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)

    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

  2. Speciation of Fe in ambient aerosol and cloudwater

    SciTech Connect (OSTI)

    Siefert, L. [California Institute of Technology, Pasadena, CA (United States)

    1996-08-15

    Atmospheric iron (Fe) is thought to play an important role in cloudwater chemistry (e.g., S(IV) oxidation, oxidant production, etc.), and is also an important source of Fe to certain regions of the worlds oceans where Fe is believed to be a rate-limiting nutrient for primary productivity. This thesis focuses on understanding the chemistry, speciation and abundance of Fe in cloudwater and aerosol in the troposphere, through observations of Fe speciation in the cloudwater and aerosol samples collected over the continental United States and the Arabian Sea. Different chemical species of atmospheric Fe were measured in aerosol and cloudwater samples to help assess the role of Fe in cloudwater chemistry.

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

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

    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...

  4. TSNo s02-arai135528-P Microscale Arsenic (As) Chemical Speciation in Poultry Litter.

    E-Print Network [OSTI]

    Sparks, Donald L.

    TSNo s02-arai135528-P Title Microscale Arsenic (As) Chemical Speciation in Poultry Litter. abstract/litter of 14-76 mg/kg. In this study, the solid state chemical speciation of As in the poultry litter biodegradation over time. The chemical speciation of As will be further characterized using microscopic

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

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

    and Physical Characteristics of Diesel Aerosol Chemical and Physical Characteristics of Diesel Aerosol 2002 DEER Conference Presentation: University of Minnesota...

  6. 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.

  7. 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.

  8. The effects of soil type and chemical treatment on nickel speciation in refinery enriched soils

    E-Print Network [OSTI]

    The effects of soil type and chemical treatment on nickel speciation in refinery enriched soils a Rhizosphere Science Research Group, Department of Plant and Soil Sciences, N122S Agricultural Sciences North Manure and Byproducts Laboratory, Beltsville, MD 20705, USA c Environmental Soil Chemistry Research Group

  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. AEROSOLS AND CLOUDS IN CHEMICAL TRANSPORT MODELS AND CLIMATE MODELS

    E-Print Network [OSTI]

    of Earth's climate system. Clouds are highly reflective in the solar spectrum, yet strongly absorbingAEROSOLS AND CLOUDS IN CHEMICAL TRANSPORT MODELS AND CLIMATE MODELS Ulrike Lohmann1 and Stephen E Forum: Perturbed Clouds in the Climate System, Frankfurt, Germany March 2-7, 2008 Environmental Sciences

  11. 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.

  12. New Chemical Aerosol Characterization Methods- Examples Using Agricultural and Urban Airborne Particulate Matter 

    E-Print Network [OSTI]

    Zhou, Lijun

    2010-10-12

    This study explored different chemical characterization methods of agricultural and urban airborne particulate matter. Three different field campaigns are discussed. For the agricultural aerosols, measurement of the chemical ...

  13. AEROSOL CHEMICAL COMPOSITION CHARACTERIZATION AT THE ARM SOUTHERN GREAT PLAINS (SGP) SITE USING AN AEROSOL CHEMICAL

    E-Print Network [OSTI]

    ) was integrated into the Aerosol Observing System (AOS) at the Atmospheric Radiation Measurement (ARM) SGP site in Oklahoma in Nov 2010. This instrument has been measuring concentrations of sulfate, ammonium, nitrate of oxygenated OA with minor contributions from hydrocarbon-like OA, indicating that the OA at the SGP site

  14. 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.

  15. 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.

  16. SUPPLEMENTARY INFORMATION FOR:1 Chemically-Resolved Aerosol Volatility Measurements from Two Megacity Field

    E-Print Network [OSTI]

    Meskhidze, Nicholas

    SUPPLEMENTARY INFORMATION FOR:1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 Chemically-Resolved Aerosol from factor analysis of AMS spectra in several studies. 2 / 13 #12;BBOA: Biomass burning organic aerosol. In Mexico City BBOA originated mostly from wildfire and agricultural burning, but wood-fired

  17. Chemical and Physical Properties of Atmospheric Aerosols (a) A Case Study in the Unique Properties of Agricultural Aerosols (b) The Role of Chemical Composition in Ice Nucleation during the Arctic Spring 

    E-Print Network [OSTI]

    Moon, Seong-Gi

    2011-08-08

    dataset is reported for these physical and chemical properties of agricultural aerosols appropriate for use in a site-specific emission inventory. The emission rate and transport of the aerosols are also discussed. In addition, mixing ratios of total...

  18. The aging of organic aerosol in the atmosphere : chemical transformations by heterogeneous oxidation

    E-Print Network [OSTI]

    Kessler, Sean Herbert

    2013-01-01

    The immense chemical complexity of atmospheric organic particulate matter ("aerosol") has left the general field of condensed-phase atmospheric organic chemistry relatively under-developed when compared with either gas-phase ...

  19. DISSERTATION THE OPTICAL, CHEMICAL, AND PHYSICAL PROPERTIES OF AEROSOLS AND

    E-Print Network [OSTI]

    Pierce, Jeffrey

    AND GASES EMITTED BY THE LABORATORY COMBUSTION OF WILDLAND FUELS Biomass burning is a major source of trace Laboratory at Missoula Experiment. Emission factors are presented as a function of modified combustion efficiency (MCE), a measure of the fire combustion conditions. The emissions of many trace gas and aerosol

  20. Production Mechanism, Number Concentration, Size Distribution, Chemical Composition, and Optical Properties of Sea Spray Aerosols Workshop, Summer 2012

    SciTech Connect (OSTI)

    Meskhidze, Nicholas [NCSU] [NCSU

    2013-10-21

    The objective of this workshop was to address the most urgent open science questions for improved quantification of sea spray aerosol-radiation-climate interactions. Sea spray emission and its influence on global climate remains one of the most uncertain components of the aerosol-radiation-climate problem, but has received less attention than other aerosol processes (e.g. production of terrestrial secondary organic aerosols). Thus, the special emphasis was placed on the production flux of sea spray aerosol particles, their number concentration and chemical composition and properties.

  1. American Institute of Aeronautics and Astronautics Aerosol-Assisted Chemical Vapor Deposited Thin Films for

    E-Print Network [OSTI]

    Rockett, Angus

    American Institute of Aeronautics and Astronautics 1 Aerosol-Assisted Chemical Vapor Deposited Thin Aeronautics and Space Administration, John H. Glenn Research Center, Cleveland, OH 44135 Michael H.-C. Jin Sci. and Eng., 1304 West Green Street. #12;American Institute of Aeronautics and Astronautics 2 I

  2. Aerosol chemical vapor deposition of metal oxide films

    DOE Patents [OSTI]

    Ott, K.C.; Kodas, T.T.

    1994-01-11

    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 substrate.

  3. Frontiers in Assessing the Role of Chemical Speciation and Natural Attenuation on the Bioavailability

    E-Print Network [OSTI]

    Sparks, Donald L.

    on the Bioavailability of Contaminants in the Terrestrial Environment Donald L. Sparks Department ofPlant and Soil of contaminants in the terrestrial environment is greatly affected by a number of chemical factors and processes. Macroscopic kinetic studies have shown that residence time effects often occur with many metals, metalloids

  4. 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.

  5. The application of size- resolved hygroscopicity measurements to understand the physical and chemical properties of ambient aerosol 

    E-Print Network [OSTI]

    Santarpia, Joshua Lee

    2005-08-29

    -1 THE APPLICATION OF SIZE-RESOLVED HYGROSCOPICITY MEASUREMENTS TO UNDERSTANDING THE PHYSICAL AND CHEMICAL PROPERTIES OF AMBIENT AEROSOL A Dissertation by JOSHUA L. SANTARPIA Submitted to the Office of Graduate Studies of Texas A&M University in partial... OF AMBIENT AEROSOL A Dissertation by JOSHUA L. SANTARPIA Submitted to the Office of Graduate Studies of Texas A&M University in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY Approved as to style and content...

  6. 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

  7. Chemical composition of dust storms in Beijing and implications for the mixing of mineral aerosol with pollution aerosol

    E-Print Network [OSTI]

    with pollution aerosol on the pathway Yele Sun,1 Guoshun Zhuang,1,2,3 Ying Wang,1 Xiujuan Zhao,1,4 Jie Li,5 Zifa direction could be seen as the ``polluted'' pathway and the north-northwesterly direction as the relatively ``less-polluted'' one. Dust storms not only delivered large amounts of mineral elements but also carried

  8. X-RAY ABSORPTION SPECTROSCOPY FOR THE CHEMICAL CHARACTERIZATION OF ATMOSPHERIC AEROSOLS

    E-Print Network [OSTI]

    Jaklevic, J. M.

    2011-01-01

    aerosol samples and on fly ash samples obtained from powerMajor elements present in fly ash samples obtained both in-

  9. 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)

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

    2015-01-01

    Multiphase OH and O? 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 O? 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 »O? is evaluated by determining the hygroscopicity parameter, ?, as a function of particle type, mixing state, and OH/O? 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 O? exposure. Following exposure to OH, ? 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 ? was observed for pure LEV particles following OH exposure. ? 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

  10. 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, ?, 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, ? 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 ? was observed for pure LEV particles following OH exposure. ? 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

  11. 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, ?, 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, ? 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 ? was observed for pure LEV particles following OH exposure. ? 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

  12. 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.

  13. Chemical Bonding and Structural Information of Black Carbon Reference Materials and Individual Carbonaceous Atmospheric Aerosols

    E-Print Network [OSTI]

    Hopkins, Rebecca J.; Tivanski, Alexei V.; Marten, Bryan D.; Gilles, Mary K.

    2007-01-01

    A. (1998), Determination of chemical- structural changes inOptical, physical, and chemical properties of tar ballsE. (2001), Study on the chemical character of water soluble

  14. 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-François

    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.

  15. 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 1275–1935 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 0.8–1.6, 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.

  16. Laboratory investigation of chemical and physical properties of soot-containing aerosols 

    E-Print Network [OSTI]

    Zhang, Dan

    2006-08-16

    are conducted using a threewavelength Nephelometer and a multi-path extinction cell. Coating of H2SO4 is found to increase the single scattering albedo (SSA) of soot particles which has impact on the aerosol direct radiative effect. Other laboratory techniques...

  17. 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 duringmore »photo-oxidation, and the final OA OS 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

  18. REPRESENTING AEROSOL DYNAMICS AND PROPERTIES IN CHEMICAL TRANSPORT MODELS BY THE METHOD OF MOMENTS

    E-Print Network [OSTI]

    shortwave (solar) radiation, affecting climate (Charlson et al., 1992; Schwartz, 1996) and visibility this distribution and its evolution in chemical transport models. Atmospheric chemical transport models to date

  19. 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.

  20. 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 ofmore »solid 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

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

    E-Print Network [OSTI]

    Lambe, A. T.

    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 ...

  2. 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

  3. 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.

  4. 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.

  5. THE LIFETIME OF AEROSOL DROPLETS IN AMBIENT AIR: CONSIDERATION OF THE EFFECTS OF SURFACTANTS AND CHEMICAL REACTIONS

    E-Print Network [OSTI]

    Toossi, R.

    2013-01-01

    OF SURFACTANT$ AND CHEMICAL REACTIONS R. Toossi and T.Absorption of gases and chemical reactions within theno catalyst, no chemical reaction) Droplet containing l0- gr

  6. Aerosol optical properties measured on board the Ronald H. Brown during ACE-Asia as a function of aerosol chemical composition and

    E-Print Network [OSTI]

    chemical composition; number size distribution; and light scattering, hemispheric backscattering, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass: Pollution--urban and regional (0305); 0365 Atmospheric Composition and Structure: Troposphere

  7. Simulation of size-segregated aerosol chemical composition over northern Italy in clear sky and wind calm conditions

    E-Print Network [OSTI]

    Curci, Gabriele

    %, for the urban site during summer. In addition, the model is able to capture both the daily evolution of the bulk and wind calm conditions T.C. Landi a, , G. Curci b , C. Carbone a , L. Menut c , B. Bessagnet d , L-D regional chemistry-transport model (CTM) CHIMERE against observations of the size-resolved aerosol

  8. A new aerosol collector for quasi on-line analysis of particulate organic matter: the Aerosol Collection Module (ACM) and first applications with a GC/MS-FID

    E-Print Network [OSTI]

    Hohaus, T.

    In many environments organic matter significantly contributes to the composition of atmospheric aerosol particles influencing its properties. Detailed chemical characterization of ambient aerosols is critical in order to ...

  9. Nighttime chemical evolution of aerosol and trace gases in a power plant plume: Implications for secondary organic nitrate and organosulfate aerosol formation, NO? radical chemistry, and N?O? heterogeneous hydrolysis

    SciTech Connect (OSTI)

    Zaveri, Rahul A.; Berkowitz, Carl M.; Brechtel, Fred J.; Gilles, Marry K.; Hubbe, John M.; Jayne, J. T.; Kleinman, Lawrence I.; Laskin, Alexander; Madronich, Sasha; Onasch, Timothy B.; Pekour, Mikhail S.; Springston, Stephen R.; Thornton, Joel A.; Tivanski, Alexei V.; Worsnop, Douglas R.

    2010-06-22

    Chemical evolution of aerosols and trace gases in the Salem Harbor power plant plume was monitored with the DOE G-1 aircraft on the night of July 30-31, 2002. Quasi-Lagrangian sampling in the plume at increasing downwind distances/processing times was guided by a constant-volume tetroon that was released near the power plant at sunset. While no evidence of fly ash particles was found, concentrations of particulate organics, sulfate, and nitrate were higher in the plume than in the nearby background air. These species were internally mixed and the particles were acidic, suggesting that particulate nitrate was in the form of organic nitrate. The enhanced particulate organic and nitrate masses in the plume were inferred to be as secondary organic aerosol, possibly formed from the NO3 radical-initiated oxidation of isoprene and other trace organic gases in the presence of acidic sulfate particles. The enhanced particulate sulfate concentrations observed in the plume were attributed to direct emissions of gaseous SO3/H2SO4 from the power plant. Furthermore, concentration of nucleation mode particles was significantly higher in the plume than in background air, suggesting that some of the emitted H2SO4 had nucleated to form new particles. Spectromicroscopic analyses of particle samples suggested that some sulfate was likely in the form of organosulfates. Constrained Lagrangian model analysis of the aircraft and tetroon observations showed that heterogeneous hydrolysis of N2O5 was negligibly slow. These results have significant implications for several scientific and regulatory issues related to the impacts of power plant emissions on atmospheric chemistry, air quality, visibility, and climate.

  10. 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, ?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 Zdanovskii–Stokes–Robinson (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) and CCNC (Cloud Condensation Nuclei Counter) measurements.« less

  11. Composition and Reactions of Atmospheric Aerosol Particles

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

    on 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...

  12. 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

  13. New approaches for the chemical and physical characterization of aerosols using a single particle mass spectrometry based technique

    E-Print Network [OSTI]

    Spencer, Matthew Todd

    2007-01-01

    California Figure 4.6 Pie charts for the particle chemical2 Figure 2 Figure 4.6 Pie charts for the particle chemicalhave d m = 250 nm. Top pie chart contains the particle

  14. Transboundary Secondary Organic Aerosol in Western Japan: An Observed Limitation of the f44 Oxidation Indicator

    E-Print Network [OSTI]

    Irei, Satoshi; Sadanaga, Yasuhiro; Miyoshi, Takao; Arakaki, Tekemitsu; Sato, Kei; Kaneyasu, Naoki; Bandow, Hiroshi; Hatakeyama, Shiro

    2015-01-01

    To obtain evidence for secondary organic aerosol formation during the long range transport of air masses over the East China Sea, we conducted field measurements in March 2012 at the Fukue atmospheric monitoring station, Nagasaki, in western Japan. The relative abundance of m/z 44 in fine organic aerosol mass spectra (f44) was measured by an Aerodyne aerosol chemical speciation monitor. The stable carbon isotope ratio (d13C) of low volatile water soluble organic carbon (LV-WSOC) in the daily filter samples of total suspended particulate matter was also analyzed using an elemental analyzer coupled with an isotope ratio mass spectrometer. Additionally, in situ measurements of NOx and NOy were performed using NOx and NOy analyzers. The measurements showed that, unlike the systematic trends observed in a previous field study, a scatter plot for d13C of LV-WSOC versus f44 indicated a random variation. Comparison of f44 with the photochemical age estimated by the NOx to NOy ratio revealed that the f44 values distri...

  15. Marine aerosols

    E-Print Network [OSTI]

    Saltzman, ES

    2009-01-01

    proper- ties found in the marine boundary layer over theand R. E. Larson (1994), Marine boundary layer measurementsand T. Hoffmann (2002), Marine aerosol formation from

  16. Stratospheric Albedo Modification by Aerosol Injection

    E-Print Network [OSTI]

    Katz, J I

    2009-01-01

    This paper reviews and develops the proposal, widely discussed but not examined in detail, to use stratospheric aerosols to increase the Earth's albedo to Solar radiation in order to control climate change. The potential of this method has been demonstrated by the "natural experiments" of volcanic injection of sulfate aerosols into the stratosphere that led to subsequent observed global cooling. I consider several hygroscopic oxides as possible aerosol materials in addition to oxides of sulfur. Aerosol chemistry, dispersion and transport have been the subject of little study and are not understood, representing a significant scientific risk. Even the optimal altitude of injection and aerosol size distribution are poorly known. Past attention focused on guns and airplanes as means of lofting aerosols or their chemical precursors, but large sounding rockets are cheap, energetically efficient, can be designed to inject aerosols at any required altitude, and involve little technical risk. Sophisticated, mass-opti...

  17. 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.

  18. Chemistry of ?-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 ?-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

  19. Correlations in the chemical composition of rural background atmospheric aerosol in the UK determined in real time using time-of-flight mass spectrometry 

    E-Print Network [OSTI]

    Beddows, David C S; Donovan, Robert J; Harrison, Roy M; Heal, Mathew R; Kinnersley, Robert P; King, Martin; Nicholson, David; Thompson, Katherine

    2004-01-01

    polluted air mass that had passed over the British mainland before reaching Eskdalemuir, interposed between two cleaner air masses that had arrived directly from the sea. Such changes in the background aerosol could clearly be very important to studies...

  20. Detailed Chemical Characterization of Unresolved Complex Mixtures (UCM) in Atmospheric Organics: Insights into Emission Sources, Atmospheric Processing and Secondary Organic Aerosol Formation

    E-Print Network [OSTI]

    Chan, Arthur W. H.

    2014-01-01

    Detailed Chemical Characterization of Unresolved Complex1,5,6 Berkeley, CA, USA Chemical Sciences Division, LawrenceCIRES), University of NOAA Chemical Sciences Division,

  1. Thorium speciation in seawater P.H. Santschi a,*, J.W. Murray b

    E-Print Network [OSTI]

    Murray, James W.

    Thorium speciation in seawater P.H. Santschi a,*, J.W. Murray b , M. Baskaran c , C.R. Benitez October 2005 Available online 7 February 2006 Abstract Since the 1960s, thorium isotopes occupy a special of these applications are possible with little knowledge of the dissolved chemical properties of thorium, other than its

  2. Aerosol Science and Technology, 45:244261, 2011 Copyright American Association for Aerosol Research

    E-Print Network [OSTI]

    Aerosol Science and Technology, 45:244­261, 2011 Copyright © American Association for Aerosol University, Cambridge, Massachusetts, USA The hygroscopic phase transitions and growth factors of mixed chemical composition on phase transitions. The hygroscopic growth factors of the mixed particles were

  3. Modeling of gas and aerosol with WRF/Chem over Europe: Evaluation and sensitivity study

    E-Print Network [OSTI]

    Curci, Gabriele

    average temperature shows a very small negative bias, the relative humidity and the wind speed at curbside sites, 18 at near-city and urban background sites [Van Dingenen et al., 2004]. Chemical speciation

  4. 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.

  5. Density functional theory study on the interstitial chemical shifts of main-group-element centered hexazirconium halide clusters; synthetic control of speciation in [(Zr6ZCl12)] (Z = B, C)-based mixed ligand complexes 

    E-Print Network [OSTI]

    Shen, Jingyi

    2005-08-29

    The correlation between NMR chemical shifts of interstitial atoms and electronic structures of boron- and carbon-centered hexazirconium halide clusters was investigated by density functional theory (DFT) calculation. The ...

  6. Sensitivity of Tropospheric Chemical Composition to Halogen-Radical Chemistry Using a Fully Coupled Size-Resolved Multiphase Chemistry-Global Climate System: Halogen Distributions, Aerosol Composition, and Sensitivity of Climate-Relevant Gases

    SciTech Connect (OSTI)

    Long, M.; Keene, W. C.; Easter, Richard C.; Sander, Rolf; Liu, Xiaohong; Kerkweg, A.; Erickson, D.

    2014-04-07

    Observations and model studies suggest a significant but highly non-linear role for halogens, primarily Cl and Br, in multiphase atmospheric processes relevant to tropospheric chemistry and composition, aerosol evolution, radiative transfer, weather, and climate. The sensitivity of global atmospheric chemistry to the production of marine aerosol and the associated activation and cycling of inorganic Cl and Br was tested using a size-resolved multiphase coupled chemistry/global climate model (National Center for Atmospheric Research’s Community Atmosphere Model (CAM); v3.6.33). Simulation results showed strong meridional and vertical gradients in Cl and Br species. The simulation reproduced most available observations with reasonable confidence permitting the formulation of potential mechanisms for several previously unexplained halogen phenomena including the enrichment of Br- in submicron aerosol, and the presence of a BrO maximum in the polar free troposphere. However, simulated total volatile Br mixing ratios were generally high in the troposphere. Br in the stratosphere was lower than observed due to the lack of long-lived organobromine species in the simulation. Comparing simulations using chemical mechanisms with and without reactive Cl and Br species demonstrated a significant temporal and spatial sensitivity of primary atmospheric oxidants (O3, HOx, NOx), CH4, and non-methane hydrocarbons (NMHC’s) to halogen cycling. Simulated O3 and NOx were globally lower (65% and 35%, respectively, less in the planetary boundary layer based on median values) in simulations that included halogens. Globally, little impact was seen in SO2 and non-sea-salt SO42- processing due to halogens. Significant regional differences were evident: The lifetime of nss-SO42- was extended downwind of large sources of SO2. The burden and lifetime of DMS (and its oxidation products) were lower by a factor of 5 in simulations that included halogens, versus those without, leading to a 20% reduction in nss-SO42- in the southern hemisphere planetary boundary layer based on median values.

  7. Speciation of Uranium in Biologically Reduced Sediments in the...

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

    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...

  8. Phylogenetic comparative methods and the geography of speciation

    E-Print Network [OSTI]

    Losos, Jonathan B.

    Phylogenetic comparative methods and the geography of speciation Jonathan B. Losos and Richard E The geography of speciation has long been contentious. In recent years, phylogenetic approaches have been a means of settling the debate about the geography of speciation, but also indicate that sympatric

  9. 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

  10. The Role of Molecular Scale Investigations in Advanci,ng the Frontiers of Contaminant Speciation and Bioavailability in Soils

    E-Print Network [OSTI]

    Sparks, Donald L.

    Speciation and Bioavailability in Soils Donald L. Sparks* Department of Plant and Soil Sciences, University. Contamination of soils and waters with metals, oxyanions, radionuclides, nutri~nts, and organic chemicals is the focus of research in a variety of fields including soil and environmental sciences and' engineering

  11. Organic Aerosol Formation Downwind from the Deepwater Horizon Oil Spill

    E-Print Network [OSTI]

    Toohey, Darin W.

    Organic Aerosol Formation Downwind from the Deepwater Horizon Oil Spill Nicole ONeill - ATOC 3500 and aerosol composition of air over the Deepwater Horizon oil spill in the Gulf of Mexico. · The lightest chemicals in the oil evaporated within hours, as scientists expected them to do. What they didn't expect

  12. Effects of aerosols on deep convective cumulus clouds 

    E-Print Network [OSTI]

    Fan, Jiwen

    2009-05-15

    in the droplet size. Ice processes are more sensitive to the changes of aerosol chemical properties than the warm rain processes. The most noticeable effect of increasing aerosol number concentrations is an increase of CDNC and cloud water content but a decrease...

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. Persistent sensitivity of Asian aerosol to emissions of nitrogen oxides

    E-Print Network [OSTI]

    Kharol, S. K.

    We use a chemical transport model and its adjoint to examine the sensitivity of secondary inorganic aerosol formation to emissions of precursor trace gases from Asia. Sensitivity simulations indicate that secondary inorganic ...

  19. 10.13 AEROSOL CHEMICAL CHARACTERIZATION ON BOARD THE DOE G1 AIRCRAFT USING A PARTICLE-INTO-LIQUID-SAMPLER DURING THE TEXAQS 2000 EXPERIMENT

    E-Print Network [OSTI]

    NAAQS was observed. Because the Houston area has a highly concentrated petroleum and chemical industry, investigating the role industrial emissions play, in addition to that of urban emission, in O3 production.1 µM of the IC and a sample air flow rate of 5.0 L min -1 . To pump, 25 L/min Steam Heater Controller

  20. Climatic effects of 1950–2050 changes in US anthropogenic aerosols – Part 1: Aerosol trends and radiative forcing

    E-Print Network [OSTI]

    Leibensperger, Eric Michael

    We use the GEOS-Chem chemical transport model combined with the GISS general circulation model to calculate the aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950–2050 ...

  1. Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

    SciTech Connect (OSTI)

    Dr. Timothy Onasch

    2009-09-09

    This SBIR Phase I project addressed the critical need for improved characterization of carbonaceous aerosol species in the atmosphere. The proposed work focused on the development of a thermodenuder (TD) system capable of systematically measuring volatility profiles of primary and secondary organic aerosol species and providing insight into the effects of absorbing and nonabsorbing organic coatings on particle absorption properties. This work provided the fundamental framework for the generation of essential information needed for improved predictions of ambient aerosol loadings and radiative properties by atmospheric chemistry models. As part of this work, Aerodyne Research, Inc. (ARI) continued to develop and test, with the final objective of commercialization, an improved thermodenuder system that can be used in series with any aerosol instrument or suite of instruments (e.g., aerosol mass spectrometers-AMS, scanning mobility particle sizers-SMPS, photoacoustic absorption spectrometers-PAS, etc.) to obtain aerosol chemical, physical, and optical properties as a function of particle volatility. In particular, we provided the proof of concept for the direct coupling of our improved TD design with a full microphysical model to obtain volatility profiles for different organic aerosol components and to allow for meaningful comparisons between different TD-derived aerosol measurements. In a TD, particles are passed through a heated zone and a denuding (activated charcoal) zone to remove semi-volatile material. Changes in particle size, number concentration, optical absorption, and chemical composition are subsequently detected with aerosol instrumentation. The aerosol volatility profiles provided by the TD will strengthen organic aerosol emission inventories, provide further insight into secondary aerosol formation mechanisms, and provide an important measure of particle absorption (including brown carbon contributions and identification, and absorption enhancements due to coatings on soot particles). The successfully completed Phase I project included construction of a prototype design for the TD with detailed physical modeling, testing with laboratory and ambient aerosol particles, and the initiation of a detailed microphysical model of the aerosol particles passing through the TD to extract vapor pressure distributions. The objective of the microphysical model is to derive vapor pressure distributions (i.e. vapor pressure ranges, including single chemical compounds, mixtures of known compounds, and complex ‘real-world’ aerosols, such as SOA, and soot particles with absorbing and nonabsorbing coatings) from TD measurements of changes in particle size, mass, and chemical composition for known TD temperatures and flow rates (i.e. residence times). The proposed Phase II project was designed to optimize several TD systems for different instrument applications and to combine the hardware and modeling into a robust package for commercial sales.

  2. Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

    SciTech Connect (OSTI)

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2007-09-30

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  3. Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

    SciTech Connect (OSTI)

    Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

    2009-03-05

    The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

  4. 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.

  5. An Improved Equilibrium-Kinetics Speciation Algorithm For Redox...

    Open Energy Info (EERE)

    Speciation Algorithm For Redox Reactions In Variably Saturated Subsurface Flow Systems Jump to: navigation, search OpenEI Reference LibraryAdd to library Journal...

  6. 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 ?(?) at visible and near-infrared wavelengths, from which best-fit values of Ĺngström'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 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 ? versus ?(0.50 ?m) showed: (i)more »a considerable increase in ?(0.50 ?m) for the Arctic aerosol from summer to winter–spring, 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-Ĺlesund. 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 surface–atmosphere system over polar regions.« less

  7. 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 Ĺngström'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 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 ? versus ?(0.50 ?m) showed: (i) a considerable increase in ?(0.50 ?m) for the Arctic aerosol from summer to winter–spring, 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-Ĺlesund. 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 surface–atmosphere system over polar regions.

  8. Direct Speciation of Phosphorus in Alum-Amended Poultry Litter

    E-Print Network [OSTI]

    Sparks, Donald L.

    Direct Speciation of Phosphorus in Alum-Amended Poultry Litter: Solid-State 31 P NMR Investigation prerequisite for the assessment of the sustainability of intensive poultry operations. Both solid- state MAS and CP-MAS 31P NMR as well as 31P{27Al}- TRAPDOR were used to investigate P speciation in alum- amended

  9. Arsenic extraction and speciation in plants: Method comparison and development

    E-Print Network [OSTI]

    Ma, Lena

    Arsenic extraction and speciation in plants: Method comparison and development Di Zhao a , Hong T S · An optimized extraction method for As speciation in plants based on three differ- ent plants and four different methods was developed. · The optimized method was based on ethanol/water extraction and used 50% less

  10. 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.

  11. Direct Aerosol Forcing Uncertainty

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

    Mccomiskey, Allison

    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.

  12. 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.

  13. 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

  14. Role of ammonia chemistry and coarse mode aerosols in global climatological inorganic aerosol distributions

    E-Print Network [OSTI]

    Moore, Keith

    , the aerosolassociated water depends on the composition of the #12;3 particles, which is determined by gas in a three dimensional chemical transport model to understand the roles of ammonia chemistry and natural precursors among modeled aerosol species selfconsistently with ambient relative humidity and natural

  15. 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.

  16. 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

  17. 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

  18. 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

  19. 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

  20. 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 wasmore »underpredicted 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

  1. Characterising an Extractive Electrospray Ionisation (EESI) source for the online mass spectrometry analysis of organic aerosols

    E-Print Network [OSTI]

    Gallimore, Peter J.; Kalberer, Markus

    2013-05-28

    is dependent only on the mass of 23   aerosol and is independent of particle size. This again points to a mechanism where particles are fully 24   dissolved in the spray regardless of size. Large particles leave no undissolved “core”. Presumably 25   11... aerosol samples collected 8   onto filters or impactors.13 The disadvantage of offline techniques is that after an extended sample 9   collection period (typically hours) where the aerosol chemical composition may change due to 10   evaporation...

  2. RACORO aerosol data processing

    SciTech Connect (OSTI)

    Elisabeth Andrews

    2011-10-31

    The RACORO aerosol data (cloud condensation nuclei (CCN), condensation nuclei (CN) and aerosol size distributions) need further processing to be useful for model evaluation (e.g., GCM droplet nucleation parameterizations) and other investigations. These tasks include: (1) Identification and flagging of 'splash' contaminated Twin Otter aerosol data. (2) Calculation of actual supersaturation (SS) values in the two CCN columns flown on the Twin Otter. (3) Interpolation of CCN spectra from SGP and Twin Otter to 0.2% SS. (4) Process data for spatial variability studies. (5) Provide calculated light scattering from measured aerosol size distributions. Below we first briefly describe the measurements and then describe the results of several data processing tasks that which have been completed, paving the way for the scientific analyses for which the campaign was designed. The end result of this research will be several aerosol data sets which can be used to achieve some of the goals of the RACORO mission including the enhanced understanding of cloud-aerosol interactions and improved cloud simulations in climate models.

  3. SPATIO-TEMPORAL CHARACTERIZATION OF AEROSOLS THROUGH ACTIVE USE OF DATA FROM MULTIPLE SENSORS

    E-Print Network [OSTI]

    Obradovic, Zoran

    climate change related studies. In recent years remote sensing instruments of various properties have been. Aerosol concentration and chemical properties are important parameters in climate change modelsSPATIO-TEMPORAL CHARACTERIZATION OF AEROSOLS THROUGH ACTIVE USE OF DATA FROM MULTIPLE SENSORS Z

  4. On the relationship between stratospheric aerosols and nitrogen dioxide

    SciTech Connect (OSTI)

    Mills, M.J.; Langford, A.O.; O'Leary, T.J.; Arpag, K.; Miller, H.L.; Proffitt, M.H.; Sanders, R.W.; Solomon, S. (Aeronomy Laboratory, NOAA, Boulder, CO (United States) Univ. of Colorado, Boulder (United States))

    1993-06-18

    The authors report measurements of stratospheric column abundances of nitrogen dioxide above the Colorado mountains during Jan, Feb, and Mar 1992, following the arrival of the aerosol loading injected by Mt. Pinatubo. The column abundance data was correlated with concurrent lidar measurements which provided vertical aerosol profiles at the same site. Chemical reactions within polar stratospheric clouds have been shown to play a major role in ozone chemistry in the polar regions, and one could ask whether such clouds at mid latitudes could play a similar role. The sulfur dioxide loading due to the volcanic eruption provides an abrupt increase in sulfuric acid aerosol surface area in mid latitude areas, providing a convenient test of this question. Column NO[sub 2] densities are observed to fall, but also found to saturate at a certain stratospheric aerosol density.

  5. Modeling aerosols and their interactions with shallow cumuli during the 2007 CHAPS field study

    SciTech Connect (OSTI)

    Shrivastava, ManishKumar B.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Laskin, Alexander; Chapman, Elaine G.; Gustafson, William I.; Liu, Ying; Berkowitz, Carl M.

    2013-02-07

    The Weather Research and Forecasting model coupled with chemistry (WRF-Chem) is used to simulate relationships between aerosols and clouds in the vicinity of Oklahoma City during the June 2007 Cumulus Humilis Aerosol Processing Study (CHAPS). The regional scale simulation completed using 2 km horizontal grid spacing evaluates four important relationships between aerosols and shallow cumulus clouds observed during CHAPS. First, the model reproduces the trends of higher nitrate volume fractions in cloud droplet residuals compared to interstitial non-activated aerosols, as measured using the Aerosol Mass Spectrometer. Comparing simulations with cloud chemistry turned on and off, we show that nitric acid vapor uptake by cloud droplets explains the higher nitrate content of cloud droplet residuals. Second, as documented using an offline code, both aerosol water and other inorganics (OIN), which are related to dust and crustal emissions, significantly affect predicted aerosol optical properties. Reducing the OIN content of wet aerosols by 50% significantly improves agreement of model predictions with measurements of aerosol optical properties. Third, the simulated hygroscopicity of aerosols is too high as compared to their hygroscopicity derived from cloud condensation nuclei and particle size distribution measurements, indicating uncertainties associated with simulating size-dependent chemical composition and treatment of aerosol mixing state within the model. Fourth, the model reasonably represents the observations of the first aerosol indirect effect where pollutants in the vicinity of Oklahoma City increase cloud droplet number concentrations and decrease the droplet effective radius. While previous studies have often focused on cloud-aerosol interactions in stratiform and deep convective clouds, this study highlights the ability of regional-scale models to represent some of the important aspects of cloud-aerosol interactions associated with fields of short-lived shallow cumuli.

  6. Characterisation of lightly oxidised organic aerosol formed from the photochemical aging of diesel exhaust particles

    E-Print Network [OSTI]

    Kroll, Jesse

    The oxidative aging of the semivolatile fraction of diesel exhaust aerosol is studied in order to better understand the influence of oxidation reactions on particle chemical composition. Exhaust is sampled from an idling ...

  7. Investigation of the correlation between odd oxygen and secondary organic aerosol in Mexico City and Houston

    E-Print Network [OSTI]

    Wood, E. C.

    Many recent models underpredict secondary organic aerosol (SOA) particulate matter (PM) concentrations in polluted regions, indicating serious deficiencies in the models' chemical mechanisms and/or missing SOA precursors. ...

  8. A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution

    E-Print Network [OSTI]

    Donahue, Neil M.

    We discuss the use of a two-dimensional volatility-oxidation space (2-D-VBS) to describe organic-aerosol chemical evolution. The space is built around two coordinates, volatility and the degree of oxidation, both of which ...

  9. Formation of semivolatile inorganic aerosols in the Mexico City Metropolitan Area during the MILAGRO campaign

    E-Print Network [OSTI]

    Karydis, V. A.

    One of the most challenging tasks for chemical transport models (CTMs) is the prediction of the formation and partitioning of the major semi-volatile inorganic aerosol components (nitrate, chloride, ammonium) between the ...

  10. Aerosol collection characteristics of ambient aerosol samplers 

    E-Print Network [OSTI]

    Ortiz, Carlos A

    1978-01-01

    when the sampler is not in operation, both as functions of particle size and wind speed. Wind velocity was a major cause of bias for the four samplers when collecting aerosol particles & 10 um. Characteristic curves were very similar for the 0. 38 m... x 0. 38 m ( 15" x 15") Hi-Vol and the 0. 29 m x 0. 36 m (11&" x 14") Hi-Vol. At 28 um and wind speeds of 2, 8, and 24 km/hr, sampling effectiveness values respectively were 70, 43, and 43 percent for the 0. 38 m x 0. 38 m Hi-Vol and 81, 56, and 43...

  11. Impact of speciation on removal of manganese and organic matter by nanofiltration 

    E-Print Network [OSTI]

    De Munari, Annalisa; Schäfer, Andrea

    2010-01-01

    The removal of manganese and humic acid (HA) by two nanofiltration membranes, TFC-SR2 and TFC-SR3, was investigated in order to highlight the influence of speciation on manganese and HA retention. Manganese speciation ...

  12. 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.

  13. Maritime Aerosol Network as a component of Aerosol Robotic A. Smirnov,1,2

    E-Print Network [OSTI]

    Maritime Aerosol Network as a component of Aerosol Robotic Network A. Smirnov,1,2 B. N. Holben,2 I of the Maritime Aerosol Network (MAN), which has been developed as a component of the Aerosol Robotic Network), Maritime Aerosol Network as a component of Aerosol Robotic Network, J. Geophys. Res., 114, D06204, doi:10

  14. 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.

  15. 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 earth’s 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.

  16. 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

  17. 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

  18. ORIGINAL PAPER Fractionation and speciation of arsenic in fresh

    E-Print Network [OSTI]

    Hu, Qinhong "Max"

    ORIGINAL PAPER Fractionation and speciation of arsenic in fresh and combusted coal wastes from in the condensates indicates that combustion or spontaneous combustion is one of the major ways for arsenic release Coal waste Á Arsenic Á Species Á HPLC-ICP-MS Á Environmental pollution Introduction Arsenic (As

  19. 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...

  20. 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."

  1. 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."

  2. 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 9–12 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 6–12 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 abundance—in 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.

  3. Aerosol Observing System Upgraded

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 OutreachProductswsicloudwsiclouddenDVA N C E D B L O O D S TA I N P A T T E R N A NA LY S IDOE Office2 Aerosol

  4. Assessing the Influence of Secondary Organic versus Primary Carbonaceous Aerosols on Long-Range Atmospheric Polycyclic Aromatic Hydrocarbon Transport

    E-Print Network [OSTI]

    Pierce, J. R.

    We use the chemical transport model GEOS-Chem to evaluate the hypothesis that atmospheric polycyclic aromatic hydrocarbons (PAHs) are trapped in secondary organic aerosol (SOA) as it forms. We test the ability of three ...

  5. Characterisation of individual airborne particles by using aerosol time-of-flight mass spectrometry (ATOFMS) at Mace Head, Ireland, 

    E-Print Network [OSTI]

    Dall'Osto, Manuel; Beddows, David C S; Kinnersley, Robert P; Harrison, Roy M; Donovan, Robert J; Heal, Mathew R

    2004-01-01

    An aerosol time-of-flight mass spectrometer was deployed at Mace Head (Ireland) during August 2002. The measurements provide qualitative chemical composition and size distribution (0.3–3 ?m) information for single ...

  6. 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.

  7. Distribution and speciation of trace elements in iron and manganese oxide cave deposits

    SciTech Connect (OSTI)

    Frierdich, Andrew J.; Catalano, Jeffrey G. (WU)

    2012-10-24

    Fe and Mn oxide minerals control the distribution and speciation of heavy metals and trace elements in soils and aquatic systems through chemical mechanisms involving adsorption, incorporation, and electron transfer. The Pautler Cave System in Southwest Illinois, an analog to other temperate carbonate-hosted karst systems, contains Fe and Mn oxide minerals that form in multiple depositional environments and have high concentrations of associated trace elements. Synchrotron-based micro-scanning X-ray fluorescence ({mu}-SXRF) shows unique spatial distributions of Fe, Mn, and trace elements in mineral samples. Profile maps of Mn oxide cave stream pebble coatings show Fe- and As-rich laminations, indicating dynamic redox conditions in the cave stream. {mu}-SXRF maps demonstrate that Ni, Cu, and Zn correlate primarily with Mn whereas As correlates with both Mn and Fe; As is more enriched in the Fe phase. Zn is concentrated in the periphery of Mn oxide stream pebble coatings, and may be an indication of recent anthropogenic surface activity. X-ray absorption fine structure spectroscopy measurements reveal that As(V) occurs as surface complexes on Mn and Fe oxides whereas Zn(II) associated with Mn oxides is adsorbed to the basal planes of phyllomanganates in a tetrahedral coordination. Co(III) and Se(IV) are also observed to be associated with Mn oxides. The observation of Fe, Mn, and trace element banding in Mn oxide cave stream pebble coatings suggests that these materials are sensitive to and document aqueous redox conditions, similar to ferromanganese nodules in soils and in marine and freshwater sediments. Furthermore, speciation and distribution measurements indicate that these minerals scavenge trace elements and limit the transport of micronutrients and contaminants in karst aquifer systems while also potentially recording changes in anthropogenic surface activity and land-use.

  8. 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.

  9. Adaptive Speciation U. Dieckmann, M. Doebeli, J.A.J. Metz, and D. Tautz

    E-Print Network [OSTI]

    Dieckmann, Ulf

    3207, Australia Ruiz de Alarcón 13, 28014 Madrid, Spain Dock House, The Waterfront, Cape Town 8001 Processes . . . . . . . . . . . 52 4 Adaptive Dynamics of Speciation: Ecological Underpinnings 54 Stefan A

  10. 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

  11. 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

  12. 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.

  13. Aerosol penetration through transport lines 

    E-Print Network [OSTI]

    Dileep, V.R.

    1996-01-01

    It is very important to minimize the losses in aerosol transport systems for the Continuous Air Monitors (CAM) to have a prompt and a meaningful alarm and the U.S. Environmental Protection Agency (EPA) also Currently mandates continuous emissions...

  14. A Study of Cloud Processing of Organic Aerosols Using Models and CHAPS Data

    SciTech Connect (OSTI)

    Ervens, Barbara

    2012-01-17

    The main theme of our work has been the identification of parameters that mostly affect the formation and modification of aerosol particles and their interaction with water vapor. Our detailed process model studies led to simplifications/parameterizations of these effects that bridge detailed aerosol information from laboratory and field studies and the need for computationally efficient expressions in complex atmospheric models. One focus of our studies has been organic aerosol mass that is formed in the atmosphere by physical and/or chemical processes (secondary organic aerosol, SOA) and represents a large fraction of atmospheric particulate matter. Most current models only describe SOA formation by condensation of low volatility (or semivolatile) gas phase products and neglect processes in the aqueous phase of particles or cloud droplets that differently affect aerosol size and vertical distribution and chemical composition (hygroscopicity). We developed and applied models of aqueous phase SOA formation in cloud droplets and aerosol particles (aqSOA). Placing our model results into the context of laboratory, model and field studies suggests a potentially significant contribution of aqSOA to the global organic mass loading. The second focus of our work has been the analysis of ambient data of particles that might act as cloud condensation nuclei (CCN) at different locations and emission scenarios. Our model studies showed that the description of particle chemical composition and mixing state can often be greatly simplified, in particular in aged aerosol. While over the past years many CCN studies have been successful performed by using such simplified composition/mixing state assumptions, much more uncertainty exists in aerosol-cloud interactions in cold clouds (ice or mixed-phase). Therefore we extended our parcel model that describes warm cloud formation by ice microphysics and explored microphysical parameters that determine the phase state and lifetime of Arctic mixed-phase clouds.

  15. 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.

  16. 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

  17. Nanomaterials from Aerosols Aerosols are suspensions of liquid or solid particles in a gas. Aerosol particles

    E-Print Network [OSTI]

    Beaucage, Gregory

    changes which are evidenced by changes in the temperature of the oceans and rapid melting of the polar and glacial ice packs. Of pollution sources, aerosols represent the least understood and could potentially

  18. Engines of speciation: a comparative study in birds of prey O. KRU GER

    E-Print Network [OSTI]

    Krüger, Oliver

    ; (2) as sexual plumage dimorphism might be an indicator of female choice (but see Dunn et al., 2001Engines of speciation: a comparative study in birds of prey O. KRU¨ GER Department of Zoology natural selection (Darwin, 1859) and sexual selection (Darwin, 1871) can drive speciation, natural

  19. A Linear Combination Analyses Approach For Directly Speciating Ni Contaminated Soils.

    E-Print Network [OSTI]

    Sparks, Donald L.

    A Linear Combination Analyses Approach For Directly Speciating Ni Contaminated Soils. (S02-trivedi215458-Oral) Abstract: To provide an accurate description of the fate of Ni in aerial- contaminated soils to combine multiple analytical techniques to accurately determine metal speciation in complex soil systems

  20. Predictive Modeling of Mercury Speciation in Combustion Flue Gases Using GMDH-Based Abductive Networks

    E-Print Network [OSTI]

    Abdel-Aal, Radwan E.

    and boiler operating conditions. Prediction performance compares favourably with neural network models for future work to further improve performance. Index Terms: Mercury speciation, Flue gases, Boiler emissions activities are coal-fired electric utility boilers, where speciation depends on the operating conditions

  1. Speciation by monobrachial centric fusions: A test of the model using nuclear DNA sequences from the bat genus Rhogeessa

    E-Print Network [OSTI]

    Hillis, David

    Speciation by monobrachial centric fusions: A test of the model using nuclear DNA sequences from chromosomal rearrangements in a model termed speciation by monobrachial centric fusions. Recently a more comprehensive test of speciation by monobrachial centric fusions in Rhogeessa. Our analysis

  2. 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.

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

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration wouldMass map shines light on dark matter ByMentor-Protege ApplicationMercury Speciation in

  4. 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 reactor’s 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.

  5. Toxicity of atmospheric aerosols on marine phytoplankton

    E-Print Network [OSTI]

    2009-01-01

    address: Center for Atmospheric Chemistry Study, Departmenttween phytoplankton, atmospheric chemistry, and climate areno. 12 ? 4601– 4605 CHEMISTRY Atmospheric aerosol deposition

  6. 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.

  7. 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.

  8. 4, 20552088, 2004 Aerosol-ozone

    E-Print Network [OSTI]

    Boyer, Edmond

    ACPD 4, 2055­2088, 2004 Aerosol-ozone correlations during dust transport episodes P. Bonasoni et al and Physics Discussions Aerosol-ozone correlations during dust transport episodes P. Bonasoni1 , P.bonasoni@isac.cnr.it) 2055 #12;ACPD 4, 2055­2088, 2004 Aerosol-ozone correlations during dust transport episodes P. Bonasoni

  9. 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.

  10. Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area

    E-Print Network [OSTI]

    Tsimpidi, A. P.

    New primary and secondary organic aerosol modules have been added to PMCAMx, a three dimensional chemical transport model (CTM), for use with the SAPRC99 chemistry mechanism based on recent smog chamber studies. The new ...

  11. 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.

  12. 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.

  13. Reactive processing of formaldehyde and acetaldehyde in aqueous aerosol mimics: Surface tension depression and secondary organic products

    E-Print Network [OSTI]

    Li, Zhi; Sareen, Neha; McNeill, V Faye

    2011-01-01

    The reactive uptake of carbonyl-containing volatile organic compounds (cVOCs) by aqueous atmospheric aerosols is a likely source of particulate organic material. The aqueous-phase secondary organic products of some cVOCs are surface-active. Therefore, cVOC uptake can lead to organic film formation at the gas-aerosol interface and changes in aerosol surface tension. We examined the chemical reactions of two abundant cVOCs, formaldehyde and acetaldehyde, in water and aqueous ammonium sulfate (AS) solutions mimicking tropospheric aerosols. Secondary organic products were identified using Aerosol Chemical Ionization Mass Spectrometry (Aerosol-CIMS), and changes in surface tension were monitored using pendant drop tensiometry. Hemiacetal oligomers and aldol condensation products were identified using Aerosol-CIMS. A hemiacetal sulfate ester was tentatively identified in the formaldehyde-AS system. Acetaldehyde depresses surface tension to 65(\\pm2) dyn/cm in pure water and 62(\\pm1) dyn/cm in AS solutions. Surface t...

  14. 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.

  15. 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 Chemistryâ??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 Earthâ??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.

  16. Stratospheric Aerosol Geoengineering ALAN ROBOCK

    E-Print Network [OSTI]

    Robock, Alan

    hydrologic responses, whitening of the skies, reduction of solar power, and impacts of diffuse radiation Project, conducting climate model experiments with standard stratospheric aerosol in- jection scenarios, which stated that ``It is extremely likely that human in- fluence has been the dominant cause

  17. DIESEL AEROSOL SAMPLING IN THE David Kittelson, Jason Johnson, and Winthrop Watts

    E-Print Network [OSTI]

    Minnesota, University of

    chemical composition of diesel particulate matter collected in laboratory and in wind tunnel #12;In OrderDIESEL AEROSOL SAMPLING IN THE ATMOSPHERE David Kittelson, Jason Johnson, and Winthrop Watts Center for Diesel Research University of Minnesota 10th CRC ON-ROAD VEHICLE EMISSIONS WORKSHOP San Diego, California

  18. Source Characterization from Ambient Measurements of Aerosol Optical Christopher D. Cappa1

    E-Print Network [OSTI]

    a given particle absorbs or scatters light depends explicitly on the particle composition and mixing state emissions, while light scattering aerosols are produced from both primary and secondary (gas-to-particle conversion of natural and anthropogenic gaseous precursors) sources [Ghan and Schwartz, 2007]. The chemical

  19. Photochemical Aging of Secondary Organic Aerosol Particles Generated from the Oxidation of d-Limonene

    E-Print Network [OSTI]

    Nizkorodov, Sergey

    Photochemical Aging of Secondary Organic Aerosol Particles Generated from the Oxidation of d are formed, they undergo both physical and chemical aging processes, which may result in large effects to be among the primary aging mechanisms. The direct effects of solar UV-radiation on the composition

  20. 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

  1. 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

  2. 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.

  3. DO AEROSOLS CHANGE CLOUD COVER AND AFFECT CLIMATE?

    E-Print Network [OSTI]

    Schwartz, Stephen E.

    IN MEXICO CITY BASIN Light scattering by aerosols decreases absorption of solar radiation. #12;AEROSOLS;AEROSOL INFLUENCES ON CLIMATE AND CLIMATE CHANGE #12;DMS #12;AEROSOL IN MEXICO CITY BASIN #12;AEROSOL AS SEEN FROM SPACE Fire plumes from southern Mexico transported north into Gulf of Mexico. #12;CLOUD

  4. Ba and Ni speciation in a nodule of binary Mn oxide phase composition from Lake Baikal

    E-Print Network [OSTI]

    , and absorption spectroscopy. Fe is speciated as goethite, and Mn as romanechite (psilomelane) and 10 A is separated from the other type by goethite. The binary Mn oxide banding pattern is interpreted by a two

  5. 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.

  6. Impact of Two Water Management Systems on Arsenic Speciation and Microbial Populations in Rice Rhizosphere 

    E-Print Network [OSTI]

    Somenahally, Anil Kumar C.

    2012-02-14

    -1 IMPACT OF TWO WATER MANAGEMENT SYSTEMS ON ARSENIC SPECIATION AND MICROBIAL POPULATIONS IN RICE RHIZOSPHERE A Dissertation by ANIL KUMAR C. SOMENAHALLY Submitted to the Office of Graduate Studies of Texas A&M University in partial... fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY December 2010 Major Subject: Soil Science Impact of Two Water Management Systems on Arsenic Speciation and Microbial Populations...

  7. An Aerosol Condensation Model for Sulfur Trioxide

    SciTech Connect (OSTI)

    Grant, K E

    2008-02-07

    This document describes a model for condensation of sulfuric acid aerosol given an initial concentration and/or source of gaseous sulfur trioxide (e.g. fuming from oleum). The model includes the thermochemical effects on aerosol condensation and air parcel buoyancy. Condensation is assumed to occur heterogeneously onto a preexisting background aerosol distribution. The model development is both a revisiting of research initially presented at the Fall 2001 American Geophysical Union Meeting [1] and a further extension to provide new capabilities for current atmospheric dispersion modeling efforts [2]. Sulfuric acid is one of the most widely used of all industrial chemicals. In 1992, world consumption of sulfuric acid was 145 million metric tons, with 42.4 Mt (mega-tons) consumed in the United States [10]. In 2001, of 37.5 Mt consumed in the U.S., 74% went into producing phosphate fertilizers [11]. Another significant use is in mining industries. Lawuyi and Fingas [7] estimate that, in 1996, 68% of use was for fertilizers and 5.8% was for mining. They note that H{sub 2}SO{sub 4} use has been and should continue to be very stable. In the United States, the elimination of MTBE (methyl tertiary-butyl ether) and the use of ethanol for gasoline production are further increasing the demand for petroleum alkylate. Alkylate producers have a choice of either a hydrofluoric acid or sulfuric acid process. Both processes are widely used today. Concerns, however, over the safety or potential regulation of hydrofluoric acid are likely to result in most of the growth being for the sulfuric acid process, further increasing demand [11]. The implication of sulfuric acid being a pervasive industrial chemical is that transport is also pervasive. Often, this is in the form of oleum tankers, having around 30% free sulfur trioxide. Although sulfuric acid itself is not a volatile substance, fuming sulfuric acid (referred to as oleum) is [7], the volatile product being sulfur trioxide. Sulfate aerosols and mist may form in the atmosphere on tank rupture. From chemical spill data from 1990-1996, Lawuyi02 and Fingas [7] prioritize sulfuric acid as sixth most serious. During this period, they note 155 spills totaling 13 Mt, out of a supply volume of 3700 Mt. Lawuyi and Fingas [7] summarize information on three major sulfuric acid spills. On 12 February 1984, 93 tons of sulfuric acid were spilled when 14 railroad cars derailed near MacTier, Parry Sound, Ontario. On 13 December 1978, 51 railroad cars derailed near Springhill, Nova Scotia. One car, containing 93% sulfuric acid, ruptured, spilling nearly its entire contents. In July 1993, 20 to 50 tons of fuming sulfuric acid spilled at the General Chemical Corp. plant in Richmond, California, a major industrial center near San Francisco. The release occurred when oleum was being loaded into a nonfuming acid railroad tank car that contained only a rupture disk as a safety device. The tank car was overheated and this rupture disk blew. The resulting cloud of sulfuric acid drifted northeast with prevailing winds over a number of populated areas. More than 3,000 people subsequently sought medical attention for burning eyes, coughing, headaches, and nausea. Almost all were treated and released on the day of the spill. By the day after the release, another 5,000 people had sought medical attention. The spill forced the closure of five freeways in the region as well as some Bay Area Rapid Transit System stations. Apart from corrosive toxicity, there is the additional hazard that the reactions of sulfur trioxide and sulfuric acid vapors with water are extremely exothermic [10, 11]. While the vapors are intrinsically denser than air, there is thus the likelihood of strong, warming-induced buoyancy from reactions with ambient water vapor, water-containing aerosol droplets, and wet environmental surface. Nordin [12] relates just such an occurrence following the Richmond, CA spill, with the plume observed to rise to 300 m. For all practical purposes, sulfur trioxide was the constituent released from the heated tank

  8. Atmos. Chem. Phys., 15, 13311349, 2015 www.atmos-chem-phys.net/15/1331/2015/

    E-Print Network [OSTI]

    Meskhidze, Nicholas

    harvest and autumn rice harvest. An Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was deployed: hydrocarbon-like mixed with cooking-related OA (HOA + COA), fresh biomass-burning OA (BBOA), oxidized biomass

  9. Examination of the Effects of Sea Salt Aerosols on Southeast Texas Ozone and Secondary Organic Aerosol 

    E-Print Network [OSTI]

    Benoit, Mark David

    2013-02-06

    of this research is to examine sea salt aerosols and their impact on polluted environments. Sea salt aerosols act as Cloud Condensation Nuclei (CCN) as well as providing a surface for heterogeneous reactions. Such reactions have implications for trace gases...

  10. 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.

  11. Dosimeter for monitoring vapors and aerosols of organic compounds

    DOE Patents [OSTI]

    Vo-Dinh, Tuan (625 Gulfwood Rd., Knoxville, TN 37923)

    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.

  12. Chemical leukoderma

    E-Print Network [OSTI]

    O'Reilly, Kathryn E; Patel, Utpal; Chu, Julie; Patel, Rishi; Machler, Brian C

    2011-01-01

    the first report, to date, of chemical leukoderma that wasreview on biological, chemical and clinical aspects. Pigment4. Briganti S, et al. Chemical and instrumental approaches

  13. 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.

  14. Aerosol Science and Technology, 43:641652, 2009 Copyright American Association for Aerosol Research

    E-Print Network [OSTI]

    Aerosol Science and Technology, 43:641­652, 2009 Copyright © American Association for Aerosol Differential Mobility Analyzer for Measurement of the Irreversibility of the Hygroscopic Growth Factor T is the irreversibility of the hygroscopic growth fac- tor of aerosol particles. The instrument uses the hysteresis

  15. Shortwave aerosol radiative forcing over cloud-free oceans from Terra: 1. Angular models for aerosols

    E-Print Network [OSTI]

    Christopher, Sundar A.

    Sensor Microwave Imager (SSM/I) data to obtain near surface wind speed. The new aerosol ADMs are built to obtain aerosol properties within a Clouds and Earth Radiant Energy System (CERES) footprint and Special as functions of near-surface ocean wind speed and MODIS aerosol optical depth at 0.55 mm (t0.55). Among the new

  16. Researchers Model Impact of Aerosols Over California

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

    Impact of Aerosols Over California Research may clarify the effectiveness of regional pollution controls May 28, 2013 | Tags: Climate Research, Hopper Contact: Linda Vu,...

  17. Aerosol Retrieval Using Remote-sensed Observations

    E-Print Network [OSTI]

    Wang, Yueqing

    2012-01-01

    4.1.2 Baltimore and the DRAGONaround Baltimore . . . . . . . . . . . . . . . . . . . 4.1.4component aerosol 1 for Baltimore-Washington region on June

  18. Composition and Reactions of Atmospheric Aerosol Particles

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

    they can have either cooling or warming effects. Lighter-colored organic carbon particles cool regions of the planet by scattering sunlight back into space. Other aerosol particles...

  19. 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)

  20. Abstract Analytical techniques used to examine the chemical speciation of multiple trace elements are impor-

    E-Print Network [OSTI]

    Hopkins, William A.

    a largemouth bass (Micropterus salmoides) collected from a coal fly ash basin and results were compared disposal method for coal fly ash is deposition and gravitational settling in aquatic settling basins. Fly elements in fish, amphibians and reptiles in- habiting fly ash settling basins [3, 4, 5, 6]. Additionally

  1. Extending the physicochemical characterization of aerosol particles in California

    E-Print Network [OSTI]

    Zauscher, Melanie Dorothy

    2012-01-01

    Combustion Aerosol, Atmospheric Chemistry and Physics, 11 (Based Receptor Modeling, Atmospheric Chemistry and Physics,Aerosols, Journal of Atmospheric Chemistry, 22 (1-2), 19-39.

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

    Energy Savers [EERE]

    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...

  3. 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.

  4. 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,...

  5. 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.

  6. How Physical and Chemical Properties Change Ice Nucleation Efficiency of Soot and Polyaromatic Hydrocarbon Particles 

    E-Print Network [OSTI]

    Suter, Katie Ann

    2012-10-19

    freezing. The mechanism by which this freezing occurs depends on the ambient conditions and composition of the IN. Aerosol properties change through chemical aging and reactions with atmospheric oxidants such as ozone. We have conducted a series...

  7. Chemical and Physical Investigation of Secondary Organic Aerosol Formation

    E-Print Network [OSTI]

    Nakao, Shunsuke

    2012-01-01

    Saunders, R. W. : Atmospheric Chemistry of Iodine, Chemicalmodelling: a review, Atmospheric Chemistry and Physics, 5,emerging issues, Atmospheric Chemistry and Physics, 9, 5155-

  8. Chemical and Physical Investigation of Secondary Organic Aerosol Formation

    E-Print Network [OSTI]

    Nakao, Shunsuke

    2012-01-01

    from the photooxidation of isoprene, 1,3-butadiene, and2,3-dimethyl-1,3- butadiene under high NOx conditions,and 2,3-dimethyl-1,3-butadiene) was investigated under high

  9. Chemical Composition and Cloud Nucleation Ability of Marine Aerosol 

    E-Print Network [OSTI]

    Deng, Chunhua

    2013-12-12

    ) concentration, particle size distribution, as well as surface seawater and atmospheric DMS concentrations were performed simultaneously during the cruise. HYSPLIT back trajectories were used to classify air mass origins. Even though continental sources increased...

  10. Chemical and Physical Investigation of Secondary Organic Aerosol Formation

    E-Print Network [OSTI]

    Nakao, Shunsuke

    2012-01-01

    from the photooxidation of isoprene, 1,3-butadiene, and 2,3-dimethyl-1,3- butadiene under high NOx conditions, Atmos.and 2,3-dimethyl-1,3-butadiene) was investigated under high

  11. 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.

  12. 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.

  13. Spectro-Microscopic Measurements of Carbonaceous Aerosol Aging in Central California

    SciTech Connect (OSTI)

    Moffet, Ryan C.; Rodel, Tobias; Kelly, Stephen T.; Yu, Xiao-Ying; Carroll, Gregory; Fast, Jerome D.; Zaveri, Rahul A.; Laskin, Alexander; Gilles, Mary K.

    2013-10-29

    Carbonaceous aerosols are responsible for large uncertainties in climate models, degraded visibility, and adverse health effects. The Carbonaceous Aerosols and Radiative Effects Study (CARES) was designed to study carbonaceous aerosols in the natural environment of Central Valley, California, and learn more about their atmospheric formation and aging. This paper presents results from spectro-microscopic measurements of carbonaceous particles collected during CARES at the time of pollution accumulation event (June 27-29, 2010), when in situ measurements indicated an increase in the organic carbon content of aerosols as the Sacramento urban plume aged. Computer controlled scanning electron microscopy coupled with an energy dispersive X-ray detector (CCSEM/EDX) and scanning transmission X-ray microscopy coupled with near edge X-ray absorption spectroscopy (STXM/NEXAFS) were used to probe the chemical composition and morphology of individual particles. It was found that the mass of organic carbon on individual particles increased through condensation of secondary organic aerosol. STXM/NEXAFS indicated that the number fraction of homogenous organic particles lacking inorganic inclusions (greater than ~50 nm diameter) increased with plume age as did the organic mass per particle. Comparison of the CARES spectro-microscopic data set with a similar dataset obtained in Mexico City during the MILAGRO campaign showed that individual particles in Mexico City contained twice as much carbon as those sampled during CARES. The number fraction of soot particles at the Mexico City urban site (30%) was larger than at the CARES urban site (10%) and the most aged samples from CARES contained less carbon-carbon double bonds. Differences between carbonaceous particles in Mexico City and California result from different sources, photochemical conditions, gas phase reactants, and secondary organic aerosol precursors. The detailed results provided by these spectro-microscopic measurements will allow for a comprehensive evaluation of aerosol process models used in climate research.

  14. The application of a chemical equilibrium model, SOLTEQ, to predict the chemical speciations in stabilized/solidified waste forms 

    E-Print Network [OSTI]

    Park, Joo-Yang

    1994-01-01

    Oz. CaCO, . 11HzO m 6Ca" + 2A)(OH)4+ 3SO4 + 4OH + 26HzO xCaO. SiOz. xHzO+ HzO ~ xCa' + HzSi04 + (2x-1)OH -5. 19 -43. 94 +0. 36 -4. 58 -27. 49 -23. 13 + 0. 40 -29. 25 +0, 5 -19. 90 Equation [2. 16] -5. 19 -43. 13 -4. 58 -19. 95 -27. 62..., ~?, ) Belite (D~n?) Aluminate (D. n?) Ferrite (DI, ?. ) Na20 fraction K20 fraction 0. 44 0. 29 0. 17 0. 41 0. 36 0. 27 0. 03 0. 03 The volume of porewater per unit cement mass is equal to that of the mixing water less that taken up by the hydration...

  15. 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 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

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

    SciTech Connect (OSTI)

    Frossard, Amanda A. [Univ. of California, San Diego, CA (United States). Scripps Inst. of Oceanography; Russell, Lynn M. [Univ. of California, San Diego, CA (United States). Scripps Inst. of Oceanography; Burrows, Susannah M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC); Elliott, Scott M. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Bates, Timothy S. [National Oceanic and Atmospheric Administration (NOAA), Seattle, WA (United States). Pacific Marine Environmental Lab. (PMEL); Quinn, Patricia K. [National Oceanic and Atmospheric Administration (NOAA), Seattle, WA (United States). Pacific Marine Environmental Lab. (PMEL)

    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 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

  17. 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.

  18. Carbonaceous Aerosol Study Using Advanced Particle Instrumentation

    E-Print Network [OSTI]

    Qi, Li

    2010-01-01

    6 6.1 Introduction Biomass combustion emissions contributeEmissions of trace gases and aerosols during the open combustion of biomassbiomass burning work explored the evolution of organic aerosol emissions as a function of modified combustion efficiency with correlations drawn between levoglucosan emissions

  19. Optimal Estimation Retrieval Aerosol Microphysical Properties

    E-Print Network [OSTI]

    Oxford, University of

    ) the validation of this algorithm on the basis of synthetic extinction data, and (3) application of the new algorithm to SAGE II measurements of stratospheric background aerosol. The validation results indicate that the new method is able to retrieve the particle size of typical background aerosols reasonably well

  20. Atmospheric aerosol light scattering and polarization peculiarities

    E-Print Network [OSTI]

    Patlashenko, Zh I

    2015-01-01

    This paper considers environmental problems of natural and anthropogenic atmospheric aerosol pollution and its global and regional monitoring. Efficient aerosol investigations may be achieved by spectropolarimetric measurements. Specifically second and fourth Stokes parameters spectral dependencies carry information on averaged refraction and absorption indexes and on particles size distribution functions characteristics.

  1. Chemical Composition of Gas-Phase Organic Carbon Emissions from Motor Vehicles and Implications for Ozone Production

    E-Print Network [OSTI]

    Goldstein, Allen

    Chemical Composition of Gas-Phase Organic Carbon Emissions from Motor Vehicles and Implications gasoline and diesel vehicles via two methods. First we use speciated measurements of exhaust emissions from-based, single vehicle dynamometer testing, and on-road measurements in roadway tunnels.3-12 Emission factors

  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. ARM Cloud Aerosol Precipitation Experiment

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity ofkandz-cm11 OutreachProductswsicloudwsicloudden Documentation Data Management Facility PlotsProducts (VAP) VAP38 ARM6Aerosol

  4. AEROSOL ABSORPTION IN CLOUDY SCENES USING PASSIVE SATELLITE INSTRUMENTS

    E-Print Network [OSTI]

    Graaf, Martin de

    AEROSOL ABSORPTION IN CLOUDY SCENES USING PASSIVE SATELLITE INSTRUMENTS M. de Graaf, L.G. Tilstra information has become available from active space-based sensors and some dedicated field campaigns on aerosol-absorption, is the Absorbing Aerosol Index (AAI), which can indicate absorbing aerosols overlying clouds. The AAI is available

  5. 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.

  6. Studying trends in biomass burning aerosol using the Absorbing Aerosol Index derived from GOME, SCIAMACHY, and GOME-2

    E-Print Network [OSTI]

    Tilstra, Gijsbert

    Studying trends in biomass burning aerosol using the Absorbing Aerosol Index derived from GOME the resulting time series, we use tropospheric NO2 data as a reference in the regions dominated by biomass sensitive to desert dust aerosols (DDA) and biomass burning aerosols (BBA). See Figure 1. The AAI

  7. 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.

  8. Kinetics of aluminum hydrolysis: speciation and coagulation at pH 8 

    E-Print Network [OSTI]

    McEwen, John Brock

    1984-01-01

    KINETICS OF ALUMINUM HYDROLYSIS: SPECIATION AND COAGULATION AT pH 8 A Thesis by JOHN BROCK McEWEN Submitted to the Graduate College of Texas AaM University in partial fulfillment of the requirement for the degree of MASTER OF SCIENCE... December 1984 Major Subject: Civil Engineering KINETICS OP ALUMINUM HYDROLYSIS: SPECIATION AND COAGULATION AT pH 8 A Thesis by JOHN BROCK McEWEN Approved as to style and content by: Bi I Batchelor (Chairman of Committee) Steven C. apra (Member...

  9. 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.

  10. Airborne measurement of inorganic ionic components of fine aerosol particles using the particle-into-liquid sampler coupled to ion

    E-Print Network [OSTI]

    many important roles in the environment, including visibility, Earth radiation budget and human health on board the NCAR C130 and NASA P-3B aircraft during the 2001 Aerosol Characterization Experiment (ACE)-Asia and the Transport and Chemical Evolution over the Pacific (TRACE-P) experiments, respectively. Concentrations of NH4

  11. Direct observations of N2O5 reactivity on ambient aerosol particles Timothy H. Bertram,1,2

    E-Print Network [OSTI]

    aerosol flow reactor coupled to a custom-built chemical ionization mass spectrometer at two urban currently implemented large-scale model parameterizations would predict. Such discrepancies have likely and thus accurate description of the processes that remove NOx radicals is critical for predicting the down-wind

  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. Group Report: Connections between Aerosol Properties

    E-Print Network [OSTI]

    effect and causes surface warming. Absorption of solar or thermal radiation within the atmospheric column-influencing constituents (such as green- house gases) by this process, anthropogenic aerosols can contribute to climate

  14. Aerosol Condensational Growth in Cloud Formation 

    E-Print Network [OSTI]

    Geng, Jun

    2010-10-12

    A code for the quasi-stationary solution of the coupled heat and mass transport equations for aerosols in a finite volume was developed. Both mass and heat are conserved effectively in the volume, which results in a ...

  15. 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.

  16. 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.

  17. Development of plutonium aerosol fractionation system 

    E-Print Network [OSTI]

    Mekala, Malla R.

    1993-01-01

    DEVELOPMENT OF A PLUTONIUM AEROSOL FRACTIONATION SYSTEM A Thesis by MALLA R. MEKALA Submitted to the Office of Graduate Studies of Texas A&M University in partial fulfillment of the requirements for the degree of MASTER OF SCIENCE August... 1993 Major Subject: Mechanical Engineering DEVELOPMENT OP A PLUTONIUM AEROSOL FRACTIONATION SYSTEM A Thesis by MALLA R. MEKALA Approved as to style and content by: A. R. McFarland (Chair of Committee) N. K. Anand (Mer toer) (', & C. B...

  18. Speciation and distribution of arsenic and localization of nutrients in rice grains

    SciTech Connect (OSTI)

    Lombi, E.; Scheckel, K.G.; Pallon, J.; Carey, A.M.; Zhu, Y.G.; Meharg, A.A. (EPA); (UCopenhagen); (Aberdeen); (Lund); (Chinese Aca. Sci.)

    2012-09-05

    Arsenic (As) contamination of rice grains and the generally low concentration of micronutrients in rice have been recognized as a major concern for human health. Here, we investigated the speciation and localization of As and the distribution of (micro)nutrients in rice grains because these are key factors controlling bioavailability of nutrients and contaminants. Bulk total and speciation analyses using high-pressure liquid chromatography (HPLC)-inductively coupled plasma mass spectrometry (ICP-MS) and X-ray absorption near-edge spectroscopy (XANES) was complemented by spatially resolved microspectroscopic techniques ({mu}-XANES, {mu}-X-ray fluorescence ({mu}-XRF) and particle induced X-ray emission (PIXE)) to investigate both speciation and distribution of As and localization of nutrients in situ. The distribution of As and micronutrients varied between the various parts of the grains (husk, bran and endosperm) and was characterized by element-specific distribution patterns. The speciation of As in bran and endosperm was dominated by As(III)-thiol complexes. The results indicate that the translocation from the maternal to filial tissues may be a bottleneck for As accumulation in the grain. Strong similarities between the distribution of iron (Fe), manganese (Mn) and phosphorus (P) and between zinc (Zn) and sulphur (S) may be indicative of complexation mechanisms in rice grains.

  19. Speciation and transport of anthropogenic 129Iodine and natural 127Iodine in surface and subsurface environments 

    E-Print Network [OSTI]

    Schwehr, Kathleen Ann

    2005-02-17

    ................................... 29 2.2 Mobile phase gradient elution profile ........................................................ 30 2.3 Iodine speciation in the vertical profile of a warm core ring, Gulf of Mexico, 26o 0.04? N, 95o 20? W. Collection was July 9...

  20. The Fitzcarrald Arch: A Vicariant Event for Chaetostoma (Siluriformes: Loricariidae) Speciation?

    E-Print Network [OSTI]

    Strauss, Richard E.

    if the lifting of the Fitzcarrald Arch, 4 Ma, triggered speciation between the disjunct populations of Chaetostoma lineopunctatum in two isolated river drainages: the Ri´o Ucayali and the Ri´o Madre de Dios. We. lineopunctatum from four river systems, three of which drain into the Ri´o Ucayali drainage, including the type

  1. The Fitzcarrald Arch: A Vicariant Event for Chaetostoma (Siluriformes: Loricariidae) Speciation?

    E-Print Network [OSTI]

    Baker, Robert J.

    a single river system. Our aim was to determine if the lifting of the Fitzcarrald Arch, 4 Ma, triggered speciation between the disjunct populations of Chaetostoma lineopunctatum in two isolated river drainages into the Ri´o Ucayali drainage, including the type locality for the species, and one river system which drains

  2. Multivariate spatial-temporal modeling and prediction of speciated fine particles 1

    E-Print Network [OSTI]

    Reich, Brian J.

    framework to speciated PM2.5 data in the United States for the year 2004. Key words: Air pollution; Bayesian.5) is an atmospheric pollutant that has been linked to serious health problems, including mortality. PM2.5 has five-temporal epidemiological stud- ies of the association of these pollutants and adverse health effects. We introduce

  3. SEASONAL MIGRATION, SPECIATION, AND MORPHOLOGICAL CONVERGENCE IN THE GENUS CATHARUS (TURDIDAE)

    E-Print Network [OSTI]

    Winker, Kevin

    of North American bird species north of Mexico are Nearctic­Neotropic migrants, migrating seasonally1052 SEASONAL MIGRATION, SPECIATION, AND MORPHOLOGICAL CONVERGENCE IN THE GENUS CATHARUS (TURDIDAE effects of seasonal migration on evolutionary change within lin- eages is poorly understood, in terms

  4. The Fate and Speciation of Arsenic in Soils and Poultry Production Systems

    E-Print Network [OSTI]

    Sparks, Donald L.

    The Fate and Speciation of Arsenic in Soils and Poultry Production Systems by: Jennifer Seiter Environmental Soil Chemistry Group University of Delaware Advisor: Dr. Donald L. Sparks Committee Members: Dr in soil environments. One source of As in Delaware soils is the incorporation of poultry litter

  5. Elucidating cadmium speciation and bioavailability in Thai paddy soils Saengdao Khaokaew1

    E-Print Network [OSTI]

    Sparks, Donald L.

    Elucidating cadmium speciation and bioavailability in Thai paddy soils GEOC 55 Saengdao Khaokaew1 Sparks, dlsparks@udel.edu1 . (1) Department of Plant and Soil Sciences and the Center for Critical Zone Research, University of Delaware, Newark, DE 19716, (2) Department of Soil Science, Kasetsart University

  6. In-situ metal speciation in soils using synchrotron based techniques David McNear1

    E-Print Network [OSTI]

    Sparks, Donald L.

    In-situ metal speciation in soils using synchrotron based techniques David McNear1 , Markus Gräfe1 remediation and legislative strategies. To provide an accurate description of the fate of metal contaminants the physicochemical properties of the contaminating heavy metals, is a valuable alternative for more expensive

  7. Quantification of water content and speciation in natural silicic glasses (phonolite, dacite, rhyolite) by

    E-Print Network [OSTI]

    Quantification of water content and speciation in natural silicic glasses (phonolite, dacite Sciences de la Terre d'Orléans, CNRS-UO, Orléans, France Abstract The determination of total water content dissolved water content and height or area of the H2OT Raman band. Accuracy of deconvolution procedure

  8. 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.

  9. 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 Earth’s 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.

  10. Aerosol analysis for the regional air pollution study. Final report

    SciTech Connect (OSTI)

    Jaklevic, J.M.; Gatti, R.C.; Goulding, F.S.; Loo, B.W.; Thompson, A.C.

    1980-05-01

    The design and operation of an aerosol sampling and analysis program implemented during the 1975 to 1977 St. Louis Regional Air Pollution Study is described. A network of ten samplers were operated at selected sites in the St. Louis area and the total mass and elemental composition of the collected particulates were determined. Sampling periods of 2 to 24 hours were employed. The samplers were capable of collecting aerosol particles in two distinct size ranges corresponding to fine (< 2.4 ..mu..m diameter) and coarse (> 2.4 ..mu..m diameter) particles. This unique feature allowed the separation of the particulate samples into two distinct fractions with differing chemical origins and health effects. The analysis methods were also newly developed for use in the St. Louis RAPS study. Total particulate mass was measured by a beta-particle attenuation method in which a precision of +- 5 ..mu..m/cm/sup 2/ could be obtained in a one minute measurement time. Elemental compositions of the samples were determined using an energy dispersive x-ray fluorescence method in which detectable limits of 5 ng/cm/sup 2/ or less were routinely achieved for elements ranging in atomic number from Al to Pb. The advantages of these analytical methods over more conventional techniques arise from the ability to automate the measurements. During the course of the two year study, a total of more than 35,000 individual samples were processed and a total of 28 concentrations measured for each sample.

  11. Aerosol-cloud radiative effects from passive satellite instruments Mar%n de Graaf

    E-Print Network [OSTI]

    Graaf, Martin de

    Satellite measurements of absorbing aerosols Reflectance Difference Method Cloud modelling Results Outlook Aerosol-Radiation Interac. Aerosol-Cloud Interac. Total anthropogenic Solar irradiance #12;Absorbing aerosols: SCIAMACHY Results Outlook #12;SCIAMACHY on ESA's Environmetal Satellite: ENVISAT Polar orbi

  12. Relative humidity and its effect on aerosol optical depth in the vicinity of convective clouds

    E-Print Network [OSTI]

    Altaratz, O

    The hygroscopic growth of aerosols is controlled by the relative humidity (RH) and changes the aerosols' physical and hence optical properties. Observational studies of aerosol–cloud interactions evaluate the aerosol ...

  13. 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.

  14. Aerosol Science and Technology, 48:803812, 2014 Copyright C American Association for Aerosol Research

    E-Print Network [OSTI]

    Aerosol Science and Technology, 48:803­812, 2014 Copyright C American Association for Aerosol of particle growth in the atmosphere, and many properties of the resulting mixed particles depend on organic. In this article, analytic equations are derived p(;d) for condensational growth in a continuously mixed flow

  15. Aerosol Science and Technology, 38:12061222, 2004 Copyright c American Association for Aerosol Research

    E-Print Network [OSTI]

    Jimenez, Jose-Luis

    to Combustion-Generated Soot Aerosols as a Function of Fuel Equivalence Ratio Jay G. Slowik,1 K. Stainken,1 Paul factor, size, and fractal dimension of soot aerosol particles generated in a propane/O2 flame were on the fuel equivalence ratio. Type 1: for propane/O2), dva was nearly constant and independent

  16. 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.

  17. 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.

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

    DOE Patents [OSTI]

    Krauter, Paula (Livermore, CA); Zalk, David (San Jose, CA); Hoffman, D. Mark (Livermore, CA)

    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.

  19. 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.

  20. 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-129’s 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.

  1. 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).

  2. 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.

  3. 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.

  4. 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 Center’s 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.

  5. 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 Ĺngström 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 Ĺngström 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

  6. Published: November 03, 2011 r 2011 American Chemical Society 1196 dx.doi.org/10.1021/ac201338x |Anal. Chem. 2012, 84, 11961201

    E-Print Network [OSTI]

    materials where road dust and black carbon soot are the most common. Secondary organic aerosols (SOA is that these aerosols contain a high mass fraction (10Ŕ90%) of organic compounds.3,4 In addition to chemical composition such as smoking, cooking activities, and burning food are significant sources of indoor particles as are particles

  7. Speciation of Lead in a Mixed Soil Component System Using X-ray Absorption Fine Structure Spectroscopy

    E-Print Network [OSTI]

    Sparks, Donald L.

    Speciation of Lead in a Mixed Soil Component System Using X-ray Absorption Fine Structure (XAFS). Lead concentrations of 6000, 18000, and 29000 µg Pb/g solid were reacted with soil components

  8. Do geological or climatic processes drive speciation in dynamic archipelagos? The tempo and mode of diversification in Southeast Asian shrews

    E-Print Network [OSTI]

    Esselstyn, Jacob Aaron; Timm, Robert M.; Brown, Rafe M.

    2009-10-01

    Geological and climatic processes potentially alter speciation rates by generating and modifying barriers to dispersal. In Southeast Asia, two processes have substantially altered the distribution of land. Volcanic uplift ...

  9. The Genetic Architecture of Ecological Speciation and the Association with Signatures of Selection in Natural Lake Whitefish (Coregonus sp. Salmonidae)

    E-Print Network [OSTI]

    Bernatchez, Louis

    The Genetic Architecture of Ecological Speciation and the Association with Signatures of Selection resources. We identified phenotype­environment associations and determined the genetic architecture. The genetic architecture of 9 adaptive traits was analyzed in 2 hybrid backcrosses individually phenotyped

  10. 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

  11. 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.

  12. Non-intrusive characterization of heat transfer fluid aerosol formation 

    E-Print Network [OSTI]

    Krishna, Kiran

    2001-01-01

    in process equipment. Predictive models relating the aerosol formation distances, aerosol droplet size, and volume concentrations to bulk liquid pressure, temperature, fluid properties, leak size and ambient conditions are developed. These models will be used...

  13. The seasonality of aerosol properties in Big Bend National Park 

    E-Print Network [OSTI]

    Allen, Christopher Lee

    2007-04-25

    ), to characterize the seasonal variability of the Big Bend regions aerosol optical properties. Mass extinction efficiencies and relative humidity scattering enhancement factors were calculated for both externally and internally mixed aerosol populations for all size...

  14. Observations of Secondary Organic Aerosol Production and Soot Aging under Atmospheric Conditions Using a Novel Environmental Aerosol Chamber 

    E-Print Network [OSTI]

    Glen, Crystal

    2012-02-14

    of the processes leading to SOA production under ambient gaseous and particulate concentrations as well as the impact these aerosol types have on climate is poorly understood. Although the majority of atmospheric aerosols scatter radiation either directly...

  15. 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 « less

  16. AEROSOL-PRECIPITATION INTERACTIONS IN THE SOUTHERN APPALACHIAN MOUNTAINS

    E-Print Network [OSTI]

    AEROSOL-PRECIPITATION INTERACTIONS IN THE SOUTHERN APPALACHIAN MOUNTAINS A Thesis by GINGER MARIE of the requirements for the degree of MASTER OF ARTS May 2011 Department of Geography and Planning #12;AEROSOL-PRECIPITATION and Graduate Studies #12;Copyright by Ginger Marie Kelly 2011 All Rights Reserved #12;iv ABSTRACT AEROSOL-PRECIPITATION

  17. 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)

  18. 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.

  19. Non-linear photochemical pathways in laser induced atmospheric aerosol formation

    E-Print Network [OSTI]

    Mongin, Denis; Schubert, Elise; Brisset, Jean-Gabriel; Berti, Nicolas; Moret, Michel; Prévôt, André S H; Baltensperger, Urs; Kasparian, Jérôme; Wolf, Jean-Pierre

    2015-01-01

    We measured the chemical composition and the size distribution of aerosols generated by femtosecond-Terawatt laser pulses in the atmosphere using an aerosol mass spectrometer (AMS). We show that nitric acid condenses in the form of ammonium nitrate, and that oxidized volatile organics also contribute to particle growth. These two components account for two thirds and one third, respectively, of the dry laser-condensed mass. They appear in two different modes centred at 380 nm and 150 nm. The number concentration of particles between 25 and 300 nm increases by a factor of 15. Pre-existing water droplets strongly increase the oxidative properties of the laser-activated atmosphere, substantially enhancing the condensation of organics under laser illumination.

  20. University of California, Irvine Environmental Health and Safety www.ehs.uci.edu Questions Call: (949) 824-6200 Version 3.0 Hazardous Chemical Waste Training

    E-Print Network [OSTI]

    Mease, Kenneth D.

    . · An aerosol container must have its contents and pressure completely dispensed, and the spray mechanism to evaporate chemicals. Empty Hazardous Material Container Management: · At no time should full or partially

  1. Flattening coefficient of aerosols collected on treated slides 

    E-Print Network [OSTI]

    Olan-Figueroa, Excel

    1981-01-01

    was found to be 1. 338, and for DOP, 1. 354. There is no apparent variation of F with particle diameter for aerosols in the 2. 7-29. 1 um range. The slightly lower value of F for oleic acid suggests that the contact angle of oleic acid with respect... monodisoerse aerosols in the 1. 5 to 50 um diameter range, the vibratino j et monodisperse aerosol generator has been used. The monodisperse aerosols generated by this device can be considered as an "aerosol standard" since the size and concentration...

  2. 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.

  3. Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry

    E-Print Network [OSTI]

    Kroll, Jesse

    In this study we compile and present results from the factor analysis of 43 Aerosol Mass Spectrometer (AMS) datasets (27 of the datasets are reanalyzed in this work). The components from all sites, when taken together, ...

  4. Effect of Hydrophobic Primary Organic Aerosols on Secondary Organic Aerosol Formation from Ozonolysis of ?-Pinene

    SciTech Connect (OSTI)

    Song, Chen; Zaveri, Rahul A.; Alexander, M. Lizabeth; Thornton, Joel A.; Madronich, Sasha; Ortega, John V.; Zelenyuk, Alla; Yu, Xiao-Ying; Laskin, Alexander; Maughan, A. D.

    2007-10-16

    Semi-empirical secondary organic aerosol (SOA) models typically assume a well-mixed organic aerosol phase even in the presence of hydrophobic primary organic aerosols (POA). This assumption significantly enhances the modeled SOA yields as additional organic mass is made available to absorb greater amounts of oxidized secondary organic gases than otherwise. We investigate the applicability of this critical assumption by measuring SOA yields from ozonolysis of ?-pinene (a major biogenic SOA precursor) in a smog chamber in the absence and in the presence of dioctyl phthalate (DOP) and lubricating oil seed aerosol. These particles serve as surrogates for urban hydrophobic POA. The results show that these POA did not enhance the SOA yields. If these results are found to apply to other biogenic SOA precursors, then the semi-empirical models used in many global models would predict significantly less biogenic SOA mass and display reduced sensitivity to anthropogenic POA emissions than previously thought.

  5. 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.

  6. 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.

  7. Results from simulated upper-plenum aerosol transport and aerosol resuspension experiments

    SciTech Connect (OSTI)

    Wright, A.L.; Pattison, W.L.

    1984-01-01

    Recent calculational results published as part of the Battelle-Columbus BMI-2104 source term study indicate that, for some LWR accident sequences, aerosol deposition in the reactor primary coolant system (PCS) can lead to significant reductions in the radionuclide source term. Aerosol transport and deposition in the PCS have been calculated in this study using the TRAP-MELT 2 computer code, which was developed at Battelle-Columbus; the status of validation of the TRAP-MELT 2 code has been described in an Oak Ridge National Laboratory (ORNL) report. The objective of the ORNL TRAP-MELT Validation Project, which is sponsored by the Fuel Systems Behavior Research Branch of the US Nuclear Regulatory Commission, is to conduct simulated reactor-vessel upper-plenum aerosol deposition and transport tests. The results from these tests will be used in the ongoing effort to validate TRAP-MELT 2. The TRAP-MELT Validation Project includes two experimental subtasks. In the Aerosol Transport Tests, aerosol transport in a vertical pipe is being studied; this geometry was chosen to simulate aerosol deposition and transport in the reactor-vessel upper-plenum. To date, four experiments have been performed; the results from these tests are presented in this paper. 7 refs., 4 figs., 4 tabs.

  8. INTRODUCTION Atmospheric aerosol particles influence the Earth's

    E-Print Network [OSTI]

    Wunderle, Stefan

    , scattering, and absorbing solar electromagnetic radiation and by modifying cloud properties due to their roleINTRODUCTION Atmospheric aerosol particles influence the Earth's radiation budget by reflecting to maximum cover a region once in the daytime. In contrary, up-to-date geostationary instruments like

  9. Experimental study of nuclear workplace aerosol samplers 

    E-Print Network [OSTI]

    Parulian, Antony

    1995-01-01

    consists of an inlet-elbow, a transport line, and a EL-900 CAM prototype manufactured by EG&G. Results show that only 12% of 10 []m aerodynamic diameter (AD) aerosol particles penetrate through the complete sampling system when it is operated at flow rate...

  10. CHEMICAL ENGINEERING AND MANUFACTURING CHEMICAL ENGINEERING

    E-Print Network [OSTI]

    Provancher, William

    CHEMICAL ENGINEERING AND MANUFACTURING CHEMICAL ENGINEERING Objective Chemical Engineers of chemicals. This lesson introduces students to one component of chemical engineering: food processing, and a chemical engineer 2. How chemical engineers are involved in food production 3. That chemical engineers need

  11. 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.

  12. Direct and semidirect aerosol effects of Southern African biomass burning aerosol

    SciTech Connect (OSTI)

    Sakaeda, Naoko; Wood, Robert; Rasch, Philip J.

    2011-06-21

    The direct and semi-direct radiative effects of biomass burning aerosols from Southern African fires during July-October are investigated using 20 year runs of the Community Atmospheric Model (CAM) coupled to a slab ocean model. The aerosol optical depth is constrained using observations in clear skies from MODIS and for aerosol layers above clouds from CALIPSO. Over the ocean, where the absorbing biomass burning aerosol layers are primarily located above cloud, negative top of atmosphere (TOA) semi-direct radiative effects associated with increased low cloud cover dominate over a weaker positive all-sky direct radiative effect (DRE). In contrast, over the land where the aerosols are often below or within cloud layers, reductions in cloud liquid water path (LWP) lead to a positive semi-direct radiative effect that dominates over a near-zero DRE. Over the ocean, the cloud response can be understood as a response to increased lower tropospheric stability (LTS) which is caused both by aerosol absorptive warming in overlying layers and surface cooling in response to direct aerosol forcing. The ocean cloud changes are robust to changes in the cloud parameterization (removal of the hard-wired dependence of clouds on LTS), suggesting that they are physically realistic. Over land where cloud cover changes are minimal, decreased LWP is consistent with weaker convection driven by increased static stability. Over the entire region the overall TOA radiative effect from the biomass burning aerosols is almost zero due to opposing effects over the land and ocean. However, the surface forcing is strongly negative requiring a reduction in precipitation. This is primarily realized through reductions in convective precipitation on both the southern and northern flanks of the convective precipitation region spanning the equatorial rainforest and the ITCZ in the southern Sahel. The changes are consistent with the low-level aerosol forced cooling pattern. The results highlight the importance of semi-direct radiative effects and precipitation responses for determining the climatic effects of aerosols in the African region.

  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. GEOC Sunday, March 21, 2010 47 -Speciation and release kinetics of cadmium and zinc in paddy soils: Application of X-ray absorption

    E-Print Network [OSTI]

    Sparks, Donald L.

    GEOC Sunday, March 21, 2010 47 - Speciation and release kinetics of cadmium and zinc in paddy soils-Vogel, PhD Donald L. Sparks, Prof., PhD . Department of Plant and Soil Sciences and the Delaware and Zn contaminated soils requires a thorough understanding of both Cd and Zn speciation and release

  15. 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.

  16. Effects of NOx on the volatility of secondary organic aerosol from isoprene photooxidation

    SciTech Connect (OSTI)

    Xu, Lu; Kollman, Matthew S.; Song, Chen; Shilling, John E.; Ng, L. N.

    2014-01-28

    The effects of NOx on the volatility of the secondary organic aerosol (SOA) formed from isoprene photooxidation are investigated in environmental chamber experiments. Two types of experiments are performed. In HO2-dominant experiments, organic peroxy radicals (RO2) primarily react with HO2. In mixed experiments, RO2 reacts through multiple pathways. The volatility and oxidation state of isoprene SOA is sensitive to and displays a non-linear dependence on NOx levels. When initial NO/isoprene ratio is approximately 3 (ppbv:ppbv), SOA are shown to be most oxidized and least volatile, associated with the highest SOA yield. A High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) is applied to characterize the key chemical properties of aerosols. While the composition of SOA in mixed experiments does not change substantially over time, SOA become less volatile and more oxidized as oxidation progresses in HO2-dominant experiments. Analysis of the SOA composition suggests that the further reactions of organic peroxides and alcohols may produce carboxylic acids, which might play a strong role in SOA aging.

  17. Aerosol Mass Spectrometry via Laser-Induced Incandescence Particle Vaporization Final Report

    SciTech Connect (OSTI)

    Timothy B. Onasch

    2011-10-20

    We have successfully developed and commercialized a soot particle aerosol mass spectrometer (SP-AMS) instrument to measure mass, size, and chemical information of soot particles in ambient environments. The SP-AMS instrument has been calibrated and extensively tested in the laboratory and during initial field studies. The first instrument paper describing the SP-AMS has been submitted for publication in a peer reviewed journal and there are several related papers covering initial field studies and laboratory studies that are in preparation. We have currently sold 5 SP-AMS instruments (either as complete systems or as SP modules to existing AMS instrument operators).

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

    SciTech Connect (OSTI)

    Rana, Mukhtar A. [Science-Admin Coherence Cell (SACC), PINSTECH Admin Blk, PAEC, Islamabad (Pakistan)] [Science-Admin Coherence Cell (SACC), PINSTECH Admin Blk, PAEC, Islamabad (Pakistan); Ali, Nawab [Physics Division, Directorate of Science, Pakistan Institute of Nuclear Science and Technology (PINSTECH), P.O. Nilore, Islamabad (Pakistan)] [Physics Division, Directorate of Science, Pakistan Institute of Nuclear Science and Technology (PINSTECH), P.O. Nilore, Islamabad (Pakistan); Akhter, Parveen [Pakistan Institute of Engineering and Applied Sciences (PIEAS), Islamabad (Pakistan)] [Pakistan Institute of Engineering and Applied Sciences (PIEAS), Islamabad (Pakistan); Khan, E.U. [Department of Physics, International Islamic University (IIU), Kettle Fields, Kashmir Highways, Islamabad (Pakistan)] [Department of Physics, International Islamic University (IIU), Kettle Fields, Kashmir Highways, Islamabad (Pakistan); Mathieson, John [International Relations, Nuclear Decommissioning Authority (NDA), Building 587, Curie Avenue, Harwell, Didcot, Oxon, OX11 0RH (United Kingdom)] [International Relations, Nuclear Decommissioning Authority (NDA), Building 587, Curie Avenue, Harwell, Didcot, Oxon, OX11 0RH (United Kingdom)

    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)

  19. 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.

  20. 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 Earth’s 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.

  1. 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.

  2. Aerosol Retrievals from ARM SGP MFRSR Data

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

    Alexandrov, Mikhail

    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.

  3. Design of Aerosol Face Masks for Children Using Computerized 3D Face Analysis

    E-Print Network [OSTI]

    Kimmel, Ron

    seal to the child's face, and thus may minimize aerosol leakage and dead space. Key words: inhaled supplied with valved aerosol hold- ing chambers used for aerosol therapy. (Adapted with per- mission from

  4. CCN Activity of Organic Aerosols Observed Downwind of Urban Emissions during CARES

    SciTech Connect (OSTI)

    Mei, Fan; Setyan, Ari; Zhang, Qi; Wang, J. X.

    2013-12-17

    During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of CCN-active particles (kCCN) with diameter from 100 to 170 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites in earlier studies. The low kCCN value was due to the high organic volume fraction, averaged over 80% at the T1 site. The derived kCCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size selected particles with diameter between 100 and 171nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (korg) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For vast majority of the cases, an increase of korg from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from kCCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m/z 44 (f44) and O:C were compared to results from previous studies. Overall, the relationships between korg and f44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in smog chamber. Compared to the relationship between korg and f44, the relationship between korg and O:C exhibits more significant differences among different studies, suggesting korg may be better parameterized using f44. A least squares fit yielded korg = 2.10 (±0.07) × f44 ?0.11 (±0.01) with the Pearson R2 value of 0.71. One possible explanation for the stronger correlation between korg and f44 is that the m/z 44 signal (mostly contributed by the CO+2 ion) is more closely related to organic acids, which may dominate the overall korg due to their relatively high water solubility and hygroscopicity.

  5. 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.

  6. Formation mechanisms and quantification of organic nitrates in atmospheric aerosol

    E-Print Network [OSTI]

    Rollins, Andrew Waite

    2010-01-01

    and J. Viidanoja, Atmospheric chemistry of c 3 -c 6organic nitrates, Atmospheric Chemistry and Physics, 9 (4),organic aerosol yields, Atmospheric Chemistry and Physics

  7. Challenge the future 1 Observations of aerosol-cloud-radiation

    E-Print Network [OSTI]

    Graaf, Martin de

    -road Industrial coal Residential solid fuel Biofuel cooking Biofuel heating Coal Open Burning Agricultural fields causes Differences in: · cloud properties · cloud fraction and location · aerosol properties · smoke

  8. Extending the physicochemical characterization of aerosol particles in California

    E-Print Network [OSTI]

    Zauscher, Melanie Dorothy

    2012-01-01

    W. T. (1997).Emissions from Smoldering Combustion of BiomassCombustion generated aerosols, including emissions from diesel and gasoline engines, biomass and

  9. Climatic effects of different aerosol types in China simulated

    E-Print Network [OSTI]

    Y. GU

    2006-01-01

    P. Shettle (1991), Atmospheric Aero- sols—Global ClimatologyEffects of stratospheric aero- sols and preliminarytypes, such as volcanic aero- sols, desert aerosols, or

  10. Relating Secondary Organic Aerosol Characteristics with Cloud Condensation Nuclei Activity

    E-Print Network [OSTI]

    Tang, Xiaochen

    2013-01-01

    by V and Ni from heavy oil combustion: Anthropogenic sourcesgeneration from heavy fuel oil (HFO) as an alternative toengines operating with heavy fuel oils. Journal of Aerosol

  11. 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...

  12. 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.

  13. 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.

  14. 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.

  15. Speciation and solubility of heavy metals in contaminated soil using X-ray microfluorescence, EXAFS spectroscopy, chemical

    E-Print Network [OSTI]

    Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA c Phytorestore--Site et-neutral pH (6.5­ 7.0) truck-farming soil contaminated by sewage irrigation for one hundred years. Zn

  16. 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.

  17. 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.

  18. Chemical Evolution

    E-Print Network [OSTI]

    Francesca Matteucci

    2007-04-05

    In this series of lectures we first describe the basic ingredients of galactic chemical evolution and discuss both analytical and numerical models. Then we compare model results for the Milky Way, Dwarf Irregulars, Quasars and the Intra-Cluster- Medium with abundances derived from emission lines. These comparisons allow us to put strong constraints on the stellar nucleosynthesis and the mechanisms of galaxy formation.

  19. 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

  20. Absorbing Aerosol Index (AAI) The residue method for the detection of aerosols

    E-Print Network [OSTI]

    Graaf, Martin de

    and calculation Main sensitivities of residue Problems with the residue Conclusions and outlook #12;#12;o = 380 scattering and absorption #12;#12;#12;Nadir View Solar zenith angle = 45o Residue = 3.5 Rayleigh atmosphere View Solar zenith angle = 45o Residue = -1.0 Rayleigh atmosphere, As = 0.16 Scattering aerosol layer

  1. Aerosol Science and Technology, 39:6883, 2005 Copyright c American Association for Aerosol Research

    E-Print Network [OSTI]

    . Coffman5 1 Finnish Meteorological Institute, Air Quality Research, Sahaajankatu, Helsinki, Finland 2¨ais¨al¨a Foundation (Finland), and the 100th Anniversary Foundation of Helsingin Sanomat (Finland). Address, 00880 Helsinki, Finland. E-mail: aki.virkkula@fmi.fi properties of aerosols depend on the wavelength

  2. Aerosol Science and Technology, 38:555573, 2004 Copyright c American Association for Aerosol Research

    E-Print Network [OSTI]

    Jimenez, Jose-Luis

    from motor vehicles are a significant source of fine particulate matter (PM) and gaseous pollutants of their emission. This work uses an Aero- dyne aerosol mass spectrometer (AMS) to provide size instrumentation, was deployed on the Aero- dyne Research Inc. (ARI) mobile laboratory, which was used to "chase

  3. Techniques for Minimizing Aerosols (aerosols are a common source of laboratoryacquired infections)

    E-Print Network [OSTI]

    Chan, Hue Sun

    " pipettes to avoid blowing out the last drop Drain pipettes gently with the tip against the inner wall glass rod to crack the glass, allow time for air to seep into the ampoule and gently remove the top than glass (less likely to break which generates aerosols) Source: Adapted from

  4. Aerosol Science and Technology, 43:486501, 2009 Copyright American Association for Aerosol Research

    E-Print Network [OSTI]

    a NOAA research vessel during the Texas Air Quality Study 2006/Gulf of Mexico Atmospheric Composition for glutaric acid in mixed glutaric acid/NH4HSO4 test aerosols was 0.22 ng collected mass, which corresponds min­1. During TexAQS 2006/GoMACCS, signals well above the detection limit were observed at a number

  5. Na, Mg, Ni and Cs distribution and speciation after long-term alteration of a simulated nuclear waste glass

    E-Print Network [OSTI]

    Farges b,c , Marika Vespa a,1 a Laboratory for Waste Management, Paul Scherrer Institut, CH-5232 Villigen distribution and speciation of Na, Mg, Ni and Cs in a simulated (inactive) nuclear waste glass were studied and Cs represent dose determining long-lived radionuclides (59 Ni, 135 Cs) in vitrified nuclear waste

  6. Distribution, Speciation, and Elemental Associations of Soil Organic Carbon under Varying Landscape Topographic Positions at the Molecular Scale

    E-Print Network [OSTI]

    Sparks, Donald L.

    Distribution, Speciation, and Elemental Associations of Soil Organic Carbon under Varying Landscape spectra and maps were collected. Results: C Distribution and Associations with the Major Elements in Soil Clay Particles Fig.1. Relative elemental distribution maps (9µm×6µm) of clay fractions from the A

  7. Does species diversity really drive speciation? Henrique M. Pereira, Va^nia M. Proenca and Luis Vicente

    E-Print Network [OSTI]

    Pereira, Henrique Miguel

    of endemics in a taxon with the number of species in that taxon, in the Canary Islands and the Hawaiian richness and speciation or extinction rates. In both the Canary Islands and the Hawaiian Islands species are the same for both taxon in each archipelago (elevation and island age for the Canary Islands, and area

  8. EQ3NR, a computer program for geochemical aqueous speciation-solubility calculations: Theoretical manual, user`s guide, and related documentation (Version 7.0); Part 3

    SciTech Connect (OSTI)

    Wolery, T.J.

    1992-09-14

    EQ3NR is an aqueous solution speciation-solubility modeling code. It is part of the EQ3/6 software package for geochemical modeling. It computes the thermodynamic state of an aqueous solution by determining the distribution of chemical species, including simple ions, ion pairs, and complexes, using standard state thermodynamic data and various equations which describe the thermodynamic activity coefficients of these species. The input to the code describes the aqueous solution in terms of analytical data, including total (analytical) concentrations of dissolved components and such other parameters as the pH, pHCl, Eh, pe, and oxygen fugacity. The input may also include a desired electrical balancing adjustment and various constraints which impose equilibrium with special pure minerals, solid solution end-member components (of specified mole fractions), and gases (of specified fugacities). The code evaluates the degree of disequilibrium in terms of the saturation index (SI = 1og Q/K) and the thermodynamic affinity (A = {minus}2.303 RT log Q/K) for various reactions, such as mineral dissolution or oxidation-reduction in the aqueous solution itself. Individual values of Eh, pe, oxygen fugacity, and Ah (redox affinity) are computed for aqueous redox couples. Equilibrium fugacities are computed for gas species. The code is highly flexible in dealing with various parameters as either model inputs or outputs. The user can specify modification or substitution of equilibrium constants at run time by using options on the input file.

  9. Microscopic Characterization of Carbonaceous Aerosol Particle Aging in the Outflow from Mexico City

    SciTech Connect (OSTI)

    Moffet, R. C.; Henn, T. R.; Tivanski, A. V.; Hopkins, R. J.; Desyaterik, Y.; Kilcoyne, A. L. D.; Tyliszczak, T.; Fast, J.; Barnard, J.; Shutthanandan, V.; Cliff, S.S.; Perry, K. D.; Laskin, A.; Gilles, M. K.

    2009-09-16

    This study was part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in Mexico City Metropolitan Area during spring 2006. The physical and chemical transformations of particles aged in the outflow from Mexico City were investigated for the transport event of 22 March 2006. A detailed chemical analysis of individual particles was performed using a combination of complementary microscopy and micro-spectroscopy techniques. The applied techniques included scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure spectroscopy (NEXAFS) and computer controlled scanning electron microscopy with an energy dispersive X-ray analyzer (CCSEM/EDX). As the aerosol plume evolves from the city center, the organic mass per particle increases and the fraction of carbon-carbon double bonds (associated with elemental carbon) decreases. Organic functional groups enhanced with particle age include: carboxylic acids, alkyl groups, and oxygen bonded alkyl groups. At the city center (T0) the most prevalent aerosol type contained inorganic species (composed of sulfur, nitrogen, oxygen, and potassium) coated with organic material. At the T1 and T2 sites, located northeast of T0 (~;;29 km and ~;;65 km, respectively), the fraction of homogenously mixed organic particles increased in both size and number. These observations illustrate the evolution of the physical mixing state and organic bonding in individual particles in a photochemically active environment.

  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. Measurements of aerosol vertical profiles and optical properties during INDOEX

    E-Print Network [OSTI]

    , and the Kaashidhoo Climate Observatory (KCO) in the Maldives. Sun photometers were used to provide aerosol optical depths (AOD) needed to calibrate the MPL. This study focuses on the height distribution and optical trajectories, radiosonde profiles of temperature and humidity, and aerosol concentration and optical

  13. SCIAMACHY'S ABSORBING AEROSOL INDEX AND THE CONSEQUENCES OF INSTRUMENT DEGRADATION

    E-Print Network [OSTI]

    Graaf, Martin de

    SCIAMACHY'S ABSORBING AEROSOL INDEX AND THE CONSEQUENCES OF INSTRUMENT DEGRADATION L. G. Tilstra1- itoring the Absorbing Aerosol Index (AAI) [1] measured by the satellite instrument SCIAMACHY [2]. We find. This we conclude from straightforward calculation of the effect of instrument degradation based

  14. Global observations of desert dust and biomass burning aerosols

    E-Print Network [OSTI]

    Graaf, Martin de

    and desert dust observations from GOME and SCIAMACHY · Conclusions and Outlook #12; · Absorbing Aerosol Transfer Model Solar zenith angle = 30° Viewing zenith angle = 0° Surface albedo = 5% #12;Reflectance at TOA with absorbing aerosols Doubling-Adding KNMI Radiative Transfer Model Solar zenith angle = 30

  15. GLOBAL AEROSOL EFFECT RETRIEVAL FROM PASSIVE HYPERSPECTRAL MEASUREMENTS

    E-Print Network [OSTI]

    Graaf, Martin de

    that can be detected using UV reflectance measurements. Since the aerosol extinction optical thickness any instrument, or a combination of instruments, that measures UV, visible and SWIR reflectancesGLOBAL AEROSOL EFFECT RETRIEVAL FROM PASSIVE HYPERSPECTRAL MEASUREMENTS M. de Graaf1,2 , L. G

  16. Carbonaceous aerosol particles from common vegetation in the Grand Canyon

    SciTech Connect (OSTI)

    Hallock, K.A.; Mazurek, M.A. (Brookhaven National Lab., Upton, NY (United States)); Cass, G.R. (California Inst. of Tech., Pasadena, CA (United States). Dept. of Environmental Engineering Science)

    1992-05-01

    The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon.

  17. Supplementary Material1 Characterization of Organic Aerosol Produced during2

    E-Print Network [OSTI]

    Meskhidze, Nicholas

    mass spectra of a dominant type (coal) of ambient aerosol in Shanghai using2 ATOFMS (m/z from 1501 Supplementary Material1 Characterization of Organic Aerosol Produced during2 Pulverized Coal diagram of combustion process of a single coal particle5 6 #12;3 10 100 10 3 10 4 10 5 Oxygen/coal ratio

  18. Effects of operating conditions on a heat transfer fluid aerosol 

    E-Print Network [OSTI]

    Sukmarg, Passaporn

    2000-01-01

    fluids are used as hot liquids at elevated pressures. If loss of containment does occur, the liquid will leak under pressure and may disperse as a fine aerosol mist. Though it has been recognized that aerosol mists can explode, very little is known about...

  19. Flood or Drought: How Do Aerosols Affect Precipitation?

    E-Print Network [OSTI]

    Daniel, Rosenfeld

    Flood or Drought: How Do Aerosols Affect Precipitation? Daniel Rosenfeld,1 * Ulrike Lohmann,2 and the initiation of precipitation. Large concentrations of human-made aerosols have been reported to both decrease hand, heavily polluted clouds evaporate much of their water before precipitation can occur, if they can

  20. Gaseous Chemistry and Aerosol Mechanism Developments for Version 3.5.1 of the Online Regional Model, WRF-Chem

    SciTech Connect (OSTI)

    Archer-Nicholls, Scott; Lowe, Douglas; Utembe, Steve; Allan, James D.; Zaveri, Rahul A.; Fast, Jerome D.; Hodnebrog, Oivind; Denier van der Gon, Hugo; McFiggans, Gordon

    2014-11-08

    We have made a number of developments in the regional coupled model WRF-Chem, with the aim of making the model more suitable for prediction of atmospheric composition and of interactions between air quality and weather. We have worked on the European domain, with a particular focus on making the model suitable for the study of night time chemistry and oxidation by the nitrate radical in the UK atmosphere. A reduced form of the Common Reactive Intermediates gas-phase chemical mechanism (CRIv2-R5) has been implemented to enable more explicit simulation of VOC degradation. N2O5 heterogeneous chemistry has been added to the existing sectional MOSAIC aerosol module, and coupled to both the CRIv2-R5 and existing CBM-Z gas phase scheme. Modifications have also been made to the sea-spray aerosol emission representation, allowing the inclusion of primary organic material in sea-spray aerosol. Driven by appropriate emissions, wind fields and chemical boundary conditions, implementation of the different developments is illustrated in order to demonstrate the impact that these changes have in the North-West European domain. These developments are now part of the freely available WRF-Chem distribution.

  1. 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.

  2. Experiments related to the resuspension of aerosols during hydrogen burns

    SciTech Connect (OSTI)

    Nelson, L.S.; Guay, K.P.

    1987-01-01

    We have performed seven ''add-on'' experiments in two large combustion facilities to investigate the capability of hydrogen burns to remove simulated structural and fission product aerosols previously deposited on small metal discs that have surfaces prototypical of those found in nuclear reactor containments. Our results suggest that hydrogen combustion provides an especially effective mechanism for removal (and, presumably, resuspension) of sedimented aerosols produced in a hypothetical nuclear reactor core-degradation or core-melting accident. The presence of condensing steam does not seem to assure adhesion of sedimented aerosols during hydrogen burns. Differences are exhibited between different surfaces as well as between types of aerosol. In-depth studies will be required to assess the impact exposure of sedimented aerosols to hydrogen burns might have on the radiological source term.

  3. Study of Aerosol Indirect Effects in China

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power AdministrationRobust,Field-effect PhotovoltaicsStructure andChallenge | Department,Aerosol Indirect Effects in

  4. Seasonal and diurnal variations of submicron organic aerosol in Tokyo observed using the Aerodyne aerosol mass spectrometer

    E-Print Network [OSTI]

    Jimenez, Jose-Luis

    with carbon monoxide (CO) and fragments of aliphatic and oxygenated organic compounds in the AMS mass spectra. Combustion-related organic aerosol (combustion OA) is defined as the primary organic aerosol (POA) fraction the combustion OA and the background OA from the total OA. The combustion OA and excess OA show good correlation

  5. 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

  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

    2004-10-01

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

  7. 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

    2004-10-01

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

  8. 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

  9. Investigation of Aerosol Sources, Lifetime and Radiative Forcing through Multi-Instrument Data Assimilation

    E-Print Network [OSTI]

    Rubin, Juli Irene

    2012-01-01

    of the various radiative mechanims associated with aerosolof the various radiative mechanims associated with aerosol

  10. Analysis of reflectance spectra of UV-absorbing aerosol scenes measured by SCIAMACHY

    E-Print Network [OSTI]

    Graaf, Martin de

    Analysis of reflectance spectra of UV-absorbing aerosol scenes measured by SCIAMACHY M. de Graaf,1 of reflectance spectra of UV-absorbing aerosol scenes measured by SCIAMACHY, J. Geophys. Res., 112, D02206, doi aerosol (DDA) and biomass burning aerosol (BBA) scenes over oceans are presented, measured by the space

  11. UNDERSTANDING THE INFLUENCES OF ATMOSPHERIC AEROSOLS ON CLIMATE AND CLIMATE CHANGE

    E-Print Network [OSTI]

    Schwartz, Stephen E.

    remarks #12;DMS #12;AEROSOL IN MEXICO CITY BASIN #12;AEROSOL IN MEXICO CITY BASIN Light scattering by aerosols decreases absorption of solar radiation. #12;AEROSOLS AS SEEN FROM SPACE Fire plumes from southern Mexico transported north into Gulf of Mexico. #12;CLOUD BRIGHTENING BY SHIP TRACKS Satellite photo off

  12. Satellite observations of the seasonal cycles of absorbing aerosols in Africa

    E-Print Network [OSTI]

    Graaf, Martin de

    Satellite observations of the seasonal cycles of absorbing aerosols in Africa related to monsoon of aerosol emissions from the wet surface. 1. Introduction The main aerosol types occurring over Africa Africa can be characterized using Absorbing Aerosol Index (AAI) data from Global Ozone Monitoring

  13. A geostatistical data fusion technique for merging remote sensing and groundbased observations of aerosol optical thickness

    E-Print Network [OSTI]

    Michalak, Anna M.

    that aerosols contrib- ute significantly to reflected solar radiation (the aerosol direct effect) and modify of aerosols in climate and atmospheric chemistry. To date, however, there have been only limited attempts of the growing concentrations of CO2 and other greenhouse gases. Although the radiative forcing of aerosols

  14. 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

  15. 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

  16. 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

  17. 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

  18. 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.

  19. 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.

  20. 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 world’s 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 4STAR’s spatially-resolved high-frequency hyperspectral products as a reliable tool for climate studies and satellite validation.

  1. 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.

  2. 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)

  3. Chemical Science

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfateSciTechtail.Theory of raregovAboutRecoveryplanning CareerNationalCNMSTHEmaterials |Chemical

  4. 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.

  5. 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.

  6. 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

  7. 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

  8. 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.

  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. Speciation and Release Kinetics of Cadmium in Alkali and Acidic Paddy Soils: Application of X-Ray Absorption Spectroscopy Monday, November 2, 2009: 10:30 AM

    E-Print Network [OSTI]

    Sparks, Donald L.

    Speciation and Release Kinetics of Cadmium in Alkali and Acidic Paddy Soils: Application of X under alkali and acidic conditions. X-ray absorption spectroscopy (XAS) was used to investigate Cd

  11. Inverse modelling of cloud-aerosol interactions - Part 2: Sensitivity tests on liquid phase clouds using a Markov chain Monte Carlo based simulation approach

    E-Print Network [OSTI]

    Partridge, D. G; Vrugt, J. A; Tunved, P.; Ekman, A. M. L; Struthers, H.; Sorooshian, A.

    2012-01-01

    Seinfeld, J. H. : Aerosol, cloud drop concentration closureof aerosol composition on cloud droplet size distribution –aerosol properties on warm cloud droplet activation, At-

  12. 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. more »Aerosol 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

  13. 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

  14. Aerosol penetration through a seismically loaded shear wall

    SciTech Connect (OSTI)

    Farrar, C.R.; Girrens, S.P.

    1992-05-01

    An experimental study was performed to measure the aerosol penetration through a reinforced concrete shear wall after simulated seismic damage. Static load-cycle testing, to stress levels sufficient to induce visible shear cracking, was used to simulate the earthquake loading. Air permeability tests were performed both before and after the simulated seismic loading damaged the structure. Aerosol penetration measurements were conducted on the cracked shear wall structure using 0.10 {mu}m monodisperse particles. The measured aerosol number penetration through the cracked shear wall was 0.5%. 7 refs.

  15. Aerosol penetration through a seismically loaded shear wall

    SciTech Connect (OSTI)

    Farrar, C.R.; Girrens, S.P.

    1992-01-01

    An experimental study was performed to measure the aerosol penetration through a reinforced concrete shear wall after simulated seismic damage. Static load-cycle testing, to stress levels sufficient to induce visible shear cracking, was used to simulate the earthquake loading. Air permeability tests were performed both before and after the simulated seismic loading damaged the structure. Aerosol penetration measurements were conducted on the cracked shear wall structure using 0.10 {mu}m monodisperse particles. The measured aerosol number penetration through the cracked shear wall was 0.5%. 7 refs.

  16. Aerosol source term in high pressure melt ejection

    SciTech Connect (OSTI)

    Brockmann, J.E.; Tarbell, W.W.

    1984-11-01

    Pressurized ejection of melt from a reactor pressure vessel has been identified as an important element of a severe reactor accident. Copious aerosol production is observed when thermitically generated melts pressurized with nitrogen or carbon dioxide to 1.3 to 17 MPa are ejected into an air atmosphere. Aerosol particle size distributions measured in the tests have modes of about 0.5, 5, and > 10 ..mu..m. Mechanisms leading to formation of these multimodal size distributions are suggested. This aerosol is a potentially important fission product source term that has not been considered in previous severe accident analyses.

  17. 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.

  18. Mexico City Aerosol Analysis During Milagro Using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0) - Part 1: Fine Particle Composition and Organic Source Apportionment.

    E-Print Network [OSTI]

    Aiken, A. C.

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive ...

  19. Simulated aerosol key optical properties over global scale using an aerosol transport model coupled with a new type of dynamic core

    E-Print Network [OSTI]

    Dong, Xiquan

    effects: (a) a direct effect in which aerosol particles scatter and absorb the solar and thermal radiation Atmospheric aerosols greatly impact the Earth's climate in many ways, and to date, not all of them are well

  20. 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.

  1. Diesel Aerosol Sampling in the Atmosphere

    SciTech Connect (OSTI)

    David Kittelson; Jason Johnson; Winthrop Watts; Qiang Wei; Marcus Drayton; Dwane Paulsen; Nicolas Bukowiecki

    2000-06-19

    The University of Minnesota Center for Diesel Research along with a research team including Caterpillar, Cummins, Carnegie Mellon University, West Virginia University (WVU), Paul Scherrer Institute in Switzerland, and Tampere University in Finland have performed measurements of Diesel exhaust particle size distributions under real-world dilution conditions. A mobile aerosol emission laboratory (MEL) equipped to measure particle size distributions, number concentrations, surface area concentrations, particle bound PAHs, as well as CO 2 and NO x concentrations in real time was built and will be described. The MEL was used to follow two different Cummins powered tractors, one with an older engine (L10) and one with a state-of-the-art engine (ISM), on rural highways and measure particles in their exhaust plumes. This paper will describe the goals and objectives of the study and will describe representative particle size distributions observed in roadway experiments with the truck powered by the ISM engine.

  2. Chemical Accelerators The phrase "chemical accelerators"

    E-Print Network [OSTI]

    Meetings Chemical Accelerators The phrase "chemical accelerators" is scarcely older than for one or two dozen people grew to include nearly a hundred. Chemical accelerators is a name sug- gested by one of us for devices that produce beams of chemically interesting species at relative kinetic

  3. Observational Insights into Aerosol Formation from Isoprene David R. Worton,*,,

    E-Print Network [OSTI]

    Goldstein, Allen

    , Ronald C. Cohen, John H. Seinfeld, and Allen H. Goldstein,$ Department of Environmental Science, Policy and Management, Department of Chemistry, University of California, Berkeley, California 94720, United States Aerosol Dynamics Inc., Berkeley, California 94710, United States § Department of Environmental Sciences

  4. A review of Secondary Organic Aerosol (SOA) formation from isoprene

    E-Print Network [OSTI]

    Kroll, Jesse

    Recent field and laboratory evidence indicates that the oxidation of isoprene, (2-methyl-1,3-butadiene, C[subscript 5]H[subscript 8]) forms secondary organic aerosol (SOA). Global biogenic emissions of isoprene (600 Tg ...

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

    Office of Scientific and Technical Information (OSTI)

    carbon (BC) with other aerosol components, merging of the MAM7 fine dust and fine sea salt modes into the accumulation mode, merging of the MAM7 coarse dust and coarse sea salt...

  6. 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.

  7. ris-r-1075(en) Quantitative Measurement of Aerosol

    E-Print Network [OSTI]

    and implications of deposition of potentially hazardous aerosol directly onto hu- mans. This state, beta doses from skin deposition to individuals in areas of Russia, where dry deposition of Chernobyl

  8. Experimental and numerical studies of aerosol penetration through screens 

    E-Print Network [OSTI]

    Han, Tae Won

    2009-05-15

    for one particular type of screen would collapse to a single curve if the collection efficiency is expressed in terms of non-dimensional parameters. Correlations characterizing the aerosol deposition process on different types of screens were developed...

  9. Aerosol-Cloud interactions : a new perspective in precipitation enhancement

    E-Print Network [OSTI]

    Gunturu, Udaya Bhaskar

    2010-01-01

    Increased industrialization and human activity modified the atmospheric aerosol composition and size-distribution during the last several decades. This has affected the structure and evolution of clouds, and precipitation ...

  10. Aerosol optical hygroscopicity measurements during the 2010 CARES campaign

    E-Print Network [OSTI]

    Atkinson, D. B.

    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 ...

  11. REPRESENTING AEROSOLS IN GLOBAL MODELS: FROM MICROMETERS TO MEGAMETERS

    E-Print Network [OSTI]

    Schwartz, Stephen E.

    mainly from gas-to- particle conversion of low-volatility gaseous species, mainly sulfuric acid to represent aerosol processes and forcing "on-line" in climate models in order to capture the feedbacks

  12. 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.

  13. ReproducedfromJournalofEnvironmentalQuality.PublishedbyASA,CSSA,andSSSA.Allcopyrightsreserved. Phosphorus Speciation in Manure-Amended Alkaline Soils

    E-Print Network [OSTI]

    Puglisi, Joseph

    JournalofEnvironmentalQuality.PublishedbyASA,CSSA,andSSSA.Allcopyrightsreserved. Phosphorus Speciation in Manure-Amended Alkaline Soils Jeremy C. Hansen, Barbara J. Cade-Menun, and Daniel G or mononucleotides, allowing it toThe manure from stockpiles is applied to soils in solid form, while lagoon manure is applied as a liquid. Soil amendment with manure form relatively stable complexes in soil that are pro

  14. 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.

  15. 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.

  16. 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.

  17. Investigations of cloud altering effects of atmospheric aerosols using a new mixed Eulerian-Lagrangian aerosol model

    E-Print Network [OSTI]

    Steele, Henry Donnan, 1974-

    2004-01-01

    Industry, urban development, and other anthropogenic influences have substantially altered the composition and size-distribution of atmospheric aerosol particles over the last century. This, in turn, has altered cloud ...

  18. 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.

  19. 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.

  20. 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'smore »prescribed 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

  1. 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.

  2. Lead exposures and biological responses in military weapons systems: Aerosol characteristics and acute lead effects among US Army artillerymen: Final report

    SciTech Connect (OSTI)

    Bhattacharyya, M.H.; Stebbings, J.H.; Peterson, D.P.; Johnson, S.A.; Kumar, R.; Goun, B.D.; Janssen, I.; Trier, J.E.

    1993-03-01

    This study was to determine the concentration and chemical nature of lead (Pb) aerosols produced during the firing of artillery and to determine the exposures and biological responses of crew members exposed to lead aerosols during such firing. The concentrations of lead-containing aerosols at crew positions depended on wind conditions, with higher concentrations when firing into a head wind. Aerosol concentrations were highest in the muzzle blast zone. Concentrations of lead in the blood of crew members rose during the first 12 days of exposure to elevated airborne lead concentrations and then leveled off. There was no rapid decrease in blood lead concentrations after completion of firing. Small decreases in hematocrit and small increases in free erythrocyte porphyrin were correlated with increasing exposure to airborne lead. These changes were reversed by seven weeks after firing. Changes in nerve conduction velocity had borderline statistical significance to airborne lead exposure. In measuring nerve conduction velocity, differences in skin temperature must be taken into account.

  3. CHEMICAL ENGINEERING Curriculum Notes

    E-Print Network [OSTI]

    Mohan, Chilukuri K.

    CHEMICAL ENGINEERING Curriculum Notes 2013-2014 1. Chemical engineering students must complete not included in the required chemical engineering curriculum. All technical electives are subject to approval be in chemical engineering. 2. Chemical engineering students must complete a minimum of 18 credits in the Social

  4. 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.

  5. Large Enhancement in the Heterogeneous Oxidation Rate of Organic Aerosols by Hydroxyl Radicals in the Presence of Nitric Oxide.

    E-Print Network [OSTI]

    Richards-Henderson, NK; Goldstein, AH; Wilson, KR

    2015-01-01

    Heterogeneous Reaction of Hydroxyl Radicals with Sub-Micronof Organic Aerosols by Hydroxyl Radicals in the Presence ofin an aerosol exposed to hydroxyl radicals (OH) is thought

  6. Effects on precipitation, clouds, and temperature from long-range transport of idealized aerosol plumes in WRF-Chem simulations

    E-Print Network [OSTI]

    Zhao, Zhan; Pritchard, Michael S; Russell, Lynn M

    2012-01-01

    on intense convective precipitation in the northeastern US,aerosols on regional precipitation over East Asia, J.of aerosols on surface precipitation from clouds: An attempt

  7. TALSPEAK EXTRACTION SYSTEM UNDER VARIABLE LOADING CONDITIONS - PART 2: SPECIATION STUDIES

    SciTech Connect (OSTI)

    Robinson, Troy A.; Bryan, Samuel A.; Levitskaia, Tatiana G.

    2011-10-03

    The reported investigation was performed to gain structural information on the organic phase complex species in the Trivalent Actinide-Lanthanide Separation by Phosphorus reagent Extraction from Aqueous Komplexes (TALSPEAK) process under various loading conditions. In conjunction with the distribution studies of the TALSPEAK system constituents, presented in Part 1 of this investigation, loaded bis(2-ethylhexyl) phosphoric acid (HDEHP)/isooctane was evaluated using various spectroscopic techniques including NMR, FTIR and visible absorbance spectroscopy. Liquid-liquid distribution and vapor pressure osmometry (VPO) aggregation results correlate with observed changes in the spectroscopic signatures as a function of organic phase loading and water partitioning. Explicit FTIR spectral interpretation of the HDEHP spectra is complex due to overlapping phosphorus absorbance bands, and in this work a combination of the spectroscopic techniques was utilized to elucidate the phosphorus-lanthanide complex structure and changes in speciation due to aggregation. The results from this research will benefit an overall improved prediction of the TALSPEAK process performance under flow conditions.

  8. 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.

  9. 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.

  10. Speciation and Attenuation of Arsenic and Selenium at Coal Combustion By-Product Management Facilities

    SciTech Connect (OSTI)

    K. Ladwig

    2005-12-31

    The overall objective of this project was to evaluate the impact of key constituents captured from power plant air streams (principally arsenic and selenium) on the disposal and utilization of coal combustion products (CCPs). Specific objectives of the project were: (1) to develop a comprehensive database of field leachate concentrations at a wide range of CCP management sites, including speciation of arsenic and selenium, and low-detection limit analyses for mercury; (2) to perform detailed evaluations of the release and attenuation of arsenic species at three CCP sites; and (3) to perform detailed evaluations of the release and attenuation of selenium species at three CCP sites. Each of these objectives was accomplished using a combination of field sampling and laboratory analysis and experimentation. All of the methods used and results obtained are contained in this report. For ease of use, the report is subdivided into three parts. Volume 1 contains methods and results for the field leachate characterization. Volume 2 contains methods and results for arsenic adsorption. Volume 3 contains methods and results for selenium adsorption.

  11. 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.

  12. Practical application of in situ aerosol measurement

    SciTech Connect (OSTI)

    O`Hern, T.J.; Rader, D.J.

    1993-09-01

    The use of in situ, real-time measurement techniques permits the characterization of airborne droplets and particles under conditions where traditional sampling methods can fail. For example, sampling method rely on the ability to sample and transport particles without biasing the properties of interest, and often are not applicable in harsh environment. Although in situ methods offer unique opportunities in these cases, these techniques introduce new concerns and must be used carefully if accurate measurement are to be made. Several in situ measurement techniques are reviewed here. As the field is rapidly evolving, the discussion is limited to those techniques which: (1) are commercially available, (2) provide real-time output, (3) measure the aerosol size distribution. Discussion is divided between single particle counters (which provide a flux-based or temporal measurement) and ensemble techniques (which provide a concentration-based or spatial measurement). Specific techniques discussed include phase Doppler, Mie scattering, and Fraunhofer diffraction, and commercial instruments based on these techniques.

  13. Laser induced chemical reactions

    E-Print Network [OSTI]

    Orel, Ann E.

    2010-01-01

    the simplest prototype chemical reaction, and since it is soLASER ENHANCEMENT OF CHEMICAL REACTIONS A. B. C. D. E.Laser Inhibition of Chemical Reaction Effect of Isotopic

  14. 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.

  15. 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...

  16. 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 (bin

  17. Mechanisms of aerosol-forced AMOC variability in a state of the art climate model

    E-Print Network [OSTI]

    with a new state-of-the-art Earth system model. Anthropogenic aerosols have previously been highlighted anthropogenic aerosols force a strengthening of the AMOC by up to 20% in our state-of-the-art Earth system model

  18. Investigation of the aerosol-cloud interaction using the WRF framework 

    E-Print Network [OSTI]

    Li, Guohui

    2009-05-15

    In this dissertation, a two-moment bulk microphysical scheme with aerosol effects is developed and implemented into the Weather Research and Forecasting (WRF) model to investigate the aerosol-cloud interaction. Sensitivities ...

  19. CHASER: An Innovative Satellite Mission Concept to Measure the Effects of Aerosols on Clouds and Climate

    E-Print Network [OSTI]

    Rosenfeld, Daniel

    The formation of cloud droplets on aerosol particles, technically known as the activation of cloud condensation nuclei (CCN), is the fundamental process driving the interactions of aerosols with clouds and precipitation. ...

  20. Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass at Bakersfield

    E-Print Network [OSTI]

    Cohen, Ronald C.

    Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass is fossil fuel combustion from gasoline- and diesel- powered vehicles and other industrial activities (e

  1. Investigation of the optical and cloud forming properties of pollution, biomass burning, and mineral dust aerosols 

    E-Print Network [OSTI]

    Lee, Yong Seob

    2006-08-16

    that were observed during this period. The predicted cloud condensation nuclei concentrations were used in a cloud model to determine the impact of the different aerosol types on the expected cloud droplet concentration. RH-dependent aerosol extinction...

  2. Computational fluid dynamics (CFD) simulations of aerosol in a u-shaped steam generator tube 

    E-Print Network [OSTI]

    Longmire, Pamela

    2009-05-15

    To quantify primary side aerosol retention, an Eulerian/Lagrangian approach was used to investigate aerosol transport in a compressible, turbulent, adiabatic, internal, wall-bounded flow. The ARTIST experimental project ...

  3. Variablity among electronic cigarettes in the pressure drop, airflow rate, and aerosol production

    E-Print Network [OSTI]

    Talbot, Prue

    2013-01-01

    on the Ruyan e-cigarette cartridge and inhaled aerosol (pp.drop, length of time cartridges lasted, and production ofdevice that aerosolizes cartridge fluid which is in turn

  4. Variability of aerosol parameters over Kanpur, northern India R. P. Singh,1

    E-Print Network [OSTI]

    Singh, Ramesh P.

    Variability of aerosol parameters over Kanpur, northern India R. P. Singh,1 Sagnik Dey, S. N Dynamics: Remote sensing; KEYWORDS: aerosol, remote sensing, Ganga basin Citation: Singh, R. P., S. Dey, S

  5. The impact of pathological ventilation on aerosol deposition : imaging, insight and intervention

    E-Print Network [OSTI]

    Greenblatt, Elliot (Elliot Eliyahu)

    2015-01-01

    Aerosol therapies are often used to treat lung diseases in which ventilation is distributed heterogeneously throughout the lung. As therapeutic aerosols are transported by the inhaled air, it is likely that deposition is ...

  6. Climate effects of seasonally varying Biomass Burning emitted Carbonaceous Aerosols (BBCA)

    E-Print Network [OSTI]

    Jeong, Gill-Ran

    The climate impact of the seasonality of Biomass Burning emitted Carbonaceous Aerosols (BBCA) is studied using an aerosol-climate model coupled with a slab ocean model in a set of 60-year long simulations, driven by BBCA ...

  7. 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 2–4 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), UV–Visible 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.

  8. 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...

  9. Institute of Chemical Engineering and High Temperature Chemical...

    Open Energy Info (EERE)

    Institute of Chemical Engineering and High Temperature Chemical Processes ICEHT Jump to: navigation, search Name: Institute of Chemical Engineering and High Temperature Chemical...

  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. 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.

  12. 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...

  13. CHALLENGE TO ARM AND ASP Determine aerosol radiative forcings at ARM site(s).

    E-Print Network [OSTI]

    Schwartz, Stephen E.

    aerosol optical thickness is 0.1: 3 W m-2 cooling. ~50 km Drone Radiometers AMF DIRECT DETERMINATION

  14. Characterization of Pre-Commercial Gasoline Engine Particulates Through Advanced Aerosol Methods

    Broader source: Energy.gov [DOE]

    Advanced aerosol analysis methods were used to examine particulates from single cylinder test engines running on gasoline and ethanol blends.

  15. Global observations of UV-absorbing aerosols from ERS-2/GOME Data

    E-Print Network [OSTI]

    Graaf, Martin de

    Absorbing Aerosol Index ­ Theory GOME AAI results Conclusions & Outlook #12; Absorbing Aerosol Index Solar zenith angle = 30° Viewing zenith angle = 0° Surface albedo = 5% #12; Reflectance at TOA with absorbing aerosols Doubling-Adding KNMI Radiative Transfer Model Solar zenith angle = 30° Viewing zenith

  16. Trends in aerosol optical properties over the Bohai Rim in Northeast China from 2004 to 2010

    E-Print Network [OSTI]

    Zeng, Ning

    Trends in aerosol optical properties over the Bohai Rim in Northeast China from 2004 to 2010 al., 2004). However, the spatial and temporal contributions of aerosol optical properties and aerosol of this growth is driven by new industry that consumes substantially more coal and fossil fuel in the region

  17. Uncertainty and interpretation of aerosol remote sensing due to vertical inhomogeneity

    E-Print Network [OSTI]

    , and aerosol column number density. Monomodal aerosol size distribution is assumed. The Cost Function (CF radiance data at the TOA have been created assuming either one or two layers of aerosols using the vector is affected by the radiative forcing associated with various sources, including total solar irradiance

  18. Mixtures of pollution, dust, sea salt, and volcanic aerosol during ACE-Asia: Radiative properties

    E-Print Network [OSTI]

    was dominated by marine, polluted, volcanic, and dust aerosols. Average total light scattering coefficients (sspMixtures of pollution, dust, sea salt, and volcanic aerosol during ACE-Asia: Radiative properties). Aerosol hygroscopicity ranged from deliquescent with hysteresis (marine frequently and polluted variably

  19. 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.

  20. Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass

    E-Print Network [OSTI]

    Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass burning in Central Amazonia (TT34 North of Manaus) and at a heavily biomass burning impacted site in south-refractory PM1 aerosol loading at TT34, while biomass burning aerosols at PVH shows a 93% content of organic

  1. AEROSOL-CLOUD INTERACTIONS CONTROL OF EARTH RADIATION AND LATENT HEAT RELEASE BUDGETS

    E-Print Network [OSTI]

    Daniel, Rosenfeld

    AEROSOL-CLOUD INTERACTIONS CONTROL OF EARTH RADIATION AND LATENT HEAT RELEASE BUDGETS D. ROSENFELD simulations show that cloud development is strongly mod- ulated by the impact of cloud-aerosol interactions on precipitation forming processes. New insights into the mechanisms by which aerosols dominate the cloud cover

  2. 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.

  3. Heterodyne lidar for chemical sensing

    SciTech Connect (OSTI)

    Oldenborg, R. C. (Richard C.); Tiee, J. J. (Joe J.); Shimada, T. (Tsutomu); Wilson, C. W. (Carl W.); Remelius, D. K. (Dennis K.); Fox, Jay; Swim, Cynthia

    2004-01-01

    The overall objective is to assess the detection performance of LWIR (long wavelength infrared) coherent Lidar systems that potentially possess enhanced effluent detection capabilities. Previous work conducted by Los Alamos has demonstrated that infrared DIfferential Absorption Lidar (DIAL) is capable of detecting chemicals in plumes from long standoff ranges. Our DIAL approach relied on the reflectivity of topographical targets to provide a strong return signal. With the inherent advantage of applying heterodyne transceivers to approach single-photon detection in LWIR, it is projected that marked improvements in detection range or in spatial coverage can be attained. In some cases, the added photon detection sensitivity could be utilized for sensing 'soft targets', such as atmospheric and threat aerosols where return signal strength is drastically reduced, as opposed to topographical targets. This would allow range resolved measurements and could lead to the mitigation of the limiting source of noise due to spectral/spatial/temporal variability of the ground scene. The ability to distinguish normal variations in the background from true chemical signatures is crucial to the further development of sensitive remote chemical sensing technologies. One main difficulty in demonstrating coherent DIAL detection is the development of suitable heterodyne transceivers that can achieve rapid multi-wavelength tuning required for obtaining spectral signature information. LANL has recently devised a novel multi-wavelength heterodyne transceiver concept that addresses this issue. A 5-KHz prototype coherent CO{sub 2} transceiver has been constructed and is being now used to help address important issues in remote CBW agent standoff detection. Laboratory measurements of signal-to-noise ratio (SNR) will be reported. Since the heterodyne detection scheme fundamentally has poor shot-to-shot signal statistics, in order to achieve sensitive detection limits, favorable averaging statistics have to be validated. The baseline coherent DIAL detection sensitivity that can be achieved averaging multiple laser pulses and by comparisons of different wavelengths will be demonstrated. Factors that are presently limiting performance and attempts to circumvent these issues will be discussed.

  4. 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

  5. Mercury speciation driven by seasonal changes in a contaminated estuarine environment

    SciTech Connect (OSTI)

    Bratki?, Arne, E-mail: arne.bratkic@ijs.si [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia)] [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia); Ogrinc, Nives, E-mail: nives.orginc@ijs.si [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia)] [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia); Kotnik, Jože, E-mail: joze.kotnik@ijs.si [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia)] [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia); Faganeli, Jadran, E-mail: faganeli@mbss.org [Marine Biology Station, Forna?e 41, 6330 Piran (Slovenia)] [Marine Biology Station, Forna?e 41, 6330 Piran (Slovenia); Žagar, Dušan, E-mail: dusan.zagar@fgg.uni-lj.si [Faculty of Civil and Geodetic Engineering, Jamova 2, 1000 Ljubljana (Slovenia)] [Faculty of Civil and Geodetic Engineering, Jamova 2, 1000 Ljubljana (Slovenia); Yano, Shinichiro [Faculty of Engineering, Kyushu University, Fukuoka 812-8581 (Japan)] [Faculty of Engineering, Kyushu University, Fukuoka 812-8581 (Japan); Tada, Akihide, E-mail: tada@civil.nagasaki-u.ac.jp [Faculty of Engineering, Nagasaki University, Bunkyo-machi 1-14, Nagasaki 852-8521 (Japan)] [Faculty of Engineering, Nagasaki University, Bunkyo-machi 1-14, Nagasaki 852-8521 (Japan); Horvat, Milena, E-mail: milena.horvat@ijs.si [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia)] [Department of Environmental Sciences, Jožef Stefan Institute, Jamova 39, 1000 Ljubljana (Slovenia)

    2013-08-15

    In this study, seasonal changes of mercury (Hg) species in the highly variable estuary of So?a/Isonzo River (northern Adriatic Sea) were investigated. Samplings were performed on a seasonal basis (September 2009, May, August and October 2010) and Hg species (total Hg, methylmercury (MeHg), dissolved gaseous Hg (DGM)) in waters, sediments and pore waters were determined. In addition, a range of ancillary parameters were measured (salinity, nutrients, organic carbon (OC), nitrogen species). Hg values were interpreted using these parameters and hydrological conditions (river flow, wave height) around the time of sampling. There were no significant changes in Hg load from river to the gulf, compared to previous studies. The load was temporarily higher in May 2010 due to higher river flow. Wave height, through changing hydrostatic pressure, was most likely to cause resuspension of already deposited Hg from the bottom (August 2010). The estuary is a net source of DGM to the atmosphere as suggested by DGM profiles, with salinity, redox potential and organic matter as the most probable controls over its production. MeHg is produced in situ in sediment or in water column, rather than transported by river, as indicated by its correlation with OC of the marine origin. Calculated fluxes for THg and MeHg showed sediment as a source for both the water column. In pore waters, OC in part affects partitioning of both THg and MeHg; however other factors (e.g. sulphide and/or oxyhydroxides precipitation and dissolution) are also probably important. -- Highlights: ? Water, sediment and pore water mercury species in front of So?a River estuary were measured. ? Seasonally variable hydrological conditions were shown to influence water column Hg speciation. ? Fluxes for total Hg and MeHg from sediment to water were calculated. ? Sediment is a source of total Hg and MeHg to the water column. ? Correlation of MeHg with organic carbon of marine origin suggests in situ formation.

  6. 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.

  7. Fate and Speciation of Gasoline-Derived Lead in Organic Horizons of the Northeastern USA

    SciTech Connect (OSTI)

    Kaste,J.; Bostick, B.; Friedland, A.; Schroth, A.; Siccama, T.

    2006-01-01

    Although legislation in the late 1970s significantly reduced atmospheric lead (Pb) inputs to ecosystems in North America, organic (O) horizons in forests of the northeastern USA still contain up to 30 kg of gasoline-derived Pb ha{sup -1}. The residence time, geochemical behavior, and fate of this contaminant Pb in soils is poorly understood. Here we use forest floor time series data and synchrotron-based X-ray techniques to examine the mobility and speciation of Pb in O horizons collected from remote sites across the northeastern USA. At high elevation (>800 m) sites in Vermont and New York, samples collected from similar locations in 1980, 1990, and early 2000 had indistinguishable Pb contents, ranging ({+-}1{sigma}) from 11 to 29 kg Pb ha{sup -1}. However, at lower elevation and lower latitude sites with mixed vegetation, significant decreases in Pb amount were observed during the two-decade study period. Lower elevation sites ranged from 10 to 20 kg Pb ha{sup -1} in 1980, and from 2 to 10 kg Pb ha{sup -1} 20 yr later. Lead-enriched soil grains were determined to be amorphous with microfocused X-ray diffraction, and Pb concentrations correlated well with Fe on maps generated via microfocused X-ray fluorescence. Bulk Pb L{sub III}-edge X-ray absorption spectroscopy of coniferous O horizon samples indicate that Pb is binding to iron-rich soil particles by inner-sphere complexes, most likely to amorphous Fe oxides. Based on our paired regional and microscopic observations, we conclude that Pb is strongly retained in well-drained O horizons, and mobility is governed by decomposition and colloidal transport.

  8. 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.

  9. 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.

  10. 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.

  11. Chemical Management Contacts

    Broader source: Energy.gov [DOE]

    Contacts for additional information on Chemical Management and brief description on Energy Facility Contractors Group

  12. 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.

  13. X-RAY METHODS FOR THE CHEMICAL CHARACTERIZATION OF ATMOSPHERIC AEROSOLS

    E-Print Network [OSTI]

    Jaklevic, J.M.

    2010-01-01

    for the routine analysis of air pollution samples, itof x-ray methods to the analysis of air particulate samples.

  14. The impact of meteorological conditions and variation in chemical composition of aerosols on regional cloud formation

    E-Print Network [OSTI]

    Creamean, Jessie Marie

    2012-01-01

    Atmospheric Analytical Chemistry, Analytical Chemistry, 83 (Particles in Seconds, Analytical Chemistry, 76 (2), 373-378,particles in seconds, Analytical Chemistry, 76 (2), 373-378,

  15. Measurements of the chemical, physical, and optical properties of single aerosol particles

    E-Print Network [OSTI]

    Moffet, Ryan Christopher

    2007-01-01

    Index and Density Analytical Chemistry 77, 6535-6541.mass spectrometer, Analytical Chemistry, 78 (24), 8281-8289,instrumentation, Analytical Chemistry, 77 (12), 3861-3885,

  16. The impact of meteorological conditions and variation in chemical composition of aerosols on regional cloud formation

    E-Print Network [OSTI]

    Creamean, Jessie Marie

    2012-01-01

    modelling: a review, Atmospheric Chemistry and Physics, 5,aliphatic amines, Atmospheric Chemistry and Physics, 7 (9),of carbon monoxide, Atmospheric Chemistry and Physics,

  17. Measurements of the chemical, physical, and optical properties of single aerosol particles

    E-Print Network [OSTI]

    Moffet, Ryan Christopher

    2007-01-01

    and M.J. Molina: Mexico City basin wind circulation duringDistinct wind convergence patterns in the Mexico City basinMexico City was strongly influenced by continually changing emission sources and strong winds

  18. Chemical Sinks of Organic Aerosol: Kinetics and Products of the Heterogeneous Oxidation of Erythritol and Levoglucosan

    E-Print Network [OSTI]

    Kessler, Sean Herbert

    The heterogeneous oxidation of pure erythritol (C[subscript 4]H[subscript 10]O[subscript 4]) and levoglucosan (C[subscript 6]H[subscript 10]O[subscript 5]) particles was studied in order to evaluate the effects of atmospheric ...

  19. Correlations between Optical, Chemical and Physical Properties of Biomass Burn Aerosols

    E-Print Network [OSTI]

    2008-01-01

    laboratory measurements of biomass-burning emissions: 1.tar balls: Particles from biomass and biofuel burning, J.Eleuterio (2005), A review of biomass burning emissions part

  20. The impact of meteorological conditions and variation in chemical composition of aerosols on regional cloud formation

    E-Print Network [OSTI]

    Creamean, Jessie Marie

    2012-01-01

    biomass burning, dust, fly ash, sea salt, and other minorchemistry was dominated by fly ash (33%) produced duringcontaining particles, fly ash, and dust decreased while the

  1. Parameterizing the Mixing State of Complex Submicron Aerosols Using Chemical Imaging

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration wouldMass mapSpeeding access| Department ofStephen PSeptember|March Study2065 Unlimited

  2. 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

  3. 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

  4. Phase partitioning and volatility of secondary organic aerosol components formed from ?-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

  5. Phase partitioning and volatility of secondary organic aerosol components formed from ?-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

  6. Methods for analyzing the concentration and speciation of major and trace elements in marine particles

    E-Print Network [OSTI]

    2015-01-01

    Goldberg, E.D. , 1954. Marine geochemistry 1. ChemicalNorth Atlantic Ocean: A16N. Marine Chemistry, 142–144, 41-2009. The Arctic Ocean marine carbon cycle: evaluation of

  7. Lubricating Oil Dominates Primary Organic Aerosol Emissions from Motor Vehicles

    E-Print Network [OSTI]

    Goldstein, Allen

    Lubricating Oil Dominates Primary Organic Aerosol Emissions from Motor Vehicles David R. Worton to "fresh" lubricating oil. The gas chromatography retention time data indicates that the cycloalkane ring with lubricating oil being the dominant source from both gasoline and diesel-powered vehicles, with an additional

  8. Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

    SciTech Connect (OSTI)

    Gerstl, S.A.W.; Zardecki, A.

    1981-08-01

    The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10/sup 1/ g is sufficient to reduce photosynthesis to 10/sup -3/ of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated.

  9. Detection of UV-absorbing aerosols using GOME and SCIAMACHY

    E-Print Network [OSTI]

    Graaf, Martin de

    using GOME and SCIAMACHY · Conclusions and Outlook #12;Last step: Only positive residues are considered-Adding KNMI Radiative Transfer Model Solar zenith angle = 30° Viewing zenith angle = 0° Surface albedo = 5% #12; Reflectance at TOA with absorbing aerosols Doubling-Adding KNMI Radiative Transfer Model Solar

  10. The coupling of winds, aerosols and chemistry in Titan's atmosphere

    E-Print Network [OSTI]

    Hourdin, Chez Frédéric

    REVIEW The coupling of winds, aerosols and chemistry in Titan's atmosphere BY SEBASTIEN LEBONNOIS 1'Ae´ronomie, IPSL, CNRS, BP3, 91371 Verrie`res le Buisson, France The atmosphere of Titan is a complex system, where the observed atmospheric structure of Titan's lower atmosphere (mainly in the stratosphere and troposphere

  11. 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.

  12. 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.

  13. DIESEL AEROSOL SAMPLING METHODOLOGY -CRC E-43 EXECUTIVE SUMMARY

    E-Print Network [OSTI]

    Minnesota, University of

    ) was to develop Diesel aerosol sampling methods for the laboratory that would produce particle size distributions used to evaluate and select basic options, or to perform feasibility studies or preliminary assessments, and dilution with ambient air. A small amount of these nuclei mode particles contain solid ash from lube oil

  14. 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 satellite 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 previousmore »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

  15. 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.

  16. Source Attribution of Light Absorbing Aerosol in Arctic Snow

    E-Print Network [OSTI]

    Source Attribution of Light Absorbing Aerosol in Arctic Snow (Preliminary analysis of 2008 Biomass/poll. Factor: all data Pollution factor: depth data #12;2009 Data set for receptor modeling with limited analytes Factor 1: biomass Factor 2: pollution Factor 3: marine Factor 4: biomass #12;Factor

  17. Design of high efficiency blowers for future aerosol applications 

    E-Print Network [OSTI]

    Chadha, Raman

    2007-04-25

    High efficiency air blowers to meet future portable aerosol sampling applications were designed, fabricated, and evaluated. A Centrifugal blower was designed to achieve a flow rate of 100 L/min (1.67 x 10^-3 m^3/s) and a pressure rise of WC " 4...

  18. Aerosol Synthesis and Growth Mechanism of Magnetic Iron Nanoparticles

    E-Print Network [OSTI]

    rapidly over the past decades, such as mechanical milling, spray drying, sol-gel, sonochemistry, etcAerosol Synthesis and Growth Mechanism of Magnetic Iron Nanoparticles D. Kim1,a , E.S. Vasilieva2,b, evaporated and transported by carrier gas flow to the preliminary heated tubular furnace for decomposition

  19. 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.

  20. CLouds and Aerosol Radiative Interaction and Forcing Investigation

    E-Print Network [OSTI]

    Graaf, Martin de

    Radiative Interaction and Forcing Investigation Version 1.0 Date March 2012 Status Final #12;#12;CLARIFI, by absorbing and scattering solar radiation, and more importantly, by modifying cloud propertiesCLARIFI CLouds and Aerosol Radiative Interaction and Forcing Investigation M. de Graaf, L

  1. Halophilic Archaea determined from geothermal steam vent aerosols

    E-Print Network [OSTI]

    Kelley, Scott

    Halophilic Archaea determined from geothermal steam vent aerosols Dean G. Ellis, Richard W. Bizzoco Hydrothermal vents, known as `fumaroles', are ubiq- uitous features of geothermal areas. Although their geology contained halophilic Archaea closely related to the Haloarcula spp. found in non-geothermal salt mats

  2. 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.

  3. Variability of Aerosol Optical Properties from Long-term

    E-Print Network [OSTI]

    Delene, David J.

    aerosols and overestimates absorption due to suspended particles by about 20-30%. Green L E D Opal Glas s O Photometer · Principle of operation is to measure the change in light transmission through a filter on which light extinction and light scattering. · Instrument exhibits a significant response to nonabsorbing

  4. Impact of anthropogenic absorbing aerosols on clouds and precipitation

    E-Print Network [OSTI]

    Impact of anthropogenic absorbing aerosols on clouds and precipitation: A review of recent and precipitation: A review of recent progresses Chien Wang Massachusetts Institute of Technology, E19-439K, 77 atmospheric circulation, and hence clouds and precipitation. Recent studies have suggested that the changes

  5. IMPACT OF AEROSOLS ON CONVECTIVE CLOUDS AND PRECIPITATION

    E-Print Network [OSTI]

    Zeng, Ning

    IMPACT OF AEROSOLS ON CONVECTIVE CLOUDS AND PRECIPITATION Wei-Kuo Tao,1 Jen-Ping Chen,2 Zhanqing Li effects on clouds could further extend to precipitation, both through the formation of cloud particles mechan- isms behind these effects, in particular, the ones connected to precipitation, are not yet well

  6. CLOUD DROPLET NUCLEATION AND ITS CONNECTION TO AEROSOL PROPERTIES

    E-Print Network [OSTI]

    influence the earth's radiation balance and climate directly, by scanering shortwave (solar) radiation in the earth radiation budget over the industrial period. exerting a radiative forcing that is of comparable. Keywords - Climate. aerosols. clouds, radiation INTRODUcnON In recent years awareness has increased

  7. 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.

  8. 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.

  9. 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

  10. Sources and Composition of Submicron Organic Mass in Marine Aerosol Particles

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

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

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMAP) 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

  11. 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

  12. 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.

  13. 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.

  14. Abstract No. Graf0532 The Speciation of Arsenate (As (V)) at the Goethite-Water Interface in the Presence of Zinc (II)

    E-Print Network [OSTI]

    Sparks, Donald L.

    Abstract No. Graf0532 The Speciation of Arsenate (As (V)) at the Goethite-Water Interface investigating the sorption behavior of As (V) at the goethite-water interface in the presence of Zn cations(II) were reacted simultaneously in 2.5 g L -1 suspensions of goethite at pH 4 and 7 with initial

  15. 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.

  16. Geogenic Nickel Speciation in Serpentine Soils and Its Relationship to Nickel Uptake in Hyperaccumulator Plants. Tuesday, November 3, 2009: 3:00 PM

    E-Print Network [OSTI]

    Sparks, Donald L.

    Geogenic Nickel Speciation in Serpentine Soils and Its Relationship to Nickel Uptake Siebecker1, Tiziana Centofanti2, Rufus Chaney2 and Donald Sparks1, (1)Plant and Soil Sciences, Univ to extract pollutants from soil. Some can accumulate up to 20g/kg nickel in dry shoot biomass. This ability

  17. Carbon dioxide in silica-undersaturated melt Part I: The effect of mixed alkalis (K and Na) on CO2 solubility and speciation.

    E-Print Network [OSTI]

    Boyer, Edmond

    . These low-silica melts can dissolve a large quantity of CO2 and are rich in alkalis. However, the way CO2 experimental results on the CO2 solubility and speciation in synthetic nephelinite in the NKCMAS system, equilibrated at high-pressure (50-300 MPa), high-temperature (1250C) with an excess C-O-H fluid phase

  18. Ni SPECIATION IN A HUMIC ACID-KAOLINITE SYSTEM Maarten Nachtegaal,l Elham A. Ghabbour,2 Geoffrey Davies2and Donald L. Sparks}

    E-Print Network [OSTI]

    Sparks, Donald L.

    Ni SPECIATION IN A HUMIC ACID-KAOLINITE SYSTEM Maarten Nachtegaal,l Elham A. Ghabbour,2 Geoffrey and desorption experiments of Ni to a kaolinite-humic acid complex (containing both 1 and 5 wt% HA). Selected structure spectroscopy (XANES) studies will be used to describe interactions of humic acids with kaolinite

  19. 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.

  20. 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.

  1. 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).

  2. 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.

  3. 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 (10–20 km) until 5–10 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).

  4. Chemical Sciences Division - CSD

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

    CSD Chemical Sciences Division CSD Organization Contact List Search Other Links Research Areas Research Highlights Organization Contacts Publications Awards Employment...

  5. MECS 2006- Chemicals

    Broader source: Energy.gov [DOE]

    Manufacturing Energy and Carbon Footprint for Chemicals Sector (NAICS 325) with Total Energy Input, October 2012 (MECS 2006)

  6. Long-term impacts of aerosols on vertical development of cloud and precipitation

    SciTech Connect (OSTI)

    Li Z.; Liu Y.; Niu, F.; Fan, J.; Rosenfeld, D.; Ding, Y.

    2011-11-13

    Aerosols alter cloud density and the radiative balance of the atmosphere. This leads to changes in cloud microphysics and atmospheric stability, which can either suppress or foster the development of clouds and precipitation. The net effect is largely unknown, but depends on meteorological conditions and aerosol properties. Here, we examine the long-term impact of aerosols on the vertical development of clouds and rainfall frequencies, using a 10-year dataset of aerosol, cloud and meteorological variables collected in the Southern Great Plains in the United States. We show that cloud-top height and thickness increase with aerosol concentration measured near the ground in mixed-phase clouds-which contain both liquid water and ice-that have a warm, low base. We attribute the effect, which is most significant in summer, to an aerosol-induced invigoration of upward winds. In contrast, we find no change in cloud-top height and precipitation with aerosol concentration in clouds with no ice or cool bases. We further show that precipitation frequency and rain rate are altered by aerosols. Rain increases with aerosol concentration in deep clouds that have a high liquid-water content, but declines in clouds that have a low liquid-water content. Simulations using a cloud-resolving model confirm these observations. Our findings provide unprecedented insights of the long-term net impacts of aerosols on clouds and precipitation.

  7. Chemical Zeolites Combinatorial . . .

    E-Print Network [OSTI]

    Servatius, Brigitte

    Chemical Zeolites Combinatorial . . . Realization 2d Zeolites Finite Zeolites The Layer . . . Holes University (Brigitte Servatius -- WPI) #12;Chemical Zeolites Combinatorial . . . Realization 2d Zeolites. Chemical Zeolites · crystalline solid · units: Si + 4O Si O O O O · two covalent bonds per oxygen #12

  8. Department of Chemical Engineering

    E-Print Network [OSTI]

    Zhigilei, Leonid V.

    Developing Leaders of Innovation Department of Chemical Engineering #12;At the University of Virginia, we educate students in traditional and nontraditional areas of chemical engineering, giving them.Va. Department of Chemical Engineering benefit from a modern academic curriculum and state

  9. Equilibrium Chemical Engines

    E-Print Network [OSTI]

    Tatsuo Shibata; Shin-ichi Sasa

    1997-10-30

    An equilibrium reversible cycle with a certain engine to transduce the energy of any chemical reaction into mechanical energy is proposed. The efficiency for chemical energy transduction is also defined so as to be compared with Carnot efficiency. Relevance to the study of protein motors is discussed. KEYWORDS: Chemical thermodynamics, Engine, Efficiency, Molecular machine.

  10. HARVARD UNIVERSITY CHEMICAL BIOLOGY

    E-Print Network [OSTI]

    Church, George M.

    HARVARD UNIVERSITY CHEMICAL BIOLOGY PHD PROGRAM 2013-2014 Student Handbook #12;Program Contacts at the beginning of each semester. Laboratory Rotations Students in the Chemical Biology Program are expected an interest in having Chemical Biology Program Students in their labs. Students may rotate in the labs

  11. High-temperature aerosol formation in wood pellets flames: Spatially resolved measurements

    SciTech Connect (OSTI)

    Wiinikka, Henrik; Gebart, Rikard [Energy Technology Centre, Box 726, S-941 28 Piteaa (Sweden); Boman, Christoffer; Bostroem, Dan; Nordin, Anders; OEhman, Marcus [Energy Technology and Thermal Process Chemistry, Umeaa University, S-901 87 Umeaa (Sweden)

    2006-12-15

    The formation and evolution of high-temperature aerosols during fixed bed combustion of wood pellets in a realistic combustion environment were investigated through spatially resolved experiments. The purpose of this work was to investigate the various stages of aerosol formation from the hot flame zone to the flue gas channel. The investigation is important both for elucidation of the formation mechanisms and as a basis for development and validation of particle formation models that can be used for design optimization. Experiments were conducted in an 8-kW-updraft fired-wood-pellets combustor. Particle samples were withdrawn from the centerline of the combustor through 10 sampling ports by a rapid dilution sampling probe. The corresponding temperatures at the sampling positions were in the range 200-1450{sup o}C. The particle sample was size-segregated in a low-pressure impactor, allowing physical and chemical resolution of the fine particles. The chemical composition of the particles was investigated by SEM/EDS and XRD analysis. Furthermore, the experimental results were compared to theoretical models for aerosol formation processes. The experimental data show that the particle size distribution has two peaks, both of which are below an aerodynamic diameter of 2.5 {mu}m (PM{sub 2.5}). The mode diameters of the fine and coarse modes in the PM{sub 2.5} region were {approx}0.1 and {approx}0.8 {mu}m, respectively. The shape of the particle size distribution function continuously changes with position in the reactor due to several mechanisms. Early, in the flame zone, both the fine mode and the coarse mode in the PM{sub 2.5} region were dominated by particles from incomplete combustion, indicated by a significant amount of carbon in the particles. The particle concentrations of both the fine and the coarse mode decrease rapidly in the hot oxygen-rich flame due to oxidation of the carbon-rich particles. After the hot flame, the fine mode concentration and particle diameter increase gradually when the temperature of the flue gas drops. The main contribution to this comes from condensation on preexisting particles in the gas of alkali sulfates, alkali chlorides, and Zn species formed from constituents vaporized in the fuel bed. The alkali sulfates were found to condense at a temperature of {approx}950{sup o} and alkali chlorides condensed later at {approx}600{sup o}. This agrees well with results of chemical equilibrium calculation of the gas-to-particle conversion temperature. After the hot flame the coarse mode concentration decreased very little when the flue gas was cooled. In addition to carbon, the coarse mode consists of refractory metals and also considerable amounts of alkali. (author)

  12. 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.

  13. Chemical Hygiene and Safety Plan

    E-Print Network [OSTI]

    Ricks Editor, R.

    2009-01-01

    V. , Ed. , Safety in the Chemical Laboratory. J. Chem.Łd. Amer/can Chemical Society. Easlon. PA. 18042. Vol. Lof Laboratory Safety. the Chemical Rubber Company Cleveland.

  14. Siphons in Chemical Reaction Networks

    E-Print Network [OSTI]

    Shiu, Anne; Sturmfels, Bernd

    2010-01-01

    strongly-connected chemical reaction, and the compu- tationcredited. Siphons in Chemical Reaction Networks Referencesto persistence analysis in chemical reaction networks. In:

  15. Solid-water detoxifying reagents for chemical and biological agents

    DOE Patents [OSTI]

    Hoffman, Dennis M. (Livermore, CA); Chiu, Ing Lap (Castro Valley, CA)

    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.

  16. Ferrocyanide Safety Program: Analysis of postulated energetic reactions and resultant aerosol generation in Hanford Site Waste Tanks

    SciTech Connect (OSTI)

    Postma, A.K. [G and P Consulting, Inc., Dallas, OR (United States); Dickinson, D.R. [Westinghouse Hanford Co., Richland, WA (United States)

    1995-09-01

    This report reviews work done to estimate the possible consequences of postulated energetic reactions in ferrocyanide waste stored in underground tanks at the Hanford Site. The issue of explosive reactions was raised in the 1987 Environmental Impact Statement (EIS), where a detonation-like explosion was postulated for the purpose of defining an upper bound on dose consequences for various disposal options. A review of the explosion scenario by the General Accounting Office (GAO) indicated that the aerosol generation and consequent radioactive doses projected for the explosion postulated in the EIS were understated by one to two orders of magnitude. The US DOE has sponsored an extensive study of the hazard posed by uncontrolled exothermic reactions in ferrocyanide waste, and results obtained during the past three years have allowed this hazard to be more realistically assessed. The objective of this report is to summarize the improved knowledge base that now indicates that explosive or vigorous chemical reactions are not credible in the ferrocyanide waste stored in underground tanks. This improved understanding supports the decision not to proceed with further analyses or predictions of the consequences of such an event or with aerosol tests in support of such predictions. 53 refs., 2 tabs.

  17. 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 Facility’s (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.

  18. The AeroCom Evaluation and Intercomparison of Organic Aerosol in Global Models

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

    Tsigaridis, Kostas [Columbia Univ., New York, NY (United States). Center for Climate Systems Research; NASA Goddard Inst. for Space Studies, New York, NY (United States); Daskalakis, N. [Univ. of Crete, Heraklion (Greece). Environmental Chemical Processes Lab.; Foundation for Research and Technology Hellas, Patras (Greece); Inst. of Chemical Engineering; Kanakidou, M. [Univ. of Crete, Heraklion (Greece). Environmental Chemical Processes Lab.; ; Adams, P. J. [Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Civil and Environmental Engineering and Dept. of Engineering and Public Policy; Artaxo, Paulo [Univ. of Sao Paulo (Brazil). Dept of Applied Physics; Bahadur, R. [Univ. of California, San Diego, CA (United States). Scripps Inst. of Oceanography; Balkanski, Y. [Lab. des Sciences du Climat et de l'Environnement, Gif-sur-Yvette (France); Bauer, S. [Columbia Univ., New York, NY (United States). Center for Climate Systems Research; NASA Goddard Inst. for Space Studies, New York, NY (United States); Bellouin, N. [Met Office Hadley Centre, Exeter (United Kingdom); Benedetti, Angela [ECMWF, Reading (United Kingdom); Bergman, T. [Finnish Meteorological Inst., Kuopio (Finland); Berntsen, T. [Univ. of Oslo (Norway). Dept. of Geosciences; CICERO, Oslo (Norway); Beukes, J. P. [North-West Univ., Potchestroom (South Africa). Environmental Sciences and Management; Bian, Huisheng [Univ. of Maryland, Baltimore County, MD (United States). Joint Center for Environmental Technology; Carslaw, K. S. [Univ. of Leeds (United Kingdom). School of Earth and Environment; Chin, M. [NASA Goddard Space Flight Center (GSFC), Greenbelt, MD (United States); Curci, Gabriele [Univ. of L'Aquila (Italy). Dept of Physics CETEMPS; Diehl, Thomas [NASA Goddard Space Flight Center (GSFC) and Universities Space Research Association, Greenbelt, MD (United States); Easter, Richard C. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Ghan, Steven J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Gong, S. [Meteorological Service of Canada, Toronto (Canada). Air Quality Research Branch; Hodzic, Alma [National Center for Atmospheric Research, Boulder, CO (United States); Hoyle, Christopher R. [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Swiss Federal Inst. for Forest Snow and Landscape Research (WSL) - Inst. for Snow and Avalanche Research (SLF), Davos (Switzerland); Iversen, T. [ECMWF, Reading (United Kingdom); Univ. of Oslo (Norway). Dept. of Geosciences; Norwegian Meteorological Inst., Oslo (Norway); Jathar, S. [Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Civil and Environmental Engineering; Jimenez, J. L. [Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Biochemistry; Kaiser, J. W. [ECMWF, Reading (United Kingdom); King's College London (United Kingdom). Dept. of Geography; Max Planck Society, Mainz (Germany). Max Planck Inst. for Chemistry, Dept. of Atmospheric Chemistry; ; Kirkevag, A. [Norwegian Meteorological Inst., Oslo (Norway); Koch, Dorothy [Columbia Univ., New York, NY (United States). Center for Climate Systems Research; NASA Goddard Inst. for Space Studies, New York, NY (United States); Kokkola, H. [Finnish Meteorological Inst., Kuopio (Finland); Lee, Y. H. [Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Civil and Environmental Engineering; Lin, G. [Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic, and Space Science; Liu, Xiaohong [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Luo, Gan [State Univ. of New York (SUNY), Albany, NY (United States); Ma, Xiaoyan [Environment Canada, Victoria, BC (Canada); Mann, G. W. [Univ. of Leeds (United Kingdom). National Centre for Atmospheric Science and School of Earth and Environment; Mihalopoulos, Nikos [Univ. of Crete, Heraklion (Greece). Environmental Chemical Processes Lab.; Morcrette, J. -J. [ECMWF, Reading (United Kingdom); Muller, J. F. [Belgian Inst. for Space Aeronomy, Brussels (Belgium); Myhre, G. [Center for International Climate and Environmental Research (CICERO), Oslo (Norway)

    2014-01-01

    This paper evaluates the current status of global modeling of the organic aerosol (OA) occurrence in the troposphere and analyzes the differences calculated between models as well as between models and observations. Thirty-one global chemistry/transport and general circulation models have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over an order of magnitude exists in the modeled vertical distribution of OA that deserves a dedicated future study. Furthermore, although the OA/OC ratio depends on OA sources and atmospheric processing and is important for model evaluation against OA and OC observations, it is resolved only by few global models. The median global primary OA source strength is 56 Tg a-1 (range 34 - 144 Tg a-1) and the median secondary OA source strength (natural and anthropogenic) is 19 Tg a-1 (range 13-121 Tg a-1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a-1 (range 16-121 Tg a-1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a-1; range 13-20 Tg a-1, with one model at 37 Tg a-1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6-2.0 Tg and 4 between 2.4-3.8 Tg) with a median OA lifetime of 5.4 days (range 3.8-9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio of is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a-1 (range 28-209 Tg a-1), which is on average 85% of the total OA deposition.

  19. Speciation and mobility of Zn, Cu and Pb in a truck farming soil

    E-Print Network [OSTI]

    Geochemistry Group, LGIT, Université J. Fourier, CNRS, BP. 53, 38041 Grenoble cedex 9, France 2 Advanced Light by chemical treatments and advanced x-ray techniques. Elemental associations and forms of metals were-dried and fractionated by sieving and centrifuging at 2000, 600, 200, 50, 20 and 2 um. Sandy fractions (2000-200 and 200

  20. Wyss Institute Chemical Hygiene Plan CHEMICAL HYGIENE PLAN

    E-Print Network [OSTI]

    Napp, Nils

    Wyss Institute Chemical Hygiene Plan CHEMICAL HYGIENE PLAN The Wyss Institute for Biologically Inspired Engineering June 2015 #12;Wyss Institute Chemical Hygiene Plan TABLE OF CONTENTS 1.0 POLICY..........................................................................................2 2.1 CHEMICAL HYGIENE OFFICER