50 ?m) and ? and the relative frequency histograms of the daily mean values of both parameters were determined for winterspring and summerautumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of ? versus ?(0.50 ?m) showed: (i) a considerable increase in ?(0.50 ?m) for the Arctic aerosol from summer to winterspring, without marked changes in ?; and (ii) a marked increase in ?(0.50 ?m) passing from the Antarctic Plateau to coastal sites, whereas ? decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of ?(?) and ? at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterise vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-lesund. Satellite-based MODIS, MISR, and AATSR retrievals of ?(?) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surfaceatmosphere system over polar regions.

  16. Particulate Matter Aerosols

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    The study of atmospheric aerosols is important because of its adverse effects on health, air quality, visibility, cultural heritage, and Earth's radiation balance. Techniques that...

  17. ARM - Measurement - Aerosol composition

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    quality assurance purposes. ARM Instruments PILS : Particle Into Liquid Sampler TDMA : Tandem Differential Mobility Analyzer Field Campaign Instruments AEROSMASSSPEC : Aerosol Mass...

  18. ARM - Measurement - Aerosol backscattered radiation

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    RLPROF : Raman LIDAR Vertical Profiles UW-AIR : University of Washington Airborne Aerosol Instruments Value-Added Products AIP : Aerosol Intensive Properties (Process) AIP1OGREN :...

  19. ARM - Measurement - Aerosol optical properties

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    : Aerosol optical properties The optical properties of aerosols, including asymmetry factor, phase-function, single-scattering albedo, refractive index, and backscatter...

  20. Spectroscopic and Microspectroscopic Investigation of Arsenic Speciation

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and Distribution in Mine Wastes | Stanford Synchrotron Radiation Lightsource Spectroscopic and Microspectroscopic Investigation of Arsenic Speciation and Distribution in Mine Wastes Monday, June 30, 2014 Figure 1. Micro-XRF maps of the (a) 250-500 µm, (b) 75-125 µm, (c) 32-45 µm, and (d) <20 µm size fractions of the Descarga mine tailings sample. Arsenic and iron Ka fluorescence signals are shown in red and blue, respectively; purple hues indicate particles that contain both elements.

  1. Direct Aerosol Forcing Uncertainty

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Mccomiskey, Allison

    2008-01-15

    Understanding sources of uncertainty in aerosol direct radiative forcing (DRF), the difference in a given radiative flux component with and without aerosol, is essential to quantifying changes in Earth's radiation budget. We examine the uncertainty in DRF due to measurement uncertainty in the quantities on which it depends: aerosol optical depth, single scattering albedo, asymmetry parameter, solar geometry, and surface albedo. Direct radiative forcing at the top of the atmosphere and at the surface as well as sensitivities, the changes in DRF in response to unit changes in individual aerosol or surface properties, are calculated at three locations representing distinct aerosol types and radiative environments. The uncertainty in DRF associated with a given property is computed as the product of the sensitivity and typical measurement uncertainty in the respective aerosol or surface property. Sensitivity and uncertainty values permit estimation of total uncertainty in calculated DRF and identification of properties that most limit accuracy in estimating forcing. Total uncertainties in modeled local diurnally averaged forcing range from 0.2 to 1.3 W m-2 (42 to 20%) depending on location (from tropical to polar sites), solar zenith angle, surface reflectance, aerosol type, and aerosol optical depth. The largest contributor to total uncertainty in DRF is usually single scattering albedo; however decreasing measurement uncertainties for any property would increase accuracy in DRF. Comparison of two radiative transfer models suggests the contribution of modeling error is small compared to the total uncertainty although comparable to uncertainty arising from some individual properties.

  2. Portable Aerosol Contaminant Extractor

    DOE Patents [OSTI]

    Carlson, Duane C. (N. Augusta, SC); DeGange, John J. (Aiken, SC); Cable-Dunlap, Paula (Waynesville, NC)

    2005-11-15

    A compact, portable, aerosol contaminant extractor having ionization and collection sections through which ambient air may be drawn at a nominal rate so that aerosol particles ionized in the ionization section may be collected on charged plate in the collection section, the charged plate being readily removed for analyses of the particles collected thereon.

  3. PILOT-SCALE EVALUATION OF THE IMPACT OF SELECTIVE CATALYTIC REDUCTION FOR NOx ON MERCURY SPECIATION

    SciTech Connect (OSTI)

    Dennis L. Laudal; John H. Pavlish; Kevin C. Galbreath; Jeffrey S. Thompson; Gregory F. Weber; Everett Sondreal

    2000-12-01

    Full-scale tests in Europe and bench-scale tests in the United States have indicated that the catalyst, normally vanadium/titanium metal oxide, used in the selective catalytic reduction (SCR) of NO{sub x}, may promote the formation of Hg{sup 2+} and/or particulate-bound mercury (Hg{sub p}). To investigate the impact of SCR on mercury speciation, pilot-scale screening tests were conducted at the Energy & Environmental Research Center. The primary research goal was to determine whether the catalyst or the injection of ammonia in a representative SCR system promotes the conversion of Hg{sup 0} to Hg{sup 2+} and/or Hg{sub p} and, if so, which coal types and parameters (e.g., rank and chemical composition) affect the degree of conversion. Four different coals, three eastern bituminous coals and a Powder River Basin (PRB) subbituminous coal, were tested. Three tests were conducted for each coal: (1) baseline, (2) NH{sub 3} injection, and (3) SCR of NO{sub x}. Speciated mercury, ammonia slip, SO{sub 3}, and chloride measurements were made to determine the effect the SCR reactor had on mercury speciation. It appears that the impact of SCR of NO{sub x} on mercury speciation is coal-dependent. Although there were several confounding factors such as temperature and ammonia concentrations in the flue gas, two of the eastern bituminous coals showed substantial increases in Hg{sub p} at the inlet to the ESP after passing through an SCR reactor. The PRB coal showed little if any change due to the presence of the SCR. Apparently, the effects of the SCR reactor are related to the chloride, sulfur and, possibly, the calcium content of the coal. It is clear that additional work needs to be done at the full-scale level.

  4. Effect of Aerosol Humidification on the Column Aerosol Optical Thickness

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    over the ARM Southern Great Plains Site Effect of Aerosol Humidification on the Column Aerosol Optical Thickness over the ARM Southern Great Plains Site Li, Zhanqing University of Maryland Jeong, Myeong-Jae University of Maryland Category: Aerosols This study investigates the aerosol humidification effect (AHE) using seventy profiles of the aerosol scattering and absorption coefficients at high (~85%) and low (~40%) relative humidity (RH) levels obtained over the Southern Great Plains (SGP)

  5. Characterization of a real-time tracer for Isoprene Epoxydiols-derived Secondary Organic Aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; et al

    2015-04-16

    Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene low-NO oxidation pathways, was quantified by applying Positive Matrix Factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of OA in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the SOAS study, 78% of IEPOX-SOA is accounted for the measured molecular tracers, making itmore » the highest level of molecular identification of an ambient SOA component to our knowledge. Enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O ( fC5H6O = C5H6O+/OA) across multiple field, chamber and source datasets. A background of ~ 1.7 ± 0.1‰ is observed in studies strongly influenced by urban, biomass-burning and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.8‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7‰). Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3‰) observed in non IEPOX-derived isoprene-SOA indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a "triangle plot" of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2 if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass resolution data is available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.« less

  6. DEVELOPMENT OF FINE PARTICULATE EMISSION FACTORS AND SPECIATION PROFILES FOR OIL AND GAS-FIRED COMBUSTION SYSTEMS

    SciTech Connect (OSTI)

    Glenn C. England; Stephanie Wien; Mingchih O. Chang

    2002-08-01

    This report provides results from the first year of this three-year project to develop dilution measurement technology for characterizing PM2.5 (particles with aerodynamic diameter smaller than 2.5 micrometers) and precursor emissions from stationary combustion sources used in oil, gas and power generation operations. Detailed emission rate and chemical speciation test results for a refinery gas-fired process heater and plans for cogeneration gas turbine tests and pilot-scale tests are presented. Tests were performed using a research dilution sampling apparatus and traditional EPA methods to compare PM2.5 mass and chemical speciation. Test plans are presented for a gas turbine facility that will be tested in the fourth quarter of 2002. A preliminary approach for pilot-scale tests is presented that will help define design constraints for a new dilution sampler design that is smaller, lighter, and less costly to use.

  7. ARM: 10-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    1998-03-01

    10-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  8. ARM: 1-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    2004-10-01

    1-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  9. ARM: 10-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    10-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  10. ARM: 1-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    1-minute Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  11. ARM - Measurement - Aerosol absorption

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    absorption ARM Data Discovery Browse Data Comments? We would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Aerosol absorption The...

  12. Monodisperse aerosol generator

    DOE Patents [OSTI]

    Ortiz, Lawrence W. (Los Alamos, NM); Soderholm, Sidney C. (Pittsford, NY)

    1990-01-01

    An aerosol generator is described which is capable of producing a monodisperse aerosol within narrow limits utilizing an aqueous solution capable of providing a high population of seed nuclei and an organic solution having a low vapor pressure. The two solutions are cold nebulized, mixed, vaporized, and cooled. During cooling, particles of the organic vapor condense onto the excess seed nuclei, and grow to a uniform particle size.

  13. Understanding sources of organic aerosol during CalNex-2010 using the CMAQ-VBS

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Woody, M. C.; Baker, K. R.; Hayes, P. L.; Jimenez, J. L.; Koo, B.; Pye, H. O. T.

    2015-10-05

    Community Multiscale Air Quality (CMAQ) model simulations utilizing the volatility basis set (VBS) treatment for organic aerosols (CMAQ-VBS) were evaluated against measurements collected at routine monitoring networks (Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE)) and those collected during the 2010 California at the Nexus of Air Quality and Climate Change (CalNex) field campaign to examine important sources of organic aerosol (OA) in southern California. CMAQ-VBS (OA lumped by volatility, semivolatile POA) underpredicted total organic carbon (OC) at CSN (?25.5 % Normalized Median Bias (NMdnB)) and IMPROVE (?63.9 % NMdnB) locations and total OC wasmoreunderpredicted to a greater degree compared to the CMAQ-AE6 (9.9 and ?55.7 % NMdnB, respectively; semi-explicit OA treatment, SOA lumped by parent hydrocarbon, nonvolatile POA). However, comparisons to aerosol mass spectrometer (AMS) measurements collected at Pasadena, CA indicated that CMAQ-VBS better represented the diurnal profile and the primary/secondary split of OA. CMAQ-VBS secondary organic aerosol (SOA) underpredicted the average measured AMS oxygenated organic aerosol (OOA, a surrogate of SOA) concentration by a factor of 5.2 (4.7 ?g m?3 measured vs. 0.9 ?g m?3 modeled), a considerable improvement to CMAQ-AE6 SOA predictions, which were approximately 24 lower than the average AMS OOA concentration. We use two new methods, based on species ratios and on a simplified SOA parameterization from the observations, to apportion the SOA underprediction for CMAQ-VBS to too slow photochemical oxidation (estimated as 1.5 lower than observed at Pasadena using ? log (NOx: NOy)), low intrinsic SOA formation efficiency (low by 1.6 to 2 for Pasadena), and too low emissions or too high dispersion for the Pasadena site (estimated to be 1.6 to 2.3 too low/high). The first and third factors will be similar for CMAQ-AE6, while the intrinsic SOA formation efficiency for that model is estimated to be too low by about 7. For CMAQ-VBS, 90 % of the anthropogenic SOA mass formed was attributed to aged secondary semivolatile vapors (70 % originating from volatile organic compounds (VOCs) and 20 % from intermediate volatility compounds (IVOCs)). From source-apportioned model results, we found most of the CMAQ-VBS modeled POA at the Pasadena CalNex site was attributable to meat cooking emissions (48 %, and consistent with a substantial fraction of cooking OA in the observations), compared to 18 % from gasoline vehicle emissions, 13 % from biomass burning (in the form of residential wood combustion), and 8 % from diesel vehicle emissions. All "other" inventoried emission sources (e.g. industrial/point sources) comprised the final 13 %. The CMAQ-VBS semivolatile POA treatment underpredicted AMS hydrocarbon-like OA (HOA) + cooking-influenced OA (CIOA) at Pasadena by a factor of 1.8 (1.16 ?g m?3 modeled vs. 2.05 ?g m?3 observed) compared to a factor of 1.4 overprediction of POA in CMAQ-AE6, but did well to capture the AMS diurnal profile of HOA and CIOA, with the exception of the midday peak. We estimated that using the National Emission Inventory (NEI) POA emissions without scaling to represent SVOCs underestimates SVOCs by ~1.7.less

  14. Zinc Speciation in Contaminated Sediments: Quantitative Determination of

    Office of Scientific and Technical Information (OSTI)

    Zinc Coordination by X-ray Absorption Spectroscopy (Journal Article) | SciTech Connect Zinc Speciation in Contaminated Sediments: Quantitative Determination of Zinc Coordination by X-ray Absorption Spectroscopy Citation Details In-Document Search Title: Zinc Speciation in Contaminated Sediments: Quantitative Determination of Zinc Coordination by X-ray Absorption Spectroscopy Authors: Webb, Samuel M. ; Gaillard, Jean-François [1] ; NWU) [2] + Show Author Affiliations (SSRL) ( Publication

  15. Detailed HCCI Exhaust Speciation - ORNL Reference Fuel Blends | Department

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    of Energy HCCI Exhaust Speciation - ORNL Reference Fuel Blends Detailed HCCI Exhaust Speciation - ORNL Reference Fuel Blends *Accurately measure exhaust profile from an HCCI engine with a variety of fuels and create a better understanding of HCCI engine emissions. PDF icon deer09_bunting.pdf More Documents & Publications A Comparison of HCCI Engine Performance Data and Kinetic Modeling Results over a Wide Rangeof Gasoline Range Surrogate Fuel Blends Combustion, Efficiency, and Fuel

  16. ARM - Field Campaign - In-situ Aerosol Profiles (Cessna Aerosol...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : In-situ Aerosol Profiles (Cessna Aerosol Flights) 2000.03.01 - 2007.10.31 Lead...

  17. ARM - Measurement - Aerosol effective radius

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    effective radius ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Aerosol effective radius Aerosol effective radius is the ratio of the third and second moments of the number size distribution of aerosol particles. Categories Aerosols Instruments The above measurement is considered scientifically relevant for the following instruments. Refer to the datastream (netcdf) file headers of each instrument for

  18. Highly stable aerosol generator

    DOE Patents [OSTI]

    DeFord, Henry S. (Kennewick, WA); Clark, Mark L. (Kennewick, WA)

    1981-01-01

    An improved compressed air nebulizer has been developed such that a uniform aerosol particle size and concentration may be produced over long time periods. This result is achieved by applying a vacuum pressure to the makeup assembly and by use of a vent tube between the atmosphere and the makeup solution. By applying appropriate vacuum pressures to the makeup solution container and by proper positioning of the vent tube, a constant level of aspirating solution may be maintained within the aspirating assembly with aspirating solution continuously replaced from the makeup solution supply. This device may also be adapted to have a plurality of aerosol generators and only one central makeup assembly.

  19. Highly stable aerosol generator

    DOE Patents [OSTI]

    DeFord, H.S.; Clark, M.L.

    1981-11-03

    An improved compressed air nebulizer has been developed such that a uniform aerosol particle size and concentration may be produced over long time periods. This result is achieved by applying a vacuum pressure to the makeup assembly and by use of a vent tube between the atmosphere and the makeup solution. By applying appropriate vacuum pressures to the makeup solution container and by proper positioning of the vent tube, a constant level of aspirating solution may be maintained within the aspirating assembly with aspirating solution continuously replaced from the makeup solution supply. This device may also be adapted to have a plurality of aerosol generators and only one central makeup assembly. 2 figs.

  20. Aerosol remote sensing in polar regions

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Tomasi, Claudio; Kokhanovsky, Alexander A.; Lupi, Angelo; Ritter, Christoph; Smirnov, Alexander; O'Neill, Norman T.; Stone, Robert S.; Holben, Brent N.; Nyeki, Stephan; Wehrli, Christoph; et al

    2015-01-01

    Multi-year sets of ground-based sun-photometer measurements conducted at 12 Arctic sites and 9 Antarctic sites were examined to determine daily mean values of aerosol optical thickness τ(λ) at visible and near-infrared wavelengths, from which best-fit values of Ångström's exponent α were calculated. Analysing these data, the monthly mean values of τ(0.50 μm) and α and the relative frequency histograms of the daily mean values of both parameters were determined for winter–spring and summer–autumn in the Arctic and for austral summer in Antarctica. The Arctic and Antarctic covariance plots of the seasonal median values of α versus τ(0.50 μm) showed: (i)more » a considerable increase in τ(0.50 μm) for the Arctic aerosol from summer to winter–spring, without marked changes in α; and (ii) a marked increase in τ(0.50 μm) passing from the Antarctic Plateau to coastal sites, whereas α decreased considerably due to the larger fraction of sea-salt aerosol. Good agreement was found when comparing ground-based sun-photometer measurements of τ(λ) and α at Arctic and Antarctic coastal sites with Microtops measurements conducted during numerous AERONET/MAN cruises from 2006 to 2013 in three Arctic Ocean sectors and in coastal and off-shore regions of the Southern Atlantic, Pacific, and Indian Oceans, and the Antarctic Peninsula. Lidar measurements were also examined to characterise vertical profiles of the aerosol backscattering coefficient measured throughout the year at Ny-Ålesund. Satellite-based MODIS, MISR, and AATSR retrievals of τ(λ) over large parts of the oceanic polar regions during spring and summer were in close agreement with ship-borne and coastal ground-based sun-photometer measurements. An overview of the chemical composition of mode particles is also presented, based on in-situ measurements at Arctic and Antarctic sites. Fourteen log-normal aerosol number size-distributions were defined to represent the average features of nuclei, accumulation and coarse mode particles for Arctic haze, summer background aerosol, Asian dust and boreal forest fire smoke, and for various background austral summer aerosol types at coastal and high-altitude Antarctic sites. The main columnar aerosol optical characteristics were determined for all 14 particle modes, based on in-situ measurements of the scattering and absorption coefficients. Diurnally averaged direct aerosol-induced radiative forcing and efficiency were calculated for a set of multimodal aerosol extinction models, using various Bidirectional Reflectance Distribution Function models over vegetation-covered, oceanic and snow-covered surfaces. These gave a reliable measure of the pronounced effects of aerosols on the radiation balance of the surface–atmosphere system over polar regions.« less

  1. ARM - Instrument - acsm

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govInstrumentsacsm Documentation ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Instrument : Aerosol Chemical Speciation Monitor (ACSM) Instrument Categories Aerosols The Aerosol Chemical Speciation Monitor is a thermal vaporization, electron impact ionization mass spectrometer that measures bulk chemical composition of the non-refractory component of sub-micron aerosol particles in real time with typically

  2. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

    SciTech Connect (OSTI)

    Davidovits, Paul

    2015-10-20

    Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in 17 manuscripts published in refereed journals.

  3. XANES Identification of Plutonium Speciation in RFETS Samples

    SciTech Connect (OSTI)

    LoPresti, V.; Conradson, S.D.; Clark, D.L.

    2009-06-03

    Using primarily X-ray absorption near edge spectroscopy (XANES) with standards run in tandem with samples, probable plutonium speciation was determined for 13 samples from contaminated soil, acid-splash or fire-deposition building interior surfaces, or asphalt pads from the Rocky Flats Environmental Technology Site (RFETS). Save for extreme oxidizing situations, all other samples were found to be of Pu(IV) speciation, supporting the supposition that such contamination is less likely to show mobility off site. EXAFS analysis conducted on two of the 13 samples supported the validity of the XANES features employed as determinants of the plutonium valence.

  4. Laboratory Investigation of Organic Aerosol Formation from Aromatic Hydrocarbons

    DOE R&D Accomplishments [OSTI]

    Molina, Luisa T.; Molina, Mario J.; Zhang, Renyi

    2006-08-23

    Our work for this DOE funded project includes: (1) measurements of the kinetics and mechanism of the gas-phase oxidation reactions of the aromatic hydrocarbons initiated by OH; (2) measurements of aerosol formation from the aromatic hydrocarbons; and (3) theoretical studies to elucidate the OH-toluene reaction mechanism using quantum-chemical and rate theories.

  5. Aerosol Observing System (AOS) Handbook

    SciTech Connect (OSTI)

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earths radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  6. Ganges Valley Aerosol Experiment

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ganges Valley Aerosol Experiment In northeastern India, the fertile land around the Ganges River supports several hundred million people. This river, the largest in India, is fed by monsoon rains and runoff from the nearby Himalayan Mountains. Through an intergovernmental agreement with India, the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility deployed its portable laboratory, the ARM Mobile Facility (AMF), to Nainital, India, in June 2011. During

  7. Cantera Aerosol Dynamics Simulator

    Energy Science and Technology Software Center (OSTI)

    2004-09-01

    The Cantera Aerosol Dynamics Simulator (CADS) package is a general library for aerosol modeling to address aerosol general dynamics, including formation from gas phase reactions, surface chemistry (growth and oxidation), bulk particle chemistry, transport by Brownian diffusion, thermophoresis, and diffusiophoresis with linkage to DSMC studies, and thermal radiative transport. The library is based upon Cantera, a C++ Cal Tech code that handles gas phase species transport, reaction, and thermodynamics. The method uses a discontinuous galerkinmore » formulation for the condensation and coagulation operator that conserves particles, elements, and enthalpy up to round-off error. Both O-D and 1-D time dependent applications have been developed with the library. Multiple species in the solid phase are handled as well. The O-D application, called Tdcads (Time Dependent CADS) is distributed with the library. Tdcads can address both constant volume and constant pressure adiabatic homogeneous problems. An extensive set of sample problems for Tdcads is also provided.« less

  8. ARM Cloud Aerosol Precipitation Experiment

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Precipitation Experiment a NOAA ship in the Pacific Ocean and on a DOE- sponsored plane over land and sea. These researchers will study: (1) water sources, evolution and structure of atmospheric rivers over the Pacific Ocean (2) long range transport of aerosols over the Pacific Ocean between Hawaii and the U.S. West Coast, and how aerosols interact with atmospheric rivers (3) the point where atmospheric rivers make landfall on the U.S. West Coast, especially how clouds form where

  9. ARM - Measurement - Aerosol optical depth

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    depth ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Measurement : Aerosol optical depth A measure of how much light aerosols prevent from passing through a column of atmosphere. Categories Aerosols Instruments The above measurement is considered scientifically relevant for the following instruments. Refer to the datastream (netcdf) file headers of each instrument for a list of all available measurements, including

  10. Direct speciation analysis of arsenic in sub-cellular compartments using micro-X-ray absorption spectroscopy

    SciTech Connect (OSTI)

    Bacquart, Thomas; Deves, Guillaume; Ortega, Richard

    2010-07-15

    Identification of arsenic chemical species at a sub-cellular level is a key to understanding the mechanisms involved in arsenic toxicology and antitumor pharmacology. When performed with a microbeam, X-ray absorption near-edge structure ({mu}-XANES) enables the direct speciation analysis of arsenic in sub-cellular compartments avoiding cell fractionation and other preparation steps that might modify the chemical species. This methodology couples tracking of cellular organelles in a single cell by confocal or epifluorescence microscopy with local analysis of chemical species by {mu}-XANES. Here we report the results obtained with a {mu}-XANES experimental setup based on Kirkpatrick-Baez X-ray focusing optics that maintains high flux of incoming radiation (>10{sup 11} ph/s) at micrometric spatial resolution (1.5x4.0 {mu}m{sup 2}). This original experimental setup enabled the direct speciation analysis of arsenic in sub-cellular organelles with a 10{sup -15} g detection limit. {mu}-XANES shows that inorganic arsenite, As(OH){sub 3}, is the main form of arsenic in the cytosol, nucleus, and mitochondrial network of cultured cancer cells exposed to As{sub 2}O{sub 3}. On the other hand, a predominance of As(III) species is observed in HepG2 cells exposed to As(OH){sub 3} with, in some cases, oxidation to a pentavalent form in nuclear structures of HepG2 cells. The observation of intra-nuclear mixed redox states suggests an inter-individual variability in a cell population that can only be evidenced with direct sub-cellular speciation analysis.

  11. Method of dispersing particulate aerosol tracer

    DOE Patents [OSTI]

    O'Holleran, Thomas P. (Belleville, MI)

    1988-01-01

    A particulate aerosol tracer which comprises a particulate carrier of sheet silicate composition having a particle size up to one micron, and a cationic dopant chemically absorbed in solid solution in the carrier. The carrier is preferably selected from the group consisting of natural mineral clays such as bentonite, and the dopant is selected from the group consisting of rare earth elements and transition elements. The tracers are dispersed by forming an aqueous salt solution with the dopant present as cations, dispersing the carriers in the solution, and then atomizing the solution under heat sufficient to superheat the solution droplets at a level sufficient to prevent reagglomeration of the carrier particles.

  12. ARM - Surface Aerosol Observing System

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    2009-2010 Shouxian, China, 2008 Black Forest, Germany, 2007 Niamey, Niger, 2006 Point Reyes, California, 2005 Surface Aerosol Observing System The ARM Mobile Facility (AMF) is...

  13. ARM: 10-minute TEMPORARY Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sivaraman, Chitra; Flynn, Connor

    2010-12-15

    10-minute TEMPORARY Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  14. ARM: 10-minute TEMPORARY Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sivaraman, Chitra; Flynn, Connor

    10-minute TEMPORARY Raman Lidar: aerosol extinction profiles and aerosol optical thickness, from first Ferrare algorithm

  15. Atmospheric Science Program Cumulus Humilis Aerosol Processing...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    aerosols - within and around them. Aerosols - particularly those associated with human activity - are thought to be changing the brightness, the lifetime, the amount of...

  16. ARM - Field Campaign - MASRAD - Aerosol Optical Properties

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsMASRAD - Aerosol Optical Properties Campaign Links AMF Point Reyes Website ARM Data Discovery Browse Data Related Campaigns MArine Stratus Radiation Aerosol and Drizzle...

  17. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Print Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion...

  18. Aerosols and Clouds: In Cahoots to Change Climate

    SciTech Connect (OSTI)

    Berg, Larry

    2014-03-29

    Key knowledge gaps persist despite advances in the scientific understanding of how aerosols and clouds evolve and affect climate. The Two-Column Aerosol Project, or TCAP, was designed to provide a detailed set of observations to tackle this area of unknowns. Led by PNNL atmospheric scientist Larry Berg, ARM's Climate Research Facility was deployed in Cape Cod, Massachusetts for the 12-month duration of TCAP, which came to a close in June 2013. "We are developing new tools to look at particle chemistry, like our mass spectrometer used in TCAP that can tell us the individual chemical composition of an aerosol," said Berg. "Then, we'll run our models and compare it with the data that we have to make sure we're getting correct answers and make sure our climate models are reflecting the best information."

  19. Aerosols and Clouds: In Cahoots to Change Climate

    ScienceCinema (OSTI)

    Berg, Larry

    2014-06-02

    Key knowledge gaps persist despite advances in the scientific understanding of how aerosols and clouds evolve and affect climate. The Two-Column Aerosol Project, or TCAP, was designed to provide a detailed set of observations to tackle this area of unknowns. Led by PNNL atmospheric scientist Larry Berg, ARM's Climate Research Facility was deployed in Cape Cod, Massachusetts for the 12-month duration of TCAP, which came to a close in June 2013. "We are developing new tools to look at particle chemistry, like our mass spectrometer used in TCAP that can tell us the individual chemical composition of an aerosol," said Berg. "Then, we'll run our models and compare it with the data that we have to make sure we're getting correct answers and make sure our climate models are reflecting the best information."

  20. Ganges Valley Aerosol Experiment: Science and Operations Plan

    SciTech Connect (OSTI)

    Kotamarthi, VR

    2010-06-21

    The Ganges Valley region is one of the largest and most rapidly developing sections of the Indian subcontinent. The Ganges River, which provides the region with water needed for sustaining life, is fed primarily by snow and rainfall associated with Indian summer monsoons. Impacts of changes in precipitation patterns, temperature, and the flow of the snow-fed rivers can be immense. Recent satellite-based measurements have indicated that the upper Ganges Valley has some of the highest persistently observed aerosol optical depth values. The aerosol layer covers a vast region, extending across the Indo-Gangetic Plain to the Bay of Bengal during the winter and early spring of each year. The persistent winter fog in the region is already a cause of much concern, and several studies have been proposed to understand the economic, scientific, and societal dimensions of this problem. During the INDian Ocean EXperiment (INDOEX) field studies, aerosols from this region were shown to affect cloud formation and monsoon activity over the Indian Ocean. This is one of the few regions showing a trend toward increasing surface dimming and enhanced mid-tropospheric warming. Increasing air pollution over this region could modify the radiative balance through direct, indirect, and semi-indirect effects associated with aerosols. The consequences of aerosols and associated pollution for surface insolation over the Ganges Valley and monsoons, in particular, are not well understood. The proposed field study is designed for use of (1) the ARM Mobile Facility (AMF) to measure relevant radiative, cloud, convection, and aerosol optical characteristics over mainland India during an extended period of 912 months and (2) the G-1 aircraft and surface sites to measure relevant aerosol chemical, physical, and optical characteristics in the Ganges Valley during a period of 612 weeks. The aerosols in this region have complex sources, including burning of coal, biomass, and biofuels; automobile emissions; and dust. The extended AMF deployment will enable measurements under different regimes of the climate and aerosol abundancein the wet monsoon period with low aerosol loading; in the dry, hot summer with aerosols dispersed throughout the atmospheric column; and in the cool, dry winter with aerosols confined mostly to the boundary later and mid-troposphere. Each regime, in addition, has its own distinct radiative and atmospheric dynamic drivers. The aircraft operational phase will assist in characterizing the aerosols at times when they have been observed to be at the highest concentrations. A number of agencies in India will collaborate with the proposed field study and provide support in terms of planning, aircraft measurements, and surface sites. The high concentration of aerosols in the upper Ganges Valley, together with hypotheses involving several possible mechanisms with direct impacts on the hydrologic cycle of the region, gives us a unique opportunity to generate data sets that will be useful both in understanding the processes at work and in providing answers regarding the effects of aerosols on climate in a region where the perturbation is the highest.

  1. Mercury Speciation in Piscivorous Fish from Mining-impacted Reservoirs

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Mercury Speciation in Piscivorous Fish from Mining-impacted Reservoirs Mercury toxicity generates environmental concerns in diverse aquatic systems because methylmercury enters the water column in diverse ways then biomagnifies through food webs. At the apex of many freshwater food webs, piscivorous fish can then extend that trophic transfer and potential for neurotoxicity to wildlife and humans. Mining activities, particularly those associated with the San Francisco Bay region, can generate

  2. X-ray Vision for Aerosol Scientists: LCLS Snapshots of Soot (Narrated)

    ScienceCinema (OSTI)

    None

    2014-06-03

    This short conceptual animation depicts how scientists can now simultaneously capture fractal morphology (structure), chemical composition and nanoscale imagery of individual aerosol particles in flight. These particles, known as "PM2.5" because they are smaller than 2.5 microns in diameter, affect climate by interacting with sunlight and impact human health by entering the lungs. The single LCLS laser pulses travel to the Atomic, Molecular and Optical Sciences (AMO) laboratory in the Near Experimental Hall. As we zoom in, we see deep inside a simplified aerosol inlet, where the complex fractal structure of the soot particles, each one completely unique, is shown. Individual soot particles are then delivered into the pulses of the LCLS beam, which destroys them. X-rays are scattered to the detector before the particle is destroyed, giving information about the morphology of the particle. Ion fragments released in the explosion are sent into a mass spectrometer, which measures their mass-to-charge ratio -- giving scientists information about the chemical composition of the particle. Many different particles are analyzed in this manner, allowing scientists to probe variations in the particles due to changes in their environment before being sent through the aerosol inlet. The final visual of aerosols emitted from a factory is representative of the goal that such LCLS aerosol dynamics experiments can provide critical feedback into modeling and understanding combustion, aerosol processes in manufacturing or aerosol effects on climate change.

  3. Carbonaceous Aerosols and Radiative Effects Study

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Carbonaceous Aerosols and Radiative Effects Study Science Objective This field campaign is designed to increase scientific knowledge about the evolution of black carbon, primary organic aerosols (POA), and secondary organic aerosols (SOA) from both man-made and biogenic sources. Black carbon and primary organic aerosols are emitted directly into the atmosphere through diesel and gasoline vehicle exhaust, as well as during meat cooking and biomass burning; secondary organic aerosols are formed

  4. ARM - Campaign Instrument - drum-aerosol

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govInstrumentsdrum-aerosol Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign Instrument : Drum Aerosol Sampler (DRUM-AEROSOL) Instrument Categories Aerosols Campaigns Aerosol IOP [ Download Data ] Southern Great Plains, 2003.05.01 - 2003.05.31 Primary Measurements Taken The following measurements are those considered scientifically relevant. Refer to the datastream (netcdf) file headers for the list of all available measurements, including

  5. AERONET: The Aerosol Robotic Network

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    AERONET collaboration provides globally distributed observations of spectral aerosol optical Depth (AOD), inversion products, and precipitable water in diverse aerosol regimes. Aerosol optical depth data are computed for three data quality levels: Level 1.0 (unscreened), Level 1.5 (cloud-screened), and Level 2.0 (cloud screened and quality-assured). Inversions, precipitable water, and other AOD-dependent products are derived from these levels and may implement additional quality checks.[Copied from http://aeronet.gsfc.nasa.gov/new_web/system_descriptions.html

  6. eDPS Aerosol Collection

    SciTech Connect (OSTI)

    Venzie, J.

    2015-10-13

    The eDPS Aerosol Collection project studies the fundamental physics of electrostatic aerosol collection for national security applications. The interpretation of aerosol data requires understanding and correcting for biases introduced from particle genesis through collection and analysis. The research and development undertaken in this project provides the basis for both the statistical correction of existing equipment and techniques; as well as, the development of new collectors and analytical techniques designed to minimize unwanted biases while improving the efficiency of locating and measuring individual particles of interest.

  7. Genomic Analysis of Adaptation and Speciation in Mimulus guttatus (2009 JGI User Meeting)

    ScienceCinema (OSTI)

    Willis, John

    2011-04-25

    John Willis of Duke University spoke about the "Genomic Analysis of Adaptation and Speciation in Mimulus guttatus" on March 26, 2009 at the 4th Annual User Meeting

  8. General circulation model calculations of the direct radiative forcing by anthropogenic sulfate and fossil-fuel soot aerosol

    SciTech Connect (OSTI)

    Haywood, J.M.; Roberts, D.L.; Slingo, A.

    1997-07-01

    A new radiation code within a general circulation model is used to assess the direct solar and thermal radiative forcing by sulfate aerosol of anthropogenic origin and soot aerosol from fossil-fuel burning. The radiative effects of different aerosol profiles, relative humidity parameterizations, chemical compositions, and internal and external mixtures of the two aerosol types are investigated. The contribution to the radiative forcing from cloudy sky regions is found to be negligible for sulfate aerosol; this is in contrast to recent studies where the cloudy sky contribution was estimated using a method in which the spatial correlation between cloud amount and sulfate burden was ignored. However, the radiative forcing due to fossil-fuel soot aerosol is enhanced in cloudy regions if soot aerosol exists within or above the cloud. The global solar radiative forcing due to sulfate aerosol is estimated to be -0.38 W m{sup -2} and the global thermal radiative forcing is estimated to be +0.01 W m{sup -2}. The hemispheric mean radiative forcings vary by only about 10% for reasonable assumptions about the chemical form of the sulfate aerosol and the relative humidity dependence; the uncertainties in the aerosol loading are far more significant. If a soot/sulfate mass ratio of 0.075 is assumed, then the global solar radiative forcing weakens to -0.18 W m{sup -2} for an external mixture and weakens further for an internal mixture. Additionally, the spatial distribution of the radiative forcing shows strong negative/positive forcing contrasts that may influence the dynamical response of the atmosphere. Although these results are extremely sensitive to the adopted soot/sulfate ratio and the assumed vertical profile, they indicate that fossil-fuel soot aerosol may exert a nonnegligible radiative forcing and emphasize the need to consider each anthropogenic aerosol species. 58 refs., 8 figs., 1 tab.

  9. Stratospheric aerosol geoengineering

    SciTech Connect (OSTI)

    Robock, Alan

    2015-03-30

    The Geoengineering Model Intercomparison Project, conducting climate model experiments with standard stratospheric aerosol injection scenarios, has found that insolation reduction could keep the global average temperature constant, but global average precipitation would reduce, particularly in summer monsoon regions around the world. Temperature changes would also not be uniform; the tropics would cool, but high latitudes would warm, with continuing, but reduced sea ice and ice sheet melting. Temperature extremes would still increase, but not as much as without geoengineering. If geoengineering were halted all at once, there would be rapid temperature and precipitation increases at 510 times the rates from gradual global warming. The prospect of geoengineering working may reduce the current drive toward reducing greenhouse gas emissions, and there are concerns about commercial or military control. Because geoengineering cannot safely address climate change, global efforts to reduce greenhouse gas emissions and to adapt are crucial to address anthropogenic global warming.

  10. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    SciTech Connect (OSTI)

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    The atmosphere is composed of a complex mixture of gases and suspended microscopic aerosol particles. The ability of these particles to take up water (hygroscopicity) and to act as nuclei for cloud droplet formation significantly impacts aerosol light scattering and absorption, and cloud formation, thereby influencing air quality, visibility, and climate in important ways. A substantial, yet poorly characterized component of the atmospheric aerosol is organic matter. Its major sources are direct emissions from combustion processes, which are referred to as primary organic aerosol (POA), or in situ processes in which volatile organic compounds (VOCs) are oxidized in the atmosphere to low volatility reaction products that subsequent condense to form particles that are referred to as secondary organic aerosol (SOA). POA and VOCs are emitted to the atmosphere from both anthropogenic and natural (biogenic) sources. The overall goal of this experimental research project was to conduct laboratory studies under simulated atmospheric conditions to investigate the effects of the chemical composition of organic aerosol particles on their hygroscopicity and cloud condensation nucleation (CCN) activity, in order to develop quantitative relationships that could be used to more accurately incorporate aerosol-cloud interactions into regional and global atmospheric models. More specifically, the project aimed to determine the products, mechanisms, and rates of chemical reactions involved in the processing of organic aerosol particles by atmospheric oxidants and to investigate the relationships between the chemical composition of organic particles (as represented by molecule sizes and the specific functional groups that are present) and the hygroscopicity and CCN activity of oxidized POA and SOA formed from the oxidation of the major classes of anthropogenic and biogenic VOCs that are emitted to the atmosphere, as well as model hydrocarbons. The general approach for this project was to carry out reactions of representative anthropogenic and biogenic VOCs and organic particles with ozone (O3), and hydroxyl (OH), nitrate (NO3), and chlorine (Cl) radicals, which are the major atmospheric oxidants, under simulated atmospheric conditions in large-volume environmental chambers. A combination of on-line and off-line analytical techniques were used to monitor the chemical and physical properties of the particles including their hygroscopicity and CCN activity. The results of the studies were used to (1) improve scientific understanding of the relationships between the chemical composition of organic particles and their hygroscopicity and CCN activity, (2) develop an improved molecular level theoretical framework for describing these relationships, and (3) establish a large database that is being used to develop parameterizations relating organic aerosol chemical properties and SOA sources to particle hygroscopicity and CCN activity for use in regional and global atmospheric air quality and climate models.

  11. ARM Aerosol Working Group Meeting

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Report ARM STM 2008 Norfolk, VA Connor Flynn for B Schmid and AWG Members AWG Instruments * Raman Lidar - SGP * Micropulse Lidars - all sites * Aerosol Sampling - SGP, NSA, AMF - scattering, absorption, number, size distribution, hygroscopicity, CCN, composition (major ions). * In situ Aerosol Profile (Cessna) - scattering, absorption, number, hygroscopicity, * Radiometers: - MFRSR, NIMFR, RSS, Cimel, AERI, SWS AWG-related Field Campaigns * Recent Past: - MASRAD (Marine Stratus Radiation,

  12. Characterization of Ambient Aerosols in Mexico City during the MCMA-2003 Campaign with Aerosol Mass Spectrometry. Results from the CENICA Supersite

    SciTech Connect (OSTI)

    Salcedo, D.; Onasch, Timothy B.; Dzepina, K.; Canagaratna, M. R.; Zhang, Q.; Huffman, A. J.; DeCarlo, Peter; Jayne, J. T.; Mortimer, P.; Worsnop, Douglas R.; Kolb, C. E.; Johnson, Kirsten S.; Zuberi, Bilal M.; Marr, L.; Volkamer, Rainer M.; Molina, Luisa; Molina, Mario J.; Cardenas, B.; Bernabe, R.; Marquez, C.; Gaffney, Jeffrey S.; Marley, Nancy A.; Laskin, Alexander; Shutthanandan, V.; Xie, YuLong; Brune, W. H.; Lesher, R.; Shirley, T.; Jiminez, J. L.

    2006-03-24

    An Aerodyne Aerosol Mass Spectrometer (AMS) was deployed at the CENICA Supersite, while another was deployed in the Aerodyne Mobile Laboratory (AML) during the Mexico City Metropolitan Area field study (MCMA-2003) from March 29-May 4, 2003 to investigate particle concentrations, sources, and processes. This is the first of a series of papers reporting the AMS results from this campaign. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 ?m (NR PM1) with high time and size resolution. For the first time, we report field results from a beam width probe, which was used to study the shape and mixing state of the particles and to quantify potential losses of irregular particles due to beam broadening inside the AMS. Data from this probe show that no significant amount of irregular particles was lost due to excessive beam broadening. A comparison of the CENICA and AML AMSs measurements is presented, being the first published intercomparison between two quadrupole AMSs. The speciation, and mass concentrations reported by the two AMSs compared well. In order to account for the refractory material in the aerosol, we also present measurements of Black Carbon (BC) using an aethalometer and an estimate of the aerosol soil component obtained from PIXE analysis of filters. Comparisons of (AMS + BC + soil) mass concentration with other collocated particle instruments (a LASAIR Optical Particle Counter, a Tapered Element Oscillating Microbalance (TEOM) and a DustTrack Aerosol Monitor) are also presented. The comparisons show that the (AMS + BC + soil) mass concentration during MCMC-2003 is a good approximation to the total PM??? mass concentration.

  13. ASSESSMENT OF MARKER PROTEINS IDENTIFIED IN WHOLE CELL EXTRACTS FOR BACTERIAL SPECIATION USING LIQUID CHROMATOGRAPHY ELECTROSPRAY IONIZATION TANDEM MASS SPECTROMETRY

    SciTech Connect (OSTI)

    Kooken, Jennifer M.; Fox, Karen F.; Fox, Alvin; Wunschel, David S.

    2014-02-02

    ASSESSMENT OF MARKER PROTEINS IDENTIFIED IN WHOLE CELL EXTRACTS FOR BACTERIAL SPECIATION USING LIQUID CHROMATOGRAPHY ELECTROSPRAY IONIZATION TANDEM MASS SPECTROMETRY

  14. Composition of carbonaceous smoke particles from prescribed burning of a Canadian boreal forest: 1. Organic aerosol characterization by gas chromatography

    SciTech Connect (OSTI)

    Mazurek, M.A.; Laterza, C.; Newman, L.; Daum, P.; Cofer, W.R. III; Levine, J.S.; Winstead, E.L.

    1995-06-01

    In this study we examine the molecular organic constituents (C8 to C40 lipid compounds) collected as smoke particles from a Canadian boreal forest prescribed burn. Of special interest are (1) the molecular identity of polar organic aerosols, and (2) the amount of polar organic matter relative to the total mass of aerosol particulate carbon. Organic extracts of smoke aerosol particles show complex distributions of the lipid compounds when analyzed by capillary gas chromatography/mass spectrometry. The molecular constituents present as smoke aerosol are grouped into non-polar (hydrocarbons) and polar {minus}2 oxygen atoms) subtractions. The dominant chemical species found in the boreal forest smoke aerosol are unaltered resin compounds (C20 terpenes) which are abundant in unburned conifer wood, plus thermally altered wood lignins and other polar aromatic hydrocarbons. Our results show that smoke aerosols contain molecular tracers which are related to the biofuel consumed. These smoke tracers can be related structurally back to the consumed softwood and hardwood vegetation. In addition, combustion of boreal forest materials produces smoke aerosol particles that are both oxygen-rich and chemically complex, yielding a carbonaceous aerosol matrix that is enriched in polar substances. As a consequence, emissions of carbonaceous smoke particles from large-scale combustion of boreal forest land may have a disproportionate effect on regional atmospheric chemistry and on cloud microphysical processes.

  15. ARM - Datastreams - aosacsm

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Datastreamsaosacsm Documentation Data Quality Plots Citation DOI: 10.5439/1046180 [ What is this? ] Generate Citation ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Datastream : AOSACSM AOS: aerosol chemical speciation monitor Active Dates 2010.11.20 - 2016.03.10 Measurement Categories Aerosols Originating Instrument Aerosol Chemical Speciation Monitor (ACSM) Measurements Only measurements considered scientifically

  16. THE INFLUENCE OF BENZENE AS A TRACE REACTANT IN TITAN AEROSOL ANALOGS

    SciTech Connect (OSTI)

    Trainer, Melissa G.; Sebree, Joshua A.; Heidi Yoon, Y.; Tolbert, Margaret A.

    2013-03-20

    Benzene has been detected in Titan's atmosphere by Cassini instruments, with concentrations ranging from sub-ppb in the stratosphere to ppm in the ionosphere. Sustained levels of benzene in the haze formation region could signify that it is an important reactant in the formation of Titan's organic aerosol. To date, there have not been laboratory investigations to assess the influence of benzene on aerosol properties. We report a laboratory study on the chemical composition of organic aerosol formed from C{sub 6}H{sub 6}/CH{sub 4}/N{sub 2} via far ultraviolet irradiation (120-200 nm). The compositional results are compared to those from aerosol generated by a more ''traditional Titan'' mixture of CH{sub 4}/N{sub 2}. Our results show that even a trace amount of C{sub 6}H{sub 6} (10 ppm) has significant impact on the chemical composition and production rates of organic aerosol. There are several pathways by which photolyzed benzene may react to form larger molecules, both with and without the presence of CH{sub 4}, but many of these reaction mechanisms are only beginning to be explored for the conditions at Titan. Continued work investigating the influence of benzene in aerosol growth will advance understanding of this previously unstudied reaction system.

  17. Technetium Inventory, Distribution, and Speciation in Hanford Tanks

    SciTech Connect (OSTI)

    Serne, R. Jeffrey; Rapko, Brian M.; Pegg, Ian L.

    2014-11-13

    The purpose of this report is three fold: 1) assemble the available information regarding Tc inventory, distribution between phases, and speciation in Hanford’s 177 storage tanks into a single, detailed, comprehensive assessment; 2) discuss the fate (distribution/speciation) of Tc once retrieved from the storage tanks and processed into final waste forms; and 3) discuss/document in less detail the available data on the inventory of Tc in other “pools” such as the vadose zone below inactive cribs and trenches, below single-shell tanks (SSTs) that have leaked, and in the groundwater below the Hanford Site. This report was revised in September 2014 to add detail and correct inaccuracies in Section 5.0 on the fate of technetium (Tc) recycle from the off-gas systems downstream of the low-activity waste (LAW) melters back to the melters, based on several reports that were not found in the original literature search on the topic. The newly provided reports, from experts active in the Hanford Tank Waste Treatment and Immobilization Plant (WTP) glass studies, the Vitreous State Laboratory at The Catholic University of America (VSL) melter and off-gas system demonstrations and overall WTP systems analysis, were not originally found on electronic databases commonly searched. The major revisions to Section 5.0 also required changes to Section 7.0 (Summary and Conclusions) and this executive summary.

  18. Aerosol Remote Sealing System - Energy Innovation Portal

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Remote Sealing System Lawrence Berkeley National Laboratory Contact LBL About This Technology Technology Marketing SummaryMark Modera and Francois Remi Carrie from Berkeley National Laboratory have developed a rapid, economical technique to seal duct and other enclosed systems by means of an internally injected aerosol. DescriptionBerkeley National Laboratory's aerosol compound seals holes in enclosed systems and is effective even after bends and junctions. A unique, in situ aerosol

  19. ARM - PI Product - Direct Aerosol Forcing Uncertainty

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ProductsDirect Aerosol Forcing Uncertainty ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send PI Product : Direct Aerosol Forcing Uncertainty Understanding sources of uncertainty in aerosol direct radiative forcing (DRF), the difference in a given radiative flux component with and without aerosol, is essential to quantifying changes in Earth's radiation budget. We examine the uncertainty in DRF due to measurement

  20. ARM - Measurement - Aerosol particle size distribution

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    AOS : Aerosol Observing System CSPHOT : Cimel Sunphotometer HTDMA : Humidified Tandem Differential Mobility Analyzer SMPS : Scanning mobility particle sizer TDMA : Tandem...

  1. Aerosol Resuspension Model for MELCOR for Fusion and Very High Temperature Reactor Applications

    SciTech Connect (OSTI)

    B.J. Merrill

    2011-01-01

    Dust is generated in fusion reactors from plasma erosion of plasma facing components within the reactors vacuum vessel (VV) during reactor operation. This dust collects in cooler regions on interior surfaces of the VV. Because this dust can be radioactive, toxic, and/or chemically reactive, it poses a safety concern, especially if mobilized by the process of resuspension during an accident and then transported as an aerosol though out the reactor confinement building, and possibly released to the environment. A computer code used at the Idaho National Laboratory (INL) to model aerosol transport for safety consequence analysis is the MELCOR code. A primary reason for selecting MELCOR for this application is its aerosol transport capabilities. The INL Fusion Safety Program (FSP) organization has made fusion specific modifications to MELCOR. Recent modifications include the implementation of aerosol resuspension models in MELCOR 1.8.5 for Fusion. This paper presents the resuspension models adopted and the initial benchmarking of these models.

  2. ARM - Field Campaign - Aerosol IOP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsAerosol IOP Campaign Links Science Plan (PDF document) ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Aerosol IOP 2003.05.01 - 2003.05.31 Lead Scientist : Richard Ferrare Data Availability The IOP participants examined the individual instrument data to assess data quality, and to initiate other data analyses. Authorized participants can read reports of planning and debrief meetings,

  3. Real time infrared aerosol analyzer

    DOE Patents [OSTI]

    Johnson, Stanley A. (Countryside, IL); Reedy, Gerald T. (Bourbonnais, IL); Kumar, Romesh (Naperville, IL)

    1990-01-01

    Apparatus for analyzing aerosols in essentially real time includes a virtual impactor which separates coarse particles from fine and ultrafine particles in an aerosol sample. The coarse and ultrafine particles are captured in PTFE filters, and the fine particles impact onto an internal light reflection element. The composition and quantity of the particles on the PTFE filter and on the internal reflection element are measured by alternately passing infrared light through the filter and the internal light reflection element, and analyzing the light through infrared spectrophotometry to identify the particles in the sample.

  4. Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

    SciTech Connect (OSTI)

    UC Davis; Cappa, Christopher D.; Wilson, Kevin R.

    2010-10-28

    Vacuum Ultraviolet (VUV) photoionization mass spectrometry has been used to measure the evolution of chemical composition for two distinct organic aerosol types as they are passed through a thermodenuder at different temperatures. The two organic aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the alpha-pinene + O3 reaction (alphaP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct changes with temperature in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In contrast, the alphaP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in agreement with expectations from absorptive partitioning theory whereas the alphaP spectra suggest that the evaporation of alphaP derived aerosol appears to not be governed by partitioning theory. We postulate that this difference arises from the alphaP particles existing as in a glassy state instead of having the expected liquid-like behavior. To reconcile these observations with decades of aerosol growth measurements, which indicate that OA formation is described by equilibrium partitioning, we present a conceptual model wherein the secondary OA is formed and then rapidly converted from an absorbing form to a non-absorbing form. The results suggest that although OA growth may be describable by equilibrium partitioning theory, the properties of organic aerosol once formed may differ significantly from the properties determined in the equilibrium framework.

  5. Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

    SciTech Connect (OSTI)

    Zaveri, Rahul A.; Shaw, William J.; Cziczo, D. J.; Schmid, Beat; Ferrare, R.; Alexander, M. L.; Alexandrov, Mikhail; Alvarez, R. J.; Arnott, W. P.; Atkinson, D.; Baidar, Sunil; Banta, Robert M.; Barnard, James C.; Beranek, Josef; Berg, Larry K.; Brechtel, Fred J.; Brewer, W. A.; Cahill, John F.; Cairns, Brian; Cappa, Christopher D.; Chand, Duli; China, Swarup; Comstock, Jennifer M.; Dubey, Manvendra K.; Easter, Richard C.; Erickson, Matthew H.; Fast, Jerome D.; Floerchinger, Cody; Flowers, B. A.; Fortner, Edward; Gaffney, Jeffrey S.; Gilles, Mary K.; Gorkowski, K.; Gustafson, William I.; Gyawali, Madhu S.; Hair, John; Hardesty, Michael; Harworth, J. W.; Herndon, Scott C.; Hiranuma, Naruki; Hostetler, Chris A.; Hubbe, John M.; Jayne, J. T.; Jeong, H.; Jobson, Bertram T.; Kassianov, Evgueni I.; Kleinman, L. I.; Kluzek, Celine D.; Knighton, B.; Kolesar, K. R.; Kuang, Chongai; Kubatova, A.; Langford, A. O.; Laskin, Alexander; Laulainen, Nels S.; Marchbanks, R. D.; Mazzoleni, Claudio; Mei, F.; Moffet, Ryan C.; Nelson, Danny A.; Obland, Michael; Oetjen, Hilke; Onasch, Timothy B.; Ortega, Ivan; Ottaviani, M.; Pekour, Mikhail S.; Prather, Kimberly A.; Radney, J. G.; Rogers, Ray; Sandberg, S. P.; Sedlacek, Art; Senff, Christoph; Senum, Gunar; Setyan, Ari; Shilling, John E.; Shrivastava, ManishKumar B.; Song, Chen; Springston, S. R.; Subramanian, R.; Suski, Kaitlyn; Tomlinson, Jason M.; Volkamer, Rainer M.; Wallace, Hoyt A.; Wang, J.; Weickmann, A. M.; Worsnop, Douglas R.; Yu, Xiao-Ying; Zelenyuk, Alla; Zhang, Qi

    2012-08-22

    Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climate-related properties in freshly polluted and 'aged' urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: a) the scientific background and motivation for the study, b) the operational and logistical information pertinent to the execution of the study, c) an overview of key observations and initial results from the aircraft and ground-based sampling platforms, and d) a roadmap of planned data analyses and focused modeling efforts that will facilitate the integration of new knowledge into improved representations of key aerosol processes in climate models.

  6. ARM - Field Campaign - Fall 1997 Aerosol IOP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsFall 1997 Aerosol IOP ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Fall 1997 Aerosol IOP 1997.09.15 - 1997.10.05 Lead Scientist : Stephen Schwartz For data sets, see below. Summary The Aerosol IOP was highlighted by the Gulfstream-1 aircraft flying clear-sky aerosol missions over the Central Facility to study the effect of aerosol loading on clear sky radiation fields, with weather

  7. ARM - Evaluation Product - Organic Aerosol Component VAP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ProductsOrganic Aerosol Component VAP ARM Data Discovery Browse Data Documentation Use the Data File Inventory tool to view data availability at the file level. Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Evaluation Product : Organic Aerosol Component VAP Organic aerosol (OA, i.e., the organic fraction of particles) accounts for 10-90% of the fine aerosol mass globally and is a key determinant of aerosol radiative forcing. But atmospheric OA

  8. Mercury Speciation in Coal-Fired Power Plant Flue Gas-Experimental Studies and Model Development

    SciTech Connect (OSTI)

    Radisav Vidic; Joseph Flora; Eric Borguet

    2008-12-31

    The overall goal of the project was to obtain a fundamental understanding of the catalytic reactions that are promoted by solid surfaces present in coal combustion systems and develop a mathematical model that described key phenomena responsible for the fate of mercury in coal-combustion systems. This objective was achieved by carefully combining laboratory studies under realistic process conditions using simulated flue gas with mathematical modeling efforts. Laboratory-scale studies were performed to understand the fundamental aspects of chemical reactions between flue gas constituents and solid surfaces present in the fly ash and their impact on mercury speciation. Process models were developed to account for heterogeneous reactions because of the presence of fly ash as well as the deliberate addition of particles to promote Hg oxidation and adsorption. Quantum modeling was used to obtain estimates of the kinetics of heterogeneous reactions. Based on the initial findings of this study, additional work was performed to ascertain the potential of using inexpensive inorganic sorbents to control mercury emissions from coal-fired power plants without adverse impact on the salability fly ash, which is one of the major drawbacks of current control technologies based on activated carbon.

  9. Genomic Speciation and Adaptation in Aquilegia (2011 JGI User Meeting)

    ScienceCinema (OSTI)

    Hodges, Scott [University of California, Santa Barbara

    2011-06-03

    The U.S. Department of Energy Joint Genome Institute (JGI) invited scientists interested in the application of genomics to bioenergy and environmental issues, as well as all current and prospective users and collaborators, to attend the annual DOE JGI Genomics of Energy & Environment Meeting held March 22-24, 2011 in Walnut Creek, Calif. The emphasis of this meeting was on the genomics of renewable energy strategies, carbon cycling, environmental gene discovery, and engineering of fuel-producing organisms. The meeting features presentations by leading scientists advancing these topics. Scott Hodges of the University of California, Santa Barbara gives a presentation on "Genomic Speciation and Adaptation in Aquilegia" at the 6th annual Genomics of Energy & Environment Meeting on March 23, 2011

  10. Genomic Speciation and Adaptation in Aquilegia (2011 JGI User Meeting)

    SciTech Connect (OSTI)

    Hodges, Scott [University of California, Santa Barbara] [University of California, Santa Barbara

    2011-03-23

    The U.S. Department of Energy Joint Genome Institute (JGI) invited scientists interested in the application of genomics to bioenergy and environmental issues, as well as all current and prospective users and collaborators, to attend the annual DOE JGI Genomics of Energy & Environment Meeting held March 22-24, 2011 in Walnut Creek, Calif. The emphasis of this meeting was on the genomics of renewable energy strategies, carbon cycling, environmental gene discovery, and engineering of fuel-producing organisms. The meeting features presentations by leading scientists advancing these topics. Scott Hodges of the University of California, Santa Barbara gives a presentation on "Genomic Speciation and Adaptation in Aquilegia" at the 6th annual Genomics of Energy & Environment Meeting on March 23, 2011

  11. Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

    SciTech Connect (OSTI)

    Baustian, Kelly J.; Cziczo, Daniel J.; Wise, M. A.; Pratt, Kerri; Kulkarni, Gourihar R.; Hallar, Anna G.; Tolbert, Margaret A.

    2012-03-30

    In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single-particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse-mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine-mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic-containing particles serve as efficient ice nuclei while others do not. For coarse-mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

  12. Technetium Inventory, Distribution, and Speciation in Hanford Tanks

    SciTech Connect (OSTI)

    Serne, R. Jeffrey; Rapko, Brian M.

    2014-05-02

    The purpose of this report is three fold: 1) assemble the available information regarding technetium (Tc) inventory, distribution between phases, and speciation in Hanford’s 177 storage tanks into a single, detailed, comprehensive assessment; 2) discuss the fate (distribution/speciation) of Tc once retrieved from the storage tanks and processed into a final waste form; and 3) discuss/document in less detail the available data on the inventory of Tc in other "pools" such as the vadose zone below inactive cribs and trenches, below single-shell tanks (SSTs) that have leaked, and in the groundwater below the Hanford Site. A thorough understanding of the inventory for mobile contaminants is key to any performance or risk assessment for Hanford Site facilities because potential groundwater and river contamination levels are proportional to the amount of contaminants disposed at the Hanford Site. Because the majority of the total 99Tc produced at Hanford (~32,600 Ci) is currently stored in Hanford’s 177 tanks (~26,500 Ci), there is a critical need for knowledge of the fate of this 99Tc as it is removed from the tanks and processed into a final solid waste form. Current flow sheets for the Hanford Waste Treatment and Immobilization Plant process show most of the 99Tc will be immobilized as low-activity waste glass that will remain on the Hanford Site and disposed at the Integrated Disposal Facility (IDF); only a small fraction will be shipped to a geologic repository with the immobilized high-level waste. Past performance assessment studies, which focused on groundwater protection, have shown that 99Tc would be the primary dose contributor to the IDF performance.

  13. Results of Hg speciation testing on tanks 30, 32, and 37 surface samples

    SciTech Connect (OSTI)

    Bannochie, C. J.

    2015-11-11

    The Savannah River National Laboratory (SRNL) was tasked with preparing and shipping samples for Hg speciation by Eurofins Frontier Global Sciences, Inc. in Seattle, WA on behalf of the Savannah River Remediation (SRR) Mercury Task Team.

  14. he Impact of Primary Marine Aerosol on Atmospheric Chemistry, Radiation and Climate: A CCSM Model Development Study

    SciTech Connect (OSTI)

    Keene, William C.; Long, Michael S.

    2013-05-20

    This project examined the potential large-scale influence of marine aerosol cycling on atmospheric chemistry, physics and radiative transfer. Measurements indicate that the size-dependent generation of marine aerosols by wind waves at the ocean surface and the subsequent production and cycling of halogen-radicals are important but poorly constrained processes that influence climate regionally and globally. A reliable capacity to examine the role of marine aerosol in the global-scale atmospheric system requires that the important size-resolved chemical processes be treated explicitly. But the treatment of multiphase chemistry across the breadth of chemical scenarios encountered throughout the atmosphere is sensitive to the initial conditions and the precision of the solution method. This study examined this sensitivity, constrained it using high-resolution laboratory and field measurements, and deployed it in a coupled chemical-microphysical 3-D atmosphere model. First, laboratory measurements of fresh, unreacted marine aerosol were used to formulate a sea-state based marine aerosol source parameterization that captured the initial organic, inorganic, and physical conditions of the aerosol population. Second, a multiphase chemical mechanism, solved using the Max Planck Institute for Chemistry??s MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) system, was benchmarked across a broad set of observed chemical and physical conditions in the marine atmosphere. Using these results, the mechanism was systematically reduced to maximize computational speed. Finally, the mechanism was coupled to the 3-mode modal aerosol version of the NCAR Community Atmosphere Model (CAM v3.6.33). Decadal-scale simulations with CAM v.3.6.33, were run both with and without reactive-halogen chemistry and with and without explicit treatment of particulate organic carbon in the marine aerosol source function. Simulated results were interpreted (1) to evaluate influences of marine aerosol production on the microphysical properties of aerosol populations and clouds over the ocean and the corresponding direct and indirect effects on radiative transfer; (2) atmospheric burdens of reactive halogen species and their impacts on O3, NOx, OH, DMS, and particulate non-sea-salt SO42-; and (3) the global production and influences of marine-derived particulate organic carbon. The model reproduced major characteristics of the marine aerosol system and demonstrated the potential sensitivity of global, decadal-scale climate metrics to multiphase marine-derived components of Earth??s troposphere. Due to the combined computational burden of the coupled system, the currently available computational resources were the limiting factor preventing the adequate statistical analysis of the overall impact that multiphase chemistry might have on climate-scale radiative transfer and climate.

  15. Investigation of critical equivalence ratio and chemical speciation in flames of ethylbenzene-ethanol blends

    SciTech Connect (OSTI)

    Therrien, Richard J.; Ergut, Ali; Levendis, Yiannis A.; Richter, Henning; Howard, Jack B.; Carlson, Joel B.

    2010-02-15

    This work investigates five different one-dimensional, laminar, atmospheric pressure, premixed ethanol/ethylbenzene flames (0%, 25%, 50%, 75% and 90% ethanol by weight) at their soot onset threshold ({phi}{sub critical}). Liquid ethanol/ethylbenzene mixtures were pre-vaporized in nitrogen, blended with an oxygen-nitrogen mixture and, upon ignition, burned in premixed one-dimensional flames at atmospheric pressure. The flames were controlled so that each was at its visual soot onset threshold, and all had similar temperature profiles (determined by thermocouples). Fixed gases, light volatile hydrocarbons, polycyclic aromatic hydrocarbons (PAH), and oxygenated aromatic hydrocarbons were directly sampled at three locations in each flame. The experimental results were compared with a detailed kinetic model, and the modeling results were used to perform a reaction flux analysis of key species. The critical equivalence ratio was observed to increase in a parabolic fashion as ethanol concentration increased in the fuel mixture. The experimental results showed increasing trends of methane, ethane, and ethylene with increasing concentrations of ethanol in the flames. Carbon monoxide was also seen to increase significantly with the increase of ethanol in the flame, which removes carbon from the PAH and soot formation pathways. The PAH and oxygenated aromatic hydrocarbon values were very similar in the 0%, 25% and 50% ethanol flames, but significantly lower in the 75% and 90% ethanol flames. These results were in general agreement with the model and were reflected by the model soot predictions. The model predicted similar soot profiles for the 0%, 25% and 50% ethanol flames, however it predicted significantly lower values in the 75% and 90% ethanol flames. The reaction flux analysis revealed benzyl to be a major contributor to single and double ring aromatics (i.e., benzene and naphthalene), which was identified in a similar role in nearly sooting or highly sooting ethylbenzene flames. The presence of this radical was significantly reduced as ethanol concentration was increased in the flames, and this effect in combination with the lower carbon to oxygen ratios and the enhanced formation of carbon monoxide, are likely what allowed higher equivalence ratios to be reached without forming soot. (author)

  16. Laboratory Product Speciation Studies of the LNT + in situ SCR NOx Emission

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Control Concept | Department of Energy Product Speciation Studies of the LNT + in situ SCR NOx Emission Control Concept Laboratory Product Speciation Studies of the LNT + in situ SCR NOx Emission Control Concept Understanding the detailed chemistry of Nox Reduction across the combined LNT+SCR system. PDF icon deer10_crocker.pdf More Documents & Publications Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems Lean NOx

  17. Study of Heterogeneouse Processes Related to the Chemistry of Tropospheric Oxidants and Aerosols

    SciTech Connect (OSTI)

    Davidovits, Paul; Worsnop, D R; Jayne, J T; Colb, C E

    2013-02-13

    The objective of the studies was to elucidate the heterogeneous chemistry of tropospheric aerosols. Experiments were designed to measure both specifically needed parameters, and to obtain systematic data required to build a fundamental understanding of the nature of gas-surface physical and chemical interactions

  18. Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Science Plan

    SciTech Connect (OSTI)

    Fast, JD; Berg, LK

    2015-12-01

    Cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle over the Southern Great Plains and over many regions of the world, particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Current convective cloud parameterizations contain uncertainties resulting in part from insufficient coincident data that couples cloud macrophysical and microphysical properties to inhomogeneities in boundary layer and aerosol properties. The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) campaign is designed to provide a detailed set of measurements that are needed to obtain a more complete understanding of the life cycle of shallow clouds by coupling cloud macrophysical and microphysical properties to land surface properties, ecosystems, and aerosols. HI-SCALE consists of 2, 4-week intensive observational periods, one in the spring and the other in the late summer, to take advantage of different stages and distribution of “greenness” for various types of vegetation in the vicinity of the Atmospheric Radiation and Measurement (ARM) Climate Research Facility’s Southern Great Plains (SGP) site as well as aerosol properties that vary during the growing season. Most of the proposed instrumentation will be deployed on the ARM Aerial Facility (AAF) Gulfstream 1 (G-1) aircraft, including those that measure atmospheric turbulence, cloud water content and drop size distributions, aerosol precursor gases, aerosol chemical composition and size distributions, and cloud condensation nuclei concentrations. Routine ARM aerosol measurements made at the surface will be supplemented with aerosol microphysical properties measurements. The G-1 aircraft will complete transects over the SGP Central Facility at multiple altitudes within the boundary layer, within clouds, and above clouds.

  19. ARM - Mobile Aerosol Observing System

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    FacilitiesMobile Aerosol Observing System AMF Information Science Architecture Baseline Instruments AMF1 AMF2 AMF3 MAOS Data Operations AMF Fact Sheet Images Contacts AMF Deployments McMurdo Station, Antarctica, 2015-2016 Pearl Harbor, Hawaii, to San Francisco, California, 2015 Hyytiälä, Finland, 2014 Manacapuru, Brazil, 2014 Oliktok Point, Alaska, 2013 Los Angeles, California, to Honolulu, Hawaii, 2012 Cape Cod, Massachusetts, 2012 Gan Island, Maldives, 2011 Ganges Valley, India, 2011

  20. Researchers Model Impact of Aerosols Over California

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Researchers Model Impact of Aerosols Over California Researchers Model Impact of Aerosols Over California Research may clarify the effectiveness of regional pollution controls May 28, 2013 Contact: Linda Vu, lvu@lbl.gov, (510) 495-2404 LosAngelesSmogv1.jpg Smog over downtown Los Angeles. Aerosols are microscopic particles-like dust, pollen and soot-that ubiquitously float around in our atmosphere. Despite their tiny stature, these particles can have a huge impact on human health, climate and the

  1. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Composition and Reactions of Atmospheric Aerosol Particles Composition and Reactions of Atmospheric Aerosol Particles Print Wednesday, 29 June 2005 00:00 Microscopic aerosol particles in the atmosphere contain carbonaceous components from mineral dust and combustion emissions released from around the world. How long these tiny particles remain in the atmosphere can have a huge impact on the global climate. Measurements based on high-resolution scanning transmission x-ray images obtained at the

  2. ARM - Campaign Instrument - aerosol-tower-eml

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govInstrumentsaerosol-tower-eml Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign Instrument : EML Tower based Aerosol Measurements (AEROSOL-TOWER-EML) Instrument Categories Aerosols Campaigns Remote Cloud Sensing (RCS) Field Evaluation [ Download Data ] Southern Great Plains, 1994.04.01 - 1994.05.31 Primary Measurements Taken The following measurements are those considered scientifically relevant. Refer to the datastream (netcdf) file

  3. ARM - Cumulus Humilis Aerosol Processing Study (CHAPS)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Study (CHAPS) Campaign Details News Field Participants Resources Status and Actions ARM Data Discovery Browse Data Cumulus Humilis Aerosol Processing Study (CHAPS) Summer 2007 ASP Field Campaign The primary goal of the CHAPS campaign is to characterize and contrast freshly emitted aerosols above, within and below fields of cumulus humilis (or fair-weather cumulus). These observations will be used to examine the aerosol optical properties and cloud nucleating properties from both below-cloud and

  4. Dosimeter for monitoring vapors and aerosols of organic compounds

    DOE Patents [OSTI]

    Vo-Dinh, T.

    1987-07-14

    A dosimeter is provided for collecting and detecting vapors and aerosols of organic compounds. The dosimeter comprises a lightweight, passive device that can be conveniently worn by a person as a badge or placed at a stationary location. The dosimeter includes a sample collector comprising a porous web treated with a chemical for inducing molecular displacement and enhancing phosphorescence. Compounds are collected onto the web by molecular diffusion. The web also serves as the sample medium for detecting the compounds by a room temperature phosphorescence technique. 7 figs.

  5. Dosimeter for monitoring vapors and aerosols of organic compounds

    DOE Patents [OSTI]

    Vo-Dinh, Tuan

    1987-01-01

    A dosimeter is provided for collecting and detecting vapors and aerosols of organic compounds. The dosimeter comprises a lightweight, passive device that can be conveniently worn by a person as a badge or placed at a stationary location. The dosimeter includes a sample collector comprising a porous web treated with a chemical for inducing molecular displacement and enhancing phosphorescence. Compounds are collected onto the web by molecular diffusion. The web also serves as the sample medium for detecting the compounds by a room temperature phosphorescence technique.

  6. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    will help climate scientists refine the computer models used to predict climate change. Tiny Specks with Large Effects Most people equate aerosols with hairspray and...

  7. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    results will help climate scientists refine the computer models used to predict climate change. Tiny Specks with Large Effects Most people equate aerosols with hairspray and...

  8. Composition and Reactions of Atmospheric Aerosol Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    refine the computer models used to predict climate change. Tiny Specks with Large Effects Most people equate aerosols with hairspray and household cleaning products, but a...

  9. The LANL Cloud-Aerosol Model

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    that incorporates two unique aspects in its formulation. First, the model employs a nonlinear solver that requires cloud-aerosol parameterizations be smooth or contain reasonable...

  10. Iodine-129 and Iodine-127 speciation in groundwater at the Hanford Site, U.S.: iodate incorporation into calcite

    SciTech Connect (OSTI)

    Zhang, Saijin; Xu, Chen; Creeley, Danielle; Ho, Yi-Fang; Li, Hsiu-Ping; Grandbois, Russell; Schwehr, Kathy; Kaplan, Daniel I.; Yeager, Chris; Wellman, Dawn M.; Santschi, Peter H.

    2013-09-03

    The Hanford Site, the most contaminated nuclear site in the United States, has large radioactive waste plumes containing high 129I levels. The geochemical transport and fate of radioiodine depends largely on its chemical speciation that is greatly affected by environmental factors. This study reports, for the first time, the speciation of stable and radioactive iodine in the groundwater from the Hanford Site. Iodate was the dominant species and accounts for up to 84%, followed by organo-iodine and minimal levels of iodide. The relatively high pH and oxidizing environment may have prevented iodate reduction. Our results identified that calcite precipitation caused by degassing of CO2 during deep groundwater sampling incorporated between 7 to 40% of dissolved iodine (including 127I and 129I) that was originally in the groundwater, transforming dissolved to particulate iodate during sampling. In order to understand the mechanisms underlying iodine incorporation by calcite, laboratory experiments were carried out to replicate this iodine sequestering processes. Two methods were utilized in this study, 1) addition of sodium carbonate; 2) addition of calcium chloride followed by sodium carbonate where the pH was well controlled at ~8.2, which is close to the average pH of Hanford Site groundwater. It was demonstrated that iodate was the main species incorporated into calcite and this incorporation process could be impeded by elevated pH and decreasing ionic strength in groundwater. This study provides critical information for predicting the long-term fate and transport of 129I at the Hanford Site and reveals a potential means for improved remediation strategies of 129I.

  11. Development of a Fast Time-Resolved Aerosol Collector (Fast TRAC)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Yu & James Cowin PNNL Fast Time-Resolved Aerosol Collector ......Fast TRAC...... Xiao-Ying Yu, Ali Hashim, Martin Iedema, and James Cowin Atmospheric Sciences, Chemical Sciences Pacific Northwest National Laboratory Richland, WA Research is supported by NOAA & DOE. *Patent Pending Xiao-Ying Yu & James Cowin PNNL Cloud Microstructures ≤ 1 m Want to know the aerosols at this resolution Aircraft flies at 150 m/s Need time resolution 1 m/150 m/s = 6 ms (!!!!!) Xiao-Ying Yu & James

  12. Development of a Fast Time-Resolved Aerosol Collector (Fast TRAC)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Yu, James Cowin PNNL Probing Aerosols in Cloud Microstructures with Single Particle "Fast TRAC" Xiao-Ying Yu, Martin Iedema, and James Cowin Atmospheric Sciences, Chemical Sciences Pacific Northwest National Laboratory Richland, WA Research is supported by NOAA & DOE. *Patent Pending Xiao-Ying Yu, James Cowin PNNL Cloud Microstructures ≤ 1 m Want to know the aerosols at this resolution Aircraft flies at 150 m/s Need time resolution 1 m/150 m/s = 6 ms (!!!!!) Xiao-Ying Yu, James

  13. ARM - Field Campaign - Aerosol and Cloud Experiments in the Eastern...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    horizontal variabilities of aerosol, trace gases, cloud, drizzle, and atmospheric thermodynamics are critically needed for understanding and quantifying the budget of MBL aerosol,...

  14. Analysis of Langley optical depth data, with aerosol and gas...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Columbia University - NASAGISS Lacis, Andrew NASAGoddard Institute for Space Studies Carlson, Barbara NASAGoddard Institute for Space Studies Category: Aerosols Bimodal aerosol...

  15. The Indirect and Semi-Direct Aerosol Campaign

    SciTech Connect (OSTI)

    Ghan, Steve

    2014-03-24

    Research projects like the Indirect and Semi-Direct Aerosol Campaign, or ISDAC, increase our knowledge of atmospheric aerosol particles and cloud physics.

  16. ARM - Field Campaign - Carbonaceous Aerosol and Radiative Effects...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsCarbonaceous Aerosol and Radiative Effects Study (CARES) Campaign Links CARES Website ARM Data Discovery Browse Data Related Campaigns Carbonaceous Aerosol and...

  17. ARM - Field Campaign - Carbonaceous Aerosol and Radiation Effects...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Photo-Acoustic Aerosol Light Absorption and Scattering Campaign Links ARM Data Discovery Browse Data Related Campaigns Carbonaceous Aerosol and Radiative Effects Study (CARES)...

  18. The Indirect and Semi-Direct Aerosol Campaign

    ScienceCinema (OSTI)

    Ghan, Steve

    2014-06-12

    Research projects like the Indirect and Semi-Direct Aerosol Campaign, or ISDAC, increase our knowledge of atmospheric aerosol particles and cloud physics.

  19. Speciation of technetium peroxo complexes in sulfuric acid revisited

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Poineau, Frederic; German, Konstantin E.; Burton-Pye, Benjamin P.; Weck, Philippe F.; Kim, Eunja; Kriyzhovets, Olga; Safonov, Aleksey; Ilin, Viktor; Francesconi, Lynn C.; Sattelberger, Alfred P.; et al

    2014-08-24

    We found that the reaction of Tc(+7) with H2O2 has been studied in H2SO4 and the speciation of technetium performed by UV–visible and 99-Tc NMR spectroscopy. UV–visible measurements show that for H2SO4 ≥ 9 M and H2O2 = 0.17 M, TcO3(OH)(H2O)2 reacts immediately and blue solutions are obtained, while no reaction occurs for H2SO42SO44 - begins to react for H2O2 = 2.12 M and red solutions are obtained. The UV–visible spectra of the red species are identical to the one obtained from the reaction of TcO4 - with H2O2 in HNO3 and consistent with the presence of TcO(O2)2(H2O)(OH). The 99-Tcmore » NMR spectrum of the red solution exhibits a broad signal centered at +5.5 ppm vs TcO4 - and is consistent with the presence of a low symmetry Tc(+7) molecule.« less

  20. Use of micro-XANES to speciate chromium in airborne fine particles in the Sacramento Valley

    SciTech Connect (OSTI)

    Michelle L. Werner; Peter S. Nico; Matthew A. Marcus; Cort Anastasio

    2007-07-15

    While particulate matter (PM) in the atmosphere can lead to a wide array of negative health effects, the cause of toxicity is largely unknown. One aspect of PM that likely affects health is the chemical composition, in particular the transition metals within the particles. Chromium is one transition metal of interest due to its two major oxidation states, with Cr(III) being much less toxic compared to Cr(VI). Using microfocused X-ray absorption near edge structure (micro-XANES), we analyzed the Cr speciation in fine particles (diameters {le} 2.5 {mu}m) collected at three sites in the Sacramento Valley of northern California: Sacramento, a large urban area, Davis, a small city, and Placerville, a rural area. These are several major stationary sources of Cr within 24 km of the site including chrome-plating plants, power plants and incinerators. The microfocused X-ray beam enables us to look at very small areas on the filter with a resolution of typically 5-7 micrometers. With XANES we are able to not only distinguish between Cr(VI) and Cr(III), but also to identify different types of Cr(III) and more reduced Cr species. At all of our sampling sites the main Cr species were Cr(III), with Cr(OH){sub 3} or a Cr-Fe, chromite-like, phase being the dominant species. Cr(VI)-containing particles were found only in the most urban site. All three sites contained some reduced Cr species, either Cr(0) or Cr{sub 3}C{sub 2}, although these were minor components. This work demonstrates that micro-XANES can be used as a minimally invasive analytical tool to investigate the composition of ambient PM. 32 refs., 6 figs.

  1. ARM - Campaign Instrument - acsm

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign Instrument : Aerosol Chemical Speciation Monitor (ACSM) Instrument Categories...

  2. AEROSOL PARTICLE COLLECTOR DESIGN STUDY

    SciTech Connect (OSTI)

    Lee, S; Richard Dimenna, R

    2007-09-27

    A computational evaluation of a particle collector design was performed to evaluate the behavior of aerosol particles in a fast flowing gas stream. The objective of the work was to improve the collection efficiency of the device while maintaining a minimum specified air throughput, nominal collector size, and minimal power requirements. The impact of a range of parameters was considered subject to constraints on gas flow rate, overall collector dimensions, and power limitations. Potential improvements were identified, some of which have already been implemented. Other more complex changes were identified and are described here for further consideration. In addition, fruitful areas for further study are proposed.

  3. Aerosol characterization study using multi-spectrum remote sensing measurement techniques.

    SciTech Connect (OSTI)

    Glen, Crystal Chanea; Sanchez, Andres L.; Lucero, Gabriel Anthony; Schmitt, Randal L.; Johnson, Mark S.; Tezak, Matthew Stephen; Servantes, Brandon Lee

    2013-09-01

    A unique aerosol flow chamber coupled with a bistatic LIDAR system was implemented to measure the optical scattering cross sections and depolarization ratio of common atmospheric particulates. Each of seven particle types (ammonium sulfate, ammonium nitrate, sodium chloride, potassium chloride, black carbon and Arizona road dust) was aged by three anthropogenically relevant mechanisms: 1. Sulfuric acid deposition, 2. Toluene ozonolysis reactions, and 3. m-Xylene ozonolysis reactions. The results of pure particle scattering properties were compared with their aged equivalents. Results show that as most particles age under industrial plume conditions, their scattering cross sections are similar to pure black carbon, which has significant impacts to our understanding of aerosol impacts on climate. In addition, evidence emerges that suggest chloride-containing aerosols are chemically altered during the organic aging process. Here we present the direct measured scattering cross section and depolarization ratios for pure and aged atmospheric particulates.

  4. Sources and composition of submicron organic mass in marine aerosol particles: Marine Aerosol Organic Mass Composition

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-26

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 6512% hydroxyl, 219% alkane, 66% amine, and 78% carboxylic acid functional groups. Contributions from photochemicalmorereactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA productionless

  5. A New WRF-Chem Treatment for Studying Regional Scale Impacts of Cloud-Aerosol Interactions in Parameterized Cumuli

    SciTech Connect (OSTI)

    Berg, Larry K.; Shrivastava, ManishKumar B.; Easter, Richard C.; Fast, Jerome D.; Chapman, Elaine G.; Liu, Ying

    2015-01-01

    A new treatment of cloud-aerosol interactions within parameterized shallow and deep convection has been implemented in WRF-Chem that can be used to better understand the aerosol lifecycle over regional to synoptic scales. The modifications to the model to represent cloud-aerosol interactions include treatment of the cloud dropletnumber mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. Thesechanges have been implemented in both the WRF-Chem chemistry packages as well as the Kain-Fritsch cumulus parameterization that has been modified to better represent shallow convective clouds. Preliminary testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS) as well as a high-resolution simulation that does not include parameterized convection. The simulation results are used to investigate the impact of cloud-aerosol interactions on the regional scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column integrated BC can be as large as -50% when cloud-aerosol interactions are considered (due largely to wet removal), or as large as +35% for sulfate in non-precipitating conditions due to the sulfate production in the parameterized clouds. The modifications to WRF-Chem version 3.2.1 are found to account for changes in the cloud drop number concentration (CDNC) and changes in the chemical composition of cloud-drop residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to WRF-Chem version 3.5, and it is anticipated that they will be included in a future public release of WRF-Chem.

  6. Canadian House Dust Study: Lead Bioaccessibility and Speciation

    SciTech Connect (OSTI)

    P Rasmussen; S Beauchemin; M Chenier; C Levesque; L MacLean; L Marrow; H Jones-Otazo; S Petrovic; L McDonald; H Gardner

    2011-12-31

    Vacuum samples were collected from 1025 randomly selected urban Canadian homes to investigate bioaccessible Pb (Pb{sub S}) concentrations in settled house dust. Results indicate a polymodal frequency distribution, consisting of three lognormally distributed subpopulations defined as 'urban background' (geomean 58 {micro}g g{sup -1}), 'elevated' (geomean 447 {micro}g g{sup -1}), and 'anomalous' (geomean 1730 {micro}g g{sup -1}). Dust Pb{sub S} concentrations in 924 homes (90%) fall into the 'urban background' category. The elevated and anomalous subpopulations predominantly consist of older homes located in central core areas of cities. The influence of house age is evidenced by a moderate correlation between house age and dust Pb{sub S} content (R{sup 2} = 0.34; n = 1025; p < 0.01), but it is notable that more than 10% of homes in the elevated/anomalous category were built after 1980. Conversely, the benefit of home remediation is evidenced by the large number of homes (33%) in the background category that were built before 1960. The dominant dust Pb species determined using X-ray Absorption Spectroscopy were as follows: Pb carbonate, Pb hydroxyl carbonate, Pb sulfate, Pb chromate, Pb oxide, Pb citrate, Pb metal, Pb adsorbed to Fe- and Al-oxyhydroxides, and Pb adsorbed to humate. Pb bioaccessibility estimated from solid phase speciation predicts Pb bioaccessibility measured using a simulated gastric extraction (R{sup 2} = 0.85; n = 12; p < 0.0001). The trend toward increased Pb bioaccessibility in the elevated and anomalous subpopulations (75% {+-} 18% and 81% {+-} 8%, respectively) compared to background (63% {+-} 18%) is explained by the higher proportion of bioaccessible compounds used as pigments in older paints (Pb carbonate and Pb hydroxyl carbonate). This population-based study provides a nationally representative urban baseline for applications in human health risk assessment and risk management.

  7. ARM - Field Campaign - Two-Column Aerosol Project (TCAP)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsTwo-Column Aerosol Project (TCAP) Campaign Links TCAP website ARM Data Discovery Browse Data Related Campaigns Two-Column Aerosol Project (TCAP): Field Evaluation of Real-time Cloud OD Sensor TWST 2013.04.15, Scott, AMF Two-Column Aerosol Project (TCAP): Winter Aerosol Effects on Cloud Formation 2013.02.04, Cziczo, AMF Two-Column Aerosol Project (TCAP): CU GMAX-DOAS Deployment 2012.07.15, Volkamer, AMF Two-Column Aerosol Project (TCAP): Aerosol Light Extinction Measurements

  8. Iron speciation in minerals and glasses probed by M [subscript 2/3] -edge

    Office of Scientific and Technical Information (OSTI)

    X-ray Raman scattering spectroscopy (Journal Article) | SciTech Connect Iron speciation in minerals and glasses probed by M [subscript 2/3] -edge X-ray Raman scattering spectroscopy Citation Details In-Document Search Title: Iron speciation in minerals and glasses probed by M [subscript 2/3] -edge X-ray Raman scattering spectroscopy Authors: Nyrow, A. ; Sternemann, C. ; Wilke, M. ; Gordon, R.A. ; Mende, K. ; Yava ; #351 ; , H. ; Simonelli, L. ; Hiraoka, N. ; Sahle, Ch.J. ; Huotari, S. ;

  9. Factors Controlling Redox Speciation of Plutonium and Neptunium in Extraction Separation Processes

    SciTech Connect (OSTI)

    Paulenova, Alena; Vandegrift, III, George F.

    2013-09-24

    The objective of the project was to examine the factors controlling redox speciation of plutonium and neptunium in UREX+ extraction in terms of redox potentials, redox mechanism, kinetics and thermodynamics. Researchers employed redox-speciation extractions schemes in parallel to the spectroscopic experiments. The resulting distribution of redox species w studied uring spectroscopic, electrochemical, and spectro-electrochemical methods. This work reulted in collection of data on redox stability and distribution of redox couples in the nitric acid/nitrate electrolyte and the development of redox buffers to stabilize the desired oxidation state of separated radionuclides. The effects of temperature and concentrations on the redox behavior of neptunium were evaluated.

  10. CARES: Carbonaceous Aerosol and Radiative Effects Study Science Plan

    SciTech Connect (OSTI)

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-05-27

    Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been previously shown to play a major role in the direct and indirect radiative forcing of climate. The primary objective of the CARES 2010 intensive field study is to investigate the evolution of carbonaceous aerosols of different types and their effects on optical and cloud formation properties.

  11. Natural Radionuclides and Isotopic Signatures for Determining Carbonaceous Aerosol Sources, Aerosol Lifetimes, and Washout Processes

    SciTech Connect (OSTI)

    Gaffney, Jeffrey

    2012-12-12

    This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

  12. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect (OSTI)

    Richard A. Ferrare; David D. Turner

    2011-09-01

    Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

  13. Long-Term Measurements of Submicrometer Aerosol

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    non-refractory submicron particulate matter (NR-PM1) including organic aerosol (OA), sulfate (SO 4 2- ), nitrate (NO 3 - ), ammonium (NH 4 + ), and chloride (Cl-). In this study,...

  14. ARM - Field Campaign - MASRAD: Marine Aerosol Properties

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsMASRAD: Marine Aerosol Properties Campaign Links AMF Point Reyes Website Comments? We would love to hear from you Send us a note below or call us at 1-888-ARM-DATA....

  15. ARM - Field Campaign - Aerosol Lidar Validation Experiment -...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsAerosol Lidar Validation Experiment - ALIVE Campaign Links ALIVE Website ARM Data Discovery Browse Data Comments? We would love to hear from you Send us a note below...

  16. ARM - Evaluation Product - Aerosol Modeling Testbed

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and satellite aerosol optical depth data is included to supplement and enhance the value of the CARES data. The software that is provided in AMT extracts model output from...

  17. Study of Aerosol Indirect Effects in China

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Indirect Effects in China In 2008, the U.S. Department of Energy (DOE)'s Atmospheric Radiation Measurement (ARM) Climate Research Facility is providing the ARM Mobile...

  18. Aerosol fabrication methods for monodisperse nanoparticles

    DOE Patents [OSTI]

    Jiang, Xingmao; Brinker, C Jeffrey

    2014-10-21

    Exemplary embodiments provide materials and methods for forming monodisperse particles. In one embodiment, the monodisperse particles can be formed by first spraying a nanoparticle-containing dispersion into aerosol droplets and then heating the aerosol droplets in the presence of a shell precursor to form core-shell particles. By removing either the shell layer or the nanoparticle core of the core-shell particles, monodisperse nanoparticles can be formed.

  19. Electrically Driven Technologies for Radioactive Aerosol Abatement

    SciTech Connect (OSTI)

    David W. DePaoli; Ofodike A. Ezekoye; Costas Tsouris; Valmor F. de Almeida

    2003-01-28

    The purpose of this research project was to develop an improved understanding of how electriexecy driven processes, including electrocoalescence, acoustic agglomeration, and electric filtration, may be employed to efficiently treat problems caused by the formation of aerosols during DOE waste treatment operations. The production of aerosols during treatment and retrieval operations in radioactive waste tanks and during thermal treatment operations such as calcination presents a significant problem of cost, worker exposure, potential for release, and increased waste volume.

  20. Emerging Technology for Measuring Atmospheric Aerosol Properties

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Technology for Measuring Atmospheric Aerosol Properties Bruce Gandrud Greg Kok Droplet Measurement Technologies Darrel Baumgardner Centro de Ciencias de la Atmósfera Universidad Nacional Autónoma de México Acknowledgements * The DMT staff * Bob Bluth and Haflidi Jonsson * Pat Arnott * Greg Roberts and Thanos Nenes * Dave Fahey, Shuka Schwarz and Ru-Shan Gao * NSF, NASA, ONR, NOAA and DOE Introducing Droplet Measurement Technologies * Founded in 1987 * Specializing in aerosol and cloud

  1. WRF-Chem Simulations of Aerosols and Anthropogenic Aerosol Radiative Forcing in East Asia

    SciTech Connect (OSTI)

    Gao, Yi; Zhao, Chun; Liu, Xiaohong; Zhang, Meigen; Leung, Lai-Yung R.

    2014-08-01

    This study aims to provide a first comprehensive evaluation of WRF-Chem for modeling aerosols and anthropogenic aerosol radiative forcing (RF) over East Asia. Several numerical experiments were conducted from November 2007 to December 2008. Comparison between model results and observations shows that the model can generally reproduce the observed spatial distributions of aerosol concentration, aerosol optical depth (AOD) and single scattering albedo (SSA) from measurements at different sites, including the relatively higher aerosol concentration and AOD over East China and the relatively lower AOD over Southeast Asia, Korean, and Japan. The model also depicts the seasonal variation and transport of pollutions over East Asia. Particulate matter of 10 um or less in the aerodynamic diameter (PM10), black carbon (BC), sulfate (SO42-), nitrate (NO3-) and ammonium (NH4+) concentrations are higher in spring than other seasons in Japan due to the pollutant transport from polluted area of East Asia. AOD is high over Southwest and Central China in winter, spring and autumn and over North China in summer while is low over South China in summer due to monsoon precipitation. SSA is lowest in winter and highest in summer. The model also captures the dust events at the Zhangye site in the semi-arid region of China. Anthropogenic aerosol RF is estimated to range from -5 to -20 W m-2 over land and -20 to -40 W m-2 over ocean at the top of atmosphere (TOA), 5 to 30 W m-2 in the atmosphere (ATM) and -15 to -40 W m-2 at the bottom (BOT). The warming effect of anthropogenic aerosol in ATM results from BC aerosol while the negative aerosol RF at TOA is caused by scattering aerosols such as SO4 2-, NO3 - and NH4+. Positive BC RF at TOA compensates 40~50% of the TOA cooling associated with anthropogenic aerosol.

  2. The First Aerosol Indirect Effect: Beyond Twomey

    SciTech Connect (OSTI)

    Liu, Y.; Dunn, M.; Daum, P.

    2008-03-10

    The traditional first aerosol indirect effect or the Twomey effect involves several fundamental assumptions. Some of the assumptions (e.g., constant liquid water content) are explicitly stated in studies of the Twomey effect whereas others are only implicitly embedded in the quantitative formulation. This work focuses on examining the implicit assumptions. In particular, we will show that anthropogenic pollution not only increases aerosol loading and droplet concentrations but also alters the relative dispersions of both the aerosol and subsequent droplet size distributions. The indirect effects resulting from the two altered relative dispersions (aerosol dispersion effect and droplet dispersion effect) are likely opposite in sign and proportional in magnitude to the conventional Twomey effect. This result suggests that the outstanding problems of the Twomey effect (i.e., large uncertainty and overestimation reported in literature) may lie with violation of the constant spectral shapes of aerosol and droplet size distributions implicitly assumed in evaluation of the Twomey effect, and therefore, further progress in understanding and quantification of the first aerosol indirect effect demands moving beyond the traditional paradigm originally conceived by Twomey.

  3. East Asian Studies of Tropospheric Aerosols and their Impact on Regional Climate (EAST-AIRC): An Overview

    SciTech Connect (OSTI)

    Li, Zhanqing; Li, C.; Chen, H.; Tsay, S. C.; Holben, B. N.; Huang, J.; Li, B.; Maring, H.; Qian, Yun; Shi, Guangyu; Xia, X.; Yin, Y.; Zheng, Y.; Zhuang, G.

    2011-02-01

    As the most populated region of the world, Asia is a major source of aerosols with potential large impact over vast downstream areas. Papers published in this special section describe the variety of aerosols observed in China and their effects and interactions with the regional climate as part of the East Asian Study of Tropospheric Aerosols and Impact on Regional Climate (EAST-AIRC). The majority of the papers are based on analyses of observations made under three field projects, namely, the Atmospheric Radiation Measurements (ARM) Mobile Facility mission in China (AMF10 China), the East Asian Study of Tropospheric Aerosols: an International Regional Experiment (EAST-AIRE), and the Atmospheric Aerosols of China and their Climate Effects (AACCE). The former two are US-China collaborative projects and the latter is a part of the China’s National Basic Research program (or often referred to as “973 project”). Routine meteorological data of China are also employed in some studies. The wealth of general and specialized measurements lead to extensive and close-up investigations of the optical, physical and chemical properties of anthropogenic, natural, and mixed aerosols; their sources, formation and transport mechanisms; horizontal, vertical and temporal variations; direct and indirect effects and interactions with the East Asian monsoon system. Particular efforts are made to advance our understanding of the mixing and interaction between dust and anthropogenic pollutants during transport. Several modeling studies were carried out to simulate aerosol impact on radiation budget, temperature, precipitation, wind and atmospheric circulation, fog, etc. In addition, impacts of the Asian monsoon system on aerosol loading are also simulated.

  4. Equilibrium Speciation of Select Lanthanides in the Presence of Acidic Ligands in Homo- and Heterogeneous Solutions

    SciTech Connect (OSTI)

    Robinson, Troy A.

    2011-08-11

    This dissertation explores lanthanide speciation in liquid solution systems related to separation schemes involving the acidic ligands: bis(2-ethylhexyl) phosphoric acid (HDEHP), lactate, and 8-hydroxyquinoline. Equilibrium speciation of neodymium (Nd3+), sodium (Na+), HDEHP, water, and lactate in the TALSPEAK liquid-liquid extraction system was explored under varied Nd3+ loading of HDEHP in the organic phase and through extraction from aqueous HCl and lactate media. System speciation was probed through vapor pressure osmometry, visible and Fourier Transform Infrared (FTIR) spectroscopy, 22Na and 13C labeled lactate radiotracer distribution measurements, Karl Fischer titrations, and equilibrium pH measurements. Distribution of Nd3+, Na+, lactate, and equilibrium pH were modeled using the SXLSQI software to obtain logKNd and logKNa extraction constants under selected conditions. Results showed that high Nd3+ loading of the HDEHP led to Nd3+ speciation that departs from the ion exchange mechanism and includes formation of highly aggregated, polynuclear [NdLactate(DEHP)2]x; (with x > 1). By substituting lanthanum (La3+) for Nd3+ in this system, NMR scoping experiments using 23Na, 31P nuclei and 13C labeled lactate were performed. Results indicated that this technique is sensitive to changes in system speciation, and that further experiments are warranted. In a homogeneous system representing the TALSPEAK aqueous phase, Lactate protonation behavior at various temperatures was characterized using a combination of potentiometric titration and modeling with the Hyperquad computer program. The temperature dependent deprotonation behavior of lactate showed little change with temperature at 2.0 M NaCl ionic strength. Cloud point extraction is a non-traditional separation technique that starts with a homogeneous phase that becomes heterogeneous by the micellization of surfactants through the increase of temperature. To better understand the behavior of europium (Eu3+) and 8-hydroxyquinoline under cloud point extraction conditions, potentiometric and spectrophotometric titrations coupled with modeling with Hyperquad and SQUAD computer programs were performed to assess europium (Eu3+) and 8-hydroxyquinoline speciation. Experiments in both water and a 1wt% Triton X-114/water mixed solvent were compared to understand the effect of Triton X-114 on the system speciation. Results indicated that increased solvation of 8-hydroxyquinoline by the mixed solvent lead to more stable complexes involving 8-hydroxyquinoline than in water, whereas competition between hydroxide and Triton X-114 for Eu3+ led to lower stability hydrolysis complexes in the mixed solvent than in water. Lanthanide speciation is challenging due to the trivalent oxidation state that leads to multiple ligand complexes, including some mixed complexes. The complexity of the system demands well-designed and precise experiments that capture the nuances of the chemistry. This work increased the understanding of lanthanide speciation in the explored systems, but more work is required to produce a comprehensive understanding of the speciation involved.

  5. Chemical deposition methods using supercritical fluid solutions

    DOE Patents [OSTI]

    Sievers, Robert E. (Boulder, CO); Hansen, Brian N. (Boulder, CO)

    1990-01-01

    A method for depositing a film of a desired material on a substrate comprises dissolving at least one reagent in a supercritical fluid comprising at least one solvent. Either the reagent is capable of reacting with or is a precursor of a compound capable of reacting with the solvent to form the desired product, or at least one additional reagent is included in the supercritical solution and is capable of reacting with or is a precursor of a compound capable of reacting with the first reagent or with a compound derived from the first reagent to form the desired material. The supercritical solution is expanded to produce a vapor or aerosol and a chemical reaction is induced in the vapor or aerosol so that a film of the desired material resulting from the chemical reaction is deposited on the substrate surface. In an alternate embodiment, the supercritical solution containing at least one reagent is expanded to produce a vapor or aerosol which is then mixed with a gas containing at least one additional reagent. A chemical reaction is induced in the resulting mixture so that a film of the desired material is deposited.

  6. Chemical Recycling | Y-12 National Security Complex

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Chemical Recycling Chemical Recycling

  7. Amine-Amine Exchange in Aminium-Methanesulfonate Aerosols

    SciTech Connect (OSTI)

    Dawson, Matthew L.; Varner, Mychel E.; Perraud, Veronique M.; Ezell, Michael J.; Wilson, Jacqueline M.; Zelenyuk, Alla; Gerber, Robert B.; Finlayson-Pitts, Barbara J.

    2014-12-18

    Aerosol particles are ubiquitous in the atmosphere and have been shown to impact the Earths climate, reduce visibility, and adversely affect human health. Modeling the evolution of aerosol systems requires an understanding of the species and mechanisms involved in particle growth, including the complex interactions between particle- and gas-phase species. Here we report studies of displacement of amines (methylamine, dimethylamine or trimethylamine) in methanesulfonate salt particles by exposure to a different gas-phase amine, using a single particle mass spectrometer, SPLAT II. The variation of the displacement with the nature of the amine suggests that behavior is dependent on water in or on the particles. Small clusters of methanesulfonic acid with amines are used as a model in quantum chemical calculations to identify key structural elements that are expected to influence water uptake, and hence the efficiency of displacement by gas-phase molecules in the aminium salts. Such molecular-level understanding of the processes affecting the ability of gas-phase amines to displace particle-phase aminium species is important for modeling the growth of particles and their impacts in the atmosphere.

  8. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    SciTech Connect (OSTI)

    Turner, David, D.; Ferrare, Richard, A.

    2011-07-06

    The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

  9. Airborne aerosol in situ measurements during TCAP: A closure study of total scattering

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Kassianov, Evgueni; Sedlacek, Arthur; Berg, Larry K.; Pekour, Mikhail; Barnard, James; Chand, Duli; Flynn, Connor; Ovchinnikov, Mikhail; Schmid, Beat; Shilling, John; et al

    2015-07-31

    We present a framework for calculating the total scattering of both non-absorbing and absorbing aerosol at ambient conditions from aircraft data. Our framework is developed emphasizing the explicit use of chemical composition data for estimating the complex refractive index (RI) of particles, and thus obtaining improved ambient size spectra derived from Optical Particle Counter (OPC) measurements. The feasibility of our framework for improved calculations of total scattering is demonstrated using three types of data collected by the U.S. Department of Energy’s (DOE) aircraft during the Two-Column Aerosol Project (TCAP). Namely, these data types are: (1) size distributions measured by amore » suite of OPC’s; (2) chemical composition data measured by an Aerosol Mass Spectrometer and a Single Particle Soot Photometer; and (3) the dry total scattering coefficient measured by a integrating nephelometer and scattering enhancement factor measured with a humidification system. We demonstrate that good agreement (~10%) between the observed and calculated scattering can be obtained under ambient conditions (RH < 80%) by applying chemical composition data for the RI-based correction of the OPC-derived size spectra. We also demonstrate that ignoring the RI-based correction or using non-representative RI values can cause a substantial underestimation (~40%) or overestimation (~35%) of the calculated scattering, respectively.« less

  10. Airborne aerosol in situ measurements during TCAP: A closure study of total scattering

    SciTech Connect (OSTI)

    Kassianov, Evgueni; Sedlacek, Arthur; Berg, Larry K.; Pekour, Mikhail; Barnard, James; Chand, Duli; Flynn, Connor; Ovchinnikov, Mikhail; Schmid, Beat; Shilling, John; Tomlinson, Jason; Fast, Jerome

    2015-07-31

    We present a framework for calculating the total scattering of both non-absorbing and absorbing aerosol at ambient conditions from aircraft data. Our framework is developed emphasizing the explicit use of chemical composition data for estimating the complex refractive index (RI) of particles, and thus obtaining improved ambient size spectra derived from Optical Particle Counter (OPC) measurements. The feasibility of our framework for improved calculations of total scattering is demonstrated using three types of data collected by the U.S. Department of Energy’s (DOE) aircraft during the Two-Column Aerosol Project (TCAP). Namely, these data types are: (1) size distributions measured by a suite of OPC’s; (2) chemical composition data measured by an Aerosol Mass Spectrometer and a Single Particle Soot Photometer; and (3) the dry total scattering coefficient measured by a integrating nephelometer and scattering enhancement factor measured with a humidification system. We demonstrate that good agreement (~10%) between the observed and calculated scattering can be obtained under ambient conditions (RH < 80%) by applying chemical composition data for the RI-based correction of the OPC-derived size spectra. We also demonstrate that ignoring the RI-based correction or using non-representative RI values can cause a substantial underestimation (~40%) or overestimation (~35%) of the calculated scattering, respectively.

  11. Chemical microsensors

    DOE Patents [OSTI]

    Li, DeQuan (Los Alamos, NM); Swanson, Basil I. (Los Alamos, NM)

    1995-01-01

    An article of manufacture is provided including a substrate having an oxide surface layer and a selective thin film of a cyclodextrin derivative chemically bound upon said substrate, said film is adapted for the inclusion of a selected organic compound therewith. Such an article can be either a chemical sensor capable of detecting a resultant mass change from inclusion of the selected organic compound or a chemical separator capable of reversibly selectively separating a selected organic compound.

  12. Chemical Science

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Chemical Science /science-innovation/_assets/images/icon-science.jpg Chemical Science National security depends on science and technology. The United States relies on Los Alamos National Laboratory for the best of both. No place on Earth pursues a broader array of world-class scientific endeavors. Actinide Chemistry» Modeling & Simulation» Synthetic and Mechanistic Chemistry» Chemistry for Measurement and Detection Science» Chemical Researcher Jeff Pietryga shows two vials of

  13. Large-Scale Spray Releases: Initial Aerosol Test Results

    SciTech Connect (OSTI)

    Schonewill, Philip P.; Gauglitz, Phillip A.; Bontha, Jagannadha R.; Daniel, Richard C.; Kurath, Dean E.; Adkins, Harold E.; Billing, Justin M.; Burns, Carolyn A.; Davis, James M.; Enderlin, Carl W.; Fischer, Christopher M.; Jenks, Jeromy WJ; Lukins, Craig D.; MacFarlan, Paul J.; Shutthanandan, Janani I.; Smith, Dennese M.

    2012-12-01

    One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of anti-foam agents was assessed with most of the simulants. Orifices included round holes and rectangular slots. The round holes ranged in size from 0.2 to 4.46 mm. The slots ranged from (width × length) 0.3 × 5 to 2.74 × 76.2 mm. Most slots were oriented longitudinally along the pipe, but some were oriented circumferentially. In addition, a limited number of multi-hole test pieces were tested in an attempt to assess the impact of a more complex breach. Much of the testing was conducted at pressures of 200 and 380 psi, but some tests were conducted at 100 psi. Testing the largest postulated breaches was deemed impractical because of the large size of some of the WTP equipment. The purpose of this report is to present the experimental results and analyses for the aerosol measurements obtained in the large-scale test stand. The report includes a description of the simulants used and their properties, equipment and operations, data analysis methodology, and test results. The results of tests investigating the role of slurry particles in plugging of small breaches are reported in Mahoney et al. 2012a. The results of the aerosol measurements in the small-scale test stand are reported in Mahoney et al. (2012b).

  14. Small-Scale Spray Releases: Initial Aerosol Test Results

    SciTech Connect (OSTI)

    Mahoney, Lenna A.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, Garrett N.; Kurath, Dean E.; Buchmiller, William C.; Smith, Dennese M.; Blanchard, Jeremy; Song, Chen; Daniel, Richard C.; Wells, Beric E.; Tran, Diana N.; Burns, Carolyn A.

    2012-11-01

    One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of anti-foam agents was assessed with most of the simulants. Orifices included round holes and rectangular slots. The round holes ranged in size from 0.2 to 4.46 mm. The slots ranged from (width × length) 0.3 × 5 to 2.74 × 76.2 mm. Most slots were oriented longitudinally along the pipe, but some were oriented circumferentially. In addition, a limited number of multi-hole test pieces were tested in an attempt to assess the impact of a more complex breach. Much of the testing was conducted at pressures of 200 and 380 psi, but some tests were conducted at 100 psi. Testing the largest postulated breaches was deemed impractical because of the large size of some of the WTP equipment. This report presents the experimental results and analyses for the aerosol measurements obtained in the small-scale test stand. It includes a description of the simulants used and their properties, equipment and operations, data analysis methodologies, and test results. The results of tests investigating the role of slurry particles in plugging small breaches are reported in Mahoney et al. (2012). The results of the aerosol measurements in the large-scale test stand are reported in Schonewill et al. (2012) along with an analysis of the combined results from both test scales.

  15. Small-Scale Spray Releases: Initial Aerosol Test Results

    SciTech Connect (OSTI)

    Mahoney, Lenna A.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, Garrett N.; Kurath, Dean E.; Buchmiller, William C.; Smith, Dennese M.; Blanchard, Jeremy; Song, Chen; Daniel, Richard C.; Wells, Beric E.; Tran, Diana N.; Burns, Carolyn A.

    2013-05-29

    One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. Two key technical areas were identified where testing results were needed to improve the technical basis by reducing the uncertainty due to extrapolating existing literature results. The first technical need was to quantify the role of slurry particles in small breaches where the slurry particles may plug and result in substantially reduced, or even negligible, respirable fraction formed by high-pressure sprays. The second technical need was to determine the aerosol droplet size distribution and volume from prototypic breaches and fluids, specifically including sprays from larger breaches with slurries where data from the literature are scarce. To address these technical areas, small- and large-scale test stands were constructed and operated with simulants to determine aerosol release fractions and net generation rates from a range of breach sizes and geometries. The properties of the simulants represented the range of properties expected in the WTP process streams and included water, sodium salt solutions, slurries containing boehmite or gibbsite, and a hazardous chemical simulant. The effect of antifoam agents was assessed with most of the simulants. Orifices included round holes and rectangular slots. For the combination of both test stands, the round holes ranged in size from 0.2 to 4.46 mm. The slots ranged from (width × length) 0.3 × 5 to 2.74 × 76.2 mm. Most slots were oriented longitudinally along the pipe, but some were oriented circumferentially. In addition, a limited number of multi-hole test pieces were tested in an attempt to assess the impact of a more complex breach. Much of the testing was conducted at pressures of 200 and 380 psi, but some tests were conducted at 100 psi. Testing the largest postulated breaches was deemed impractical because of the much larger flow rates and equipment that would be required. This report presents the experimental results and analyses for the aerosol measurements obtained in the small-scale test stand. It includes a description of the simulants used and their properties, equipment and operations, data analysis methodologies, and test results. The results of tests investigating the role of slurry particles in plugging small breaches are reported in Mahoney et al. (2012). The results of the aerosol measurements in the large-scale test stand are reported in Schonewill et al. (2012) along with an analysis of the combined results from both test scales.

  16. Hazardous particle binder, coagulant and re-aerosolization inhibitor

    DOE Patents [OSTI]

    Krauter, Paula; Zalk, David; Hoffman, D. Mark

    2011-04-12

    A copolymer and water/ethanol solvent solution capable of binding with airborne contaminants or potential airborne contaminants, such as biological weapon agents or toxic particulates, coagulating as the solvent evaporates, and adhering the contaminants to a surface so as to inhibit the re-suspension of such contaminants. The solution uses a water or ethanol/water mixture for the solvent, and a copolymer having one of several functional group sets so as to have physical and chemical characteristics of high adhesion, low viscosity, low surface tension, negative electrostatic charge, substantially neutral pH, and a low pKa. Use of the copolymer solution prevents re-aerosolization and transport of unwanted, reactive species thus increasing health and safety for personnel charged with decontamination of contaminated buildings and areas.

  17. Hazardous particle binder, coagulant and re-aerosolization inhibitor

    DOE Patents [OSTI]

    Krauter, Paula; Zalk, David; Hoffman, D. Mark

    2012-07-10

    A copolymer and water/ethanol solvent solution capable of binding with airborne contaminants or potential airborne contaminants, such as biological weapon agents or toxic particulates, coagulating as the solvent evaporates, and adhering the contaminants to a surface so as to inhibit the re-suspension of such contaminants. The solution uses a water or ethanol/water mixture for the solvent, and a copolymer having one of several functional group sets so as to have physical and chemical characteristics of high adhesion, low viscosity, low surface tension, negative electrostatic charge, substantially neutral pH, and a low pKa. Use of the copolymer solution prevents re-aerosolization and transport of unwanted, reactive species thus increasing health and safety for personnel charged with decontamination of contaminated buildings and areas.

  18. Removal of Sarin Aerosol and Vapor by Water Sprays

    SciTech Connect (OSTI)

    Brockmann, John E.

    1998-09-01

    Falling water drops can collect particles and soluble or reactive vapor from the gas through which they fall. Rain is known to remove particles and vapors by the process of rainout. Water sprays can be used to remove radioactive aerosol from the atmosphere of a nuclear reactor containment building. There is a potential for water sprays to be used as a mitigation technique to remove chemical or bio- logical agents from the air. This paper is a quick-look at water spray removal. It is not definitive but rather provides a reasonable basic model for particle and gas removal and presents an example calcu- lation of sarin removal from a BART station. This work ~ a starting point and the results indicate that further modeling and exploration of additional mechanisms for particle and vapor removal may prove beneficial.

  19. LABORATORY REPORT ON IODINE ({sup 129}I AND {sup 127}I) SPECIATION, TRANSFORMATION AND MOBILITY IN HANFORD GROUNDWATER, SUSPENDED PARTICLES AND SEDIMENTS

    SciTech Connect (OSTI)

    Kaplan, D.; Santschi, P.; Xu, C.; Zhang, S.; Ho, Y.; Li, H.; Schwehr, K.

    2012-09-30

    The Hanford Site in eastern Washington produced plutonium for several decades and in the process generated billions of gallons of radioactive waste. Included in this complex mixture of waste was 50 Ci of iodine-129 ({sup 129}I). Iodine-129s high abundance, due to its high fission yield, and extreme toxicity result in iodine-129 becoming a key risk driver at many Department of Energy (DOE) sites. The mobility of radioiodine in arid environments, such as the Hanford Site, depends largely on its chemical speciation and is also greatly affected by many other environmental factors, especially natural sediment organic matter (SOM). Groundwater radioiodine speciation has not been measured in arid regions with major plumes or large disposed {sup 129}I inventories, including the Hanford Site, Idaho National Laboratory, and Nevada Test Site. In this study, stable iodine-127 and radioiodine-129 speciation, pH, and dissolved organic carbon (DOC) of groundwater samples collected from seven wells located in the 200-West Area of the Hanford site were investigated. The most striking finding was that iodate (IO{sub 3}{sup -}) was the most abundant species. Unexpectedly, iodide (I{sup -}), which was likely the form of iodine in the source materials and the expected dominant groundwater species based on thermodynamic considerations, only accounted for 1-2% of the total iodine concentration. It is likely that the relatively high pH and the low abundance of sedimentary organic matter (SOM) that is present at the site slowed down or even inhibited the reduction of iodate, as SOM abiotically reduce iodate into iodide. Moreover, a study on the kinetics of iodide and iodate uptake and aqueous speciation transformation by three representative subsurface Hanford sediments was performed over a period of about one month. This study was carried out by using iodide-125 or iodate-125 at the ambient iodine-127concentration found at the site. Iodate K{sub d} values were on average 89% greater than iodide K{sub d} values, and the K{sub d} values for both species tended to increase with the amount of organic carbon (OC) present in the sediment. It is especially noteworthy that this trend existed at the very low OC concentrations that naturally exist in the Hanford sediments. Iodine and OC can form essentially irreversible covalent bonds, thereby providing a yet unstudied {sup 129}I retardation reaction at the Hanford Site. In addition to the transformation of iodine species, the sediment collected from the vadose zone also released stable iodide into the aqueous phase. It was found that the three sediments all took up the ambient iodate from the groundwater and slowly transformed it into iodide under the laboratory conditions, likely dependent on the abundance of reducing agents such as organic matter and Fe{sup 2+}. Therefore two competitive iodine processes were identified, the tendency for the sediment to reduce iodate to iodide, and the groundwater chemistry to maintain the iodine as iodate, presumably it is largely the result of natural pH and dissolved O{sub 2}/Eh levels. Suspended carbonate (and silica) particles collected from Hanford groundwater contained elevated amounts of iodine (142 8 ?g/g iodine), consisting mainly of iodate (>99%). Iodate was likely incorporated into the carbonate structure during calcite precipitation upon degasing of CO{sub 2} as the groundwater samples were removed from the subsurface. This concentration of groundwater iodate in precipitated carbonate has implication to long-term fate and transport of 129I and on active in-situ {sup 129}I groundwater remediation. This study provides some of the first groundwater radioiodine speciation studies conducted in arid environments and provides much needed mechanistic descriptions to permit making informed decisions about low-cost/high intellectual input remediation options, such as monitored natural attenuation, or long-term stewardship of nuclear waste disposal sites.

  20. ARM - VAP Process - oacomp

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Productsoacomp Documentation & Plots Technical Report Data Management Facility Plots (Quick Looks) ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send VAP : Organic Aerosol Component (OACOMP) Instrument Categories Aerosols Both the aerosol mass spectrometer (AMS) and aerosol chemical speciation monitor (ACSM) routinely report the concentrations of inorganic species and total organic matter. Significantly improved

  1. Lidar Measurements of the Vertical Distribution of Aerosol Optical and Physical Properties over Central Asia

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Chen, Boris B.; Sverdlik, Leonid G.; Imashev, Sanjar A.; Solomon, Paul A.; Lantz, Jeffrey; Schauer, James J.; Shafer, Martin M.; Artamonova, Maria S.; Carmichael, Gregory R.

    2013-01-01

    The vertical structure of aerosol optical and physical properties was measured by Lidar in Eastern Kyrgyzstan, Central Asia, from June 2008 to May 2009. Lidar measurements were supplemented with surface-based measurements of PM 2.5 and PM 10 mass and chemical composition in both size fractions. Dust transported into the region is common, being detected 33% of the time. The maximum frequency occurred in the spring of 2009. Dust transported to Central Asia comes from regional sources, for example, Taklimakan desert and Aral Sea basin, and from long-range transport, for example, deserts of Arabia, Northeast Africa, Iran, and Pakistan. Regionalmore » sources are characterized by pollution transport with maximum values of coarse particles within the planetary boundary layer, aerosol optical thickness, extinction coefficient, integral coefficient of aerosol backscatter, and minimum values of the Ångström exponent. Pollution associated with air masses transported over long distances has different characteristics during autumn, winter, and spring. During winter, dust emissions were low resulting in high values of the Ångström exponent (about 0.51) and the fine particle mass fraction (64%). Dust storms were more frequent during spring with an increase in coarse dust particles in comparison to winter. The aerosol vertical profiles can be used to lower uncertainty in estimating radiative forcing.« less

  2. Project Overview: Cumulus Humilis Aerosol Processing Study (CHAPS): Proposed Summer 2007 ASP Field Campaign

    SciTech Connect (OSTI)

    Berkowitz, Carl M.; Berg, Larry K.; Ogren, J. A.; Hostetler, Chris A.; Ferrare, Richard

    2006-05-18

    This white paper presents the scientific motivation and preliminary logistical plans for a proposed ASP field campaign to be carried out in the summer of 2007. The primary objective of this campaign is to use the DOE Gulfstream-1 aircraft to make measurements characterizing the chemical, physical and optical properties of aerosols below, within and above large fields of fair weather cumulus and to use the NASA Langley Research Centers High Spectral Resolution Lidar (HSRL) to make independent measurements of aerosol backscatter and extinction profiles in the vicinity of these fields. Separate from the science questions to be addressed by these observations will be information to add in the development of a parameterized cumulus scheme capable of including multiple cloud fields within a regional or global scale model. We will also be able to compare and contrast the cloud and aerosol properties within and outside the Oklahoma City plume to study aerosol processes within individual clouds. Preliminary discussions with the Cloud and Land Surface Interaction Campaign (CLASIC) science team have identified overlap between the science questions posed for the CLASIC Intensive Operation Period (IOP) and the proposed ASP campaign, suggesting collaboration would benefit both teams.

  3. Next-Generation Genetics in Plants: Evolutionary Trade-off, Immunity and Speciation (2010 JGI User Meeting)

    ScienceCinema (OSTI)

    Wiegel, Detlef

    2011-04-25

    Detlef Wiegel from the Max Planck Institute for Developmental Biology on "Next-generation genetics in plants: Evolutionary tradeoffs, immunity and speciation" on March 25, 2010 at the 5th Annual DOE JGI User Meeting

  4. Aerosol beam-focus laser-induced plasma spectrometer device

    DOE Patents [OSTI]

    Cheng, Meng-Dawn (Oak Ridge, TN)

    2002-01-01

    An apparatus for detecting elements in an aerosol includes an aerosol beam focuser for concentrating aerosol into an aerosol beam; a laser for directing a laser beam into the aerosol beam to form a plasma; a detection device that detects a wavelength of a light emission caused by the formation of the plasma. The detection device can be a spectrometer having at least one grating and a gated intensified charge-coupled device. The apparatus may also include a processor that correlates the wavelength of the light emission caused by the formation of the plasma with an identity of an element that corresponds to the wavelength. Furthermore, the apparatus can also include an aerosol generator for forming an aerosol beam from bulk materials. A method for detecting elements in an aerosol is also disclosed.

  5. ARM - Field Campaign - Two-Column Aerosol Project (TCAP): Aerial...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsTwo-Column Aerosol Project (TCAP): Aerial Campaign ARM Data Discovery Browse Data Related Campaigns Two-Column Aerosol Project (TCAP) 2012.07.01, Berg, AMF Comments? We...

  6. Chemical preconcentrator

    DOE Patents [OSTI]

    Manginell, Ronald P. (Albuquerque, NM); Frye-Mason, Gregory C. (Cedar Crest, NM)

    2001-01-01

    A chemical preconcentrator is disclosed with applications to chemical sensing and analysis. The preconcentrator can be formed by depositing a resistive heating element (e.g. platinum) over a membrane (e.g. silicon nitride) suspended above a substrate. A coating of a sorptive material (e.g. a microporous hydrophobic sol-gel coating or a polymer coating) is formed on the suspended membrane proximate to the heating element to selective sorb one or more chemical species of interest over a time period, thereby concentrating the chemical species in the sorptive material. Upon heating the sorptive material with the resistive heating element, the sorbed chemical species are released for detection and analysis in a relatively high concentration and over a relatively short time period. The sorptive material can be made to selectively sorb particular chemical species of interest while not substantially sorbing other chemical species not of interest. The present invention has applications for use in forming high-sensitivity, rapid-response miniaturized chemical analysis systems (e.g. a "chem lab on a chip").

  7. Chemical sensors

    DOE Patents [OSTI]

    Lowell, J.R. Jr.; Edlund, D.J.; Friesen, D.T.; Rayfield, G.W.

    1991-07-02

    Sensors responsive to small changes in the concentration of chemical species are disclosed. The sensors comprise a mechanochemically responsive polymeric film capable of expansion or contraction in response to a change in its chemical environment. They are operatively coupled to a transducer capable of directly converting the expansion or contraction to a measurable electrical response. 9 figures.

  8. Aerosol can puncture device test report

    SciTech Connect (OSTI)

    Leist, K.J.

    1994-10-01

    This test report documents the evaluation of an aerosol can puncture device to replace a system currently identified for use in the WRAP-1 facility. The new system is based upon a commercially available puncture device, as recommended by WHC Fire Protection. With modifications found necessary through the testing program, the Aerosol Can Puncture Device was found able to puncture and drain aerosol cans without incident. Modifications include the addition of a secondary collection bottle and the modification of the can puncture needle. In the course of testing, a variety of absorbents were tested to determine their performance in immobilizing drained fluids. The visibility of the puncture with Non-Destructive Examination techniques were also reviewed.

  9. Atmospheric Radiation Measurement (ARM) Data from Shouxian, China for the Study of Aerosol Indirect Effects in China

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    In a complex ARM Mobile Facility (AMF) deployment, monitoring data was collected at four locations in China during 2008. The various sites are located in regions with different climate regimes and with high aerosol loadings of different optical, physical, and chemical properties. Measurements obtained at all the AMF sites during the 8-month deployment in China will help scientists to validate satellite-based findings, understand the mechanisms of the aerosol indirect effects in the region, and examine the roles of aerosols in affecting regional climate and atmospheric circulation, with a special focus on the impact of the East Asian monsoon system. As with other collections from the ARM Mobile Facility, the datasets are available from the ARM Archive. The ARM Archive physically resides at the Oak Ridge National Laboratory.

  10. Bio-butanol: Combustion properties and detailed chemical kinetic model

    SciTech Connect (OSTI)

    Black, G.; Curran, H.J.; Pichon, S.; Simmie, J.M.; Zhukov, V.

    2010-02-15

    Autoignition delay time measurements were performed at equivalence ratios of 0.5, 1 and 2 for butan-1-ol at reflected shock pressures of 1, 2.6 and 8 atm at temperatures from 1100 to 1800 K. High-level ab initio calculations were used to determine enthalpies of formation and consequently bond dissociation energies for each bond in the alcohol. A detailed chemical kinetic model consisting of 1399 reactions involving 234 species was constructed and tested against the delay times and also against recent jet-stirred reactor speciation data with encouraging results. The importance of enol chemistry is highlighted. (author)

  11. Apparatus for sampling and characterizing aerosols

    DOE Patents [OSTI]

    Dunn, Patrick F. (Downers Grove, IL); Herceg, Joseph E. (Naperville, IL); Klocksieben, Robert H. (Park Forest, IL)

    1986-01-01

    Apparatus for sampling and characterizing aerosols having a wide particle size range at relatively low velocities may comprise a chamber having an inlet and an outlet, the chamber including: a plurality of vertically stacked, successive particle collection stages; each collection stage includes a separator plate and a channel guide mounted transverse to the separator plate, defining a labyrinthine flow path across the collection stage. An opening in each separator plate provides a path for the aerosols from one collection stage to the next. Mounted within each collection stage are one or more particle collection frames.

  12. Aerodynamic Focusing Of High-Density Aerosols

    SciTech Connect (OSTI)

    Ruiz, D. E.; Fisch, Nathaniel

    2014-02-24

    High-density micron-sized particle aerosols might form the basis for a number of applications in which a material target with a particular shape might be quickly ionized to form a cylindrical or sheet shaped plasma. A simple experimental device was built in order to study the properties of high-density aerosol focusing for 1#22; m silica spheres. Preliminary results recover previous findings on aerodynamic focusing at low densities. At higher densities, it is demonstrated that the focusing properties change in a way which is consistent with a density dependent Stokes number.

  13. ARM - PI Product - Niamey Aerosol Optical Depths

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Optical Depths ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send PI Product : Niamey Aerosol Optical Depths MFRSR irradiance data collected during the ACRF AMF deployment in Niamey, Niger have been used to derive AOD for five wavelength channels of the MFRSR. These data have been corrected to adjust for filter drift over the course of the campaign and contamination due to forward scattering as a result of

  14. Chemical sensors

    DOE Patents [OSTI]

    Lowell, J.R. Jr.; Edlund, D.J.; Friesen, D.T.; Rayfield, G.W.

    1992-06-09

    Sensors responsive to small changes in the concentration of chemical species are disclosed, comprising a mechanicochemically responsive polymeric film capable of expansion or contraction in response to a change in its chemical environment, either operatively coupled to a transducer capable of directly converting the expansion or contraction to a measurable electrical or optical response, or adhered to a second inert polymeric strip, or doped with a conductive material. 12 figs.

  15. Two Hundred Fifty Years of Aerosols and Climate: The End of the Age of Aerosols

    SciTech Connect (OSTI)

    Smith, Steven J.; Bond, Tami C.

    2014-01-20

    Carbonaceous and sulfur aerosols have a substantial global and regional influence on climate in addition to their impact on health and ecosystems. The magnitude of this influence has changed substantially over the past and is expected to continue to change into the future. An integrated picture of the changing climatic influence of black carbon, organic carbon and sulfate over the period 1850 through 2100, focusing on uncertainty, is presented using updated historical inventories and a coordinated set of emission projections. While aerosols have had a substantial impact on climate over the past century, by the end of the 21st century aerosols will likely be only a minor contributor to radiative forcing due to increases in greenhouse gas forcing and a global decrease in pollutant emissions. This outcome is even more certain under a successful implementation of a policy to limit greenhouse gas emissions as low-carbon energy technologies that do not emit appreciable aerosol or SO2 are deployed.

  16. Near real time vapor detection and enhancement using aerosol adsorption

    DOE Patents [OSTI]

    Novick, V.J.; Johnson, S.A.

    1999-08-03

    A vapor sample detection method is described where the vapor sample contains vapor and ambient air and surrounding natural background particles. The vapor sample detection method includes the steps of generating a supply of aerosol that have a particular effective median particle size, mixing the aerosol with the vapor sample forming aerosol and adsorbed vapor suspended in an air stream, impacting the suspended aerosol and adsorbed vapor upon a reflecting element, alternatively directing infrared light to the impacted aerosol and adsorbed vapor, detecting and analyzing the alternatively directed infrared light in essentially real time using a spectrometer and a microcomputer and identifying the vapor sample. 13 figs.

  17. Near real time vapor detection and enhancement using aerosol adsorption

    DOE Patents [OSTI]

    Novick, Vincent J. (Downers Grove, IL); Johnson, Stanley A. (Countryside, IL)

    1999-01-01

    A vapor sample detection method where the vapor sample contains vapor and ambient air and surrounding natural background particles. The vapor sample detection method includes the steps of generating a supply of aerosol that have a particular effective median particle size, mixing the aerosol with the vapor sample forming aerosol and adsorbed vapor suspended in an air stream, impacting the suspended aerosol and adsorbed vapor upon a reflecting element, alternatively directing infrared light to the impacted aerosol and adsorbed vapor, detecting and analyzing the alternatively directed infrared light in essentially real time using a spectrometer and a microcomputer and identifying the vapor sample.

  18. Raman Lidar Measurements of Aerosols and Water Vapor During the May 2003 Aerosol IOP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Raman Lidar Measurements of Aerosols and Water Vapor During the May 2003 Aerosol IOP R. A. Ferrare National Aeronautics and Space Administration Langley Research Center Hampton, Virginia D. D. Turner Pacific Northwest National Laboratory Richland, Washington M. Clayton Science Applications International Corporation National Aeronautics and Space Administration Langley Research Center Hampton, Virginia B. S. Schmid and J. Redemann BAER/NASA Ames Research Institute Moffett Field, California D.

  19. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    SciTech Connect (OSTI)

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  20. Indirect and Semi-Direct Aerosol Campaign: The Impact of Arctic Aerosols on Clouds

    SciTech Connect (OSTI)

    McFarquhar, Greg; Ghan, Steven J.; Verlinde, J.; Korolev, Alexei; Strapp, J. Walter; Schmid, Beat; Tomlinson, Jason M.; Wolde, Mengistu; Brooks, Sarah D.; Cziczo, Daniel J.; Dubey, Manvendra K.; Fan, Jiwen; Flynn, Connor J.; Gultepe, Ismail; Hubbe, John M.; Gilles, Mary K.; Laskin, Alexander; Lawson, Paul; Leaitch, W. R.; Liu, Peter S.; Liu, Xiaohong; Lubin, Dan; Mazzoleni, Claudio; Macdonald, A. M.; Moffet, Ryan C.; Morrison, H.; Ovchinnikov, Mikhail; Shupe, Matthew D.; Turner, David D.; Xie, Shaocheng; Zelenyuk, Alla; Bae, Kenny; Freer, Matthew; Glen, Andrew

    2011-02-01

    A comprehensive dataset of microphysical and radiative properties of aerosols and clouds in the arctic boundary layer in the vicinity of Barrow, Alaska was collected in April 2008 during the Indirect and Semi-Direct Aerosol Campaign (ISDAC) sponsored by the Department of Energy Atmospheric Radiation Measurement (ARM) and Atmospheric Science Programs. The primary aim of ISDAC was to examine indirect effects of aerosols on clouds that contain both liquid and ice water. The experiment utilized the ARM permanent observational facilities at the North Slope of Alaska (NSA) in Barrow. These include a cloud radar, a polarized micropulse lidar, and an atmospheric emitted radiance interferometer as well as instruments specially deployed for ISDAC measuring aerosol, ice fog, precipitation and spectral shortwave radiation. The National Research Council of Canada Convair-580 flew 27 sorties during ISDAC, collecting data using an unprecedented 42 cloud and aerosol instruments for more than 100 hours on 12 different days. Data were obtained above, below and within single-layer stratus on 8 April and 26 April 2008. These data enable a process-oriented understanding of how aerosols affect the microphysical and radiative properties of arctic clouds influenced by different surface conditions. Observations acquired on a heavily polluted day, 19 April 2008, are enhancing this understanding. Data acquired in cirrus on transit flights between Fairbanks and Barrow are improving our understanding of the performance of cloud probes in ice. Ultimately the ISDAC data will be used to improve the representation of cloud and aerosol processes in models covering a variety of spatial and temporal scales, and to determine the extent to which long-term surface-based measurements can provide retrievals of aerosols, clouds, precipitation and radiative heating in the Arctic.

  1. Incorporating an advanced aerosol activation parameterization into WRF-CAM5: Model evaluation and parameterization intercomparison

    SciTech Connect (OSTI)

    Zhang, Yang; Zhang, Xin; Wang, Kai; He, Jian; Leung, Lai-Yung R.; Fan, Jiwen; Nenes, Athanasios

    2015-07-22

    Aerosol activation into cloud droplets is an important process that governs aerosol indirect effects. The advanced treatment of aerosol activation by Fountoukis and Nenes (2005) and its recent updates, collectively called the FN series, have been incorporated into a newly developed regional coupled climate-air quality model based on the Weather Research and Forecasting model with the physics package of the Community Atmosphere Model version 5 (WRF-CAM5) to simulate aerosol-cloud interactions in both resolved and convective clouds. The model is applied to East Asia for two full years of 2005 and 2010. A comprehensive model evaluation is performed for model predictions of meteorological, radiative, and cloud variables, chemical concentrations, and column mass abundances against satellite data and surface observations from air quality monitoring sites across East Asia. The model performs overall well for major meteorological variables including near-surface temperature, specific humidity, wind speed, precipitation, cloud fraction, precipitable water, downward shortwave and longwave radiation, and column mass abundances of CO, SO2, NO2, HCHO, and O3 in terms of both magnitudes and spatial distributions. Larger biases exist in the predictions of surface concentrations of CO and NOx at all sites and SO2, O3, PM2.5, and PM10 concentrations at some sites, aerosol optical depth, cloud condensation nuclei over ocean, cloud droplet number concentration (CDNC), cloud liquid and ice water path, and cloud optical thickness. Compared with the default Abdul-Razzack Ghan (2000) parameterization, simulations with the FN series produce ~107113% higher CDNC, with half of the difference attributable to the higher aerosol activation fraction by the FN series and the remaining half due to feedbacks in subsequent cloud microphysical processes. With the higher CDNC, the FN series are more skillful in simulating cloud water path, cloud optical thickness, downward shortwave radiation, shortwave cloud forcing, and precipitation. The model evaluation identifies several areas of provements including emissions and their vertical allocation as well as model formulations such as aerosol formation, cloud droplet nucleation, and ice nucleation.

  2. Radiological/biological/aerosol removal system

    DOE Patents [OSTI]

    Haslam, Jeffery J

    2015-03-17

    An air filter replacement system for existing buildings, vehicles, arenas, and other enclosed airspaces includes a replacement air filter for replacing a standard air filter. The replacement air filter has dimensions and air flow specifications that allow it to replace the standard air filter. The replacement air filter includes a filter material that removes radiological or biological or aerosol particles.

  3. Chemical Occurrences

    Broader source: Energy.gov [DOE]

    Classification of Chemical Occurrence Reports into the following four classes: Occurrences characterized by serious energy release, injury or exposure requiring medical treatment, or severe environmental damage, Occurrences characterized by minor injury or exposure, or reportable environmental release, Occurrences that were near misses including notable safety violations and Minor occurrences.

  4. Stackable differential mobility analyzer for aerosol measurement

    DOE Patents [OSTI]

    Cheng, Meng-Dawn; Chen, Da-Ren

    2007-05-08

    A multi-stage differential mobility analyzer (MDMA) for aerosol measurements includes a first electrode or grid including at least one inlet or injection slit for receiving an aerosol including charged particles for analysis. A second electrode or grid is spaced apart from the first electrode. The second electrode has at least one sampling outlet disposed at a plurality different distances along its length. A volume between the first and the second electrode or grid between the inlet or injection slit and a distal one of the plurality of sampling outlets forms a classifying region, the first and second electrodes for charging to suitable potentials to create an electric field within the classifying region. At least one inlet or injection slit in the second electrode receives a sheath gas flow into an upstream end of the classifying region, wherein each sampling outlet functions as an independent DMA stage and classifies different size ranges of charged particles based on electric mobility simultaneously.

  5. Aerosol Retrievals from ARM SGP MFRSR Data

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Alexandrov, Mikhail

    2008-01-15

    The Multi-Filter Rotating Shadowband Radiometer (MFRSR) makes precise simultaneous measurements of the solar direct normal and diffuse horizontal irradiances at six wavelengths (nominally 415, 500, 615, 673, 870, and 940 nm) at short intervals (20 sec for ARM instruments) throughout the day. Time series of spectral optical depth are derived from these measurements. Besides water vapor at 940 nm, the other gaseous absorbers within the MFRSR channels are NO2 (at 415, 500, and 615 nm) and ozone (at 500, 615, and 670 nm). Aerosols and Rayleigh scattering contribute atmospheric extinction in all MFRSR channels. Our recently updated MFRSR data analysis algorithm allows us to partition the spectral aerosol optical depth into fine and coarse modes and to retrieve the fine mode effective radius. In this approach we rely on climatological amounts of NO2 from SCIAMACHY satellite retrievals and use daily ozone columns from TOMS.

  6. Multiscale Speciation of U and Pu at Chernobyl, Hanford, Los Alamos,

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    McGuire AFB, Mayak, and Rocky Flats | Stanford Synchrotron Radiation Lightsource Multiscale Speciation of U and Pu at Chernobyl, Hanford, Los Alamos, McGuire AFB, Mayak, and Rocky Flats Friday, June 26, 2015 X-ray fluorescence maps of (clockwise from upper right) Ga, U, Ca, Pu, Ti, and K in a 350 micron PuO2-UO2 composite particle produced by the fire that consumed a nuclear armed BOMARC missile at McGuire AFB in 1960, measured with the two micron focused x-ray beam at SSRL. EST June 2,

  7. Influence of uranyl speciation and iron oxides on uranium biogeochemical redox reactions

    SciTech Connect (OSTI)

    Stewart, B.D.; Amos, R.T.; Nico, P.S.; Fendorf, S.

    2010-03-15

    Uranium is a pollutant of concern to both human and ecosystem health. Uranium's redox state often dictates its partitioning between the aqueous- and solid-phases, and thus controls its dissolved concentration and, coupled with groundwater flow, its migration within the environment. In anaerobic environments, the more oxidized and mobile form of uranium (UO{sub 2}{sup 2+} and associated species) may be reduced, directly or indirectly, by microorganisms to U(IV) with subsequent precipitation of UO{sub 2}. However, various factors within soils and sediments may limit biological reduction of U(VI), inclusive of alterations in U(VI) speciation and competitive electron acceptors. Here we elucidate the impact of U(VI) speciation on the extent and rate of reduction with specific emphasis on speciation changes induced by dissolved Ca, and we examine the impact of Fe(III) (hydr)oxides (ferrihydrite, goethite and hematite) varying in free energies of formation on U reduction. The amount of uranium removed from solution during 100 h of incubation with S. putrefaciens was 77% with no Ca or ferrihydrite present but only 24% (with ferrihydrite) and 14% (no ferrihydrite) were removed for systems with 0.8 mM Ca. Imparting an important criterion on uranium reduction, goethite and hematite decrease the dissolved concentration of calcium through adsorption and thus tend to diminish the effect of calcium on uranium reduction. Dissimilatory reduction of Fe(III) and U(VI) can proceed through different enzyme pathways, even within a single organism, thus providing a potential second means by which Fe(III) bearing minerals may impact U(VI) reduction. We quantify rate coefficients for simultaneous dissimilatory reduction of Fe(III) and U(VI) in systems varying in Ca concentration (0 to 0.8 mM), and using a mathematical construct implemented with the reactive transport code MIN3P, we reveal the predominant influence of uranyl speciation, specifically the formation of uranyl-calcium-carbonato complexes, and ferrihydrite on the rate and extent of uranium reduction in complex geochemical systems.

  8. Total aerosol effect: forcing or radiative flux perturbation?

    SciTech Connect (OSTI)

    Lohmann, Ulrike; Storelvmo, Trude; Jones, Andy; Rotstayn, Leon; Menon, Surabi; Quaas, Johannes; Ekman, Annica; Koch, Dorothy; Ruedy, Reto

    2009-09-25

    Uncertainties in aerosol forcings, especially those associated with clouds, contribute to a large extent to uncertainties in the total anthropogenic forcing. The interaction of aerosols with clouds and radiation introduces feedbacks which can affect the rate of rain formation. Traditionally these feedbacks were not included in estimates of total aerosol forcing. Here we argue that they should be included because these feedbacks act quickly compared with the time scale of global warming. We show that for different forcing agents (aerosols and greenhouse gases) the radiative forcings as traditionally defined agree rather well with estimates from a method, here referred to as radiative flux perturbations (RFP), that takes these fast feedbacks and interactions into account. Thus we propose replacing the direct and indirect aerosol forcing in the IPCC forcing chart with RFP estimates. This implies that it is better to evaluate the total anthropogenic aerosol effect as a whole.

  9. Climate Engineering with Stratospheric Aerosols and Associated Engineering Parameters

    SciTech Connect (OSTI)

    Kravitz, Benjamin S.

    2013-02-12

    Climate engineering with stratospheric aerosols, an idea inspired by large volcaniceruptions, could cool the Earths surface and thus alleviate some of the predicted dangerous impacts of anthropogenic climate change. However, the effectiveness of climate engineering to achieve a particular climate goal, and any associated side effects, depend on certain aerosol parameters and how the aerosols are deployed in the stratosphere. Through the examples of sulfate and black carbon aerosols, this paper examines "engineering" parameters-aerosol composition, aerosol size, and spatial and temporal variations in deployment-for stratospheric climate engineering. The effects of climate engineering are sensitive to these parameters, suggesting that a particle could be found ordesigned to achieve specific desired climate outcomes. This prospect opens the possibility for discussion of societal goals for climate engineering.

  10. Indirect and Semi-Direct Aerosol Campaign

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Campaign For the month of April, researchers are descending on and above Barrow, Alaska, to obtain data from the atmosphere that will help them understand the impacts that aerosols have on Arctic clouds and climate. Scientists sponsored by the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility are using a heavily instrumented aircraft to collect data from the sky, while instruments based at surface sites in Barrow and Atqasuk, Alaska, are obtaining

  11. Indirect and Semi-Direct Aerosol Campaign

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Campaign (ISDAC) The Influence of Arctic Aerosol on Clouds PIs: Steve Ghan, Greg McFarquhar, Hans Verlinde ARM AVP: Beat Schmid, Greg McFarquhar, John Hubbe, Debbie Ronfeld In situ measurements: Sarah Brooks, Don Collins, Dan Cziczo, Manvendra Dubey, Greg Kok, Alexei Korolev, Alex Laskin, Paul Lawson, Peter Liu, Claudio Mazzoleni, Ann-Marie McDonald, Greg McFarquhar, Walter Strapp, Alla Zelenyuk Retrievals: Connor Flynn, Dan Lubin, Mengistu Wolde, David Mitchell, Matthew Shupe, David Turner

  12. Chemical Sciences

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Chemical Sciences - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Fuel Cycle Defense Waste Management Programs Advanced

  13. Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J.-F.; Yu, P.

    2015-12-08

    Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but it can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR (National Center for Atmospheric Research) Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product volatility basis set (VBS) scheme, including NOx-dependent SOA yields and aging parameterizations. Small differences are found for themore » no-aging VBS and 2-product schemes; large increases in SOA production and the SOA-to-OA ratio are found for the aging scheme. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of 2 compared to aerosol mass spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different regions and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9–5.6, 6.4–12.0 and 0.9–2.8 % for global, southeast US and Amazon NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.« less

  14. Liquid-liquid phase separation in aerosol particles: Imaging at the Nanometer Scale

    SciTech Connect (OSTI)

    O'Brien, Rachel; Wang, Bingbing; Kelly, Stephen T.; Lundt, Nils; You, Yuan; Bertram, Allan K.; Leone, Stephen R.; Laskin, Alexander; Gilles, Mary K.

    2015-04-21

    Atmospheric aerosols can undergo phase transitions including liquid-liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission x-ray microscopy (STXM) to investigate the LLPS of micron sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), a, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS with apparent core-shell particle morphology were observed for all samples with both techniques. Chemical imaging with STXM showed that both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RHs above the deliquescence point and that the majority of the organic component was located in the shell. The shell composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89-92% RH with an estimated 50:50% organic to inorganic mix in the shell. These two chemical imaging techniques are well suited for in-situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.

  15. A New Assessment of the Aerosol First Indirect Effect

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    New Assessment of the Aerosol First Indirect Effect Shao, Hongfei Florida State University Liu, Guosheng Florida State University Category: Aerosols The aerosol first indirect effect is known to cool the Earth radiatively. However, its magnitude is very uncertain; large discrepancies exist among the observed values published in the literature. In this study, we first survey the published values of those parameters used for describing the first indirect effect. By analyzing the discrepancies

  16. Aerosol Simulations by LLNL IMPACT and Comparisons with Field Measurements

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Simulations by LLNL IMPACT and Comparisons with Field Measurements C. C. Chuang, D. Bergman, J. Dignon, and P. Connell Lawrence Livermore National Laboratory Livermore, California Introduction The first step needed to assess aerosol climate effects is to provide the global concentrations and vertical profiles of different aerosol components. These distributions cannot be easily obtained from satellite retrievals or field measurements but are key to estimating the magnitude of aerosol forcing. A

  17. Discrimination between thin cirrus and and tropospheric aerosol using

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    multiple measurements from Darwin ARCS Discrimination between thin cirrus and and tropospheric aerosol using multiple measurements from Darwin ARCS Mitchell, Ross CSIRO Category: Aerosols Thin cirrus cloud occurs frequently in the tropics, and is often difficult to distinguish from tropospheric aerosol on the basis of temporal variations in ground based measurements, since both can be rather spatially uniform. In this study we investigate their discrimination by combining data from three

  18. Importance of Iron Mineralogy to Aerosol Solubility: Potential Effects of

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Aerosol Source on Ocean Photosynthesis Importance of Iron Mineralogy to Aerosol Solubility: Potential Effects of Aerosol Source on Ocean Photosynthesis figure 1 Figure 1. Dust storm blowing glacial dusts from the Copper River Basin of southeast Alaska into the North Pacific Ocean, which depends on this and other external iron sources to support its biological communities. (Image: NASA MODIS satellite image, Nov. 1, 2006. http://earthobservatory.nasa.gov/IOTD/view.php?id=7094) Iron is one of

  19. Toward a Minimal Representation of Aerosols in Climate Models: Description

    Office of Scientific and Technical Information (OSTI)

    and Evaluation in the Community Atmosphere Model CAM5 (Journal Article) | SciTech Connect Toward a Minimal Representation of Aerosols in Climate Models: Description and Evaluation in the Community Atmosphere Model CAM5 Citation Details In-Document Search Title: Toward a Minimal Representation of Aerosols in Climate Models: Description and Evaluation in the Community Atmosphere Model CAM5 A modal aerosol module (MAM) has been developed for the Community Atmosphere Model version 5 (CAM5), the

  20. Building America Webinar: Sealing of Home Enclosures with Aerosol Particles

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    | Department of Energy Sealing of Home Enclosures with Aerosol Particles Building America Webinar: Sealing of Home Enclosures with Aerosol Particles This webinar was presented by research team Building Industry Research Alliance (BIRA), and provided information about a project that uses existing aerosol duct sealing technology to seal the entire building enclosure in order to achieve greater airtightness and energy and cost savings. File webinar_bira_20111014.wmv More Documents &

  1. Laboratory Experiments and Instrument Development for the Study of Atmospheric Aerosols

    SciTech Connect (OSTI)

    Davidovits, Paul

    2011-12-10

    Soot particles are generated by incomplete combustion of fossil and biomass fuels. Through direct effects clear air aerosols containing black carbon (BC) such as soot aerosols, absorb incoming light heating the atmosphere, while most other aerosols scatter light and produce cooling. Even though BC represents only 1-2% of the total annual emissions of particulate mass to the atmosphere, it has been estimated that the direct radiative effect of BC is the second-most important contributor to global warming after absorption by CO2. Ongoing studies continue to underscore the climate forcing importance of black carbon. However, estimates of the radiative effects of black carbon on climate remain highly uncertain due to the complexity of particles containing black carbon. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. Freshly emitted soot particles are typically fractal hydrophobic aggregates. The aggregates consist of black carbon spherules with diameters typically in the range of about 15-40 nm, and they are usually coated by adsorbed polyaromatic hydrocarbons (PAHs) produced during combustion. Diesel-generated soot particles are often emitted with an organic coating composed primarily of lubricating oil and unburned fuel, as well as well as PAH compounds. Sulfuric acid has also been detected in diesel and aircraft-emitted soot particles. In the course of aging, these particle coatings may be substantially altered by chemical reactions and/or the deposition of other materials. Such processes transform the optical and CCN properties of the soot aerosols in ways that are not yet well understood. Our work over the past seven years consisted of laboratory research, instrument development and characterization, and field studies with the central focus of improving our understanding of the black carbon aerosol climate impacts. During the sixth year as well as during this seventh year (no-cost extension period) of our grant, we extended our studies to perform experiments on the controlled production and characterization of secondary organic aerosol.

  2. Nuclear Emergency and the Atmospheric Dispersion of Nuclear Aerosols: Discussion of the Shared Nuclear Future - 13163

    SciTech Connect (OSTI)

    Rana, Mukhtar A.; Ali, Nawab; Akhter, Parveen; Khan, E.U.; Mathieson, John

    2013-07-01

    This paper has a twofold objective. One is to analyze the current status of high-level nuclear waste disposal along with presentation of practical perspectives about the environmental issues involved. Present disposal designs and concepts are analyzed on a scientific basis and modifications to existing designs are proposed from the perspective of environmental safety. Other is to understand the aerosol formation in the atmosphere for the case of the leakage from the nuclear waste containers or a nuclear accident. Radio-nuclides released from the waste will attach themselves to the existing aerosols in the atmosphere along with formation of new aerosols. Anticipating the nuclear accident when a variety of radioactive aerosols will form and exist in the atmosphere, as a simple example, measurement of naturally existing radioactive aerosols are made in the atmosphere of Islamabad and Murree. A comparison with similar measurements in 3 cities of France is provided. Measurement of radionuclides in the atmosphere, their attachment to aerosols and follow up transport mechanisms are key issues in the nuclear safety. It is studied here how {sup 7}Be concentration in the atmospheric air varies in the capital city of Islamabad and a Himalaya foothill city of Murree (Pakistan). Present results are compared with recent related published results to produce a {sup 7}Be concentration versus altitude plot up to an altitude of 4000 m (a.s.l.). Origin and variance of {sup 7}Be concentration at different altitudes is discussed in detail. The relevance of results presented here with the evaluation of implications of Chernobyl and Fukushima nuclear disasters has been discussed in a conclusive manner. It is the first international report of a joint collaboration/project. The project is being generalized to investigate and formulate a smooth waste storage and disposal policy. The project will address the fission and fusion waste reduction, its storage, its recycling, air, water and soil quality monitoring, and the final disposal with the major foci of dealing with related chemical, biogical, physical, geophysical, engineering, management and administration aspects. (authors)

  3. Quantifying Aerosol Direct Effects from Broadband Irradiance and Spectral Aerosol Optical Depth Observations

    SciTech Connect (OSTI)

    Creekmore, Torreon N.; Joseph, Everette; Long, Charles N.; Li, Siwei

    2014-05-16

    We outline a methodology using broadband and spectral irradiances to quantify aerosol direct effects on the surface diffuse shortwave (SW) irradiance. Best Estimate Flux data span a 13 year timeframe at the Department of Energy Atmospheric Radiation Measurement Program’s Southern Great Plains (SGP) site. Screened clear-sky irradiances and aerosol optical depth (AOD), for solar zenith angles ≤ 65°, are used to estimate clear-sky diffuse irradiances. We validate against detected clear-sky observations from SGP’s Basic Radiation System (BRS). BRS diffuse irradiances were in accordance with estimates, producing a root-mean-square error and mean bias errors of 4.0 W/m2 and -1.4 W/m2, respectively. Absolute differences show 99% of estimates within ±10 W/m2 (10%) of the mean BRS observations. Clear-sky diffuse estimates are used to derive quantitative estimates of aerosol radiative effects, represented as the aerosol diffuse irradiance (ADI). ADI is the contribution of diffuse SW to global SW, attributable to scattering of atmospheric transmission by natural plus anthropogenic aerosols. Estimated slope for the ADI as a function of AOD indicates an increase of ~22 W/m2 in diffuse SW for every 0.1 increase in AOD. Such significant increases in the diffuse fraction could possibly increase photosynthesis. Annual mean ADI is 28.2 W/m2, and heavy aerosol loading at SGP provides up to a maximum increase of 120 W/m2 in diffuse SW over background conditions. With regard to seasonal variation, the mean diffuse forcings are 17.2, 33.3, 39.0, and 23.6 W/m2 for winter, spring, summer, and fall, respectively.

  4. Light Absorption of Primary Organic Aerosol Paper Named ACS Editors...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Absorption of Primary Organic Aerosol Paper Named ACS Editors' Choice For original submission and image(s), see ARM Research Highlights http:www.arm.govsciencehighlights...

  5. ARM - Field Campaign - Two-Column Aerosol Project (TCAP): Winter...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    on atmospheric particulate matter. The effect of aerosol properties such as size, morphology and composition on cloud droplet formation has been studied theoretically as well as...

  6. ARM - Publications: Science Team Meeting Documents: A decade long aerosol

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    and cloud statistics and aerosol indirect effect at the ARM SGP site A decade long aerosol and cloud statistics and aerosol indirect effect at the ARM SGP site Min, Qilong State University of New York at Albany Duan, Minzheng State University of New York at Albany Harrison, Lee State University of New York Joseph, Everette Howard University Twelve-year data of MFRSR and MWR have been used to derive aerosol and cloud optical properties at the ARM SGP. Diurnal, monthly, seasonal and

  7. Building America Webinar: Sealing of Home Enclosures with Aerosol...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Sealing of Home Enclosures with Aerosol Particles This webinar was presented by research team Building Industry Research Alliance (BIRA), and provided information about a project...

  8. ARM - Field Campaign - Azores: Clouds, Aerosol and Precipitation...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Campaigns Azores: Above-Cloud Radiation Budget near Graciosa Island 2010.04.15, Miller, AMF Azores: Extension to Clouds, Aerosol and Precipitation in the Marine Boundary...

  9. Study of in-duct spray drying using condensation aerosol

    SciTech Connect (OSTI)

    Chen, W.J.R.; Chang, S.M.; Adikesavalu, R. )

    1992-06-01

    Sulfur removal efficiency of in-duct spray drying is limited by sorbent content and surface properties of the sorbent-water aerosol. It was the purpose of this study to improve the sulfur removal efficiency for in-duct spray drying by injecting condensation aerosol instead of conventional dispersion aerosol. The program was composed of three phases. In Phase I, a novel pulsed fluid bed feeder was developed and was used to feed hydrated lime for subsequent experiments. A small condensation aerosol generator was then built, which produces a lime-water condensation aerosol by condensing steam on lime particles. The results show that novel lime-water aerosols less than 10 microns were generated. The central task in Phase II was to simulate experimentally in-duct spray drying using condensation aerosols and compare the results with those using dispersion aerosols reported in the literature. A small entrained-flow reactor was constructed to simulate an in-duct spray dryer. The condensation aerosol was then introduced to the reactor at various approach to saturation temperature, calcium/sulfur stoichiometry and sulfur dioxide concentration for desulfurization study. The results show that we have improved the sulfur removal efficiency for in-duct spray drying to 90 percent or above. Thus we have met and exceeded the stated project goal of 70 percent sulfur removal. A comprehensive computer code was employed to calculate sulfur removal efficiency in Phase III.

  10. ARM - Field Campaign - Carbonaceous Aerosol and Radiative Effects...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    of representative organic aerosols within the boundary layer. By combining a SMPS and a dual column CCN counter, the size-resolved CCN concentrations were measured. This allowed...

  11. Preliminary Results of in-situ Measurements of Aerosol Optical...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    of Aerosol Optical and Water Uptake Properties from the ARM Mobile Facility in Niger Jefferson, Anne NOAA CMDL Ogren, John NOAACMDL Category: Field Campaigns The second...

  12. Clouds, Aerosols and Precipitation in the Marine Boundary Layer...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Framework, extend to investigation of aerosol-cloud interactions in models - Ensemble Kalman Filter (DART) Satellite activities with CAP-MBL Minnis: CAP-MBL subset MBL depth,...

  13. ARM - Field Campaign - Carbonaceous Aerosol and Radiation Effects...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    - Surface Meteorological Sounding Campaign Links ARM Data Discovery Browse Data Related Campaigns Carbonaceous Aerosol and Radiative Effects Study (CARES) 2010.06.02, Zaveri, AAF...

  14. ARM - Field Campaign - Cirrus Clouds and Aerosol Properties Campaign

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsCirrus Clouds and Aerosol Properties Campaign ARM Data Discovery Browse Data Related Campaigns Vaisala Laser Ceilometer CL51 Demonstration 2013.11.14, Winston, SGP...

  15. ARM - Field Campaign - Indirect and Semi-Direct Aerosol Campaign...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsIndirect and Semi-Direct Aerosol Campaign (ISDAC) Campaign Links ISDAC Website ARM Data Discovery Browse Data Related Campaigns Parameterization of Extinction...

  16. Analysis of Aerosol Indirect Effects in California Coastal Stratus...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Andrew Brookhaven National Laboratory Andrews, Betsy NOAACMDL Ogren, John NOAACMDL Turner, David University of Wisconsin-Madison Category: Field Campaigns Impacts of aerosol...

  17. ARM - Field Campaign - Biogenic Aerosols - Effects on Clouds...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    relevant to DOE's goals in understanding the impact of clouds and aerosols on climate change. TWST contributes significantly to the body of data used for extracting cloud...

  18. Toward a Minimal Representation of Aerosols in Climate Models...

    Office of Scientific and Technical Information (OSTI)

    Minimal Representation of Aerosols in Climate Models: Description and Evaluation in the Community Atmosphere Model CAM5 Citation Details In-Document Search Title: Toward a Minimal ...

  19. The Radiative Role of Free Tropospheric Aerosols and Marine Clouds...

    Office of Scientific and Technical Information (OSTI)

    Technical Report: The Radiative Role of Free Tropospheric Aerosols and Marine Clouds over the Central North Atlantic Citation Details In-Document Search Title: The Radiative Role...

  20. ARM AOS Processing Status and Aerosol Intensive Properties VAP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    AOS Processing Status and Aerosol Intensive Properties VAP A. S. Koontz and C. J. Flynn Pacific Northwest National Laboratory Richland, Washington J. A. Ogren, E. Andrews, and P....

  1. ARM - Publications: Science Team Meeting Documents: The SGP Aerosol...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    The SGP Aerosol Best-Estimate Value-Added Procedure and Its Impact on the BBHRP Project Turner, David Pacific Northwest National Laboratory Sivaraman, Chitra Pacific Northwest...

  2. About the Rhythms of Variability of the Submicron Aerosol Characterist...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    of the distribution of the aerosol characteristics were considered. The periodograms (Fourier spectra of the discrete data set) were calculated for all data arrays using...

  3. Speciation model selection by Monte Carlo analysis of optical absorption spectra: Plutonium(IV) nitrate complexes

    SciTech Connect (OSTI)

    Berg, John M.; Veirs, D. Kirk; Vaughn, Randolph B.; Cisneros, Michael R.; Smith, Coleman A.

    2000-06-01

    Standard modeling approaches can produce the most likely values of the formation constants of metal-ligand complexes if a particular set of species containing the metal ion is known or assumed to exist in solution equilibrium with complexing ligands. Identifying the most likely set of species when more than one set is plausible is a more difficult problem to address quantitatively. A Monte Carlo method of data analysis is described that measures the relative abilities of different speciation models to fit optical spectra of open-shell actinide ions. The best model(s) can be identified from among a larger group of models initially judged to be plausible. The method is demonstrated by analyzing the absorption spectra of aqueous Pu(IV) titrated with nitrate ion at constant 2 molal ionic strength in aqueous perchloric acid. The best speciation model supported by the data is shown to include three Pu(IV) species with nitrate coordination numbers 0, 1, and 2. Formation constants are {beta}{sub 1}=3.2{+-}0.5 and {beta}{sub 2}=11.2{+-}1.2, where the uncertainties are 95% confidence limits estimated by propagating raw data uncertainties using Monte Carlo methods. Principal component analysis independently indicates three Pu(IV) complexes in equilibrium. (c) 2000 Society for Applied Spectroscopy.

  4. Chemical Management

    Office of Environmental Management (EM)

    DOE-HDBK-1139/1-2006 May 2006 DOE HANDBOOK CHEMICAL MANAGEMENT (Volume 1 of 3) U.S. Department of Energy AREA SAFT Washington, D.C. 20585 DISTRIBUTION STATEMENT A. Approved for public release; distribution is unlimited. NOT MEASUREMENT SENSITIVE This document has been reproduced from the best available copy. Available to DOE and DOE contractors from ES&H Technical Information Services, U.S. Department of Energy, (800) 473-4375, fax: (301) 903-9823. Available to the public from the U.S.

  5. Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

    SciTech Connect (OSTI)

    McMeeking, Gavin R.; Kreidenweis, Sonia M.; Baker, Stephen; Carrico, Christian M.; Chow, Judith C.; Collett, Jr., Jeffrey L.; Hao, Wei Min; Holden, Amanda S.; Kirchstetter, Thomas W.; Malm, William C.; Moosmuller, Hans; Sullivan, Amy P.; Wold, Cyle E.

    2009-05-15

    We characterized the gas- and speciated aerosol-phase emissions from the open combustion of 33 different plant species during a series of 255 controlled laboratory burns during the Fire Laboratory at Missoula Experiments (FLAME). The plant species we tested were chosen to improve the existing database for U.S. domestic fuels: laboratory-based emission factors have not previously been reported for many commonly-burned species that are frequently consumed by fires near populated regions and protected scenic areas. The plants we tested included the chaparral species chamise, manzanita, and ceanothus, and species common to the southeastern US (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, and wax myrtle). Fire-integrated emission factors for gas-phase CO{sub 2}, CO, CH{sub 4}, C{sub 2-4} hydrocarbons, NH{sub 3}, SO{sub 2}, NO, NO{sub 2}, HNO{sub 3} and particle-phase organic carbon (OC), elemental carbon (EC), SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, Cl{sup -}, Na{sup +}, K{sup +}, and NH{sub 4}{sup +} generally varied with both fuel type and with the fire-integrated modified combustion efficiency (MCE), a measure of the relative importance of flaming- and smoldering-phase combustion to the total emissions during the burn. Chaparral fuels tended to emit less particulate OC per unit mass of dry fuel than did other fuel types, whereas southeastern species had some of the largest observed EF for total fine particulate matter. Our measurements often spanned a larger range of MCE than prior studies, and thus help to improve estimates for individual fuels of the variation of emissions with combustion conditions.

  6. Selenium Accumulation, Distribution, and Speciation in Spineless Prickly Pear Cactus: A Drought- and Salt-Tolerant, Selenium-Enriched Nutraceutical Fruit Crop for Biofortified Foods

    SciTech Connect (OSTI)

    Banuelos, Gary S.; Fakra, Sirine C.; Walse, Spencer S.; Marcus, Matthew A.; Yang, Soo In; Pickering, Ingrid J.; Pilon-Smits, Elizabeth A.H.; Freeman, John L.

    2011-07-01

    The organ-specific accumulation, spatial distribution, and chemical speciation of selenium (Se) were previously unknown for any species of cactus. We investigated Se in Opuntia ficus-indica using inductively coupled plasma mass spectrometry, microfocused x-ray fluorescence elemental and chemical mapping ({micro}XRF), Se K-edge x-ray absorption near-edge structure (XANES) spectroscopy, and liquid chromatography-mass spectrometry (LC-MS). {micro}XRF showed Se concentrated inside small conic, vestigial leaves (cladode tips), the cladode vasculature, and the seed embryos. Se K-edge XANES demonstrated that approximately 96% of total Se in cladode, fruit juice, fruit pulp, and seed is carbon-Se-carbon (C-Se-C). Micro and bulk XANES analysis showed that cladode tips contained both selenate and C-Se-C forms. Inductively coupled plasma mass spectrometry quantification of Se in high-performance liquid chromatography fractions followed by LC-MS structural identification showed selenocystathionine-to-selenomethionine (SeMet) ratios of 75:25, 71:29, and 32:68, respectively in cladode, fruit, and seed. Enzymatic digestions and subsequent analysis confirmed that Se was mainly present in a 'free' nonproteinaceous form inside cladode and fruit, while in the seed, Se was incorporated into proteins associated with lipids. {micro}XRF chemical mapping illuminated the specific location of Se reduction and assimilation from selenate accumulated in the cladode tips into the two LC-MS-identified C-Se-C forms before they were transported into the cladode mesophyll. We conclude that Opuntia is a secondary Se-accumulating plant whose fruit and cladode contain mostly free selenocystathionine and SeMet, while seeds contain mainly SeMet in protein. When eaten, the organic Se forms in Opuntia fruit, cladode, and seed may improve health, increase Se mineral nutrition, and help prevent multiple human cancers.

  7. Chemical Dynamics, Molecular Energetics, and Kinetics at the Synchrotron

    SciTech Connect (OSTI)

    Leone, Stephen R.; Ahmed, Musahid; Wilson, Kevin R.

    2010-03-14

    Scientists at the Chemical Dynamics Beamline of the Advanced Light Source in Berkeley are continuously reinventing synchrotron investigations of physical chemistry and chemical physics with vacuum ultraviolet light. One of the unique aspects of a synchrotron for chemical physics research is the widely tunable vacuum ultraviolet light that permits threshold ionization of large molecules with minimal fragmentation. This provides novel opportunities to assess molecular energetics and reaction mechanisms, even beyond simple gas phase molecules. In this perspective, significant new directions utilizing the capabilities at the Chemical Dynamics Beamline are presented, along with an outlook for future synchrotron and free electron laser science in chemical dynamics. Among the established and emerging fields of investigations are cluster and biological molecule spectroscopy and structure, combustion flame chemistry mechanisms, radical kinetics and product isomer dynamics, aerosol heterogeneous chemistry, planetary and interstellar chemistry, and secondary neutral ion-beam desorption imaging of biological matter and materials chemistry.

  8. Limited effect of anthropogenic nitrogen oxides on Secondary Organic Aerosol formation

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J.-F.; Yu, P.

    2015-08-28

    Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product Volatility Basis Set (VBS) scheme, including NOx-dependent SOA yields and aging parameterizations. The predicted organic aerosol amounts capture both the magnitude and distribution ofmore » US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of two compared to Aerosol Mass Spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different region and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9 to 5.6, 6.4 to 12.0 and 0.9 to 2.8 % for global, the southeast US and the Amazon NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.« less

  9. Characterization of Aerosols Containing Zn, Pb, and Cl from an Industrial Region of Mexico City

    SciTech Connect (OSTI)

    Moffet, Ryan C.; Desyaterik, Yury; Hopkins, Rebecca J.; Tivanski, Alexei V.; Gilles, Marry K.; Wang, Yan A.; Shutthanandan, V.; Molina, Luisa T.; Abraham, Rodrigo G.; Johnson, Kirsten S.; Mugica, Violeta; Molina, Mario J.; Laskin, Alexander; Prather, Kimberly A.

    2008-10-01

    During the March, 2006 MILAGRO campaign, measurements in the Northern Mexico City Metropolitan Area revealed the frequent appearance of particles with a characteristically high content of internally mixed Zn, Pb, Cl, and P. A comprehensive study of the chemical and physical properties of these particles was performed using a complementary combination of aerosol measurement techniques. Individual particles were analyzed using Aerosol Time-of-Flight Mass Spectrometry (ATOFMS) and Computer Controlled Scanning Electron Microscopy/Energy Dispersive X-Ray spectroscopy (CCSEM/EDX). Proton Induced X-Ray Emission (PIXE) analysis of bulk aerosol samples provided time-resolved mass concentrations of individual elements. The PIXE measurements indicated that Zn is more strongly correlated with Cl than with any other element and that Zn concentrations are higher than other non-ferrous transition metals. The Zn- and Pb - containing particles have both spherical and non-spherical morphologies. Many metal rich particles had needle-like structures and were found to be composed of ZnO and/or Zn(NO3)2?6H2O as indicated by scanning transmission x-ray microscopy/near edge X-ray absorption spectroscopy (STXM/NEXAFS). The Zn and Pb rich particles were primarily in the submicron size range and internally mixed with elemental carbon. The unique chemical associations most closely match signatures acquired for garbage incineration. This unique combination of complementary analytical techniques has allowed for a comprehensive evaluation of Zn- and Pb- containing particles in a complex urban environment, highlighting unique characteristics that give powerful insight into their origin.

  10. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2015-01-16

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  11. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2014-07-03

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1–2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products ofmore » both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  12. CARES Helps Explain Secondary Organic Aerosols

    SciTech Connect (OSTI)

    Zaveri, Rahul

    2014-03-28

    What happens when urban man-made pollution mixes with what we think of as pristine forest air? To know more about what this interaction means for the climate, the Carbonaceous Aerosol and Radiative Effects Study, or CARES, field campaign was designed in 2010. The sampling strategy during CARES was coordinated with CalNex 2010, another major field campaign that was planned in California in 2010 by the California Air Resources Board (CARB), the National Oceanic and Atmospheric Administration (NOAA), and the California Energy Commission (CEC). "We found two things. When urban pollution mixes with forest pollutions we get more secondary organic aerosols," said Rahul Zaveri, FCSD scientist and project lead on CARES. "SOAs are thought to be formed primarily from forest emissions but only when they interact with urban emissions. The data is saying that there will be climate cooling over the central California valley because of these interactions." Knowledge gained from detailed analyses of data gathered during the CARES campaign, together with laboratory experiments, is being used to improve existing climate models.

  13. Asthmatic responses to airborne acid aerosols

    SciTech Connect (OSTI)

    Ostro, B.D.; Lipsett, M.J.; Wiener, M.B.; Selner, J.C. )

    1991-06-01

    Controlled exposure studies suggest that asthmatics may be more sensitive to the respiratory effects of acidic aerosols than individuals without asthma. This study investigates whether acidic aerosols and other air pollutants are associated with respiratory symptoms in free-living asthmatics. Daily concentrations of hydrogen ion (H+), nitric acid, fine particulates, sulfates and nitrates were obtained during an intensive air monitoring effort in Denver, Colorado, in the winter of 1987-88. A panel of 207 asthmatics recorded respiratory symptoms, frequency of medication use, and related information in daily diaries. We used a multiple regression time-series model to analyze which air pollutants, if any, were associated with health outcomes reported by study participants. Airborne H+ was found to be significantly associated with several indicators of asthma status, including moderate or severe cough and shortness of breath. Cough was also associated with fine particulates, and shortness of breath with sulfates. Incorporating the participants' time spent outside and exercise intensity into the daily measure of exposure strengthened the association between these pollutants and asthmatic symptoms. Nitric acid and nitrates were not significantly associated with any respiratory symptom analyzed. In this population of asthmatics, several outdoor air pollutants, particularly airborne acidity, were associated with daily respiratory symptoms.

  14. Hyperspectral Aerosol Optical Depths from TCAP Flights

    SciTech Connect (OSTI)

    Shinozuka, Yohei; Johnson, Roy R.; Flynn, Connor J.; Russell, P. B.; Schmid, Beat; Redemann, Jens; Dunagan, Stephen; Kluzek, Celine D.; Hubbe, John M.; Segal-Rosenheimer, Michal; Livingston, J. M.; Eck, T.; Wagener, Richard; Gregory, L.; Chand, Duli; Berg, Larry K.; Rogers, Ray; Ferrare, R. A.; Hair, John; Hostetler, Chris A.; Burton, S. P.

    2013-11-13

    4STAR (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research), the worlds first hyperspectral airborne tracking sunphotometer, acquired aerosol optical depths (AOD) at 1 Hz during all July 2012 flights of the Two Column Aerosol Project (TCAP). Root-mean square differences from AERONET ground-based observations were 0.01 at wavelengths between 500-1020 nm, 0.02 at 380 and 1640 nm and 0.03 at 440 nm in four clear-sky fly-over events, and similar in ground side-by-side comparisons. Changes in the above-aircraft AOD across 3-km-deep spirals were typically consistent with integrals of coincident in situ (on DOE Gulfstream 1 with 4STAR) and lidar (on NASA B200) extinction measurements within 0.01, 0.03, 0.01, 0.02, 0.02, 0.02 at 355, 450, 532, 550, 700, 1064 nm, respectively, despite atmospheric variations and combined measurement uncertainties. Finer vertical differentials of the 4STAR measurements matched the in situ ambient extinction profile within 14% for one homogeneous column. For the AOD observed between 350-1660 nm, excluding strong water vapor and oxygen absorption bands, estimated uncertainties were ~0.01 and dominated by (then) unpredictable throughput changes, up to +/-0.8%, of the fiber optic rotary joint. The favorable intercomparisons herald 4STARs spatially-resolved high-frequency hyperspectral products as a reliable tool for climate studies and satellite validation.

  15. CARES Helps Explain Secondary Organic Aerosols

    ScienceCinema (OSTI)

    Zaveri, Rahul

    2014-06-02

    What happens when urban man-made pollution mixes with what we think of as pristine forest air? To know more about what this interaction means for the climate, the Carbonaceous Aerosol and Radiative Effects Study, or CARES, field campaign was designed in 2010. The sampling strategy during CARES was coordinated with CalNex 2010, another major field campaign that was planned in California in 2010 by the California Air Resources Board (CARB), the National Oceanic and Atmospheric Administration (NOAA), and the California Energy Commission (CEC). "We found two things. When urban pollution mixes with forest pollutions we get more secondary organic aerosols," said Rahul Zaveri, FCSD scientist and project lead on CARES. "SOAs are thought to be formed primarily from forest emissions but only when they interact with urban emissions. The data is saying that there will be climate cooling over the central California valley because of these interactions." Knowledge gained from detailed analyses of data gathered during the CARES campaign, together with laboratory experiments, is being used to improve existing climate models.

  16. Dose rate dependence of the speciation of neptunium in irradiated solutions of nitric acid

    SciTech Connect (OSTI)

    Precek, M.; Paulenova, A.; Mincher, B.J.; Mezyk, S.P.

    2013-07-01

    The effects of radiation on the redox speciation of neptunium are of interest due to their impact on the performance of separation of neptunium from highly radioactive solutions of dissolved used nuclear fuel. In this study, the influence of dose rate change from 0.4 kGy/h to 6 kGy/h was examined during irradiation of solutions of initially hexavalent 2.0-2.5 mM neptunium in nitric acid of two different concentrations (0.5 and 1 M). Results indicate that the immediate radiolytic steady-state concentration of neptunium(V) were depressed and its initial radiolytic yield was up to 2-times lower (in 1 M HNO{sub 3} solutions)during irradiations with the higher dose rate. The finding is explained on the basis of the enhancement of the role of oxidizing radicals during the radiolytic process. (authors)

  17. Modeling of distribution and speciation of plutonium in the Urex extraction system

    SciTech Connect (OSTI)

    Paulenova, A.; Tkac, P.; Vandegrift, G.F.; Krebs, J.F.

    2008-07-01

    The PUREX extraction process is used worldwide to recover uranium and plutonium from dissolved spent nuclear fuel using the tributylphosphate-nitric acid extraction system. In the recent decade, significant research progress was achieved with the aim to modify this system by addition of a salt-free agent to optimize stripping of plutonium from the tributylphosphate (TBP) extraction product (UREX). Experimental results on the extraction of Pu(IV) with and without acetohydroxamic acid in the HNO{sub 3}/TBP (30 vol %) were used for the development of a thermodynamic model of distribution and speciation of Pu(IV) in this separation process. Extraction constants for several sets of nitric acid, nitrate, and acetohydroxamic acid concentrations were used to model the obtained data. The extraction model AMUSE (Argonne Model for Universal Solvent Extraction) was employed in our calculations. (authors)

  18. Speciation of Selenium, Arsenic, and Zinc in Class C Fly Ash

    SciTech Connect (OSTI)

    Luo, Yun; Giammar, Daniel E.; Huhmann, Brittany L.; Catalano, Jeffrey G.

    2011-11-17

    A major environmental concern associated with coal fly ash is the mobilization of trace elements that may contaminate water. To better evaluate proper use of fly ash, determine appropriate disposal methods, and monitor postdisposal conditions, it is important to understand the speciation of trace elements in fly ash and their possible environmental impact. The speciation of selenium, arsenic, and zinc was determined in five representative Class C fly ash samples from combustion of sub-bituminous Powder River Basin coal using synchrotron-based X-ray absorption spectroscopy to provide an improved understanding of the mechanisms of trace element association with the fly ash. Selenium in all fly ash samples occurs predominantly as Se(IV), with the exception of one sample, in which there was a minor amount of Se(0). Se(0) is likely associated with the high content of unburned coal in the sample. Arsenic exists in the fly ash as a single phase most consistent with calcium pyroarsenate. In contrast, zinc occurs as two distinct species in the silicate glass matrix of the fly ash. This work demonstrates that residual carbon in fly ash may reduce potential Se mobility in the environment by retaining it as less soluble elemental Se instead of Se(IV). Further, this work suggests that As and Zn in Class C fly ash will display substantially different release and mobilization behaviors in aquatic environments. While As release will primarily depend upon the dissolution and hydrolysis of calcium pyroarsenate, Zn release will be controlled by the dissolution of alkaline aluminosilicate glass in the ash.

  19. ARM: 10-second Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    2004-10-01

    10-second Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  20. ARM: 2-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    2004-10-01

    2-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  1. ARM: 1-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    2004-10-01

    1-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  2. ARM: 10-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Newsom, Rob; Goldsmith, John

    1998-03-01

    10-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  3. ARM: 10-second Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    10-second Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  4. ARM: 10-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    10-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  5. ARM: 2-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sivaraman, Chitra; Flynn, Connor

    2-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  6. ARM: 1-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    1-minute Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  7. Fire aerosol experiment and comparisons with computer code predictions

    SciTech Connect (OSTI)

    Gregory, W.S.; Nichols, B.D.; White, B.W.; Smith, P.R.; Leslie, I.H.; Corkran, J.R.

    1988-01-01

    Los Alamos National Laboratory, in cooperation with New Mexico State University, has carried on a series of tests to provide experimental data on fire-generated aerosol transport. These data will be used to verify the aerosol transport capabilities of the FIRAC computer code. FIRAC was developed by Los Alamos for the US Nuclear Regulatory Commission. It is intended to be used by safety analysts to evaluate the effects of hypothetical fires on nuclear plants. One of the most significant aspects of this analysis deals with smoke and radioactive material movement throughout the plant. The tests have been carried out using an industrial furnace that can generate gas temperatures to 300/degree/C. To date, we have used quartz aerosol with a median diameter of about 10 ..mu..m as the fire aerosol simulant. We also plan to use fire-generated aerosols of polystyrene and polymethyl methacrylate (PMMA). The test variables include two nominal gas flow rates (150 and 300 ft/sup 3//min) and three nominal gas temperatures (ambient, 150/degree/C, and 300/degree/C). The test results are presented in the form of plots of aerosol deposition vs length of duct. In addition, the mass of aerosol caught in a high-efficiency particulate air (HEPA) filter during the tests is reported. The tests are simulated with the FIRAC code, and the results are compared with the experimental data. 3 refs., 10 figs., 1 tab.

  8. Implementing marine organic aerosols into the GEOS-Chem model

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2015-03-17

    Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Modelmore » predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

  9. The Two-Column Aerosol Project (TCAP) Science Plan

    SciTech Connect (OSTI)

    Berkowitz, CM; Berg, LK; Cziczo, DJ; Flynn, CJ; Kassianov, EI; Fast, JD; Rasch, PJ; Shilling, JE; Zaveri, RA; Zelenyuk, A; Ferrare, RA; Hostetler, CA; Cairns, B; Russell, PB; Ervens, B

    2011-07-27

    The Two-Column Aerosol Project (TCAP) field campaign will provide a detailed set of observations with which to (1) perform radiative and cloud condensation nuclei (CCN) closure studies, (2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing, (3) extend a previously developed technique to investigate aerosol indirect effects, and (4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the Atmospheric Radiation Measurement (ARM) Climate Research Facility will deploy the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) on Cape Cod, Massachusetts, for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation, and cloud characteristics at a location subject to both clear and cloudy conditions, and clean and polluted conditions. These observations will be supplemented by two aircraft intensive observation periods (IOPs), one in the summer and a second in the winter. Each IOP will deploy one, and possibly two, aircraft depending on available resources. The first aircraft will be equipped with a suite of in situ instrumentation to provide measurements of aerosol optical properties, particle composition and direct-beam irradiance. The second aircraft will fly directly over the first and use a multi-wavelength high spectral resolution lidar (HSRL) and scanning polarimeter to provide continuous optical and cloud properties in the column below.

  10. Implementing marine organic aerosols into the GEOS-Chem model

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Gantt, B.; Johnson, M. S.; Crippa, M.; Prévôt, A. S. H.; Meskhidze, N.

    2014-09-09

    Marine organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in goodmore » agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having > 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.« less

  11. GCM parameterization of radiative forcing by Pinatubo aerosols

    SciTech Connect (OSTI)

    Lacis, A.A.; Mishchenko, M.I.

    1996-12-31

    This paper addresses the question of whether the general circulation model (GCM) parameterization of volcanic aerosol forcing can be adequately described in terms of just two physical aerosol parameters: (1) the aerosol column optical thickness and (2) the effective radius of the aerosol size distribution. Data recorded from the eruption of Mt. Pinatubo in the Philippines in June 1991 was analyzed to attempt to answer this question. The spatial distribution of the particle size showed considerable variability and was found to increase steadily following the eruption. The time evolution of the Pinatubo aerosol particle size distribution as derived from satellite data differed significantly, particularly in the early phases of the eruption, from that assumed in the initial GCM simulation of the Pinatubo eruption. A bimodal distribution was used to examine the possibility that the actual size distribution of the volcanic aerosol was multimodal. However, results suggested that in most cases the aerosol size distribution was essentially monomodal in nature. Results from the radiative model used in the calculations are also presented. 11 refs., 6 figs.

  12. Method of Producing Ultra-heavy Homogeneous Aerosol of Sub-micron Particles

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Ernest J. Valeo and Nathaniel J. Fisch | Princeton Plasma Physics Lab Method of Producing Ultra-heavy Homogeneous Aerosol of Sub-micron Particles Ernest J. Valeo and Nathaniel J. Fisch This invention forms a heavy homogeneous aerosol by agitating sub-micron particles throughacoustic forces and then releasing the aerosol into a low-pressure reservoir. Through this method, the aerosol particulates comprise the dominant mass of the aerosol to produce plasma of the requisite homogeneity,

  13. ARM - Field Campaign - Pajarito Aerosol Coupling to Ecosystems PACE

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsPajarito Aerosol Coupling to Ecosystems PACE ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Pajarito Aerosol Coupling to Ecosystems PACE 2011.12.16 - 2012.04.29 Lead Scientist : Manvendra Dubey For data sets, see below. Abstract The primary goal of the Pajarito Aerosol Couplings to Ecosystems (PACE) IOP is to demonstrate routine MAOS field operations and finesse instrumental and operational

  14. ARM - Field Campaign - Shortwave Radiation and Aerosol Intensive

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Observation Periods govCampaignsShortwave Radiation and Aerosol Intensive Observation Periods ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Shortwave Radiation and Aerosol Intensive Observation Periods 1998.08.03 - 1998.08.28 Lead Scientist : Warren Wiscombe For data sets, see below. Summary Wednesday, August 5, 1998: IOP Opening Activities: The IOP updates for the Shortwave/Aerosol/BDRF will be

  15. Evaluation of New and Proposed Organic Aerosol Sources and Mechanisms using the Aerosol Modeling Testbed. MILAGRO, CARES, CalNex, BEACHON, and GVAX

    SciTech Connect (OSTI)

    Hodzic, Alma; Jimenez, Jose L.

    2015-04-09

    This work investigated the formation and evolution of organic aerosols (OA) arising from anthropogenic and biogenic sources in a framework that combined state-of-the-science process and regional modeling, and their evaluation against advanced and emerging field measurements. Although OA are the dominant constituents of submicron particles, our understanding of their atmospheric lifecycle is limited, and current models fail to describe the observed amounts and properties of chemically formed secondary organic aerosols (SOA), leaving large uncertainties on the effects of SOA on climate. Our work has provided novel modeling constraints on sources, formation, aging and removal of SOA by investigating in particular (i) the contribution of trash burning emissions to OA levels in a megacity, (ii) the contribution of glyoxal to SOA formation in aqueous particles in California during CARES/CalNex and over the continental U.S., (iii) SOA formation and regional growth over a pine forest in Colorado and its sensitivity to anthropogenic NOx levels during BEACHON, and the sensitivity of SOA to (iv) the sunlight exposure during its atmospheric lifetime, and to (v) changes in solubility and removal of organic vapors in the urban plume (MILAGRO, Mexico City), and over the continental U.S.. We have also developed a parameterization of water solubility for condensable organic gases produced from major anthropogenic and biogenic precursors based on explicit chemical modeling, and made it available to the wider community. This work used for the first time constraints from the explicit model GECKO-A to improve SOA representation in 3D regional models such as WRF-Chem.

  16. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Young, D. E.; Kim, H.; Parworth, C.; Zhou, S.; Zhang, X.; Cappa, C. D.; Seco, R.; Kim, S.; Zhang, Q.

    2015-12-15

    The San Joaquin Valley (SJV) in California experiences persistent air quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physico-chemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air quality models. moreAerosol Mass Spectrometer (HR-ToF-AMS) and an Ionicon Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 ?g m?3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O / C), hydrogen-to-carbon (H / C), and nitrogen-to-carbon (N / C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA; O / C = 0.09) associated with local traffic, cooking OA (COA; 28 % of total OA; O / C = 0.19) associated with food cooking activities, two biomass burning OAs (BBOA1; 13 % of total OA; O / C = 0.33 and BBOA2; 20 % of total OA; O / C = 0.60) most likely associated with residential space heating from wood combustion, and semi-volatile oxygenated OA (SV-OOA; 16 % of total OA; O / C = 0.63) and low volatility oxygenated OA (LV-OOA; 24 % of total OA; O / C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a~previous wintertime campaign (winter 2010), most notably that PM1 concentrations were nearly three times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 to 12:00 PST. This is an indication that nighttime chemistry might also be higher in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. The greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.less

  17. Aerosol mass spectrometry systems and methods

    DOE Patents [OSTI]

    Fergenson, David P.; Gard, Eric E.

    2013-08-20

    A system according to one embodiment includes a particle accelerator that directs a succession of polydisperse aerosol particles along a predetermined particle path; multiple tracking lasers for generating beams of light across the particle path; an optical detector positioned adjacent the particle path for detecting impingement of the beams of light on individual particles; a desorption laser for generating a beam of desorbing light across the particle path about coaxial with a beam of light produced by one of the tracking lasers; and a controller, responsive to detection of a signal produced by the optical detector, that controls the desorption laser to generate the beam of desorbing light. Additional systems and methods are also disclosed.

  18. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    SciTech Connect (OSTI)

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is anticipated that they will be included in a future public release of WRF-Chem.

  19. A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.; Ferrare, R. A.

    2015-02-24

    A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convectivemore » cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain–Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud–aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the column-integrated BC can be as large as –50% when cloud–aerosol interactions are considered (due largely to wet removal), or as large as +40% for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRF-Chem, and it is anticipated that they will be included in a future public release of WRF-Chem.« less

  20. Techniques and Methods Used to Determine the Aerosol Best Estimate...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    I: Aerosol Optical Properties. J. Geophys. Res., 109, D06208, doi:10.10292003JD004025. Daniel, J. S., and coauthors, 2002: Cloud liquid water and ice measurements from...

  1. Pressure-flow reducer for aerosol focusing devices

    DOE Patents [OSTI]

    Gard, Eric (San Francisco, CA); Riot, Vincent (Oakland, CA); Coffee, Keith (Diablo Grande, CA); Woods, Bruce (Livermore, CA); Tobias, Herbert (Kensington, CA); Birch, Jim (Albany, CA); Weisgraber, Todd (Brentwood, CA)

    2008-04-22

    A pressure-flow reducer, and an aerosol focusing system incorporating such a pressure-flow reducer, for performing high-flow, atmosphere-pressure sampling while delivering a tightly focused particle beam in vacuum via an aerodynamic focusing lens stack. The pressure-flow reducer has an inlet nozzle for adjusting the sampling flow rate, a pressure-flow reduction region with a skimmer and pumping ports for reducing the pressure and flow to enable interfacing with low pressure, low flow aerosol focusing devices, and a relaxation chamber for slowing or stopping aerosol particles. In this manner, the pressure-flow reducer decouples pressure from flow, and enables aerosol sampling at atmospheric pressure and at rates greater than 1 liter per minute.

  2. Overview of the COPS Aerosol and Cloud Microphysics (ACM) Subgroup...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    at the AMF for Jun-Aug 2007 - Multi-wavelength aerosol and water vapor lidar (BERTHA) - Doppler wind lidar * Mainly in vertical-pointing mode * Operated primarily in the daytime,...

  3. Microsoft Word - Aerosol Working Group_Norfolk 2008.doc

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Interactions Under Varying Meteorological Conditions: Southern Great Plains Vs. Pt. Reyes 15:52 0:13 Jefferson AOS mentor report 16:05 0:13 Kassianov Retrieval of Aerosol...

  4. ARM - Field Campaign - ARM Cloud Aerosol Precipitation Experiment...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : ARM Cloud Aerosol Precipitation Experiment (ACAPEX) 2015.01.14 - 2015.02.12 Lead...

  5. ARM - Field Campaign - MArine Stratus Radiation Aerosol and Drizzle...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsMArine Stratus Radiation Aerosol and Drizzle (MASRAD) IOP Campaign Links Science Plan AMF Point Reyes Website AMF Point Reyes Data Plots ARM Data Discovery Browse Data...

  6. ARM - Field Campaign - Aerosol Life Cycle IOP at BNL

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsAerosol Life Cycle IOP at BNL Campaign Links Images Wiki 2011 ASR STM Presentation: Sedlacek 2011 ASR STM Presentation: Springston 2010 ASR Fall Meeting: Sedlacek News,...

  7. ARM - Field Campaign - ARM Cloud Aerosol Precipitation Experiment...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : ARM Cloud Aerosol Precipitation Experiment (ACAPEX): Aerial Observations 2015.01.14...

  8. ARM - Field Campaign - 2007 Cumulus Humilis Aerosol Process Study...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : 2007 Cumulus Humilis Aerosol Process Study (CHAPS) 2007.06.04 - 2007.06.25 Lead...

  9. ARM - Field Campaign - Biogenic Aerosols - Effects on Clouds...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Climate Campaign Links BAECC Website ARM Data Discovery Browse Data Related Campaigns Biogenic Aerosols - Effects on Clouds and Climate: Cloud OD Sensor TWST 2014.06.15, Scott, AMF...

  10. ARM - Field Campaign - Two-Column Aerosol Project (TCAP): Airborne...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    would love to hear from you Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Two-Column Aerosol Project (TCAP): Airborne HSRL and RSP Measurements 2012.07.01 -...

  11. The Atmosphere as a Laboratory: Aerosols, Air Quality, and Climate...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    to 11:00am Science On Saturday MBG Auditorium The Atmosphere as a Laboratory: Aerosols, Air Quality, and Climate Peter DeCarlo, Assistant Professor of Environmental Engineering...

  12. Field Trial of an Aerosol-Based Enclosure Sealing Technology

    SciTech Connect (OSTI)

    Harrington, Curtis; Springer, David

    2015-09-01

    This report presents the results from several demonstrations of a new method for sealing building envelope air leaks using an aerosol sealing process developed by the Western Cooling Efficiency Center at UC Davis. The process involves pressurizing a building while applying an aerosol sealant to the interior. As air escapes through leaks in the building envelope, the aerosol particles are transported to the leaks where they collect and form a seal that blocks the leak. Standard blower door technology is used to facilitate the building pressurization, which allows the installer to track the sealing progress during the installation and automatically verify the final building tightness. Each aerosol envelope sealing installation was performed after drywall was installed and taped, and the process did not appear to interrupt the construction schedule or interfere with other trades working in the homes. The labor needed to physically seal bulk air leaks in typical construction will not be replaced by this technology.

  13. Ganges Valley Aerosol Experiment (GVAX) Final Campaign Report

    SciTech Connect (OSTI)

    Kotamarthi, VR

    2013-12-01

    In general, the Indian Summer Monsoon (ISM) as well as the and the tropical monsoon climate is influenced by a wide range of factors. Under various climate change scenarios, temperatures over land and into the mid troposphere are expected to increase, intensifying the summer pressure gradient differential between land and ocean and thus strengthening the ISM. However, increasing aerosol concentration, air pollution, and deforestation result in changes to surface albedo and insolation, potentially leading to low monsoon rainfall. Clear evidence points to increasing aerosol concentrations over the Indian subcontinent with time, and several hypotheses regarding the effect on monsoons have been offered. The Ganges Valley Aerosol Experiment (GVAX) field study aimed to provide critical data to address these hypotheses and contribute to developing better parameterizations for tropical clouds, convection, and aerosol-cloud interactions. The primary science questions for the mission were as follows:

  14. Aerosol Optical Depth Value-Added Product Report

    SciTech Connect (OSTI)

    Koontz, A; Hodges, G; Barnard, J; Flynn, C; Michalsky, J

    2013-03-17

    This document describes the process applied to retrieve aerosol optical depth (AOD) from multifilter rotating shadowband radiometers (MFRSR) and normal incidence multifilter radiometers (NIMFR) operated at the ARM Climate Research Facility’s ground-based facilities.

  15. Aerosol Radiative Forcing Under Cloudless Conditions.in Winter...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ARF in the shortwave range is determined by the difference between the net fluxes of the solar radiation, calculated with and without the aerosol component of the atmosphere. The...

  16. COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

    SciTech Connect (OSTI)

    Worsnop, Douglas R.

    2014-07-28

    This project funded the participation of scientists from seven research groups, running more than thirty instruments, in the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London. The primary science questions for the ClearfLo Winter IOP were, 1) what is the urban increment of particulate matter (PM) and other pollutants in the greater London area, and, 2) what is the contribution of solid fuel use for home heating to wintertime PM? An additional motivation for the Detling measurements was the question of whether coatings on black carbon particles enhance absorption. The following four key accomplishments have been identified so far: 1) Chemical, physical and optical characterization of PM from local and regional sources (Figures 2, 4, 5 and 6). 2) Measurement of urban increment in particulate matter and gases in London (Figure 3). 3) Measurement of optical properties and chemical composition of coatings on black carbon containing particles indicates absorption enhancement. 4) First deployment of chemical ionization instrument (MOVI-CI-TOFMS) to measure both particle-phase and gas-phase organic acids. (See final report from Joel Thornton, University of Washington, for details.) Analysis of the large dataset acquired in Detling is ongoing and will yield further key accomplishments. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal. The measurement of absorption enhancement by coatings on black carbon will contribute to improved modeling of the direct radiative properties of PM.

  17. Determination of vertical profiles of aerosol extinction, single scatter

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    albedo and asymmetry parameter at Barrow. Determination of vertical profiles of aerosol extinction, single scatter albedo and asymmetry parameter at Barrow. Sivaraman, Chitra Pacific Northwest National Laboratory Flynn, Connor Pacific Northwest National Laboratory Turner, David University of Wisconsin-Madison Category: Aerosols Efforts are currently underway to run and evaluate the Broadband Heating Rate Profile project at the ARM North Slope of Alaska (NSA) Barrow site for the time period

  18. Direct Aerosol Forcing in the Infrared at the SGP Site?

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Direct Aerosol Forcing in the Infrared at the SGP Site? D. D. Turner and C. N. Long Pacific Northwest National Laboratory Richland, Washington Introduction Low level haze is often observed during the night and early morning hours in many locations. This haze is typically formed during quiescent conditions by radiative cooling of the surface, which lowers the ambient temperature and consequently increases the near-surface relative humidity (RH). Many aerosols start to deliquesce around 75%

  19. Organic Aerosol Component (OACOMP) Value-Added Product Report

    SciTech Connect (OSTI)

    Fast, J; Zhang, Q; Tilp, A; Shippert, T; Parworth, C; Mei, F

    2013-08-23

    Significantly improved returns in their aerosol chemistry data can be achieved via the development of a value-added product (VAP) of deriving OA components, called Organic Aerosol Components (OACOMP). OACOMP is primarily based on multivariate analysis of the measured organic mass spectral matrix. The key outputs of OACOMP are the concentration time series and the mass spectra of OA factors that are associated with distinct sources, formation and evolution processes, and physicochemical properties.

  20. Lead Speciation in House Dust from Canadian Urban Homes Using EXAFS Micro-XRF and Micro-XRD

    SciTech Connect (OSTI)

    L MacLean; S Beauchemin; P Rasmussen

    2011-12-31

    X-ray absorption fine-structure (XAFS) spectroscopy, micro-X-ray fluorescence ({mu}XRF), and micro-X-ray diffraction ({mu}XRD) were used to determine the speciation of Pb in house dust samples from four Canadian urban homes having elevated Pb concentrations (>1000 mg Pb kg{sup -1}). Linear combination fitting of the XAFS data, supported by {mu}XRF and {mu}XRD, shows that Pb is complexed in a variety of molecular environments, associated with both the inorganic and organic fractions of the dust samples. The inorganic species of lead identified were as follows: Pb metal, Pb carbonate, Pb hydroxyl carbonate, Pb oxide, and Pb adsorbed to iron oxyhydroxides. Pb carbonate and/or Pb hydroxyl carbonate occurred in all four dust samples and accounted for 28 to 75% of total Pb. Pb citrate and Pb bound to humate were the organic species identified. The results of this study demonstrate the ability of XAFS to identify Pb speciation in house dust and show the potential to identify Pb sources from new homes versus older homes. Understanding Pb speciation and how it influences bioaccessibility is important for human health risk assessment and risk management decisions which aim to improve indoor environmental health.

  1. On modification of global warming by sulfate aerosols

    SciTech Connect (OSTI)

    Mitchell, J.F.B.; Johns, T.C.

    1997-02-01

    There is increasing evidence that the response of climate to increasing greenhouse gases may be modified by accompanying increases in sulfate aerosols. In this study, the patterns of response in the surface climatology of a coupled ocean-atmosphere general circulation model forced by increases in carbon dioxide alone is compared with those obtained by increasing carbon dioxide and aerosol forcing. The simulations are run from early industrial times using the estimated historical forcing and continued to the end of the twenty-first century assuming a nonintervention emissions scenario for greenhouse gases and aerosols. The comparison is made for the period 2030-2050 when the aerosol forcing is a maximum. In winter, the cooling due to aerosols merely tends to reduce the response to carbon dioxide, whereas in summer, it weakens the monsoon circulations and reverses some of the changes in the hydrological cycle on increasing carbon dioxide. This response is in some respects similar to that found in simulations with changed orbital parameters, as between today and the middle Holocene. The hydrological response in the palaeosimulations is supported by palaeoclimatic reconstructions. The results of changes in aerosol concentrations of the magnetic projected in the scenarios would have a major effect on regional climate, especially over Europe and Southeast Asia. 74 refs., 12 figs., 6 tabs.

  2. Thermodynamic Characterization of Mexico City Aerosol during MILAGRO 2006

    SciTech Connect (OSTI)

    Fountoukis, C.; Nenes, A.; Sullivan, A.; Weber, R.; VanReken, T.; Fischer, M.; Matias, E.; Moya, M.; Farmer, D.; Cohen, R.C.

    2008-12-05

    Fast measurements of aerosol and gas-phase constituents coupled with the ISORROPIA-II thermodynamic equilibrium model are used to study the partitioning of semivolatile inorganic species and phase state of Mexico City aerosol sampled at the T1 site during the MILAGRO 2006 campaign. Overall, predicted semivolatile partitioning agrees well with measurements. PM{sub 2.5} is insensitive to changes in ammonia but is to acidic semivolatile species. For particle sizes up to 1 {micro}m diameter, semi-volatile partitioning requires 30-60 min to equilibrate; longer time is typically required during the night and early morning hours. When the aerosol sulfate-to-nitrate molar ratio is less than unity, predictions improve substantially if the aerosol is assumed to follow the deliquescent phase diagram. Treating crustal species as 'equivalent sodium' (rather than explicitly) in the thermodynamic equilibrium calculations introduces important biases in predicted aerosol water uptake, nitrate and ammonium; neglecting crustals further increases errors dramatically. This suggests that explicitly considering crustals in the thermodynamic calculations is required to accurately predict the partitioning and phase state of aerosols.

  3. Microfluidic chemical reaction circuits

    DOE Patents [OSTI]

    Lee, Chung-cheng (Irvine, CA); Sui, Guodong (Los Angeles, CA); Elizarov, Arkadij (Valley Village, CA); Kolb, Hartmuth C. (Playa del Rey, CA); Huang, Jiang (San Jose, CA); Heath, James R. (South Pasadena, CA); Phelps, Michael E. (Los Angeles, CA); Quake, Stephen R. (Stanford, CA); Tseng, Hsian-rong (Los Angeles, CA); Wyatt, Paul (Tipperary, IE); Daridon, Antoine (Mont-Sur-Rolle, CH)

    2012-06-26

    New microfluidic devices, useful for carrying out chemical reactions, are provided. The devices are adapted for on-chip solvent exchange, chemical processes requiring multiple chemical reactions, and rapid concentration of reagents.

  4. Sandia Energy - Chemical Dynamics

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Chemical Dynamics Home Transportation Energy Predictive Simulation of Engines Combustion Chemistry Chemical Dynamics Chemical DynamicsAshley Otero2015-10-28T02:45:37+00:00...

  5. Coordination chemistry of two heavy metals: I, Ligand preferences in lead(II) complexation, toward the development of therapeutic agents for lead poisoning: II, Plutonium solubility and speciation relevant to the environment

    SciTech Connect (OSTI)

    Neu, M.P.

    1993-11-01

    The coordination chemistry and solution behavior of the toxic ions lead(II) and plutonium(IV, V, VI) have been investigated. The ligand pK{sub a}s and ligand-lead(II) stability constants of one hydroxamic acid and four thiohydroaxamic acids were determined. Solution thermodynamic results indicate that thiohydroxamic acids are more acidic and slightly better lead chelators than hydroxamates, e.g., N-methylthioaceto-hydroxamic acid, pK{sub a} = 5.94, log{beta}{sub 120} = 10.92; acetohydroxamic acid, pK{sub a} = 9.34, log{beta}{sub l20} = 9.52. The syntheses of lead complexes of two bulky hydroxamate ligands are presented. The X-ray crystal structures show the lead hydroxamates are di-bridged dimers with irregular five-coordinate geometry about the metal atom and a stereochemically active lone pair of electrons. Molecular orbital calculations of a lead hydroxamate and a highly symmetric pseudo octahedral lead complex were performed. The thermodynamic stability of plutonium(IV) complexes of the siderophore, desferrioxamine B (DFO), and two octadentate derivatives of DFO were investigated using competition spectrophotometric titrations. The stability constant measured for the plutonium(IV) complex of DFO-methylterephthalamide is log{beta}{sub 110} = 41.7. The solubility limited speciation of {sup 242}Pu as a function of time in near neutral carbonate solution was measured. Individual solutions of plutonium in a single oxidation state were added to individual solutions at pH = 6.0, T = 30.0, 1.93 mM dissolved carbonate, and sampled over intervals up to 150 days. Plutonium solubility was measured, and speciation was investigated using laser photoacoustic spectroscopy and chemical methods.

  6. Development of an aerosol microphysical module: Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS)

    SciTech Connect (OSTI)

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Fast, Jerome D.; Takigawa, M.

    2014-09-30

    Number concentrations, size distributions, and mixing states of aerosols are essential parameters for accurate estimation of aerosol direct and indirect effects. In this study, we developed an aerosol module, designated Aerosol Two-dimensional bin module for foRmation and Aging Simulation (ATRAS), that can represent these parameters explicitly by considering new particle formation (NPF), black carbon (BC) aging, and secondary organic aerosol (SOA) processes. A two-dimensional bin representation is used for particles with dry diameters from 40 nm to 10 m to resolve both aerosol size (12 bins) and BC mixing state (10 bins) for a total of 120 bins. The particles with diameters from 1 to 40 nm are resolved using an additional 8 size bins to calculate NPF. The ATRAS module was implemented in the WRF-chem model and applied to examine the sensitivity of simulated mass, number, size distributions, and optical and radiative parameters of aerosols to NPF, BC aging and SOA processes over East Asia during the spring of 2009. BC absorption enhancement by coating materials was about 50% over East Asia during the spring, and the contribution of SOA processes to the absorption enhancement was estimated to be 10 20% over northern East Asia and 20 35% over southern East Asia. A clear north-south contrast was also found between the impacts of NPF and SOA processes on cloud condensation nuclei (CCN) concentrations: NPF increased CCN concentrations at higher supersaturations (smaller particles) over northern East Asia, whereas SOA increased CCN concentrations at lower supersaturations (larger particles) over southern East Asia. Application of ATRAS to East Asia also showed that the impact of each process on each optical and radiative parameter depended strongly on the process and the parameter in question. The module can be used in the future as a benchmark model to evaluate the accuracy of simpler aerosol models and examine interactions between NPF, BC aging, and SOA processes under different meteorological conditions and emissions.

  7. Solar thermal aerosol flow reaction process

    DOE Patents [OSTI]

    Weimer, Alan W.; Dahl, Jaimee K.; Pitts, J. Roland; Lewandowski, Allan A.; Bingham, Carl; Tamburini, Joseph R.

    2005-03-29

    The present invention provides an environmentally beneficial process using concentrated sunlight to heat radiation absorbing particles to carry out highly endothermic gas phase chemical reactions ultimately resulting in the production of hydrogen or hydrogen synthesis gases.

  8. Chemical Management System

    Energy Science and Technology Software Center (OSTI)

    1998-10-30

    CMS provides an inventory of all chemicals on order or being held in the laboratory, to provide a specific location for all chemical containers, to ensure that health and safety regulatory codes are being upheld, and to provide PNNL staff with hazardous chemical information to better manage their inventories. CMS is comprised of five major modules: 1) chemical purchasing, 2) chemical inventory, 3) chemical names, properties, and hazard groups, 4) reporting, and 5) system administration.

  9. Chemical structure and dynamics. Annual report 1994

    SciTech Connect (OSTI)

    Colson, S.D.

    1995-07-01

    The Chemical Structure and Dynamics program was organized as a major component of Pacific Northwest Laboratory`s Environmental and Molecular Sciences Laboratory (EMSL), a state-of-the-art collaborative facility for studies of chemical structure and dynamics. Our program responds to the need for a fundamental, molecular-level understanding of chemistry at the wide variety of environmentally important interfaces by (1) extending the experimental characterization and theoretical description of chemical reactions to encompass the effects of condensed media and interfaces, and (2) developing a multidisciplinary capability for describing interfacial chemical processes within which the new knowledge generated can be brought to bear on complex phenomena in environmental chemistry and in nuclear waste processing and storage. This research effort was initiated in 1989 and will continue to evolve over the next few years into a program of rigorous studies of fundamental molecular processes in model systems, such as well-characterized surfaces, single-component solutions, clusters, and biological molecules; and studies of complex systems found in the environment (multispecies, multiphase solutions; solid/liquid, liquid/liquid, and gas/surface interfaces; colloidal dispersions; ultrafine aerosols; and functioning biological systems). The success of this program will result in the achievement of a quantitative understanding of chemical reactions at interfaces, and more generally in condensed media, that is comparable to that currently available for gas-phase reactions. This understanding will form the basis for the development of a priori theories for predictions of macroscopic chemical behavior in condensed and heterogeneous media, adding significantly to the value of field-scale environmental models, the prediction of short- and long-term nuclear waste storage stabilities, and other problems related to the primary missions of the DOE.

  10. Chemical Industry Corrosion Management

    SciTech Connect (OSTI)

    2003-02-01

    Improved Corrosion Management Could Provide Significant Cost and Energy Savings for the Chemical Industry. In the chemical industry, corrosion is often responsible for significant shutdown and maintenance costs.

  11. Aerosol specification in single-column CAM5

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lebassi-Habtezion, B.; Caldwell, P.

    2014-11-17

    The ability to run a global climate model in single-column mode is very useful for testing model improvements because single-column models (SCMs) are inexpensive to run and easy to interpret. A major breakthrough in Version 5 of the Community Atmosphere Model (CAM5) is the inclusion of prognostic aerosol. Unfortunately, this improvement was not coordinated with the SCM version of CAM5 and as a result CAM5-SCM initializes aerosols to zero. In this study we explore the impact of running CAM5-SCM with aerosol initialized to zero (hereafter named Default) and test three potential fixes. The first fix is to use CAM5's prescribedmore » aerosol capability, which specifies aerosols at monthly climatological values. The second method is to prescribe aerosols at observed values. The third approach is to fix droplet and ice crystal numbers at prescribed values. We test our fixes in four different cloud regimes to ensure representativeness: subtropical drizzling stratocumulus (based on the DYCOMS RF02 case study), mixed-phase Arctic stratocumulus (using the MPACE-B case study), tropical shallow convection (using the RICO case study), and summertime mid-latitude continental convection (using the ARM95 case study). Stratiform cloud cases (DYCOMS RF02 and MPACE-B) were found to have a strong dependence on aerosol concentration, while convective cases (RICO and ARM95) were relatively insensitive to aerosol specification. This is perhaps expected because convective schemes in CAM5 do not currently use aerosol information. Adequate liquid water content in the MPACE-B case was only maintained when ice crystal number concentration was specified because the Meyers et al. (1992) deposition/condensation ice nucleation scheme used by CAM5 greatly overpredicts ice nucleation rates, causing clouds to rapidly glaciate. Surprisingly, predicted droplet concentrations for the ARM95 region in both SCM and global runs were around 25 cm−3, which is much lower than observed. This finding suggests that CAM5 has problems capturing aerosol effects in this climate regime.« less

  12. ARM - Field Campaign - Two-Column Aerosol Project (TCAP): Ground-Based

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Radiation and Aerosol Validation Using the NOAA Mobile SURFRAD Station govCampaignsTwo-Column Aerosol Project (TCAP): Ground-Based Radiation and Aerosol Validation Using the NOAA Mobile SURFRAD Station ARM Data Discovery Browse Data Related Campaigns Two-Column Aerosol Project (TCAP) 2012.07.01, Berg, AMF Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Two-Column Aerosol Project (TCAP): Ground-Based Radiation and Aerosol Validation

  13. Spent fuel sabotage aerosol test program :FY 2005-06 testing and aerosol data summary.

    SciTech Connect (OSTI)

    Gregson, Michael Warren; Brockmann, John E.; Nolte, O. (Fraunhofer institut fur toxikologie und experimentelle Medizin, Germany); Loiseau, O. (Institut de radioprotection et de Surete Nucleaire, France); Koch, W. (Fraunhofer institut fur toxikologie und experimentelle Medizin, Germany); Molecke, Martin Alan; Autrusson, Bruno (Institut de radioprotection et de Surete Nucleaire, France); Pretzsch, Gunter Guido (Gesellschaft fur anlagen- und Reaktorsicherheit, Germany); Billone, M. C. (Argonne National Laboratory, USA); Lucero, Daniel A.; Burtseva, T. (Argonne National Laboratory, USA); Brucher, W (Gesellschaft fur anlagen- und Reaktorsicherheit, Germany); Steyskal, Michele D.

    2006-10-01

    This multinational, multi-phase spent fuel sabotage test program is quantifying the aerosol particles produced when the products of a high energy density device (HEDD) interact with and explosively particulate test rodlets that contain pellets of either surrogate materials or actual spent fuel. This program has been underway for several years. This program provides source-term data that are relevant to some sabotage scenarios in relation to spent fuel transport and storage casks, and associated risk assessments. This document focuses on an updated description of the test program and test components for all work and plans made, or revised, primarily during FY 2005 and about the first two-thirds of FY 2006. It also serves as a program status report as of the end of May 2006. We provide details on the significant findings on aerosol results and observations from the recently completed Phase 2 surrogate material tests using cerium oxide ceramic pellets in test rodlets plus non-radioactive fission product dopants. Results include: respirable fractions produced; amounts, nuclide content, and produced particle size distributions and morphology; status on determination of the spent fuel ratio, SFR (the ratio of respirable particles from real spent fuel/respirables from surrogate spent fuel, measured under closely matched test conditions, in a contained test chamber); and, measurements of enhanced volatile fission product species sorption onto respirable particles. We discuss progress and results for the first three, recently performed Phase 3 tests using depleted uranium oxide, DUO{sub 2}, test rodlets. We will also review the status of preparations and the final Phase 4 tests in this program, using short rodlets containing actual spent fuel from U.S. PWR reactors, with both high- and lower-burnup fuel. These data plus testing results and design are tailored to support and guide, follow-on computer modeling of aerosol dispersal hazards and radiological consequence assessments. This spent fuel sabotage--aerosol test program, performed primarily at Sandia National Laboratories, with support provided by both the U.S. Department of Energy and the Nuclear Regulatory Commission, had significant inputs from, and is strongly supported and coordinated by both the U.S. and international program participants in Germany, France, and the U.K., as part of the international Working Group for Sabotage Concerns of Transport and Storage Casks, WGSTSC.

  14. Release of aged contaminants from weathered sediments: Effects of sorbate speciation on scaling of reactive transport

    SciTech Connect (OSTI)

    Chorover, Jon; Perdrial, Nico; Mueller, Karl; Strepka, Caleb; O???¢????????Day, Peggy; Rivera, Nelson; Um, Wooyong; Chang, Hyun-Shik; Steefel, Carl; Thompson, Aaron

    2012-11-05

    Hanford sediments impacted by hyperalkaline high level radioactive waste have undergone incongruent silicate mineral weathering concurrent with contaminant uptake. In this project, we studied the impact of background pore water (BPW) on strontium, cesium and iodine desorption and transport in Hanford sediments that were experimentally weathered by contact with simulated hyperalkaline tank waste leachate (STWL) solutions. Using those lab-weathered Hanford sediments (HS) and model precipitates formed during nucleation from homogeneous STWL solutions (HN), we (i) provided thorough characterization of reaction products over a matrix of field-relevant gradients in contaminant concentration, partial pressure of carbon dioxide, and reaction time; (ii) improved molecular-scale understanding of how sorbate speciation controls contaminant desorption from weathered sediments upon removal of caustic sources; and (iii) developed a mechanistic, predictive model of meso- to field-scale contaminant reactive transport under these conditions. In this final report, we provide detailed descriptions of our results from this three-year study, completed in 2012 following a one-year no cost extension.

  15. Concentration Dependent Speciation and Mass Transport Properties of Switchable Polarity Solvents

    SciTech Connect (OSTI)

    Aaron D. Wilson; Christopher J. Orme

    2014-12-01

    Tertiary amine switchable polarity solvents (SPS) consisting of predominantly water, tertiary amine, and tertiary ammonium and bicarbonate ions were produced at various concentrations for three different amines: N,N-dimethylcyclohexylamine, N,N-dimethyloctylamine, and 1 cyclohexylpiperidine. For all concentrations, physical properties were measured including viscosity, molecular diffusion coefficients, freezing point depression, and density. Based on these measurements a variation on the Mark Houwink equation was developed to predict the viscosity of any tertiary amine SPS as a function of concentration using the amines molecular mass. The observed physical properties allowed the identification of solution state speciation of non-osmotic SPS, where the amine to carbonic acid ratio is significantly greater than one. These results indicate that at most concentrations the stoichiometric excess amine is involved in solvating a proton with two amines. The physical properties of osmotic SPS have consistent concentration dependence behavior over a wide range of concentrations; this consistence suggests osmotic pressures based on low concentrations freezing point studies can be reliably extrapolated to higher concentrations.

  16. Relating Pore-Scale Uranium Aquatic Speciation to Intermediate-Scale Aquifer Heterogeneity

    SciTech Connect (OSTI)

    Ranville, James

    2013-04-01

    The speciation and transport of uranium (VI) through porous media is highly dependent on solution conditions, the presence of complexing ligands, and the nature of the porous media. The dependency on many variables makes prediction of U transport in bench-scale experiments and in the field difficult. In particular, the identification of colloidal U phases poses a technical challenge. Transport of U in the presence and absence of natural organic matter (Suwannee River humic acid, SRHA) through silica sand and hematite coated silica sand was tested at pH 4 and 5 using static columns, where flow is controlled by gravity and residence time between advective pore volume exchanges can be strictly controlled. The column effluents were characterized by traditional techniques including ICPMS quantification of total [U] and [Fe], TOC analysis of [DOC], and pH analysis, and also by non-traditional techniques: flow field flow fractionation with online ICPMS detection (FlFFF-ICPMS) and specific UV absorbance (SUVA) characterization of effluent fractions. Key results include that the transport of U through the columns was enhanced by pre-equilibration with SRHA, and previously deposited U was remobilized by the addition of SRHA. The advanced techniques yielded important insights on the mechanisms of transport: FlFFF-ICPMS identified a U?SRHA complex as the mobile U species and directly quantified relative amounts of the complex, while specific UV absorbance (SUVA) measurements indicated a composition-based fractionation onto the porous media.

  17. Selenium And Arsenic Speciation in Fly Ash From Full-Scale Coal-Burning Utility Plants

    SciTech Connect (OSTI)

    Huggins, F.E.; Senior, C.L.; Chu, P.; Ladwig, K.; Huffman, G.P.; /Kentucky U. /Reaction Engin. Int. /Elect. Power Res. Inst., Palo Alto

    2007-07-09

    X-ray absorption fine structure spectroscopy has been used to determine directly the oxidation states and speciation of selenium and arsenic in 10 fly ash samples collected from full-scale utility plants. Such information is needed to assess the health risk posed by these elements in fly ash and to understand their behavior during combustion and in fly ash disposal options, such as sequestration in tailings ponds. Selenium is found predominantly as Se(IV) in selenite (SeO{sub 3}{sup 2-}) species, whereas arsenic is found predominantly as As(V) in arsenate (AsO{sub 4}{sup 3-}) species. Two distinct types of selenite and arsenate spectra were observed depending upon whether the fly ash was derived from eastern U.S. bituminous (Fe-rich) coals or from western subbituminous or lignite (Ca-rich) coals. Similar spectral details were observed for both arsenic and selenium in the two different types of fly ash, suggesting that the post-combustion behavior and capture of both of these elements are likely controlled by the same dominant element or phase in each type of fly ash.

  18. New Technique for Speciation of Uranium in Sediments Following Acetate-Stimulated Bioremediation

    SciTech Connect (OSTI)

    Not Available

    2011-06-22

    Acetate-stimulated bioremediation is a promising new technique for sequestering toxic uranium contamination from groundwater. The speciation of uranium in sediments after such bioremediation attempts remains unknown as a result of low uranium concentration, and is important to analyzing the stability of sequestered uranium. A new technique was developed for investigating the oxidation state and local molecular structure of uranium from field site sediments using X-Ray Absorption Spectroscopy (XAS), and was implemented at the site of a former uranium mill in Rifle, CO. Glass columns filled with bioactive Rifle sediments were deployed in wells in the contaminated Rifle aquifer and amended with a hexavalent uranium (U(VI)) stock solution to increase uranium concentration while maintaining field conditions. This sediment was harvested and XAS was utilized to analyze the oxidation state and local molecular structure of the uranium in sediment samples. Extended X-Ray Absorption Fine Structure (EXAFS) data was collected and compared to known uranium spectra to determine the local molecular structure of the uranium in the sediment. Fitting was used to determine that the field site sediments did not contain uraninite (UO{sub 2}), indicating that models based on bioreduction using pure bacterial cultures are not accurate for bioremediation in the field. Stability tests on the monomeric tetravalent uranium (U(IV)) produced by bioremediation are needed in order to assess the efficacy of acetate-stimulation bioremediation.

  19. Institute of Chemical Engineering and High Temperature Chemical...

    Open Energy Info (EERE)

    Chemical Engineering and High Temperature Chemical Processes ICEHT Jump to: navigation, search Name: Institute of Chemical Engineering and High Temperature Chemical Processes...

  20. ITP Chemicals: Chemical Industry of the Future: New Biocatalysts...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Chemical Industry of the Future: New Biocatalysts: Essential Tools for a Sustainable 21st Century Chemical Industry ITP Chemicals: Chemical Industry of the Future: New...

  1. A Physically Based Framework for Modelling the Organic Fractionation of Sea Spray Aerosol from Bubble Film Langmuir Equilibria

    SciTech Connect (OSTI)

    Burrows, Susannah M.; Ogunro, O.; Frossard, Amanda; Russell, Lynn M.; Rasch, Philip J.; Elliott, S.

    2014-12-19

    The presence of a large fraction of organic matter in primary sea spray aerosol (SSA) can strongly affect its cloud condensation nuclei activity and interactions with marine clouds. Global climate models require new parameterizations of the SSA composition in order to improve the representation of these processes. Existing proposals for such a parameterization use remotely-sensed chlorophyll-a concentrations as a proxy for the biogenic contribution to the aerosol. However, both observations and theoretical considerations suggest that existing relationships with chlorophyll-a, derived from observations at only a few locations, may not be representative for all ocean regions. We introduce a novel framework for parameterizing the fractionation of marine organic matter into SSA based on a competitive Langmuir adsorption equilibrium at bubble surfaces. Marine organic matter is partitioned into classes with differing molecular weights, surface excesses, and Langmuir adsorption parameters. The classes include a lipid-like mixture associated with labile dissolved organic carbon (DOC), a polysaccharide-like mixture associated primarily with semi-labile DOC, a protein-like mixture with concentrations intermediate between lipids and polysaccharides, a processed mixture associated with recalcitrant surface DOC, and a deep abyssal humic-like mixture. Box model calculations have been performed for several cases of organic adsorption to illustrate the underlying concepts. We then apply the framework to output from a global marine biogeochemistry model, by partitioning total dissolved organic carbon into several classes of macromolecule. Each class is represented by model compounds with physical and chemical properties based on existing laboratory data. This allows us to globally map the predicted organic mass fraction of the nascent submicron sea spray aerosol. Predicted relationships between chlorophyll-\\textit{a} and organic fraction are similar to existing empirical parameterizations, but can vary between biologically productive and non-productive regions, and seasonally within a given region. Major uncertainties include the bubble film thickness at bursting and the variability of organic surfactant activity in the ocean, which is poorly constrained. In addition, marine colloids and cooperative adsorption of polysaccharides may make important contributions to the aerosol, but are not included here. This organic fractionation framework is an initial step towards a closer linking of ocean biogeochemistry and aerosol chemical composition in Earth system models. Future work should focus on improving constraints on model parameters through new laboratory experiments or through empirical fitting to observed relationships in the real ocean and atmosphere, as well as on atmospheric implications of the variable composition of organic matter in sea spray.

  2. Sampling microbial aerosols. Summary report, 1 October 1985-30 September 1986

    SciTech Connect (OSTI)

    Chatigny, M.A.

    1986-09-01

    Collecting microbial aerosols is not substantially different from collecting any other airborne particulates. After collection, however, the processing of the sample is all important. These particles have life and the capacity to grow, multiply, and as parasites - cause undesirable effects in the multiplicity of hosts. No chemical or physical measurement(s) available today can assess all these characteristics. Even detection of their presence often requires the bio-amplification provided by the growth characteristics. Both indoor and outdoor air are seas of microbial particles. Depending on local conditions, concentrations of viable particles will range from a few per ft. to many thousands or even millions. Particles are nearly indistinguishable so that detecting a specific viable and infective type is a little like selecting a specific raindrop in a rainstorm. Only by careful choice of growth and assay procedures, can the microbes of interest be selected out of the collectate.

  3. Chemical Management Contacts

    Broader source: Energy.gov [DOE]

    Contacts for additional information on Chemical Management and brief description on Energy Facility Contractors Group

  4. Electrohydrodynamic atomization (EHDA) assisted wet chemical synthesis of nickel nanoparticles

    SciTech Connect (OSTI)

    Barzegar Vishlaghi, M. [Department of Mechanical Engineering, University of Tabriz, Tabriz (Iran, Islamic Republic of)] [Department of Mechanical Engineering, University of Tabriz, Tabriz (Iran, Islamic Republic of); Farzalipour Tabriz, M., E-mail: meisam.fa@gmail.com [Department of Mechanical Engineering, University of Tabriz, Tabriz (Iran, Islamic Republic of); Mohammad Moradi, O. [Department of Mechanical Engineering, University of Tabriz, Tabriz (Iran, Islamic Republic of)] [Department of Mechanical Engineering, University of Tabriz, Tabriz (Iran, Islamic Republic of)

    2012-07-15

    Highlights: ? Electrohydrodynamic atomization (EHDA) assisted chemical synthesis of nickel nanoparticles is reported. ? Substituting water with non-aqueous media prevents the formation of nickel hydroxide. ? Size of particles decreased from 10 to 20 nm down to 24 nm by using multi-jet mode. ? Synthesized nanoparticles have diffraction patterns similar to amorphous materials. -- Abstract: In this study nickel nanoparticles were prepared via chemical reduction of nickel acetate using sodium borohydride using electrohydrodynamic atomization (EHDA) technique. This technique was used to spray a finely dispersed aerosol of nickel precursor solution into the reductive bath. Obtained particles were characterized by means of X-ray diffraction (XRD), UVVisible spectroscopy, and transmission electron microscopy (TEM). Results confirmed the formation of nickel nanoparticles and showed that applying EHDA technique to chemical reduction method results in producing smaller particles with narrower size distribution in comparison with conventional reductive precipitation method.

  5. PINS chemical identification software

    DOE Patents [OSTI]

    Caffrey, Augustine J.; Krebs, Kennth M.

    2004-09-14

    An apparatus and method for identifying a chemical compound. A neutron source delivers neutrons into the chemical compound. The nuclei of chemical elements constituting the chemical compound emit gamma rays upon interaction with the neutrons. The gamma rays are characteristic of the chemical elements constituting the chemical compound. A spectrum of the gamma rays is generated having a detection count and an energy scale. The energy scale is calibrated by comparing peaks in the spectrum to energies of pre-selected chemical elements in the spectrum. A least-squares fit completes the calibration. The chemical elements constituting the chemical compound can be readily determined, which then allows for identification of the chemical compound.

  6. ATMOSPHERIC AEROSOL SOURCE-RECEPTOR RELATIONSHIPS: THE ROLE OF COAL-FIRED POWER PLANTS

    SciTech Connect (OSTI)

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2004-04-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of September 2003 through February 2004. Significant progress was made this project period on the analysis of ambient data, source apportionment, and deterministic modeling activities. Results highlighted in this report include chemical fractionation of the organic fraction to quantify the ratio of organic mass to organic carbon (OM/OC). The average OM/OC ratio for the 31 samples analyzed so far is 1.89, ranging between 1.62 and 2.53, which is consistent with expectations for an atmospherically processed regional aerosol. Analysis of the single particle data reveals that a on a particles in Pittsburgh consist of complex mixture of primary and secondary components. Approximately 79% of all particles measured with the instrument containing some form of carbon, with Carbonaceous Ammonium Nitrate (54.43%) being the dominant particle class. PMCAMx predictions were compared with data from more than 50 sites of the STN network located throughout the Eastern United States for the July 2001 period. OC and sulfate concentrations predicted by PMCAMx are within {+-}30% of the observed concentration at most of these sites. Spherical Aluminum Silicate particle concentrations (SAS) were used to estimate the contribution of primary coal emissions to fine particle levels at the central monitoring site. Primary emissions from coal combustion contribute on average 0.44 {+-} 0.3 {micro}g/m{sup 3} to PM{sub 2.5} at the site or 1.4 {+-} 1.3% of the total PM{sub 2.5} mass. Chemical mass balance analysis was performed to apportion the primary organic aerosol. About 70% of the primary OC emissions are from vehicular sources, with the gasoline contribution being on average three times greater than the diesel emissions in the summer.

  7. Chemicals | Department of Energy

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Chemicals Chemicals The U.S. chemicals industry is maturing and optimizing its business portfolio for more competitive global markets. Over the past decade, the industry has reduced its energy use, shifting its status from the largest to the second-largest energy user among U.S. industries. The chemicals industry has worked in partnership with AMO to develop a range of resources for improving energy efficiency. Some current R&D projects and Energy Management resources will benefit chemicals

  8. Chemical Sector Analysis | NISAC

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    NISACChemical Sector Analysis content top Chemical Supply Chain Analysis Posted by Admin on Mar 1, 2012 in | Comments 0 comments Chemical Supply Chain Analysis NISAC has developed a range of capabilities for analyzing the consequences of disruptions to the chemical manufacturing industry. Each capability provides a different but complementary perspective on the questions of interest-questions like Given an event, will the entire chemical sector be impacted or just parts? Which chemicals, plants,

  9. Indirect aerosol effect increases CMIP5 models projected Arctic warming

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Chylek, Petr; Vogelsang, Timothy J.; Klett, James D.; Hengartner, Nicholas; Higdon, Dave; Lesins, Glen; Dubey, Manvendra K.

    2016-02-20

    Phase 5 of the Coupled Model Intercomparison Project (CMIP5) climate models’ projections of the 2014–2100 Arctic warming under radiative forcing from representative concentration pathway 4.5 (RCP4.5) vary from 0.9° to 6.7°C. Climate models with or without a full indirect aerosol effect are both equally successful in reproducing the observed (1900–2014) Arctic warming and its trends. However, the 2014–2100 Arctic warming and the warming trends projected by models that include a full indirect aerosol effect (denoted here as AA models) are significantly higher (mean projected Arctic warming is about 1.5°C higher) than those projected by models without a full indirect aerosolmore » effect (denoted here as NAA models). The suggestion is that, within models including full indirect aerosol effects, those projecting stronger future changes are not necessarily distinguishable historically because any stronger past warming may have been partially offset by stronger historical aerosol cooling. In conclusion, the CMIP5 models that include a full indirect aerosol effect follow an inverse radiative forcing to equilibrium climate sensitivity relationship, while models without it do not.« less

  10. CARES: Carbonaceous Aerosol and Radiative Effects Study Operations Plan

    SciTech Connect (OSTI)

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-07-12

    The CARES field campaign is motivated by the scientific issues described in the CARES Science Plan. The primary objectives of this field campaign are to investigate the evolution and aging of carbonaceous aerosols and their climate-affecting properties in the urban plume of Sacramento, California, a mid-size, mid-latitude city that is located upwind of a biogenic volatile organic compound (VOC) emission region. Our basic observational strategy is to make comprehensive gas, aerosol, and meteorological measurements upwind, within, and downwind of the urban area with the DOE G-1 aircraft and at strategically located ground sites so as to study the evolution of urban aerosols as they age and mix with biogenic SOA precursors. The NASA B-200 aircraft, equipped with the High Spectral Resolution Lidar (HSRL), digital camera, and the Research Scanning Polarimeter (RSP), will be flown in coordination with the G-1 to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties, and to provide the vertical context for the G-1 and ground in situ measurements.

  11. BAECC Biogenic Aerosols - Effects on Clouds and Climate

    SciTech Connect (OSTI)

    Petäjä, Tuukka; Moisseev, Dmitri; Sinclair, Victoria; O'Connor, Ewan J.; Manninen, Antti J.; Levula, Janne; Väänänen, Riikka; Heikkinen, Liine; Äijälä, Mikko; Aalto, Juho; Bäck, Jaana

    2015-11-01

    “Biogenic Aerosols - Effects on Clouds and Climate (BAECC)”, featured the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program’s 2nd Mobile Facility (AMF2) in Hyytiälä, Finland. It operated for an 8-month intensive measurement campaign from February to September 2014. The main research goal was to understand the role of biogenic aerosols in cloud formation. One of the reasons to perform BAECC study in Hyytiälä was the fact that it hosts SMEAR-II (Station for Measuring Forest Ecosystem-Atmosphere Relations), which is one of the world’s most comprehensive surface in-situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions and an extensive suite of parameters relevant to atmosphere-biosphere interactions continuously since 1996. The BAECC enables combining vertical profiles from AMF2 with surface-based in-situ SMEAR-II observations and allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. With the inclusion of extensive surface precipitation measurements, and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations of AMF2 and SMEAR-II provide a unique opportunity for investigating aerosol-cloud interactions, and cloud-to-precipitation processes. The BAECC dataset will initiate new opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary-layer structures.

  12. Elemental speciation in biomolecules by LC-ICP-MS with magnetic sector and collision cell instruments

    SciTech Connect (OSTI)

    Wang, Jin

    1999-11-08

    A methodology that can monitor and identify inorganic elements in biological and environmental systems was developed. Size exclusion chromatography (SEC) separates biomolecules, which are then nebulized by a microconcentric nebulizer. The resulting aerosol is desolved and introduced into either a high resolution ICP-MS device or a quadrupole device with a collision cell. Because of the high sensitivity and spectral resolution and high sample introduction efficiency, many unusual or difficult elements, such as Cr, Se, Cd and U, can be observed at ambient levels bound to proteins in human serum. These measurements are made in only a few minutes without preliminary isolation and preconcentration steps. Serum samples can be titrated with spikes of various elements to determine which proteins bind a given metal and oxidation state. Experiments concerning the effects of breaking disulfide linkages and denaturation on metal binding in proteins were also investigated. Elemental distribution in liver extract was also obtained.

  13. Correlation between speciated hydrocarbon emissions and flame ionization detector response for gasoline/alcohol blends .

    SciTech Connect (OSTI)

    Wallner, T.

    2011-08-01

    The U.S. renewable fuel standard has made it a requirement to increase the production of ethanol and advanced biofuels to 36 billion by 2022. Ethanol will be capped at 15 billion, which leaves 21 billion to come from other sources such as butanol. Butanol has a higher energy density and lower affinity for water than ethanol. Moreover, alcohol fueled engines in general have been shown to positively affect engine-out emissions of oxides of nitrogen and carbon monoxide compared with their gasoline fueled counterparts. In light of these developments, the variety and blend levels of oxygenated constituents is likely to increase in the foreseeable future. The effect on engine-out emissions for total hydrocarbons is less clear due to the relative insensitivity of the flame ionization detector (FID) toward alcohols and aldehydes. It is well documented that hydrocarbon (HC) measurement using a conventional FID in the presence of oxygenates in the engine exhaust stream can lead to a misinterpretation of HC emissions trends for alcohol fuel blends. Characterization of the exhaust stream for all expected hydrocarbon constituents is required to accurately determine the actual concentration of unburned fuel components in the exhaust. In addition to a conventional exhaust emissions bench, this characterization requires supplementary instrumentation capable of hydrocarbon speciation and response factor independent quantification. Although required for certification testing, this sort of instrumentation is not yet widely available in engine development facilities. Therefore, an attempt is made to empirically determine FID correction factors for oxygenate fuels. Exhaust emissions of an engine fueled with several blends of gasoline and ethanol, n-butanol and iso-Butanol were characterized using both a conventional FID and a Fourier transform infrared. Based on these results, a response factor predicting the actual hydrocarbon emissions based solely on FID results as a function of alcohol type and content is presented. Finally, the correlation derived from data presented in this study is compared with equations and results found in the literature.

  14. Results of Hg speciation testing on tanks 30, 32, and 37 depth samples

    SciTech Connect (OSTI)

    Bannochie, C. J.

    2015-11-30

    The Savannah River National Laboratory (SRNL) was tasked with preparing and shipping samples for Hg speciation by Eurofins Frontier Global Sciences, Inc. in Seattle, WA on behalf of the Savannah River Remediation (SRR) Mercury Task Team. The twelfth shipment of samples was designated to include 3H evaporator system Tank 30, 32, and 37 depth samples. The Tank 30 depth sample (HTF-30-15-70) was taken at 190 inches from the tank bottom and the Tank 32 depth sample (HTF-32-15-68) was taken at 89 inches from the tank bottom and both were shipped to SRNL on June 29, 2015 in an 80 mL stainless steel dip bottles. The Tank 37 surface sample (HTF-37-15-94) was taken around 253.4 inches from the tank bottom and shipped to SRNL on July 21, 2015 in an 80 mL stainless steel dip bottle. All samples were placed in the SRNL Shielded Cells and left unopened until intermediate dilutions were made on July 24, 2015 using 1.00 mL of sample diluted to 100.00 mL with deionized H2O. A 30 mL Teflon bottle was rinsed twice with the diluted tank sample and then filled leaving as little headspace as possible. It was immediately removed from the Shielded Cells and transferred to refrigerated storage where it remained at 4 C until final dilutions were made on October 20. A second portion of the cells diluted tank sample was poured into a shielded polyethylene bottle and transferred to Analytical Development for radiochemical analysis data needed for Hazardous Material Transportation calculations.

  15. Experience with Aerosol Generation During Rotary Mode Core Sampling in the Hanford Single Shell Waste Tanks

    SciTech Connect (OSTI)

    SCHOFIELD, J.S.

    2000-01-24

    This document provides data on aerosol concentrations in tank head spaces, total mass of aerosols in the tank head space and mass of aerosols sent to the exhauster during Rotary Mode Core Sampling from November 1994 through June 1999. A decontamination factor for the RMCS exhauster filter housing is calculated based on operation data.

  16. Distinguishing Aerosol Impacts on Climate Over the Past Century

    SciTech Connect (OSTI)

    Koch, Dorothy; Menon, Surabi; Del Genio, Anthony; Ruedy, Reto; Alienov, Igor; Schmidt, Gavin A.

    2008-08-22

    Aerosol direct (DE), indirect (IE), and black carbon-snow albedo (BAE) effects on climate between 1890 and 1995 are compared using equilibrium aerosol-climate simulations in the Goddard Institute for Space Studies General Circulation Model coupled to a mixed layer ocean. Pairs of control(1890)-perturbation(1995) with successive aerosol effects allow isolation of each effect. The experiments are conducted both with and without concurrent changes in greenhouse gases (GHG's). A new scheme allowing dependence of snow albedo on black carbon snow concentration is introduced. The fixed GHG experiments global surface air temperature (SAT) changed -0.2, -1.0 and +0.2 C from the DE, IE, and BAE. Ice and snow cover increased 1.0% from the IE and decreased 0.3% from the BAE. These changes were a factor of 4 larger in the Arctic. Global cloud cover increased by 0.5% from the IE. Net aerosol cooling effects are about half as large as the GHG warming, and their combined climate effects are smaller than the sum of their individual effects. Increasing GHG's did not affect the IE impact on cloud cover, however they decreased aerosol effects on SAT by 20% and on snow/ice cover by 50%; they also obscure the BAE on snow/ice cover. Arctic snow, ice, cloud, and shortwave forcing changes occur mostly during summer-fall, but SAT, sea level pressure, and long-wave forcing changes occur during winter. An explanation is that aerosols impact the cryosphere during the warm-season but the associated SAT effect is delayed until winter.

  17. Final Project Report - ARM CLASIC CIRPAS Twin Otter Aerosol

    SciTech Connect (OSTI)

    John A. Ogren

    2010-04-05

    The NOAA/ESRL/GMD aerosol group made three types of contributions related to airborne measurements of aerosol light scattering and absorption for the Cloud and Land Surface Interaction Campaign (CLASIC) in June 2007 on the Twin Otter research airplane operated by the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS). GMD scientists served as the instrument mentor for the integrating nephelometer and particle soot absorption photometer (PSAP) on the Twin Otter during CLASIC, and were responsible for (1) instrument checks/comparisons; (2) instrument trouble shooting/repair; and (3) data quality control (QC) and submittal to the archive.

  18. Aerosol Modeling at LLNL - Our capability, results, and perspective

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    of Aerosol Indirect Effects to Cloud Parameterizations in Short-Range Weather Forecasts with CAM3 Over the Southern Great Plains during May 2003 IOP Lawrence Livermore National Laboratory This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 Catherine Chuang, James Boyle Shaocheng Xie and James Kelly LLNL-POST-401948 March 11, 2008 Why are aerosol/cloud interactions important? The greatest uncertainty in

  19. ARM - Field Campaign - Biogenic Aerosols - Effects on Clouds and Climate:

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Extended Radiosonde IOP Extended Radiosonde IOP ARM Data Discovery Browse Data Related Campaigns Biogenic Aerosols - Effects on Clouds and Climate 2014.02.01, Petäjä, AMF Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Biogenic Aerosols - Effects on Clouds and Climate: Extended Radiosonde IOP 2014.05.01 - 2014.08.31 Lead Scientist : Keri Nicoll For data sets, see below. Abstract Modified meteorological radiosondes have been

  20. ARM - Field Campaign - Carbonaceous Aerosol and Radiative Effects Study

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    (CARES) Ground Based Instruments Ground Based Instruments ARM Data Discovery Browse Data Related Campaigns Carbonaceous Aerosol and Radiative Effects Study (CARES) 2010.06.02, Zaveri, AAF Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Carbonaceous Aerosol and Radiative Effects Study (CARES) Ground Based Instruments 2010.04.01 - 2010.07.15 Lead Scientist : Daniel Cziczo For data sets, see below. Abstract New ARRA funded ARM

  1. ARM - Field Campaign - Ganges Valley Aerosol Experiment (GVAX)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsGanges Valley Aerosol Experiment (GVAX) Campaign Links Science Plan AMF India Deployment Website Field Campaign Report Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Ganges Valley Aerosol Experiment (GVAX) 2011.06.13 - 2012.03.31 Website : http://www.arm.gov/sites/amf/pgh/ Lead Scientist : V. Rao Kotamarthi Abstract The Ganges valley region is one of the largest and most rapidly developing sections of the Indian

  2. Advancing Models and Evaluation of Cumulus, Climate and Aerosol Interactions

    SciTech Connect (OSTI)

    Gettelman, Andrew

    2015-10-27

    This project was successfully able to meet its’ goals, but faced some serious challenges due to personnel issues. Nonetheless, it was largely successful. The Project Objectives were as follows: 1. Develop a unified representation of stratifom and cumulus cloud microphysics for NCAR/DOE global community models. 2. Examine the effects of aerosols on clouds and their impact on precipitation in stratiform and cumulus clouds. We will also explore the effects of clouds and precipitation on aerosols. 3. Test these new formulations using advanced evaluation techniques and observations and release

  3. Thermophoretic separation of aerosol particles from a sampled gas stream

    DOE Patents [OSTI]

    Postma, Arlin K. (Halfway, OR)

    1986-01-01

    A method for separating gaseous samples from a contained atmosphere that includes aerosol particles uses the step of repelling particles from a gas permeable surface or membrane by heating the surface to a temperature greater than that of the surrounding atmosphere. The resulting thermophoretic forces maintain the gas permeable surface clear of aerosol particles. The disclosed apparatus utilizes a downwardly facing heated plate of gas permeable material to combine thermophoretic repulsion and gravity forces to prevent particles of any size from contacting the separating plate surfaces.

  4. ARM - PI Product - Aerosol Retrievals from ARM SGP MFRSR Data

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ProductsAerosol Retrievals from ARM SGP MFRSR Data ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send PI Product : Aerosol Retrievals from ARM SGP MFRSR Data The Multi-Filter Rotating Shadowband Radiometer (MFRSR) makes precise simultaneous measurements of the solar direct normal and diffuse horizontal irradiances at six wavelengths (nominally 415, 500, 615, 673, 870, and 940 nm) at short intervals (20 sec for ARM

  5. Thermophoretic separation of aerosol particles from a sampled gas stream

    DOE Patents [OSTI]

    Postma, A.K.

    1984-09-07

    This disclosure relates to separation of aerosol particles from gas samples withdrawn from within a contained atmosphere, such as containment vessels for nuclear reactors or other process equipment where remote gaseous sampling is required. It is specifically directed to separation of dense aerosols including particles of any size and at high mass loadings and high corrosivity. The United States Government has rights in this invention pursuant to Contract DE-AC06-76FF02170 between the US Department of Energy and Westinghouse Electric Corporation.

  6. Chemical Industry Bandwidth Study

    SciTech Connect (OSTI)

    none,

    2006-12-01

    The Chemical Bandwidth Study provides a snapshot of potentially recoverable energy losses during chemical manufacturing. The advantage of this study is the use of "exergy" analysis as a tool for pinpointing inefficiencies.

  7. Capacitive chemical sensor

    DOE Patents [OSTI]

    Manginell, Ronald P; Moorman, Matthew W; Wheeler, David R

    2014-05-27

    A microfabricated capacitive chemical sensor can be used as an autonomous chemical sensor or as an analyte-sensitive chemical preconcentrator in a larger microanalytical system. The capacitive chemical sensor detects changes in sensing film dielectric properties, such as the dielectric constant, conductivity, or dimensionality. These changes result from the interaction of a target analyte with the sensing film. This capability provides a low-power, self-heating chemical sensor suitable for remote and unattended sensing applications. The capacitive chemical sensor also enables a smart, analyte-sensitive chemical preconcentrator. After sorption of the sample by the sensing film, the film can be rapidly heated to release the sample for further analysis. Therefore, the capacitive chemical sensor can optimize the sample collection time prior to release to enable the rapid and accurate analysis of analytes by a microanalytical system.

  8. Chemicals Industry Vision

    SciTech Connect (OSTI)

    none,

    1996-12-01

    Chemical industry leaders articulated a long-term vision for the industry, its markets, and its technology in the groundbreaking 1996 document Technology Vision 2020 - The U.S. Chemical Industry. (PDF 310 KB).

  9. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-10-14

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer® Spectrometermore » (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.« less

  10. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    SciTech Connect (OSTI)

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-10-14

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer Spectrometer (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.

  11. Chemical Hydrogen Storage Materials

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Troy A. Semelsberger Los Alamos National Laboratory Hydrogen Storage Summit Jan 27-29, 2015 Denver, CO Chemical Hydrogen Storage Materials 2 Objectives 1. Assess chemical hydrogen storage materials that can exceed 700 bar compressed hydrogen tanks 2. Status (state-of-the-art) of chemical hydrogen storage materials 3. Identify key material characteristics 4. Identify obstacles, challenges and risks for the successful deployment of chemical hydrogen materials in a practical on-board hydrogen

  12. ARM - Site Instruments

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    AtlanticInstruments ENA Related Links Facilities and Instruments ES&H Guidance Statement Operations Science Field Campaigns Visiting the Site ENA Fact Sheet (PDF, 512KB) Images Information for Guest Scientists Contacts Instruments : Eastern North Atlantic Active Retired Active instruments are currently deployed at fixed or mobile facilities or are available through the ARM Aerial Facility. ACSM Aerosol Chemical Speciation Monitor Aerosols Browse Plots Browse Data [ Single installation ] AOS

  13. ARM - Instrument Location Table

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govInstrumentsLocation Table Instruments Location Table Contacts Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Instrument Locations Site abbreviations explained in the key. Instrument Name Abbreviation ENA NSA SGP AMF C1 C1 EF BF CF EF IF Aerosol Chemical Speciation Monitor ACSM Atmospheric Emitted Radiance Interferometer AERI Aethalometer AETH Ameriflux Measurement Component AMC Aerosol Observing System AOS Meteorological Measurements

  14. ARM: 10-minute TEMPORARY Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sivaraman, Chitra; Flynn, Connor

    2010-12-15

    10-minute TEMPORARY Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  15. ARM: 10-minute TEMPORARY Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sivaraman, Chitra; Flynn, Connor

    10-minute TEMPORARY Raman Lidar: aerosol scattering ratio and backscattering coefficient profiles, from first Ferrare algorithm

  16. Lead Speciation in Indoor Dust: A Case Study to Assess Old Paint Contribution in a Canadian Urban House

    SciTech Connect (OSTI)

    S Beauchemin; L MacLean; P Rasmussen

    2011-12-31

    Residents in older homes may experience increased lead (Pb) exposures due to release of lead from interior paints manufactured in past decades, especially pre-1960s. The objective of the study was to determine the speciation of Pb in settled dust from an urban home built during WWII. X-ray absorption near-edge structure (XANES) and micro-X-ray diffraction (XRD) analyses were performed on samples of paint (380-2,920 mg Pb kg{sup -1}) and dust (200-1,000 mg Pb kg{sup -1}) collected prior to renovation. All dust samples exhibited a Pb XANES signature similar to that of Pb found in paint. Bulk XANES and micro-XRD identified Pb species commonly found as white paint pigments (Pb oxide, Pb sulfate, and Pb carbonate) as well as rutile, a titanium-based pigment, in the <150 m house dust samples. In the dust fraction <36 {mu}m, half of the Pb was associated with the Fe-oxyhydroxides, suggesting additional contribution of outdoor sources to Pb in the finer dust. These results confirm that old paints still contribute to Pb in the settled dust for this 65-year-old home. The Pb speciation also provided a clearer understanding of the Pb bioaccessibility: Pb carbonate > Pb oxide > Pb sulfate. This study underscores the importance of taking precautions to minimize exposures to Pb in house dust, especially in homes where old paint is exposed due to renovations or deterioration of painted surfaces.

  17. Lead speciation in indoor dust: a case study to assess old paint contribution in a Canadian urban house

    SciTech Connect (OSTI)

    Beauchemin, Suzanne; MacLean, Lachlan C.W.; Rasmussen, Pat E.

    2012-10-23

    Residents in older homes may experience increased lead (Pb) exposures due to release of lead from interior paints manufactured in past decades, especially pre-1960s. The objective of the study was to determine the speciation of Pb in settled dust from an urban home built during WWII. X-ray absorption near-edge structure (XANES) and micro-X-ray diffraction (XRD) analyses were performed on samples of paint (380-2,920 mg Pb kg{sup -1}) and dust (200-1,000 mg Pb kg{sup -1}) collected prior to renovation. All dust samples exhibited a Pb XANES signature similar to that of Pb found in paint. Bulk XANES and micro-XRD identified Pb species commonly found as white paint pigments (Pb oxide, Pb sulfate, and Pb carbonate) as well as rutile, a titanium-based pigment, in the <150 {micro}m house dust samples. In the dust fraction <36 {micro}m, half of the Pb was associated with the Fe-oxyhydroxides, suggesting additional contribution of outdoor sources to Pb in the finer dust. These results confirm that old paints still contribute to Pb in the settled dust for this 65-year-old home. The Pb speciation also provided a clearer understanding of the Pb bioaccessibility: Pb carbonate > Pb oxide > Pb sulfate. This study underscores the importance of taking precautions to minimize exposures to Pb in house dust, especially in homes where old paint is exposed due to renovations or deterioration of painted surfaces.

  18. Surface speciation of yttrium and neodymium sorbed on rutile: Interpretations using the change distribution model.

    SciTech Connect (OSTI)

    Ridley, Mora K.; Hiemstra, T; Machesky, Michael L.; Wesolowski, David J; Van Riemsdijk, Willem H.

    2012-01-01

    The adsorption of Y3+ and Nd3+ onto rutile has been evaluated over a wide range of pH (3 11) and surface loading conditions, as well as at two ionic strengths (0.03 and 0.3 m), and temperatures (25 and 50 C). The experimental results reveal the same adsorption behavior for the two trivalent ions onto the rutile surface, with Nd3+ first adsorbing at slightly lower pH values. The adsorption of both Y3+ and Nd3+ commences at pH values below the pHznpc of rutile. The experimental results were evaluated using a charge distribution (CD) and multisite complexation (MUSIC) model, and Basic Stern layer description of the electric double layer (EDL). The coordination geometry of possible surface complexes were constrained by molecular-level information obtained from X-ray standing wave measurements and molecular dynamic (MD) simulation studies. X-ray standing wave measurements showed an inner-sphere tetradentate complex for Y3+ adsorption onto the (110) rutile surface (Zhang et al., 2004b). TheMDsimulation studies suggest additional bidentate complexes may form. The CD values for all surface species were calculated based on a bond valence interpretation of the surface complexes identified by X-ray and MD. The calculated CD values were corrected for the effect of dipole orientation of interfacial water. At low pH, the tetradentate complex provided excellent fits to the Y3+ and Nd3+ experimental data. The experimental and surface complexation modeling results show a strong pH dependence, and suggest that the tetradentate surface species hydrolyze with increasing pH. Furthermore, with increased surface loading of Y3+ on rutile the tetradentate binding mode was augmented by a hydrolyzed-bidentate Y3+ surface complex. Collectively, the experimental and surface complexation modeling results demonstrate that solution chemistry and surface loading impacts Y3+ surface speciation. The approach taken of incorporating molecular-scale information into surface complexation models (SCMs) should aid in elucidating a fundamental understating of ion-adsorption reactions.

  19. Soft ionization of thermally evaporated hypergolic ionic liquid aerosols

    SciTech Connect (OSTI)

    University of California; ERC, Incorporated, Edwards Air Force Base; Air Force Research Laboratory, Edwards Air Force Base; National Synchrotron Radiation Research Center; Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; L.Vaghjiani, Ghanshyam; Leone, Stephen R.

    2012-03-16

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N?]), and a reactive hypergolic ionic liquid, 1- Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca?]), are generated by vaporizing ionic liquid submicron aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Photoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N?] ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~;;0.3 eV), attributed to reduced internal energy of the isolated ion pairs. The method of ionic liquid submicron aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally ?cooler? source of isolated intact ion pairs in the gas phase compared to effusive sources.

  20. Soft ionization of thermally evaporated hypergolic ionic liquid aerosols

    SciTech Connect (OSTI)

    University of California; ERC, Incorporated, Edwards Air Force Base; Air Force Research Laboratory, Edwards Air Force Base; National Synchrotron Radiation Research Center; Institute of Chemistry, Hebrew University; Koh, Christine J.; Liu, Chen-Lin; Harmon, Christopher W.; Strasser, Daniel; Golan, Amir; Kostko, Oleg; Chambreau, Steven D.; Vaghjiani, Ghanshyam L.; Leone, Stephen R.

    2011-07-19

    Isolated ion pairs of a conventional ionic liquid, 1-Ethyl-3-Methyl-Imidazolium Bis(trifluoromethylsulfonyl)imide ([Emim+][Tf2N?]), and a reactive hypergolic ionic liquid, 1-Butyl-3-Methyl-Imidazolium Dicyanamide ([Bmim+][Dca?]), are generated by vaporizing ionic liquid submicron aerosol particles for the first time; the vaporized species are investigated by dissociative ionization with tunable vacuum ultraviolet (VUV) light, exhibiting clear intact cations, Emim+ and Bmim+, presumably originating from intact ion pairs. Mass spectra of ion pair vapor from an effusive source of the hypergolic ionic liquid show substantial reactive decomposition due to the internal energy of the molecules emanating from the source. Photoionization efficiency curves in the near threshold ionization region of isolated ion pairs of [Emim+][Tf2N?]ionic liquid vapor are compared for an aerosol source and an effusive source, revealing changes in the appearance energy due to the amount of internal energy in the ion pairs. The aerosol source has a shift to higher threshold energy (~;;0.3 eV), attributed to reduced internal energy of the isolated ion pairs. The method of ionic liquid submicron aerosol particle vaporization, for reactive ionic liquids such as hypergolic species, is a convenient, thermally ?cooler? source of isolated intact ion pairs in the gas phase compared to effusive sources.

  1. LESSONS LEARNED IN AEROSOL MONITORING WITH THE RASA

    SciTech Connect (OSTI)

    Forrester, Joel B.; Bowyer, Ted W.; Carty, Fitz; Comes, Laura; Eslinger, Paul W.; Greenwood, Lawrence R.; Haas, Derek A.; Hayes, James C.; Kirkham, Randy R.; Lepel, Elwood A.; Litke, Kevin E.; Miley, Harry S.; Morris, Scott J.; Schrom, Brian T.; Van Davelaar, Peter; Woods, Vincent T.

    2011-09-14

    The Radionuclide Aerosol Sampler/Analyzer (RASA) is an automated aerosol collection and analysis system designed by Pacific Northwest National Laboratory (PNNL) in the 1990's and is deployed in several locations around the world as part of the International Monitoring System (IMS) required under the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The RASA operates unattended, save for regularly scheduled maintenance, iterating samples through a three-step process on a 24-hour interval. In its 15-year history, much has been learned from the operation and maintenance of the RASA that can benefit engineering updates or future aerosol systems. On 11 March 2011, a 9.0 magnitude earthquake and tsunami rocked the eastern coast of Japan, resulting in power loss and cooling failures at the Daiichi nuclear power plants in Fukushima Prefecture. Aerosol collections were conducted with the RASA in Richland, WA. We present a summary of the lessons learned over the history of the RASA, including lessons taken from the Fukushima incident, regarding the RASA IMS stations operated by the United States.

  2. Black carbon aerosols and the third polar ice cap

    SciTech Connect (OSTI)

    Menon, Surabi; Koch, Dorothy; Beig, Gufran; Sahu, Saroj; Fasullo, John; Orlikowski, Daniel

    2010-04-15

    Recent thinning of glaciers over the Himalayas (sometimes referred to as the third polar region) have raised concern on future water supplies since these glaciers supply water to large river systems that support millions of people inhabiting the surrounding areas. Black carbon (BC) aerosols, released from incomplete combustion, have been increasingly implicated as causing large changes in the hydrology and radiative forcing over Asia and its deposition on snow is thought to increase snow melt. In India BC emissions from biofuel combustion is highly prevalent and compared to other regions, BC aerosol amounts are high. Here, we quantify the impact of BC aerosols on snow cover and precipitation from 1990 to 2010 over the Indian subcontinental region using two different BC emission inventories. New estimates indicate that Indian BC emissions from coal and biofuel are large and transport is expected to expand rapidly in coming years. We show that over the Himalayas, from 1990 to 2000, simulated snow/ice cover decreases by {approx}0.9% due to aerosols. The contribution of the enhanced Indian BC to this decline is {approx}36%, similar to that simulated for 2000 to 2010. Spatial patterns of modeled changes in snow cover and precipitation are similar to observations (from 1990 to 2000), and are mainly obtained with the newer BC estimates.

  3. Effects of Ocean Ecosystem on Marine Aerosol-Cloud Interaction

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Meskhidze, Nicholas; Nenes, Athanasios

    2010-01-01

    Using smore » atellite data for the surface ocean, aerosol optical depth (AOD), and cloud microphysical parameters, we show that statistically significant positive correlations exist between ocean ecosystem productivity, the abundance of submicron aerosols, and cloud microphysical properties over different parts of the remote oceans. The correlation coefficient for remotely sensed surface chlorophyll a concentration ([Chl- a ]) and liquid cloud effective radii over productive areas of the oceans varies between − 0.2 and − 0.6 . Special attention is given to identifying (and addressing) problems from correlation analysis used in the previous studies that can lead to erroneous conclusions. A new approach (using the difference between retrieved AOD and predicted sea salt aerosol optical depth, AOD diff ) is developed to explore causal links between ocean physical and biological systems and the abundance of cloud condensation nuclei (CCN) in the remote marine atmosphere. We have found that over multiple time periods, 550 nm AOD diff (sensitive to accumulation mode aerosol, which is the prime contributor to CCN) correlates well with [Chl- a ] over the productive waters of the Southern Ocean. Since [Chl- a ] can be used as a proxy of ocean biological productivity, our analysis demonstrates the role of ocean ecology in contributing CCN, thus shaping the microphysical properties of low-level marine clouds.« less

  4. Field Trial of an Aerosol-Based Enclosure Sealing Technology

    SciTech Connect (OSTI)

    Harrington, Curtis; Springer, David

    2015-09-01

    This report presents the results from several demonstrations of a new method for sealing building envelope air leaks using an aerosol sealing process developed by the Western Cooling Efficiency Center at UC Davis. The process involves pressurizing a building while applying an aerosol sealant to the interior. As air escapes through leaks in the building envelope, the aerosol particles are transported to the leaks where they collect and form a seal that blocks the leak. Standard blower door technology is used to facilitate the building pressurization, which allows the installer to track the sealing progress during the installation and automatically verify the final building tightness. Each aerosol envelope sealing installation was performed after drywall was installed and taped, and the process did not appear to interrupt the construction schedule or interfere with other trades working in the homes. The labor needed to physically seal bulk air leaks in typical construction will not be replaced by this technology. However, this technology is capable of bringing the air leakage of a building that was built with standard construction techniques and HERS-verified sealing down to levels that would meet DOE Zero Energy Ready Homes program requirements. When a developer is striving to meet a tighter envelope leakage specification, this technology could greatly reduce the cost to achieve that goal by providing a simple and relatively low cost method for reducing the air leakage of a building envelope with little to no change in their common building practices.

  5. Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lopez-Hilfiker, F. D.; Mohr, C.; Ehn, M.; Rubach, F.; Kleist, E.; Wildt, J.; Mentel, Th. F.; Carrasquillo, A.; Daumit, K.; Hunter, J.; et al

    2015-02-18

    We measured a large suite of gas and particle phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gasmore » and particle phases, the latter being detected upon temperature programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO HR-ToF-CIMS are highly correlated with, and explain at least 25–50% of, the organic aerosol mass measured by an Aerodyne Aerosol Mass Spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from large molecular weight organics and/or oligomers (i.e. multi-phase accretion reaction products). Approximately 50% of the HR-ToF-CIMS particle phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption temperature based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas–particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the conversion of lower volatility components into the detected higher volatility compounds.« less

  6. Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lopez-Hilfiker, F. D.; Mohr, C.; Ehn, M.; Rubach, F.; Kleist, E.; Wildt, J.; Mentel, Th. F.; Carrasquillo, A. J.; Daumit, K. E.; Hunter, J. F.; et al

    2015-07-16

    We measured a large suite of gas- and particle-phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gas andmore » particle phases, the latter being detected by temperature-programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO–HR-ToF-CIMS are highly correlated with, and explain at least 25–50 % of, the organic aerosol mass measured by an Aerodyne aerosol mass spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from high molecular weight organics and/or oligomers (i.e., multi-phase accretion reaction products). Approximately 50 % of the HR-ToF-CIMS particle-phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption-temperature-based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas-particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the conversion of lower volatility components into the detected higher volatility compounds.« less

  7. Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Lopez-Hilfiker, F. D.; Mohr, C.; Ehn, M.; Rubach, F.; Kleist, E.; Wildt, J.; Mentel, Th. F.; Carrasquillo, A.; Daumit, K.; Hunter, J.; et al

    2015-02-18

    We measured a large suite of gas and particle phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gasmore »and particle phases, the latter being detected upon temperature programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO HR-ToF-CIMS are highly correlated with, and explain at least 25–50% of, the organic aerosol mass measured by an Aerodyne Aerosol Mass Spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from large molecular weight organics and/or oligomers (i.e. multi-phase accretion reaction products). Approximately 50% of the HR-ToF-CIMS particle phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption temperature based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas–particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the conversion of lower volatility components into the detected higher volatility compounds.« less

  8. Sources and composition of submicron organic mass in marine aerosol particles

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA production« less

  9. Sources and composition of submicron organic mass in marine aerosol particles

    SciTech Connect (OSTI)

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak location is closer to that of polysaccharides. This may result from the larger saccharides preferentially remaining in the seawater during gPMA and aPMA production

  10. Aerosol cluster impact and break-up : II. Atomic and Cluster Scale Models.

    SciTech Connect (OSTI)

    Lechman, Jeremy B.; Takato, Yoichi

    2010-09-01

    Understanding the interaction of aerosol particle clusters/flocs with surfaces is an area of interest for a number of processes in chemical, pharmaceutical, and powder manufacturing as well as in steam-tube rupture in nuclear power plants. Developing predictive capabilities for these applications involves coupled phenomena on multiple length and timescales from the process macroscopic scale ({approx}1m) to the multi-cluster interaction scale (1mm-0.1m) to the single cluster scale ({approx}1000 - 10000 particles) to the particle scale (10nm-10{micro}m) interactions, and on down to the sub-particle, atomic scale interactions. The focus of this report is on the single cluster scale; although work directed toward developing better models of particle-particle interactions by considering sub-particle scale interactions and phenomena is also described. In particular, results of mesoscale (i.e., particle to single cluster scale) discrete element method (DEM) simulations for aerosol cluster impact with rigid walls are presented. The particle-particle interaction model is based on JKR adhesion theory and is implemented as an enhancement to the granular package in the LAMMPS code. The theory behind the model is outlined and preliminary results are shown. Additionally, as mentioned, results from atomistic classical molecular dynamics simulations are also described as a means of developing higher fidelity models of particle-particle interactions. Ultimately, the results from these and other studies at various scales must be collated to provide systems level models with accurate 'sub-grid' information for design, analysis and control of the underlying systems processes.

  11. Results of Hg speciation testing on 3Q15 tank 50, salt solution feed tank (SSFT), and solvent hold tank (SHT) materials

    SciTech Connect (OSTI)

    Bannochie, C.

    2015-08-13

    The Savannah River National Laboratory (SRNL) was tasked with preparing and shipping samples for Hg speciation by Eurofins Frontier Global Sciences, Inc. in Seattle, WA on behalf of the Savannah River Remediation (SRR) Mercury Task Team. The results are documented in this report.

  12. FY 2011 Second Quarter: Demonstration of New Aerosol Measurement Verification Testbed for Present-Day Global Aerosol Simulations

    SciTech Connect (OSTI)

    Koch, D

    2011-03-20

    The regional-scale Weather Research and Forecasting (WRF) model is being used by a DOE Earth System Modeling (ESM) project titled Improving the Characterization of Clouds, Aerosols and the Cryosphere in Climate Models to evaluate the performance of atmospheric process modules that treat aerosols and aerosol radiative forcing in the Arctic. We are using a regional-scale modeling framework for three reasons: (1) It is easier to produce a useful comparison to observations with a high resolution model; (2) We can compare the behavior of the CAM parameterization suite with some of the more complex and computationally expensive parameterizations used in WRF; (3) we can explore the behavior of this parameterization suite at high resolution. Climate models like the Community Atmosphere Model version 5 (CAM5) being used within the Community Earth System Model (CESM) will not likely be run at mesoscale spatial resolutions (1020 km) until 510 years from now. The performance of the current suite of physics modules in CAM5 at such resolutions is not known, and current computing resources do not permit high-resolution global simulations to be performed routinely. We are taking advantage of two tools recently developed under PNNL Laboratory Directed Research and Development (LDRD) projects for this activity. The first is the Aerosol Modeling Testbed (Fast et al., 2011b), a new computational framework designed to streamline the process of testing and evaluating aerosol process modules over a range of spatial and temporal scales. The second is the CAM5 suite of physics parameterizations that have been ported into WRF so that their performance and scale dependency can be quantified at mesoscale spatial resolutions (Gustafson et al., 2010; with more publications in preparation).

  13. 2014 CHEMICAL REACTIONS AT SURFACES GORDON RESEARCH CONFERENCE AND GORDON RESEARCH SEMINAR (APRIL 28-MAY 3, 2013 - LES DIABLERETS CONFERENCE CENTER, LES DIABLERETS, SWITZERLAND)

    SciTech Connect (OSTI)

    Stair, Peter C.

    2013-02-03

    presentations on chemistry at solid and liquid surfaces of relevance to catalysis, synthesis, photochemistry, environmental science, and tribology. Topics include: Fundamental Surface Chemistry; Catalysis; Solid Liquid and Aerosol Interfaces; Surface Photochemistry; Synthesis of Surfaces; Environmental Interfaces; Hot Topics in Surface Chemical Reactions; Tribology; Gas-Surface Scattering and Reactions; Novel Materials and Environments.

  14. Enhanced Chemical Cleaning

    Office of Environmental Management (EM)

    Enhanced Chemical Cleaning Renee H. Spires Enhanced Chemical Cleaning Project Manager July 29, 2009 Tank Waste Corporate Board 2 Objective Provide an overview of the ECC process and plan 3 Chemical Cleaning * Oxalic Acid can get tanks clean - Tank 16 set a standard in 1982 - Tanks 5-6 Bulk OA cleaning results under evaluation * However, the downstream flowsheet and financial impacts of handling the spent acid were unacceptable Before After Tank 16 Tank 16 4 Oxalic Acid Flowsheet Impacts Evap

  15. Chemical Sciences Project Description

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Modeling & Simulation Data Analysis and Modeling & Simulation for the Chemical Sciences Project Description Almos every scientific activity at Los Alamos involves data analysis and modeling. From a chemical sciences point of view, such work transforms "raw" data into a form that provides useful information that is predictive, confirmatory, or exploratory. The key to understanding the world around us is the ability to put the chemical data we collect into a meaningful context

  16. EMSP Final Report: Electrically Driven Technologies for Radioactive Aerosol Abatement

    SciTech Connect (OSTI)

    DePaoli, D.W.

    2003-01-22

    The purpose of this research project was to develop an improved understanding of how electrically driven processes, including electrocoalescence, acoustic agglomeration, and electric filtration, may be employed to efficiently treat problems caused by the formation of aerosols during DOE waste treatment operations. The production of aerosols during treatment and retrieval operations in radioactive waste tanks and during thermal treatment operations such as calcination presents a significant problem of cost, worker exposure, potential for release, and increased waste volume. There was anecdotal evidence in the literature that acoustic agglomeration and electrical coalescence could be used together to change the size distribution of aerosol particles in such a way as to promote easier filtration and less frequent maintenance of filtration systems. As such, those electrically driven technologies could potentially be used as remote technologies for improved treatment; however, existing theoretical models are not suitable for prediction and design. To investigate the physics of such systems, and also to prototype a system for such processes, a collaborative project was undertaken between Oak Ridge National Laboratory (ORNL) and the University of Texas at Austin (UT). ORNL was responsible for the larger-scale prototyping portion of the project, while UT was primarily responsible for the detailed physics in smaller scale unit reactors. It was found that both electrical coalescence and acoustic agglomeration do in fact increase the rate of aggregation of aerosols. Electrical coalescence requires significantly less input power than acoustic agglomeration, but it is much less effective in its ability to aggregate/coalesce aerosols. The larger-scale prototype showed qualitatively similar results as the unit reactor tests, but presented more difficulty in interpretation of the results because of the complex multi-physics coupling that necessarily occur in all larger-scale system tests. An additional finding from this work is that low-amplitude oscillation may provide an alternative, non-invasive, non-contact means of controlling settling and/or suspension of solids. Further investigation would be necessary to evaluate its utility for radioactive waste treatment applications. This project did not uncover a new technology for radioactive waste treatment. While it may be possible that an efficient electrically driven technology for aerosol treatment could be developed, it appears that other technologies, such as steel and ceramic HEPA filters, can suitably solve this problem. If further studies are to be undertaken, additional fundamental experimentation and modeling is necessary to fully capture the physics; in addition, larger-scale tests are needed to demonstrate the treatment of flowing gas streams through the coupling of acoustic agglomeration with electrocoalescence.

  17. American Chemical Society Fellow

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Laboratory (LANL) scientist Kristin Omberg was named as an American Chemical Society (ACS) Fellow for her contributions to national security as a "technical leader in detecting...

  18. Apparatus for chemical synthesis

    DOE Patents [OSTI]

    Kong, Peter C.; Herring, J. Stephen; Grandy, Jon D.

    2011-05-10

    A method and apparatus for forming a chemical hydride is described and which includes a pseudo-plasma-electrolysis reactor which is operable to receive a solution capable of forming a chemical hydride and which further includes a cathode and a movable anode, and wherein the anode is moved into and out of fluidic, ohmic electrical contact with the solution capable of forming a chemical hydride and which further, when energized produces an oxygen plasma which facilitates the formation of a chemical hydride in the solution.

  19. Field emission chemical sensor

    DOE Patents [OSTI]

    Panitz, J.A.

    1983-11-22

    A field emission chemical sensor for specific detection of a chemical entity in a sample includes a closed chamber enclosing two field emission electrode sets, each field emission electrode set comprising (a) an electron emitter electrode from which field emission electrons can be emitted when an effective voltage is connected to the electrode set; and (b) a collector electrode which will capture said electrons emitted from said emitter electrode. One of the electrode sets is passive to the chemical entity and the other is active thereto and has an active emitter electrode which will bind the chemical entity when contacted therewith.

  20. Solid-water detoxifying reagents for chemical and biological agents

    DOE Patents [OSTI]

    Hoffman, Dennis M.; Chiu, Ing Lap

    2006-04-18

    Formation of solid-water detoxifying reagents for chemical and biological agents. Solutions of detoxifying reagent for chemical and biological agents are coated using small quantities of hydrophobic nanoparticles by vigorous agitation or by aerosolization of the solution in the presence of the hydrophobic nanoparticles to form a solid powder. For example, when hydrophobic fumed silica particles are shaken in the presence of IN oxone solution in approximately a 95:5-weight ratio, a dry powder results. The hydrophobic silica forms a porous coating of insoluble fine particles around the solution. Since the chemical or biological agent tends to be hydrophobic on contact with the weakly encapsulated detoxifying solution, the porous coating breaks down and the detoxifying reagent is delivered directly to the chemical or biological agent for maximum concentration at the point of need. The solid-water (coated) detoxifying solutions can be blown into contaminated ventilation ducting or other difficult to reach sites for detoxification of pools of chemical or biological agent. Once the agent has been detoxified, it can be removed by flushing the area with air or other techniques.

  1. Science Overview Document Indirect and Semi-Direct Aerosol Campaign (ISDAC) April 2008

    SciTech Connect (OSTI)

    SJ Ghan; B Schmid; JM Hubbe; CJ Flynn; A Laskin; AA Zelenyuk; DJ Czizco; CN Long; G McFarquhar; J Verlinde; J Harrington; JW Strapp; P Liu; A Korolev; A McDonald; M Wolde; A Fridlind; T Garrett; G Mace; G Kok; S Brooks; D Collins; D Lubin; P Lawson; M Dubey; C Mazzoleni; M Shupe; S Xie; DD Turner; Q Min; EJ Mlawer; D Mitchell

    2007-11-01

    The ARM Climate Research Facilitys (ACRF) Aerial Vehicle Program (AVP) will deploy an intensive cloud and aerosol observing system to the ARM North Slope of Alaska (NSA) locale for a five week Indirect and Semi-Direct Aerosol Campaign (ISDAC) during period 29 March through 30 April 2008. The deployment period is within the International Polar Year, thus contributing to and benefiting from the many ancillary observing systems collecting data synergistically. We will deploy the Canadian National Research Council Convair 580 aircraft to measure temperature, humidity, total particle number, aerosol size distribution, single particle composition, concentrations of cloud condensation nuclei and ice nuclei, optical scattering and absorption, updraft velocity, cloud liquid water and ice contents, cloud droplet and crystal size distributions, cloud particle shape, and cloud extinction. In addition to these aircraft measurements, ISDAC will deploy two instruments at the ARM site in Barrow: a spectroradiometer to retrieve cloud optical depth and effective radius, and a tandem differential mobility analyzer to measure the aerosol size distribution and hygroscopicity. By using many of the same instruments used during Mixed-Phase Arctic Cloud Experiment (M-PACE), conducted in October 2004, we will be able to contrast the arctic aerosol and cloud properties during the fall and spring transitions. The aerosol measurements can be used in cloud models driven by objectively analyzed boundary conditions to test whether the cloud models can simulate the aerosol influence on the clouds. The influence of aerosol and boundary conditions on the simulated clouds can be separated by running the cloud models with all four combinations of M-PACE and ISDAC aerosol and boundary conditions: M-PACE aerosol and boundary conditions, M-PACE aerosol and ISDAC boundary conditions, ISDAC aerosol and M-PACE boundary conditions, and ISDAC aerosol and boundary conditions. ISDAC and M-PACE boundary conditions are likely to be very different because of the much more extensive ocean water during M-PACE. The uniformity of the surface conditions during ISDAC greatly simplifies the objective analysis (surface fluxes and precipitation are very weak), so that it can largely rely on the European Centre for Medium-Range Weather Forecasts analysis. The aerosol measurements can also be used as input to the cloud models and to evaluate the aerosol retrievals. By running the cloud models with and without solar absorption by the aerosols, we can determine the semidirect effect of the aerosol on the clouds.

  2. Final Project Report: Release of aged contaminants from weathered sediments: Effects of sorbate speciation on scaling of reactive transport

    SciTech Connect (OSTI)

    Jon Chorover, University of Arizona; Peggy O'????Day, University of California, Merced; Karl Mueller, Penn State University; Wooyong Um, Pacific Northwest National Laboratory; Carl Steefel, Lawrence Berkeley National Laboratory

    2012-10-01

    Hanford sediments impacted by hyperalkaline high level radioactive waste have undergone incongruent silicate mineral weathering concurrent with contaminant uptake. In this project, we studied the impact of background pore water (BPW) on strontium, cesium and iodine desorption and transport in Hanford sediments that were experimentally weathered by contact with simulated hyperalkaline tank waste leachate (STWL) solutions. Using those lab-weathered Hanford sediments (HS) and model precipitates formed during nucleation from homogeneous STWL solutions (HN), we (i) provided detailed characterization of reaction products over a matrix of field-relevant gradients in contaminant concentration, PCO2, and reaction time; (ii) improved molecular-scale understanding of how sorbate speciation controls contaminant desorption from weathered sediments upon removal of caustic sources; and (iii) developed a mechanistic, predictive model of meso- to field-scale contaminant reactive transport under these conditions.

  3. X-ray absorption fine structure spectroscopic determination of plutonium speciation at the Rocky Flats environmental technology

    SciTech Connect (OSTI)

    Lezama-pacheco, Juan S; Conradson, Steven D; Clark, David L

    2008-01-01

    X-ray Absorption Fine Structure spectroscopy was used to probe the speciation of the ppm level Pu in thirteen soil and concrete samples from the Rocky Flats Environmental Technology Site in support of the site remediation effort that has been successfully completed since these measurements. In addition to X-ray Absorption Near Edge Spectra, two of the samples yielded Extended X-ray Absorption Fine Structure spectra that could be analyzed by curve-fits. Most of these spectra exhibited features consistent with PU(IV), and more specificaJly, PuO{sub 2+x}-type speciation. Two were ambiguous, possibly indicating that Pu that was originally present in a different form was transforming into PuO{sub 2+x}, and one was interpreted as demonstrating the presence of an unusual Pu(VI) compound, consistent with its source being spills from a PUREX purification line onto a concrete floor and the resultant extreme conditions. These experimental results therefore validated models that predicted that insoluble PuO{sub 2+x} would be the most stable form of Pu in equilibrium with air and water even when the source terms were most likely Pu metal with organic compounds or a Pu fire. A corollary of these models' predictions and other in situ observations is therefore that the minimal transport of Pu that occurred on the site was via the resuspension and mobilization of colloidal particles. Under these conditions, the small amounts of diffusely distributed Pu that were left on the site after its remediation pose only a negligible hazard.

  4. Parameterizations of Cloud Microphysics and Indirect Aerosol Effects

    SciTech Connect (OSTI)

    Tao, Wei-Kuo

    2014-05-19

    1. OVERVIEW Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds [NRC, 2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path [Twomey, 1977] and the "semi-direct" effect on cloud coverage [e.g., Ackerman et al., 2000]. Enhanced aerosol concentrations can also suppress warm rain processes by producing a narrow droplet spectrum that inhibits collision and coalescence processes [e.g., Squires and Twomey, 1961; Warner and Twomey, 1967; Warner, 1968; Rosenfeld, 1999]. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect [Albrecht, 1989], is even more complex, especially for mixed-phase convective clouds. Table 1 summarizes the key observational studies identifying the microphysical properties, cloud characteristics, thermodynamics and dynamics associated with cloud systems from high-aerosol continental environments. For example, atmospheric aerosol concentrations can influence cloud droplet size distributions, warm-rain process, cold-rain process, cloud-top height, the depth of the mixed phase region, and occurrence of lightning. In addition, high aerosol concentrations in urban environments could affect precipitation variability by providing an enhanced source of cloud condensation nuclei (CCN). Hypotheses have been developed to explain the effect of urban regions on convection and precipitation [van den Heever and Cotton, 2007 and Shepherd, 2005]. Recently, a detailed spectral-bin microphysical scheme was implemented into the Goddard Cumulus Ensemble (GCE) model. Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and summertime convection over a mid-latitude continent with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. The impact of atmospheric aerosol concentration on cloud and precipitation will be investigated. 2. MODEL DESCRIPTION AND CASE STUDIES 2.1 GCE MODEL The model used in this study is the 2D version of the GCE model. Modeled flow is anelastic. Second- or higher-order advection schemes can produce negative values in the solution. Thus, a Multi-dimensional Positive Definite Advection Transport Algorithm (MPDATA) has been implemented into the model. All scalar variables (potential temperature, water vapor, turbulent coefficient and all five hydrometeor classes) use forward time differencing and the MPDATA for advection. Dynamic variables, u, v and w, use a second-order accurate advection scheme and a leapfrog time integration (kinetic energy semi-conserving method). Short-wave (solar) and long-wave radiation as well as a subgrid-scale TKE turbulence scheme are also included in the model. Details of the model can be found in Tao and Simpson (1993) and Tao et al. (2003). 2.2 Microphysics (Bin Model) The formulation of the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (cloud droplets and raindrops), and six types of ice particles: pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail. Each type is described by a special size distribution function containing 33 categories (bins). Atmospheric aerosols are also described using number density size-distribution functions (containing 33 bins). Droplet nucleation (activation) is derived from the analytical calculation of super-saturation, which is used to determine the sizes of aerosol particles to be activated and the corresponding sizes of nucleated droplets. Primary nucleation of each type of ice crystal takes place within certain temperature ranges. A detailed description of these explicitly parameterized processes can be found in Khain and Sednev (1996) and Khain et al. (1999, 2001). 2.3 Case Studies Three cases, a tropical oceanic squall system observed during TOGA COARE (Tropical Ocean and Global Atmosphere Coupled Ocean-Atmosphere Response Experiment, which occurred over the Pacific Ocean warm pool from November 1992 to February 1993), a midlatitude continental squall system observed during PRESTORM (Preliminary Regional Experiment for STORM-Central, which occurred in Kansas and Oklahoma during May-June 1985), and mid-afternoon convection observed during CRYSTAL-FACE (Cirrus Regional Study of Tropical Anvils and Cirrus Layers – Florida Area Cumulus Experiment, which occurred in Florida during July 2002), will be used to examine the impact of aerosols on deep, precipitating systems. 3. SUMMARY of RESULTS • For all three cases, higher CCN produces smaller cloud droplets and a narrower spectrum. Dirty conditions delay rain formation, increase latent heat release above the freezing level, and enhance vertical velocities at higher altitude for all cases. Stronger updrafts, deeper mixed-phase regions, and more ice particles are simulated with higher CCN in good agreement with observations. • In all cases, rain reaches the ground early with lower CCN. Rain suppression is also evident in all three cases with high CCN in good agreement with observations (Rosenfeld, 1999, 2000 and others). Rain suppression, however, only occurs during the first hour of simulation. This result suggests that microphysical processes dominate the impact of aerosols on precipitation in the early stage of precipitation development. • During the mature stage of the simulations, the effect of increasing aerosol concentration ranges from rain suppression in the PRESTORM case to little effect on surface rainfall in the CRYSTAL-FACE case to rain enhancement in the TOGA COARE case. • The model results suggest that evaporative cooling is a key process in determining whether higher CCN reduces or enhances precipitation. Cold pool strength can be enhanced by stronger evaporation. When cold pool interacts with the near surface wind shear, the low-level convergence can be stronger, facilitating secondary cloud formation and more vigorous precipitation processes. Evaporative cooling is more than two times stronger at low levels with higher CCN for the TOGA COARE case during the early stages of precipitation development. However, evaporative cooling is slightly stronger at lower levels with lower CCN for the PRESTORM case. The early formation of rain in the clean environment could allow for the formation of an earlier and stronger cold pool compared to a dirty environment. PRESTORM has a very dry environment and both large and small rain droplets can evaporate. Consequently, the cold pool is relatively weaker, and the system is relatively less intense with higher CCN. • Sensitivity tests are conducted to determine the impact of ice processes on aerosol-precipitation interaction. The results suggested that ice processes are crucial for suppressing precipitation due to high CCN for the PRESTORM case. More and smaller ice particles are generated in the dirty case and transported to the trailing stratiform region. This reduces the heavy convective rain and contributes to the weakening of the cold pool. Warm rain processes dominate the TOGA COARE case. Therefore, ice processes only play a secondary role in terms of aerosol-precipitation interaction. • Two of the three cloud systems presented in this paper formed a line structure (squall system). A 2D simulation, therefore, gives a good approximation to such a line of convective clouds. Since the real atmosphere is 3D, further 3D cloud-resolving simulations are needed to address aerosol-precipitation interactions. 4. REFERENCES Tao, W.-K., X. Li, A. Khain, T. Matsui, S. Lang, and J. Simpson, 2007: The role of atmospheric aerosol concentration on deep convective precipitation: Cloud-resolving model simulations. J. Geophy. Res., 112, D24S18, doi:10.1029/2007JD008728. All other references can be found in above paper. 5. Acknowledgements The GCE model is mainly supported by the NASA Headquarters Atmospheric Dynamics and Thermodynamics Program and the NASA Tropical Rainfall Measuring Mission (TRMM). The research was also supported by the Office of Science (BER), U. S. Department of Energy/Atmospheric Radiation Measurement (DOE/ARM) Interagency. The authors acknowledge NASA Goddard Space Flight Center for computer time used in this research.

  5. The impact of atmospheric aerosols on trace metal chemistry in open ocean surface seawater 3. Lead

    SciTech Connect (OSTI)

    Maring, H.B.; Duce, R.A. )

    1990-04-15

    Atmospheric aerosols collected at Enewetak Atoll in the tropical North Pacific were exposed to seawater in laboratory experiments to assess the impact of atmospheric aerosols on lead chemistry in surface seawater. The net atmospheric flux of soluble lead to the ocean is between 16 and 32 pmol cm{sup {minus}2}/yr at Enewetak. The stable lead isotopic composition of soluble aerosol lead indicates that it is of anthropogenic origin. Anthropogenic aerosol lead from Central and North America appears to be less soluble and/or to dissolve less rapidly than that from Asia. Dissolved organic matter and possibly lower pH appear to increase the nonaluminosilicate aerosol lead solubility and/or dissolution rate. The isotopic composition of lead in air, seawater and dry deposition suggests that after deposition in the ocean, nonaluminosilicate particulate lead can be reinjected into the atmosphere during sea salt aerosol production.

  6. Unintended consequences of atmospheric injection of sulphate aerosols.

    SciTech Connect (OSTI)

    Brady, Patrick Vane; Kobos, Peter Holmes; Goldstein, Barry

    2010-10-01

    Most climate scientists believe that climate geoengineering is best considered as a potential complement to the mitigation of CO{sub 2} emissions, rather than as an alternative to it. Strong mitigation could achieve the equivalent of up to -4Wm{sup -2} radiative forcing on the century timescale, relative to a worst case scenario for rising CO{sub 2}. However, to tackle the remaining 3Wm{sup -2}, which are likely even in a best case scenario of strongly mitigated CO{sub 2} releases, a number of geoengineering options show promise. Injecting stratospheric aerosols is one of the least expensive and, potentially, most effective approaches and for that reason an examination of the possible unintended consequences of the implementation of atmospheric injections of sulphate aerosols was made. Chief among these are: reductions in rainfall, slowing of atmospheric ozone rebound, and differential changes in weather patterns. At the same time, there will be an increase in plant productivity. Lastly, because atmospheric sulphate injection would not mitigate ocean acidification, another side effect of fossil fuel burning, it would provide only a partial solution. Future research should aim at ameliorating the possible negative unintended consequences of atmospheric injections of sulphate injection. This might include modeling the optimum rate and particle type and size of aerosol injection, as well as the latitudinal, longitudinal and altitude of injection sites, to balance radiative forcing to decrease negative regional impacts. Similarly, future research might include modeling the optimum rate of decrease and location of injection sites to be closed to reduce or slow rapid warming upon aerosol injection cessation. A fruitful area for future research might be system modeling to enhance the possible positive increases in agricultural productivity. All such modeling must be supported by data collection and laboratory and field testing to enable iterative modeling to increase the accuracy and precision of the models, while reducing epistemic uncertainties.

  7. Aerosol Radiative Effects in the Tropical Western Pacific

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Effects in the Tropical Western Pacific A. M. Vogelmann Center for Atmospheric Sciences Scripps Institution of Oceanography University of California San Diego, California Introduction Atmospheric Radiation Measurement (ARM) Program observations are used to quantify the aerosol radiative effects in the climatically important Tropical Western Pacific (TWP). This quantification addresses two primary ARM objectives by (1) ascertaining the existing variability of the radiative forcing and its

  8. Laboratory Testing of Aerosol for Enclosure Air Sealing

    SciTech Connect (OSTI)

    Harrington, C.; Modera, M.

    2012-05-01

    Space conditioning energy use can be significantly reduced by addressing uncontrolled infiltration and exfiltration through the envelope of a building. A process for improving the air tightness of a building envelope by sealing shell leaks with an aerosol sealing technology is presented. Both retrofit and new construction applications are possible through applying this process either in attics and crawlspaces or during rough-in stage.

  9. ARM - Carbonaceous Aerosols and Radiative Effects Study (CARES)

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Related Links CARES Home AAF Home ARM Data Discovery Browse Data Post-Campaign Data Sets Field Updates CARES Wiki Campaign Images Experiment Planning Proposal Abstract and Related Campaigns Science Plan Operations Plan Measurements Forecasts News News & Press Backgrounder (PDF, 1.45MB) G-1 Aircraft Fact Sheet (PDF, 1.3MB) Contacts Rahul Zaveri, Lead Scientist Carbonaceous Aerosols and Radiative Effects Study (CARES) Proposed ground sites (T0 and T1) and G-1 airborne instrumentation sampling

  10. Aerosol reactor production of uniform submicron powders

    DOE Patents [OSTI]

    Flagan, Richard C. (Pasadena, CA); Wu, Jin J. (Pasadena, CA)

    1991-02-19

    A method of producing submicron nonagglomerated particles in a single stage reactor includes introducing a reactant or mixture of reactants at one end while varying the temperature along the reactor to initiate reactions at a low rate. As homogeneously small numbers of seed particles generated in the initial section of the reactor progress through the reactor, the reaction is gradually accelerated through programmed increases in temperature along the length of the reactor to promote particle growth by chemical vapor deposition while minimizing agglomerate formation by maintaining a sufficiently low number concentration of particles in the reactor such that coagulation is inhibited within the residence time of particles in the reactor. The maximum temperature and minimum residence time is defined by a combination of temperature and residence time that is necessary to bring the reaction to completion. In one embodiment, electronic grade silane and high purity nitrogen are introduced into the reactor and temperatures of approximately 770.degree. K. to 1550.degree. K. are employed. In another embodiment silane and ammonia are employed at temperatures from 750.degree. K. to 1800.degree. K.

  11. Tortuous path chemical preconcentrator

    DOE Patents [OSTI]

    Manginell, Ronald P. (Albuquerque, NM); Lewis, Patrick R. (Albuquerque, NM); Adkins, Douglas R. (Albuquerque, NM); Wheeler, David R. (Albuquerque, NM); Simonson, Robert J. (Cedar Crest, NM)

    2010-09-21

    A non-planar, tortuous path chemical preconcentrator has a high internal surface area having a heatable sorptive coating that can be used to selectively collect and concentrate one or more chemical species of interest from a fluid stream that can be rapidly released as a concentrated plug into an analytical or microanalytical chain for separation and detection. The non-planar chemical preconcentrator comprises a sorptive support structure having a tortuous flow path. The tortuosity provides repeated twists, turns, and bends to the flow, thereby increasing the interfacial contact between sample fluid stream and the sorptive material. The tortuous path also provides more opportunities for desorption and readsorption of volatile species. Further, the thermal efficiency of the tortuous path chemical preconcentrator is comparable or superior to the prior non-planar chemical preconcentrator. Finally, the tortuosity can be varied in different directions to optimize flow rates during the adsorption and desorption phases of operation of the preconcentrator.

  12. High air volume to low liquid volume aerosol collector

    DOE Patents [OSTI]

    Masquelier, Donald A. (Tracy, CA); Milanovich, Fred P. (Lafayette, CA); Willeke, Klaus (Cincinnati, OH)

    2003-01-01

    A high air volume to low liquid volume aerosol collector. A high volume flow of aerosol particles is drawn into an annular, centripetal slot in a collector which directs the aerosol flow into a small volume of liquid pool contained is a lower center section of the collector. The annular jet of air impinges into the liquid, imbedding initially airborne particles in the liquid. The liquid in the pool continuously circulates in the lower section of the collector by moving to the center line, then upwardly, and through assistance by a rotating deflector plate passes back into the liquid at the outer area adjacent the impinging air jet which passes upwardly through the liquid pool and through a hollow center of the collector, and is discharged via a side outlet opening. Any liquid droplets escaping with the effluent air are captured by a rotating mist eliminator and moved back toward the liquid pool. The collector includes a sensor assembly for determining, controlling, and maintaining the level of the liquid pool, and includes a lower centrally located valve assembly connected to a liquid reservoir and to an analyzer for analyzing the particles which are impinged into the liquid pool.

  13. Source terms for plutonium aerosolization from nuclear weapon accidents

    SciTech Connect (OSTI)

    Stephens, D.R.

    1995-07-01

    The source term literature was reviewed to estimate aerosolized and respirable release fractions for accidents involving plutonium in high-explosive (HE) detonation and in fuel fires. For HE detonation, all estimates are based on the total amount of Pu. For fuel fires, all estimates are based on the amount of Pu oxidized. I based my estimates for HE detonation primarily upon the results from the Roller Coaster experiment. For hydrocarbon fuel fire oxidation of plutonium, I based lower bound values on laboratory experiments which represent accident scenarios with very little turbulence and updraft of a fire. Expected values for aerosolization were obtained from the Vixen A field tests, which represent a realistic case for modest turbulence and updraft, and for respirable fractions from some laboratory experiments involving large samples of Pu. Upper bound estimates for credible accidents are based on experiments involving combustion of molten plutonium droplets. In May of 1991 the DOE Pilot Safety Study Program established a group of experts to estimate the fractions of plutonium which would be aerosolized and respirable for certain nuclear weapon accident scenarios.

  14. Alveolar targeting of aerosol pentamidine. Toward a rational delivery system

    SciTech Connect (OSTI)

    Simonds, A.K.; Newman, S.P.; Johnson, M.A.; Talaee, N.; Lee, C.A.; Clarke, S.W. )

    1990-04-01

    Nebulizer systems that deposit a high proportion of aerosolized pentamidine on large airways are likely to be associated with marked adverse side effects, which may lead to premature cessation of treatment. We have measured alveolar deposition and large airway-related side effects (e.g., cough, breathlessness, and effect on pulmonary function) after aerosolization of 150 mg pentamidine isethionate labeled with {sup 99m}Tc-Sn-colloid. Nine patients with AIDS were studied using three nebulizer systems producing different droplet size profiles: the Acorn System 22, Respirgard II, and Respirgard II with the inspiratory baffle removed. Alveolar deposition was greatest and side effects least with the nebulizer producing the smallest droplet size profile (Respirgard II), whereas large airway-related side effects were prominent and alveolar deposition lowest with the nebulizer producing the largest droplet size (Acorn System 22). Values for alveolar deposition and adverse airway effects were intermediate using the Respirgard with inspiratory baffle removed, thus indicating the importance of the baffle valve in determining droplet size. Addition of a similar baffle valve to the Acorn System 22 produced a marked improvement in droplet size profile. Selection of a nebulizer that produces an optimal droplet size range offers the advantage of enhancing alveolar targeting of aerosolized pentamidine while reducing large airway-related side effects.

  15. ITP Chemicals: Chemical Industry of the Future: New Biocatalysts: Essential

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Tools for a Sustainable 21st Century Chemical Industry | Department of Energy Chemical Industry of the Future: New Biocatalysts: Essential Tools for a Sustainable 21st Century Chemical Industry ITP Chemicals: Chemical Industry of the Future: New Biocatalysts: Essential Tools for a Sustainable 21st Century Chemical Industry PDF icon biocatalysis_roadmap.pdf More Documents & Publications TECHNOLOGY VISION 2020: The U.S. Chemical Industry Gasoline Biodesulfurization Fact Sheet Breaking the

  16. Chemical Disposition of Plutonium in Hanford Site Tank Wastes

    SciTech Connect (OSTI)

    Delegard, Calvin H.; Jones, Susan A.

    2015-05-07

    This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used to recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers occurs only if they are physically proximal in solution or the plutonium present in the solid phase is intimately mixed with compounds or solutions of these absorbers. No information on the potential chemical interaction of plutonium with cadmium was found in the technical literature. Definitive evidence of sorption or adsorption of plutonium onto various solid phases from strongly alkaline media is less clear-cut, perhaps owing to fewer studies and to some well-attributed tests run under conditions exceeding the very low solubility of plutonium. The several studies that are well-founded show that only about half of the plutonium is adsorbed from waste solutions onto sludge solid phases. The organic complexants found in many Hanford tank waste solutions seem to decrease plutonium uptake onto solids. A number of studies show plutonium sorbs effectively onto sodium titanate. Finally, this report presents findings describing the behavior of plutonium vis-à-vis other elements during sludge dissolution in nitric acid based on Hanford tank waste experience gained by lab-scale tests, chemical and radiochemical sample characterization, and full-scale processing in preparation for strontium-90 recovery from PUREX sludges.

  17. Some Results of Joint Measurements of Aerosol Extinction of Solar Radiation on Horizontal and Slant Paths

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Results of Joint Measurements of Aerosol Extinction of Solar Radiation on Horizontal and Slant Paths S. M. Sakerin, D. M. Kabanov, Yu. A. Pkhalagov, and V. N. Uzhegov Institute of Atmospheric Optics Tomsk, Russia Introduction It's a well-known fact that the contribution atmospheric aerosol makes in the total extinction of radiation in calculations and models of radiation must be considered; the quantitative measure of this contribution is the aerosol optical thickness of the atmosphere. The

  18. Posters Cloud Parameterizations in Global Climate Models: The Role of Aerosols

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    3 Posters Cloud Parameterizations in Global Climate Models: The Role of Aerosols J. E. Penner and C. C. Chuang Lawrence Livermore National Laboratory Livermore, California Introduction Aerosols influence warm clouds in two ways. First, they determine initial drop size distributions, thereby influencing the albedo of clouds. Second, they determine the lifetime of clouds, thereby possibly changing global cloud cover statistics. At the present time, neither effect of aerosols on clouds is included

  19. One ARM, Two Columns and a Whole Lot of Aerosols | Department of Energy

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    ARM, Two Columns and a Whole Lot of Aerosols One ARM, Two Columns and a Whole Lot of Aerosols July 25, 2012 - 5:49pm Addthis This observatory is part of an air particles research initiative at Cape Cod National Seashore in Massachusetts, and includes dozens of sophisticated instruments that take continuous ground-based measurements of clouds, aerosols, and other atmospheric properties. | Photo courtesy of the ARM Climate Research Facility. This observatory is part of an air particles research

  20. Investigation of Absorption Properties of Submicron Aerosol in the Troposphere Over West Siberia

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Investigation of Absorption Properties of Submicron Aerosol in the Troposphere Over West Siberia M. V. Panchenko, V. S. Kozlov, and V. P. Shmargunov Institute of Atmospheric Optics Tomsk, Russia Introduction Improving radiative climate models for the cloudless atmosphere depends largely on the correct way to simulate single-scattering albedo of atmospheric aerosol. Solving this problem requires performing detailed experiments on the study of the aerosol absorption characteristics in the

  1. Metal-supported De-NOx SCR Catalysts Prepared by Room Temperature Aerosol

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    Deposition for Potential Marine Applications | Department of Energy supported De-NOx SCR Catalysts Prepared by Room Temperature Aerosol Deposition for Potential Marine Applications Metal-supported De-NOx SCR Catalysts Prepared by Room Temperature Aerosol Deposition for Potential Marine Applications Presents preparation of SCR catalyst coatings on cost effective metallic substrates using aerosol deposition technique and their catalytic De-NOx performance PDF icon p-06_choi.pdf More Documents

  2. Following iron speciation in the early stages of magnetite magnetosome biomineralization

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Firlar, Emre; Perez-Gonzalez, Teresa; Olszewska, Agata; Faivre, Damien; Prozorov, Tanya

    2016-02-26

    Understanding magnetosome magnetite biomineralization is of fundamental interest to devising the strategies for bioinspired synthesis of magnetic materials at the nanoscale. Thus, we investigated the early stages of magnetosome formation in this work and correlated the size and emergent crystallinity of magnetosome nanoparticles with the changes in chemical environment of iron and oxygen by utilizing advanced analytical electron microscopy techniques. We observed that magnetosomes in the early stages of biomineralization with the sizes of 5–10 nm were amorphous, with a majority of iron present as Fe3+, indicative of ferric hydroxide. The magnetosomes with intermediate sizes showed partially crystalline structure withmore » a majority of iron present as Fe3+ and trace amounts of Fe2+. The fully maturated magnetosomes were indexed to magnetite. Furthermore, our approach provides spatially resolved structural and chemical information of individual magnetosomes with different particle sizes, attributed to magnetosomes at different stages of biomineralization.« less

  3. On Board, In-use Sensitivity Study of an Electrical Aerosol Detector...

    Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site

    (EAD) and Condensation Particle Counter (CPC) for Second by Second Diesel PM Measurements On Board, In-use Sensitivity Study of an Electrical Aerosol Detector (EAD) and...

  4. Assessing the Effects of Anthropogenic Aerosols on Pacific Storm Track Using a Multiscale Global Climate Model

    SciTech Connect (OSTI)

    Wang, Yuan; Wang, Minghuai; Zhang, Renyi; Ghan, Steven J.; Lin, Yun; Hu, Jiaxi; Pan, Bowen; Levy, Misti; Jiang, Jonathan; Molina, Mario J.

    2014-05-13

    Atmospheric aerosols impact weather and global general circulation by modifying cloud and precipitation processes, but the magnitude of cloud adjustment by aerosols remains poorly quantified and represents the largest uncertainty in estimated forcing of climate change. Here we assess the impacts of anthropogenic aerosols on the Pacific storm track using a multi-scale global aerosol-climate model (GCM). Simulations of two aerosol scenarios corresponding to the present day and pre-industrial conditions reveal long-range transport of anthropogenic aerosols across the north Pacific and large resulting changes in the aerosol optical depth, cloud droplet number concentration, and cloud and ice water paths. Shortwave and longwave cloud radiative forcing at the top of atmosphere are changed by - 2.5 and + 1.3 W m-2, respectively, by emission changes from pre-industrial to present day, and an increased cloud-top height indicates invigorated mid-latitude cyclones. The overall increased precipitation and poleward heat transport reflect intensification of the Pacific storm track by anthropogenic aerosols. Hence, this work provides for the first time a global perspective of the impacts of Asian pollution outflows from GCMs. Furthermore, our results suggest that the multi-scale modeling framework is essential in producing the aerosol invigoration effect of deep convective clouds on the global scale.

  5. DOE/SC-ARM-14-011 Ganges Valley Aerosol Experiment (GVAX) Final...

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    ... ISM. However, increasing aerosol concentration, air pollution, and deforestation result in changes to surface albedo and insolation, potentially leading to low monsoon rainfall. ...

  6. Large-Scale Spray Releases: Additional Aerosol Test Results

    SciTech Connect (OSTI)

    Daniel, Richard C.; Gauglitz, Phillip A.; Burns, Carolyn A.; Fountain, Matthew S.; Shimskey, Rick W.; Billing, Justin M.; Bontha, Jagannadha R.; Kurath, Dean E.; Jenks, Jeromy WJ; MacFarlan, Paul J.; Mahoney, Lenna A.

    2013-08-01

    One of the events postulated in the hazard analysis for the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak event involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids that behave as a Newtonian fluid. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and in processing facilities across the DOE complex. To expand the data set upon which the WTP accident and safety analyses were based, an aerosol spray leak testing program was conducted by Pacific Northwest National Laboratory (PNNL). PNNLs test program addressed two key technical areas to improve the WTP methodology (Larson and Allen 2010). The first technical area was to quantify the role of slurry particles in small breaches where slurry particles may plug the hole and prevent high-pressure sprays. The results from an effort to address this first technical area can be found in Mahoney et al. (2012a). The second technical area was to determine aerosol droplet size distribution and total droplet volume from prototypic breaches and fluids, including sprays from larger breaches and sprays of slurries for which literature data are mostly absent. To address the second technical area, the testing program collected aerosol generation data at two scales, commonly referred to as small-scale and large-scale testing. The small-scale testing and resultant data are described in Mahoney et al. (2012b), and the large-scale testing and resultant data are presented in Schonewill et al. (2012). In tests at both scales, simulants were used to mimic the relevant physical properties projected for actual WTP process streams.

  7. Small-Scale Spray Releases: Additional Aerosol Test Results

    SciTech Connect (OSTI)

    Schonewill, Philip P.; Gauglitz, Phillip A.; Kimura, Marcia L.; Brown, G. N.; Mahoney, Lenna A.; Tran, Diana N.; Burns, Carolyn A.; Kurath, Dean E.

    2013-08-01

    One of the events postulated in the hazard analysis at the Waste Treatment and Immobilization Plant (WTP) and other U.S. Department of Energy (DOE) nuclear facilities is a breach in process piping that produces aerosols with droplet sizes in the respirable range. The current approach for predicting the size and concentration of aerosols produced in a spray leak involves extrapolating from correlations reported in the literature. These correlations are based on results obtained from small engineered spray nozzles using pure liquids with Newtonian fluid behavior. The narrow ranges of physical properties on which the correlations are based do not cover the wide range of slurries and viscous materials that will be processed in the WTP and across processing facilities in the DOE complex. To expand the data set upon which the WTP accident and safety analyses were based, an aerosol spray leak testing program was conducted by Pacific Northwest National Laboratory (PNNL). PNNLs test program addressed two key technical areas to improve the WTP methodology (Larson and Allen 2010). The first technical area was to quantify the role of slurry particles in small breaches where slurry particles may plug the hole and prevent high-pressure sprays. The results from an effort to address this first technical area can be found in Mahoney et al. (2012a). The second technical area was to determine aerosol droplet size distribution and total droplet volume from prototypic breaches and fluids, including sprays from larger breaches and sprays of slurries for which literature data are largely absent. To address the second technical area, the testing program collected aerosol generation data at two scales, commonly referred to as small-scale and large-scale. The small-scale testing and resultant data are described in Mahoney et al. (2012b) and the large-scale testing and resultant data are presented in Schonewill et al. (2012). In tests at both scales, simulants were used to mimic the relevant physical properties projected for actual WTP process streams.

  8. Chemical process hazards analysis

    SciTech Connect (OSTI)

    1996-02-01

    The Office of Worker Health and Safety (EH-5) under the Assistant Secretary for the Environment, Safety and Health of the US Department (DOE) has published two handbooks for use by DOE contractors managing facilities and processes covered by the Occupational Safety and Health Administration (OSHA) Rule for Process Safety Management of Highly Hazardous Chemicals (29 CFR 1910.119), herein referred to as the PSM Rule. The PSM Rule contains an integrated set of chemical process safety management elements designed to prevent chemical releases that can lead to catastrophic fires, explosions, or toxic exposures. The purpose of the two handbooks, ``Process Safety Management for Highly Hazardous Chemicals`` and ``Chemical Process Hazards Analysis,`` is to facilitate implementation of the provisions of the PSM Rule within the DOE. The purpose of this handbook ``Chemical Process Hazards Analysis,`` is to facilitate, within the DOE, the performance of chemical process hazards analyses (PrHAs) as required under the PSM Rule. It provides basic information for the performance of PrHAs, and should not be considered a complete resource on PrHA methods. Likewise, to determine if a facility is covered by the PSM rule, the reader should refer to the handbook, ``Process Safety Management for Highly Hazardous Chemicals`` (DOE- HDBK-1101-96). Promulgation of the PSM Rule has heightened the awareness of chemical safety management issues within the DOE. This handbook is intended for use by DOE facilities and processes covered by the PSM rule to facilitate contractor implementation of the PrHA element of the PSM Rule. However, contractors whose facilities and processes not covered by the PSM Rule may also use this handbook as a basis for conducting process hazards analyses as part of their good management practices. This handbook explains the minimum requirements for PrHAs outlined in the PSM Rule. Nowhere have requirements been added beyond what is specifically required by the rule.

  9. Selecting chemical treatment programs

    SciTech Connect (OSTI)

    Miller, J.E. )

    1988-09-01

    Many process equipment performance and reliability problems can be solved economically by the proper selection and application of chemical treatment programs. It is important to choose an experienced chemical vendor and to work closely with the vendor to develop a good chemical treatment program. This requires devoting sufficient manpower to ensure that the treatment program development is thorough and timely. After the treatment program is installed, the system operation and performance should be routinely monitored to ensure that expected benefits are achieved and unexpected problems do not develop.

  10. The impact of biogenic carbon emissions on aerosol absorption inMexico City

    SciTech Connect (OSTI)

    Marley, N; Gaffney, J; Tackett, M J; Sturchio, N; Hearty, L; Martinez, N; Hardy, K D; Machany-Rivera, A; Guilderson, T P; MacMillan, A; Steelman, K

    2009-02-24

    In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbing secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.

  11. Quantitative study on the chemical solution deposition of zinc oxysulfide

    SciTech Connect (OSTI)

    Reinisch, Michael; Perkins, Craig L.; Steirer, K. Xerxes

    2015-11-21

    Zinc Oxysulfide (ZnOS) has demonstrated potential in the last decade to replace CdS as a buffer layer material since it is a wide-band-gap semiconductor with performance advantages over CdS (Eg = 2.4 eV) in the near UV-range for solar energy conversion. However, questions remain on the growth mechanisms of chemical bath deposited ZnOS. In this study, a detailed model is employed to calculate solubility diagrams that describe simple conditions for complex speciation control using only ammonium hydroxide without additional base. For these conditions, ZnOS is deposited via aqueous solution deposition on a quartz crystal microbalance in a continuous flow cell. Data is used to analyze the growth rate dependence on temperature and also to elucidate the effects of dimethylsulfoxide (DMSO) when used as a co-solvent. Activation energies (EA) of ZnOS are calculated for different flow rates and solution compositions. As a result, the measured EA relationships are affected by changes in the primary growth mechanism when DMSO is included.

  12. Quantitative study on the chemical solution deposition of zinc oxysulfide

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Reinisch, Michael; Perkins, Craig L.; Steirer, K. Xerxes

    2015-11-21

    Zinc Oxysulfide (ZnOS) has demonstrated potential in the last decade to replace CdS as a buffer layer material since it is a wide-band-gap semiconductor with performance advantages over CdS (Eg = 2.4 eV) in the near UV-range for solar energy conversion. However, questions remain on the growth mechanisms of chemical bath deposited ZnOS. In this study, a detailed model is employed to calculate solubility diagrams that describe simple conditions for complex speciation control using only ammonium hydroxide without additional base. For these conditions, ZnOS is deposited via aqueous solution deposition on a quartz crystal microbalance in a continuous flow cell.more » Data is used to analyze the growth rate dependence on temperature and also to elucidate the effects of dimethylsulfoxide (DMSO) when used as a co-solvent. Activation energies (EA) of ZnOS are calculated for different flow rates and solution compositions. As a result, the measured EA relationships are affected by changes in the primary growth mechanism when DMSO is included.« less

  13. Beyond single particle mass spectrometry: multidimensional characterisation of individual aerosol particles

    SciTech Connect (OSTI)

    Zelenyuk, Alla; Imre, D.

    2009-09-10

    The behavior of small aerosol particles depends on a number of their physical and chemical properties, many of which are strongly coupled. The size, internal composition, density, shape, morphology, hygroscopicity, index of refraction, activity as cloud condensation nuclei and ice nuclei, and other attributes of individual particles - all play a role in determining particle properties and their impacts. The traditional particle characterization approaches rely on separate parallel measurements that average over an ensemble of particles of different sizes and/or compositions and later attempt to draw correlations between them. As a result such studies overlook critical differences between particles and bulk and miss the fact that individual particles often exhibit major differences. Here we review the recently developed methods to simultaneously measure in-situ and in real time several of the attributes for individual particles using single particle mass spectrometer, SPLAT or its second generation SPLAT II. We also discuss novel approaches developed for classification, visualization and mining of large datasets produced by the multidimensional single particle characterization.

  14. ITP Chemicals: Chemical Bandwidth Study - Energy Analysis: A...

    Broader source: Energy.gov (indexed) [DOE]

    Ethylene Oxide, Ammonia, and Terephthalic Acid, December 2007 Bandwidth Study U.S. Chemical Manufacturing ITP Chemicals: Energy and Environmental Profile of the U.S....

  15. Implementation of equilibrium aqueous speciation and solubility (EQ3 type) calculations into Cantera for electrolyte solutions.

    SciTech Connect (OSTI)

    Moffat, Harry K.; Jove-Colon, Carlos F.

    2009-06-01

    In this report, we summarize our work on developing a production level capability for modeling brine thermodynamic properties using the open-source code Cantera. This implementation into Cantera allows for the application of chemical thermodynamics to describe the interactions between a solid and an electrolyte solution at chemical equilibrium. The formulations to evaluate the thermodynamic properties of electrolytes are based on Pitzer's model to calculate molality-based activity coefficients using a real equation-of-state (EoS) for water. In addition, the thermodynamic properties of solutes at elevated temperature and pressures are computed using the revised Helgeson-Kirkham-Flowers (HKF) EoS for ionic and neutral aqueous species. The thermodynamic data parameters for the Pitzer formulation and HKF EoS are from the thermodynamic database compilation developed for the Yucca Mountain Project (YMP) used with the computer code EQ3/6. We describe the adopted equations and their implementation within Cantera and also provide several validated examples relevant to the calculations of extensive properties of electrolyte solutions.

  16. ARM: 10-minute Raman Lidar: aerosol depolarization profiles and single layer cloud optical depths from first Turner algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    1998-03-01

    10-minute Raman Lidar: aerosol depolarization profiles and single layer cloud optical depths from first Turner algorithm

  17. ARM: 10-minute Raman Lidar: aerosol depolarization profiles and single layer cloud optical depths from first Turner algorithm

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Chitra Sivaraman; Connor Flynn

    10-minute Raman Lidar: aerosol depolarization profiles and single layer cloud optical depths from first Turner algorithm

  18. Optical Properties of Mixed Black Carbon, Inorganic and Secondary Organic Aerosols

    SciTech Connect (OSTI)

    Paulson, S E

    2012-05-30

    Summarizes the achievements of the project, which are divided into four areas: 1) Optical properties of secondary organic aerosols; 2) Development and of a polar nephelometer to measure aerosol optical properties and theoretical approaches to several optical analysis problems, 3) Studies on the accuracy of measurements of absorbing carbon by several methods, and 4) Environmental impacts of biodiesel.

  19. Carbonaceous Aerosols and Radiative Effects Study (CARES), g1-aircraft, sedlacek sp2

    DOE Data Explorer [Office of Scientific and Technical Information (OSTI)]

    Sedlacek, Art

    The primary objective of the Carbonaceous Aerosol and Radiative Effects Study (CARES) in 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume.

  20. Method and device for producing and delivering an aerosol for remote sealing and coating

    DOE Patents [OSTI]

    Modera, Mark P.; Carrie, Francois R.

    1996-01-01

    The invention is a method and device for sealing leaks remotely by means of injecting a previously prepared aerosol into the enclosure being sealed. Specifically the invention is a method and device for preparing, transporting, and depositing and solid phase aerosol to the interior surface of the enclosure.

  1. Method and device for producing and delivering an aerosol for remote sealing and coating

    DOE Patents [OSTI]

    Modera, M.P.; Carrie, F.R.

    1996-06-04

    The invention is a method and device for sealing leaks remotely by means of injecting a previously prepared aerosol into the enclosure being sealed. Specifically the invention is a method and device for preparing, transporting, and depositing and solid phase aerosol to the interior surface of the enclosure. 1 fig.

  2. Cloud/Aerosol Parameterizations: Application and Improvement of General Circulation Models

    SciTech Connect (OSTI)

    Penner, Joyce

    2012-06-30

    One of the biggest uncertainties associated with climate models and climate forcing is the treatment of aerosols and their effects on clouds. The effect of aerosols on clouds can be divided into two components: The first indirect effect is the forcing associated with increases in droplet concentrations; the second indirect effect is the forcing associated with changes in liquid water path, cloud morphology, and cloud lifetime. Both are highly uncertain. This project applied a cloud-resolving model to understand the response of clouds under a variety of conditions to changes in aerosols. These responses are categorized according to the large-scale meteorological conditions that lead to the response. Meteorological conditions were sampled from various fields, which, together with a global aerosol model determination of the change in aerosols from present day to pre-industrial conditions, was used to determine a first order estimate of the response of global cloud fields to changes in aerosols. The response of the clouds in the NCAR CAM3 GCM coupled to our global aerosol model were tested by examining whether the response is similar to that of the cloud resolving model and methods for improving the representation of clouds and cloud/aerosol interactions were examined.

  3. Carbonaceous Aerosols and Radiative Effects Study (CARES), g1-aircraft, sedlacek sp2

    SciTech Connect (OSTI)

    Sedlacek, Art

    2011-08-30

    The primary objective of the Carbonaceous Aerosol and Radiative Effects Study (CARES) in 2010 was to investigate the evolution of carbonaceous aerosols of different types and their optical and hygroscopic properties in central California, with a focus on the Sacramento urban plume.

  4. Evaluate and characterize mechanisms controlling transport, fate, and effects of army smokes in the aerosol wind tunnel: Transport, transformations, fate, and terrestrial ecological effects of hexachloroethane obscurant smokes

    SciTech Connect (OSTI)

    Cataldo, D.A.; Ligotke, M.W.; Bolton, H. Jr.; Fellows, R.J.; Van Voris, P.; McVeety, B.D.; Li, Shu-mei W.; McFadden, K.M.

    1989-09-01

    The terrestrial transport, chemical fate, and ecological effects of hexachloroethane (HC) smoke were evaluated under controlled wind tunnel conditions. The primary objectives of this research program are to characterize and assess the impacts of smoke and obscurants on: (1) natural vegetation characteristic of US Army training sites in the United States; (2) physical and chemical properties of soils representative of these training sites; and (3) soil microbiological and invertebrate communities. Impacts and dose/responses were evaluated based on exposure scenarios, including exposure duration, exposure rate, and sequential cumulative dosing. Key to understanding the environmental impacts of HC smoke/obscurants is establishing the importance of environmental parameters such as relative humidity and wind speed on airborne aerosol characteristics and deposition to receptor surfaces. Direct and indirect biotic effects were evaluated using five plant species and two soil types. HC aerosols were generated in a controlled atmosphere wind tunnel by combustion of hexachloroethane mixtures prepared to simulate normal pot burn rates and conditions. The aerosol was characterized and used to expose plant, soil, and other test systems. Particle sizes of airborne HC ranged from 1.3 to 2.1 {mu}m mass median aerodynamic diameter (MMAD), and particle size was affected by relative humidity over a range of 20% to 85%. Air concentrations employed ranged from 130 to 680 mg/m{sup 3}, depending on exposure scenario. Chlorocarbon concentrations within smokes, deposition rates for plant and soil surfaces, and persistence were determined. The fate of principal inorganic species (Zn, Al, and Cl) in a range of soils was assessed.

  5. Process Intensification - Chemical Sector Focus

    Energy Savers [EERE]

    Process Intensification - Chemical Sector Focus 1 Technology Assessment 2 Contents 3 1. Introduction ..................................................................................................................................................................... 1 4 2. Technology Assessment and Potential ................................................................................................................. 5 5 2.1 Chemical Industry Focus

  6. Collaborative research. Study of aerosol sources and processing at the GVAX Pantnagar Supersite

    SciTech Connect (OSTI)

    Worsnop, Doug; Volkamer, Rainer

    2012-08-13

    The Two Column Aerosol Project (TCAP) investigated uncertainties in the aerosol direct effect in the northern hemisphere mid-latitudes. The University of Colorado 2D-MAX-DOAS and LED-CE-DOAS instruments were collocated with DOE’s Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) and Mobile Aerosol Observing System (MAOS) during the TCAP-1 campaign at Cape Cod, MA (1 July to 13 August 2012). We have performed atmospheric radiation closure studies to evaluate the use of a novel parameter, i.e., the Raman Scattering Probability (RSP). We have performed first measurements of RSP almucantar scans, and measure RSP in spectra of scattered solar photons at 350nm and 430nm. Radiative Transfer Modelling of RSP demonstrate that the RSP measurement is maximally sensitive to infer even extremely low aerosol optical depth (AOD < 0.01) reliably by DOAS at low solar relative azimuth angles. We further assess the role of elevated aerosol layers on near surface observations of oxygen collision complexes, O 2-O2. Elevated aerosol layers modify the near surface absorption of O2-O2 and RSP. The combination of RSP and O2-O2 holds largely unexplored potential to better constrain elevated aerosol layers and measure column aerosol optical properties such as aerosol effective radius, extinction, aerosol phase functions and refractive indices. The TCAP deployment also provides a time series of reactive trace gas vertical profiles, i.e., nitrogen dioxide (NO2) and glyoxal (C2H2O2), which are measured simultaneously with the aerosol optical properties by DOAS. NO2 is an important precursor for ozone (O3) that modifies oxidative capacity. Glyoxal modifies oxidative capacity and is a source for brown carbon by forming secondary organic aerosol (SOA) via multiphase reactions in aerosol and cloud water. We have performed field measurements of these gases during TCAP, and conducted laboratory experiments to quantify for the first time the Setschenow salting constant, KS, of glyoxal in sulfate aerosols. Knowledge about KS is prerequisite to predict how increasing sulfate concentrations since pre-industrial times have modified the formation of SOA from biogenic gases in atmospheric models.

  7. Aerosol Sample Inhomogeneity with Debris from the Fukushima Daiichi Nuclear Accident

    SciTech Connect (OSTI)

    Gomez, Reynaido; Biegalski, Steven R.; Woods, Vincent T.

    2014-09-01

    Radionuclide aerosol sampling is a vital component in the detection of nuclear explosions, nuclear accidents, and other radiation releases. This was proven by the detection and tracking of emissions from the Fukushima Daiichi incident across the globe by IMS stations. Two separate aerosol samplers were operated in Richland, WA following the event and debris from the accident were measured at levels well above detection limits. While the atmospheric activity concentration of radionuclides generally compared well between the two stations, they did not agree within uncertainties. This paper includes a detailed study of the aerosol sample homogeneity of 134Cs and 137Cs, then relates it to the overall uncertainty of the original measurement. Our results show that sample inhomogeneity adds an additional 5–10% uncertainty to each aerosol measurement and that this uncertainty is in the same range as the discrepancies between the two aerosol sample measurements from Richland, WA.

  8. Electron mean free path from angle-dependent photoelectron spectroscopy of aerosol particles

    SciTech Connect (OSTI)

    Goldmann, Maximilian; Miguel-Sánchez, Javier; West, Adam H. C.; Yoder, Bruce L.; Signorell, Ruth

    2015-06-14

    We propose angle-resolved photoelectron spectroscopy of aerosol particles as an alternative way to determine the electron mean free path of low energy electrons in solid and liquid materials. The mean free path is obtained from fits of simulated photoemission images to experimental ones over a broad range of different aerosol particle sizes. The principal advantage of the aerosol approach is twofold. First, aerosol photoemission studies can be performed for many different materials, including liquids. Second, the size-dependent anisotropy of the photoelectrons can be exploited in addition to size-dependent changes in their kinetic energy. These finite size effects depend in different ways on the mean free path and thus provide more information on the mean free path than corresponding liquid jet, thin film, or bulk data. The present contribution is a proof of principle employing a simple model for the photoemission of electrons and preliminary experimental data for potassium chloride aerosol particles.

  9. Apparatus having reduced background for measuring radiation activity in aerosol particles

    DOE Patents [OSTI]

    Rodgers, John C. (Santa Fe, NM); McFarland, Andrew R. (College Station, TX); Oritz, Carlos A. (Bryan, TX); Marlow, William H. (College Station, TX)

    1992-01-01

    Apparatus having reduced background for measuring radiation activity in aerosol particles. A continuous air monitoring sampler is described for use in detecting the presence of alpha-emitting aerosol particles. An inlet fractionating screen has been demonstrated to remove about 95% of freshly formed radon progeny from the aerosol sample, and approximately 33% of partially aged progeny. Addition of an electrical condenser and a modified dichotomous virtual impactor are expected to produce considerable improvement in these numbers, the goal being to enrich the transuranic (TRU) fraction of the aerosols. This offers the possibility of improving the signal-to-noise ratio for the detected alpha-particle energy spectrum in the region of interest for detecting TRU materials associated with aerosols, thereby enhancing the performance of background-compensation algorithms for improving the quality of alarm signals intended to warn personnel of potentially harmful quantities of TRU materials in the ambient air.

  10. Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

    SciTech Connect (OSTI)

    Petäjä, T

    2013-12-01

    Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

  11. Measurement and Modeling of Vertically Resolved Aerosol Optical Properties and Radiative Fluxes Over the ARM SGP Site During the May 2003 Aerosol IOP

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Measurement and Modeling of Vertically Resolved Aerosol Optical Properties and Radiative Fluxes Over the ARM SGP Site During the May 2003 Aerosol IOP B. Schmid and J. Redemann Bay Area Environmental Research Institute National Aeronautics and Space Administration Ames Research Center Moffett Field, California W. P. Arnott Desert Research Institute Reno, Nevada A. Bucholtz and J. Reid Naval Research Laboratory Monterey, California P. Colarco Earth System Science Interdisciplinary Center

  12. Micromachined chemical jet dispenser

    DOE Patents [OSTI]

    Swierkowski, S.P.

    1999-03-02

    A dispenser is disclosed for chemical fluid samples that need to be precisely ejected in size, location, and time. The dispenser is a micro-electro-mechanical systems (MEMS) device fabricated in a bonded silicon wafer and a substrate, such as glass or silicon, using integrated circuit-like fabrication technology which is amenable to mass production. The dispensing is actuated by ultrasonic transducers that efficiently produce a pressure wave in capillaries that contain the chemicals. The 10-200 {micro}m diameter capillaries can be arranged to focus in one spot or may be arranged in a larger dense linear array (ca. 200 capillaries). The dispenser is analogous to some ink jet print heads for computer printers but the fluid is not heated, thus not damaging certain samples. Major applications are in biological sample handling and in analytical chemical procedures such as environmental sample analysis, medical lab analysis, or molecular biology chemistry experiments. 4 figs.

  13. Micromachined chemical jet dispenser

    DOE Patents [OSTI]

    Swierkowski, Steve P. (Livermore, CA)

    1999-03-02

    A dispenser for chemical fluid samples that need to be precisely ejected in size, location, and time. The dispenser is a micro-electro-mechanical systems (MEMS) device fabricated in a bonded silicon wafer and a substrate, such as glass or silicon, using integrated circuit-like fabrication technology which is amenable to mass production. The dispensing is actuated by ultrasonic transducers that efficiently produce a pressure wave in capillaries that contain the chemicals. The 10-200 .mu.m diameter capillaries can be arranged to focus in one spot or may be arranged in a larger dense linear array (.about.200 capillaries). The dispenser is analogous to some ink jet print heads for computer printers but the fluid is not heated, thus not damaging certain samples. Major applications are in biological sample handling and in analytical chemical procedures such as environmental sample analysis, medical lab analysis, or molecular biology chemistry experiments.

  14. Development of RAMS-CMAQ to Simulate Aerosol Optical Depth and Aerosol Direct Radiative Forcing and Its Application to East Asia

    SciTech Connect (OSTI)

    Han, Xiao; Zhang, Meigen; Liu, Xiaohong; Ghan, Steven J.; Xin, Jin-Yuan; Wang, Li-Li

    2009-11-16

    The air quality modeling system RAMS (Regional Atmospheric Modeling System)-CMAQ (Models-3 Community Multi-scale Air Quality) is developed to simulate the aerosol optical depth (AOD) and aerosol direct forcing (DF). The aerosol-specific extinction, single scattering albedo, and asymmetry factor are parameterized based on Mie theory taking into account the aerosol size distribution, composition, refractive index, and water uptake of solution particles. A two-stream solar radiative model considers all gaseous molecular absorption, Rayleigh scattering, and aerosols and clouds. RAMSCMAQ is applied to simulate all major aerosol concentrations (e.g., sulfate, nitrate, ammonium, organic carbon, black carbon, fine soil, and sea salt) and AOD and DF over East Asia in 2005. To evaluate its performance, the simulated AOD values were compared with ground-based in situ measurements. The comparison shows that RAMSCMAQ performed well in most of the model domain and generally captured the observed variations. High AOD values (0.2?1.0) mainly appear in the Sichuan Basin as well as in central and southeastern China. The geographic distribution of DF generally follows the AOD distribution patterns, and the DF at the top-of-the-atmosphere is less than ?25 and ?20 W m?2 in clear-sky and all-sky over the Sichuan Basin. Both AOD and DF exhibit seasonal variations with lower values in July and higher ones in January. The DF could obviously be impacted by high cloud fractions.

  15. Equilibria in Chemical Systems

    Energy Science and Technology Software Center (OSTI)

    1992-01-01

    SOLGASMIX-PV calculates equilibrium relationships in complex chemical systems. Chemical equilibrium calculations involve finding the system composition, within certain constraints, which contains the minimum free energy. The constraints are the preservation of the masses of each element present and either constant pressure or volume. SOLGASMIX-PV can calculate equilibria in systems containing a gaseous phase, condensed phase solutions, and condensed phases of invariant and variable stoichiometry. Either a constant total gas volume or a constant total pressuremore » can be assumed. Unit activities for condensed phases and ideality for solutions are assumed, although nonideal systems can be handled provided activity coefficient relationships are available.« less

  16. Results of Hg speciation testing on MCU strip effluent hold tank (SEHT) and decontaminated salt solution hold tank (DSSHT) materials

    SciTech Connect (OSTI)

    Bannochie, C. J.

    2015-09-17

    The Savannah River National Laboratory (SRNL) was tasked with preparing and shipping samples for Hg speciation by Eurofins Frontier Global Sciences, Inc. in Seattle, WA on behalf of the Savannah River Remediation (SRR) Mercury Task Team.i,ii The tenth shipment of samples was designated to include Modular Caustic Side Solvent Extraction Unit (MCU) Strip Effluent Hold Tank (SEHT) and MCU Decontaminated Salt Solution Hold Tank (DSSHT) materials from processing Salt Batch 7b. The MCU SEHT (MCU-15-722) and DSSHT (MCU-15-709) samples were pulled on June 15, 2015. All MCU samples were received at SRNL on June 16, 2015. The DSSHT sample was moved the same day to refrigeration, while the SEHT sample was placed in the Shielded Cells. On July 9, 2015 it was opened and an aliquot diluted 1:100 with Eurofins deionized water and a portion of the diluted sample transferred to a Teflon® bottle prior to moving it to refrigeration that same day. All samples were kept in the dark and refrigerated until final dilutions were prepared for shipment to Eurofins.

  17. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Atkinson, D. B.; Radney, J. G.; Lum, J.; Kolesar, K. R.; Cziczo, D. J.; Pekour, M. S.; Zhang, Q.; Setyan, A.; Zelenyuk, A.; Cappa, C. D.

    2015-04-17

    Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined heremore » as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.« less

  18. Deposition of biological aerosols on HVAC heat exchangers

    SciTech Connect (OSTI)

    Siegel, Jeffrey; Walker, Ian

    2001-09-01

    Many biologically active materials are transported as bioaerosols 1-10 {micro}m in diameter. These particles can deposit on cooling and heating coils and lead to serious indoor air quality problems. This paper investigates several of the mechanisms that lead to aerosol deposition on fin and tube heat exchangers. A model has been developed that incorporates the effects of several deposition mechanisms, including impaction, Brownian and turbulent diffusion, turbophoresis, thermophoresis, diffusiophoresis, and gravitational settling. The model is applied to a typical range of air velocities that are found in commercial and residential HVAC systems 1 - 6 m/s (200 - 1200 ft/min), particle diameters from 1 - 8 {micro}m, and fin spacings from 3.2 - 7.9 fins/cm (8 - 16 fins/inch or FPI). The results from the model are compared to results from an experimental apparatus that directly measures deposition on a 4.7 fins/cm (12 FPI) coil. The model agrees reasonably well with this measured data and suggests that cooling coils are an important sink for biological aerosols and consequently a potential source of indoor air quality problems.

  19. ARM Cloud Aerosol Precipitation Experiment (ACAPEX) Science Plan

    SciTech Connect (OSTI)

    Leung, L. R.; Prather, K.; Ralph, R.; Rosenfeld, D.; Spackman, R.; DeMott, P.; Fairall, C.; Fan, J.; Hagos, S.; Hughes, M.; Long, C.; Rutledge, S.; Waliser, D.; Wang, H.

    2014-09-01

    The western U.S. receives precipitation predominantly during the cold season when storms approach from the Pacific Ocean. The snowpack that accumulates during winter storms provides about 70-90% of water supply for the region. Understanding and modeling the fundamental processes that govern the large precipitation variability and extremes in the western U.S. is a critical test for the ability of climate models to predict the regional water cycle, including floods and droughts. Two elements of significant importance in predicting precipitation variability in the western U.S. are atmospheric rivers and aerosols. Atmospheric rivers (ARs) are narrow bands of enhanced water vapor associated with the warm sector of extratropical cyclones over the Pacific and Atlantic oceans. Because of the large lower-tropospheric water vapor content, strong atmospheric winds and neutral moist static stability, some ARs can produce heavy precipitation by orographic enhancement during landfall on the U.S. West Coast. While ARs are responsible for a large fraction of heavy precipitation in that region during winter, much of the rest of the orographic precipitation occurs in post-frontal clouds, which are typically quite shallow, with tops just high enough to pass the mountain barrier. Such clouds are inherently quite susceptible to aerosol effects on both warm rain and ice precipitation-forming processes.

  20. NETL - Chemical Looping Reactor

    SciTech Connect (OSTI)

    2013-07-24

    NETL's Chemical Looping Reactor unit is a high-temperature integrated CLC process with extensive instrumentation to improve computational simulations. A non-reacting test unit is also used to study solids flow at ambient temperature. The CLR unit circulates approximately 1,000 pounds per hour at temperatures around 1,800 degrees Fahrenheit.

  1. NETL - Chemical Looping Reactor

    ScienceCinema (OSTI)

    None

    2014-06-26

    NETL's Chemical Looping Reactor unit is a high-temperature integrated CLC process with extensive instrumentation to improve computational simulations. A non-reacting test unit is also used to study solids flow at ambient temperature. The CLR unit circulates approximately 1,000 pounds per hour at temperatures around 1,800 degrees Fahrenheit.

  2. Category:Chemical Logging | Open Energy Information

    Open Energy Info (EERE)

    Chemical Logging Jump to: navigation, search Geothermalpower.jpg Looking for the Chemical Logging page? For detailed information on Chemical Logging, click here. Category:Chemical...

  3. Chemical Supply Chain Analysis | NISAC

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    NISACCapabilitiesChemical Supply Chain Analysis content top Chemical Supply Chain Analysis NISAC has developed a range of capabilities for analyzing the consequences of disruptions to the chemical manufacturing industry. Each capability provides a different but complementary perspective on the questions of interest-questions like Given an event, will the entire chemical sector be impacted or just parts? Which chemicals, plants, and complexes could be impacted? In which regions of the country?

  4. Chemical Resources | Sample Preparation Laboratories

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Chemical Resources Chemical Inventory All Sample Preparation Labs are stocked with an assortment of common solvents, acids, bases, buffers, and other reagents. See our Chemical Inventories for a list of available reagents. If you need large quantities of any chemicals, please order or bring your own supply (see below). Chemical Inventories Standard Operating Procedures (SOPs) If you will be working with any samples or reagents that are significantly toxic, reactive, corrosive, flammable, or

  5. Development of Aerosol Models for Radiative Flux Calculations at ARM Sites

    SciTech Connect (OSTI)

    Ogren, John A.; Dutton, Ellsworth G.; McComiskey, Allison C.

    2006-09-30

    The direct radiative forcing (DRF) of aerosols, the change in net radiative flux due to aerosols in non-cloudy conditions, is an essential quantity for understanding the human impact on climate change. Our work has addressed several key issues that determine the accuracy, and identify the uncertainty, with which aerosol DRF can be modeled. These issues include the accuracy of several radiative transfer models when compared to measurements and to each other in a highly controlled closure study using data from the ARM 2003 Aerosol IOP. The primary focus of our work has been to determine an accurate approach to assigning aerosol properties appropriate for modeling over averaged periods of time and space that represent the observed regional variability of these properties. We have also undertaken a comprehensive analysis of the aerosol properties that contribute most to uncertainty in modeling aerosol DRF, and under what conditions they contribute the most uncertainty. Quantification of these issues enables the community to better state accuracies of radiative forcing calculations and to concentrate efforts in areas that will decrease uncertainties in these calculations in the future.

  6. Residence times of fine tropospheric aerosols as determined by {sup 210}Pb progeny.

    SciTech Connect (OSTI)

    Marley, N. A.; Gaffney, J. S.; Drayton, P. J.; Cunningham, M. M.; Mielcarek, C.; Ravelo, R.; Wagner, C.

    1999-10-05

    Fine tropospheric aerosols can play important roles in the radiative balance of the atmosphere. The fine aerosols can act directly to cool the atmosphere by scattering incoming solar radiation, as well as indirectly by serving as cloud condensation nuclei. Fine aerosols, particularly carbonaceous soots, can also warm the atmosphere by absorbing incoming solar radiation. In addition, aerosols smaller than 2.5 {micro}m have recently been implicated in the health effects of air pollution. Aerosol-active radioisotopes are ideal tracers for the study of atmospheric transport processes. The source terms of these radioisotopes are relatively well known, and they are removed from the atmosphere only by radioactive decay or by wet or dry deposition of the host aerosol. The progeny of the primordial radionuclide {sup 238}U are of particular importance to atmospheric studies. Uranium-238 is common throughout Earth's crust and decays to the inert gas {sup 222}Rn, which escapes into the atmosphere. Radon-222 decays by the series of alpha and beta emissions shown in Figure 1 to the long-lived {sup 210}Pb. Once formed, {sup 210}Pb becomes attached to aerosol particles with average attachment times of 40 s to 3 min.

  7. On the characteristics of aerosol indirect effect based on dynamic regimes in global climate models

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Zhang, S.; Wang, M.; Ghan, S. J.; Ding, A.; Wang, H.; Zhang, K.; Neubauer, D.; Lohmann, U.; Ferrachat, S.; Takeamura, T.; et al

    2015-09-02

    Aerosol-cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (?500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascendmore(?500 ?1) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is as large as that in stratocumulus regimes, which indicates that regimes with strong large-scale ascend are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm d?1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes than that globally, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.less

  8. Simulation of aerosol direct radiative forcing with RAMS-CMAQ in East Asia

    SciTech Connect (OSTI)

    Han, Xiao; Zhang, Meigen; Han, Zhiewi; Xin, Jin-Yuan; Liu, Xiaohong

    2011-11-14

    The air quality modeling system RAMS-CMAQ is developed to assess aerosol direct radiative forcing by linking simulated meteorological parameters and aerosol mass concentration with the aerosol optical properties/radiative transfer module in this study. The module is capable of accounting for important factors that affect aerosol optical properties and radiative effect, such as incident wave length, aerosol size distribution, water uptake, and internal mixture. Subsequently, the modeling system is applied to simulate the temporal and spatial variations in mass burden, optical properties, and direct radiative forcing of diverse aerosols, including sulfate, nitrate, ammonium, black carbon, organic carbon, dust, and sea salt over East Asia throughout 2005. Model performance is fully evaluated using various observational data, including satellite monitoring of MODIS and surface measurements of EANET (Acid Deposition Monitoring Network), AERONET (Aerosol Robotic Network), and CSHNET (Chinese Sun Hazemeter Network). The correlation coefficients of the comparisons of daily average mass concentrations of sulfate, PM2.5, and PM10 between simulations and EANET measurements are 0.70, 0.61, and 0.64, respectively. It is also determined that the modeled aerosol optical depth (AOD) is in congruence with the observed results from the AERONET, the CSHNET, and the MODIS. The model results suggest that the high AOD values ranging from 0.8 to 1.2 are mainly distributed over the Sichuan Basin as well as over central and southeastern China, in East Asia. The aerosol direct radiative forcing patterns generally followed the AOD patterns. The strongest forcing effect ranging from -12 to -8 W m-2 was mainly distributed over the Sichuan Basin and the eastern China's coastal regions in the all-sky case at TOA, and the forcing effect ranging from -8 to -4 W m-2 could be found over entire eastern China, Korea, Japan, East China Sea, and the sea areas of Japan

  9. An Observed Signature of Aerosol Effect on Cloud Droplet Radii from a

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Decade of Observations at a Mid-Continental Site An Observed Signature of Aerosol Effect on Cloud Droplet Radii from a Decade of Observations at a Mid-Continental Site Min, Qilong State University of New York at Albany Duan, Minzheng State University of New York at Albany Harrison, Lee State University of New York Joseph, Everette Howard University Category: Aerosols Continuing observations of aerosol and cloud optical property have been made using MFRSR and MWR at the ARM SGP site since

  10. ARM - Field Campaign - 2004 NEAX (Northeast Aerosol Experiment), G-1 data

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    4 NEAX (Northeast Aerosol Experiment), G-1 data ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : 2004 NEAX (Northeast Aerosol Experiment), G-1 data 2004.07.20 - 2004.08.15 Lead Scientist : Peter Daum For data sets, see below. Abstract Brookhaven National Laboratory conducted a series of aircraft flights with the DOE G-1 aircraft during the 2004 Northeast Aerosol Experiment (NEAX). The flights accomplished

  11. ARM - Field Campaign - 2006 MAX-Mex-Megacity Aerosol eXperiment - Mexico

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    City 6 MAX-Mex-Megacity Aerosol eXperiment - Mexico City ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : 2006 MAX-Mex-Megacity Aerosol eXperiment - Mexico City 2006.03.03 - 2006.03.28 Lead Scientist : Jeffrey Gaffney For data sets, see below. Abstract A 4-week field campaign was conducted in and downwind of Mexico City during March 2006. The Megacity Aerosol eXperiment - MEXico City (MAX-MEX)

  12. ARM - Field Campaign - Aerosol Life Cycle: UV-APS and Nano-SMPS

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    govCampaignsAerosol Life Cycle: UV-APS and Nano-SMPS ARM Data Discovery Browse Data Related Campaigns Aerosol Life Cycle IOP at BNL 2011.06.01, Sedlacek, OSC Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Aerosol Life Cycle: UV-APS and Nano-SMPS 2011.06.10 - 2011.06.25 Lead Scientist : Gannet Hallar For data sets, see below. Abstract Current estimates indicate that new particle formation globally account for a majority of Cloud

  13. ARM - Field Campaign - Aerosol and Cloud Experiments in the Eastern North

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Atlantic (ACE-ENA) govCampaignsAerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) Related Campaigns Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) 2017.06.01, Wang, ENA Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send Campaign : Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) 2017.06.01 - 2018.02.28 Lead Scientist : Jian Wang Abstract With their extensive coverage, low clouds

  14. Electrospray neutralization process and apparatus for generation of nano-aerosol and nano-structured materials

    DOE Patents [OSTI]

    Bailey, Charles L. (Cross Junction, VA); Morozov, Victor (Manassas, VA); Vsevolodov, Nikolai N. (Kensington, MD)

    2010-08-17

    The claimed invention describes methods and apparatuses for manufacturing nano-aerosols and nano-structured materials based on the neutralization of charged electrosprayed products with oppositely charged electrosprayed products. Electrosprayed products include molecular ions, nano-clusters and nano-fibers. Nano-aerosols can be generated when neutralization occurs in the gas phase. Neutralization of electrospan nano-fibers with molecular ions and charged nano-clusters may result in the formation of fibrous aerosols or free nano-mats. Nano-mats can also be produced on a suitable substrate, forming efficient nano-filters.

  15. Externally pressurized porous cylinder for multiple surface aerosol generation and method of generation

    DOE Patents [OSTI]

    Apel, Charles T. (Los Alamos, NM); Layman, Lawrence R. (Los Alamos, NM); Gallimore, David L. (Los Alamos, NM)

    1988-01-01

    A nebulizer for generating aerosol having small droplet sizes and high efficiency at low sample introduction rates. The nebulizer has a cylindrical gas permeable active surface. A sleeve is disposed around the cylinder and gas is provided from the sleeve to the interior of the cylinder formed by the active surface. In operation, a liquid is provided to the inside of the gas permeable surface. The gas contacts the wetted surface and forms small bubbles which burst to form an aerosol. Those bubbles which are large are carried by momentum to another part of the cylinder where they are renebulized. This process continues until the entire sample is nebulized into aerosol sized droplets.

  16. ARM - PI Product - Black Carbon aerosol mass concentration in snow and rain

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    samples over Barrow in the Arctic ProductsBlack Carbon aerosol mass concentration in snow and rain samples over Barrow in the Arctic ARM Data Discovery Browse Data Comments? We would love to hear from you! Send us a note below or call us at 1-888-ARM-DATA. Send PI Product : Black Carbon aerosol mass concentration in snow and rain samples over Barrow in the Arctic [ ARM research ] Deposition of black carbon aerosol (BC) on snow (i.e. wet deposition) is considered to lower snow albedo and

  17. Electro-Chemical Processes

    Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)

    Electro-Chemical Processes - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Fuel Cycle Defense Waste Management Programs

  18. Description and Evaluation of Tropospheric Chemistry and Aerosols in the Community Earth System Model (CESM1.2)

    SciTech Connect (OSTI)

    Tilmes, S.; Lamarque, J. -F.; Emmons, L.; Kinnison, Douglas E.; Ma, Po-Lun; Liu, Xiaohong; Ghan, Steven J.; Bardeen, C.; Arnold, S.; Deeter, M.; Vitt, Francis; Ryerson, T. B.; Elkins, J. W.; Moore, F.; Spackman, R.; Martin, M. V.

    2015-05-13

    The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric-chemistry modeling studies in the troposphere and lower stratosphere, whether with internally derived free running (FR) meteorology, or specified dynamics (SD). The main focus of this paper is to compare the performance of these configurations against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We particularly focus on comparing present-day methane lifetime estimates within the different model configurations, which range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem. We find that tropospheric surface area density is an important factor in controlling the burden of the hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of nitrogen oxides (NOx) produced from lightning production explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss, but also by transport and mixing. For future studies, we recommend the use of CAM5-chem, due to improved aerosol description and inclusion of aerosol-cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.

  19. Description and Evaluation of Tropospheric Chemistry and Aerosols in the Community Earth System Model (CESM1.2)

    SciTech Connect (OSTI)

    Tilmes, S.; Lamarque, J.-F.; Emmons, L.; Kinnison, Douglas E.; Ma, Po-Lun; Liu, Xiaohong; Ghan, Steven J.; Bardeen, C.; Arnold, S.; Deeter, M.; Vitt, Francis; Ryerson, T. B.; Elkins, J. W.; Moore, F.; Spackman, R.; Martin, M. V.

    2015-01-01

    The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric-chemistry modeling studies in the troposphere and lower stratosphere, whether with internally derived free running (FR) meteorology, or specified dynamics (SD). The main focus of this paper is to compare the performance of these configurations against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We particularly focus on comparing present-day methane lifetime estimates within the different model configurations, which range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem. We find that tropospheric surface area density is an important factor in controlling the burden of the hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of nitrogen oxides (NOx) produced from lightning production explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss, but also by transport and mixing. For future studies, we recommend the use of CAM5-chem, due to improved aerosol description and inclusion of aerosol-cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.

  20. Description and Evaluation of Tropospheric Chemistry and Aerosols in the Community Earth System Model (CESM1.2)

    DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)

    Tilmes, S.; Lamarque, J. -F.; Emmons, L.; Kinnison, Douglas E.; Ma, Po-Lun; Liu, Xiaohong; Ghan, Steven J.; Bardeen, C.; Arnold, S.; Deeter, M.; et al

    2015-05-13

    The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric-chemistry modeling studies in the troposphere and lower stratosphere, whether with internally derived “free running” (FR) meteorology, or “specified dynamics” (SD). The main focus of this paper is to compare the performance of these configurations against observations from surface, aircraft, and satellite, as well as understand the origin of the identified differences. We particularly focus on comparing present-daymore » methane lifetime estimates within the different model configurations, which range between 7.8 years in the SD configuration of CAM5-chem and 8.8 years in the FR configuration of CAM4-chem. We find that tropospheric surface area density is an important factor in controlling the burden of the hydroxyl radical (OH), which causes differences in tropical methane lifetime of about half a year between CAM4-chem and CAM5-chem. In addition, different distributions of nitrogen oxides (NOx) produced from lightning production explain about half of the difference between SD and FR model versions in both CAM4-chem and CAM5-chem. Remaining differences in the tropical OH burden are due to enhanced tropical ozone burden in SD configurations compared to the FR versions, which are not only caused by differences in chemical production or loss, but also by transport and mixing. For future studies, we recommend the use of CAM5-chem, due to improved aerosol description and inclusion of aerosol-cloud interactions. However, smaller tropospheric surface area density in the current version of CAM5-chem compared to CAM4-chem results in larger oxidizing capacity in the troposphere and therefore a shorter methane lifetime.« less