National Library of Energy BETA

Sample records for homogeneous catalysis heterogeneous

  1. Converting Homogeneous to Heterogeneous in Electrophilic Catalysis using Monodisperse Metal Nanoparticles

    SciTech Connect (OSTI)

    Witham, Cole A.; Huang, Wenyu; Tsung, Chia-Kuang; Kuhn, John N.; Somorjai, Gabor A.; Toste, F. Dean

    2009-10-15

    A continuing goal in catalysis is the transformation of processes from homogeneous to heterogeneous. To this end, nanoparticles represent a new frontier in heterogeneous catalysis, where this conversion is supplemented by the ability to obtain new or divergent reactivity and selectivity. We report a novel method for applying heterogeneous catalysts to known homogeneous catalytic reactions through the design and synthesis of electrophilic platinum nanoparticles. These nanoparticles are selectively oxidized by the hypervalent iodine species PhICl{sub 2}, and catalyze a range of {pi}-bond activation reactions previously only homogeneously catalyzed. Multiple experimental methods are utilized to unambiguously verify the heterogeneity of the catalytic process. The discovery of treatments for nanoparticles that induce the desired homogeneous catalytic activity should lead to the further development of reactions previously inaccessible in heterogeneous catalysis. Furthermore, our size and capping agent study revealed that Pt PAMAM dendrimer-capped nanoparticles demonstrate superior activity and recyclability compared to larger, polymer-capped analogues.

  2. ISHHC XIII International Symposium on the Relations betweenHomogeneous and Heterogeneous Catalysis

    SciTech Connect (OSTI)

    Somorjai , G.A.

    2007-06-11

    The International Symposium on Relations between Homogeneous and Heterogeneous Catalysis (ISHHC) has a long and distinguished history. Since 1974, in Brussels, this event has been held in Lyon, France (1977), Groeningen, The Netherlands (1981); Asilomar, California (1983); Novosibirsk, Russia (1986); Pisa, Italy (1989); Tokyo, Japan (1992); Balatonfuered, Hungary (1995); Southampton, United Kingdom (1999); Lyon, France (2001); Evanston, Illinois (2001) and Florence, Italy (2005). The aim of this international conference in Berkeley is to bring together practitioners in the three fields of catalysis, heterogeneous, homogeneous and enzyme, which utilize mostly nanosize particles. Recent advances in instrumentation, synthesis and reaction studies permit the nanoscale characterization of the catalyst systems, often for the same reaction, under similar experimental conditions. It is hoped that this circumstance will permit the development of correlations of these three different fields of catalysis on the molecular level. To further this goal we aim to uncover and focus on common concepts that emerge from nanoscale studies of structures and dynamics of the three types of catalysts. Another area of focus that will be addressed is the impact on and correlation of nanosciences with catalysis. There is information on the electronic and atomic structures of nanoparticles and their dynamics that should have importance in catalyst design and catalytic activity and selectivity.

  3. Homogeneous and Interfacial Catalysis in 3D Controlled Environment | The

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

    Ames Laboratory Homogeneous and Interfacial Catalysis in 3D Controlled Environment FWP/Project Description: Project Leader(s): Marek Pruski Principal Investigators: Marek Pruski, Aaron Sadow, Igor Slowing Key Scientific Personnel: Takeshi Kobayashi This collaborative research effort is geared toward bringing together the best features of homogeneous and heterogeneous catalysis for developing new catalytic principles. Novel silica-based, single-site mesoporous catalysts with controlled,

  4. Is It Homogeneous or Heterogeneous Catalysis Derived from [RhCp*Cl2]2? In Operando-XAFS, Kinetic and Crucial Kinetic Poisoning Evidence for Subnanometer Rh4 Cluster-Based Benzene Hydrogenation Catalysis

    SciTech Connect (OSTI)

    Bayram, Ercan; Linehan, John C.; Fulton, John L.; Roberts, John A.; Szymczak, Nathaniel; Smurthwaite, Tricia D.; Ozkar, Saim; Balasubramanian, Mahalingam; Finke, Richard G.

    2011-11-23

    Determining the true, kinetically dominant catalytically active species, in the classic benzene hydrogenation system pioneered by Maitlis and co-workers 34 years ago starting with [RhCp*Cl2]2 (Cp* = [{eta}5-C5(CH3)5]), has proven to be one of the most challenging case studies in the quest to distinguish single-metal-based 'homogeneous' from polymetallic, 'heterogeneous' catalysis. The reason, this study will show, is the previous failure to use the proper combination of (i) operando spectroscopy to determine the dominant form(s) of the precatalyst's mass under catalysis (i.e., operating) conditions, plus then and crucially also (ii) the previous lack of the necessary kinetic studies, catalysis being a 'wholly kinetic phenomenon' as J. Halpern long ago noted. An important contribution from this study will be to reveal the power of quantitiative kinetic poisoning experiments for distinguishing single-metal, or in this case subnanometer Rh4 cluster-based catalysis from larger, polymetallic Rh(0)n nanoparticle catalysis, at least under favorable conditions. The combined operando-XAFS (X-ray absorption fine structure) spectroscopy and kinetic evidences provide a compelling case for Rh4-based, with average stoichiometry 'Rh4Cp*2.4Cl4Hc', benzene hydrogenation catalysis in 2-propanol with added Et3N and at 100 C and 50 atm initial H2 pressure. The results also reveal, however, that if even ca. 1.4% of the total soluble Rh(0)n had formed nanoparticles, then those Rh(0)n nanoparticles would have been able to account for all the observed benzene hydrogenation catalytic rate (using commercial, ca. 2 nm, polyethyleneglycol-dodecylether hydrosol stabilized Rh(0)n nanoparticles as a model system). The results 'especially the poisoning methodology developed and employed' are of significant, broader interest since determining the nature of the true catalyst continues to be a central, often vexing issue in any and all catalytic reactions. The results are also of fundamental interest in that they add to a growing body of evidence indicating that certain, appropriately ligated, coordinatively unsaturated, subnanometer M4 transition-metal clusters can be relatively robust catalysts. Also demonstrated herein is that Rh4 clusters are poisoned by Hg(0), demonstrating for the first time that the classic Hg(0) poisoning test of 'homogeneous' vs 'heterogeneous'catalysts cannot distinguish Rh4-based subnanometer catalysts from Rh(0)n nanoparticle catalysts, at least for the present examples of these two specific, Rh-based catalysts.

  5. Reaction Selectivity in Heterogeneous Catalysis

    SciTech Connect (OSTI)

    Somorjai, Gabor A.; Kliewer, Christopher J.

    2009-02-02

    The understanding of selectivity in heterogeneous catalysis is of paramount importance to our society today. In this review we outline the current state of the art in research on selectivity in heterogeneous catalysis. Current in-situ surface science techniques have revealed several important features of catalytic selectivity. Sum frequency generation vibrational spectroscopy has shown us the importance of understanding the reaction intermediates and mechanism of a heterogeneous reaction, and can readily yield information as to the effect of temperature, pressure, catalyst geometry, surface promoters, and catalyst composition on the reaction mechanism. DFT calculations are quickly approaching the ability to assist in the interpretation of observed surface spectra, thereby making surface spectroscopy an even more powerful tool. HP-STM has revealed three vitally important parameters in heterogeneous selectivity: adsorbate mobility, catalyst mobility, and selective site-blocking. The development of size controlled nanoparticles from 0.8 to 10 nm, of controlled shape, and of controlled bimetallic composition has revealed several important variables for catalytic selectivity. Lastly, DFT calculations may be paving the way to guiding the composition choice for multi-metallic heterogeneous catalysis for the intelligent design of catalysts incorporating the many factors of selectivity we have learned.

  6. Control Heterogeneous Catalysis at Atomic and Electronic-level...

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

    Control Heterogeneous Catalysis at Atomic and Electronic-level Using Intermetallic Compounds Precious metals and metal alloys are important heterogeneous catalysts for renewable...

  7. Heterogeneous Catalysis for Thermochemical Conversion | Bioenergy | NREL

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

    Heterogeneous Catalysis for Thermochemical Conversion Our mission is to transform thermal biomass deconstruction products (syngas and pyrolysis oil) into the fuels and chemicals that keep society moving forward. Figure includes three panels. The first pane, labeled single-source precursors, depicts a bis(triphenylphosphine)rhodium(I) carbonyl chloride single-source precursor for producing rhodium phosphide nanoparticles, shown by a vertical line labeled PPh3 at the top, Rh in the middle, and

  8. Molecular-Level Design of Heterogeneous Chiral Catalysis

    SciTech Connect (OSTI)

    Francisco Zaera

    2012-03-21

    The following is a proposal to continue our multi-institutional research on heterogeneous chiral catalysis. Our team combines the use of surface-sensitive analytical techniques for the characterization of model systems with quantum and statistical mechanical calculations to interpret experimental data and guide the design of future research. Our investigation focuses on the interrelation among the three main mechanisms by which enantioselectivity can be bestowed to heterogeneous catalysts, namely: (1) by templating chirality via the adsorption of chiral supramolecular assemblies, (2) by using chiral modifiers capable of forming chiral complexes with the reactant and force enantioselective surface reactions, and (3) by forming naturally chiral surfaces using imprinting chiral agents. Individually, the members of our team are leaders in these various aspects of chiral catalysis, but the present program provides the vehicle to generate and exploit the synergies necessary to address the problem in a comprehensive manner. Our initial work has advanced the methodology needed for these studies, including an enantioselective titration procedure to identify surface chiral sites, infrared spectroscopy in situ at the interface between gases or liquids and solids to mimic realistic catalytic conditions, and DFT and Monte Carlo algorithms to simulate and understand chirality on surfaces. The next step, to be funded by the monies requested in this proposal, is to apply those methods to specific problems in chiral catalysis, including the identification of the requirements for the formation of supramolecular surface structures with enantioselective behavior, the search for better molecules to probe the chiral nature of the modified surfaces, the exploration of the transition from supramolecular to one-to-one chiral modification, the correlation of the adsorption characteristics of one-to-one chiral modifiers with their physical properties, in particular with their configuration, and the development of ways to imprint chiral centers on achiral solid surfaces. Chiral catalysis is not only a problem of great importance in its own right, but also the ultimate test of how to control selectivity in catalysis. The time is ripe for fundamental work in heterogeneous chiral catalysis to provide the U.S. with a leadership role in developing the next generation of catalytic processes for medicinal and agrochemical manufacturing. Our team provides the required expertise for a synergistic and comprehensive integration of physical and chemical experimentation with solid state and molecular reactivity theories to solve this problem.

  9. Application of solid ash based catalysts in heterogeneous catalysis

    SciTech Connect (OSTI)

    Shaobin Wang

    2008-10-01

    Solid wastes, fly ash, and bottom ash are generated from coal and biomass combustion. Fly ash is mainly composed of various metal oxides and possesses higher thermal stability. Utilization of fly ash for other industrial applications provides a cost-effective and environmentally friendly way of recycling this solid waste, significantly reducing its environmental effects. On the one hand, due to the higher stability of its major component, aluminosilicates, fly ash could be employed as catalyst support by impregnation of other active components for various reactions. On the other hand, other chemical compounds in fly ash such as Fe{sub 2}O{sub 3} could also provide an active component making fly ash a catalyst for some reactions. In this paper, physicochemical properties of fly ash and its applications for heterogeneous catalysis as a catalyst support or catalyst in a variety of catalytic reactions were reviewed. Fly-ash-supported catalysts have shown good catalytic activities for H{sub 2} production, deSOx, deNOx, hydrocarbon oxidation, and hydrocracking, which are comparable to commercially used catalysts. As a catalyst itself, fly ash can also be effective for gas-phase oxidation of volatile organic compounds, aqueous-phase oxidation of organics, solid plastic pyrolysis, and solvent-free organic synthesis. 107 refs., 4 figs., 2 tabs.

  10. Cryogenic homogenization and sampling of heterogeneous multi-phase feedstock

    DOE Patents [OSTI]

    Doyle, Glenn Michael (Lakewood, CO); Ideker, Virgene Linda (Arvada, CO); Siegwarth, James David (Boulder, CO)

    2002-01-01

    An apparatus and process for producing a homogeneous analytical sample from a heterogenous feedstock by: providing the mixed feedstock, reducing the temperature of the feedstock to a temperature below a critical temperature, reducing the size of the feedstock components, blending the reduced size feedstock to form a homogeneous mixture; and obtaining a representative sample of the homogeneous mixture. The size reduction and blending steps are performed at temperatures below the critical temperature in order to retain organic compounds in the form of solvents, oils, or liquids that may be adsorbed onto or absorbed into the solid components of the mixture, while also improving the efficiency of the size reduction. Preferably, the critical temperature is less than 77 K (-196.degree. C.). Further, with the process of this invention the representative sample may be maintained below the critical temperature until being analyzed.

  11. DOE Laboratory Catalysis Research Symposium - Abstracts

    SciTech Connect (OSTI)

    Dunham, T.

    1999-02-01

    The conference consisted of two sessions with the following subtopics: (1) Heterogeneous Session: Novel Catalytic Materials; Photocatalysis; Novel Processing Conditions; Metals and Sulfides; Nuclear Magnetic Resonance; Metal Oxides and Partial Oxidation; Electrocatalysis; and Automotive Catalysis. (2) Homogeneous Catalysis: H-Transfer and Alkane Functionalization; Biocatalysis; Oxidation and Photocatalysis; and Novel Medical, Methods, and Catalyzed Reactions.

  12. Highly Dispersed Pseudo-Homogeneous and Heterogeneous Catalysts Synthesized via Inverse Micelle Solutions for the Liquefaction of Coal

    SciTech Connect (OSTI)

    Hampden-Smith, M.; Kawola, J.S.; Martino, A.; Sault, A.G.; Yamanaka, S.A.

    1999-01-05

    The mission of this project was to use inverse micelle solutions to synthesize nanometer sized metal particles and test the particles as catalysts in the liquefaction of coal and other related reactions. The initial focus of the project was the synthesis of iron based materials in pseudo-homogeneous form. The frost three chapters discuss the synthesis, characterization, and catalyst testing in coal liquefaction and model coal liquefaction reactions of iron based pseudo-homogeneous materials. Later, we became interested in highly dispersed catalysts for coprocessing of coal and plastic waste. Bifunctional catalysts . to hydrogenate the coal and depolymerize the plastic waste are ideal. We began studying, based on our previously devised synthesis strategies, the synthesis of heterogeneous catalysts with a bifunctional nature. In chapter 4, we discuss the fundamental principles in heterogeneous catalysis synthesis with inverse micelle solutions. In chapter 5, we extend the synthesis of chapter 4 to practical systems and use the materials in catalyst testing. Finally in chapter 6, we return to iron and coal liquefaction now studied with the heterogeneous catalysts.

  13. Wavelet-based surrogate time series for multiscale simulation of heterogeneous catalysis

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

    Savara, Aditya Ashi; Daw, C. Stuart; Xiong, Qingang; Gur, Sourav; Danielson, Thomas L.; Hin, Celine N.; Pannala, Sreekanth; Frantziskonis, George N.

    2016-01-28

    We propose a wavelet-based scheme that encodes the essential dynamics of discrete microscale surface reactions in a form that can be coupled with continuum macroscale flow simulations with high computational efficiency. This makes it possible to simulate the dynamic behavior of reactor-scale heterogeneous catalysis without requiring detailed concurrent simulations at both the surface and continuum scales using different models. Our scheme is based on the application of wavelet-based surrogate time series that encodes the essential temporal and/or spatial fine-scale dynamics at the catalyst surface. The encoded dynamics are then used to generate statistically equivalent, randomized surrogate time series, which canmore » be linked to the continuum scale simulation. As a result, we illustrate an application of this approach using two different kinetic Monte Carlo simulations with different characteristic behaviors typical for heterogeneous chemical reactions.« less

  14. A numerical homogenization method for heterogeneous, anisotropic elastic media based on multiscale theory

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

    Gao, Kai; Chung, Eric T.; Gibson, Richard L.; Fu, Shubin; Efendiev, Yalchin

    2015-06-05

    The development of reliable methods for upscaling fine scale models of elastic media has long been an important topic for rock physics and applied seismology. Several effective medium theories have been developed to provide elastic parameters for materials such as finely layered media or randomly oriented or aligned fractures. In such cases, the analytic solutions for upscaled properties can be used for accurate prediction of wave propagation. However, such theories cannot be applied directly to homogenize elastic media with more complex, arbitrary spatial heterogeneity. We therefore propose a numerical homogenization algorithm based on multiscale finite element methods for simulating elasticmore » wave propagation in heterogeneous, anisotropic elastic media. Specifically, our method used multiscale basis functions obtained from a local linear elasticity problem with appropriately defined boundary conditions. Homogenized, effective medium parameters were then computed using these basis functions, and the approach applied a numerical discretization that is similar to the rotated staggered-grid finite difference scheme. Comparisons of the results from our method and from conventional, analytical approaches for finely layered media showed that the homogenization reliably estimated elastic parameters for this simple geometry. Additional tests examined anisotropic models with arbitrary spatial heterogeneity where the average size of the heterogeneities ranged from several centimeters to several meters, and the ratio between the dominant wavelength and the average size of the arbitrary heterogeneities ranged from 10 to 100. Comparisons to finite-difference simulations proved that the numerical homogenization was equally accurate for these complex cases.« less

  15. A numerical homogenization method for heterogeneous, anisotropic elastic media based on multiscale theory

    SciTech Connect (OSTI)

    Gao, Kai; Chung, Eric T.; Gibson, Richard L.; Fu, Shubin; Efendiev, Yalchin

    2015-06-05

    The development of reliable methods for upscaling fine scale models of elastic media has long been an important topic for rock physics and applied seismology. Several effective medium theories have been developed to provide elastic parameters for materials such as finely layered media or randomly oriented or aligned fractures. In such cases, the analytic solutions for upscaled properties can be used for accurate prediction of wave propagation. However, such theories cannot be applied directly to homogenize elastic media with more complex, arbitrary spatial heterogeneity. We therefore propose a numerical homogenization algorithm based on multiscale finite element methods for simulating elastic wave propagation in heterogeneous, anisotropic elastic media. Specifically, our method used multiscale basis functions obtained from a local linear elasticity problem with appropriately defined boundary conditions. Homogenized, effective medium parameters were then computed using these basis functions, and the approach applied a numerical discretization that is similar to the rotated staggered-grid finite difference scheme. Comparisons of the results from our method and from conventional, analytical approaches for finely layered media showed that the homogenization reliably estimated elastic parameters for this simple geometry. Additional tests examined anisotropic models with arbitrary spatial heterogeneity where the average size of the heterogeneities ranged from several centimeters to several meters, and the ratio between the dominant wavelength and the average size of the arbitrary heterogeneities ranged from 10 to 100. Comparisons to finite-difference simulations proved that the numerical homogenization was equally accurate for these complex cases.

  16. Surface functionalization of metal?organic polyhedron for homogeneous cyclopropanation catalysis

    SciTech Connect (OSTI)

    Lu, Weigang; Yuan, Daqiang; Yakovenko, Andrey; Zhou, Hong-Cai

    2012-03-13

    A super-paddlewheel (comprised of two paddlewheels) metal-organic polyhedron (MOP) containing surface hydroxyl groups was synthesized and characterized. Condensation reactions with linear alkyl anhydrides lead to new MOPs with enhanced solubility. As a result, the surface-modified MOP 4 was demonstrated as a homogeneous Lewis-acid catalyst.

  17. Workshop: Synchrotron Applications in Chemical Catalysis | Stanford

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

    Synchrotron Radiation Lightsource Synchrotron Applications in Chemical Catalysis Tuesday, October 25, 2011 - 8:00am 2011 SSRL/LCLS Annual Users Conference This workshop, part of the 2011 SSRL/LCLS Annual Users Conference, will focus on understanding processes in homogeneous (both biological and small molecule) and heterogeneous catalysis, using synchrotron-based methods. The workshop will cover more traditional applications (using XANES and EXAFS), as well as applications of XES, RIXS and

  18. Impact of heterogeneous ice nuclei on homogeneous freezing events in cirrus clouds

    SciTech Connect (OSTI)

    Spichtinger, Peter; Cziczo, Daniel J.

    2010-07-29

    The influence of initial heterogeneous nucleation on subsequent homogeneous nucleation events in cirrus clouds is investigated using a box model which includes the explicit impact of aerosols on the nucleation of ice crystals and sedimentation. Different effects are discussed, namely the impact of external mixtures of heterogeneous ice nuclei and the influence of size-dependent freezing thresholds. Several idealized experiments are carried out, which show that the treatment of external mixtures of ice nuclei can strongly change later homogeneous nucleation events (i.e., the ice crystal number densities) in different matters. The use of size-dependent freezing thresholds can also change the cloud prop erties when compared to more simple parameterizations. This size effect is most important for large IN concentrations. Based upon these findings, recommendations for future modeling and measurement efforts are presented.

  19. The performance of 3500 MWth homogeneous and heterogeneous metal fueled core designs

    SciTech Connect (OSTI)

    Turski, R.; Yang, Shi-tien

    1987-11-01

    Performance parameters are calculated for a representative 3500 MWth homogeneous and a heterogeneous metal fueled reactor design. The equilibrium cycle neutronic characteristics, safety coefficients, control system requirements, and control rod worths are evaluated. The thermal-hydraulic characteristics for both configurations are also compared. The heavy metal fuel loading requirements and neutronic performance characteristics are also evaluated for the uranium startup option. 14 refs., 14 figs., 20 tabs.

  20. An Experimental Investigation of Foam Flow in Homogeneous and Heterogeneous Porous Media, SUPRI TR-112

    SciTech Connect (OSTI)

    Apaydin, Osman G.; Bertin, Henri; Castanier, Louis M.; Kovscek, Anthony R.

    1999-08-09

    Foam is used to reduce the high mobility of gas-drive fluids and improve the contact between oil and these injected fluids. We require a better understanding of the effect of surfactant concentration on foam flow in porous media. Besides this, the literature on foam flow and transport in heterogeneous systems is sparse although the field situation is primarily heterogeneous and multidimensional. In this study, foam flow experiments were conducted first in homogeneous sand packs to investigate the effect of surfactant concentration on foam flow and then a heterogeneous experimental setup was prepared to observe heterogeneity and multidimensional flow effects on foam propagation. The homogeneous core experiments were conducted in a cylindrical aluminum core holder that was packed with a uniform Ottawa sand. Sand permeability is about 7.0 Darcy. The experiments were interpreted in terms of evolution of in-situ water saturation as a function of time by the usage of CT scanner, cumulative water, and pressure drop across the core. At very low surfactant concentration, no significant benefit was observed. But when stable foam generation started sweep efficiency (water recovery), breakthrough time, and pressure drop increased as surfactant concentration increased.

  1. Virtual special issue on catalysis at the U.S. Department of Energy's National Laboratories

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

    Pruski, Marek; Sadow, Aaron D.; Slowing, Igor I.; Marshall, Christopher L.; Stair, Peter; Rodriguez, Jose; Harris, Alex; Somorjai, Gabor A.; Biener, Juergen; Matranga, Christopher; et al

    2016-04-21

    Here the catalysis research at the U.S. Department of Energy's (DOE's) National Laboratories covers a wide range of research topics in heterogeneous catalysis, homogeneous/molecular catalysis, biocatalysis, electrocatalysis, and surface science. Since much of the work at National Laboratories is funded by DOE, the research is largely focused on addressing DOE's mission to ensure America's security and prosperity by addressing its energy, environmental, and nuclear challenges through transformative science and technology solutions.

  2. Homogeneous and Heterogeneous Reaction and Transformation of Hg and Trace Metals in Combustion Systems

    SciTech Connect (OSTI)

    J. Helble; Clara Smith; David Miller

    2009-08-31

    The overall goal of this project was to produce a working dynamic model to predict the transformation and partitioning of trace metals resulting from combustion of a broad range of fuels. The information provided from this model will be instrumental in efforts to identify fuels and conditions that can be varied to reduce metal emissions. Through the course of this project, it was determined that mercury (Hg) and arsenic (As) would be the focus of the experimental investigation. Experiments were therefore conducted to examine homogeneous and heterogeneous mercury oxidation pathways, and to assess potential interactions between arsenic and calcium. As described in this report, results indicated that the role of SO{sub 2} on Hg oxidation was complex and depended upon overall gas phase chemistry, that iron oxide (hematite) particles contributed directly to heterogeneous Hg oxidation, and that As-Ca interactions occurred through both gas-solid and within-char reaction pathways. Modeling based on this study indicated that, depending upon coal type and fly ash particle size, vaporization-condensation, vaporization-surface reaction, and As-CaO in-char reaction all play a role in arsenic transformations under combustion conditions.

  3. Lattice Boltzmann simulation of immiscible fluid displacement in porous media: Homogeneous versus heterogeneous pore network

    SciTech Connect (OSTI)

    Liu, Haihu; Zhang, Yonghao; Valocchi, Albert J.

    2015-05-15

    Injection of anthropogenic carbon dioxide (CO{sub 2}) into geological formations is a promising approach to reduce greenhouse gas emissions into the atmosphere. Predicting the amount of CO{sub 2} that can be captured and its long-term storage stability in subsurface requires a fundamental understanding of multiphase displacement phenomena at the pore scale. In this paper, the lattice Boltzmann method is employed to simulate the immiscible displacement of a wetting fluid by a non-wetting one in two microfluidic flow cells, one with a homogeneous pore network and the other with a randomly heterogeneous pore network. We have identified three different displacement patterns, namely, stable displacement, capillary fingering, and viscous fingering, all of which are strongly dependent upon the capillary number (Ca), viscosity ratio (M), and the media heterogeneity. The non-wetting fluid saturation (S{sub nw}) is found to increase nearly linearly with logCa for each constant M. Increasing M (viscosity ratio of non-wetting fluid to wetting fluid) or decreasing the media heterogeneity can enhance the stability of the displacement process, resulting in an increase in S{sub nw}. In either pore networks, the specific interfacial length is linearly proportional to S{sub nw} during drainage with equal proportionality constant for all cases excluding those revealing considerable viscous fingering. Our numerical results confirm the previous experimental finding that the steady state specific interfacial length exhibits a linear dependence on S{sub nw} for either favorable (M ? 1) or unfavorable (M < 1) displacement, and the slope is slightly higher for the unfavorable displacement.

  4. Theoretical Studies in Heterogenous Catalysis: Towards a Rational Design of Novel Catalysts for Hydrodesulfurization and Hydrogen Production

    SciTech Connect (OSTI)

    Rodriguez,J.A.; Liu, P.

    2008-10-01

    Traditionally, knowledge in heterogeneous catalysis has come through empirical research. Nowadays, there is a clear interest to change this since millions of dollars in products are generated every year in the chemical and petrochemical industries through catalytic processes. To obtain a fundamental knowledge of the factors that determine the activity of heterogeneous catalysts is a challenge for modern science since many of these systems are very complex in nature. In principle, when a molecule adsorbs on the surface of a heterogeneous catalyst, it can interact with a large number of bonding sites. It is known that the chemical properties of these bonding sites depend strongly on the chemical environment around them. Thus, there can be big variations in chemical reactivity when going from one region to another in the surface of a heterogeneous catalyst. A main objective is to understand how the structural and electronic properties of a surface affect the energetics for adsorption processes and the paths for dissociation and chemical reactions. In recent years, advances in instrumentation and experimental procedures have allowed a large series of detailed works on the surface chemistry of heterogeneous catalysts. In many cases, these experimental studies have shown interesting and unique phenomena. Theory is needed to unravel the basic interactions behind these phenomena and to provide a general framework for the interpretation of experimental results. Ideally, theoretical calculations based on density-functional theory have evolved to the point that one should be able to predict patterns in the activity of catalytic surfaces. As in the case of experimental techniques, no single theoretical approach is able to address the large diversity of phenomena occurring on a catalyst. Catalytic surfaces are usually modeled using either a finite cluster or a two-dimensionally periodic slab. Many articles have been published comparing the results of these two approaches. An important advantage of the cluster approach is that one can use the whole spectrum of quantum-chemical methods developed for small molecules with relatively minor modifications. On the other hand, the numerical effort involved in cluster calculations increases rather quickly with the size of the cluster. This problem does not exist when using slab models. Due to the explicit incorporation of the periodicity of the crystal lattice through the Bloch theorem, the actual dimension of a slab calculation depends only on the size of the unit cell. In practical terms, the slab approach is mainly useful for investigating the behavior of adsorbates at medium and high coverages. Very large unit cells are required at the limit of low to zero coverage, or when examining the properties and chemical behavior of isolated defect sites in a surface. In these cases, from a computational viewpoint, the cluster approach can be much more cost effective than the slab approach. Slab and cluster calculations can be performed at different levels of sophistication: semi-empirical methods, simple ab initio Hartree-Fock, ab initio post-Hartree-Fock (CI, MP2, etc), and density functional theory. Density-functional (DF) based calculations frequently give adsorption geometries with a high degree of accuracy and predict reliable trends for the energetics of adsorption reactions. This article provides a review of recent theoretical studies that deal with the behavior of novel catalysts used for hydrodesulfurization (HDS) reactions and the production of hydrogen (i.e. catalytic processes employed in the generation of clean fuels). These studies involve a strong coupling of theory and experiment. A significant fraction of the review is focused on the importance of size-effects and correlations between the electronic and chemical properties of catalytic materials. The article begins with a discussion of results for the desulfurization of thiophene on metal carbides and phosphides, systems which have the potential to become the next generation of industrial HDS catalysts. Then, systematic studies con

  5. Comparison of Homogeneous and Heterogeneous CFD Fuel Models for Phase I of the IAEA CRP on HTR Uncertainties Benchmark

    SciTech Connect (OSTI)

    Gerhard Strydom; Su-Jong Yoon

    2014-04-01

    Computational Fluid Dynamics (CFD) evaluation of homogeneous and heterogeneous fuel models was performed as part of the Phase I calculations of the International Atomic Energy Agency (IAEA) Coordinate Research Program (CRP) on High Temperature Reactor (HTR) Uncertainties in Modeling (UAM). This study was focused on the nominal localized stand-alone fuel thermal response, as defined in Ex. I-3 and I-4 of the HTR UAM. The aim of the stand-alone thermal unit-cell simulation is to isolate the effect of material and boundary input uncertainties on a very simplified problem, before propagation of these uncertainties are performed in subsequent coupled neutronics/thermal fluids phases on the benchmark. In many of the previous studies for high temperature gas cooled reactors, the volume-averaged homogeneous mixture model of a single fuel compact has been applied. In the homogeneous model, the Tristructural Isotropic (TRISO) fuel particles in the fuel compact were not modeled directly and an effective thermal conductivity was employed for the thermo-physical properties of the fuel compact. On the contrary, in the heterogeneous model, the uranium carbide (UCO), inner and outer pyrolytic carbon (IPyC/OPyC) and silicon carbide (SiC) layers of the TRISO fuel particles are explicitly modeled. The fuel compact is modeled as a heterogeneous mixture of TRISO fuel kernels embedded in H-451 matrix graphite. In this study, a steady-state and transient CFD simulations were performed with both homogeneous and heterogeneous models to compare the thermal characteristics. The nominal values of the input parameters are used for this CFD analysis. In a future study, the effects of input uncertainties in the material properties and boundary parameters will be investigated and reported.

  6. Fabrication of Carbon-Platinum Interdigitated Array Electrodes and Their Application for Investigating Homogeneous Hydrogen Evolution Catalysis

    SciTech Connect (OSTI)

    Liu, Fei; Divan, Ralu; Parkinson, Bruce A.

    2015-06-29

    Carbon interdigitated array (IDA) electrodes have been applied to study the homogeneous hydrogen evolution electrocatalyst [Ni(PPh2NBn2)2]2+ (where PPh2NBn2 is 1,5-dibenzyl-3,7-diphenyl-1,5-diaza-3,7-diphosphacyclooctane). The existence of reaction intermediates in the catalytic cycle is inferred from the electrochemical behavior of a glassy carbon disk electrodes and carbon IDA electrodes. The currents on IDA electrodes for an EC (electron transfer reaction followed by a catalytic reaction) mechanism are derived from the number of redox cycles and the contribution of non-catalytic currents. The catalytic reaction rate constant was then extracted from the IDA current equations. Applying the IDA current and kinetic equations to the electrochemical response of the [Ni(PPh2NBn2)2]2+ catalyst yielded a rate constant of 0.10 s-1 for the hydrogen evolution reaction that agrees with the literature value. The quantitative analysis of IDA cyclic voltammetry can be used as a simple and straightforward method for determining rate constants in other catalytic systems. This work was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for DOE. Use of the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

  7. 2012 Catalysis Lectures

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

    Catalysis Lectures May 21-24 2012 Bert Weckhuysen Bert Weckhuysen, who holds the chair of Inorganic Chemistry and Catalysis at Utrecht University, will give a series of catalysis lectures during his sabbatical period at Stanford University and SLAC. (1) "Characterization of Heterogeneous Catalysts: Possibilities and Limitations of In-situ Spectroscopy" (Part I) Monday, May 21, 2012, 4.30-6 p.m. Location: SLAC Redwood Conference Room C&D (2) "Characterization of Heterogeneous

  8. Shining Light on Catalysis | Stanford Synchrotron Radiation Lightsourc...

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

    Shining Light on Catalysis Tuesday, July 19, 2011 - 4:38pm SSRL Conference Room 137-322 Jeroen A. van Bokhoven, Professor for Heterogeneous Catalysis Institute for Chemical and...

  9. Catalysis Workshop

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

    Opportunities in Catalysis Research Using Synchrotron Radiation Stanford Synchrotron Radiation Laboratory October 8-9, 2002 Organizer: Anders Nilsson Chemical catalysis is one of the research areas of enormous importance for the industrial society. There are important challenges to be met in the near future where development of new processes and catalysts are a necessity. We need to find a way to make methanol from methane, split water into hydrogen using sunlight, find replacement of platinum

  10. Experimental and numerical analysis of parallel reactant flow and transverse mixing with mineral precipitation in homogeneous and heterogeneous porous media

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

    Fox, Don T.; Guo, Luanjing; Fujita, Yoshiko; Huang, Hai; Redden, George

    2015-12-17

    Formation of mineral precipitates in the mixing interface between two reactant solutions flowing in parallel in porous media is governed by reactant mixing by diffusion and dispersion and is coupled to changes in porosity/permeability due to precipitation. The spatial and temporal distribution of mixing-dependent precipitation of barium sulfate in porous media was investigated with side-by-side injection of barium chloride and sodium sulfate solutions in thin rectangular flow cells packed with quartz sand. The results for homogeneous sand beds were compared to beds with higher or lower permeability inclusions positioned in the path of the mixing zone. In the homogeneous andmore » high permeability inclusion experiments, BaSO4 precipitate (barite) formed in a narrow deposit along the length and in the center of the solution–solution mixing zone even though dispersion was enhanced within, and downstream of, the high permeability inclusion. In the low permeability inclusion experiment, the deflected BaSO4 precipitation zone broadened around one side and downstream of the inclusion and was observed to migrate laterally toward the sulfate solution. A continuum-scale fully coupled reactive transport model that simultaneously solves the nonlinear governing equations for fluid flow, transport of reactants and geochemical reactions was used to simulate the experiments and provide insight into mechanisms underlying the experimental observations. Lastly, migration of the precipitation zone in the low permeability inclusion experiment could be explained by the coupling effects among fluid flow, reactant transport and localized mineral precipitation reaction.« less

  11. In situ measurements of a homogeneous to heterogeneous transition in the plastic response of ion-irradiated Ni microspecimens

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

    Zhao, Xinyu; Strickland, Daniel J.; Derlet, Peter M.; He, Mo-rigen; Cheng, You -Jung; Pu, Jue; Stanford Univ., Stanford, CA; Hattar, Khalid; Gianola, Daniel S.

    2015-02-11

    We report on the use of quantitative in situ microcompression experiments in a scanning electron microscope to systematically investigate the effect of self-ion irradiation damage on the full plastic response of Ni. In addition to the well-known irradiationinduced increases in the yield and flow strengths with increasing dose, we measure substantial changes in plastic flow intermittency behavior, manifested as stress drops accompanying energy releases as the driven material transits critical states. At low irradiation doses, the magnitude of stress drops reduces relative to the unirradiated material and plastic slip proceeds on multiple slip systems, leading to quasi-homogeneous plastic flow.more »In contrast, highly irradiated specimens exhibit pronounced shear localization on parallel slip planes, which we ascribe to the onset of defect free channels normally seen in bulk irradiated materials. Our in situ testing system and approach allows for a quantitative study of the energy release and dynamics associated with defect free channel formation and subsequent localization. As a result, this study provides fundamental insight to the nature of interactions between mobile dislocations and irradiation-mediated and damage-dependent defect structures.« less

  12. In situ measurements of a homogeneous to heterogeneous transition in the plastic response of ion-irradiated <111> Ni microspecimens

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

    Zhao, Xinyu; Strickland, Daniel J.; Derlet, Peter M.; He, Mo-rigen; Cheng, You -Jung; Pu, Jue; Stanford Univ., Stanford, CA; Hattar, Khalid; Gianola, Daniel S.

    2015-02-11

    We report on the use of quantitative in situ microcompression experiments in a scanning electron microscope to systematically investigate the effect of self-ion irradiation damage on the full plastic response of <111> Ni. In addition to the well-known irradiationinduced increases in the yield and flow strengths with increasing dose, we measure substantial changes in plastic flow intermittency behavior, manifested as stress drops accompanying energy releases as the driven material transits critical states. At low irradiation doses, the magnitude of stress drops reduces relative to the unirradiated material and plastic slip proceeds on multiple slip systems, leading to quasi-homogeneous plastic flow.more » In contrast, highly irradiated specimens exhibit pronounced shear localization on parallel slip planes, which we ascribe to the onset of defect free channels normally seen in bulk irradiated materials. Our in situ testing system and approach allows for a quantitative study of the energy release and dynamics associated with defect free channel formation and subsequent localization. As a result, this study provides fundamental insight to the nature of interactions between mobile dislocations and irradiation-mediated and damage-dependent defect structures.« less

  13. Applying Metal-Organic Frameworks in heterogeneous Catalyisis...

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

    Metal-Organic Frameworks in heterogeneous Catalyisis To control heterogeneous catalysis at atomic and electronic-level represents one of the most challenge research areas....

  14. Combining X-ray Absorption and X-ray Diffraction Techniques for in Situ Studies of Chemical Transformations in Heterogeneous Catalysis: Advantages and Limitations

    SciTech Connect (OSTI)

    Frenkel, A.I.; Hanson, J.; Wang, Q.; Marinkovic, N.; Chen, J.G.; Barrio, L.; Si, R.; Lopez Camara, A.; Estrella, A.M.; Rodriguez, J.A.

    2011-08-05

    Recent advances in catalysis instrumentations include synchrotron-based facilities where time-resolved X-ray scattering and absorption techniques are combined in the same in situ or operando experiment to study catalysts at work. To evaluate the advances and limitations of this method, we performed a series of experiments at the new XAFS/XRD instrument in the National Synchrotron Light Source. Nearly simultaneous X-ray diffraction (XRD) and X-ray absorption fine-structure (XAFS) measurements of structure and kinetics of several catalysts under reducing or oxidizing conditions have been performed and carefully analyzed. For CuFe{sub 2}O{sub 4} under reducing conditions, the combined use of the two techniques allowed us to obtain accurate data on kinetics of nucleation and growth of metallic Cu. For the inverse catalyst CuO/CeO{sub 2} that underwent isothermal reduction (with CO) and oxidation (with O{sub 2}), the XAFS data measured in the same experiment with XRD revealed strongly disordered Cu species that went undetected by diffraction. These and other examples emphasize the unique sensitivity of these two complementary methods to follow catalytic processes in the broad ranges of length and time scales.

  15. Combining X-ray Absorption and X-ray Diffraction Techniques for in Situ Studies of Chemical Transformations in Heterogeneous Catalysis:Advantages and Limitations

    SciTech Connect (OSTI)

    A Frenkel; Q Wang; N Marinkovic; J Chen; L Barrio; R Si; A Lopez Camara; A Estella; J Rodriquez; J Hanson

    2011-12-31

    Recent advances in catalysis instrumentations include synchrotron-based facilities where time-resolved X-ray scattering and absorption techniques are combined in the same in situ or operando experiment to study catalysts at work. To evaluate the advances and limitations of this method, we performed a series of experiments at the new XAFS/XRD instrument in the National Synchrotron Light Source. Nearly simultaneous X-ray diffraction (XRD) and X-ray absorption fine-structure (XAFS) measurements of structure and kinetics of several catalysts under reducing or oxidizing conditions have been performed and carefully analyzed. For CuFe{sub 2}O{sub 4} under reducing conditions, the combined use of the two techniques allowed us to obtain accurate data on kinetics of nucleation and growth of metallic Cu. For the inverse catalyst CuO/CeO{sub 2} that underwent isothermal reduction (with CO) and oxidation (with O{sub 2}), the XAFS data measured in the same experiment with XRD revealed strongly disordered Cu species that went undetected by diffraction. These and other examples emphasize the unique sensitivity of these two complementary methods to follow catalytic processes in the broad ranges of length and time scales.

  16. Shining Light on Catalysis | Stanford Synchrotron Radiation Lightsource

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

    Shining Light on Catalysis Tuesday, July 19, 2011 - 4:38pm SSRL Conference Room 137-322 Jeroen A. van Bokhoven, Professor for Heterogeneous Catalysis Institute for Chemical and Bioengineering ETH Zurich Head of Laboratory for Catalysis and Sustainable Chemistry (LSK) Swiss Light Source Paul Scherrer Institute Understanding a functioning catalyst requires understanding at the atomic scales in a time-resolved manner. X-rays can be readily used to accomplish that task, because of the large

  17. Seventh BES (Basic Energy Sciences) catalysis and surface chemistry research conference

    SciTech Connect (OSTI)

    Not Available

    1990-03-01

    Research programs on catalysis and surface chemistry are presented. A total of fifty-seven topics are included. Areas of research include heterogeneous catalysis; catalysis in hydrogenation, desulfurization, gasification, and redox reactions; studies of surface properties and surface active sites; catalyst supports; chemical activation, deactivation; selectivity, chemical preparation; molecular structure studies; sorption and dissociation. Individual projects are processed separately for the data bases. (CBS)

  18. Heterogeneous Catalysis and Surface Science - JCAP

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

    Hermann Muller and Mutations in Drosophila Resources with Additional Information Hermann Muller Credit: Hermann Muller, 1956, Hermann J. Muller Collection I; Box 11: Folder 04: Cold Spring Harbor Laboratory Archives Geneticist and Nobel prize laureate [Hermann J.] Muller was born and schooled in New York City, receiving an A.B., M.A. and, in 1915, his Ph.D. from Columbia University. His first faculty appointment was at Rice University in Houston, Texas. He then accepted a two-year appointment as

  19. The impact of nanoscience on heterogeneous catalysis

    SciTech Connect (OSTI)

    Bell, Alexis T.

    2003-03-03

    Most catalysts consist of nanometer-sized particles dispersed on a high-surface area support. Advances in characterization methods have led to a molecular level understanding of the relationships between nanoparticle properties and catalytic performance. Together with novel approaches to nanoparticle synthesis, this knowledge is contributing to the design and development of new catalysts.

  20. Textured Metal Catalysts for Heterogeneous Catalysis - Energy...

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

    access to micropores Highly effective for aqueous phase hydrogenations Applications and Industries Bioproductsbiofuels manufacturing Chemical manufacturing Patents and Patent...

  1. A Hydrogen-Evolving Ni(P2N2)2 Electrocatalyst Covalently Attached to a Glassy Carbon Electrode: Preparation, Characterization, and Catalysis. Comparisons With the Homogeneous Analog

    SciTech Connect (OSTI)

    Das, Atanu K.; Engelhard, Mark H.; Bullock, R. Morris; Roberts, John A.

    2014-07-07

    A hydrogen-evolving homogeneous Ni(P2N2)2 electrocatalyst with peripheral ester groups has been covalently attached to a 1,2,3-triazolyllithium-terminated glassy carbon electrode. The surface-confined complex is an electroctalyst for hydrogen evolution, showing onset of catalytic current at the same potential as the soluble parent complex. X-ray photoemission spectra show excellent agreement between the coupled and homogeneous species. Coverage approaches a dense monolayer. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy. The XPS measurements were performed at EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory.

  2. Methanol Synthesis over Cu/ZnO/Al2O3: The Active Site in Industrial Catalysis

    SciTech Connect (OSTI)

    Behrens, Malte

    2012-03-28

    Unlike homogeneous catalysts, heterogeneous catalysts that have been optimized through decades are typically so complex and hard to characterize that the nature of the catalytically active site is not known. This is one of the main stumbling blocks in developing rational catalyst design strategies in heterogeneous catalysis. We show here how to identify the crucial atomic structure motif for the industrial Cu/ZnO/Al{sub 2}O{sub 3} methanol synthesis catalyst. Using a combination of experimental evidence from bulk-, surface-sensitive and imaging methods collected on real high-performance catalytic systems in combination with DFT calculations. We show that the active site consists of Cu steps peppered with Zn atoms, all stabilized by a series of well defined bulk defects and surface species that need jointly to be present for the system to work.

  3. In situ measurements of a homogeneous to heterogeneous transition in the plastic response of ion-irradiated <111> Ni microspecimens

    SciTech Connect (OSTI)

    Zhao, Xinyu; Strickland, Daniel J.; Derlet, Peter M.; He, Mo-rigen; Cheng, You -Jung; Pu, Jue; Hattar, Khalid; Gianola, Daniel S.

    2015-02-11

    We report on the use of quantitative in situ microcompression experiments in a scanning electron microscope to systematically investigate the effect of self-ion irradiation damage on the full plastic response of <111> Ni. In addition to the well-known irradiationinduced increases in the yield and flow strengths with increasing dose, we measure substantial changes in plastic flow intermittency behavior, manifested as stress drops accompanying energy releases as the driven material transits critical states. At low irradiation doses, the magnitude of stress drops reduces relative to the unirradiated material and plastic slip proceeds on multiple slip systems, leading to quasi-homogeneous plastic flow. In contrast, highly irradiated specimens exhibit pronounced shear localization on parallel slip planes, which we ascribe to the onset of defect free channels normally seen in bulk irradiated materials. Our in situ testing system and approach allows for a quantitative study of the energy release and dynamics associated with defect free channel formation and subsequent localization. As a result, this study provides fundamental insight to the nature of interactions between mobile dislocations and irradiation-mediated and damage-dependent defect structures.

  4. Center for Catalysis at Iowa State University

    SciTech Connect (OSTI)

    Kraus, George A.

    2006-10-17

    The overall objective of this proposal is to enable Iowa State University to establish a Center that enjoys world-class stature and eventually enhances the economy through the transfer of innovation from the laboratory to the marketplace. The funds have been used to support experimental proposals from interdisciplinary research teams in areas related to catalysis and green chemistry. Specific focus areas included: Catalytic conversion of renewable natural resources to industrial materials Development of new catalysts for the oxidation or reduction of commodity chemicals Use of enzymes and microorganisms in biocatalysis Development of new, environmentally friendly reactions of industrial importance These focus areas intersect with barriers from the MYTP draft document. Specifically, section 2.4.3.1 Processing and Conversion has a list of bulleted items under Improved Chemical Conversions that includes new hydrogenation catalysts, milder oxidation catalysts, new catalysts for dehydration and selective bond cleavage catalysts. Specifically, the four sections are: 1. Catalyst development (7.4.12.A) 2. Conversion of glycerol (7.4.12.B) 3. Conversion of biodiesel (7.4.12.C) 4. Glucose from starch (7.4.12.D) All funded projects are part of a soybean or corn biorefinery. Two funded projects that have made significant progress toward goals of the MYTP draft document are: Catalysts to convert feedstocks with high fatty acid content to biodiesel (Kraus, Lin, Verkade) and Conversion of Glycerol into 1,3-Propanediol (Lin, Kraus). Currently, biodiesel is prepared using homogeneous base catalysis. However, as producers look for feedstocks other than soybean oil, such as waste restaurant oils and rendered animal fats, they have observed a large amount of free fatty acids contained in the feedstocks. Free fatty acids cannot be converted into biodiesel using homogeneous base-mediated processes. The CCAT catalyst system offers an integrated and cooperative catalytic system that performs both esterification (of free fatty acids) and transesterification (of soybean oil) in a one-pot fashion. This will allow the biodiesel producers to use the aforementioned cheap feedstocks without any pretreatment. In addition, the catalyst system is heterogeneous and is highly recyclable and reusable. Although markets currently exist for glycerin, concern is mounting that the price of glycerin may plummet to $.05 - $.10 per pound if future production exceeds demand. Developing a system to make high value chemicals such as 1,3-propanediol from the glycerin stream will add value for biodiesel producers who implement the new technology. Given the fact that both DuPont and Shell chemicals have announced the commercialization of two new PDO-based polymers, a rapid increase of market demand for a cheaper PDO source is very likely. 4. Comparison of actual accomplishments with goals and objectives From our progress reports, the four areas are: 1. Catalyst development (7.4.12.A) 2. Conversion of glycerol (7.4.12.B) 3. Conversion of biodiesel (7.4.12.C) 4. Glucose from starch (7.4.12.D)

  5. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis ... (4) catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, ...

  6. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis ... (27) catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, ...

  7. Multiferroicity of Carbon-Based Charge-Transfer Magnets (Journal...

    Office of Scientific and Technical Information (OSTI)

    Research Org: Energy Frontier Research Centers (EFRC); Argonne-Northwestern Solar Energy ... Subject: catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar ...

  8. A bioinspired redox relay that mimics radical interactions of...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, ...

  9. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, charge ...

  10. Mimicking the electron transfer chain in photosystem II with...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, ...

  11. Optical and electrochemical properties of hydrogen-bondedphenol...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), photosynthesis (natural and artificial), bio-inspired, hydrogen and fuel cells, electrodes - solar, ...

  12. Nanoscale Imaging of Lithium Ion Distribution During In Situ...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (homogeneous), catalysis (heterogeneous), energy storage (including batteries and capacitors), hydrogen and fuel cells, defects, charge transport, membrane, ...

  13. In Situ Electron Energy-Loss Spectroscopy in Liquids (Journal...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (homogeneous), catalysis (heterogeneous), energy storage (including batteries and capacitors), hydrogen and fuel cells, defects, charge transport, membrane, ...

  14. Neutrons for Catalysis: A Workshop on Neutron Scattering Techniques for Studies in Catalysis

    SciTech Connect (OSTI)

    Overbury, Steven {Steve} H; Coates, Leighton; Herwig, Kenneth W; Kidder, Michelle

    2011-10-01

    This report summarizes the Workshop on Neutron Scattering Techniques for Studies in Catalysis, held at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL) on September 16 and 17, 2010. The goal of the Workshop was to bring experts in heterogeneous catalysis and biocatalysis together with neutron scattering experimenters to identify ways to attack new problems, especially Grand Challenge problems in catalysis, using neutron scattering. The Workshop locale was motivated by the neutron capabilities at ORNL, including the High Flux Isotope Reactor (HFIR) and the new and developing instrumentation at the SNS. Approximately 90 researchers met for 1 1/2 days with oral presentations and breakout sessions. Oral presentations were divided into five topical sessions aimed at a discussion of Grand Challenge problems in catalysis, dynamics studies, structure characterization, biocatalysis, and computational methods. Eleven internationally known invited experts spoke in these sessions. The Workshop was intended both to educate catalyst experts about the methods and possibilities of neutron methods and to educate the neutron community about the methods and scientific challenges in catalysis. Above all, it was intended to inspire new research ideas among the attendees. All attendees were asked to participate in one or more of three breakout sessions to share ideas and propose new experiments that could be performed using the ORNL neutron facilities. The Workshop was expected to lead to proposals for beam time at either the HFIR or the SNS; therefore, it was expected that each breakout session would identify a few experiments or proof-of-principle experiments and a leader who would pursue a proposal after the Workshop. Also, a refereed review article will be submitted to a prominent journal to present research and ideas illustrating the benefits and possibilities of neutron methods for catalysis research.

  15. 2012 Catalysis Lectures

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

    his sabbatical period at Stanford University and SLAC. (1) "Characterization of Heterogeneous Catalysts: Possibilities and Limitations of In-situ Spectroscopy" (Part I) Monday,...

  16. Zeolite catalysis: technology

    SciTech Connect (OSTI)

    Heinemann, H.

    1980-07-01

    Zeolites have been used as catalysts in industry since the early nineteen sixties. The great majority of commercial applications employ one of three zeolite types: zeolite Y; Mordenite; ZSM-5. By far the largest use of zeolites is in catalytic cracking, and to a lesser extent in hydrocracking. This paper reviews the rapid development of zeolite catalysis and its application in industries such as: the production of gasoline by catalytic cracking of petroleum; isomerization of C/sub 5/ and C/sub 6/ paraffin hydrocarbons; alkylation of aromatics with olefins; xylene isomerization; and conversion of methanol to gasoline.

  17. Electron Microscopy Catalysis Projects: Success Stories from...

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

    Electron Microscopy Catalysis Projects: Success Stories from the High Temperature Materials Laboratory (HTML) User Program Electron Microscopy Catalysis Projects: Success Stories ...

  18. Catalysis and Synthesis | Argonne National Laboratory

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

    Catalysis and Synthesis Catalysis and Synthesis Many different types of chemical reactions depend on catalysts in order to work, and the hunt for better catalysts has deep...

  19. Catalysis Capabilities | Argonne National Laboratory

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

    Catalysis Research Areas Facilities and Equipment Intellectual Property Publications Staff Partnerships Licensing Sponsored Research Technical Services Technologist in Residence News Press Releases Feature Stories In the News Photos Videos Ombudsman Ombudsman Argonne National Laboratory Technology Development and Commercialization About Technologies Available for Licensing Capabilities Partnerships News Capabilities Catalysis Research Areas Facilities and Equipment Intellectual Property

  20. Catalysis Center for Energy Innovation (CCEI) | U.S. DOE Office of Science

    Office of Science (SC) Website

    (SC) Catalysis Center for Energy Innovation (CCEI) Energy Frontier Research Centers (EFRCs) EFRCs Home Centers EFRC External Websites Research Science Highlights News & Events Publications History Contact BES Home Centers Catalysis Center for Energy Innovation (CCEI) Print Text Size: A A A FeedbackShare Page CCEI Header Director Dionisios Vlachos Lead Institution University of Delaware Year Established 2009 Mission To focus on developing innovative, transformational heterogeneous

  1. 2013 DOE Catalysis Working Group Meeting Agenda | Department...

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

    DOE Catalysis Working Group Meeting Agenda 2013 DOE Catalysis Working Group Meeting Agenda Agenda for the 2013 DOE Catalysis Working Group Meeting on May 15, 2013. PDF icon...

  2. Enhanced Micellar Catalysis LDRD.

    SciTech Connect (OSTI)

    Betty, Rita G.; Tucker, Mark David; Taggart, Gretchen; Kinnan, Mark K.; Glen, Crystal Chanea; Rivera, Danielle; Sanchez, Andres; Alam, Todd Michael

    2012-12-01

    The primary goals of the Enhanced Micellar Catalysis project were to gain an understanding of the micellar environment of DF-200, or similar liquid CBW surfactant-based decontaminants, as well as characterize the aerosolized DF-200 droplet distribution and droplet chemistry under baseline ITW rotary atomization conditions. Micellar characterization of limited surfactant solutions was performed externally through the collection and measurement of Small Angle X-Ray Scattering (SAXS) images and Cryo-Transmission Electron Microscopy (cryo-TEM) images. Micellar characterization was performed externally at the University of Minnesota's Characterization Facility Center, and at the Argonne National Laboratory Advanced Photon Source facility. A micellar diffusion study was conducted internally at Sandia to measure diffusion constants of surfactants over a concentration range, to estimate the effective micelle diameter, to determine the impact of individual components to the micellar environment in solution, and the impact of combined components to surfactant phase behavior. Aerosolized DF-200 sprays were characterized for particle size and distribution and limited chemical composition. Evaporation rates of aerosolized DF-200 sprays were estimated under a set of baseline ITW nozzle test system parameters.

  3. Biomimetic Chalcogels for Solar Fuel Catalysis | ANSER Center...

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

    Biomimetic Chalcogels for Solar Fuel Catalysis Home > Research > ANSER Research Highlights > Biomimetic Chalcogels for Solar Fuel Catalysis...

  4. Recent advances of lanthanum-based perovskite oxides for catalysis

    SciTech Connect (OSTI)

    Zhu, Huiyuan; Zhang, Pengfei; Dai, Sheng

    2015-09-21

    There is a need to reduce the use of noble metal elements especially in the field of catalysis, where noble metals are ubiquitously applied. To this end, perovskite oxides, an important class of mixed oxide, have been attracting increasing attention for decades as potential replacements. Benefiting from the extraordinary tunability of their compositions and structures, perovskite oxides can be rationally tailored and equipped with targeted physical and chemical properties e.g. redox behavior, oxygen mobility, and ion conductivity for enhanced catalysis. Recently, the development of highly efficient perovskite oxide catalysts has been extensively studied. This review article summarizes the recent development of lanthanum-based perovskite oxides as advanced catalysts for both energy conversion applications and traditional heterogeneous reactions.

  5. Recent advances of lanthanum-based perovskite oxides for catalysis

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

    Zhu, Huiyuan; Zhang, Pengfei; Dai, Sheng

    2015-09-21

    There is a need to reduce the use of noble metal elements especially in the field of catalysis, where noble metals are ubiquitously applied. To this end, perovskite oxides, an important class of mixed oxide, have been attracting increasing attention for decades as potential replacements. Benefiting from the extraordinary tunability of their compositions and structures, perovskite oxides can be rationally tailored and equipped with targeted physical and chemical properties e.g. redox behavior, oxygen mobility, and ion conductivity for enhanced catalysis. Recently, the development of highly efficient perovskite oxide catalysts has been extensively studied. This review article summarizes the recent developmentmore » of lanthanum-based perovskite oxides as advanced catalysts for both energy conversion applications and traditional heterogeneous reactions.« less

  6. Integrated Mesoscale Architectures for Sustainable Catalysis...

    Office of Science (SC) Website

    Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC) Energy Frontier ... science, molecular dynamics (MD), density functional theory (DFT), quantum ...

  7. Catalysis Working Group Meeting: June 2015

    Broader source: Energy.gov [DOE]

    Agenda and presentations from the Catalysis Working Group meeting held on June 8, 2015, in Arlington, Virginia.

  8. Fuel Synthesis Catalysis Laboratory: Catalytic Testing for Thermochemical Transformations of Molecules (Fact Sheet), NREL (National Renewable Energy Laboratory)

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

    Synthesis Catalysis Laboratory Catalytic testing for thermochemical transformations of molecules NREL is a national laboratory of the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, operated by the Alliance for Sustainable Energy, LLC. NREL's Fuel Synthesis Catalysis Laboratory (FSCL) provides a wide range of capabilities in heterogeneous catalyst testing. Current research areas of emphasis include the transformation of biomass pyrolysis and gasification products to

  9. University of Delaware | Catalysis Center for Energy Innovation | Furans

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

    Research Thrust Sugars to Furans Converting sugars to high-value intermediates. CCEI introduced an iconic technology for the isomerization of aldoses to ketoses production via Sn-beta zeolite and other related heterogeneous and homogeneous Lewis acid catalysts in water and demonstrated that this technology is broadly applicable to the conversion of C6 and C5 sugars. Researchers discovered the first single-pot process that combines heterogeneous Lewis acidity with Bronsted acidity to carry

  10. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    Filter Results Filter by Subject materials science (2) air conditioning (1) alloys (1) austenite (1) catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), solar ...

  11. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    Filter Results Filter by Subject absorption spectroscopy (1) aging (1) air (1) anisotropy (1) armor (1) catalysis (homogeneous), catalysis (heterogeneous), solar (photovoltaic), ...

  12. CABS | U.S. DOE Office of Science (SC)

    Office of Science (SC) Website

    Research Topics: catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), ... GC5 Non-equilibrium BRN Addressed CombustionTransportation Fuels Solar Energy Utilization

  13. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... Filter Results Filter by Subject materials science (23) catalysis (homogeneous), catalysis (heterogeneous), solar (fuels), photosynthesis (natural and artificial), bio-inspired, ...

  14. Workshop: Synchrotron Applications in Chemical Catalysis | Stanford...

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

    Applications in Chemical Catalysis Tuesday, October 25, 2011 - 8:00am 2011 SSRLLCLS Annual Users Conference This workshop, part of the 2011 SSRLLCLS Annual Users...

  15. Biochemical Conversion: Using Hydrolysis, Fermentation, and Catalysis...

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

    Biochemical Conversion: Using Hydrolysis, Fermentation, and Catalysis to Make Fuels and Chemicals BETO works with the emerging U.S. bioindustry to sustainably convert non-food ...

  16. Basic Research Needs: Catalysis for Energy

    SciTech Connect (OSTI)

    Bell, Alexis T.; Gates, Bruce C.; Ray, Douglas; Thompson, Michael R.

    2008-03-11

    The report presents results of a workshop held August 6-8, 2007, by DOE SC Basic Energy Sciences to determine the basic research needs for catalysis research.

  17. The energy landscape of ;#8203;adenylate kinase during catalysis...

    Office of Scientific and Technical Information (OSTI)

    The energy landscape of ;8203;adenylate kinase during catalysis Citation Details In-Document Search Title: The energy landscape of ;8203;adenylate kinase during catalysis ...

  18. Materials Design and Discovery: Catalysis and Energy Storage...

    Office of Scientific and Technical Information (OSTI)

    Materials Design and Discovery: Catalysis and Energy Storage (Mira Early Science Program ... Citation Details In-Document Search Title: Materials Design and Discovery: Catalysis and ...

  19. Pre-Competitive Catalysis Research: Fundamental Sulfation/Desulfation...

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

    Pre-Competitive Catalysis Research: Fundamental SulfationDesulfation Studies of Lean NOx Traps Pre-Competitive Catalysis Research: Fundamental SulfationDesulfation Studies of...

  20. Low-Temperature Hydrocarbon/CO Oxidation Catalysis in Support...

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

    More Documents & Publications Low-Temperature HydrocarbonCO Oxidation Catalysis in Support of HCCI Emission Control Low-Temperature HydrocarbonCO Oxidation Catalysis in Support ...

  1. Biomimetic Chalcogels for Solar Fuel Catalysis | ANSER Center |

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

    Argonne-Northwestern National Laboratory Biomimetic Chalcogels for Solar Fuel Catalysis Home > Research > ANSER Research Highlights > Biomimetic Chalcogels for Solar Fuel Catalysis

  2. Transmural Catalysis - High Efficiency Catalyst Systems for NOx...

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

    Transmural Catalysis - High Efficiency Catalyst Systems for NOx Adsorbers and SCR Transmural Catalysis - High Efficiency Catalyst Systems for NOx Adsorbers and SCR Presentation ...

  3. "Nanocrystal bilayer for tandem catalysis"

    SciTech Connect (OSTI)

    Yamada, Yusuke; Tsung, Chia Kuang; Huang, Wenyu; Huo, Ziyang; E.Habas, Susan E; Soejima, Tetsuro; Aliaga, Cesar E; Samorjai, Gabor A; Yang, Peidong

    2011-01-24

    Supported catalysts are widely used in industry and can be optimized by tuning the composition and interface of the metal nanoparticles and oxide supports. Rational design of metal-metal oxide interfaces in nanostructured catalysts is critical to achieve better reaction activities and selectivities. We introduce here a new class of nanocrystal tandem catalysts that have multiple metal-metal oxide interfaces for the catalysis of sequential reactions. We utilized a nanocrystal bilayer structure formed by assembling platinum and cerium oxide nanocube monolayers of less than 10 nm on a silica substrate. The two distinct metal-metal oxide interfaces, CeO2-Pt and Pt-SiO2, can be used to catalyse two distinct sequential reactions. The CeO2-Pt interface catalysed methanol decomposition to produce CO and H2, which were subsequently used for ethylene hydroformylation catalysed by the nearby Pt-SiO2 interface. Consequently, propanal was produced selectively from methanol and ethylene on the nanocrystal bilayer tandem catalyst. This new concept of nanocrystal tandem catalysis represents a powerful approach towards designing high-performance, multifunctional nanostructured catalysts

  4. Theoretical/Computational Tools for Energy-Relevant Catalysis | The Ames

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

    Laboratory Theoretical/Computational Tools for Energy-Relevant Catalysis FWP/Project Description: Project Leader(s): James Evans, Mark Gordon Principal Investigators: James Evans, Mark Gordon This project will develop new strategies for and integrated combinations of electronic structure analysis and statistical mechanical, coarse-grained, and multi-scale modeling approaches to treat energy-relevant heterogeneous catalytic systems. Currently, there is a lack of effective molecular-level

  5. Nanocrystal assembly for tandem catalysis

    DOE Patents [OSTI]

    Yang, Peidong; Somorjai, Gabor; Yamada, Yusuke; Tsung, Chia-Kuang; Huang, Wenyu

    2014-10-14

    The present invention provides a nanocrystal tandem catalyst comprising at least two metal-metal oxide interfaces for the catalysis of sequential reactions. One embodiment utilizes a nanocrystal bilayer structure formed by assembling sub-10 nm platinum and cerium oxide nanocube monolayers on a silica substrate. The two distinct metal-metal oxide interfaces, CeO.sub.2--Pt and Pt--SiO.sub.2, can be used to catalyze two distinct sequential reactions. The CeO.sub.2--Pt interface catalyzed methanol decomposition to produce CO and H.sub.2, which were then subsequently used for ethylene hydroformylation catalyzed by the nearby Pt--SiO.sub.2 interface. Consequently, propanal was selectively produced on this nanocrystal bilayer tandem catalyst.

  6. [Zeolite catalysis in conversion of cellulosics

    SciTech Connect (OSTI)

    Tsao, G.T.

    1992-12-31

    To transform biomass into fermentable substrate for yeast, we are using zeolites instead of enzymes to catalyze the two bottleneck reactions in biomass conversion, xylose isomerization and ceuobiose hydrolysis. The experimental results on these reactions carried out over various zeolites and other catalysts are presented herein. The advantages and disadvantages of using these catalysts over enzymes are also discussed. Heterogeneous solid catalysts other than zeolites has been employed for cellobiose-to-glucose hydrolysis. The size and shape selectivity that makes zeoutes unique for some reactions can add diffusional hindrance. We have spent some time screening various known solid acidic catalysts. We report that a class of cationic ion exchange resins in the acidified form (e.g. Amberlite) has worked well as an acidic catalyst in hydrolyzing cellobiose to glucose. Our experimental results, together with those obtained from a homogeneous acid catalyst (e.g. sulfuric acid) for comparison are provided. Having succeeded in finding an alternative solid acid catalyst for hydrolysis, we explored other solid resin or other homogeneous but non-enzyme catalyst to carry out the xylose-to-xylulose isomerization. A fairly extensive search has been made. We explored the use of sodium aluminates in the homogeneous phase isomerization of glucose to fructose and obtained a very high conversion of glucose to fructose with the final mixture containing 85% of fructose instead of the common 45%. Fructose apparently complexes with aluminates, and its equilibrium concentration is shifted to considerably higher values than permitted by simple glucose/fructose equilibrium. We have recently found a number of catalysts capable of promoting isomerization between aldoses and ketoses. One solid resin, known as polyvinyl pyridine (PVP), is able to convert xylose to xylulose at a pH below 7. Our usage of alternative isomerization catalysts, including PVP, are described.

  7. [Zeolite catalysis in conversion of cellulosics

    SciTech Connect (OSTI)

    Tsao, G.T.

    1992-01-01

    To transform biomass into fermentable substrate for yeast, we are using zeolites instead of enzymes to catalyze the two bottleneck reactions in biomass conversion, xylose isomerization and ceuobiose hydrolysis. The experimental results on these reactions carried out over various zeolites and other catalysts are presented herein. The advantages and disadvantages of using these catalysts over enzymes are also discussed. Heterogeneous solid catalysts other than zeolites has been employed for cellobiose-to-glucose hydrolysis. The size and shape selectivity that makes zeoutes unique for some reactions can add diffusional hindrance. We have spent some time screening various known solid acidic catalysts. We report that a class of cationic ion exchange resins in the acidified form (e.g. Amberlite) has worked well as an acidic catalyst in hydrolyzing cellobiose to glucose. Our experimental results, together with those obtained from a homogeneous acid catalyst (e.g. sulfuric acid) for comparison are provided. Having succeeded in finding an alternative solid acid catalyst for hydrolysis, we explored other solid resin or other homogeneous but non-enzyme catalyst to carry out the xylose-to-xylulose isomerization. A fairly extensive search has been made. We explored the use of sodium aluminates in the homogeneous phase isomerization of glucose to fructose and obtained a very high conversion of glucose to fructose with the final mixture containing 85% of fructose instead of the common 45%. Fructose apparently complexes with aluminates, and its equilibrium concentration is shifted to considerably higher values than permitted by simple glucose/fructose equilibrium. We have recently found a number of catalysts capable of promoting isomerization between aldoses and ketoses. One solid resin, known as polyvinyl pyridine (PVP), is able to convert xylose to xylulose at a pH below 7. Our usage of alternative isomerization catalysts, including PVP, are described.

  8. Catalysis Working Group Meeting: June 2014

    Broader source: Energy.gov [DOE]

    Agenda and presentations from the Catalysis Working Group held on June 16, 2014, in Washington, D.C., in conjunction with the DOE Hydrogen and Fuel Cells Program Annual Merit Review and Peer Evaluation Meeting.

  9. Catalysis Working Group Meeting: May 2013

    Broader source: Energy.gov [DOE]

    Information from the Catalysis Working Group meeting held on May 15, 2013, in Arlington, Virginia, in conjunction with the DOE Hydrogen and Fuel Cells Program Annual Merit Review and Peer Evaluation Meeting.

  10. Advanced Resources for Catalysis Science; Recommendations for a National Catalysis Research Institute

    SciTech Connect (OSTI)

    Peden, Charles HF.; Ray, Douglas

    2005-10-05

    Catalysis is one of the most valuable contributors to our economy and historically an area where the United States has enjoyed, but is now losing, international leadership. While other countries are stepping up their work in this area, support for advanced catalysis research and development in the U.S. has diminished. Yet, more than ever, innovative and improved catalyst technologies are imperative for new energy production processes to ease our dependence on imported resources, for new energy-efficient and environmentally benign chemical production processes, and for new emission reduction technologies to minimize the environmental impact of an active and growing economy. Addressing growing concerns about the future direction of U.S. catalysis science, experts from the catalysis community met at a workshop to determine and recommend advanced resources needed to address the grand challenges for catalysis research and development. The workshop's primary conclusion: To recapture our position as the leader in catalysis innovation and practice, and promote crucial breakthroughs, the U.S. must establish one or more well-funded and well-equipped National Catalysis Research Institutes competitively selected, centered in the national laboratories and, by charter, networked to other national laboratories, universities, and industry. The Institute(s) will be the center of a national collaboratory that gives catalysis researchers access to the most advanced techniques available in the scientific enterprise. The importance of catalysis to our energy, economic, and environmental security cannot be overemphasized. Catalysis is a vital part of our core industrial infrastructure, as it is integral to chemical processing and petroleum refining, and is critical to proposed advances needed to secure a sustainable energy future. Advances in catalysis could reduce our need for foreign oil by making better use of domestic carbon resources, for example, allowing cost-effective and zero emission conversion of coal into transportation fuels. No matter what energy sources are being considered (oil, natural gas, coal, biomass, solar, or nuclear based), a clean, sustainable energy future will involve catalysis to improve energy efficiency and storage and use options, and to mitigate environmental impacts. Recent revolutionary advances in nanotechnology and high-performance computing are enabling the breakthroughs in catalysis science and technology essential for a secure energy future. Thus, the time is right for substantially increased investments in catalysis science and technology.

  11. HOMOGENEOUS NUCLEAR POWER REACTOR

    DOE Patents [OSTI]

    King, L.D.P.

    1959-09-01

    A homogeneous nuclear power reactor utilizing forced circulation of the liquid fuel is described. The reactor does not require fuel handling outside of the reactor vessel during any normal operation including complete shutdown to room temperature, the reactor being selfregulating under extreme operating conditions and controlled by the thermal expansion of the liquid fuel. The liquid fuel utilized is a uranium, phosphoric acid, and water solution which requires no gus exhaust system or independent gas recombining system, thereby eliminating the handling of radioiytic gas.

  12. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis ALS X-Rays Shine a New Light on Catalysis Print Thursday, 21 May 2015 11:16 Electrocatalysts are responsible for expediting reactions in...

  13. Catalysis Science | U.S. DOE Office of Science (SC)

    Office of Science (SC) Website

    Catalysis Science Chemical Sciences, Geosciences, & Biosciences (CSGB) Division CSGB Home ... principles enabling rational catalyst design and chemical transformation control. ...

  14. Opportunities in Catalysis Research Using Synchrotron Radiation

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

    in Catalysis Research Using Synchrotron Radiation Tuesday 10/8/02 Chair: Lars Pettersson 1:30-1:40 Anders Nilsson Welcome 1:40-2:30 Gabor Somorjai University of California, Berkeley and LBLN Need for New Directions of Research at the Frontiers of Catalysis Science 2:30-3:00 Geoff Thornton University of Manchester Influence of defects on the reactivity of ZnO 3:00-3:30 Anders Nilsson Stanford Synchrotron Radiation Laboratory Soft X-ray Spectroscopy of Surfaces and Reactions 3:30-3:45 Break Chair:

  15. HOMOGENEOUS NUCLEAR REACTOR

    DOE Patents [OSTI]

    Hammond, R.P.; Busey, H.M.

    1959-02-17

    Nuclear reactors of the homogeneous liquid fuel type are discussed. The reactor is comprised of an elongated closed vessel, vertically oriented, having a critical region at the bottom, a lower chimney structure extending from the critical region vertically upwardly and surrounded by heat exchanger coils, to a baffle region above which is located an upper chimney structure containing a catalyst functioning to recombine radiolyticallydissociated moderator gages. In operation the liquid fuel circulates solely by convection from the critical region upwardly through the lower chimney and then downwardly through the heat exchanger to return to the critical region. The gases formed by radiolytic- dissociation of the moderator are carried upwardly with the circulating liquid fuel and past the baffle into the region of the upper chimney where they are recombined by the catalyst and condensed, thence returning through the heat exchanger to the critical region.

  16. USD Catalysis Group for Alternative Energy

    SciTech Connect (OSTI)

    Hoefelmeyer, James D.; Koodali, Ranjit; Sereda, Grigoriy; Engebretson, Dan; Fong, Hao; Puszynski, Jan; Shende, Rajesh; Ahrenkiel, Phil

    2012-03-13

    The South Dakota Catalysis Group (SDCG) is a collaborative project with mission to develop advanced catalysts for energy conversion with two primary goals: (1) develop photocatalytic systems in which polyfunctionalized TiO2 are the basis for hydrogen/oxygen synthesis from water and sunlight (solar fuels group), (2) develop new materials for hydrogen utilization in fuel cells (fuel cell group). In tandem, these technologies complete a closed chemical cycle with zero emissions.

  17. Nanoscale Advances in Catalysis and Energy Applications

    SciTech Connect (OSTI)

    Li, Yimin; Somorjai, Gabor A.

    2010-05-12

    In this perspective, we present an overview of nanoscience applications in catalysis, energy conversion, and energy conservation technologies. We discuss how novel physical and chemical properties of nanomaterials can be applied and engineered to meet the advanced material requirements in the new generation of chemical and energy conversion devices. We highlight some of the latest advances in these nanotechnologies and provide an outlook at the major challenges for further developments.

  18. Thermochemical Conversion: Using Heat and Catalysis to Make Biofuels and

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

    Bioproducts | Department of Energy Conversion: Using Heat and Catalysis to Make Biofuels and Bioproducts Thermochemical Conversion: Using Heat and Catalysis to Make Biofuels and Bioproducts The Bioenergy Technologies Office works with industry to develop pathways that use heat, pressure, and catalysis to convert domestic, non-food biomass into gasoline, jet fuel, and other products. PDF icon thermochemical_four_pager.pdf More Documents & Publications 2013 Peer Review

  19. Catalysis Working Group Meeting: January 2015 | Department of Energy

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

    January 2015 Catalysis Working Group Meeting: January 2015 The Catalysis Working Group held a meeting on January 21, 2015, in Los Alamos, New Mexico. Meeting Agenda and Presentations PDF icon Catalysis Working Group January 2015 Meeting Agenda PDF icon Electrocatalysts with Ultra-Low PGM Loadings-Vojislav Stamenkovic, Argonne National Laboratory PDF icon Improving Stability and Activity of Pt Monolayer in Non-Pt Core-Shell Electrocatalysts-Radoslav Adzic, Brookhaven National Laboratory PDF icon

  20. Catalysis by Design: Bridging the Gap between Theory and Experiments...

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

    Catalysis by Design: Bridging the Gap between Theory and Experiments Poster presentation at the 2007 Diesel Engine-Efficiency & Emissions Research Conference (DEER 2007). 13-16 ...

  1. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme...

  2. Center for Biological Electron Transfer and Catalysis (BETCy...

    Office of Science (SC) Website

    Research Topics solar (fuels), biofuels (including algae and biomass), bio-inspired, ... 5 GrandChallenge 2 Grand Challenge 2 BES Reports Catalysis Hydrogen Solar Energy

  3. Materials Design and Discovery: Catalysis and Energy Storage...

    Office of Scientific and Technical Information (OSTI)

    Materials Design and Discovery: Catalysis and Energy Storage (Mira Early Science Program Final Technical Report): ALCF-2 Early Science Program Technical Report Citation Details ...

  4. Catalysis by Design - Theoretical and Experimental Studies of...

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

    Design - Theoretical and Experimental Studies of Model Catalysts for Lean NOx Treatment Catalysis by Design - Theoretical and Experimental Studies of Model Catalysts for Lean NOx ...

  5. Catalysis | U.S. DOE Office of Science (SC)

    Office of Science (SC) Website

    Catalysis Basic Energy Sciences Advisory Committee (BESAC) BESAC Home Meetings Meeting Presentations History Logistics BESAC 2016-2017 Membership ChargesReports Charter .pdf file ...

  6. Plasma-Activated Lean NOx Catalysis for Heavy-Duty Diesel Emissions...

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

    Plasma-Activated Lean NOx Catalysis for Heavy-Duty Diesel Emissions Control Plasma-Activated Lean NOx Catalysis for Heavy-Duty Diesel Emissions Control PDF icon ...

  7. Computationally Optimized Homogenization Heat Treatment of Metal...

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

    Return to Search Computationally Optimized Homogenization Heat Treatment of Metal Alloys ... PDF Document Publication Computationally Optimized Homogenization Heat Treatment of Metal ...

  8. Microgrids and Heterogeneous Power Quality and Reliability

    SciTech Connect (OSTI)

    LaCommare, Kristina; Marnay, Chris

    2007-10-01

    This paper describes two stylized alternative visions of how the power system might evolve to meet future requirements for the high quality electricity service that modern digital economies demand, a supergrids paradigm and a dispersed paradigm. Some of the economics of the dispersed vision are explored, and perspectives are presented on both the choice of homogeneous universal power quality upstream in the electricity supply chain and on the extremely heterogeneous requirements of end-use loads. It is argued that meeting the demanding requirements of sensitive loads by local provision of high quality power may be more cost effective than increasing the quality of universal homogeneous supply upstream in the legacy grid. Finally, the potential role of microgrids in delivering heterogeneous power quality is demonstrated by reference to two ongoing microgrid tests in the U.S. and Japan.

  9. Wetting of a Chemically Heterogeneous Surface

    SciTech Connect (OSTI)

    Frink, L.J.D.; Salinger, A.G.

    1998-11-20

    Theories for inhomogeneous fluids have focused in recent years on wetting, capillary conden- sation, and solvation forces for model systems where the surface(s) is(are) smooth homogeneous parallel plates, cylinders, or spherical drops. Unfortunately natural systems are more likely to be hetaogeneous both in surt%ce shape and surface chemistry. In this paper we discuss the conse- quences of chemical heterogeneity on wetting. Specifically, a 2-dimensional implementation of a nonlocal density functional theory is solved for a striped surface model. Both the strength and range of the heterogeneity are varied. Contact angles are calculated, and phase transitions (both the wetting transition and a local layering transition) are located. The wetting properties of the surface ase shown to be strongly dependent on the nature of the surface heterogeneity. In addition highly ordered nanoscopic phases are found, and the operational limits for formation of ordered or crystalline phases of nanoscopic extent are discussed.

  10. Modeling aspects of the dynamic response of heterogeneous materials

    SciTech Connect (OSTI)

    Ionita, Axinte; Clements, Brad; Mas, Eric

    2009-01-01

    In numerical simulations of engineering applications involving heterogeneous materials capturing the local response coming from a distribution of heterogeneities can lead to a very large model thus making simulations difficult. The use of homogenization techniques can reduce the size of the problem but will miss the local effects. Homogenization can also be difficult if the constituents obey different types of constitutive laws. Additional complications arise if inelastic deformation. In such cases a two-scale approach is prefened and tills work addresses these issues in the context of a two-scale Finite Element Method (FEM). Examples of using two-scale FEM approaches are presented.

  11. Catalysis Working Group Kick-Off Meeting Agenda

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

    Arlington, VA - May 14, 2012 Catalysis Working Group Kick-off Meeting Co-Chairs: Piotr Zelenay Los Alamos National Laboratory Nancy L. Garland U.S. Department of Energy 2 2...

  12. Catalysis Working Group Kick-Off Meeting Agenda

    Broader source: Energy.gov [DOE]

    Agenda for the kick-off meeting of the U.S. Department of Energy Fuel Cell Technologies Program's Catalysis Working Group, held May 14, 2012, in Arlington, Virginia.

  13. Materials Design and Discovery: Catalysis and Energy Storage (Mira Early

    Office of Scientific and Technical Information (OSTI)

    Science Program Final Technical Report): ALCF-2 Early Science Program Technical Report (Technical Report) | SciTech Connect Materials Design and Discovery: Catalysis and Energy Storage (Mira Early Science Program Final Technical Report): ALCF-2 Early Science Program Technical Report Citation Details In-Document Search Title: Materials Design and Discovery: Catalysis and Energy Storage (Mira Early Science Program Final Technical Report): ALCF-2 Early Science Program Technical Report Authors:

  14. Theoretical Study on Catalysis by Protein Enzymes and Ribozyme

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

    Theoretical Study on Catalysis by Protein Enzymes and Ribozyme Theoretical Study on Catalysis by Protein Enzymes and Ribozyme 2000 NERSC Annual Report 17shkarplus.jpg The energetics were determined for three mechanisms proposed for TIM catalyzed reactions. Results from reaction path calculations suggest that the two mechanisms that involve an enediol intermediate are likely to occur, while the direct intra-substrate proton transfer mechanism (in green) is energetically unfavorable due to the

  15. Biochemical Conversion: Using Hydrolysis, Fermentation, and Catalysis to

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

    Make Fuels and Chemicals | Department of Energy Biochemical Conversion: Using Hydrolysis, Fermentation, and Catalysis to Make Fuels and Chemicals Biochemical Conversion: Using Hydrolysis, Fermentation, and Catalysis to Make Fuels and Chemicals BETO works with the emerging U.S. bioindustry to sustainably convert non-food biomass resources into cost-competitive biofuels, biopower, and bioproducts. PDF icon biochemical_four_pager.pdf More Documents & Publications Replacing the Whole

  16. Visualizing Group II Intron Catalysis through the Stages of Splicing

    Office of Scientific and Technical Information (OSTI)

    (Journal Article) | SciTech Connect SciTech Connect Search Results Journal Article: Visualizing Group II Intron Catalysis through the Stages of Splicing Citation Details In-Document Search Title: Visualizing Group II Intron Catalysis through the Stages of Splicing Authors: Marcia, Marco ; Pyle, Anna Marie [1] ; HHMI) [2] + Show Author Affiliations (Yale) ( Publication Date: 2013-01-10 OSTI Identifier: 1054354 Resource Type: Journal Article Resource Relation: Journal Name: Cell; Journal

  17. Outer sphere hydrogenation catalysis (Journal Article) | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    Outer sphere hydrogenation catalysis Citation Details In-Document Search Title: Outer sphere hydrogenation catalysis Authors: Eisenstein, Odile ; Crabtree, Robert H Publication Date: 2013-01-01 OSTI Identifier: 1080563 DOE Contract Number: SC0001055 Resource Type: Journal Article Resource Relation: Journal Name: New J. Chem.; Journal Volume: 37; Related Information: CETM partners with General Electric Global Research (lead); Lawrence Berkeley National Laboratory; Stanford University; Yale

  18. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis ALS X-Rays Shine a New Light on Catalysis Print Thursday, 21 May 2015 11:16 Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab

  19. Dedicated Beamline Facilities for Catalytic Research. Synchrotron Catalysis Consortium (SCC)

    SciTech Connect (OSTI)

    Chen, Jingguang; Frenkel, Anatoly; Rodriguez, Jose; Adzic, Radoslav; Bare, Simon R.; Hulbert, Steve L.; Karim, Ayman; Mullins, David R.; Overbury, Steve

    2015-03-04

    Synchrotron spectroscopies offer unique advantages over conventional techniques, including higher detection sensitivity and molecular specificity, faster detection rate, and more in-depth information regarding the structural, electronic and catalytic properties under in-situ reaction conditions. Despite these advantages, synchrotron techniques are often underutilized or unexplored by the catalysis community due to various perceived and real barriers, which will be addressed in the current proposal. Since its establishment in 2005, the Synchrotron Catalysis Consortium (SCC) has coordinated significant efforts to promote the utilization of cutting-edge catalytic research under in-situ conditions. The purpose of the current renewal proposal is aimed to provide assistance, and to develop new sciences/techniques, for the catalysis community through the following concerted efforts: Coordinating the implementation of a suite of beamlines for catalysis studies at the new NSLS-II synchrotron source; Providing assistance and coordination for catalysis users at an SSRL catalysis beamline during the initial period of NSLS to NSLS II transition; Designing in-situ reactors for a variety of catalytic and electrocatalytic studies; Assisting experimental set-up and data analysis by a dedicated research scientist; Offering training courses and help sessions by the PIs and co-PIs.

  20. Dynamic nuclear polarization solid-state NMR in heterogeneous catalysis research

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

    Kobayashi, Takeshi; Perras, Frédéric A.; Slowing, Igor I.; Sadow, Aaron D.; Pruski, Marek

    2015-10-20

    In this study, a revolution in solid-state nuclear magnetic resonance (SSNMR) spectroscopy is taking place, attributable to the rapid development of high-field dynamic nuclear polarization (DNP), a technique yielding sensitivity improvements of 2–3 orders of magnitude. This higher sensitivity in SSNMR has already impacted materials research, and the implications of new methods on catalytic sciences are expected to be profound.

  1. Some General Themes in Catalysis at LANL

    SciTech Connect (OSTI)

    Gordon, John C.

    2012-07-19

    Some general themes in catalysis at LANL are: (1) Storage and release of energy within chemical bonds (e.g. H{sub 2} storage in and release from covalent bonds, N{sub 2} functionalization, CO{sub 2} functionalization, H{sub 2} oxidation/evolution, O{sub 2} reduction/evolution); (2) Can we control the chemistry of reactive substrates to effect energy relevant transformations in non-traditional media (e.g. can we promote C-C couplings, dehydrations, or hydrogenations in water under relatively mild conditions)? (3) Can we supplant precious metal or rare earth catalysts to effect these transformations, by using earth abundant metals/elements instead? Can we use organocatalysis and circumvent the use of metals completely? (4) Can we improve upon existing rare earth catalyst systems (e.g. in rare earth oxides pertinent to fluid cracking or polymerization) and reduce amounts required for catalytic efficacy? Carbohydrates can be accessed from non-food based biomass sources such as woody residues and switchgrass. After extracted from the plant source, our goal is to upgrade these classes of molecules into useful fuels.

  2. Coherence delay augmented laser beam homogenizer

    DOE Patents [OSTI]

    Rasmussen, P.; Bernhardt, A.

    1993-06-29

    The geometrical restrictions on a laser beam homogenizer are relaxed by ug a coherence delay line to separate a coherent input beam into several components each having a path length difference equal to a multiple of the coherence length with respect to the other components. The components recombine incoherently at the output of the homogenizer, and the resultant beam has a more uniform spatial intensity suitable for microlithography and laser pantogography. Also disclosed is a variable aperture homogenizer, and a liquid filled homogenizer.

  3. Invariant distributions on compact homogeneous spaces

    SciTech Connect (OSTI)

    Gorbatsevich, V V

    2013-12-31

    In this paper, we study distributions on compact homogeneous spaces, including invariant distributions and also distributions admitting asub-Riemannian structure. We first consider distributions of dimension 1 and 2 on compact homogeneous spaces. After this, we study the cases of compact homogeneous spaces of dimension 2, 3, and 4 in detail. Invariant distributions on simply connected compact homogeneous spaces are also treated. Bibliography: 18 titles.

  4. Coherence delay augmented laser beam homogenizer

    DOE Patents [OSTI]

    Rasmussen, Paul (Livermore, CA); Bernhardt, Anthony (Berkeley, CA)

    1993-01-01

    The geometrical restrictions on a laser beam homogenizer are relaxed by ug a coherence delay line to separate a coherent input beam into several components each having a path length difference equal to a multiple of the coherence length with respect to the other components. The components recombine incoherently at the output of the homogenizer, and the resultant beam has a more uniform spatial intensity suitable for microlithography and laser pantogography. Also disclosed is a variable aperture homogenizer, and a liquid filled homogenizer.

  5. One- and two-dimensional infrared spectroscopic studies of solution-phase homogeneous catalysis and spin-forbidden reactions

    SciTech Connect (OSTI)

    Sawyer, Karma Rae

    2008-12-12

    Understanding chemical reactions requires the knowledge of the elementary steps of breaking and making bonds, and often a variety of experimental techniques are needed to achieve this goal. The initial steps occur on the femto- through picosecond time-scales, requiring the use of ultrafast spectroscopic methods, while the rate-limiting steps often occur more slowly, requiring alternative techniques. Ultrafast one and two-dimensional infrared and step-scan FTIR spectroscopies are used to investigate the photochemical reactions of four organometallic complexes. The analysis leads to a detailed understanding of mechanisms that are general in nature and may be applicable to a variety of reactions.

  6. Study of catalysis of coal gasification at elevated pressures. [Evaluation

    Office of Scientific and Technical Information (OSTI)

    of 20 compounds at 850/sup 0/C] (Journal Article) | SciTech Connect Study of catalysis of coal gasification at elevated pressures. [Evaluation of 20 compounds at 850/sup 0/C] Citation Details In-Document Search Title: Study of catalysis of coal gasification at elevated pressures. [Evaluation of 20 compounds at 850/sup 0/C] Authors: Haynes, W.P. ; Neilson, H. [1] ; Field, J.H. + Show Author Affiliations (US Bur. Mines, Pittsburgh, PA) Publication Date: 1971-01-01 OSTI Identifier: 5238924

  7. Surfkin: A program to solve transient and steady state heterogeneous reaction kinetics

    SciTech Connect (OSTI)

    COLTRIN,MICHAEL E.; WIXOM,RYAN R.; DANDY,DAVID S.

    2000-05-01

    Heterogeneous chemical reactions occurring at a gas/surface interface are fundamental in a variety of important applications, such as combustion, catalysis, chemical vapor deposition and plasma processing. Detailed simulation of these processes may involve complex, coupled fluid flow, heat transfer, gas-phase chemistry, in addition to heterogeneous reaction chemistry. This report documents the Surfkin program, which simulates the kinetics of heterogeneous chemical reactions. The program is designed for use with the Chemkin and Surface Chemkin (heterogeneous chemistry) programs. It calculates time-dependent or steady state surface site fractions and bulk-species production/destruction rates. The surface temperature may be specified as a function of time to simulate a temperature-programmed desorption experiment, for example. This report serves as a user's manual for the program, explaining the required input and format of the output. Two detailed example problems are included to further illustrate the use of this program.

  8. Dedicated heterogeneous node scheduling including backfill scheduling

    DOE Patents [OSTI]

    Wood, Robert R. (Livermore, CA); Eckert, Philip D. (Livermore, CA); Hommes, Gregg (Pleasanton, CA)

    2006-07-25

    A method and system for job backfill scheduling dedicated heterogeneous nodes in a multi-node computing environment. Heterogeneous nodes are grouped into homogeneous node sub-pools. For each sub-pool, a free node schedule (FNS) is created so that the number of to chart the free nodes over time. For each prioritized job, using the FNS of sub-pools having nodes useable by a particular job, to determine the earliest time range (ETR) capable of running the job. Once determined for a particular job, scheduling the job to run in that ETR. If the ETR determined for a lower priority job (LPJ) has a start time earlier than a higher priority job (HPJ), then the LPJ is scheduled in that ETR if it would not disturb the anticipated start times of any HPJ previously scheduled for a future time. Thus, efficient utilization and throughput of such computing environments may be increased by utilizing resources otherwise remaining idle.

  9. AQUEOUS HOMOGENEOUS REACTORTECHNICAL PANEL REPORT

    SciTech Connect (OSTI)

    Diamond, D.J.; Bajorek, S.; Bakel, A.; Flanagan, G.; Mubayi, V.; Skarda, R.; Staudenmeier, J.; Taiwo, T.; Tonoike, K.; Tripp, C.; Wei, T.; Yarsky, P.

    2010-12-03

    Considerable interest has been expressed for developing a stable U.S. production capacity for medical isotopes and particularly for molybdenum- 99 (99Mo). This is motivated by recent re-ductions in production and supply worldwide. Consistent with U.S. nonproliferation objectives, any new production capability should not use highly enriched uranium fuel or targets. Conse-quently, Aqueous Homogeneous Reactors (AHRs) are under consideration for potential 99Mo production using low-enriched uranium. Although the Nuclear Regulatory Commission (NRC) has guidance to facilitate the licensing process for non-power reactors, that guidance is focused on reactors with fixed, solid fuel and hence, not applicable to an AHR. A panel was convened to study the technical issues associated with normal operation and potential transients and accidents of an AHR that might be designed for isotope production. The panel has produced the requisite AHR licensing guidance for three chapters that exist now for non-power reactor licensing: Reac-tor Description, Reactor Coolant Systems, and Accident Analysis. The guidance is in two parts for each chapter: 1) standard format and content a licensee would use and 2) the standard review plan the NRC staff would use. This guidance takes into account the unique features of an AHR such as the fuel being in solution; the fission product barriers being the vessel and attached systems; the production and release of radiolytic and fission product gases and their impact on operations and their control by a gas management system; and the movement of fuel into and out of the reactor vessel.

  10. Homogeneous catalysts in hypersonic combustion

    SciTech Connect (OSTI)

    Harradine, D.M.; Lyman, J.L.; Oldenborg, R.C.; Pack, R.T.; Schott, G.L.

    1989-01-01

    Density and residence time both become unfavorably small for efficient combustion of hydrogen fuel in ramjet propulsion in air at high altitude and hypersonic speed. Raising the density and increasing the transit time of the air through the engine necessitates stronger contraction of the air flow area. This enhances the kinetic and thermodynamic tendency of H/sub 2/O to form completely, accompanied only by N/sub 2/ and any excess H/sub 2/(or O/sub 2/). The by-products to be avoided are the energetically expensive fragment species H and/or O atoms and OH radicals, and residual (2H/sub 2/ plus O/sub 2/). However, excessive area contraction raises air temperature and consequent combustion-product temperature by adiabatic compression. This counteracts and ultimately overwhelms the thermodynamic benefit by which higher density favors the triatomic product, H/sub 2/O, over its monatomic and diatomic alternatives. For static pressures in the neighborhood of 1 atm, static temperature must be kept or brought below ca. 2400 K for acceptable stability of H/sub 2/O. Another measure, whose requisite chemistry we address here, is to extract propulsive work from the combustion products early in the expansion. The objective is to lower the static temperature of the combustion stream enough for H/sub 2/O to become adequately stable before the exhaust flow is massively expanded and its composition ''frozen.'' We proceed to address this mechanism and its kinetics, and then examine prospects for enhancing its rate by homogeneous catalysts. 9 refs.

  11. MRI of Heterogeneous Hydrogenation Reactions Using Parahydrogen Polarization

    SciTech Connect (OSTI)

    Burt, Scott R; Burt, Scott R.

    2008-06-25

    The power of magnetic resonance imaging (MRI) is its ability to image the internal structure of optically opaque samples and provide detailed maps of a variety of important parameters, such as density, diffusion, velocity and temperature. However, one of the fundamental limitations of this technique is its inherent low sensitivity. For example, the low signal to noise ratio (SNR) is particularly problematic for imaging gases in porous materials due to the low density of the gas and the large volume occluded by the porous material. This is unfortunate, as many industrially relevant chemical reactions take place at gas-surface interfaces in porous media, such as packed catalyst beds. Because of this severe SNR problem, many techniques have been developed to directly increase the signal strength. These techniques work by manipulating the nuclear spin populations to produce polarized} (i.e., non-equilibrium) states with resulting signal strengths that are orders of magnitude larger than those available at thermal equilibrium. This dissertation is concerned with an extension of a polarization technique based on the properties of parahydrogen. Specifically, I report on the novel use of heterogeneous catalysis to produce parahydrogen induced polarization and applications of this new technique to gas phase MRI and the characterization of micro-reactors. First, I provide an overview of nuclear magnetic resonance (NMR) and how parahydrogen is used to improve the SNR of the NMR signal. I then present experimental results demonstrating that it is possible to use heterogeneous catalysis to produce parahydrogen-induced polarization. These results are extended to imaging void spaces using a parahydrogen polarized gas. In the second half of this dissertation, I demonstrate the use of parahydrogen-polarized gas-phase MRI for characterizing catalytic microreactors. Specifically, I show how the improved SNR allows one to map parameters important for characterizing the heat and mass transport in a heterogeneous catalyst bed. This is followed by appendices containing detailed information regarding the design and use of my experimental setup.

  12. Lean NOx Trap Catalysis for Lean Natural Gas Engine Applications

    SciTech Connect (OSTI)

    Parks, II, James E; Storey, John Morse; Theiss, Timothy J; Ponnusamy, Senthil; Ferguson, Harley Douglas; Williams, Aaron M; Tassitano, James B

    2007-09-01

    Distributed energy is an approach for meeting energy needs that has several advantages. Distributed energy improves energy security during natural disasters or terrorist actions, improves transmission grid reliability by reducing grid load, and enhances power quality through voltage support and reactive power. In addition, distributed energy can be efficient since transmission losses are minimized. One prime mover for distributed energy is the natural gas reciprocating engine generator set. Natural gas reciprocating engines are flexible and scalable solutions for many distributed energy needs. The engines can be run continuously or occasionally as peak demand requires, and their operation and maintenance is straightforward. Furthermore, system efficiencies can be maximized when natural gas reciprocating engines are combined with thermal energy recovery for cooling, heating, and power applications. Expansion of natural gas reciprocating engines for distributed energy is dependent on several factors, but two prominent factors are efficiency and emissions. Efficiencies must be high enough to enable low operating costs, and emissions must be low enough to permit significant operation hours, especially in non-attainment areas where emissions are stringently regulated. To address these issues the U.S. Department of Energy and the California Energy Commission launched research and development programs called Advanced Reciprocating Engine Systems (ARES) and Advanced Reciprocating Internal Combustion Engines (ARICE), respectively. Fuel efficiency and low emissions are two primary goals of these programs. The work presented here was funded by the ARES program and, thus, addresses the ARES 2010 goals of 50% thermal efficiency (fuel efficiency) and <0.1 g/bhp-hr emissions of oxides of nitrogen (NOx). A summary of the goals for the ARES program is given in Table 1-1. ARICE 2007 goals are 45% thermal efficiency and <0.015 g/bhp-hr NOx. Several approaches for improving the efficiency and emissions of natural gas reciprocating engines are being pursued. Approaches include: stoichiometric engine operation with exhaust gas recirculation and three-way catalysis, advanced combustion modes such as homogeneous charge compression ignition, and extension of the lean combustion limit with advanced ignition concepts and/or hydrogen mixing. The research presented here addresses the technical approach of combining efficient lean spark-ignited natural gas combustion with low emissions obtained from a lean NOx trap catalyst aftertreatment system. This approach can be applied to current lean engine technology or advanced lean engines that may result from related efforts in lean limit extension. Furthermore, the lean NOx trap technology has synergy with hydrogen-assisted lean limit extension since hydrogen is produced from natural gas during the lean NOx trap catalyst system process. The approach is also applicable to other lean engines such as diesel engines, natural gas turbines, and lean gasoline engines; other research activities have focused on those applications. Some commercialization of the technology has occurred for automotive applications (both diesel and lean gasoline engine vehicles) and natural gas turbines for stationary power. The research here specifically addresses barriers to commercialization of the technology for large lean natural gas reciprocating engines for stationary power. The report presented here is a comprehensive collection of research conducted by Oak Ridge National Laboratory (ORNL) on lean NOx trap catalysis for lean natural gas reciprocating engines. The research was performed in the Department of Energy's ARES program from 2003 to 2007 and covers several aspects of the technology. All studies were conducted at ORNL on a Cummins C8.3G+ natural gas engine chosen based on industry input to simulate large lean natural gas engines. Specific technical areas addressed by the research include: NOx reduction efficiency, partial oxidation and reforming chemistry, and the effects of sulfur poisons on the partial oxidation, reformer, and lean NOx trap catalysts. The initial work on NOx reduction efficiency demonstrated that NOx emissions <0.1 g/bhp-hr (the ARES goal) can be achieved with the lean NOx trap catalyst technology. Subsequent work focused on cost and size optimization and durability issues which addressed two specific ARES areas of interest to industry ('Cost of Power' and 'Availability, Reliability, and Maintainability', respectively). Thus, the research addressed the approach of the lean NOx trap catalyst technology toward the ARES goals as shown in Table 1-1.

  13. Determining whether metals nucleate homogeneously on graphite: A case study with copper

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

    Appy, David; Lei, Huaping; Han, Yong; Wang, Cai -Zhuang; Tringides, Michael C.; Shao, Dahai; Kwolek, Emma J.; Evans, J. W.; Thiel, P. A.

    2014-11-05

    In this study, we observe that Cu clusters grow on surface terraces of graphite as a result of physical vapor deposition in ultrahigh vacuum. We show that the observation is incompatible with a variety of models incorporating homogeneous nucleation and calculations of atomic-scale energetics. An alternative explanation, ion-mediated heterogeneous nucleation, is proposed and validated, both with theory and experiment. This serves as a case study in identifying when and whether the simple, common observation of metal clusters on carbon-rich surfaces can be interpreted in terms of homogeneous nucleation. We describe a general approach for making system-specific and laboratory-specific predictions.

  14. Low temperature, sulfur tolerant homogeneous catalysts for the water-gas shift reaction

    SciTech Connect (OSTI)

    Laine, R.M.

    1986-01-20

    The purpose of this report is to update and reorganize our recent review on homogeneous catalysis of the water-gas shift reaction (WGSR) based on recent literature publications and patents. This updated version will serve as a means of selecting 10 candidate catalyst systems for use in developing effective, sulfur-tolerant, low temperature WGSR catalysts. This report discusses the variations possible in the basic chemistry associated with WGSR catalytic cycles, including basic, acidic, and neutral conditions. Then individual mechanism for specific WGSR catalyst systems are discussed. Finally, on the basis of the literature reports, a list is presented of candidate catalysts and basic systems we have chosen for study in Task 3.

  15. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis ... catalysis (heterogeneous), solar (photovoltaic), solar (fuels), photosynthesis ...

  16. Heterogeneous waste processing

    DOE Patents [OSTI]

    Vanderberg, Laura A.; Sauer, Nancy N.; Brainard, James R.; Foreman, Trudi M.; Hanners, John L.

    2000-01-01

    A combination of treatment methods are provided for treatment of heterogeneous waste including: (1) treatment for any organic compounds present; (2) removal of metals from the waste; and, (3) bulk volume reduction, with at least two of the three treatment methods employed and all three treatment methods emplyed where suitable.

  17. Iron Catalysis in Oxidations by Ozone - Energy Innovation Portal

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

    Find More Like This Return to Search Iron Catalysis in Oxidations by Ozone Ames Laboratory Contact AMES About This Technology Technology Marketing Summary Ozone is used commercially for treatment of potable and non-potable water, and as an industrial oxidant. ISU and Ames Laboratory researchers have developed a method for using iron in ozone oxidation that significantly improves the speed of oxidation reactions. Description Ozone is recognized as potent and effective oxidizing agent, and has a

  18. ECIS and Compass Metals: Platinum Nanostructures for Enhanced Catalysis

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

    ECIS and Compass Metals: Platinum Nanostructures for Enhanced Catalysis - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Fuel

  19. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  20. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  1. University of Delaware | Catalysis Center for Energy Innovation | Modeling

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

    Modeling Activity map produced from the new high-throughput computational engine. Example for ethylene glycol catalysis. Reforming, hydrodeoxygenation, dehydrogenation, and catalyst poisoning (e.g., coking) occur at different regions of the map. Major developments have taken place in first-principles-based prediction of reforming and hydrodeoxygenation catalysts for key biomass derivatives. These developments can eventually assist in catalyst and process design for bio-oil upgrade and conversion

  2. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  3. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  4. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  5. ALS X-Rays Shine a New Light on Catalysis

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

    ALS X-Rays Shine a New Light on Catalysis Print Electrocatalysts are responsible for expediting reactions in many promising renewable energy technologies. However, the extreme sensitivity of their surface redox states to temperatures, to gas pressures, and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Recently a team of Stanford and Berkeley Lab researchers used x-rays at the ALS in a novel way to observe the behavior of

  6. Catalysis by Design - Theoretical and Experimental Studies of Model

    Broader source: Energy.gov (indexed) [DOE]

    Catalysis Working Group (CWG) meets twice per year to exchange information, create synergies, and collaboratively develop both an understanding of and tools for studying electrocatalysis for polymer electrolyte fuel cells (PEFCs) and other low- and intermediate-temperature fuel cell systems, including direct methanol fuel cells (DMFCs), alkaline fuel cells (AFCs), alkaline membrane fuel cells (AMFCs), and phosphoric acid fuel cells (PAFCs). The CWG members include principal and co-principal

  7. Ionization of large homogeneous and heterogeneous clusters generated in acetylene-Ar expansions: Cluster ion polymerization

    SciTech Connect (OSTI)

    Kocisek, J.; Lengyel, J.; Farnik, M.

    2013-03-28

    Pure acetylene and mixed Ar-acetylene clusters are formed in supersonic expansions of acetylene/argon mixtures and analysed using reflectron time-of-flight mass spectrometer with variable electron energy ionization source. Acetylene clusters composed of more than a hundred acetylene molecules are generated at the acetylene concentration of Almost-Equal-To 8%, while mixed species are produced at low concentrations ( Almost-Equal-To 0.7%). The electron energy dependence of the mass spectra revealed the ionization process mechanisms in clusters. The ionization above the threshold for acetylene molecule of 11.5 eV results in the main ionic fragment progression (C{sub 2}H{sub 2}){sub n}{sup +}. At the electron energies Greater-Than-Or-Slanted-Equal-To 21.5 eV above the CH+CH{sup +} dissociative ionization limit of acetylene the fragment ions nominally labelled as (C{sub 2}H{sub 2}){sub n}CH{sup +}, n Greater-Than-Or-Slanted-Equal-To 2, are observed. For n Less-Than-Or-Slanted-Equal-To 7 these fragments correspond to covalently bound ionic structures as suggested by the observed strong dehydrogenation [(C{sub 2}H{sub 2}){sub n}-k Multiplication-Sign H]{sup +} and [(C{sub 2}H{sub 2}){sub n}CH -k Multiplication-Sign H]{sup +}. The dehydrogenation is significantly reduced in the mixed clusters where evaporation of Ar instead of hydrogen can stabilize the nascent molecular ion. The C{sub 3}H{sub 3}{sup +} ion was previously assigned to originate from the benzene molecular ion; however, the low appearance energy of Almost-Equal-To 13.7 eV indicates that a less rigid covalently bound structure of C{sub 6}H{sub 6}{sup +} ion must also be formed upon the acetylene cluster electron ionization. The appearance energy of Ar{sub n}(C{sub 2}H{sub 2}){sup +} fragments above Almost-Equal-To 15.1 eV indicates that the argon ionization is the first step in the fragment ion production, and the appearance energy of Ar{sub n{>=}2}(C{sub 2}H{sub 2}){sub m{>=}2}{sup +} at Almost-Equal-To 13.7 eV is discussed in terms of an exciton transfer mechanism.

  8. Untangling the Chemical Evolution of Titan's Atmosphere and Surface -- From Homogeneous to Heterogeneous Chemistry

    SciTech Connect (OSTI)

    Kaiser, Ralf I.; Maksyutenko, Pavlo; Ennis, Courtney; Zhang, Fangtong; Gu, Xibin; Krishtal, Sergey P.; Mebel, Alexander M.; Kostko, Oleg; Ahmed, Musahid

    2010-03-16

    The arrival of the Cassini-Huygens probe at Saturn's moon Titan - the only Solar System body besides Earth and Venus with a solid surface and a thick atmosphere with a pressure of 1.4 atm at surface level - in 2004 opened up a new chapter in the history of Solar System exploration. The mission revealed Titan as a world with striking Earth-like landscapes involving hydrocarbon lakes and seas as well as sand dunes and lava-like features interspersed with craters and icy mountains of hitherto unknown chemical composition. The discovery of a dynamic atmosphere and active weather system illustrates further the similarities between Titan and Earth. The aerosol-based haze layers, which give Titan its orange-brownish color, are not only Titan's most prominent optically visible features, but also play a crucial role in determining Titan's thermal structure and chemistry. These smog-like haze layers are thought to be very similar to those that were present in Earth's atmosphere before life developed more than 3.8 billion years ago, absorbing the destructive ultraviolet radiation from the Sun, thus acting as 'prebiotic ozone' to preserve astrobiologically important molecules on Titan. Compared to Earth, Titan's low surface temperature of 94 K and the absence of liquid water preclude the evolution of biological chemistry as we know it. Exactly because of these low temperatures, Titan provides us with a unique prebiotic 'atmospheric laboratory' yielding vital clues - at the frozen stage - on the likely chemical composition of the atmosphere of the primitive Earth. However, the underlying chemical processes, which initiate the haze formation from simple molecules, have been not understood well to date.

  9. Error Assessment of Homogenized Cross Sections Generation for Whole Core Neutronic Calculation

    SciTech Connect (OSTI)

    Hursin, Mathieu; Kochunas, Brendan; Downar, Thomas J.

    2007-10-26

    The objective of the work here was to assess the errors introduced by using 2D, few group homogenized cross sections to perform neutronic analysis of BWR problems with significant axial heterogeneities. The 3D method of characteristics code DeCART is used to generate 2-group assembly homogenized cross sections first using a conventional 2D lattice model and then using a full 3D solution of the assembly. A single BWR fuel assembly model based on an advanced BWR lattice design is used with a typical void distribution applied to the fuel channel coolant. This model is validated against an MCNP model. A comparison of the cross sections is performed for the assembly homogenized planar cross sections from the DeCART 3D and DeCART 2D solutions.

  10. Low-Temperature Hydrocarbon/CO Oxidation Catalysis in Support...

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

    ...-temperature oxidation of hydrocarbons and CO in homogeneous charge compression ignition (HCCI) emissions. PDF icon deer08rappe.pdf More Documents & Publications Low-Temperature ...

  11. EERE Success Story-Fundamental Studies in Catalysis Enabled the use of

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

    Efficient "Lean-Burn" Engines for Vehicle Transportation | Department of Energy Fundamental Studies in Catalysis Enabled the use of Efficient "Lean-Burn" Engines for Vehicle Transportation EERE Success Story-Fundamental Studies in Catalysis Enabled the use of Efficient "Lean-Burn" Engines for Vehicle Transportation May 7, 2015 - 1:29pm Addthis Building on a catalysis research program sponsored by EERE's Vehicles Technology Office (VTO) and DOE's Office of

  12. Hydrogen catalysis and scavenging action of Pd-POSS nanoparticles

    SciTech Connect (OSTI)

    Maiti, A; Gee, R H; Maxwell, R; Saab, A

    2007-02-01

    Prompted by the need for a self-supported, chemically stable, and functionally flexible catalytic nanoparticle system, we explore a system involving Pd clusters coated with a monolayer of polyhedral oligomeric silsesquioxane (POSS) cages. With an initial theoretical focus on hydrogen catalysis and sequestration in the Pd-POSS system, we report Density Functional Theory (DFT) results on POSS binding energies to the Pd(110) surface, hydrogen storing ability of POSS, and possible pathways of hydrogen radicals from the catalyst surface to unsaturated bonds away from the surface.

  13. Fuels and energy for the future: The role of catalysis

    SciTech Connect (OSTI)

    Rostrup-Nielsen, J.R.; Nielsen, R.

    2004-07-01

    There are many reasons to decrease the dependency on oil and to increase the use of other energy sources than fossil fuels. The wish for energy security is balanced by a wish for sustainable growth. Catalysis plays an important role in creating new routes and flexibility in the network of energy sources, energy carriers, and energy conversion. The process technologies resemble those applied in the large scale manufacture of commodities. This is illustrated by examples from refinery fuels, synfuels, and hydrogen and the future role of fossil fuels is discussed.

  14. USD Catalysis Group for Alternative Energy - Final report

    SciTech Connect (OSTI)

    Hoefelmeyer, James

    2014-10-03

    I. Project Summary Catalytic processes are a major technological underpinning of modern society, and are essential to the energy sector in the processing of chemical fuels from natural resources, fine chemicals synthesis, and energy conversion. Advances in catalyst technology are enormously valuable since these lead to reduced chemical waste, reduced energy loss, and reduced costs. New energy technologies, which are critical to future economic growth, are also heavily reliant on catalysts, including fuel cells and photo-electrochemical cells. Currently, the state of South Dakota is underdeveloped in terms of research infrastructure related to catalysis. If South Dakota intends to participate in significant economic growth opportunities that result from advances in catalyst technology, then this area of research needs to be made a high priority for investment. To this end, a focused research effort is proposed in which investigators from The University of South Dakota (USD) and The South Dakota School of Mines and Technology (SDSMT) will contribute to form the South Dakota Catalysis Group (SDCG). The multidisciplinary team of the (SDCG) include: (USD) Dan Engebretson, James Hoefelmeyer, Ranjit Koodali, and Grigoriy Sereda; (SDSMT) Phil Scott Ahrenkiel, Hao Fong, Jan Puszynski, Rajesh Shende, and Jacek Swiatkiewicz. The group is well suited to engage in a collaborative project due to the resources available within the existing programs. Activities within the SDCG will be monitored through an external committee consisting of three distinguished professors in chemistry. The committee will provide expert advice and recommendations to the SDCG. Advisory meetings in which committee members interact with South Dakota investigators will be accompanied by individual oral and poster presentations in a materials and catalysis symposium. The symposium will attract prominent scientists, and will enhance the visibility of research in the state of South Dakota. The SDCG requests funding through the Department of Energy (DoE) to establish this multidisciplinary research cluster in the area of catalysis. This long-term approach includes synthesis, characterization, catalyst evaluation, modeling, and scale-up. The project includes plans to acquire instrumentation critical to enabling competitive research. These acquisitions will complement existing resources in the state. The effect of implementation of the proposed efforts will be to significantly enhance state infrastructure in personnel and equipment, and lead to a nationally and internationally recognized research center.

  15. Assessment of Homogeneous Thorium/Uranium Fuel for Pressurized...

    Office of Scientific and Technical Information (OSTI)

    Fuel for Pressurized Water Reactors Citation Details In-Document Search Title: Assessment of Homogeneous ThoriumUranium Fuel for Pressurized Water Reactors The homogeneous ...

  16. Final technical report, Symposium on New Theoretical Concepts and Directions in Catalysis

    SciTech Connect (OSTI)

    Metiu, Horia

    2014-08-22

    We organized in August 2013 a “Symposium on New Theoretical Concepts and Directions in Catalysis” with the participation of 20 invited distinguished quantum chemists and other researchers who use computations to study catalysis. Symposium website; http://catalysis.cnsi.ucsb.edu/

  17. Plasma-Activated Lean NOx Catalysis for Heavy-Duty Diesel Emissions Control

    Broader source: Energy.gov (indexed) [DOE]

    | Department of Energy PDF icon 2002_deer_aardahl.pdf More Documents & Publications Heavy-Duty NOx Emissions Control: Reformer-Assisted vs. Plasma-Facilitated Lean NOx Catalysis Selective reduction of NOx in oxygen rich environments with plasma-assisted catalysis: Catalyst development and mechanistic studies

  18. Application of cryogenic grinding to achieve homogenization of transuranic wastes

    SciTech Connect (OSTI)

    Atkins, W.H.; Hill, D.D.; Lucero, M.E.; Jaramillo, L.; Martinez, H.E.

    1996-08-01

    This paper describes work done at Los Alamos National Laboratory (LANL) in collaboration with the Department of Energy Rocky Flats Field Office (DOE/RFFO) and with the National Institute of Standards and Technology (NIST), Boulder, Colorado. Researchers on this project have developed a method for cryogenic grinding of mixed wastes to homogenize and, thereby, to acquire a representative sample of the materials. There are approximately 220,000 waste drums owned by the Rocky Flats Environmental Technology Site (RFETS)-50,000 at RFETS and 170,000 at the Idaho National Engineering Laboratory. The cost of sampling the heterogeneous distribution of waste in each drum is prohibitive. In an attempt to produce a homogeneous mixture of waste that would reduce greatly the cost of sampling, researchers at NIST and RFETS are developing a cryogenic grinder. The Los Alamos work herein described addresses the implementation issues of the task. The first issue was to ascertain whether samples of the {open_quotes}small particle{close_quotes} mixtures of materials present in the waste drums at RFETS were representative of actual drum contents. Second, it was necessary to determine at what temperature the grinding operation must be performed in order to minimize or to eliminate the release of volatile organic compounds present in the waste. Last, it was essential to evaluate any effect the liquid cryogen might have on the structural integrity and ventilation capacity of the glovebox system. Results of this study showed that representative samples could be and had been obtained, that some release of organics occurred below freezing because of sublimation, and that operation of the cryogenic grinding equipment inside the glovebox was feasible.

  19. Surface Catalysis of Water Oxidation by the Blue Ruthenium Dimer

    SciTech Connect (OSTI)

    Jurss, Jonah W.; Concepcion, Javier C.; Norris, Michael R.; Templeton, Joseph L.; Meyer, Thomas J.

    2010-04-08

    Single-electron activation of multielectron catalysis has been shown to be viable in catalytic water oxidation with stepwise proton-coupled electron transfer, leading to high-energy catalytic precursors. For the blue dimer, cis,cis-[(bpy)2(H2O)RuIIIORuIII(H2O)(bpy)2]4+, the first well-defined molecular catalyst for water oxidation, stepwise 4e-/4H+ oxidation occurs to give the reactive precursor [(O)RuVORuV(O)]4+. This key intermediate is kinetically inaccessible at an unmodified metal oxide surface, where the only available redox pathway is electron transfer. We report here a remarkable surface activation of indium-tin oxide (In2O3:Sn) electrodes toward catalytic water oxidation by the blue dimer at electrodes derivatized by surface phosphonate binding of [Ru(4,4'-((HO)2P(O)CH2)2bpy)2(bpy)]2+. Surface binding dramatically improves the rate of surface oxidation of the blue dimer and induces water oxidation catalysis.

  20. Monodisperse Platinum and Rhodium Nanoparticles as Model Heterogeneous Catalysts

    SciTech Connect (OSTI)

    Coble, Inger M

    2008-08-15

    Model heterogeneous catalysts have been synthesized and studied to better understand how the surface structure of noble metal nanoparticles affects catalytic performance. In this project, monodisperse rhodium and platinum nanoparticles of controlled size and shape have been synthesized by solution phase polyol reduction, stabilized by polyvinylpyrrolidone (PVP). Model catalysts have been developed using these nanoparticles by two methods: synthesis of mesoporous silica (SBA-15) in the presence of nanoparticles (nanoparticle encapsulation, NE) to form a composite of metal nanoparticles supported on SBA-15 and by deposition of the particles onto a silicon wafer using Langmuir-Blodgett (LB) monolayer deposition. The particle shapes were analyzed by transmission electron microscopy (TEM) and high resolution TEM (HRTEM) and the sizes were determined by TEM, X-ray diffraction (XRD), and in the case of NE samples, room temperature H2 and CO adsorption isotherms. Catalytic studies were carried out in homebuilt gas-phase reactors. For the nanoparticles supported on SBA-15, the catalysts are in powder form and were studied using the homebuilt systems as plug-flow reactors. In the case of nanoparticles deposited on silicon wafers, the same systems were operated as batch reactors. This dissertation has focused on the synthesis, characterization, and reaction studies of model noble metal heterogeneous catalysts. Careful control of particle size and shape has been accomplished though solution phase synthesis of Pt and Rh nanoparticles in order to elucidate further structure-reactivity relationships in noble metal catalysis.

  1. Characterization of the homogeneous tissue mixture approximation in breast imaging dosimetry

    SciTech Connect (OSTI)

    Sechopoulos, Ioannis; Bliznakova, Kristina; Qin Xulei; Fei Baowei; Feng, Steve Si Jia

    2012-08-15

    Purpose: To compare the estimate of normalized glandular dose in mammography and breast CT imaging obtained using the actual glandular tissue distribution in the breast to that obtained using the homogeneous tissue mixture approximation. Methods: Twenty volumetric images of patient breasts were acquired with a dedicated breast CT prototype system and the voxels in the breast CT images were automatically classified into skin, adipose, and glandular tissue. The breasts in the classified images underwent simulated mechanical compression to mimic the conditions present during mammographic acquisition. The compressed thickness for each breast was set to that achieved during each patient's last screening cranio-caudal (CC) acquisition. The volumetric glandular density of each breast was computed using both the compressed and uncompressed classified images, and additional images were created in which all voxels representing adipose and glandular tissue were replaced by a homogeneous mixture of these two tissues in a proportion corresponding to each breast's volumetric glandular density. All four breast images (compressed and uncompressed; heterogeneous and homogeneous tissue) were input into Monte Carlo simulations to estimate the normalized glandular dose during mammography (compressed breasts) and dedicated breast CT (uncompressed breasts). For the mammography simulations the x-ray spectra used was that used during each patient's last screening CC acquisition. For the breast CT simulations, two x-ray spectra were used, corresponding to the x-ray spectra with the lowest and highest energies currently being used in dedicated breast CT prototype systems under clinical investigation. The resulting normalized glandular dose for the heterogeneous and homogeneous versions of each breast for each modality was compared. Results: For mammography, the normalized glandular dose based on the homogeneous tissue approximation was, on average, 27% higher than that estimated using the true heterogeneous glandular tissue distribution (Wilcoxon Signed Rank Test p= 0.00046). For dedicated breast CT, the overestimation of normalized glandular dose was, on average, 8% (49 kVp spectrum, p= 0.00045) and 4% (80 kVp spectrum, p= 0.000089). Only two cases in mammography and two cases in dedicated breast CT with a tube voltage of 49 kVp resulted in lower dose estimates for the homogeneous tissue approximation compared to the heterogeneous tissue distribution. Conclusions: The normalized glandular dose based on the homogeneous tissue mixture approximation results in a significant overestimation of dose to the imaged breast. This overestimation impacts the use of dose estimates in absolute terms, such as for risk estimates, and may impact some comparative studies, such as when modalities or techniques with different x-ray energies are used. The error introduced by the homogeneous tissue mixture approximation in higher energy x-ray modalities, such as dedicated breast CT, although statistically significant, may not be of clinical concern. Further work is required to better characterize this overestimation and potentially develop new metrics or correction factors to better estimate the true glandular dose to breasts undergoing imaging with ionizing radiation.

  2. Low temperature, sulfur tolerant homogeneous catalysts for the water-gas shift reaction. Task 1, Topical report No. 1

    SciTech Connect (OSTI)

    Laine, R.M.

    1986-01-20

    The purpose of this report is to update and reorganize our recent review on homogeneous catalysis of the water-gas shift reaction (WGSR) based on recent literature publications and patents. This updated version will serve as a means of selecting 10 candidate catalyst systems for use in developing effective, sulfur-tolerant, low temperature WGSR catalysts. This report discusses the variations possible in the basic chemistry associated with WGSR catalytic cycles, including basic, acidic, and neutral conditions. Then individual mechanism for specific WGSR catalyst systems are discussed. Finally, on the basis of the literature reports, a list is presented of candidate catalysts and basic systems we have chosen for study in Task 3.

  3. Conceptual design of a new homogeneous reactor for medical radioisotope Mo-99/Tc-99m production

    SciTech Connect (OSTI)

    Liem, Peng Hong [Nippon Advanced Information Service (NAIS Co., Inc.) Scientific Computational Division, 416 Muramatsu, Tokaimura, Ibaraki (Japan); Tran, Hoai Nam [Chalmers University of Technology, Dept. of Applied Physics, Div. of Nuclear Engineering, SE-412 96 Gothenburg (Sweden); Sembiring, Tagor Malem [National Nuclear Energy Agency (BATAN), Center for Reactor Technology and Nuclear Safety, Kawasan Puspiptek, Serpong, Tangerang Selatan, Banten (Indonesia); Arbie, Bakri [PT MOTAB Technology, Kedoya Elok Plaza Blok DA 12, Jl. Panjang, Kebun Jeruk, Jakarta Barat (Indonesia)

    2014-09-30

    To partly solve the global and regional shortages of Mo-99 supply, a conceptual design of a nitrate-fuel-solution based homogeneous reactor dedicated for Mo-99/Tc-99m medical radioisotope production is proposed. The modified LEU Cintichem process for Mo-99 extraction which has been licensed and demonstrated commercially for decades by BATAN is taken into account as a key design consideration. The design characteristics and main parameters are identified and the advantageous aspects are shown by comparing with the BATAN's existing Mo-99 supply chain which uses a heterogeneous reactor (RSG GAS multipurpose reactor)

  4. Microgrids and Heterogeneous Security, Quality, Reliability, andAvailability

    SciTech Connect (OSTI)

    Marnay, Chris

    2007-01-31

    This paper describes two stylized alternative visions inpopular currencyof how the power system might evolve to meet futurerequirements for the high quality electricity service that modern digitaleconomies demand, a supergrids paradigm and a dispersed paradigm. Some ofthe economics of the dispersed vision are explored. Economic perspectivesare presented on both the choice of homogeneous universal power qualityupstream in the electricity supply, and also on the extremelyheterogeneous require-ments of end-use loads. Finally, the potential roleof microgrids in delivering heterogeneous power quality is demonstratedby reference to two ongoing microgrid tests in the U.S. andJapan.

  5. Fundamental Studies in Catalysis Enabled the use of Efficient Lean-Burn Engines for Vehicle Transportation

    Broader source: Energy.gov [DOE]

    Building on a catalysis research program sponsored by EEREs Vehicles Technology Office (VTO) and DOEs Office of Science, researchers at Cummins, Inc. and Pacific Northwest National Laboratory ...

  6. Improving Catalysis by Putting the Best Face Forward | U.S. DOE Office of

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

    Science (SC) Improving Catalysis by Putting the Best Face Forward Basic Energy Sciences (BES) BES Home About Research Facilities Science Highlights Benefits of BES Funding Opportunities Basic Energy Sciences Advisory Committee (BESAC) Community Resources Contact Information Basic Energy Sciences U.S. Department of Energy SC-22/Germantown Building 1000 Independence Ave., SW Washington, DC 20585 P: (301) 903-3081 F: (301) 903-6594 E: Email Us More Information » 04.01.12 Improving Catalysis by

  7. Density Functional Theory in Surface Chemistry and Catalysis

    SciTech Connect (OSTI)

    Norskov, Jens

    2011-05-19

    Recent advances in the understanding of reactivity trends for chemistry at transition metal surfaces have enabled in silico design of heterogeneous catalysts in a few cases. Current status of the field is discussed with an emphasis on the role of coupling between theory and experiment and future challenges.

  8. Studies of Immobilized Homogeneous Metal Catalysts on Silica Supports

    SciTech Connect (OSTI)

    Keith James Stanger

    2003-05-31

    The tethered, chiral, chelating diphosphine rhodium complex, which catalyzes the enantioselective hydrogenation of methyl-{alpha}-acetamidocinnamate (MAC), has the illustrated structure as established by {sup 31}P NMR and IR studies. Spectral and catalytic investigations also suggest that the mechanism of action of the tethered complex is the same as that of the untethered complex in solution. The rhodium complexes, [Rh(COD)H]{sub 4}, [Rh(COD){sub 2}]{sup +}BF{sub 4}{sup -}, [Rh(COD)Cl]{sub 2}, and RhCl{sub 3} {center_dot} 3H{sub 2}O, adsorbed on SiO{sub 2} are optimally activated for toluene hydrogenation by pretreatment with H{sub 2} at 200 C. The same complexes on Pd-SiO{sub 2} are equally active without pretreatments. The active species in all cases is rhodium metal. The catalysts were characterized by XPS, TEM, DRIFTS, and mercury poisoning experiments. Rhodium on silica catalyzes the hydrogenation of fluorobenzene to produce predominantly fluorocyclohexane in heptane and 1,2-dichloroethane solvents. In heptane/methanol and heptane/water solvents, hydrodefluorination to benzene and subsequent hydrogenation to cyclohexane occurs exclusively. Benzene inhibits the hydrodefluorination of fluorobenzene. In DCE or heptane solvents, fluorocyclohexane reacts with hydrogen fluoride to form cyclohexene. Reaction conditions can be chosen to selectively yield fluorocyclohexane, cyclohexene, benzene, or cyclohexane. The oxorhenium(V) dithiolate catalyst [-S(CH{sub 2}){sub 3}s-]Re(O)(Me)(PPh{sub 3}) was modified by linking it to a tether that could be attached to a silica support. Spectroscopic investigation and catalytic oxidation reactivity showed the heterogenized catalyst's structure and reactivity to be similar to its homogeneous analog. However, the immobilized catalyst offered additional advantages of recyclability, extended stability, and increased resistance to deactivation.

  9. Soliton production with nonlinear homogeneous lines

    SciTech Connect (OSTI)

    Elizondo-Decanini, Juan M.; Coleman, Phillip D.; Moorman, Matthew W.; Petney, Sharon Joy Victor; Dudley, Evan C.; Youngman, Kevin; Penner, Tim Dwight; Fang, Lu; Myers, Katherine M.

    2015-11-24

    Low- and high-voltage Soliton waves were produced and used to demonstrate collision and compression using diode-based nonlinear transmission lines. Experiments demonstrate soliton addition and compression using homogeneous nonlinear lines. We built the nonlinear lines using commercially available diodes. These diodes are chosen after their capacitance versus voltage dependence is used in a model and the line design characteristics are calculated and simulated. Nonlinear ceramic capacitors are then used to demonstrate high-voltage pulse amplification and compression. The line is designed such that a simple capacitor discharge, input signal, develops soliton trains in as few as 12 stages. We also demonstrated output voltages in excess of 40 kV using Y5V-based commercial capacitors. The results show some key features that determine efficient production of trains of solitons in the kilovolt range.

  10. Homogeneous catalyst formulations for methanol production

    DOE Patents [OSTI]

    Mahajan, Devinder; Sapienza, Richard S.; Slegeir, William A.; O'Hare, Thomas E.

    1990-01-01

    There is disclosed synthesis of CH.sub.3 OH from carbon monoxide and hydrogen using an extremely active homogeneous catalyst for methanol synthesis directly from synthesis gas. The catalyst operates preferably between 100.degree.-150.degree. C. and preferably at 100-150 psia synthesis gas to produce methanol. Use can be made of syngas mixtures which contain considerable quantities of other gases, such as nitrogen, methane or excess hydrogen. The catalyst is composed of two components: (a) a transition metal carbonyl complex and (b) an alkoxide component. In the simplest formulation, component (a) is a complex of nickel tetracarbonyl and component (b) is methoxide (CH.sub.3 O.sup.13 ), both being dissolved in a methanol solvent system. The presence of a co-solvent such as p-dioxane, THF, polyalcohols, ethers, hydrocarbons, and crown ethers accelerates the methanol synthesis reaction.

  11. Homogeneous catalyst formulations for methanol production

    DOE Patents [OSTI]

    Mahajan, Devinder; Sapienza, Richard S.; Slegeir, William A.; O'Hare, Thomas E.

    1991-02-12

    There is disclosed synthesis of CH.sub.3 OH from carbon monoxide and hydrogen using an extremely active homogeneous catalyst for methanol synthesis directly from synthesis gas. The catalyst operates preferably between 100.degree.-150.degree. C. and preferably at 100-150 psia synthesis gas to produce methanol. Use can be made of syngas mixtures which contain considerable quantities of other gases, such as nitrogen, methane or excess hydrogen. The catalyst is composed of two components: (a) a transition metal carbonyl complex and (b) an alkoxide component. In the simplest formulation, component (a) is a complex of nickel tetracarbonyl and component (b) is methoxide (CH.sub.3 O.sup.-), both being dissolved in a methanol solvent system. The presence of a co-solvent such as p-dioxane, THF, polyalcohols, ethers, hydrocarbons, and crown ethers accelerates the methanol synthesis reaction.

  12. Soliton production with nonlinear homogeneous lines

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

    Elizondo-Decanini, Juan M.; Coleman, Phillip D.; Moorman, Matthew W.; Petney, Sharon Joy Victor; Dudley, Evan C.; Youngman, Kevin; Penner, Tim Dwight; Fang, Lu; Myers, Katherine M.

    2015-11-24

    Low- and high-voltage Soliton waves were produced and used to demonstrate collision and compression using diode-based nonlinear transmission lines. Experiments demonstrate soliton addition and compression using homogeneous nonlinear lines. We built the nonlinear lines using commercially available diodes. These diodes are chosen after their capacitance versus voltage dependence is used in a model and the line design characteristics are calculated and simulated. Nonlinear ceramic capacitors are then used to demonstrate high-voltage pulse amplification and compression. The line is designed such that a simple capacitor discharge, input signal, develops soliton trains in as few as 12 stages. We also demonstrated outputmore » voltages in excess of 40 kV using Y5V-based commercial capacitors. The results show some key features that determine efficient production of trains of solitons in the kilovolt range.« less

  13. Foam Generation in Homogeneous Porous Media

    SciTech Connect (OSTI)

    Gauglitz, Phillip A.; Friedman, F.; Kam, S. I.; Rossen, W. R.

    2002-10-01

    In steady gas-liquid flow in homogeneous porous media with surfactant present, there is often observed a critical injection velocity or pressure gradient ?grad p min? at which ?weak? or ?coarse? foam is abruptly converted into ?strong foam,? with reduction of one to two orders of magnitude in total mobility: i.e., ?foam generation.? Earlier research on foam generation is extended here with extensive data for a variety of porous media, permeabilities, gases (N2 and C02), surfactants, and temperatures. For bead and sandpacks, ?grad p min? scales like (1/k), where k is permeability, over 2 1/2 orders of magnitude in k; for consolidated media the relation is more complex. For dense C02 foam, ?grad p min? exists but can be less than 1 psi/ft. If pressure drop, rather than flow rates, is fixed, one observes and unstable regime between stable ?strong? and ?coarse? foam regimes; in the unstable regime ?grad p? is nonuniform in space or variable in time.

  14. Homogeneously dispersed, multimetal oxygen-evolving catalysts

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

    Zhang, Bo; Zheng, Xueli; Voznyy, Oleksandr; Comin, Riccardo; Bajdich, Michal; Garcia-Melchor, Max; Han, Lili; Xu, Jixian; Liu, Min; Zheng, Lirong; et al

    2016-03-24

    Earth-abundant first-row (3d) transition-metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials significantly above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing near-optimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxy-hydroxide materials with an atomically homogeneous metal distribution. These gelled FeCoW oxy-hydroxide exhibits the lowest overpotential (191 mV) reported at 10 mA per square centimeter in alkaline electrolyte. Here, the catalyst shows no evidence of degradation following more than 500 hours of operation. X-ray absorption and computationalmore » studies reveal a synergistic interplay between W, Fe and Co in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER.« less

  15. A New Equivalence Theory Method for Treating Doubly Heterogeneous Fuel - I. Theory

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

    Williams, Mark L.; Lee, Deokjung; Choi, Sooyoung

    2015-03-04

    A new methodology has been developed to treat resonance self-shielding in doubly heterogeneous very high temperature gas-cooled reactor systems in which the fuel compact region of a reactor lattice consists of small fuel grains dispersed in a graphite matrix. This new method first homogenizes the fuel grain and matrix materials using an analytically derived disadvantage factor from a two-region problem with equivalence theory and intermediate resonance method. This disadvantage factor accounts for spatial self-shielding effects inside each grain within the framework of an infinite array of grains. Then the homogenized fuel compact is self-shielded using a Bondarenko method to accountmore » for interactions between the fuel compact regions in the fuel lattice. In the final form of the equations for actual implementations, the double-heterogeneity effects are accounted for by simply using a modified definition of a background cross section, which includes geometry parameters and cross sections for both the grain and fuel compact regions. With the new method, the doubly heterogeneous resonance self-shielding effect can be treated easily even with legacy codes programmed only for a singly heterogeneous system by simple modifications in the background cross section for resonance integral interpolations. This paper presents a detailed derivation of the new method and a sensitivity study of double-heterogeneity parameters introduced during the derivation. The implementation of the method and verification results for various test cases are presented in the companion paper.« less

  16. A New Equivalence Theory Method for Treating Doubly Heterogeneous Fuel - I. Theory

    SciTech Connect (OSTI)

    Williams, Mark L.; Lee, Deokjung; Choi, Sooyoung

    2015-03-04

    A new methodology has been developed to treat resonance self-shielding in doubly heterogeneous very high temperature gas-cooled reactor systems in which the fuel compact region of a reactor lattice consists of small fuel grains dispersed in a graphite matrix. This new method first homogenizes the fuel grain and matrix materials using an analytically derived disadvantage factor from a two-region problem with equivalence theory and intermediate resonance method. This disadvantage factor accounts for spatial self-shielding effects inside each grain within the framework of an infinite array of grains. Then the homogenized fuel compact is self-shielded using a Bondarenko method to account for interactions between the fuel compact regions in the fuel lattice. In the final form of the equations for actual implementations, the double-heterogeneity effects are accounted for by simply using a modified definition of a background cross section, which includes geometry parameters and cross sections for both the grain and fuel compact regions. With the new method, the doubly heterogeneous resonance self-shielding effect can be treated easily even with legacy codes programmed only for a singly heterogeneous system by simple modifications in the background cross section for resonance integral interpolations. This paper presents a detailed derivation of the new method and a sensitivity study of double-heterogeneity parameters introduced during the derivation. The implementation of the method and verification results for various test cases are presented in the companion paper.

  17. Structural Insights into the Mechanism of PEPCK Catalysis

    SciTech Connect (OSTI)

    Holyoak,T.; Sullivan, S.; Nowak, T.

    2006-01-01

    Phosphoenolpyruvate carboxykinase catalyzes the reversible decarboxylation of oxaloacetic acid with the concomitant transfer of the {gamma}-phosphate of GTP to form PEP and GDP as the first committed step of gluconeogenesis and glyceroneogenesis. The three structures of the mitochondrial isoform of PEPCK reported are complexed with Mn{sup 2+}, Mn{sup 2+}-PEP, or Mn{sup 2+}-malonate-Mn{sup 2+}GDP and provide the first observations of the structure of the mitochondrial isoform and insight into the mechanism of catalysis mediated by this enzyme. The structures show the involvement of the hyper-reactive cysteine (C307) in the coordination of the active site Mn{sup 2+}. Upon formation of the PEPCK-Mn{sup 2+}-PEP or PEPCK-Mn{sup 2+}-malonate-Mn{sup 2+}GDP complexes, C307 coordination is lost as the P-loop in which it resides adopts a different conformation. The structures suggest that stabilization of the cysteine-coordinated metal geometry holds the enzyme as a catalytically incompetent metal complex and may represent a previously unappreciated mechanism of regulation. A third conformation of the mobile P-loop in the PEPCK-Mn{sup 2+}-malonate-Mn{sup 2+}GDP complex demonstrates the participation of a previously unrecognized, conserved serine residue (S305) in mediating phosphoryl transfer. The ordering of the mobile active site lid in the PEPCK-Mn{sup 2+}-malonate-Mn{sup 2+}GDP complex yields the first observation of this structural feature and provides additional insight into the mechanism of phosphoryl transfer.

  18. Shape-selective catalysis in dimethyl ether conversion

    SciTech Connect (OSTI)

    Sardesai, A.; Lee, S.

    1999-07-01

    Coal-derived syngas can be effectively converted to dimethyl ether (DME) in a single-stage, liquid-phase process. This Liquid Phase Dimethyl Ether (LPDME) process utilizes a dual catalytic system, which comprises of a physical blend between the methanol synthesis and the methanol dehydration catalyst slurried in an inert mineral oil. Such produced DME has vast potential as a building block chemical in the petrochemical industry to produce value-added specialty chemicals. The current research efforts are made to exploit the utilization of shape-selective catalysis using zeolites to produce targeted petrochemicals, including lower olefinic hydrocarbons. The catalysts probed in this investigation include zeolites of different physical, morphological, and chemical configurations. The effect of acidity of ZSM-5 type zeolites as well as the effect of the different channel size and orientation of the zeolites on product selectivity and catalyst deactivation are examined. Results obtained from experimentation of this study show that ZSM-5 type zeolite with low acidity (high SiO{sub 2}/Al{sub 2}O{sub 3} ratio, in this case 150) exhibits the highest selectivity towards lower (C{sub 2}-C{sub 4}) olefins in general. Controlled selectivity toward targeted olefinic species can be accomplished via devising catalytic reaction systems in such a way that the structural property of the catalyst and reactive interaction between molecules in the pores are geared toward formation of targeted molecular species which also at the same time prevent the formation of less desirable products. The internal morphology of the catalyst also has a pronounced effect on the deactivation phenomenon, where it is observed that zeolites possessing high acidity and a unidimensional channel structure are prone towards catalyst deactivation by coking and pore blockage.

  19. Assessment of Homogeneous Thorium/Uranium Fuel for Pressurized Water

    Office of Scientific and Technical Information (OSTI)

    Reactors (Journal Article) | SciTech Connect Assessment of Homogeneous Thorium/Uranium Fuel for Pressurized Water Reactors Citation Details In-Document Search Title: Assessment of Homogeneous Thorium/Uranium Fuel for Pressurized Water Reactors The homogeneous ThO{sub 2}-UO{sub 2} fuel cycle option for a pressurized water reactor (PWR) of current technology is investigated. The fuel cycle assessment was carried out by calculating the main performance parameters: natural uranium and separative

  20. Organusulfur Catalysis With Reduced Molybdenum Sulfides Containing the Mo6S8 Cluster

    SciTech Connect (OSTI)

    Thomas Jay Paskach

    2002-08-27

    Industrial synthesis of sulfur-containing organic chemicals basically focuses on the broad categories of mercaptans (thiols), alkylsulfides (thioethers), polysulfides, and thiophenes. Of the organo-sulfur compounds produced, by far the most important in terms of quantities produced is methyl mercaptan (methanethiol or MeSH), which is produced mainly for the downstream production of methionine and methanesulfonyl chloride. Higher thiols are also used in the manufacture of rubber and plastics as polymerization regulators, chain transfer agents, or initiators. Other important organosulfur chemicals are dimethyl sulfide (DMS) and dimethyl disulfide (DMDS), both of which are used extensively for presulfiding of industrial hydroprocessing catalysts, and substituted thiophenes which are used as intermediates for production of agrochemicals, dyes, and pharmaceuticals. Thiols are produced commercially at the rate of about 10{sup 4} ton/yr from hydrogen sulfide (H{sub 2}S) and alcohols or olefins, using homogeneous free-radical synthesis, or heterogeneous catalysts based on solid acids or supported metal oxides and/or sulfides. Despite this large production rate, and the industrial importance of the organosulfur compounds, only limited research has been devoted to the development of new catalytic materials for their synthesis. Additionally, for most organosulfur catalytic reactions, only limited information exists about reaction mechanisms, active sites, adsorbed surface species, and especially the nature of the catalysts under reaction conditions.

  1. Molecular-level Design of Heterogeneous Chiral Catalysts

    SciTech Connect (OSTI)

    Gellman, Andrew John; Sholl, David S.; Tysoe, Wilfred T.; Zaera, Francisco

    2013-04-28

    Understanding and controlling selectivity is one of the key challenges in heterogeneous catalysis. Among problems in catalytic selectivity enantioselectivity is perhaps the most the most challenging. The primary goal of the project on Molecular-level Design of Heterogeneous Chiral Catalysts is to understand the origins of enantioselectivity on chiral heterogeneous surfaces and catalysts. The efforts of the project team include preparation of chiral surfaces, characterization of chiral surfaces, experimental detection of enantioselectivity on such surfaces and computational modeling of the interactions of chiral probe molecules with chiral surfaces. Over the course of the project period the team of PIs has made some of the most detailed and insightful studies of enantioselective chemistry on chiral surfaces. This includes the measurement of fundamental interactions and reaction mechanisms of chiral molecules on chiral surfaces and leads all the way to rationale design and synthesis of chiral surfaces and materials for enantioselective surface chemistry. The PIs have designed and prepared new materials for enantioselective adsorption and catalysis. Naturally Chiral Surfaces Completion of a systematic study of the enantiospecific desorption kinetics of R-3-methylcyclohexanone (R-3-MCHO) on 9 achiral and 7 enantiomeric pairs of chiral Cu surfaces with orientations that span the stereographic triangle. Discovery of super-enantioselective tartaric acid (TA) and aspartic acid (Asp) decomposition as a result of a surface explosion mechanism on Cu(643)R&S. Systematic study of super-enantiospecific TA and Asp decomposition on five enantiomeric pairs of chiral Cu surfaces. Initial observation of the enantiospecific desorption of R- and S-propylene oxide (PO) from Cu(100) imprinted with {3,1,17} facets by L-lysine adsorption. Templated Chiral Surfaces Initial observation of the enantiospecific desorption of R- and S-PO from Pt(111) and Pd(111) modified by a variety of chiral templates. Demonstrated enantioselective separation of racemic PO on chemically synthesized chiral gold nanoparticles. Discovery of zwitterionic adsorption states of amino acids on Pd(111). First structure determinations of adsorbed amino acids and identification of tetrameric chiral template structures. Exploration of the enantiospecific interaction of PO and R-3-MCHO adsorption on chirally modified Cu(100), Cu(110) and Cu(111). One-to-One Interactions Determination of cinchona orientation on Pt surfaces in situ at the solid-liquid interface using FT-IRAS. Systematic study of the influence of solution properties on the adsorption of modified cinchonas alkaloids onto Pt surfaces. Correlation of cinchona adsorption with catalytic activity, as affected by concentration, the nature of the solvent, and dissolved gases in the liquid phase. Measurement of enantioselective chemisorption on 1-(1-naphthyl) ethylamine (NEA) modified Pt(111) and Pd(111) surfaces. Imaging of chiral docking complexes between NEA and methyl pyruvate on Pd(111). Chiral Catalyst Synthesis Anchoring of cinchona alkaloid to surfaces Synthesis of chiral Au nanoparticles and demonstration of their enantiospecific interactions with R- and S-PO. Elucidation of the driving forces for chiral imprinting of Cu(100) by L- and D-lysine to form Cu(3,1,17)R&S facets.

  2. 2010 CATALYSIS GORDON RESEARCH CONFERENCE, JUNE 27 - JULY 2, 2010, NEW LONDON, NEW HAMPSHIRE

    SciTech Connect (OSTI)

    Abhaya Datye

    2010-07-02

    Catalysis is a key technology for improving the quality of life while simultaneously reducing the adverse impact of human activities on the environment. The discovery of new catalytic processes and the improvement of existing ones are also critically important for securing the nation's energy supply. The GRC on Catalysis is considered one the most prestigious conference for catalysis research, bringing together leading researchers from both academia, industry and national labs to discuss the latest, most exciting research in catalysis and the future directions for the field. The 2010 GRC on Catalysis will follow time-honored traditions and feature invited talks from the world's leading experts in the fundamentals and applications of catalytic science and technology. We plan to have increased participation from industry. The extended discussions in the company of outstanding thinkers will stimulate and foster new science. The conference will include talks in the following areas: Alternative feedstocks for chemicals and fuels, Imaging and spectroscopy, Design of novel catalysts, Catalyst preparation fundamentals, Molecular insights through theory, Surface Science, Catalyst stability and dynamics. In 2010, the Catalysis conference will move to a larger conference room with a new poster session area that will allow 40 posters per session. The dorm rooms provide single and double accommodations, free WiFi and the registration fee includes all meals and the famous lobster dinner on Thursday night. Afternoons are open to enjoy the New England ambiance with opportunities for hiking, sailing, golf and tennis to create an outstanding conference that will help you network with colleagues, and make long lasting connections.

  3. Geek-Up[3.11.2011]: Energy Efficiency, Catalysis and Open Source Tools |

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

    Department of Energy 11.2011]: Energy Efficiency, Catalysis and Open Source Tools Geek-Up[3.11.2011]: Energy Efficiency, Catalysis and Open Source Tools March 11, 2011 - 4:37pm Addthis L. Keith Woo | Photo courtesy of Ames National Laboratory L. Keith Woo | Photo courtesy of Ames National Laboratory Niketa Kumar Niketa Kumar Public Affairs Specialist, Office of Public Affairs Ames Laboratory researcher and Iowa State University professor L. Keith Woo is on the search for catalysts that lead

  4. Growth mechanism of graphene on platinum: Surface catalysis and carbon segregation

    SciTech Connect (OSTI)

    Sun, Jie Lindvall, Niclas; Yurgens, August; Nam, Youngwoo; Cole, Matthew T.; Teo, Kenneth B. K.; Woo Park, Yung

    2014-04-14

    A model of the graphene growth mechanism of chemical vapor deposition on platinum is proposed and verified by experiments. Surface catalysis and carbon segregation occur, respectively, at high and low temperatures in the process, representing the so-called balance and segregation regimes. Catalysis leads to self-limiting formation of large area monolayer graphene, whereas segregation results in multilayers, which evidently grow from below. By controlling kinetic factors, dominantly monolayer graphene whose high quality has been confirmed by quantum Hall measurement can be deposited on platinum with hydrogen-rich environment, quench cooling, tiny but continuous methane flow and about 1000?C growth temperature.

  5. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ... catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy ...

  6. Th/U-233 multi-recycle in pressurized water reactors : feasibility study of multiple homogeneous and heterogeneous assembly designs.

    SciTech Connect (OSTI)

    Yun, D.; Taiwo, T. A.; Kim, T. K.; Mohamed, A.; Nuclear Engineering Division

    2010-10-01

    The use of thorium in current or advanced light water reactors (LWRs) has been of interest in recent years. These interests have been associated with the need to increase nuclear fuel resources and the perceived non-proliferation advantages of the utilization of thorium in the fuel cycle. Various options have been considered for the use of thorium in the LWR fuel cycle. The possibility for thorium utilization in a multi-recycle system has also been considered in past literature, primarily because of the potential for near breeders with Th/U-233 in the thermal energy range. The objective of this study is to evaluate the potential of Th/U-233 fuel multi-recycle in current LWRs, focusing on pressurized water reactors (PWRs). Approaches for sustainable multi-recycle without the need for external fissile material makeup have been investigated. The intent is to obtain a design that allows existing PWRs to be used with minimal modifications.

  7. Solvation and Acid Strength Effects on Catalysis by Faujasite Zeolites

    SciTech Connect (OSTI)

    Gounder, Rajamani P.; Jones, Andrew J.; Carr, Robert T.; Iglesia, Enrique

    2012-02-01

    Kinetic, spectroscopic, and chemical titration data indicate that differences in monomolecular isobutane cracking and dehydrogenation and methanol dehydration turnover rates (per H+) among FAU zeolites treated thermally with steam (H-USY) and then chemically with ammonium hexafluorosilicate (CDHUSY) predominantly reflect differences in the size and solvating properties of their supercage voids rather than differences in acid strength. The number of protons on a given sample was measured consistently by titrations with Na+, with CH3 groups via reactions of dimethyl ether, and with 2,6-di-tert-butylpyridine during methanol dehydration catalysis; these titration values were also supported by commensurate changes in acidic OH infrared band areas upon exposure to titrant molecules. The number of protons, taken as the average of the three titration methods, was significantly smaller than the number of framework Al atoms (Alf) obtained from X-ray diffraction and 27Al magic angle spinning nuclear magnetic resonance spectroscopy on H-USY (0.35 H+/Alf) and CD-HUSY (0.69 H+/Alf). These data demonstrate that the ubiquitous use of Alf sites as structural proxies for active H+ sites in zeolites can be imprecise, apparently because distorted Al structures that are not associated with acidic protons are sometimes detected as Alf sites. Monomolecular isobutane cracking and dehydrogenation rate constants, normalized non-rigorously by the number of Alf species, decreased with increasing Na+ content on both H-USY and CD-HUSY samples and became undetectable at sub-stoichiometric exchange levels (0.32 and 0.72 Na+/Alf ratios, respectively), an unexpected finding attributed incorrectly in previous studies to the presence of minority ‘‘super-acidic’’ sites. These rate constants, when normalized rigorously by the number of residual H+ sites were independent of Na+ content on both H-USY and CD-HUSY samples, reflecting the stoichiometric replacement of protons that are uniform in reactivity by Na+ cations. Monomolecular isobutane cracking and dehydrogenation rate constants (per H+; 763 K), however, were higher on H-USY than CD-HUSY (by a factor of 1.4). Equilibrium constants for the formation of protonated methanol dimers via adsorption of gaseous methanol onto adsorbed methanol monomers, determined from kinetic studies of methanol dehydration to dimethyl ether (433 K), were also higher on H-USY than CD-HUSY (by a factor of 2.1). These larger constants predominantly reflect stronger dispersive interactions in H-USY, consistent with its smaller supercage voids that result from the occlusion of void space by extraframework Al (Alex) residues. These findings appear to clarify enduring controversies about the mechanistic interpretation of the effects of Na+ and Alex species on the catalytic reactivity of FAU zeolites. They also illustrate the need to normalize rates by the number of active sites instead of more convenient but less accurate structural proxies for such sites.

  8. At tank Low Activity Feed Homogeneity Analysis Verification

    SciTech Connect (OSTI)

    DOUGLAS, J.G.

    2000-09-28

    This report evaluates the merit of selecting sodium, aluminum, and cesium-137 as analytes to indicate homogeneity of soluble species in low-activity waste (LAW) feed and recommends possible analytes and physical properties that could serve as rapid screening indicators for LAW feed homogeneity. The three analytes are adequate as screening indicators of soluble species homogeneity for tank waste when a mixing pump is used to thoroughly mix the waste in the waste feed staging tank and when all dissolved species are present at concentrations well below their solubility limits. If either of these conditions is violated, then the three indicators may not be sufficiently chemically representative of other waste constituents to reliably indicate homogeneity in the feed supernatant. Additional homogeneity indicators that should be considered are anions such as fluoride, sulfate, and phosphate, total organic carbon/total inorganic carbon, and total alpha to estimate the transuranic species. Physical property measurements such as gamma profiling, conductivity, specific gravity, and total suspended solids are recommended as possible at-tank methods for indicating homogeneity. Indicators of LAW feed homogeneity are needed to reduce the U.S. Department of Energy, Office of River Protection (ORP) Program's contractual risk by assuring that the waste feed is within the contractual composition and can be supplied to the waste treatment plant within the schedule requirements.

  9. Hydrogen storage materials and method of making by dry homogenation

    DOE Patents [OSTI]

    Jensen, Craig M.; Zidan, Ragaiy A.

    2002-01-01

    Dry homogenized metal hydrides, in particular aluminum hydride compounds, as a material for reversible hydrogen storage is provided. The reversible hydrogen storage material comprises a dry homogenized material having transition metal catalytic sites on a metal aluminum hydride compound, or mixtures of metal aluminum hydride compounds. A method of making such reversible hydrogen storage materials by dry doping is also provided and comprises the steps of dry homogenizing metal hydrides by mechanical mixing, such as be crushing or ball milling a powder, of a metal aluminum hydride with a transition metal catalyst. In another aspect of the invention, a method of powering a vehicle apparatus with the reversible hydrogen storage material is provided.

  10. Tritium Technology Program TTP-1-3089 TPBAR Homogenized Composition

    SciTech Connect (OSTI)

    Love, Edward F.

    2014-10-12

    Homogenized TPBAR number densities contained herein have been derived for unclassified core physics calculations. The use of this information may not provide accurate, conservative or representative results and must be evaluated for applicability to the specific problem.

  11. Distribution of Radiation Density in a Homogeneous Cloudy Laye

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

    of Radiation Density in a Homogeneous Cloudy Layer S. V. Dvoryashin, K. A. Shukorov, A. H. Shukurov, and G. S. Golitsyn A. M. Obukhov Institute of Atmospheric Physics Russian...

  12. Surface functionalization of metal-organic polyhedron for homogeneous...

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

    reactions with linear alkyl anhydrides lead to new MOPs with enhanced solubility. As a result, the surface-modified MOP 4 was demonstrated as a homogeneous Lewis-acid catalyst...

  13. Homogeneously dispersed, multimetal oxygen-evolving catalysts (Journal

    Office of Scientific and Technical Information (OSTI)

    Article) | SciTech Connect Homogeneously dispersed, multimetal oxygen-evolving catalysts Citation Details In-Document Search This content will become publicly available on March 24, 2017 Title: Homogeneously dispersed, multimetal oxygen-evolving catalysts Earth-abundant first-row (3d) transition-metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials significantly above thermodynamic requirements. Density functional theory

  14. Modelling long-distance seed dispersal in heterogeneous landscapes.

    SciTech Connect (OSTI)

    Levey, Douglas, J.; Tewlsbury, Joshua, J.; Bolker, Benjamin, M.

    2008-01-01

    1. Long-distance seed dispersal is difficult to measure, yet key to understanding plant population dynamics and community composition. 2. We used a spatially explicit model to predict the distribution of seeds dispersed long distances by birds into habitat patches of different shapes. All patches were the same type of habitat and size, but varied in shape. They occurred in eight experimental landscapes, each with five patches of four different shapes, 150 m apart in a matrix of mature forest. The model was parameterized with smallscale movement data collected from field observations of birds. In a previous study we validated the model by testing its predictions against observed patterns of seed dispersal in real landscapes with the same types and spatial configuration of patches as in the model. 3. Here we apply the model more broadly, examining how patch shape influences the probability of seed deposition by birds into patches, how dispersal kernels (distributions of dispersal distances) vary with patch shape and starting location, and how movement of seeds between patches is affected by patch shape. 4. The model predicts that patches with corridors or other narrow extensions receive higher numbers of seeds than patches without corridors or extensions. This pattern is explained by edgefollowing behaviour of birds. Dispersal distances are generally shorter in heterogeneous landscapes (containing patchy habitat) than in homogeneous landscapes, suggesting that patches divert the movement of seed dispersers, holding them long enough to increase the probability of seed defecation in the patches. Dispersal kernels for seeds in homogeneous landscapes were smooth, whereas those in heterogenous landscapes were irregular. In both cases, long-distance (> 150 m) dispersal was surprisingly common, usually comprising approximately 50% of all dispersal events. 5. Synthesis . Landscape heterogeneity has a large influence on patterns of long-distance seed dispersal. Our results suggest that long-distance dispersal events can be predicted using spatially explicit modelling to scale-up local movements, placing them in a landscape context. Similar techniques are commonly used by landscape ecologists to model other types of movement; they offer much promise to the study of seed dispersal.

  15. Imaging Heterogeneous Ion Transfer: Lithium Ion Quantification...

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

    October 24, 2014, Research Highlights Imaging Heterogeneous Ion Transfer: Lithium Ion Quantification using Mercury Amalgams as In Situ Electrochemical Probes in Nonaqueous Media ...

  16. Comprehensive Monitoring for Heterogeneous Geographically Distributed...

    Office of Scientific and Technical Information (OSTI)

    Comprehensive Monitoring for Heterogeneous Geographically Distributed Storage Citation ... Sponsoring Org: USDOE Office of Science (SC), High Energy Physics (HEP) (SC-25) Country of ...

  17. The effect of reservoir heterogeneity on gas production from hydrate accumulations in the permafrost

    SciTech Connect (OSTI)

    Reagan, M. T.; Kowalsky, M B.; Moridis, G. J.; Silpngarmlert, S.

    2010-05-01

    The quantity of hydrocarbon gases trapped in natural hydrate accumulations is enormous, leading to significant interest in the evaluation of their potential as an energy source. Large volumes of gas can be readily produced at high rates for long times from methane hydrate accumulations in the permafrost by means of depressurization-induced dissociation combined with conventional technologies and horizontal or vertical well configurations. Initial studies on the possibility of natural gas production from permafrost hydrates assumed homogeneity in intrinsic reservoir properties and in the initial condition of the hydrate-bearing layers (either due to the coarseness of the model or due to simplifications in the definition of the system). These results showed great promise for gas recovery from Class 1, 2, and 3 systems in the permafrost. This work examines the consequences of inevitable heterogeneity in intrinsic properties, such as in the porosity of the hydrate-bearing formation, or heterogeneity in the initial state of hydrate saturation. Heterogeneous configurations are generated through multiple methods: (1) through defining heterogeneous layers via existing well-log data, (2) through randomized initialization of reservoir properties and initial conditions, and (3) through the use of geostatistical methods to create heterogeneous fields that extrapolate from the limited data available from cores and well-log data. These extrapolations use available information and established geophysical methods to capture a range of deposit properties and hydrate configurations. The results show that some forms of heterogeneity, such as horizontal stratification, can assist in production of hydrate-derived gas. However, more heterogeneous structures can lead to complex physical behavior within the deposit and near the wellbore that may obstruct the flow of fluids to the well, necessitating revised production strategies. The need for fine discretization is crucial in all cases to capture dynamic behavior during production.

  18. This research was supported as part of the Catalysis Center for Energy Innovatio

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

    This research was supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Improving Efficiencies in Fuel, Chemical and Pharmaceutical Industries Repetitive branching, a novel and simple synthesis method, produces zeolite crystals with large-pore "highways" that improve transport and utilization of chemicals within the crystal This research was

  19. Low-Temperature Hydrocarbon/CO Oxidation Catalysis in Support of HCCI

    Broader source: Energy.gov (indexed) [DOE]

    Emission Control | Department of Energy Presentation given at the 2007 Diesel Engine-Efficiency & Emissions Research Conference (DEER 2007). 13-16 August, 2007, Detroit, Michigan. Sponsored by the U.S. Department of Energy's (DOE) Office of FreedomCAR and Vehicle Technologies (OFCVT). PDF icon deer07_rappe.pdf More Documents & Publications Low-Temperature Hydrocarbon/CO Oxidation Catalysis in Support of HCCI Emission Control Selectlive Catalytic Reducution of NOx wilth Diesel-Based

  20. Kokes Awards for the 22nd North American Catalysis Society Meeting, June 5-10, 2011

    SciTech Connect (OSTI)

    Fabio H. Ribeiro

    2011-06-05

    The biennial North American Catalysis Society (NACS) Meetings are the premiere conferences in the area of catalysis, surface science, and reaction engineering. The 22nd meeting will be held the week of June 5-10, 2011 in Detroit, Michigan. The objective of the Meetings is to bring together leading researchers for intensive scientific exchange and interactions. Financial support that offsets some of the associated costs (specifically, registration fee, airline tickets, and hotel accommodations) would encourage graduate students, and for the first time undergraduate students, to attend and participate meaningfully in this conference. The funds sought in this proposal will help support the Richard J. Kokes Travel Award program. Graduate students eligible for these merit-based Awards are those who study at a North American university and who will present at the Meeting. We have currently 209 applications and we expect to be able to fund about half of them. The NACS has traditionally sought to encourage graduate student, and this year for the first time undergraduate studies, participation at the National Meetings and providing financial support is the most effective means to do so. Their attendance would contribute significantly to their scientific training and communication and presentation skills. They would be exposed to the leading researchers from the US and abroad; they would meet their peers from other universities; they would learn about cutting-edge results that could benefit their research projects; and they may become interested in becoming active participants in the catalysis community. These young investigators represent the next generation of scientists and engineers, and their proper training will lead to future scientific breakthroughs and technological innovations that benefit the US economy. Advances in catalysis can come in the form of more energy-efficient and environmentally-friendly chemical processes, improved fuel cell performance, efficient hydrogen production, and a cleaner environment.

  1. Kokes Awards for the 23rd North American Catalysis Society Meeting

    SciTech Connect (OSTI)

    Jacobs, Gary

    2014-01-31

    The Tri-State Catalysis Society awarded 107 Kokes Travel Awards. The program was very successful and to date this was the most Kokes Travel Awards ever awarded at a North American Catalysis Society Meeting. It provided students who merited an award the opportunity to attend the meeting, present a paper in the form of either an oral presentation or a poster presentation, and to serve the North American Catalysis Society by participating in the organization of the meeting. Students worked very hard during the week of the meeting to make it a success. Financial support for the Kokes awards was provided by DOE, NSF, NACS, as well as the Tri-State Catalysis Society, the latter through fund raising activities, and other donations. AT the meeting, each student received over $1050 in kind to offset the costs of registration fees ($260), hotel accommodations ($295.7), transportation ($400 travel allowance), as well as T-shirts ($20), and banquet tickets ($95 provided by donations from society members). In addition, for the first time, students received certificates that were signed by the President of NACS, Professor Enrique Iglesia, and by the Kokes Awards Chair, Gary Jacobs (see last page). A list of meeting co-chairs (i.e., Uschi M. Graham, Umit S. Ozkan, and Madan Bhassin) and the honorary chair (Burtron H. Davis) was also included on the certificate, along with the name of the recipient. The awardees were chosen on a merit-based guideline which also included the requirements of having a presentation accepted at the meeting and being a student at a North American University. The Richard J. Kokes Student Travel Award Committee (Gary Jacobs, Rodney Andrews, and Peter Smirniotis) with help from the Organizing Committee were able to secure money from four sources as detailed in Table 1. As detailed by our Treasurer, Dr. Helge Toufar of Clariant, the total amount spent was $105,000.

  2. Catalysis by Design: Bridging the Gap Between Theory and Experiments at

    Broader source: Energy.gov (indexed) [DOE]

    Nanoscale Level | Department of Energy Studies on a simple platinum-alumina system constitute a first step toward a "catalyst by design" approach. PDF icon deer08_narula.pdf More Documents & Publications Catalysis by Design: Bridging the Gap between Theory and Experiments Catalyst by Design - Theoretical, Nanostructural, and Experimental Studies of Oxidation Catalyst for Diesel Engine Emission Treatment

  3. NMR Computational Studies of Solid Acidity/Fundamental Studies of Catalysis by Solid Acids

    SciTech Connect (OSTI)

    James F. Haw

    2008-06-28

    This project focused on catalysis by zeolites and the synergy of spectroscopic characterization and theoretical modeling. In collaboration with the Waroquier group in Belgium we used state-of-the-art quantum chemical simulations on a supramolecular model of both the HZSM-5 zeolite and the co-catalytic hydrocarbon pool species and calculated a full catalytic cycle (including all rate constants) for methanol-to-olefin (MTO) catalysis involving a hydrocarbon pool species. This work not only represents the most robust computational analysis of a successful MTO route to date, but it also succeeds in tying together the many experimental clues. That work was featured on the cover of Angewandte Chemie. More recently we elucidated several unsuspected roles for formaldehyde in methanol to olefin catalysis. Formaldehyde proves to be a key species responsible for both the growth of the catalytically active hydrocarbon pool and its inevitable aging into deactivated polycyclic aromatic species. The apparent inevitability of formaldehyde formation at high temperatures, in particular in contact with active metal or metal oxide surfaces, may put some fundamental limitations on the economic potential of conversion of methanol to olefins.

  4. DEFLECTION OF A HETEROGENEOUS WIDE-BEAM UNDER UNIFORM PRESSURE LOAD

    SciTech Connect (OSTI)

    T. V. Holschuh; T. K. Howard; W. R. Marcum

    2014-07-01

    Oregon State University (OSU) and the Idaho National Laboratory (INL) are currently collaborating on a test program which entails hydro-mechanical testing of a generic plate type fuel element, or generic test plate assembly (GTPA), for the purpose of qualitatively demonstrating mechanical integrity of uranium-molybdenum monolithic plates as compared to that of uranium aluminum dispersion, and aluminum fuel plates onset by hydraulic forces. This test program supports ongoing work conducted for/by the Global Threat Reduction Initiative (GTRI) Fuels Development Program. This study’s focus supports the ongoing collaborative effort by detailing the derivation of an analytic solution for deflection of a heterogeneous plate under a uniform, distributed load in order to predict the deflection of test plates in the GTPA. The resulting analytical solutions for three specific boundary condition sets are then presented against several test cases of a homogeneous plate. In all test cases considered, the results for both homogeneous and heterogeneous plates are numerically identical to one another, demonstrating correct derivation of the heterogeneous solution. Two additional problems are presents herein that provide a representative deflection profile for the plates under consideration within the GTPA. Furthermore, qualitative observations are made about the influence of a more-rigid internal fuel-meat region and its influence on the overall deflection profile of a plate. Present work is being directed to experimentally confirm the analytical solution’s results using select materials.

  5. Variable valve timing in a homogenous charge compression ignition engine

    DOE Patents [OSTI]

    Lawrence, Keith E.; Faletti, James J.; Funke, Steven J.; Maloney, Ronald P.

    2004-08-03

    The present invention relates generally to the field of homogenous charge compression ignition engines, in which fuel is injected when the cylinder piston is relatively close to the bottom dead center position for its compression stroke. The fuel mixes with air in the cylinder during the compression stroke to create a relatively lean homogeneous mixture that preferably ignites when the piston is relatively close to the top dead center position. However, if the ignition event occurs either earlier or later than desired, lowered performance, engine misfire, or even engine damage, can result. The present invention utilizes internal exhaust gas recirculation and/or compression ratio control to control the timing of ignition events and combustion duration in homogeneous charge compression ignition engines. Thus, at least one electro-hydraulic assist actuator is provided that is capable of mechanically engaging at least one cam actuated intake and/or exhaust valve.

  6. A Computationally Based Approach to Homogenizing Advanced Alloys

    SciTech Connect (OSTI)

    Jablonski, P D; Cowen, C J

    2011-02-27

    We have developed a computationally based approach to optimizing the homogenization heat treatment of complex alloys. The Scheil module within the Thermo-Calc software is used to predict the as-cast segregation present within alloys, and DICTRA (Diffusion Controlled TRAnsformations) is used to model the homogenization kinetics as a function of time, temperature and microstructural scale. We will discuss this approach as it is applied to both Ni based superalloys as well as the more complex (computationally) case of alloys that solidify with more than one matrix phase as a result of segregation. Such is the case typically observed in martensitic steels. With these alloys it is doubly important to homogenize them correctly, especially at the laboratory scale, since they are austenitic at high temperature and thus constituent elements will diffuse slowly. The computationally designed heat treatment and the subsequent verification real castings are presented.

  7. Probing oxygen vacancy concentration and homogeneity in solid-oxide

    Office of Scientific and Technical Information (OSTI)

    fuel-cell cathode materials on the subunit-cell level (Journal Article) | SciTech Connect Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level Citation Details In-Document Search Title: Probing oxygen vacancy concentration and homogeneity in solid-oxide fuel-cell cathode materials on the subunit-cell level Oxygen vacancy distributions and dynamics directly control the operation of solid-oxide fuel cells and are

  8. Bedload sheets in heterogeneous sediment

    SciTech Connect (OSTI)

    Whiting, P.J.; Dietrich, W.E.; Leopold, L.B.; Drake, T.G.; Shreve, R.L.

    1988-02-01

    Field observations in streams with beds of coarse sand and fine gravel have revealed that bedload moves primarily as thin, migrating accumulations of sediment, and coarse grains cluster at their leading edge. These accumulations are one or two coarse grains high and are much longer (0.2-0.6 m long in sand; 0.5-2.0 m in fine gravel) than their height. The authors propose the term bedload sheet for these features, and the authors argue that they result from an instability inherent to bedload movement of moderately and poorly sorted sediment. In essence, coarse particles in the bedload slow or stop each other, trap finer particles in their interstices, and thus cause the coarse particles to become mobile again. Bedload sheets develop on the stoss side of dunes, causing the dune to advance incrementally with the arrival of each sheet. Successive deposition of coarse sediment from the leading edge followed by fine sediment may generate the grain-size sorting that distinguishes cross-bedding. Available flume experiments and field observations indicate that bedload sheets are a common, but generally unrecognized, feature of heterogeneous sediment transport.

  9. Low-Temperature Hydrocarbon/CO Oxidation Catalysis in Support of HCCI Emission Control

    Broader source: Energy.gov [DOE]

    Development of catalyst materials to facilitate the low-temperature oxidation of hydrocarbons and CO in homogeneous charge compression ignition (HCCI) emissions.

  10. Heterogeneous Recycling in Fast Reactors

    SciTech Connect (OSTI)

    Forget, Benoit; Pope, Michael; Piet, Steven J.; Driscoll, Michael

    2012-07-30

    Current sodium fast reactor (SFR) designs have avoided the use of depleted uranium blankets over concerns of creating weapons grade plutonium. While reducing proliferation risks, this restrains the reactor design space considerably. This project will analyze various blanket and transmutation target configurations that could broaden the design space while still addressing the non-proliferation issues. The blanket designs will be assessed based on the transmutation efficiency of key minor actinide (MA) isotopes and also on mitigation of associated proliferation risks. This study will also evaluate SFR core performance under different scenarios in which depleted uranium blankets are modified to include minor actinides with or without moderators (e.g. BeO, MgO, B4C, and hydrides). This will be done in an effort to increase the sustainability of the reactor and increase its power density while still offering a proliferation resistant design with the capability of burning MA waste produced from light water reactors (LWRs). Researchers will also analyze the use of recycled (as opposed to depleted) uranium in the blankets. The various designs will compare MA transmutation efficiency, plutonium breeding characteristics, proliferation risk, shutdown margins and reactivity coefficients with a current reference sodium fast reactor design employing homogeneous recycling. The team will also evaluate the out-of-core accumulation and/or burn-down rates of MAs and plutonium isotopes on a cycle-by-cycle basis. This cycle-by-cycle information will be produced in a format readily usable by the fuel cycle systems analysis code, VISION, for assessment of the sustainability of the deployment scenarios.

  11. HYPERSONIC BUCKSHOT: ASTROPHYSICAL JETS AS HETEROGENEOUS COLLIMATED PLASMOIDS

    SciTech Connect (OSTI)

    Yirak, Kristopher; Frank, Adam; Cunningham, Andrew J.; Mitran, Sorin

    2009-04-20

    Herbig-Haro jets are commonly thought of as homogeneous beams of plasma traveling at hypersonic velocities. Structure within jet beams is often attributed to periodic or 'pulsed' variations of conditions at the jet source. Simulations based on this scenario result in knots extending across the jet diameter. Observations and recent high energy density laboratory experiments shed new light on structures below this scale and indicate they may be important for understanding the fundamentals of jet dynamics. In this paper, we offer an alternative to 'pulsed' models of protostellar jets. Using direct numerical simulations we explore the possibility that jets are chains of subradial clumps propagating through a moving interclump medium. Our models explore an idealization of this scenario by injecting small (r < r {sub jet}), dense ({rho}>{rho}{sub jet}) spheres embedded in an otherwise smooth interclump jet flow. The spheres are initialized with velocities differing from the jet velocity by {approx}15%. We find that the consequences of shifting from homogeneous to heterogeneous flows are significant as clumps interact with each other and with the interclump medium in a variety of ways. Structures which mimic what is expected from pulsed-jet models can form, as can be previously unseen, 'subradial' behaviors including backward facing bow shocks and off-axis working surfaces. While these small-scale structures have not been seen before in simulation studies, they are found in high-resolution jet observations. We discuss implications of our simulations for the interpretation of protostellar jets with regard to characterization of knots by a 'lifetime' or 'velocity history' approach as well as linking observed structures with central engines which produce the jets.

  12. Linkage heterogeneity among 59 Dutch hereditary breast cancer families

    SciTech Connect (OSTI)

    Cornelis, R.S.; Vliet, M. van; Leeuwen, I. van

    1994-09-01

    We have investigated 59 Dutch kindreds with at least three first-degree relatives with breast and/or ovarian cancer for linkage to BRCA1 on 17q12-q21, using at least 4 microsatellite markers flanking BRCA1 on either side. Assuming no heterogeneity, the overall multipoint lod score in this group of families was -7.59. A marked clustering of lod scores >0.5 was observed among the 13 families with a mean age of onset lower than 45 (total lod score: +3.36). Among the 8 kindreds with a mean age of onset lower than 45 and {ge}3 cases diagnosed under 45, the lod score was +4.43. Interestingly, most of the evidence against linkage was found in 17 families with a mean age of onset between 45 and 54 (total lod score of -8.72). It was estimated that 28% of the breast-only families might be caused by BRCA1. Over the 16 breast-ovarian cancer families a lod score of -3.78 was obtained under homogeneity. The highest lod score was +0.57, assuming heterogeneity with 33% of the families being linked to BRCA1. One family gave a multipoint lod score of -2.01 and thereby satisfies the conventional criterion of an unlinked family. Our results support the conclusions from earlier work by others, namely that BRCA1 predisposes particularly to early-onset breast cancer. The proportion of breast-ovarian cancer families we found linked to BRCA1 is much lower than that found by the Breast Cancer Linkage Consortium. This might be caused by the single unlinked family against an insufficient number of families able to give conclusive positive lod scores.

  13. The Role of Solvent Heterogeneity in Determining the Dispersion...

    Office of Scientific and Technical Information (OSTI)

    The Role of Solvent Heterogeneity in Determining the Dispersion Interaction Between Nanoassemblies Citation Details In-Document Search Title: The Role of Solvent Heterogeneity in ...

  14. Electric-field enhanced performance in catalysis and solid-state devices involving gases

    DOE Patents [OSTI]

    Blackburn, Bryan M.; Wachsman, Eric D.; Van Assche, IV, Frederick Martin

    2015-05-19

    Electrode configurations for electric-field enhanced performance in catalysis and solid-state devices involving gases are provided. According to an embodiment, electric-field electrodes can be incorporated in devices such as gas sensors and fuel cells to shape an electric field provided with respect to sensing electrodes for the gas sensors and surfaces of the fuel cells. The shaped electric fields can alter surface dynamics, system thermodynamics, reaction kinetics, and adsorption/desorption processes. In one embodiment, ring-shaped electric-field electrodes can be provided around sensing electrodes of a planar gas sensor.

  15. Homogeneous charge engines -- Basis of cyclic variations. Final report

    SciTech Connect (OSTI)

    Whitelaw, J.H.

    1997-06-30

    The objectives of the Grant required investigations of cyclic variations in a homogeneous-charge engine initially with gas combustion and the air from ranging from near quiescent to the incorporation of swirl and tumble by valve inserts. Later experiments were performed with unleaded gasoline. The measurements included local velocity and cylinder pressure through the four strokes of a single-cylinder engine, under motored and firing conditions and with examination of the flame kernel growth by combinations of photography and flame-ionization gauges. In all cases, the measurements of in-cylinder characteristics were linked to performance as measured in terms of speed and its variability, load and emissions. The experiments progressed to consider deviations from homogeneous charge and included consideration of stratified charge with local injection of a rich mixture in the vicinity of the spark gap so as to establish a flame kernel which would propagate securely into an overall weak mixture.

  16. Apparatus for unilateral generation of a homogeneous magnetic field

    DOE Patents [OSTI]

    Fukushima, E.; Rath, A.R.; Roeder, S.B.W.

    1984-05-01

    An apparatus for unilaterally producing a substantially homogeneous magnetic field. The apparatus includes two circular electromagnet coils, a small coil and a large coil, which are coaxial with one another and which are separated by a distance equal to one-half the difference in the radius of the two coils. By appropriate selection of electrical currents, which are passed through the coils in opposite directions, a region of homogeneous magnetic field is formed. This region is centered on the common axis of the two coils, at a point on the axis which is at a distance from the small coil equal to one-half the radius of the small coil, and which is on the opposite side of the small coil from the large coil. The apparatus has particular application in the field of diagnostic medical NMR and other NMR applications.

  17. Apparatus for unilateral generation of a homogeneous magnetic field

    DOE Patents [OSTI]

    Fukushima, Eiichi; Rath, Alan R.; Roeder, Stephen B. W.

    1988-01-01

    An apparatus for unilaterally producing a substantially homogeneous magnetic field. The apparatus includes two circular electromagnet coils, a small coil and a large coil, which are coaxial with one another and which are separated by a distance equal to one-half the difference in the radius of the two coils. By appropriate selection of electrical currents, which are passed through the coil in opposite directions, a region of homogeneous magnetic field is formed. This region is centered on the common axis of the two coils, at a point on the axis which is at a distance from the small coil equal to one-half the radius of the small coil, and which is on the opposite side of the small coil from the large coil. The apparatus has particular application in the field of diagnostic medical NMR and other NMR applications.

  18. Environment-based pin-power reconstruction method for homogeneous core calculations

    SciTech Connect (OSTI)

    Leroyer, H.; Brosselard, C.; Girardi, E.

    2012-07-01

    Core calculation schemes are usually based on a classical two-step approach associated with assembly and core calculations. During the first step, infinite lattice assemblies calculations relying on a fundamental mode approach are used to generate cross-sections libraries for PWRs core calculations. This fundamental mode hypothesis may be questioned when dealing with loading patterns involving several types of assemblies (UOX, MOX), burnable poisons, control rods and burn-up gradients. This paper proposes a calculation method able to take into account the heterogeneous environment of the assemblies when using homogeneous core calculations and an appropriate pin-power reconstruction. This methodology is applied to MOX assemblies, computed within an environment of UOX assemblies. The new environment-based pin-power reconstruction is then used on various clusters of 3x3 assemblies showing burn-up gradients and UOX/MOX interfaces, and compared to reference calculations performed with APOLLO-2. The results show that UOX/MOX interfaces are much better calculated with the environment-based calculation scheme when compared to the usual pin-power reconstruction method. The power peak is always better located and calculated with the environment-based pin-power reconstruction method on every cluster configuration studied. This study shows that taking into account the environment in transport calculations can significantly improve the pin-power reconstruction so far as it is consistent with the core loading pattern. (authors)

  19. Simulator for SUPO, a Benchmark Aqueous Homogeneous Reactor (AHR)

    SciTech Connect (OSTI)

    Klein, Steven Karl; Determan, John C.

    2015-10-14

    A simulator has been developed for SUPO (Super Power) an aqueous homogeneous reactor (AHR) that operated at Los Alamos National Laboratory (LANL) from 1951 to 1974. During that period SUPO accumulated approximately 600,000 kWh of operation. It is considered the benchmark for steady-state operation of an AHR. The SUPO simulator was developed using the process that resulted in a simulator for an accelerator-driven subcritical system, which has been previously reported.

  20. High load operation in a homogeneous charge compression ignition engine

    DOE Patents [OSTI]

    Duffy, Kevin P.; Kieser, Andrew J.; Liechty, Michael P.; Hardy, William L.; Rodman, Anthony; Hergart, Carl-Anders

    2008-12-23

    A homogeneous charge compression ignition engine is set up by first identifying combinations of compression ratio and exhaust gas percentages for each speed and load across the engines operating range. These identified ratios and exhaust gas percentages can then be converted into geometric compression ratio controller settings and exhaust gas recirculation rate controller settings that are mapped against speed and load, and made available to the electronic

  1. Multicomponent homogeneous alloys and method for making same

    DOE Patents [OSTI]

    Dutta, Partha S.; Miller, Thomas R.

    2003-09-02

    The present application discloses a method for preparing a homogeneous ternary or quaternary alloy from a quaternary melt. The method includes providing a family of phase diagrams for the quaternary melt which shows (i) composition/temperature data, (ii) tie lines connecting equilibrium liquid and solid compositions, and (iii) isotherms representing boundaries of a miscibility gap. Based on the family of phase diagrams, a quaternary melt composition and an alloy growth temperature is selected. A quaternary melt having the selected quaternary melt composition is provided and a ternary or quaternary alloy is grown from the quaternary melt at the selected alloy growth temperature. A method for making homogeneous ternary or quaternary alloy from a ternary or quaternary melt is also disclosed, as are homogeneous quaternary single-crystal alloys which are substantially free from crystal defects and which have the formula A.sub.x B.sub.1-x C.sub.y D.sub.1-y, x and y being the same or different and in the range of 0.001 to 0.999.

  2. Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.

    SciTech Connect (OSTI)

    Chou, Stanley Shihyao; Sai, Na; Lu, Ping; Coker, Eric Nicholas; Liu, Sheng; Artyushkova, Kateryna; Luk, Ting S.; Kaehr, Bryan James; Brinker, C. Jeffrey

    2015-10-07

    Establishing processing–structure–property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T' (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔGH), and, with respect to catalysis, the 1T' transformation renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Furthermore, we show basal plane activation of 1T' molybdenum disulfide and a lowering of ΔGH from +1.6 eV for 2H to +0.18 eV for 1T', comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.

  3. Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.

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

    Chou, Stanley Shihyao; Sai, Na; Lu, Ping; Coker, Eric Nicholas; Liu, Sheng; Artyushkova, Kateryna; Luk, Ting S.; Kaehr, Bryan James; Brinker, C. Jeffrey

    2015-10-07

    Establishing processing–structure–property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T' (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔGH), and, with respect to catalysis, the 1T' transformationmore » renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Furthermore, we show basal plane activation of 1T' molybdenum disulfide and a lowering of ΔGH from +1.6 eV for 2H to +0.18 eV for 1T', comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.« less

  4. Controlling And Operating Homogeneous Charge Compression Ignition (Hcci) Engines

    DOE Patents [OSTI]

    Flowers, Daniel L. (San Leandro, CA)

    2005-08-02

    A Homogeneous Charge Compression Ignition (HCCI) engine system includes an engine that produces exhaust gas. A vaporization means vaporizes fuel for the engine an air induction means provides air for the engine. An exhaust gas recirculation means recirculates the exhaust gas. A blending means blends the vaporized fuel, the exhaust gas, and the air. An induction means inducts the blended vaporized fuel, exhaust gas, and air into the engine. A control means controls the blending of the vaporized fuel, the exhaust gas, and the air and for controls the inducting the blended vaporized fuel, exhaust gas, and air into the engine.

  5. Exhaust gas recirculation in a homogeneous charge compression ignition engine

    DOE Patents [OSTI]

    Duffy, Kevin P.; Kieser, Andrew J.; Rodman, Anthony; Liechty, Michael P.; Hergart, Carl-Anders; Hardy, William L.

    2008-05-27

    A homogeneous charge compression ignition engine operates by injecting liquid fuel directly in a combustion chamber, and mixing the fuel with recirculated exhaust and fresh air through an auto ignition condition of the fuel. The engine includes at least one turbocharger for extracting energy from the engine exhaust and using that energy to boost intake pressure of recirculated exhaust gas and fresh air. Elevated proportions of exhaust gas recirculated to the engine are attained by throttling the fresh air inlet supply. These elevated exhaust gas recirculation rates allow the HCCI engine to be operated at higher speeds and loads rendering the HCCI engine a more viable alternative to a conventional diesel engine.

  6. Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2

    SciTech Connect (OSTI)

    Appel, Aaron M.; Bercaw, John E.; Bocarsly, Andrew B.; Dobbek, Holger; DuBois, Daniel L.; Dupuis, Michel; Ferry, James G.; Fujita, Etsuko; Hille, Russ; Kenis, Paul; Kerfeld, Cheryl A.; Morris, Robert H.; Peden, Charles HF; Portis, Archie; Ragsdale, Steve; Rauchfuss, Thomas B.; Reek, Joost; Seefeldt, Lance C.; Thauer, Rudolf K.; Waldrop, Grover L.

    2013-08-14

    Our central premise is that catalytic scientists can learn by studying how these important metabolic processes occur in nature. Complementarily, biochemists can learn by studying how catalytic scientists view these same chemical transformations promoted by synthetic catalysts. From these studies, hypotheses can be developed and tested through manipulation of enzyme structure and by synthesizing simple molecular catalysts to incorporate different structural features of the enzymes. It is hoped that these studies will lead to new and useful concepts in catalyst design for fuel production and utilization. This paper describes the results of a workshop held to explore these concepts in regard to the development of new and more efficient catalytic processes for the conversion of CO2 to a variety of carbon-based fuels. The organization of this overview/review is as follows: 1) The first section briefly explores how interactions between the catalysis and biological communities have been fruitful in developing new catalysts for the reduction of protons to hydrogen, the simplest fuel generation reaction. 2) The second section assesses the state of the art in both biological and chemical reduction of CO2 by two electrons to form either carbon monoxide (CO) or formate (HCOO-). It also attempts to identify common principles between biological and synthetic catalysts and productive areas for future research. 3) The third section explores both biological and chemical processes that result in the reduction of CO2 beyond the level of CO and formate, again seeking to identify common principles and productive areas of future research. 4) The fourth section explores the formation of carbon-carbon bonds in biological and chemical systems in the same vein as the other sections. 5) A fifth section addresses the role of non-redox reactions of CO2 in biological systems and their role in carbon metabolism, with a parallel discussion of chemical systems. 6) In section 6, the topics of electrode modification, photochemical systems, and tandem catalysis are briefly discussed. These areas may be important for developing practical systems for CO2 reduction, and they share the common theme of coupling chemical reactions. 7) Section 7 describes some of the crosscutting activities that are critical for advancing the science underpinning catalyst development. 8) The last section attempts to summarize common issues in biological and chemical catalysis and to identify challenges that must be addressed to achieve practical catalysts that are suitable for the reduction of CO2 to fuels.

  7. Design, Synthesis and Mechanistic Evaluation of Iron-Based Catalysis for Synthesis Gas Conversion to Fuels and Chemicals

    SciTech Connect (OSTI)

    Akio Ishikawa; Manuel Ojeda; Nan Yao; Enrique Iglesia

    2007-03-31

    This project extends previously discovered Fe-based catalysts to hydrogen-poor synthesis gas streams derived from coal and biomass sources. These catalysts have shown unprecedented Fischer-Tropsch synthesis rates and selectivities for synthesis gas derived from methane. During the first reporting period, we certified a microreactor, installed required analytical equipment, and reproduced synthetic protocols and catalytic results previously reported. During the second reporting period, we prepared several Fe-based compositions for Fischer-Tropsch Synthesis and tested the effects of product recycle under both subcritical and supercritical conditions. During the third and fourth reporting periods, we improved the catalysts preparation method, which led to Fe-based materials with the highest FTS reaction rates and selectivities so far reported, a finding that allowed their operation at lower temperatures and pressures with high selectivity to desired products (C{sub 5+}, olefins). During the fifth and sixth reporting period, we studied the effects of different promoters on catalytic performance, specifically how their sequence of addition dramatically influenced the performance of these materials in the Fischer-Tropsch synthesis. We also continued our studies of the kinetic behavior of these materials during the sixth reporting period. Specifically, the effects of H{sub 2}, CO, and CO{sub 2} on the rates and selectivities of Fischer-Tropsch Synthesis reactions led us to propose a new sequence of elementary steps on Fe and Co Fischer-Tropsch catalysts. Finally, we also started a study of the use of colloidal precipitation methods for the synthesis small Co clusters using recently developed methods to explore possible further improvements in FTS rates and selectivities. We found that colloidal synthesis makes possible the preparation of small cobalt particles, although large amount of cobalt silicate species, which are difficult to reduce, were formed. During this seventh reporting period, we have explored several methods to modify the silanol groups on SiO{sub 2} by using either a homogeneous deposition-precipitation method or surface titration of Si-OH on SiO{sub 2} with zirconium (IV) ethoxide to prevent the formation of unreducible and unreactive CoO{sub x} species during synthesis and FTS catalysis. We have synthesized monometallic Co/ZrO{sub 2}/SiO{sub 2} catalysts with different Co loadings (11-20 wt%) by incipient wetness impregnation methods and characterized the prepared Co supported catalysts by H{sub 2} temperature-programmed reduction (H{sub 2}-TPR) and H{sub 2}-chemisorption. We have measured the catalytic performance in FTS reactions and shown that although the hydroxyl groups on the SiO{sub 2} surface are difficult to be fully titrated by ZrO{sub 2}, modification of ZrO{sub 2} on SiO{sub 2} surface can improve the Co clusters dispersion and lead to a larger number of exposed Co surface atoms after reduction and during FTS reactions. During this seventh reporting period, we have also advanced our development of the reaction mechanism proposed in the previous reporting period. Specifically, we have shown that our novel proposal for the pathways involved in CO activation on Fe and Co catalysts is consistent with state-of-the-art theoretical calculations carried out in collaboration with Prof. Manos Mavrikakis (University of Wisconsin-Madison). Finally, we have also worked on the preparation of several manuscripts describing our findings about the preparation, activation and mechanism of the FTS with Fe-based catalysts and we have started redacting the final report for this project.

  8. Homogenization limit for a multiband effective mass model in heterostructures

    SciTech Connect (OSTI)

    Morandi, O.

    2014-06-15

    We study the homogenization limit of a multiband model that describes the quantum mechanical motion of an electron in a quasi-periodic crystal. In this approach, the distance among the atoms that constitute the material (lattice parameter) is considered a small quantity. Our model include the description of materials with variable chemical composition, intergrowth compounds, and heterostructures. We derive the effective multiband evolution system in the framework of the kp approach. We study the well posedness of the mathematical problem. We compare the effective mass model with the standard kp models for uniform and non-uniforms crystals. We show that in the limit of vanishing lattice parameter, the particle density obtained by the effective mass model, converges to the exact probability density of the particle.

  9. Crystallization in supercooled liquid Cu: Homogeneous nucleation and growth

    SciTech Connect (OSTI)

    E, J. C.; Wang, L.; Luo, S. N.; Cai, Y.; Wu, H. A.

    2015-02-14

    Homogeneous nucleation and growth during crystallization of supercooled liquid Cu are investigated with molecular dynamics simulations, and the microstructure is characterized with one- and two-dimensional x-ray diffraction. The resulting solids are single-crystal or nanocrystalline, containing various defects such as stacking faults, twins, fivefold twins, and grain boundaries; the microstructure is subject to thermal fluctuations and extent of supercooling. Fivefold twins form via sequential twinning from the solid-liquid interfaces. Critical nucleus size and nucleation rate at 31% supercooling are obtained from statistical runs with the mean first-passage time and survival probability methods, and are about 14 atoms and 10{sup 32} m{sup −3}s{sup −1}, respectively. The bulk growth dynamics are analyzed with the Johnson-Mehl-Avrami law and manifest three stages; the Avrami exponent varies in the range of 1–19, which also depends on thermal fluctuations and supercooling.

  10. The manufacture and performance of homogeneous microstructure SBR MOX fuel

    SciTech Connect (OSTI)

    Barker, Matthew A.; Stephenson, Keith; Weston, Rebecca

    2007-07-01

    In the early 1980's, British experience in the manufacture of mixed-oxide fast reactor fuel was used to develop a new thermal MOX manufacturing route called the Short Binder-less Route (SBR). Laboratory- scale development led to the manufacture of commercial PWR fuel in a small pilot plant, and the construction of the full-scale dual-line Sellafield MOX Plant (SMP). SMP's first MOX assemblies are now under irradiation. SBR MOX is manufactured with 100% co-milled feedstock, leading to a microstructure dominated by a solid solution of (U,Pu)O{sub 2} at the nominal enrichment. A comprehensive fuel performance research programme has demonstrated the benign performance of SBR MOX up to 54 MWd/kgHM. In particular, the homogeneous microstructure is believed to be instrumental in the favourable fission gas retention and PCI resistance properties. (authors)

  11. Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2

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

    Hod, Idan; Sampson, Matthew D.; Deria, Pravas; Kubiak, Clifford P.; Farha, Omar K.; Hupp, Joseph T.

    2015-09-18

    Realization of heterogeneous electrochemical CO2-to-fuel conversion via molecular catalysis under high-flux conditions requires the assembly of large quantities of reactant-accessible catalysts on conductive surfaces. As a proof of principle, we demonstrate that electrophoretic deposition of thin films of an appropriately chosen metal–organic framework (MOF) material is an effective method for immobilizing the needed quantity of catalyst. For electrocatalytic CO2 reduction, we used a material that contains functionalized Fe-porphyrins as catalytically competent, redox-conductive linkers. The approach yields a high effective surface coverage of electrochemically addressable catalytic sites (~1015 sites/cm2). The chemical products of the reduction, obtained with ~100% Faradaic efficiency, aremore » mixtures of CO and H2. The results validate the strategy of using MOF chemistry to obtain porous, electrode-immobilized, networks of molecular catalysts having competency for energy-relevant electrochemical reactions.« less

  12. Carbon-Based and Carbon-Supported Heterogeneous Catalysts for...

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

    Carbon-Based and Carbon-Supported Heterogeneous Catalysts for the Conversion of Biomass Carbon-based heterogeneous catalysts play a central role in the conversion of biomass to...

  13. Computational Spectroscopy of Heterogeneous Interfaces | Argonne Leadership

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

    Computing Facility Complex interfaces between nanoparticles and a solvent Complex interfaces between nanoparticles and a solvent. N. Brawand, University of Chicago Computational Spectroscopy of Heterogeneous Interfaces PI Name: Giulia Galli PI Email: gagalli@uchicago.edu Institution: University of Chicago Allocation Program: INCITE Allocation Hours at ALCF: 150 Million Year: 2016 Research Domain: Materials Science The interfaces between solids, nanoparticles and liquids play a fundamental

  14. A Nth-order linear algorithm for extracting diffuse correlation spectroscopy blood flow indices in heterogeneous tissues

    SciTech Connect (OSTI)

    Shang, Yu; Yu, Guoqiang

    2014-09-29

    Conventional semi-infinite analytical solutions of correlation diffusion equation may lead to errors when calculating blood flow index (BFI) from diffuse correlation spectroscopy (DCS) measurements in tissues with irregular geometries. Very recently, we created an algorithm integrating a Nth-order linear model of autocorrelation function with the Monte Carlo simulation of photon migrations in homogenous tissues with arbitrary geometries for extraction of BFI (i.e., αD{sub B}). The purpose of this study is to extend the capability of the Nth-order linear algorithm for extracting BFI in heterogeneous tissues with arbitrary geometries. The previous linear algorithm was modified to extract BFIs in different types of tissues simultaneously through utilizing DCS data at multiple source-detector separations. We compared the proposed linear algorithm with the semi-infinite homogenous solution in a computer model of adult head with heterogeneous tissue layers of scalp, skull, cerebrospinal fluid, and brain. To test the capability of the linear algorithm for extracting relative changes of cerebral blood flow (rCBF) in deep brain, we assigned ten levels of αD{sub B} in the brain layer with a step decrement of 10% while maintaining αD{sub B} values constant in other layers. Simulation results demonstrate the accuracy (errors < 3%) of high-order (N ≥ 5) linear algorithm in extracting BFIs in different tissue layers and rCBF in deep brain. By contrast, the semi-infinite homogenous solution resulted in substantial errors in rCBF (34.5% ≤ errors ≤ 60.2%) and BFIs in different layers. The Nth-order linear model simplifies data analysis, thus allowing for online data processing and displaying. Future study will test this linear algorithm in heterogeneous tissues with different levels of blood flow variations and noises.

  15. Reducing the effects of acoustic heterogeneity with an iterative reconstruction method from experimental data in microwave induced thermoacoustic tomography

    SciTech Connect (OSTI)

    Wang, Jinguo; Zhao, Zhiqin Song, Jian; Chen, Guoping; Nie, Zaiping; Liu, Qing-Huo

    2015-05-15

    Purpose: An iterative reconstruction method has been previously reported by the authors of this paper. However, the iterative reconstruction method was demonstrated by solely using the numerical simulations. It is essential to apply the iterative reconstruction method to practice conditions. The objective of this work is to validate the capability of the iterative reconstruction method for reducing the effects of acoustic heterogeneity with the experimental data in microwave induced thermoacoustic tomography. Methods: Most existing reconstruction methods need to combine the ultrasonic measurement technology to quantitatively measure the velocity distribution of heterogeneity, which increases the system complexity. Different to existing reconstruction methods, the iterative reconstruction method combines time reversal mirror technique, fast marching method, and simultaneous algebraic reconstruction technique to iteratively estimate the velocity distribution of heterogeneous tissue by solely using the measured data. Then, the estimated velocity distribution is used subsequently to reconstruct the highly accurate image of microwave absorption distribution. Experiments that a target placed in an acoustic heterogeneous environment are performed to validate the iterative reconstruction method. Results: By using the estimated velocity distribution, the target in an acoustic heterogeneous environment can be reconstructed with better shape and higher image contrast than targets that are reconstructed with a homogeneous velocity distribution. Conclusions: The distortions caused by the acoustic heterogeneity can be efficiently corrected by utilizing the velocity distribution estimated by the iterative reconstruction method. The advantage of the iterative reconstruction method over the existing correction methods is that it is successful in improving the quality of the image of microwave absorption distribution without increasing the system complexity.

  16. Dose homogeneity specification for reference dosimetry of nonstandard fields

    SciTech Connect (OSTI)

    Chung, Eunah; Soisson, Emilie; Seuntjens, Jan [Medical Physics Unit, McGill University, Montreal General Hospital (L5-113), 1650 Cedar Avenue, Montreal, Quebec H3G 1A4 (Canada); Medical Physics Unit, McGill University and Department of Medical Physics, McGill University Health Centre, Montreal General Hospital (L5-113), 1650 Cedar Avenue, Montreal, Quebec H3G 1A4 (Canada); Medical Physics Unit, McGill University, Montreal General Hospital (L5-113), 1650 Cedar Avenue, Montreal, Quebec H3G 1A4 (Canada)

    2012-01-15

    Purpose: To investigate the sensitivity of the plan-class specific correction factor to dose distributions in composite nonstandard field dosimetry. Methods: A cylindrical water-filled PMMA phantom was constructed at the center of which reference absorbed dose could be measured. Ten different TomoTherapy-based IMRT fields were created on the CT images of the phantom. The dose distribution for each IMRT field was estimated at the position of a radiation detector or ionization chamber. The dose in each IMRT field normalized to that in a reference 10 x 10 cm{sup 2} field was measured using a PTW micro liquid ion chamber. Based on the new dosimetry formalism, a plan-class specific correction factor k{sub Q{sub p{sub c{sub s{sub r,Q}{sup f{sub p}{sub c}{sub s}{sub r},f{sub r}{sub e}{sub f}}}}}} for each field was measured for two Farmer-type chambers, Exradin A12 and NE2571, as well as for a smaller Exradin A1SL chamber. The dependence of the measured correction factor on parameters characterizing dose distribution was analyzed. Results: Uncertainty on the plan-class specific correction factor measurement was in the range of 0.3%-0.5% and 0.3%-0.8% for the Farmer-type chambers and the Exradin A1SL, respectively. When the heterogeneity of the central region of the target volume was less than 5%, the correction factor did not differ from unity by more than 0.7% for the three air-filled ionization chambers. For more heterogeneous dose deliveries, the correction factor differed from unity by up to 2.4% for the Farmer-type chambers. For the Exradin A1SL, the correction factor was closer to unity due to the reduced effect of dose gradients, while it was highly variable in different IMRT fields because of a more significant impact of positioning uncertainties on the response of this chamber. Conclusions: The authors have shown that a plan-class specific correction factor can be specified as a function of plan evaluation parameters especially for Farmer-type chambers. This work provides a recipe based on quantifying dose distribution to accurately select air-filled ionization chamber correction factors for nonstandard fields.

  17. Research | The Ames Laboratory

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

    Research Division of Chemical and Biological Sciences - This Division develops and applies theoretical, computational and experimental methods to the study of surface reaction phenomena, cluster science and nucleation, biological processes and catalysis. World-leading research is conducted at the interface between homogenous and heterogenous catalysis. This research has led to improved processes for biodiesel production. New characterization techniques and theoretical methods to enable improved

  18. Experimental investigation of supercritical CO2 trapping mechanisms at the Intermediate Laboratory Scale in well-defined heterogeneous porous media

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

    Trevisan, Luca; Pini, Ronny; Cihan, Abdullah; Birkholzer, Jens T.; Zhou, Quanlin; Illangasekare, Tissa H.

    2014-12-31

    The heterogeneous nature of typical sedimentary formations can play a major role in the propagation of the CO2 plume, eventually dampening the accumulation of mobile phase underneath the caprock. From core flooding experiments, it is also known that contrasts in capillary threshold pressure due to different pore size can affect the flow paths of the invading and displaced fluids and consequently influence the build- up of non-wetting phase (NWP) at interfaces between geological facies. The full characterization of the geologic variability at all relevant scales and the ability to make observations on the spatial and temporal distribution of the migrationmore » and trapping of supercritical CO2 is not feasible from a practical perspective. To provide insight into the impact of well-defined heterogeneous systems on the flow dynamics and trapping efficiency of supercritical CO2 under drainage and imbibition conditions, we present an experimental investigation at the meter scale conducted in synthetic sand reservoirs packed in a quasi-two-dimensional flow-cell. Two immiscible displacement experiments have been performed to observe the preferential entrapment of NWP in simple heterogeneous porous media. The experiments consisted of an injection, a fluid redistribution, and a forced imbibition stages conducted in an uncorrelated permeability field and a homogeneous base case scenario. We adopted x-ray attenuation analysis as a non-destructive technique that allows a precise measurement of phase saturations throughout the entire flow domain. By comparing a homogeneous and a heterogeneous scenario we have identified some important effects that can be attributed to capillary barriers, such as dampened plume advancement, higher non-wetting phase saturations, larger contact area between the injected and displaced phases, and a larger range of non-wetting phase saturations.« less

  19. Dynamic control of a homogeneous charge compression ignition engine

    DOE Patents [OSTI]

    Duffy, Kevin P.; Mehresh, Parag; Schuh, David; Kieser, Andrew J.; Hergart, Carl-Anders; Hardy, William L.; Rodman, Anthony; Liechty, Michael P.

    2008-06-03

    A homogenous charge compression ignition engine is operated by compressing a charge mixture of air, exhaust and fuel in a combustion chamber to an autoignition condition of the fuel. The engine may facilitate a transition from a first combination of speed and load to a second combination of speed and load by changing the charge mixture and compression ratio. This may be accomplished in a consecutive engine cycle by adjusting both a fuel injector control signal and a variable valve control signal away from a nominal variable valve control signal. Thereafter in one or more subsequent engine cycles, more sluggish adjustments are made to at least one of a geometric compression ratio control signal and an exhaust gas recirculation control signal to allow the variable valve control signal to be readjusted back toward its nominal variable valve control signal setting. By readjusting the variable valve control signal back toward its nominal setting, the engine will be ready for another transition to a new combination of engine speed and load.

  20. HIGH TEMPERATURE, HIGH POWER HETEROGENEOUS NUCLEAR REACTOR

    DOE Patents [OSTI]

    Hammond, R.P.; Wykoff, W.R.; Busey, H.M.

    1960-06-14

    A heterogeneous nuclear reactor is designed comprising a stationary housing and a rotatable annular core being supported for rotation about a vertical axis in the housing, the core containing a plurality of radial fuel- element supporting channels, the cylindrical empty space along the axis of the core providing a central plenum for the disposal of spent fuel elements, the core cross section outer periphery being vertically gradated in radius one end from the other to provide a coolant duct between the core and the housing, and means for inserting fresh fuel elements in the supporting channels under pressure and while the reactor is in operation.

  1. Heterogeneously integrated microsystem-on-a-chip

    DOE Patents [OSTI]

    Chanchani, Rajen

    2008-02-26

    A microsystem-on-a-chip comprises a bottom wafer of normal thickness and a series of thinned wafers can be stacked on the bottom wafer, glued and electrically interconnected. The interconnection layer comprises a compliant dielectric material, an interconnect structure, and can include embedded passives. The stacked wafer technology provides a heterogeneously integrated, ultra-miniaturized, higher performing, robust and cost-effective microsystem package. The highly integrated microsystem package, comprising electronics, sensors, optics, and MEMS, can be miniaturized both in volume and footprint to the size of a bottle-cap or less.

  2. Sulfation of metal-organic framework: Opportunities for acid catalysis and proton conductivity

    SciTech Connect (OSTI)

    Goesten, M.G.; Stavitski, E.; Juan-Alcaniz, J.; Ramos-Fernandez, E.V.; Sai Sankar Gupta, K.B.; van Bekkum, H.; Gascon, J. and Kapteijn, F.

    2011-05-24

    A new post-functionalization method for metal-organic frameworks (MOFs) has been developed to introduce acidity for catalysis. Upon treatment with a mixture of triflic anhydride and sulfuric acid, chemically stable MOF structures MIL-101(Cr) and MIL-53(Al) can be sulfated, resulting in a Broensted sulfoxy acid group attached to up to 50% of the aromatic terephthalate linkers of the structure. The sulfated samples have been extensively characterized by solid-state NMR, XANES, and FTIR spectroscopy. The functionalized acidic frameworks show catalytic activity similar to that of acidic polymers like Nafion{reg_sign} display in the esterification of n-butanol with acetic acid (TOF {approx} 1 min{sup -1} {at} 343 K). Water adsorbs strongly up to 4 molecules per sulfoxy acid group, and an additional 2 molecules are taken up at lower temperatures in the 1-D pore channels of S-MIL-53(Al). The high water content and Broensted acidity provide the structure S-MIL-53(Al) a high proton conductivity up to moderate temperatures.

  3. Microstructure and nonlinear signatures of yielding in a heterogeneous colloidal gel under large amplitude oscillatory shear

    SciTech Connect (OSTI)

    Kim, Juntae; Helgeson, Matthew E.; Merger, Dimitri; Wilhelm, Manfred

    2014-09-01

    We investigate yielding in a colloidal gel that forms a heterogeneous structure, consisting of a two-phase bicontinuous network of colloid-rich domains of fractal clusters and colloid-poor domains. Combining large amplitude oscillatory shear measurements with simultaneous small and ultra-small angle neutron scattering (rheo-SANS/USANS), we characterize both the nonlinear mechanical processes and strain amplitude-dependent microstructure underlying yielding. We observe a broad, three-stage yielding process that evolves over an order of magnitude in strain amplitude between the onset of nonlinearity and flow. Analyzing the intracycle response as a sequence of physical processes reveals a transition from elastic straining to elastoplastic thinning (which dominates in region I) and eventually yielding (which evolves through region II) and flow (which saturates in region III), and allows quantification of instantaneous nonlinear parameters associated with yielding. These measures exhibit significant strain rate amplitude dependence above a characteristic frequency, which we argue is governed by poroelastic effects. Correlating these results with time-averaged rheo-USANS measurements reveals that the material passes through a cascade of structural breakdown from large to progressively smaller length scales. In region I, compression of the fractal domains leads to the formation of large voids. In regions II and III, cluster-cluster correlations become increasingly homogeneous, suggesting breakage and eventually depercolation of intercluster bonds at the yield point. All significant structural changes occur on the micron-scale, suggesting that large-scale rearrangements of hundreds or thousands of particles, rather than the homogeneous rearrangement of particle-particle bonds, dominate the initial yielding of heterogeneous colloidal gels.

  4. Final Report: Experimental and Theoretical Studies of Surface Oxametallacycles - Connections to Heterogeneous Olefin Epoxidation

    SciTech Connect (OSTI)

    Mark A. Barteau

    2009-09-15

    This project has aimed at the rational design of catalysts for direct epoxidation of olefins. This chemistry remains one of the most challenging problems in heterogeneous catalysis. Although the epoxidation of ethylene by silver catalysts to form ethylene oxide (EO) has been practiced for decades, little progress has been made in expanding this technology to other products and processes. We have made significant advances through the combination of surface science experiments, Density Functional Theory (DFT) calculations, and catalytic reactor experiments, toward understanding the mechanism of this reaction on silver catalysts, and to the rational improvement of selectivity. The key has been our demonstration of surface oxametallacycle intermediates as the species that control reaction selectivity. This discovery permits the influence of catalyst promoters on selectivity to be probed, and new catalyst formulations to be developed. It also guides the development of new chemistry with potential for direct epoxidation of more complex olefins. During the award period we have focused on 1. the formation and reaction selectivity of complex olefin epoxides on silver surfaces, and 2. the influence of co-adsorbed oxygen atoms on the reactions of surface oxametallacycles on silver, and 3. the computational prediction, synthesis, characterization and experimental evaluation of bimetallic catalysts for ethylene epoxidation. The significance of these research thrusts is as follows. Selective epoxidation of olefins more complex than ethylene requires suppression of not only side reactions available to the olefin such as C-H bond breaking, but it requires formation and selective ring closure of the corresponding oxametallacycle intermediates. The work carried out under this grant has significantly advanced the field of catalyst design from first principles. The combination of computational tools, surface science, and catalytic reactor experiments in a single laboratory has few other examples. We have successfully predicted and validated new bimetallic catalyst for ethylene epoxidation. In so doing, we have established one of the first examples of successful catalyst design from first principles to achieve improved reaction selectivity.

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

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

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

  6. Method of fabricating a homogeneous wire of inter-metallic alloy

    DOE Patents [OSTI]

    Ohriner, Evan Keith (Knoxville, TN); Blue, Craig Alan (Knoxville, TN)

    2001-01-01

    A method for fabricating a homogeneous wire of inter-metallic alloy comprising the steps of providing a base-metal wire bundle comprising a metal, an alloy or a combination thereof; working the wire bundle through at least one die to obtain a desired dimension and to form a precursor wire; and, controllably heating the precursor wire such that a portion of the wire will become liquid while simultaneously maintaining its desired shape, whereby substantial homogenization of the wire occurs in the liquid state and additional homogenization occurs in the solid state resulting in a homogenous alloy product.

  7. SU-E-T-76: Comparing Homogeneity Between Gafchromic Film EBT2 and EBT3

    Office of Scientific and Technical Information (OSTI)

    (Journal Article) | SciTech Connect SciTech Connect Search Results Journal Article: SU-E-T-76: Comparing Homogeneity Between Gafchromic Film EBT2 and EBT3 Citation Details In-Document Search Title: SU-E-T-76: Comparing Homogeneity Between Gafchromic Film EBT2 and EBT3 Purpose: We found out that homogeneity of EBT2 was different among lot numbers in previous study. Variation in local homogeneity of EBT3 among several lot numbers has not been reported. In this study, we investigated film

  8. High Efficiency, Low Emissions Homogeneous Charge Compression Ignition (HCCI) Engines

    SciTech Connect (OSTI)

    2011-01-31

    This is the final report of the High Efficiency Clean Combustion (HECC) Research Program for the U.S. Department of Energy. Work under this co-funded program began in August 2005 and finished in July 2010. The objective of this program was to develop and demonstrate a low emission, high thermal efficiency engine system that met 2010 EPA heavy-duty on-highway truck emissions requirements (0.2g/bhp-hr NOx, 0.14g/bhp-hr HC and 0.01g/bhp-hr PM) with a thermal efficiency of 46%. To achieve this goal, development of diesel homogenous charge compression ignition (HCCI) combustion was the chosen approach. This report summarizes the development of diesel HCCI combustion and associated enabling technologies that occurred during the HECC program between August 2005 and July 2010. This program showed that although diesel HCCI with conventional US diesel fuel was not a feasible means to achieve the program objectives, the HCCI load range could be increased with a higher volatility, lower cetane number fuel, such as gasoline, if the combustion rate could be moderated to avoid excessive cylinder pressure rise rates. Given the potential efficiency and emissions benefits, continued research of combustion with low cetane number fuels and the effects of fuel distillation are recommended. The operation of diesel HCCI was only feasible at part-load due to a limited fuel injection window. A 4% fuel consumption benefit versus conventional, low-temperature combustion was realized over the achievable operating range. Several enabling technologies were developed under this program that also benefited non-HCCI combustion. The development of a 300MPa fuel injector enabled the development of extended lifted flame combustion. A design methodology for minimizing the heat transfer to jacket water, known as precision cooling, will benefit conventional combustion engines, as well as HCCI engines. An advanced combustion control system based on cylinder pressure measurements was developed. A Well-to-wheels analysis of the energy flows in a mobile vehicle system and a 2nd Law thermodynamic analysis of the engine system were also completed under this program.

  9. Equilibrium and heat of adsorption of diethyl phthalate on heterogeneous adsorbents

    SciTech Connect (OSTI)

    Zhang, W.M.; Xu, Z.W.; Pan, B.C.; Hong, C.H.; Jia, K.; Jiang, P.J.; Zhang, Q.J.; Pan, B.J.

    2008-09-15

    Removal of phthalate esters from water has been of considerable concern recently. In the present study, the adsorptive removal performance of diethyl phthalate (DEP) from water was investigated with the aminated polystyrene resin (NDA-101) and oxidized polystyrene resin (NDA-702). In addition, the commercial homogeneous polystyrene resin (XAD-4) and acrylic ester resin (Amberlite XAD-7) as well as coal-based granular activated carbon (AC-750) were chosen for comparison. The corresponding equilibrium isotherms are well described by the Freundlich equation and the adsorption capacities for DEP followed the order NDA-702 > NDA-101 > AC-750 > XAD-4 > XAD-7. Analysis of adsorption mechanisms suggested that these adsorbents spontaneously adsorb DEP molecules driven mainly by enthalpy change, and the adsorption process was derived by multiple adsorbent-adsorbate interactions such as hydrogen bonding, {pi}-{pi} stacking, and micropore filling. The information related to the adsorbent surface heterogeneity and the adsorbate-adsorbate interaction was obtained by Do's model. All the results indicate that heterogeneous resins NDA-702 and NDA-101 have excellent potential as an adsorption material for the removal of DEP from the contaminated water.

  10. Effects of Porous Medium Heterogeneity on Vadose Zone Desiccation: Intermediate-scale Laboratory Experiments and Simulations

    SciTech Connect (OSTI)

    Oostrom, Martinus; Freedman, Vicky L.; Wietsma, Thomas W.; Dane, Jacob H.; Truex, Michael J.

    2012-11-01

    Soil desiccation (drying), involving water evaporation induced by dry gas injection, is a potentially robust vadose zone remediation process to limit contaminant transport through the vadose zone. A series of four intermediate-scale flow cell experiments was conducted in homogeneous and simple layered heterogeneous porous medium systems to investigate the effects of heterogeneity on desiccation of unsaturated porous media. The permeability ratios of porous medium layers ranged from about five to almost two orders of magnitude. The insulated flow cell was equipped with twenty humidity and temperature sensors and a dual-energy gamma system was used to determine water saturations at various times. The multiphase code STOMP was used to simulate the desiccation process. Results show that injected dry gas flowed predominantly in the higher permeability layer and delayed water removal from the lower permeability material. For the configurations tested, water vapor diffusion from the lower to the higher permeability zone was considerable over the duration of the experiments, resulting in much larger relative humidity values of the outgoing air than based on permeability ratios alone. Acceptable numerical matches with the experimental data were obtained when an extension of the saturation-capillary pressure relation below the residual water saturation was used. The agreements between numerical and experimental results suggest that the correct physics are implemented in the simulator and that the thermal and hydraulic properties of the porous media, flow cell wall and insulation materials were properly represented.

  11. Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K

    SciTech Connect (OSTI)

    Wang, Bingbing; Laskin, Alexander; Roedel, Tobias R.; Gilles, Marry K.; Moffet, Ryan C.; Tivanski, Alexei V.; Knopf, Daniel A.

    2012-09-25

    Atmospheric ice formation induced by particles with complex chemical and physical properties through heterogeneous nucleation is not well understood. Heterogeneous ice nucleation and water uptake by ambient particles collected from urban environments in Los Angeles and Mexico City are presented. Using a vapour controlled cooling system equipped with an optical microscopy, the range of onset conditions for ice nucleation and water uptake by the collected particles was determined as a function of temperature (200{273 K) and relative humidity with respect to ice (RHice) up to water saturation. Three distinctly different types of authentic atmospheric particles were investigated including soot particles associated with organics/inorganics, inorganic particles of marine origin coated with organic material, and Pb/Zn containing inorganic particles apportioned to anthropogenic emissions relevant to waste incineration. Single particle characterization was provided by micro-spectroscopic analyses using computer controlled scanning electron microscopy with energy dispersive analysis of X-rays (CCSEM/EDX) and scanning transmission X-ray microscopy with near edge X-ray absorption ne structure spectroscopy (STXM/NEXAFS). Above 230 K, signicant differences in water uptake and immersion freezing effciencies of the different particle types were observed. Below 230 K, the particles exhibited high deposition ice nucleation effciencies and formed ice at RHice values well below homogeneous ice nucleation limits. The data show that the chemical composition of these eld{collected particles plays an important role in determining water uptake and immersion freezing. Heterogeneous ice nucleation rate coeffcients, cumulative ice nuclei (IN) spectrum, and IN activated fraction for deposition ice nucleation are derived. The presented ice nucleation data demonstrate that anthropogenic and marine particles comprising of various chemical and physical properties exhibit distinctly different ice nucleation effciencies and can serve as effcient IN at atmospheric conditions typical for cirrus and mixed phase clouds. This indicates a potential link between human activities and cloud formation, and thus climate.

  12. Simulation of CO2 Sequestration at Rock Spring Uplift, Wyoming: Heterogeneity and Uncertainties in Storage Capacity, Injectivity and Leakage

    SciTech Connect (OSTI)

    Deng, Hailin; Dai, Zhenxue; Jiao, Zunsheng; Stauffer, Philip H.; Surdam, Ronald C.

    2011-01-01

    Many geological, geochemical, geomechanical and hydrogeological factors control CO{sub 2} storage in subsurface. Among them heterogeneity in saline aquifer can seriously influence design of injection wells, CO{sub 2} injection rate, CO{sub 2} plume migration, storage capacity, and potential leakage and risk assessment. This study applies indicator geostatistics, transition probability and Markov chain model at the Rock Springs Uplift, Wyoming generating facies-based heterogeneous fields for porosity and permeability in target saline aquifer (Pennsylvanian Weber sandstone) and surrounding rocks (Phosphoria, Madison and cap-rock Chugwater). A multiphase flow simulator FEHM is then used to model injection of CO{sub 2} into the target saline aquifer involving field-scale heterogeneity. The results reveal that (1) CO{sub 2} injection rates in different injection wells significantly change with local permeability distributions; (2) brine production rates in different pumping wells are also significantly impacted by the spatial heterogeneity in permeability; (3) liquid pressure evolution during and after CO{sub 2} injection in saline aquifer varies greatly for different realizations of random permeability fields, and this has potential important effects on hydraulic fracturing of the reservoir rock, reactivation of pre-existing faults and the integrity of the cap-rock; (4) CO{sub 2} storage capacity estimate for Rock Springs Uplift is 6614 {+-} 256 Mt at 95% confidence interval, which is about 36% of previous estimate based on homogeneous and isotropic storage formation; (5) density profiles show that the density of injected CO{sub 2} below 3 km is close to that of the ambient brine with given geothermal gradient and brine concentration, which indicates CO{sub 2} plume can sink to the deep before reaching thermal equilibrium with brine. Finally, we present uncertainty analysis of CO{sub 2} leakage into overlying formations due to heterogeneity in both the target saline aquifer and surrounding formations. This uncertainty in leakage will be used to feed into risk assessment modeling.

  13. Damping of linear waves via ionization and recombination in homogeneous plasmas

    SciTech Connect (OSTI)

    Dodin, I. Y.; Fisch, N. J.

    2010-11-15

    An oscillation-center model is proposed that analytically describes transformation of an arbitrary homogeneous linear wave at gradual ionization and recombination in homogeneous plasma. For the case when either of the processes dominates, general adiabatic invariants are found, from which the wave energy is derived as a function of the frequency.

  14. Homogeneous, dual layer, solid state, thin film deposition for structural and/or electrochemical characteristics

    DOE Patents [OSTI]

    Pitts, J. Roland; Lee, Se-Hee; Tracy, C. Edwin; Li, Wenming

    2014-04-08

    Solid state, thin film, electrochemical devices (10) and methods of making the same are disclosed. An exemplary device 10 includes at least one electrode (14) and an electrolyte (16) deposited on the electrode (14). The electrolyte (16) includes at least two homogenous layers of discrete physical properties. The two homogenous layers comprise a first dense layer (15) and a second porous layer (16).

  15. Structures of trihydroxynaphthalene reductase-fungicide complexes: implications for structure-based design and catalysis

    SciTech Connect (OSTI)

    Liao, D.-I.; Basarab, G.S.; Gatenby, A.A.; Valent, B.; Jordan, D.B.

    2010-03-08

    Trihydroxynaphthalene reductase catalyzes two intermediate steps in the fungal melanin biosynthetic pathway. The enzyme, a typical short-chain dehydrogenase, is the biochemical target of three commercial fungicides. The fungicides bind preferentially to the NADPH form of the enzyme. Three X-ray structures of the Magnaporthe grisea enzyme complexed with NADPH and two commercial and one experimental fungicide were determined at 1.7 {angstrom} (pyroquilon), 2.0 {angstrom} (2,3-dihydro-4-nitro-1H-inden-1-one, 1), and 2.1 {angstrom} (phthalide) resolutions. The chemically distinct inhibitors occupy similar space within the enzyme's active site. The three inhibitors share hydrogen bonds with the side chain hydroxyls of Ser-164 and Tyr-178 via a carbonyl oxygen (pyroquilon and 1) or via a carbonyl oxygen and a ring oxygen (phthalide). Active site residues occupy similar positions among the three structures. A buried water molecule that is hydrogen bonded to the NZ nitrogen of Lys-182 in each of the three structures likely serves to stabilize the cationic form of the residue for participation in catalysis. The pro S hydrogen of NADPH (which is transferred as a hydride to the enzyme's naphthol substrates) is directed toward the carbonyl carbon of the inhibitors that mimic an intermediate along the reaction coordinate. Modeling tetrahydroxynaphthalene and trihydroxynaphthalene in the active site shows steric and electrostatic repulsion between the extra hydroxyl oxygen of the former substrate and the sulfur atom of Met-283 (the C-terminal residue), which accounts, in part, for the 4-fold greater substrate specificity for trihydroxynaphthalene over tetrahydroxynaphthalene.

  16. Heterogeneous Catalyst for Improved Selectivity of Biomass-Derived

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

    Molecules - Energy Innovation Portal Biomass and Biofuels Biomass and Biofuels Advanced Materials Advanced Materials Find More Like This Return to Search Heterogeneous Catalyst for Improved Selectivity of Biomass-Derived Molecules University of Colorado Contact CU About This Technology Publications: PDF Document Publication CU2380B (Heterogenous Catalyst) Marketing Summary (137 KB) Technology Marketing Summary In today's industrial processes, heterogeneous catalysts are widely used because

  17. Assessing the relative permeability of heterogeneous reservoir rock

    Office of Scientific and Technical Information (OSTI)

    (Conference) | SciTech Connect Conference: Assessing the relative permeability of heterogeneous reservoir rock Citation Details In-Document Search Title: Assessing the relative permeability of heterogeneous reservoir rock Reservoir engineers are often faced with heterogeneous core material, for which conventional methods of estimating relative permeability are susceptible to error and may lead to incorrect conclusions regarding displacement efficiency, wettability and reservoir performance.

  18. Effect of heterogeneous aqueous reactions on the secondary formation of

    Office of Scientific and Technical Information (OSTI)

    inorganic aerosols during haze events (Journal Article) | SciTech Connect Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events Citation Details In-Document Search This content will become publicly available on September 30, 2016 Title: Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events In this study, the effect of heterogeneous aqueous reactions on the secondary formation of

  19. Dynamics on modular networks with heterogeneous correlations

    SciTech Connect (OSTI)

    Melnik, Sergey; Oxford Centre for Industrial and Applied Mathematics, Mathematical Institute, University of Oxford, Oxford OX2 6GG; CABDyN Complexity Centre, University of Oxford, Oxford OX1 1HP ; Porter, Mason A.; CABDyN Complexity Centre, University of Oxford, Oxford OX1 1HP ; Mucha, Peter J.; Institute for Advanced Materials, Nanoscience and Technology, University of North Carolina, Chapel Hill, North Carolina 27599-3216 ; Gleeson, James P.

    2014-06-15

    We develop a new ensemble of modular random graphs in which degree-degree correlations can be different in each module, and the inter-module connections are defined by the joint degree-degree distribution of nodes for each pair of modules. We present an analytical approach that allows one to analyze several types of binary dynamics operating on such networks, and we illustrate our approach using bond percolation, site percolation, and the Watts threshold model. The new network ensemble generalizes existing models (e.g., the well-known configuration model and Lancichinetti-Fortunato-Radicchi networks) by allowing a heterogeneous distribution of degree-degree correlations across modules, which is important for the consideration of nonidentical interacting networks.

  20. Comprehensive Monitoring for Heterogeneous Geographically Distributed Storage

    SciTech Connect (OSTI)

    Ratnikova, N.; Karavakis, E.; Lammel, S.; Wildish, T.

    2015-12-23

    Storage capacity at CMS Tier-1 and Tier-2 sites reached over 100 Petabytes in 2014, and will be substantially increased during Run 2 data taking. The allocation of storage for the individual users analysis data, which is not accounted as a centrally managed storage space, will be increased to up to 40%. For comprehensive tracking and monitoring of the storage utilization across all participating sites, CMS developed a space monitoring system, which provides a central view of the geographically dispersed heterogeneous storage systems. The first prototype was deployed at pilot sites in summer 2014, and has been substantially reworked since then. In this paper we discuss the functionality and our experience of system deployment and operation on the full CMS scale.

  1. INITIAL ANALYSIS OF TRANSIENT POWER TIME LAG DUE TO HETEROGENEITY WITHIN THE TREAT FUEL MATRIX.

    SciTech Connect (OSTI)

    D.M. Wachs; A.X. Zabriskie, W.R. Marcum

    2014-06-01

    The topic Nuclear Safety encompasses a broad spectrum of focal areas within the nuclear industry; one specific aspect centers on the performance and integrity of nuclear fuel during a reactivity insertion accident (RIA). This specific accident has proven to be fundamentally difficult to theoretically characterize due to the numerous empirically driven characteristics that quantify the fuel and reactor performance. The Transient Reactor Test (TREAT) facility was designed and operated to better understand fuel behavior under extreme (i.e. accident) conditions; it was shutdown in 1994. Recently, efforts have been underway to commission the TREAT facility to continue testing of advanced accident tolerant fuels (i.e. recently developed fuel concepts). To aid in the restart effort, new simulation tools are being used to investigate the behavior of nuclear fuels during facility’s transient events. This study focuses specifically on the characterizing modeled effects of fuel particles within the fuel matrix of the TREAT. The objective of this study was to (1) identify the impact of modeled heterogeneity within the fuel matrix during a transient event, and (2) demonstrate acceptable modeling processes for the purpose of TREAT safety analyses, specific to fuel matrix and particle size. Hypothetically, a fuel that is dominantly heterogeneous will demonstrate a clearly different temporal heating response to that of a modeled homogeneous fuel. This time difference is a result of the uniqueness of the thermal diffusivity within the fuel particle and fuel matrix. Using MOOSE/BISON to simulate the temperature time-lag effect of fuel particle diameter during a transient event, a comparison of the average graphite moderator temperature surrounding a spherical particle of fuel was made for both types of fuel simulations. This comparison showed that at a given time and with a specific fuel particle diameter, the fuel particle (heterogeneous) simulation and the homogeneous simulation were related by a multiplier relative to the average moderator temperature. As time increases the multiplier is comparable to the factor found in a previous analytical study from literature. The implementation of this multiplier and the method of analysis may be employed to remove assumptions and increase fidelity for future research on the effect of fuel particles during transient events.

  2. Accelerating Subsurface Transport Simulation on Heterogeneous Clusters

    SciTech Connect (OSTI)

    Villa, Oreste; Gawande, Nitin A.; Tumeo, Antonino

    2013-09-23

    Reactive transport numerical models simulate chemical and microbiological reactions that occur along a flowpath. These models have to compute reactions for a large number of locations. They solve the set of ordinary differential equations (ODEs) that describes the reaction for each location through the Newton-Raphson technique. This technique involves computing a Jacobian matrix and a residual vector for each set of equation, and then solving iteratively the linearized system by performing Gaussian Elimination and LU decomposition until convergence. STOMP, a well known subsurface flow simulation tool, employs matrices with sizes in the order of 100x100 elements and, for numerical accuracy, LU factorization with full pivoting instead of the faster partial pivoting. Modern high performance computing systems are heterogeneous machines whose nodes integrate both CPUs and GPUs, exposing unprecedented amounts of parallelism. To exploit all their computational power, applications must use both the types of processing elements. For the case of subsurface flow simulation, this mainly requires implementing efficient batched LU-based solvers and identifying efficient solutions for enabling load balancing among the different processors of the system. In this paper we discuss two approaches that allows scaling STOMP's performance on heterogeneous clusters. We initially identify the challenges in implementing batched LU-based solvers for small matrices on GPUs, and propose an implementation that fulfills STOMP's requirements. We compare this implementation to other existing solutions. Then, we combine the batched GPU solver with an OpenMP-based CPU solver, and present an adaptive load balancer that dynamically distributes the linear systems to solve between the two components inside a node. We show how these approaches, integrated into the full application, provide speed ups from 6 to 7 times on large problems, executed on up to 16 nodes of a cluster with two AMD Opteron 6272 and a Tesla M2090 per node.

  3. Performance Modeling for 3D Visualization in a Heterogeneous...

    Office of Scientific and Technical Information (OSTI)

    The analytic models are shown to be accurate on a testbed of distributed heterogeneous systems. The prediction methodology will form the foundation of a more robust resource ...

  4. Plane wave method for elastic wave scattering by a heterogeneous...

    Office of Scientific and Technical Information (OSTI)

    Plane wave method for elastic wave scattering by a heterogeneous fracture Citation Details In-Document Search Title: Plane wave method for elastic wave scattering by a ...

  5. Opportunities for Catalysis in The 21st Century. A report from the Basic Energy Sciences Advisory Committee

    SciTech Connect (OSTI)

    White, J. M.; Bercaw, J.

    2002-05-16

    Chemical catalysis affects our lives in myriad ways. Catalysis provides a means of changing the rates at which chemical bonds are formed and broken and of controlling the yields of chemical reactions to increase the amounts of desirable products from these reactions and reduce the amounts of undesirable ones. Thus, it lies at the heart of our quality of life: The reduced emissions of modern cars, the abundance of fresh food at our stores, and the new pharmaceuticals that improve our health are made possible by chemical reactions controlled by catalysts. Catalysis is also essential to a healthy economy: The petroleum, chemical, and pharmaceutical industries, contributors of $500 billion to the gross national product of the United States, rely on catalysts to produce everything from fuels to ''wonder drugs'' to paints to cosmetics. Today, our Nation faces a variety of challenges in creating alternative fuels, reducing harmful by-products in manufacturing, cleaning up the environment and preventing future pollution, dealing with the causes of global warming, protecting citizens from the release of toxic substances and infectious agents, and creating safe pharmaceuticals. Catalysts are needed to meet these challenges, but their complexity and diversity demand a revolution in the way catalysts are designed and used. This revolution can become reality through the application of new methods for synthesizing and characterizing molecular and material systems. Opportunities to understand and predict how catalysts work at the atomic scale and the nanoscale are now appearing, made possible by breakthroughs in the last decade in computation, measurement techniques, and imaging and by new developments in catalyst design, synthesis, and evaluation.

  6. Contact: Paul Dauenhauer (hauer@umn.edu) UD's Catalysis Center for Energy Innovation Invents New Chemical Detector

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

    Information Contact (If you're a human, don't change the following field) Enter your name: 8c7f598568c7f Your first name. Please enable Javascript to use this form. Your name: * Your e-mail address: * Subject: * Category: * - Please choose - STIP Website Subscribe to the OSTI.gov Newsletter Message: * Send message

    immediate release Contact: Paul Dauenhauer (hauer@umn.edu) UD's Catalysis Center for Energy Innovation Invents New Chemical Detector (NEWARK, DE) January 12, 2015 -- A team of

  7. Support for Speakers and Attendees at 2008 GRC Conference Catalysis (to be held at Colby Sawyer College, New London, New Hampshire on June 22-27, 2008)

    SciTech Connect (OSTI)

    Stuart L. Soled and Nancy Ryan Gray

    2009-01-01

    The GRC on Catalysis is one of the most prestigious catalysis conferences as it brings together leading researchers from around the world to discuss their latest, most exciting work in catalysis. The 2008 conference will continue this tradition. The conference will cover a variety of themes including new catalytic materials, theoretical and experimental approaches to improve understanding of kinetics and transport phenomena, and state of the art nanoscale characterization probes to monitor active sites. The conference promotes interactions among established researchers and young scientists. It provides a venue for students to meet, talk to and learn from some of the world leading researchers in the area. It also gives them a platform for displaying their own work during the poster sessions. The informal nature of the meeting, excellent quality of the presentations and posters, and ability to meet many outstanding colleagues makes this an excellent conference.

  8. Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials

    SciTech Connect (OSTI)

    Beale, Andrew M.; Gao, Feng; Lezcano-Gonzalez, Ines; Peden, Charles HF; Szanyi, Janos

    2015-10-05

    The ever increasing demand to develop highly fuel efficient engines coincides with the need to minimize air pollution originating from the exhaust gases of internal combustion engines. Dramatically improved fuel efficiency can be achieved at air-to-fuel ratios much higher than stoichiometric. In the presence of oxygen in large excess, however, traditional three-way catalysts are unable to reduce NOx. Among the number of lean-NOx reduction technologies, selective catalytic reduction (SCR) of NOx by NH3 over Cu- and Fe-ion exchanged zeolite catalysts has been extensively studied over the past 30+ years. Despite the significant advances in developing a viable practical zeolite-based catalyst for lean NOx reduction, the insufficient hydrothermal stabilities of the zeolite structures considered cast doubts about their real-world applicability. During the past decade a renewed interest in zeolite-based lean NOx reduction was spurred by the discovery of the very high activity of Cu-SSZ-13 (and the isostructural Cu-SAPO-34) in the NH3 SCR of NOx. These new, small-pore zeolite-based catalysts not only exhibited very high NOx conversion and N2 selectivity, but also exhibited exceptional high hydrothermal stability at high temperatures. In this review we summarize the key discoveries of the past ~5 years that lead to the introduction of these catalysts into practical application. The review first briefly discusses the structure and preparation of the CHA structure-based zeolite catalysts, and then summarizes the key learnings of the rather extensive (but not complete) characterisation work. Then we summarize the key findings of reaction kinetics studies, and provide some mechanistic details emerging from these investigations. At the end of the review we highlight some of the issues that are still need to be addressed in automotive exhaust control catalysis. Funding A.M.B. and I.L.G. would like to thank EPSRC for funding. F.G., C.H.F.P. and J.Sz. gratefully acknowledge financial support from the US Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program.

  9. Coordinated Collaboration between Heterogeneous Distributed Energy Resources

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

    Abdollahy, Shahin; Lavrova, Olga; Mammoli, Andrea

    2014-01-01

    A power distribution feeder, where a heterogeneous set of distributed energy resources is deployed, is examined by simulation. The energy resources include PV, battery storage, natural gas GenSet, fuel cells, and active thermal storage for commercial buildings. The resource scenario considered is one that may exist in a not too distant future. Two cases of interaction between different resources are examined. One interaction involves a GenSet used to partially offset the duty cycle of a smoothing battery connected to a large PV system. The other example involves the coordination of twenty thermal storage devices, each associated with a commercial building.more » Storage devices are intended to provide maximum benefit to the building, but it is shown that this can have a deleterious effect on the overall system, unless the action of the individual storage devices is coordinated. A network based approach is also introduced to calculate some type of effectiveness metric to all available resources which take part in coordinated operation. The main finding is that it is possible to achieve synergy between DERs on a system; however this required a unified strategy to coordinate the action of all devices in a decentralized way.« less

  10. Organo-Lewis acid as cocatalyst for cationic homogenous metallocene Ziegler-Natta olefin polymerizations

    DOE Patents [OSTI]

    Marks, Tobin J.; Chen, You-Xian

    2000-01-01

    The synthesis of the organo-Lewis acid perfluorobiphenylborane (PBB) and the activation of metallocenes for the formation of a variety of highly active homogeneous Ziegler-Natta metallocene olefin polymerization, copolymerization and ring-opening polymerization catalysts is described.

  11. SU-E-T-76: Comparing Homogeneity Between Gafchromic Film EBT2...

    Office of Scientific and Technical Information (OSTI)

    SciTech Connect Search Results Journal Article: SU-E-T-76: Comparing Homogeneity Between Gafchromic Film EBT2 and EBT3 Citation Details In-Document Search Title: SU-E-T-76: ...

  12. A novel approach to make homogeneous protease-stable monovalent streptavidin

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

    Zhang, M.; Shao, J; Xiao, J.; Deng, W.; Yu, H.

    2015-06-11

    The interaction between the tetramer streptavidin and biotin is recognized as one of the strongest non-covalent associations. Owing to the tight and specific binding, the streptavidin-biotin system has been used widely for bimolecular labeling, purification, immobilization, and even for targeted delivery of therapeutics drugs. Here, we report a novel approach to make homogeneous monovalent tetramer streptavidin. The purified monovalent protein showed both thermal stability and protease stability. Unexpectedly, we found that two proteases, Proteinase K (PK) and Subtilisin (SU), can efficiently remove the His8-tag from the wild-type subunit without affecting the tetramer architecture of monovalent streptavidin, thus making it moremore » homogeneous. In addition, crystallization was performed to assure the homogeneity of the monovalent protein prepared. Overall, monovalent streptavidin shows increased homogeneity and will likely be valuable for many future applications in a wide range of research areas.« less

  13. Direct current dielectric barrier assistant discharge to get homogeneous plasma in capacitive coupled discharge

    SciTech Connect (OSTI)

    Du, Yinchang; Li, Yangfang; Cao, Jinxiang; Liu, Yu; Wang, Jian; Zheng, Zhe

    2014-06-15

    In this paper, we propose a method to get more homogeneous plasma in the geometrically asymmetric capacitive coupled plasma (CCP) discharge. The dielectric barrier discharge (DBD) is used for the auxiliary discharge system to improve the homogeneity of the geometrically asymmetric CCP discharge. The single Langmuir probe measurement shows that the DBD can increase the electron density in the low density volume, where the DBD electrodes are mounted, when the pressure is higher than 5?Pa. By this manner, we are able to improve the homogeneity of the plasma production and increase the overall density in the target volume. At last, the finite element simulation results show that the DC bias, applied to the DBD electrodes, can increase the homogeneity of the electron density in the CCP discharge. The simulation results show a good agreement with the experiment results.

  14. New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven

    Office of Scientific and Technical Information (OSTI)

    Reduction of Carbon Dioxide (Technical Report) | SciTech Connect New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven Reduction of Carbon Dioxide Citation Details In-Document Search Title: New Homogeneous Chromophore/Catalyst Concepts for the Solar-Driven Reduction of Carbon Dioxide One of the major scientific and technical challenges of this century is to develop chemical means to store solar energy in the form of fuels. This can be accomplished by developing light-absorbing

  15. Simultaneous dual mode combustion engine operating on spark ignition and homogenous charge compression ignition

    DOE Patents [OSTI]

    Fiveland, Scott B.; Wiggers, Timothy E.

    2004-06-22

    An engine particularly suited to single speed operation environments, such as stationary power generators. The engine includes a plurality of combustion cylinders operable under homogenous charge compression ignition, and at least one combustion cylinder operable on spark ignition concepts. The cylinder operable on spark ignition concepts can be convertible to operate under homogenous charge compression ignition. The engine is started using the cylinders operable under spark ignition concepts.

  16. SU-E-J-63: Estimating the Effects of Respiratory Motion On Dose Heterogeneity for ITV-Based Treatments

    SciTech Connect (OSTI)

    Williams, C; Lewis, J

    2014-06-01

    Purpose: To quantify the relationship between the amount of dose heterogeneity in a treatment plan that uses an internal target volume (ITV) to account for respiratory motion and the true amount of heterogeneity in the dose delivered to the tumor contained within that ITV. Methods: We develop a convolution-based framework for calculating dose delivered to a tumor moving inside an ITV according to a common sinusoid-based breathing model including asymmetry. We model the planned ITV dose distribution as a centrally peaked analytic function approximating the profile of clinical stereotactic body radiotherapy treatments. Expressions for the minimum and maximum dose received by the tumor are derived and evaluated for a range of clinically relevant parameters. Results of the model are validated with phantom measurements using an ion chamber array. Results: An analytic expression is presented for the maximum and minimum doses received by the tumor relative to the planned ITV dose. The tumor dose heterogeneity depends solely on the ratio of tumor size to ITV size, the peak dose in the planned ITV dose distribution, and the respiratory asymmetry parameter. Under the assumptions of this model, using a typical breathing asymmetry parameter and a dose distribution with a fixed size ITV covered by the 100% line and with a 130% hotspot, the maximum dose to the tumor varies between 113%130%, and the minimum dose varies between 100%116% depending on the amount of tumor motion. Conclusion: This modeling exercise demonstrates the interplay between motion and dose heterogeneity. Tumors that exhibit large amounts of respiratory motion relative to their size will receive a more homogeneous dose and a larger minimum dose than would be inferred from the ITV dose distribution. This effect is not captured in current clinical treatment planning methods unless 4D dose calculation techniques are used. This work was partially supported by a Varian Medical Systems research grant.

  17. Effects of H{sub 2}O, SO{sub 2}, and NO on homogeneous Hg oxidation...

    Office of Scientific and Technical Information (OSTI)

    Effects of Hsub 2O, SOsub 2, and NO on homogeneous Hg oxidation by Clsub 2 Citation Details In-Document Search Title: Effects of Hsub 2O, SOsub 2, and NO on homogeneous Hg ...

  18. FY16 SBIR Phase II Release 1 Awards Announced: Includes Hydrogen Contaminants Detection, Fuel Cell and Hydrogen Catalysis, and Alkaline Membrane Electrolysis

    Broader source: Energy.gov [DOE]

    The Energy Department has announced the 2016 Small Business Innovation Research and Small Business Technology Transfer (SBIR/STTR) Phase II Release 1 awards, including three projects focused on catalysis for fuel cell and hydrogen production as well as hydrogen contaminants detection.

  19. An Innovative Three-Dimensional Heterogeneous Coarse-Mesh Transport Method for Advanced and Generation IV Reactor Core Analysis and Design

    SciTech Connect (OSTI)

    Farzad Rahnema

    2009-11-12

    This project has resulted in a highly efficient method that has been shown to provide accurate solutions to a variety of 2D and 3D reactor problems. The goal of this project was to develop (1) an accurate and efficient three-dimensional whole-core neutronics method with the following features: based sollely on transport theory, does not require the use of cross-section homogenization, contains a highly accurate and self-consistent global flux reconstruction procedure, and is applicable to large, heterogeneous reactor models, and to (2) create new numerical benchmark problems for code cross-comparison.

  20. Experimental investigation of supercritical CO2 trapping mechanisms at the Intermediate Laboratory Scale in well-defined heterogeneous porous media

    SciTech Connect (OSTI)

    Trevisan, Luca; Pini, Ronny; Cihan, Abdullah; Birkholzer, Jens T.; Zhou, Quanlin; Illangasekare, Tissa H.

    2014-12-31

    The heterogeneous nature of typical sedimentary formations can play a major role in the propagation of the CO2 plume, eventually dampening the accumulation of mobile phase underneath the caprock. From core flooding experiments, it is also known that contrasts in capillary threshold pressure due to different pore size can affect the flow paths of the invading and displaced fluids and consequently influence the build- up of non-wetting phase (NWP) at interfaces between geological facies. The full characterization of the geologic variability at all relevant scales and the ability to make observations on the spatial and temporal distribution of the migration and trapping of supercritical CO2 is not feasible from a practical perspective. To provide insight into the impact of well-defined heterogeneous systems on the flow dynamics and trapping efficiency of supercritical CO2 under drainage and imbibition conditions, we present an experimental investigation at the meter scale conducted in synthetic sand reservoirs packed in a quasi-two-dimensional flow-cell. Two immiscible displacement experiments have been performed to observe the preferential entrapment of NWP in simple heterogeneous porous media. The experiments consisted of an injection, a fluid redistribution, and a forced imbibition stages conducted in an uncorrelated permeability field and a homogeneous base case scenario. We adopted x-ray attenuation analysis as a non-destructive technique that allows a precise measurement of phase saturations throughout the entire flow domain. By comparing a homogeneous and a heterogeneous scenario we have identified some important effects that can be attributed to capillary barriers, such as dampened plume advancement, higher non-wetting phase saturations, larger contact area between the injected and displaced phases, and a larger range of non-wetting phase saturations.

  1. Discrete Feature Approach for Heterogeneous Reservoir Production Enhancement

    SciTech Connect (OSTI)

    Dershowitz, William S.; Curran, Brendan; Einstein, Herbert; LaPointe, Paul; Shuttle, Dawn; Klise, Kate

    2002-07-26

    The report presents summaries of technology development for discrete feature modeling in support of the improved oil recovery (IOR) for heterogeneous reservoirs. In addition, the report describes the demonstration of these technologies at project study sites.

  2. Ganglion dynamics of Supercritical CO2 in heterogeneous media. (Conference)

    Office of Scientific and Technical Information (OSTI)

    | SciTech Connect Ganglion dynamics of Supercritical CO2 in heterogeneous media. Citation Details In-Document Search Title: Ganglion dynamics of Supercritical CO2 in heterogeneous media. Abstract not provided. Authors: Wang, Yifeng Publication Date: 2015-04-01 OSTI Identifier: 1247107 Report Number(s): SAND2015-2548C 579865 DOE Contract Number: AC04-94AL85000 Resource Type: Conference Resource Relation: Conference: Proposed for presentation at the CFSES Carbon Sequestration PI meetings held

  3. Hot spot-derived shock initiation phenomena in heterogeneous nitromethane

    Office of Scientific and Technical Information (OSTI)

    (Conference) | SciTech Connect Conference: Hot spot-derived shock initiation phenomena in heterogeneous nitromethane Citation Details In-Document Search Title: Hot spot-derived shock initiation phenomena in heterogeneous nitromethane The addition of solid silica particles to gelled nitromethane offers a tractable model system for interrogating the role of impedance mismatches as one type of hot spot 'seed' on the initiation behaviors of explosive formulations. Gas gun-driven plate impact

  4. Performance Modeling for 3D Visualization in a Heterogeneous Computing

    Office of Scientific and Technical Information (OSTI)

    Environment (Technical Report) | SciTech Connect Performance Modeling for 3D Visualization in a Heterogeneous Computing Environment Citation Details In-Document Search Title: Performance Modeling for 3D Visualization in a Heterogeneous Computing Environment The visualization of large, remotely located data sets necessitates the development of a distributed computing pipeline in order to reduce the data, in stages, to a manageable size. The required baseline infrastructure for launching such

  5. The Role of Solvent Heterogeneity in Determining the Dispersion Interaction

    Office of Scientific and Technical Information (OSTI)

    Between Nanoassemblies (Journal Article) | SciTech Connect The Role of Solvent Heterogeneity in Determining the Dispersion Interaction Between Nanoassemblies Citation Details In-Document Search Title: The Role of Solvent Heterogeneity in Determining the Dispersion Interaction Between Nanoassemblies Understanding fundamental nanoassembly processes on intermediate scales beween the molecular and the continuum requires an in-depth analysis of the coupling between particle interactions and

  6. Chemical Heterogeneity of a Large Cluster CP IDP: Clues to its...

    Office of Scientific and Technical Information (OSTI)

    SciTech Connect Search Results Conference: Chemical Heterogeneity of a Large Cluster CP ... Citation Details In-Document Search Title: Chemical Heterogeneity of a Large Cluster CP ...

  7. Operando X-ray absorption and EPR evidence for a single electron redox process in copper catalysis

    SciTech Connect (OSTI)

    Lu, Qingquan; Zhang, Jian; Peng, Pan; Zhang, Guanghui; Huang, Zhiliang; Yi, Hong; Miller, Jeffrey T.; Lei, Aiwen

    2015-05-26

    An unprecedented single electron redox process in copper catalysis is confirmed using operando X-ray absorption and EPR spectroscopies. The oxidation state of the copper species in the interaction between Cu(II) and a sulfinic acid at room temperature, and the accurate characterization of the formed Cu(I) are clearly shown using operando X-ray absorption and EPR evidence. Further investigation of anion effects on Cu(II) discloses that bromine ions can dramatically increase the rate of the redox process. Moreover, it is proven that the sulfinic acids are converted into sulfonyl radicals, which can be trapped by 2-arylacrylic acids and various valuable β-keto sulfones are synthesized with good to excellent yields under mild conditions.

  8. Operando X-ray absorption and EPR evidence for a single electron redox process in copper catalysis

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

    Lu, Qingquan; Zhang, Jian; Peng, Pan; Zhang, Guanghui; Huang, Zhiliang; Yi, Hong; Miller, Jeffrey T.; Lei, Aiwen

    2015-05-26

    An unprecedented single electron redox process in copper catalysis is confirmed using operando X-ray absorption and EPR spectroscopies. The oxidation state of the copper species in the interaction between Cu(II) and a sulfinic acid at room temperature, and the accurate characterization of the formed Cu(I) are clearly shown using operando X-ray absorption and EPR evidence. Further investigation of anion effects on Cu(II) discloses that bromine ions can dramatically increase the rate of the redox process. Moreover, it is proven that the sulfinic acids are converted into sulfonyl radicals, which can be trapped by 2-arylacrylic acids and various valuable β-keto sulfonesmore » are synthesized with good to excellent yields under mild conditions.« less

  9. Crystal Structure of 12-Lipoxygenase Catalytic-Domain-Inhibitor Complex Identifies a Substrate-Binding Channel for Catalysis

    SciTech Connect (OSTI)

    Xu, Shu; Mueser, Timothy C.; Marnett, Lawrence J.; Funk, Jr., Max O.

    2014-10-02

    Lipoxygenases are critical enzymes in the biosynthesis of families of bioactive lipids including compounds with important roles in the initiation and resolution of inflammation and in associated diseases such as diabetes, cardiovascular disease, and cancer. Crystals diffracting to high resolution (1.9 {angstrom}) were obtained for a complex between the catalytic domain of leukocyte 12-lipoxygenase and the isoform-specific inhibitor, 4-(2-oxapentadeca-4-yne)phenylpropanoic acid (OPP). In the three-dimensional structure of the complex, the inhibitor occupied a new U-shaped channel open at one end to the surface of the protein and extending past the redox-active iron site that is essential for catalysis. In models, the channel accommodated arachidonic acid, defining the binding site for the substrate of the catalyzed reaction. There was a void adjacent to the OPP binding site connecting to the surface of the enzyme and providing a plausible access channel for the other substrate, oxygen.

  10. Point matching: A new electronic method for homogenizing the phase characteristics of giant magnetoimpedance sensors

    SciTech Connect (OSTI)

    Silva, E. Costa Gusmo, L. A. P.; Barbosa, C. R. Hall; Leipner, Y.; Fortaleza, L. G. S.; Monteiro, E. Costa

    2014-08-15

    Recently, our research group at PUC-Rio discovered that magnetic transducers based on the impedance phase characteristics of GMI sensors have the potential to multiply by one hundred the sensitivity values when compared to magnitude-based GMI transducers. Those GMI sensors can be employed in the measurement of ultra-weak magnetic fields, which intensities are even lower than the environmental magnetic noise. A traditional solution for cancelling the electromagnetic noise and interference makes use of gradiometric configurations, but the performance is strongly tied to the homogeneity of the sensing elements. This paper presents a new method that uses electronic circuits to modify the equivalent impedance of the GMI samples, aiming at homogenizing their phase characteristics and, consequently, improving the performance of gradiometric configurations based on GMI samples. It is also shown a performance comparison between this new method and another homogenization method previously developed.

  11. Homogenous charge compression ignition engine having a cylinder including a high compression space

    DOE Patents [OSTI]

    Agama, Jorge R.; Fiveland, Scott B.; Maloney, Ronald P.; Faletti, James J.; Clarke, John M.

    2003-12-30

    The present invention relates generally to the field of homogeneous charge compression engines. In these engines, fuel is injected upstream or directly into the cylinder when the power piston is relatively close to its bottom dead center position. The fuel mixes with air in the cylinder as the power piston advances to create a relatively lean homogeneous mixture that preferably ignites when the power piston is relatively close to the top dead center position. However, if the ignition event occurs either earlier or later than desired, lowered performance, engine misfire, or even engine damage, can result. Thus, the present invention divides the homogeneous charge between a controlled volume higher compression space and a lower compression space to better control the start of ignition.

  12. Enhancement of crystal homogeneity of protein crystals under application of an external alternating current electric field

    SciTech Connect (OSTI)

    Koizumi, H.; Uda, S.; Fujiwara, K.; Nozawa, J.; Tachibana, M.; Kojima, K.

    2014-10-06

    X-ray diffraction rocking-curve measurements were performed on tetragonal hen egg white (HEW) lysozyme crystals grown with and without the application of an external alternating current (AC) electric field. The crystal quality was assessed by the full width at half maximum (FWHM) value for each rocking curve. For two-dimensional maps of the FWHMs measured on the 440 and the 12 12 0 reflection, the crystal homogeneity was improved under application of an external electric field at 1 MHz, compared with that without. In particular, the significant improvement of the crystal homogeneity was observed for the 12 12 0 reflection.

  13. Two stroke homogenous charge compression ignition engine with pulsed air supplier

    DOE Patents [OSTI]

    Clarke, John M.

    2003-08-05

    A two stroke homogenous charge compression ignition engine includes a volume pulsed air supplier, such as a piston driven pump, for efficient scavenging. The usage of a homogenous charge tends to decrease emissions. The use of a volume pulsed air supplier in conjunction with conventional poppet type intake and exhaust valves results in a relatively efficient scavenging mode for the engine. The engine preferably includes features that permit valving event timing, air pulse event timing and injection event timing to be varied relative to engine crankshaft angle. The principle use of the invention lies in improving diesel engines.

  14. Neutronic Assessment of Transmutation Target Compositions in Heterogeneous Sodium Fast Reactor Geometries

    SciTech Connect (OSTI)

    Samuel E. Bays; Rodolfo M. Ferrer; Michael A. Pope; Benoit Forget; Mehdi Asgari

    2008-02-01

    The sodium fast reactor is under consideration for consuming the transuranic waste in the spent nuclear fuel generated by light water reactors. This work is concerned with specialized target assemblies for an oxide-fueled sodium fast reactor that are designed exclusively for burning the americium and higher mass actinide component of light water reactor spent nuclear fuel (SNF). The associated gamma and neutron radioactivity, as well as thermal heat, associated with decay of these actinides may significantly complicate fuel handling and fabrication of recycled fast reactor fuel. The objective of using targets is to isolate in a smaller number of assemblies these concentrations of higher actinides, thus reducing the volume of fuel having more rigorous handling requirements or a more complicated fabrication process. This is in contrast to homogeneous recycle where all recycled actinides are distributed among all fuel assemblies. Several heterogeneous core geometries were evaluated to determine the fewest target assemblies required to burn these actinides without violating a set of established fuel performance criteria. The DIF3D/REBUS code from Argonne National Laboratory was used to perform the core physics and accompanying fuel cycle calculations in support of this work. Using the REBUS code, each core design was evaluated at the equilibrium cycle condition.

  15. Simulation of Heterogeneous Atom Probe Tip Shapes Evolution during Field Evaporation Using a Level Set Method and Different Evaporation Models

    SciTech Connect (OSTI)

    Xu, Zhijie; Li, Dongsheng; Xu, Wei; Devaraj, Arun; Colby, Robert J.; Thevuthasan, Suntharampillai; Geiser, B. P.; Larson, David J.

    2015-04-01

    In atom probe tomography (APT), accurate reconstruction of the spatial positions of field evaporated ions from measured detector patterns depends upon a correct understanding of the dynamic tip shape evolution and evaporation laws of component atoms. Artifacts in APT reconstructions of heterogeneous materials can be attributed to the assumption of homogeneous evaporation of all the elements in the material in addition to the assumption of a steady state hemispherical dynamic tip shape evolution. A level set method based specimen shape evolution model is developed in this study to simulate the evaporation of synthetic layered-structured APT tips. The simulation results of the shape evolution by the level set model qualitatively agree with the finite element method and the literature data using the finite difference method. The asymmetric evolving shape predicted by the level set model demonstrates the complex evaporation behavior of heterogeneous tip and the interface curvature can potentially lead to the artifacts in the APT reconstruction of such materials. Compared with other APT simulation methods, the new method provides smoother interface representation with the aid of the intrinsic sub-grid accuracy. Two evaporation models (linear and exponential evaporation laws) are implemented in the level set simulations and the effect of evaporation laws on the tip shape evolution is also presented.

  16. Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2

    SciTech Connect (OSTI)

    Hod, Idan; Sampson, Matthew D.; Deria, Pravas; Kubiak, Clifford P.; Farha, Omar K.; Hupp, Joseph T.

    2015-09-18

    Realization of heterogeneous electrochemical CO2-to-fuel conversion via molecular catalysis under high-flux conditions requires the assembly of large quantities of reactant-accessible catalysts on conductive surfaces. As a proof of principle, we demonstrate that electrophoretic deposition of thin films of an appropriately chosen metal–organic framework (MOF) material is an effective method for immobilizing the needed quantity of catalyst. For electrocatalytic CO2 reduction, we used a material that contains functionalized Fe-porphyrins as catalytically competent, redox-conductive linkers. The approach yields a high effective surface coverage of electrochemically addressable catalytic sites (~1015 sites/cm2). The chemical products of the reduction, obtained with ~100% Faradaic efficiency, are mixtures of CO and H2. The results validate the strategy of using MOF chemistry to obtain porous, electrode-immobilized, networks of molecular catalysts having competency for energy-relevant electrochemical reactions.

  17. SU-E-T-477: An Efficient Dose Correction Algorithm Accounting for Tissue Heterogeneities in LDR Brachytherapy

    SciTech Connect (OSTI)

    Mashouf, S; Lai, P; Karotki, A; Keller, B; Beachey, D; Pignol, J

    2014-06-01

    Purpose: Seed brachytherapy is currently used for adjuvant radiotherapy of early stage prostate and breast cancer patients. The current standard for calculation of dose surrounding the brachytherapy seeds is based on American Association of Physicist in Medicine Task Group No. 43 (TG-43 formalism) which generates the dose in homogeneous water medium. Recently, AAPM Task Group No. 186 emphasized the importance of accounting for tissue heterogeneities. This can be done using Monte Carlo (MC) methods, but it requires knowing the source structure and tissue atomic composition accurately. In this work we describe an efficient analytical dose inhomogeneity correction algorithm implemented using MIM Symphony treatment planning platform to calculate dose distributions in heterogeneous media. Methods: An Inhomogeneity Correction Factor (ICF) is introduced as the ratio of absorbed dose in tissue to that in water medium. ICF is a function of tissue properties and independent of source structure. The ICF is extracted using CT images and the absorbed dose in tissue can then be calculated by multiplying the dose as calculated by the TG-43 formalism times ICF. To evaluate the methodology, we compared our results with Monte Carlo simulations as well as experiments in phantoms with known density and atomic compositions. Results: The dose distributions obtained through applying ICF to TG-43 protocol agreed very well with those of Monte Carlo simulations as well as experiments in all phantoms. In all cases, the mean relative error was reduced by at least 50% when ICF correction factor was applied to the TG-43 protocol. Conclusion: We have developed a new analytical dose calculation method which enables personalized dose calculations in heterogeneous media. The advantages over stochastic methods are computational efficiency and the ease of integration into clinical setting as detailed source structure and tissue segmentation are not needed. University of Toronto, Natural Sciences and Engineering Research Council of Canada.

  18. State-of-the-art in Heterogeneous Computing

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

    Brodtkorb, Andre R.; Dyken, Christopher; Hagen, Trond R.; Hjelmervik, Jon M.; Storaasli, Olaf O.

    2010-01-01

    Node level heterogeneous architectures have become attractive during the last decade for several reasons: compared to traditional symmetric CPUs, they offer high peak performance and are energy and/or cost efficient. With the increase of fine-grained parallelism in high-performance computing, as well as the introduction of parallelism in workstations, there is an acute need for a good overview and understanding of these architectures. We give an overview of the state-of-the-art in heterogeneous computing, focusing on three commonly found architectures: the Cell Broadband Engine Architecture, graphics processing units (GPUs), and field programmable gate arrays (FPGAs). We present a review of hardware, availablemore » software tools, and an overview of state-of-the-art techniques and algorithms. Furthermore, we present a qualitative and quantitative comparison of the architectures, and give our view on the future of heterogeneous computing.« less

  19. CATALYSIS SCIENCE INITIATIVE: From First Principles Design to Realization of Bimetallic Catalysts for Enhanced Selectivity

    SciTech Connect (OSTI)

    MAVRIKAKIS, MANOS DUMESIC, JAMES A.

    2007-05-03

    In this project, we have integrated state-of-the-art Density Functional Theory (DFT) models of heterogeneous catalytic processes with high-throughput screening of bimetallic catalytic candidates for important industrial problems. We have studied a new class of alloys characterized by a surface composition different from the bulk composition, and investigated their stability and activity for the water-gas shift reaction and the oxygen reduction reaction. The former reaction is an essential part of hydrogen production; the latter is the rate-limiting step in low temperature H2 fuel cells. We have identified alloys that have remarkable stability and activity, while having a much lower material cost for both of these reactions. Using this knowledge of bimetallic interactions, we have also made progress in the industrially relevant areas of carbohydrate reforming and conversion of biomass to liquid alkanes. One aspect of this work is the conversion of glycerol (a byproduct of biodiesel production) to synthesis gas. We have developed a bifunctional supported Pt catalyst that can cleave the carbon-carbon bond while also performing the water-gas shift reaction, which allows us to better control the H2:CO ratio. Knowledge gained from the theoretical metal-metal interactions was used to develop bimetallic catalysts that perform this reaction at low temperature, allowing for an efficient coupling of this endothermic reaction with other reactions, such as Fischer-Tropsch or methanol synthesis. In our work on liquid alkane production from biomass, we have studied deactivation and selectivity in these areas as a function of metal-support interactions and reaction conditions, with an emphasis on the bifunctionality of the catalysts studied. We have identified a stable, active catalyst for this process, where the selectivity and yield can be controlled by the reaction conditions. While complete rational design of catalysts is still elusive, this work demonstrates the power of combining the insights gained from theoretical models and the work of experiments to develop new catalysts for current and future industrial challenges.

  20. High-Potential Electrocatalytic O2 Reduction with Nitroxyl / NOx Mediators: Implications for Fuel Cells and Aerobic Oxidation Catalysis

    SciTech Connect (OSTI)

    Gerken, James B.; Stahl, Shannon S.

    2015-07-15

    Efficient reduction of O2 to water is a central challenge in energy conversion and aerobic oxidation catalysis. In the present study, we investigate the electrochemical reduction of O2 with soluble organic nitroxyl and nitrogen oxide (NOx) mediators. When used alone, neither organic nitroxyls, such as TEMPO (2,2,6,6-tetramethyl-1-piperidinyl-N-oxyl), nor NOx species, such as sodium nitrite, are effective mediators of electrochemical O2 reduction. The combination of nitroxyl/NOx species, however, mediates sustained O2 reduction at electrochemical potentials of 0.19–0.33 V (vs. Fc/Fc+) in acetonitrile containing trifluoroacetic acid. Mechanistic analysis of the coupled redox reactions supports a process in which the nitrogen oxide catalyst drives aerobic oxidation of a nitroxyl mediator to an oxoammonium species, which then is reduced back to the nitroxyl at the cathode. The electrolysis potential is dictated by the oxoammonium/nitroxyl reduction potential. The high potentials observed with this ORR system benefit from the mechanism-based specificity for four-electron reduction of oxygen to water mediated by NOx species, together with kinetically efficient reduction of oxidized NOx species by TEMPO and other organic nitroxyls. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center, funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.

  1. MFT homogeneity study at TNX: Final report on the low weight percent solids concentration

    SciTech Connect (OSTI)

    Jenkins, W.J.

    1993-09-21

    A statistical design and analysis of both elemental analyses and weight percent solids analyses data was utilized to evaluate the MFT homogeneity at low heel levels and low agitator speed at both high and low solids feed concentrations. The homogeneity was also evaluated at both low and high agitator speed at the 6000+ gallons static level. The dynamic level portion of the test simulated feeding the Melter from the MFT to evaluate the uniformity of the solids slurry composition (Frit-PHA-Sludge) entering the melter from the MFT. This final report provides the results and conclusions from the second half of the study, the low weight percent solids concentration portion, as well as a comparison with the results from the first half of the study, the high weight percent solids portion.

  2. Method for preparing homogeneous single crystal ternary III-V alloys

    DOE Patents [OSTI]

    Ciszek, Theodore F.

    1991-01-01

    A method for producing homogeneous, single-crystal III-V ternary alloys of high crystal perfection using a floating crucible system in which the outer crucible holds a ternary alloy of the composition desired to be produced in the crystal and an inner floating crucible having a narrow, melt-passing channel in its bottom wall holds a small quantity of melt of a pseudo-binary liquidus composition that would freeze into the desired crystal composition. The alloy of the floating crucilbe is maintained at a predetermined lower temperature than the alloy of the outer crucible, and a single crystal of the desired homogeneous alloy is pulled out of the floating crucible melt, as melt from the outer crucible flows into a bottom channel of the floating crucible at a rate that corresponds to the rate of growth of the crystal.

  3. Some mismatches occurred when simulating fractured reservoirs as homogeneous porous media

    SciTech Connect (OSTI)

    Mario Cesar Suarez Arriaga; Fernando Samaniego V.; Fernando Rodriguez

    1996-01-24

    The understanding of transport processes that occur in naturally fractured geothermal systems is far from being complete. Often, evaluation and numerical simulations of fractured geothermal reservoirs, are carried out by assuming equivalent porous media and homogeneous petrophysical properties within big matrix blocks. The purpose of this paper, is to present a comparison between results obtained from numerical studies of a naturally fractured reservoir treated as a simple porous medium and the simulation of some real aspects of the fractured reservoir. A general conclusion outlines the great practical importance of considering even approximately, the true nature of such systems. Our results show that the homogeneous simplified evaluation of the energy resource in a fractured system, could result in unrealistic estimates of the reservoir capacity to generate electricity.

  4. Closely spaced mirror pair for reshaping and homogenizing pump beams in laser amplifiers

    SciTech Connect (OSTI)

    Bass, I.L.

    1992-12-01

    Channeling a laser beam by multiple reflections between two closely-spaced, parallel or nearly parallel mirrors, serves to reshape and homogenize the beam at the output gap between the mirrors. Application of this device to improve the spatial overlap of a copper laser pump beam with the signal beam in a dye laser amplifier is described. This technique has been applied to the AVLIS program at the Lawrence Livermore National Laboratory.

  5. Homogeneous piecewise polynomial Lyapunov function for robust stability of uncertain piecewise linear system

    SciTech Connect (OSTI)

    BenAbdallah, Abdallah; Hammami, Mohamed Ali; Kallel, Jalel

    2009-03-05

    In this paper we present some sufficient conditions for the robust stability and stabilization of time invariant uncertain piecewise linear system using homogenous piecewise polynomial Lyapunov function. The proposed conditions are given in terms of linear matrix inequalities which can be numerically solved. An application of the obtained result is given. It consists in resolving the stabilization of piecewise uncertain linear control systems by using a state piecewise linear feedback.

  6. Beam Homogeneity Dependence on the Magnetic Filter Field at the IPP Test Facility MANITU

    SciTech Connect (OSTI)

    Franzen, P.; Fantz, U.

    2011-09-26

    The homogeneity of the extracted current density from the large RF driven negative hydrogen ion sources of the ITER neutral beam system is a critical issue for the transmission of the negative ion beam through the accelerator and the beamline components. As a first test, the beam homogeneity at the IPP long pulse test facility MANITU is measured by means of the divergence and the stripping profiles obtained with a spatially resolved Doppler-shift spectroscopy system. Since MANITU is typically operating below the optimum perveance, an increase in the divergence corresponds to a lower local extracted negative ion current density if the extraction voltage is constant. The beam H{sub {alpha}} Doppler-shift spectroscopy is a rather simple tool, as no absolute calibration - both for the wavelength and the emission - is necessary. Even no relative calibration of the different used lines of sight is necessary for divergence and stripping profiles as these quantities can be obtained by the line broadening of the Doppler-shifted peak and the ratio of the integral of the stripping peak to the integral of the Doppler-shifted peak, respectively. The paper describes the H{sub {alpha}} MANITU Doppler-shift spectroscopy system which is now operating routinely and the evaluation methods of the divergence and the stripping profiles. Beam homogeneity measurements are presented for different extraction areas and magnetic filter field configurations both for Hydrogen and Deuterium operation; the results are compared with homogeneity measurements of the source plasma. The stripping loss measurements are compared with model calculations.

  7. Scalar and tensor spherical harmonics expansion of the velocity correlation in homogeneous anisotropic turbulence

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

    Rubinstein, Robert; Kurien, Susan; Cambon, Claude

    2015-06-22

    The representation theory of the rotation group is applied to construct a series expansion of the correlation tensor in homogeneous anisotropic turbulence. The resolution of angular dependence is the main analytical difficulty posed by anisotropic turbulence; representation theory parametrises this dependence by a tensor analogue of the standard spherical harmonics expansion of a scalar. As a result, the series expansion is formulated in terms of explicitly constructed tensor bases with scalar coefficients determined by angular moments of the correlation tensor.

  8. Non-homogeneous solutions of a Coulomb Schrdinger equation as basis set for scattering problems

    SciTech Connect (OSTI)

    Del Punta, J. A.; Ambrosio, M. J.; Gasaneo, G.; Zaytsev, S. A.; Ancarani, L. U.

    2014-05-15

    We introduce and study two-body Quasi Sturmian functions which are proposed as basis functions for applications in three-body scattering problems. They are solutions of a two-body non-homogeneous Schrdinger equation. We present different analytic expressions, including asymptotic behaviors, for the pure Coulomb potential with a driven term involving either Slater-type or Laguerre-type orbitals. The efficiency of Quasi Sturmian functions as basis set is numerically illustrated through a two-body scattering problem.

  9. Effect of high pressure homogenization on aqueous phase solvent extraction of lipids from Nannochloris Oculata microalgae

    SciTech Connect (OSTI)

    Samarasinghe, Nalin; Fernando, Sandun; Faulkner, William B.

    2012-12-01

    The ability to extract lipids from high-moisture Nannochloris Oculata algal biomass disrupted with high pressure homogenization was investigated. During the first phase, the effect of high pressure homogenization (system pressure and number of passes) on disrupting aqueous algae (of different concentrations and degree of stress) was investigated. Secondly, the effect of degree of cell wall disruption on the amount of lipids extracted with three solvents, namely: hexane, dichloromethane and chloroform, were compared. Studies reveled that high pressure homogenization is effective on cell disruption while the amount of system pressure being the most significant factor affecting the degree of cell breakage. Although the number of passes had some impact, the level of disruption seemed to level-off after a certain number of passes. The study revealed that slightly polar solvents (such as chloroform and dichloromethane) performed better in aqueous-phase lipid extractions as compared to hexane. Also, it was revealed that it was not necessary to disrupt the algal cells completely to achieve appreciable levels of lipid yields. In fact, conditions that exerted only 20% of the cells to completely disrupt, allowed sufficient damage to liberate most of the lipids contained in the remainder of the cells.

  10. Effect of high pressure homogenization on aqueous phase solvent extraction of lipids from Nannochloris Oculata microalgae

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

    Samarasinghe, Nalin; Fernando, Sandun; Faulkner, William B.

    2012-12-01

    The ability to extract lipids from high-moisture Nannochloris Oculata algal biomass disrupted with high pressure homogenization was investigated. During the first phase, the effect of high pressure homogenization (system pressure and number of passes) on disrupting aqueous algae (of different concentrations and degree of stress) was investigated. Secondly, the effect of degree of cell wall disruption on the amount of lipids extracted with three solvents, namely: hexane, dichloromethane and chloroform, were compared. Studies reveled that high pressure homogenization is effective on cell disruption while the amount of system pressure being the most significant factor affecting the degree of cell breakage.more » Although the number of passes had some impact, the level of disruption seemed to level-off after a certain number of passes. The study revealed that slightly polar solvents (such as chloroform and dichloromethane) performed better in aqueous-phase lipid extractions as compared to hexane. Also, it was revealed that it was not necessary to disrupt the algal cells completely to achieve appreciable levels of lipid yields. In fact, conditions that exerted only 20% of the cells to completely disrupt, allowed sufficient damage to liberate most of the lipids contained in the remainder of the cells.« less

  11. Catalyst system comprising a first catalyst system tethered to a supported catalyst

    DOE Patents [OSTI]

    Angelici, R.J.; Gao, H.

    1998-08-04

    The present invention provides new catalyst formats which comprise a supported catalyst tethered to a second and different catalyst by a suitable tethering ligand. A preferred system comprises a heterogeneous supported metal catalyst tethered to a homogeneous catalyst. This combination of homogeneous and heterogeneous catalysts has a sufficient lifetime and unusually high catalytic activity in arene hydrogenations, and potentially many other reactions as well, including, but not limited to hydroformylation, hydrosilication, olefin oxidation, isomerization, hydrocyanidation, olefin metathesis, olefin polymerization, carbonylation, enantioselective catalysis and photoduplication. These catalysts are easily separated from the products, and can be reused repeatedly, making these systems very economical. 2 figs.

  12. Catalyst system comprising a first catalyst system tethered to a supported catalyst

    DOE Patents [OSTI]

    Angelici, Robert J.; Gao, Hanrong

    1998-08-04

    The present invention provides new catalyst formats which comprise a supported catalyst tethered to a second and different catalyst by a suitable tethering ligand. A preferred system comprises a heterogeneous supported metal catalyst tethered to a homogeneous catalyst. This combination of homogeneous and heterogeneous catalysts has a sufficient lifetime and unusually high catalytic activity in arene hydrogenations, and potentially many other reactions as well, including, but not limited to hydroformylation, hydrosilation, olefin oxidation, isomerization, hydrocyanation, olefin metathesis, olefin polymerization, carbonylation, enantioselective catalysis and photoduplication. These catalysts are easily separated from the products, and can be reused repeatedly, making these systems very economical.

  13. Mining Large Heterogeneous Graphs using Cray s Urika

    SciTech Connect (OSTI)

    Sukumar, Sreenivas R; Bond, Nathaniel A

    2013-01-01

    Pattern discovery and predictive modeling from seemingly related Big Data represented as massive, ad-hoc, heterogeneous networks (e.g., extremely large graphs with complex, possibly unknown structure) is an outstanding problem in many application domains. To address this problem, we are designing graph-mining algorithms capable of discovering relationship-patterns from such data and using those discovered patterns as features for classification and predictive modeling. Specifically, we are: (i) exploring statistical properties, mechanics and generative models of behavior patterns in heterogeneous information networks, (ii) developing novel, automated and scalable graph-pattern discovery algorithms and (iii) applying our relationship-analytics (data science + network science) expertise to domains spanning healthcare to homeland security.

  14. Computational Modeling of Heterogeneous Reactive Materials at the Mesoscale

    SciTech Connect (OSTI)

    BAER, MARVIN R.

    1999-09-22

    The mesoscopic processes of consolidation, deformation and reaction of shocked porous energetic materials are studied using shock physics analysis of impact on a collection of discrete ''crystals.'' Highly resolved three-dimensional CTH simulations indicate that rapid deformation occurs at material contact points causing large amplitude fluctuations of stress states with wavelengths of the order of several particle diameters. Localization of energy produces ''hot-spots'' due to shock focusing and plastic work near internal boundaries as material flows into interstitial regions. Numerical experiments indicate that ''hot-spots'' are strongly influenced by multiple crystal interactions. Chemical reaction processes also produce multiple wave structures associated with particle distribution effects. This study provides new insights into the micromechanical behavior of heterogeneous energetic materials strongly suggesting that initiation and sustained reaction of shocked heterogeneous materials involves states distinctly different from single jump state descriptions.

  15. Imaging Heterogeneous Ion Transfer: Lithium Ion Quantification using

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

    Mercury Amalgams as In Situ Electrochemical Probes in Nonaqueous Media - Joint Center for Energy Storage Research October 24, 2014, Research Highlights Imaging Heterogeneous Ion Transfer: Lithium Ion Quantification using Mercury Amalgams as In Situ Electrochemical Probes in Nonaqueous Media Quantitative micro- and nano- probes were used for the in situ imaging of alkaline ion transfer processes at an electroactive surface. Detection of Li+, Na+ and K+ is possible. Scientific Achievement

  16. The Effect of Surface Heterogeneity on Cloud Absorption Estimates

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

    Effect of Surface Heterogeneity on Cloud Absorption Estimates W. J. Wiscombe and A. Marshak National Aeronautics and Space Administration - Goddard Space Flight Center Climate and Radiation Branch Greenbelt, Maryland J.-Y. C. Chiu Joint Center for Earth Systems Technology University of Maryland Baltimore, Maryland Introduction "Enhanced shortwave cloud absorption" (the difference between measured and model-calculated absorptions) has been a major concern in the climate community. The

  17. Incorporating reservoir heterogeneity with geostatistics to investigate waterflood recoveries

    SciTech Connect (OSTI)

    Wolcott, D.S. ); Chopra, A.K. )

    1993-03-01

    This paper presents an investigation of infill drilling performance and reservoir continuity with geostatistics and a reservoir simulator. The geostatistical technique provides many possible realizations and realistic descriptions of reservoir heterogeneity. Correlation between recovery efficiency and thickness of individual sand subunits is shown. Additional recovery from infill drilling results from thin, discontinuous subunits. The technique may be applied to variations in continuity for other sandstone reservoirs.

  18. Instruments for preparation of heterogeneous catalysts by an impregnation method

    SciTech Connect (OSTI)

    Yamada, Yusuke; Akita, Tomoki; Ueda, Atsushi; Shioyama, Hiroshi; Kobayashi, Tetsuhiko

    2005-06-15

    Instruments for the preparation of heterogeneous catalysts in powder form have been developed. The instruments consist of powder dispensing robot and an automated liquid handling machine equipped with an ultrasonic and a vortex mixer. The combination of these two instruments achieves the catalyst preparation by incipient wetness and ion exchange methods. The catalyst library prepared with these instruments were tested for dimethyl ether steam reforming and characterized by transmission electron microscopy observations.

  19. Correlating Spatial Heterogeneities in Porosity and Permeability with Metal

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

    Poisoning within an Individual Catalyst Particle using X-ray Microscopy | Stanford Synchrotron Radiation Lightsource Correlating Spatial Heterogeneities in Porosity and Permeability with Metal Poisoning within an Individual Catalyst Particle using X-ray Microscopy Wednesday, August 21, 2013 - 1:30pm SLAC, Conference Room 137-226 Presented by Darius Morris, Stanford Synchrotron Radiation Lightsource Fluid catalytic cracking (FCC) is a refining process for converting large and/or heavy

  20. Superacid catalysis of light hydrocarbon conversion. DOE PETC third quarterly report, February 25, 1994--May 24, 1994

    SciTech Connect (OSTI)

    Gates, B.C.

    1995-12-31

    Environmental concerns are leading to the replacement of aromatic hydrocarbons in gasoline by high-octane-number branched paraffins and oxygenated compounds such as methyl t-butyl ether. The ether is produced from methanol and isobutylene, and the latter can be formed from n-butane by isomerization followed by dehydrogenation. Paraffin isomerization reactions are catalyzed by very strong acids such as aluminum chloride supported on alumina. The aluminum chloride-containing catalysts are corrosive, and their disposal is expensive. Alternatively, hydroisomerization is catalyzed by zeolite-supported metals at high temperatures, but high temperatures do not favor branched products at equilibrium. Thus there is a need for improved catalysts and processes for the isomerization of n-butane and other straight-chain paraffins. Consequently, researchers have sought for solid acids that are noncorrosive and active enough to catalyze isomerization of paraffins at low temperatures. For example, sulfated zirconia catalyzes isomerization of n-butane at temperatures as low as 25{degrees}C. The addition of iron and manganese promoters has been reported to increase the activity of sulfated zirconia for n-butane isomerization by three orders of magnitude. Although the high activity of this catalyst is now established, the reaction network is not known, and the mechanism has not been investigated. The goal of this work is to investigate low-temperature reactions of light paraffins catalyzed by solid superacids of the sulfated zirconia type. The present report is concerned with catalysis of n-butane conversion catalyzed by the Fe- and Mn- promoted sulfated zirconia described in the previous report in this series.

  1. Heterogeneous composite bodies with isolated lenticular shaped cermet regions

    DOE Patents [OSTI]

    Sherman, Andrew J.

    2009-12-22

    A heterogeneous body having ceramic rich cermet regions in a more ductile metal matrix. The heterogeneous bodies are formed by thermal spray operations on metal substrates. The thermal spray operations apply heat to a cermet powder and project it onto a solid substrate. The cermet powder is composed of complex composite particles in which a complex ceramic-metallic core particle is coated with a matrix precursor. The cermet regions are generally comprised of complex ceramic-metallic composites that correspond approximately to the core particles. The cermet regions are approximately lenticular shaped with an average width that is at least approximately twice the average thickness. The cermet regions are imbedded within the matrix phase and generally isolated from one another. They have obverse and reverse surfaces. The matrix phase is formed from the matrix precursor coating on the core particles. The amount of heat applied during the formation of the heterogeneous body is controlled so that the core particles soften but do not become so fluid that they disperse throughout the matrix phase. The force of the impact on the surface of the substrate tends to flatten them. The flattened cermet regions tend to be approximately aligned with one another in the body.

  2. HeNCE: A Heterogeneous Network Computing Environment

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

    Beguelin, Adam; Dongarra, Jack J.; Geist, George Al; Manchek, Robert; Moore, Keith

    1994-01-01

    Network computing seeks to utilize the aggregate resources of many networked computers to solve a single problem. In so doing it is often possible to obtain supercomputer performance from an inexpensive local area network. The drawback is that network computing is complicated and error prone when done by hand, especially if the computers have different operating systems and data formats and are thus heterogeneous. The heterogeneous network computing environment (HeNCE) is an integrated graphical environment for creating and running parallel programs over a heterogeneous collection of computers. It is built on a lower level package called parallel virtual machine (PVM).more » The HeNCE philosophy of parallel programming is to have the programmer graphically specify the parallelism of a computation and to automate, as much as possible, the tasks of writing, compiling, executing, debugging, and tracing the network computation. Key to HeNCE is a graphical language based on directed graphs that describe the parallelism and data dependencies of an application. Nodes in the graphs represent conventional Fortran or C subroutines and the arcs represent data and control flow. This article describes the present state of HeNCE, its capabilities, limitations, and areas of future research.« less

  3. Heterogeneity analysis in 40 X-linked retinitis pigmentosa families

    SciTech Connect (OSTI)

    Teague, P.W.; Aldred, M.A.; Dempster, M.; Harrison, C.; Carothers, A.D.; Hardwick, L.J.; Evans, H.J.; Wright, A.F.; Strain, L.; Brock, D.J.H. )

    1994-07-01

    Analysis of genetic heterogeneity in 40 kindreds with X-linked retinitis pigmentosa (XLRP), with 20 polymorphic markers, showed that significant heterogeneity is present (P=.001) and that 56% of kindreds are of RP3 type and that 26% are of RP2 type. The location of the RP3 locus was found to be 0.4 cM distal to OTC in the Xp21.1 region, and that of the RP2 locus was 6.5 cM proximal to DXS7 in Xp11.2-p11.3. Bayesian probabilities of linkage to RP2, RP3, or to neither locus were calculated. This showed that 20 of 40 kindreds could be assigned to one or the other locus, with a probability >.70 (14 kindreds with RP3 and 6 kindreds with RP2 disease). A further three kindreds were found to be unlinked to either locus, with a probability >.8. The remaining 17 kindreds could not be classified unambiguously. This highlights the difficulty of classifying families in the presence of genetic heterogeneity, where two loci are separated by an estimated 16 cM. 34 refs., 1 fig., 4 tabs.

  4. Modification of heterogeneous chemistry by complex substrate morphology

    SciTech Connect (OSTI)

    Henson, B.F.; Buelow, S.J.; Robinson, J.M.

    1998-12-31

    This is the final report of a one-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). Chemistry in many environmental systems is determined at some stage by heterogeneous reaction with a surface. Typically the surface exists as a dispersion or matrix of particulate matter or pores, and a determination of the heterogeneous chemistry of the system must address the extent to which the complexity of the environmental surface affects the reaction rates. Reactions that are of current interest are the series of chlorine nitrate reactions important in polar ozone depletion. The authors have applied surface spectroscopic techniques developed at LANL to address the chemistry of chlorine nitrate reactions on porous nitric and sulfuric acid ice surfaces as a model study of the measurement of complex, heterogeneous reaction rates. The result of the study is an experimental determination of the surface coverage of one adsorbed reagent and a mechanism of reactivity based on the dependence of this coverage on temperature and vapor pressure. The resulting mechanism allows the first comprehensive modeling of chlorine nitrate reaction probability data from several laboratories.

  5. Impact of homogeneous strain on uranium vacancy diffusion in uranium dioxide

    SciTech Connect (OSTI)

    Goyal, Anuj; Phillpot, Simon R.; Subramanian, Gopinath; Andersson, David A.; Stanek, Chris R.; Uberuaga, Blas P.

    2015-03-03

    We present a detailed mechanism of, and the effect of homogeneous strains on, the migration of uranium vacancies in UO2. Vacancy migration pathways and barriers are identified using density functional theory and the effect of uniform strain fields are accounted for using the dipole tensor approach. We report complex migration pathways and noncubic symmetry associated with the uranium vacancy in UO2 and show that these complexities need to be carefully accounted for to predict the correct diffusion behavior of uranium vacancies. We show that under homogeneous strain fields, only the dipole tensor of the saddle with respect to the minimum is required to correctly predict the change in the energy barrier between the strained and the unstrained case. Diffusivities are computed using kinetic Monte Carlo simulations for both neutral and fully charged state of uranium single and divacancies. We calculate the effect of strain on migration barriers in the temperature range 800–1800 K for both vacancy types. Homogeneous strains as small as 2% have a considerable effect on diffusivity of both single and divacancies of uranium, with the effect of strain being more pronounced for single vacancies than divacancies. In contrast, the response of a given defect to strain is less sensitive to changes in the charge state of the defect. Further, strain leads to anisotropies in the mobility of the vacancy and the degree of anisotropy is very sensitive to the nature of the applied strain field for strain of equal magnitude. Our results indicate that the influence of strain on vacancy diffusivity will be significantly greater when single vacancies dominate the defect structure, such as sintering, while the effects will be much less substantial under irradiation conditions where divacancies dominate.

  6. Impact of homogeneous strain on uranium vacancy diffusion in uranium dioxide

    SciTech Connect (OSTI)

    Goyal, Anuj; Phillpot, Simon R.; Subramanian, Gopinath; Andersson, David A.; Stanek, Chris R.; Uberuaga, Blas P.

    2015-03-03

    We present a detailed mechanism of, and the effect of homogeneous strains on, the migration of uranium vacancies in UO2. Vacancy migration pathways and barriers are identified using density functional theory and the effect of uniform strain fields are accounted for using the dipole tensor approach. We report complex migration pathways and noncubic symmetry associated with the uranium vacancy in UO2 and show that these complexities need to be carefully accounted for to predict the correct diffusion behavior of uranium vacancies. We show that under homogeneous strain fields, only the dipole tensor of the saddle with respect to the minimum is required to correctly predict the change in the energy barrier between the strained and the unstrained case. Diffusivities are computed using kinetic Monte Carlo simulations for both neutral and fully charged state of uranium single and divacancies. We calculate the effect of strain on migration barriers in the temperature range 8001800 K for both vacancy types. Homogeneous strains as small as 2% have a considerable effect on diffusivity of both single and divacancies of uranium, with the effect of strain being more pronounced for single vacancies than divacancies. In contrast, the response of a given defect to strain is less sensitive to changes in the charge state of the defect. Further, strain leads to anisotropies in the mobility of the vacancy and the degree of anisotropy is very sensitive to the nature of the applied strain field for strain of equal magnitude. Our results indicate that the influence of strain on vacancy diffusivity will be significantly greater when single vacancies dominate the defect structure, such as sintering, while the effects will be much less substantial under irradiation conditions where divacancies dominate.

  7. Impact of homogeneous strain on uranium vacancy diffusion in uranium dioxide

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

    Goyal, Anuj; Phillpot, Simon R.; Subramanian, Gopinath; Andersson, David A.; Stanek, Chris R.; Uberuaga, Blas P.

    2015-03-03

    We present a detailed mechanism of, and the effect of homogeneous strains on, the migration of uranium vacancies in UO2. Vacancy migration pathways and barriers are identified using density functional theory and the effect of uniform strain fields are accounted for using the dipole tensor approach. We report complex migration pathways and noncubic symmetry associated with the uranium vacancy in UO2 and show that these complexities need to be carefully accounted for to predict the correct diffusion behavior of uranium vacancies. We show that under homogeneous strain fields, only the dipole tensor of the saddle with respect to the minimummore » is required to correctly predict the change in the energy barrier between the strained and the unstrained case. Diffusivities are computed using kinetic Monte Carlo simulations for both neutral and fully charged state of uranium single and divacancies. We calculate the effect of strain on migration barriers in the temperature range 800–1800 K for both vacancy types. Homogeneous strains as small as 2% have a considerable effect on diffusivity of both single and divacancies of uranium, with the effect of strain being more pronounced for single vacancies than divacancies. In contrast, the response of a given defect to strain is less sensitive to changes in the charge state of the defect. Further, strain leads to anisotropies in the mobility of the vacancy and the degree of anisotropy is very sensitive to the nature of the applied strain field for strain of equal magnitude. Our results indicate that the influence of strain on vacancy diffusivity will be significantly greater when single vacancies dominate the defect structure, such as sintering, while the effects will be much less substantial under irradiation conditions where divacancies dominate.« less

  8. High-throughput method for optimum solubility screening for homogeneity and crystallization of proteins

    DOE Patents [OSTI]

    Kim, Sung-Hou; Kim, Rosalind; Jancarik, Jamila

    2012-01-31

    An optimum solubility screen in which a panel of buffers and many additives are provided in order to obtain the most homogeneous and monodisperse protein condition for protein crystallization. The present methods are useful for proteins that aggregate and cannot be concentrated prior to setting up crystallization screens. A high-throughput method using the hanging-drop method and vapor diffusion equilibrium and a panel of twenty-four buffers is further provided. Using the present methods, 14 poorly behaving proteins have been screened, resulting in 11 of the proteins having highly improved dynamic light scattering results allowing concentration of the proteins, and 9 were crystallized.

  9. Homogeneous versus spiral phases of hole-doped antiferromagnets: A systematic effective field theory investigation

    SciTech Connect (OSTI)

    Bruegger, C.; Kaempfer, F.; Wiese, U.-J.; Hofmann, C. P.; Pepe, M.

    2007-01-01

    Using the low-energy effective field theory for magnons and holes--the condensed matter analog of baryon chiral perturbation theory for pions and nucleons in QCD--we study different phases of doped antiferromagnets. We systematically investigate configurations of the staggered magnetization that provide a constant background field for doped holes. The most general configuration of this type is either constant itself or represents a spiral in the staggered magnetization. Depending on the values of the low-energy parameters, a homogeneous phase, a spiral phase, or an inhomogeneous phase is energetically favored. The reduction of the staggered magnetization upon doping is also investigated.

  10. Method of producing homogeneous mixed metal oxides and metal-metal oxide mixtures

    DOE Patents [OSTI]

    Quinby, Thomas C.

    1978-01-01

    Metal powders, metal oxide powders, and mixtures thereof of controlled particle size are provided by reacting an aqueous solution containing dissolved metal values with excess urea. Upon heating, urea reacts with water from the solution leaving a molten urea solution containing the metal values. The molten urea solution is heated to above about 180.degree. C. whereupon metal values precipitate homogeneously as a powder. The powder is reduced to metal or calcined to form oxide particles. One or more metal oxides in a mixture can be selectively reduced to produce metal particles or a mixture of metal and metal oxide particles.

  11. Fuel mixture stratification as a method for improving homogeneous charge compression ignition engine operation

    DOE Patents [OSTI]

    Dec, John E.; Sjoberg, Carl-Magnus G.

    2006-10-31

    A method for slowing the heat-release rate in homogeneous charge compression ignition ("HCCI") engines that allows operation without excessive knock at higher engine loads than are possible with conventional HCCI. This method comprises injecting a fuel charge in a manner that creates a stratified fuel charge in the engine cylinder to provide a range of fuel concentrations in the in-cylinder gases (typically with enough oxygen for complete combustion) using a fuel with two-stage ignition fuel having appropriate cool-flame chemistry so that regions of different fuel concentrations autoignite sequentially.

  12. Cohesive Modeling of Dynamic Crack Growth in Homogeneous and Functionally Graded Materials

    SciTech Connect (OSTI)

    Zhang Zhengyu; Paulino, Glaucio H.; Celes, Waldemar

    2008-02-15

    This paper presents a Cohesive Zone Model (CZM) approach for investigating dynamic crack propagation in homogeneous and Functionally Graded Materials (FGMs). The failure criterion is incorporated in the CZM using both a finite cohesive strength and work to fracture in the material description. A novel CZM for FGMs is explored and incorporated into a finite element framework. The material gradation is approximated at the element level using a graded element formulation. A numerical example is provided to demonstrate the efficacy of the CZM approach, in which the influence of the material gradation on the crack growth pattern is studied.

  13. Search for: All records | SciTech Connect

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  18. Bioinspired design of redox-active ligands for multielectron catalysis: Effects of positioning pyrazine reservoirs on cobalt for electro- and photocatalytic generation of hydrogen from water

    SciTech Connect (OSTI)

    Jurss, Jonah W.; Khnayzer, Rony S.; Panetier, Julien A.; El Roz, Karim A.; Nichols, Eva M.; Head-Gordon, Martin; Long, Jeffrey R.; Castellano, Felix N.; Chang, Christopher J.

    2015-06-09

    Mononuclear metalloenzymes in nature can function in cooperation with precisely positioned redox-active organic cofactors in order to carry out multielectron catalysis. Inspired by the finely tuned redox management of these bioinorganic systems, we present the design, synthesis, and experimental and theoretical characterization of a homologous series of cobalt complexes bearing redox-active pyrazines. These donor moieties are locked into key positions within a pentadentate ligand scaffold in order to evaluate the effects of positioning redox non-innocent ligands on hydrogen evolution catalysis. Both metal- and ligand-centered redox features are observed in organic as well as aqueous solutions over a range of pH values, and comparison with analogs bearing redox-inactive zinc(II) allows for assignments of ligand-based redox events. Varying the geometric placement of redox non-innocent pyrazine donors on isostructural pentadentate ligand platforms results in marked effects on observed cobalt-catalyzed proton reduction activity. Electrocatalytic hydrogen evolution from weak acids in acetonitrile solution, under diffusion-limited conditions, reveals that the pyrazine donor of axial isomer 1-Co behaves as an unproductive electron sink, resulting in high overpotentials for proton reduction, whereas the equatorial pyrazine isomer complex 2-Co is significantly more active for hydrogen generation at lower voltages. Addition of a second equatorial pyrazine in complex 3-Co further minimizes overpotentials required for catalysis. The equatorial derivative 2-Co is also superior to its axial 1-Co congener for electrocatalytic and visible-light photocatalytic hydrogen generation in biologically relevant, neutral pH aqueous media. Density functional theory calculations (B3LYP-D2) indicate that the first reduction of catalyst isomers 1-Co, 2-Co, and 3-Co is largely metal-centered while the second reduction occurs at pyrazine. Taken together, the data establish that proper positioning of non-innocent pyrazine ligands on a single cobalt center is indeed critical for promoting efficient hydrogen catalysis in aqueous media, akin to optimally positioned redox-active cofactors in metalloenzymes. In a broader sense, these findings highlight the significance of electronic structure considerations in the design of effective electron–hole reservoirs for multielectron transformations.

  19. Bioinspired design of redox-active ligands for multielectron catalysis: Effects of positioning pyrazine reservoirs on cobalt for electro- and photocatalytic generation of hydrogen from water

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

    Jurss, Jonah W.; Khnayzer, Rony S.; Panetier, Julien A.; El Roz, Karim A.; Nichols, Eva M.; Head-Gordon, Martin; Long, Jeffrey R.; Castellano, Felix N.; Chang, Christopher J.

    2015-06-09

    Mononuclear metalloenzymes in nature can function in cooperation with precisely positioned redox-active organic cofactors in order to carry out multielectron catalysis. Inspired by the finely tuned redox management of these bioinorganic systems, we present the design, synthesis, and experimental and theoretical characterization of a homologous series of cobalt complexes bearing redox-active pyrazines. These donor moieties are locked into key positions within a pentadentate ligand scaffold in order to evaluate the effects of positioning redox non-innocent ligands on hydrogen evolution catalysis. Both metal- and ligand-centered redox features are observed in organic as well as aqueous solutions over a range of pHmore » values, and comparison with analogs bearing redox-inactive zinc(II) allows for assignments of ligand-based redox events. Varying the geometric placement of redox non-innocent pyrazine donors on isostructural pentadentate ligand platforms results in marked effects on observed cobalt-catalyzed proton reduction activity. Electrocatalytic hydrogen evolution from weak acids in acetonitrile solution, under diffusion-limited conditions, reveals that the pyrazine donor of axial isomer 1-Co behaves as an unproductive electron sink, resulting in high overpotentials for proton reduction, whereas the equatorial pyrazine isomer complex 2-Co is significantly more active for hydrogen generation at lower voltages. Addition of a second equatorial pyrazine in complex 3-Co further minimizes overpotentials required for catalysis. The equatorial derivative 2-Co is also superior to its axial 1-Co congener for electrocatalytic and visible-light photocatalytic hydrogen generation in biologically relevant, neutral pH aqueous media. Density functional theory calculations (B3LYP-D2) indicate that the first reduction of catalyst isomers 1-Co, 2-Co, and 3-Co is largely metal-centered while the second reduction occurs at pyrazine. Taken together, the data establish that proper positioning of non-innocent pyrazine ligands on a single cobalt center is indeed critical for promoting efficient hydrogen catalysis in aqueous media, akin to optimally positioned redox-active cofactors in metalloenzymes. In a broader sense, these findings highlight the significance of electronic structure considerations in the design of effective electron–hole reservoirs for multielectron transformations.« less

  20. Memristive behavior and forming mechanism of homogeneous TiO{sub x} device

    SciTech Connect (OSTI)

    Dong, Ruixin; Yan, Xunling; Zhang, Zhang; Wang, Minghong

    2015-01-15

    Highlights: • We fabricated a homogeneity TiO{sub x} device with excellent memristive behavior. • The double-interface conductive filament model is suggested. • The calculated I–V curve is in agreement with the experimental results. • The switching voltage could be adjusted by selecting the proper electrode materials. - Abstract: A homogeneous titanium oxide device is fabricated by Molecular Beam Epitaxy and the excellent memristive behavior could be observed. The resistance ratio between high resistance state and low resistance state increases as the thickness of titanium oxide or the oxygen content reduces. The forming voltage is lower than the previous report. Based on the experimental results, we suggest a double-interface conductive filament model and calculate the current–voltage curve of the device in agreement with experimental measurements. The result indicates that the forming voltage of the device will rise with increasing of the chemical potential differences across the two interfaces. In other words, the switching voltage could be adjusted by selecting a proper electrode and oxide materials.

  1. Development of a HEX-Z Partially Homogenized Benchmark Model for the FFTF Isothermal Physics Measurements

    SciTech Connect (OSTI)

    John D. Bess

    2012-05-01

    A series of isothermal physics measurements were performed as part of an acceptance testing program for the Fast Flux Test Facility (FFTF). A HEX-Z partially-homogenized benchmark model of the FFTF fully-loaded core configuration was developed for evaluation of these measurements. Evaluated measurements include the critical eigenvalue of the fully-loaded core, two neutron spectra, 32 reactivity effects measurements, an isothermal temperature coefficient, and low-energy gamma and electron spectra. Dominant uncertainties in the critical configuration include the placement of radial shielding around the core, reactor core assembly pitch, composition of the stainless steel components, plutonium content in the fuel pellets, and boron content in the absorber pellets. Calculations of criticality, reactivity effects measurements, and the isothermal temperature coefficient using MCNP5 and ENDF/B-VII.0 cross sections with the benchmark model are in good agreement with the benchmark experiment measurements. There is only some correlation between calculated and measured spectral measurements; homogenization of many of the core components may have impacted computational assessment of these measurements. This benchmark evaluation has been added to the IRPhEP Handbook.

  2. Process for forming a homogeneous oxide solid phase of catalytically active material

    DOE Patents [OSTI]

    Perry, Dale L.; Russo, Richard E.; Mao, Xianglei

    1995-01-01

    A process is disclosed for forming a homogeneous oxide solid phase reaction product of catalytically active material comprising one or more alkali metals, one or more alkaline earth metals, and one or more Group VIII transition metals. The process comprises reacting together one or more alkali metal oxides and/or salts, one or more alkaline earth metal oxides and/or salts, one or more Group VIII transition metal oxides and/or salts, capable of forming a catalytically active reaction product, in the optional presence of an additional source of oxygen, using a laser beam to ablate from a target such metal compound reactants in the form of a vapor in a deposition chamber, resulting in the deposition, on a heated substrate in the chamber, of the desired oxide phase reaction product. The resulting product may be formed in variable, but reproducible, stoichiometric ratios. The homogeneous oxide solid phase product is useful as a catalyst, and can be produced in many physical forms, including thin films, particulate forms, coatings on catalyst support structures, and coatings on structures used in reaction apparatus in which the reaction product of the invention will serve as a catalyst.

  3. DESIGN, SYNTHESIS, AND MECHANISTIC EVALUATION OF IRON-BASED CATALYSIS FOR SYNTHESIS GAS CONVERSION TO FUELS AND CHEMICALS

    SciTech Connect (OSTI)

    Akio Ishikawa; Manuel Ojeda; Enrique Iglesia

    2005-03-31

    This project explores the extension of previously discovered Fe-based catalysts to hydrogen-poor synthesis gas streams derived from coal and biomass sources. These catalysts have previously shown unprecedented Fischer-Tropsch synthesis rate, selectivity with synthesis gas derived from methane. During the first reporting period, we certified a microreactor, installed required analytical equipment, and reproduced synthetic protocols and catalytic performance previously reported. During the second reporting period, we prepared several Fe-based compositions for Fischer-Tropsch synthesis and tested the effects of product recycle under both subcritical and supercritical conditions. During this third reporting period, we have prepared a large number of Fe-based catalyst compositions using precipitation and impregnations methods with both supercritical and subcritical drying and with the systematic use of surface active agents to prevent pore collapse during drying steps required in synthetic protocols. These samples were characterized during this period using X-ray diffraction, surface area, and temperature-programmed reduction measurements. These studies have shown that these synthesis methods lead to even higher surface areas than in our previous studies and confirm the crystalline structures of these materials and their reactivity in both oxide-carbide interconversions and in Fischer-Tropsch synthesis catalysis. Fischer-Tropsch synthesis reaction rates and selectivities with low H{sub 2}/CO ratio feeds (H{sub 2}/CO = 1) were the highest reported in the literature at the low-temperature and relatively low pressure in our measurements. Current studies are exploring the optimization of the sequence of impregnation of Cu, K, and Ru promoters, of the activation and reaction conditions, and of the co-addition of light hydrocarbons to increase diffusion rates of primary olefin products so as to increase the selectivity to unsaturated products. Finally, we are also addressing the detailed kinetic response of optimized catalysts to reaction conditions (temperature, partial pressures of H{sub 2}, CO, H{sub 2}O, CO{sub 2}, olefins) in an effort to further increase rates and olefin and C{sub 5+} selectivities.

  4. Superacid catalysis of light hydrocarbon conversion. DOE PETC seventh quarterly progress report, April 1, 1995--July 31, 1995

    SciTech Connect (OSTI)

    Gates, B.C.

    1996-02-01

    Iron- and manganese-promoted sulfated zirconia is a catalyst for the conversion of propane, but the rate of conversion of propane is much less than the rate of conversion of butane. Whereas this catalyst appears to be a good candidate for practical, industrial conversion of butane, it appears to lack sufficient activity for practical conversion of propane. The propane conversion data reported here provide excellent insights into the chemistry of the catalytic conversion. Solid and catalysts, namely, sulfated zirconia, iron- and manganese-promoted sulfated zirconia, and USY zeolite, were tested for conversion of propane at 1 atm, 200-450{degrees}C, and propane partial pressures in the range of 0.01-0.05 atm. Both promoted and unpromoted sulfated zirconia were found to be active for conversion of propane into butanes, pentanes, methane, ethane, ethylene, and propylene in the temperature range of 200-350{degrees}C, but catalyst deactivation was rapid. At the higher temperatures, only cracking and dehydrogenation products were observed. In contrast to the zirconia-supported catalysts, USY zeolite was observed to convert propane (into propylene, methane, and ethylene) only at temperatures {ge}400{degrees}C. The initial (5 min on stream) rates of propane conversion in the presence of iron- and manganese-promoted sulfated zirconia, sulfated zirconia, and USY zeolite at 450{degrees}C and 0.01 atm propane partial pressure were 3.3 x 10{sup -8}, 0.3 x 10{sup -8}, and 0.06 x 10{sup -8} mol/(s{center_dot}g), respectively. The product distributions in the temperature range 200-450{degrees}C are those of acid-base catalysis, being similar to what has been observed in superacid solution chemistry at temperatures <0{degrees}C. If propane conversion at 450{degrees}C can be considered as a probe of acid strength of the catalyst, the activity comparison suggests that the promoted sulfated zirconia is a stronger acid than sulfated zirconia, which is a stronger acid than USY zeolite.

  5. A heterogeneous hierarchical architecture for real-time computing

    SciTech Connect (OSTI)

    Skroch, D.A.; Fornaro, R.J.

    1988-12-01

    The need for high-speed data acquisition and control algorithms has prompted continued research in the area of multiprocessor systems and related programming techniques. The result presented here is a unique hardware and software architecture for high-speed real-time computer systems. The implementation of a prototype of this architecture has required the integration of architecture, operating systems and programming languages into a cohesive unit. This report describes a Heterogeneous Hierarchial Architecture for Real-Time (H{sup 2} ART) and system software for program loading and interprocessor communication.

  6. Oxygenates from synthesis gas

    SciTech Connect (OSTI)

    Falter, W.; Keim, W.

    1994-12-31

    The direct synthesis of oxygenates starting from synthesis gas is feasible by homogeneous and heterogeneous catalysis. Homogeneous Rh and Ru based catalysts yielding methyl formate and alcohols will be presented. Interestingly, modified heterogeneous catalysts based on {open_quotes}Isobutyl Oel{close_quotes} catalysis, practized in Germany (BRD) up to 1952 and in the former DDR until recently, yield isobutanol in addition to methanol. These {open_quotes}Isobutyl Oel{close_quotes} catalysts are obtained by adding a base such as Li < Na < K < Cs to a Zn-Cr{sub 2}O{sub 3} methanol catalyst. Isobutanol is obtained in up to 15% yield. Our best catalyst a Zr-Zn-Mn-Li-Pd catalyst produced isobotanol up to 60% at a rate of 740g isobutanol per liter catalyst and hour.

  7. The generation of efficient supported (Heterogeneous) olefin metathesis catalysts

    SciTech Connect (OSTI)

    Grubbs, Robert H

    2013-04-05

    Over the past decade, a new family of homogeneous metathesis catalysts has been developed that will tolerate most organic functionalities as well as water and air. These homogeneous catalysts are finding numerous applications in the pharmaceutical industry as well as in the production of functional polymers. In addition the catalysts are being used to convert seed oils into products that can substitute for those that are now made from petroleum products. Seed oils are unsaturated, contain double bonds, and are a ready source of linear hydrocarbon fragments that are specifically functionalized. To increase the number of applications in the area of biomaterial conversion to petrol chemicals, the activity and efficiency of the catalysts need to be as high as possible. The higher the efficiency of the catalysts, the lower the cost of the conversion and a larger number of practical applications become available. Active supported catalysts were prepared and tested in the conversion of seed oils and other important starting materials. The outcome of the work was successful and the technology has been transferred to a commercial operation to develop viable applications of the discovered systems. A biorefinery that converts seed oils is under construction in Indonesia. The catalysts developed in this study will be considered for the next generation of operations.

  8. Optimal utilization of heterogeneous resources for biomolecular simulations

    SciTech Connect (OSTI)

    Hampton, Scott S; Agarwal, Pratul K

    2010-01-01

    Biomolecular simulations have traditionally benefited from increases in the processor clock speed and coarse-grain inter-node parallelism on large-scale clusters. With stagnating clock frequencies, the evolutionary path for performance of microprocessors is maintained by virtue of core multiplication. Graphical processing units (GPUs) offer revolutionary performance potential at the cost of increased programming complexity. Furthermore, it has been extremely challenging to effectively utilize heterogeneous resources (host processor and GPU cores) for scientific simulations, as underlying systems, programming models and tools are continually evolving. In this paper, we present a parametric study demonstrating approaches to exploit resources of heterogeneous systems to reduce time-to-solution of a production-level application for biological simulations. By overlapping and pipelining computation and communication, we observe up to 10-fold application acceleration in multi-core and multi-GPU environments illustrating significant performance improvements over code acceleration approaches, where the host-to-accelerator ratio is static, and is constrained by a given algorithmic implementation.

  9. Optimal utilization of heterogeneous resources for biomolecular simulations.

    SciTech Connect (OSTI)

    Alam, Sadaf R.; Agarwal, Pratul K.; Hampton, Scott; Crozier, Paul Stewart

    2010-04-01

    Biomolecular simulations have traditionally benefited from increases in the processor clock speed and coarse-grain inter-node parallelism on large-scale clusters. With stagnating clock frequencies, the evolutionary path for performance of microprocessors is maintained by virtue of core multiplication. Graphical processing units (GPUs) offer revolutionary performance potential at the cost of increased programming complexity. Furthermore, it has been extremely challenging to effectively utilize heterogeneous resources (host processor and GPU cores) for scientific simulations, as underlying systems, programming models and tools are continually evolving. In this paper, we present a parametric study demonstrating approaches to exploit resources of heterogeneous systems to reduce time-to-solution of a production-level application for biological simulations. By overlapping and pipelining computation and communication, we observe up to 10-fold application acceleration in multi-core and multi-GPU environments illustrating significant performance improvements over code acceleration approaches, where the host-to-accelerator ratio is static, and is constrained by a given algorithmic implementation.

  10. Modeling flow in a pressure-sensitive, heterogeneous medium

    SciTech Connect (OSTI)

    Vasco, Donald W.; Minkoff, Susan E.

    2009-06-01

    Using an asymptotic methodology, including an expansion in inverse powers of {radical}{omega}, where {omega} is the frequency, we derive a solution for flow in a medium with pressure dependent properties. The solution is valid for a heterogeneous medium with smoothly varying properties. That is, the scale length of the heterogeneity must be significantly larger then the scale length over which the pressure increases from it initial value to its peak value. The resulting asymptotic expression is similar in form to the solution for pressure in a medium in which the flow properties are not functions of pressure. Both the expression for pseudo-phase, which is related to the 'travel time' of the transient pressure disturbance, and the expression for pressure amplitude contain modifications due to the pressure dependence of the medium. We apply the method to synthetic and observed pressure variations in a deforming medium. In the synthetic test we model one-dimensional propagation in a pressure-dependent medium. Comparisons with both an analytic self-similar solution and the results of a numerical simulation indicate general agreement. Furthermore, we are able to match pressure variations observed during a pulse test at the Coaraze Laboratory site in France.

  11. Application of Gold Electrodes for the Study of Nickel Based Homogeneous Catalysts for Hydrogen Oxidation

    SciTech Connect (OSTI)

    Nepomnyashchii, Alexander B.; Liu, Fei; Roberts, John A.; Parkinson, Bruce A.

    2013-08-12

    Gold and glassy carbon working electrode materials are compared as suitable substrates for the hydrogen oxidation reaction with Ni(PCy2Nt-Bu2)2(BF4)2 used as a catalyst. Voltammetric responses showing electrocatalytic hydrogen oxidation mediated by the homogeneous electrocatalyst Ni(PCy2Nt-Bu2)2(BF4)2 are identical at glassy carbon and gold electrodes, which shows that gold electrode can be used for hydrogen oxidation reaction. This work is supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under FWP 56073.

  12. Homogenization of a thin plate reinforced with periodic families of rigid rods

    SciTech Connect (OSTI)

    Nazarov, Sergei A; Sweers, Guido H; Slutskij, Andrey S

    2011-08-31

    The asymptotics of the solution to the elastic bending problem for a thin plate reinforced with several periodic families of closely spaced but disjoint rods are constructed and justified, the result of homogenization being substantially different from the case when the rods are welded together into a single periodic mesh. The material in the rods is assumed to be appreciably more rigid than that in the plate. An averaged fourth-order differential operator is obtained from summing the nonelliptic operators generated by each of the families of the rods. This operator is shown to be elliptic if and only if the rods from at least two families are nonparallel. As a simplified example, the paper examines a similar stationary heat conduction problem. Bibliography: 24 titles.

  13. Particle dispersion in homogeneous turbulence using the one-dimensional turbulence model

    SciTech Connect (OSTI)

    Sun, Guangyuan; Lignell, David O.; Hewson, John C.; Gin, Craig R.

    2014-10-09

    Lagrangian particle dispersion is studied using the one-dimensional turbulence (ODT) model in homogeneous decaying turbulence configurations. The ODT model has been widely and successfully applied to a number of reacting and nonreacting flow configurations, but only limited application has been made to multiphase flows. We present a version of the particle implementation and interaction with the stochastic and instantaneous ODT eddy events. The model is characterized by comparison to experimental data of particle dispersion for a range of intrinsic particle time scales and body forces. Particle dispersion, velocity, and integral time scale results are presented. Moreover, the particle implementation introduces a single model parameter β p , and sensitivity to this parameter and behavior of the model are discussed. Good agreement is found with experimental data and the ODT model is able to capture the particle inertial and trajectory crossing effects. Our results serve as a validation case of the multiphase implementations of ODT for extensions to other flow configurations.

  14. Effects of non-homogeneous flow on ADCP data processing in a hydroturbine forebay

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

    Harding, S. F.; Richmond, M. C.; Romero-Gomez, P.; Serkowski, J. A.

    2016-01-02

    Accurate modeling of the velocity field in the forebay of a hydroelectric power station is important for both power generation and fish passage, and is able to be increasingly well represented by computational fluid dynamics (CFD) simulations. Acoustic Doppler Current Profiler (ADCP) are investigated herein as a method of validating the numerical flow solutions, particularly in observed and calculated regions of non-homogeneous flow velocity. By using a numerical model of an ADCP operating in a velocity field calculated using CFD, the errors due to the spatial variation of the flow velocity are quantified. Furthermore, the numerical model of the ADCPmore » is referred to herein as a Virtual ADCP (VADCP).« less

  15. Final Technical Report - Investigation into the Relationship between Heterogeneity and Heavy-Tailed Solute Transport

    SciTech Connect (OSTI)

    Weissmann, Gary S

    2013-12-06

    The objective of this project was to characterize the influence that naturally complex geologic media has on anomalous dispersion and to determine if the nature of dispersion can be estimated from the underlying heterogeneous media. The UNM portion of this project was to provide detailed representations of aquifer heterogeneity through producing highly-resolved models of outcrop analogs to aquifer materials. This project combined outcrop-scale heterogeneity characterization (conducted at the University of New Mexico), laboratory experiments (conducted at Sandia National Laboratory), and numerical simulations (conducted at Sandia National Laboratory and Colorado School of Mines). The study was designed to test whether established dispersion theory accurately predicts the behavior of solute transport through heterogeneous media and to investigate the relationship between heterogeneity and the parameters that populate these models. The dispersion theory tested by this work was based upon the fractional advection-dispersion equation (fADE) model. Unlike most dispersion studies that develop a solute transport model by fitting the solute transport breakthrough curve, this project explored the nature of the heterogeneous media to better understand the connection between the model parameters and the aquifer heterogeneity. We also evaluated methods for simulating the heterogeneity to see whether these approaches (e.g., geostatistical) could reasonably replicate realistic heterogeneity. The UNM portion of this study focused on capturing realistic geologic heterogeneity of aquifer analogs using advanced outcrop mapping methods.

  16. 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.

  17. A Light-Stimulated Molecular Switch Driven by Radical-Radical...

    Office of Scientific and Technical Information (OSTI)

    United States Language: English Subject: catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, mesostructured materials, materials and chemistry...

  18. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    (2) catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, ... improve both the photovoltaic and mechanical properties of polymeric materials. ...

  19. Center for Molecular Electrocatalysis (CME) | U.S. DOE Office...

    Office of Science (SC) Website

    To understand and design molecular electrocatalysts for conversions between electrical energy and chemical energy. Research Topics catalysis (homogeneous), solar (fuels), ...

  20. Heterogeneous nucleation of naphthalene vapor on water surface

    SciTech Connect (OSTI)

    Smolik, J.; Schwarz, J.

    1997-01-15

    Transfer processes between drops and gas play an important role in many natural and industrial processes, as absorption of gaseous pollutants by water drops in the atmosphere, combustion of fuel droplets, spray drying, synthesis of nanopowders, wet-dry desulfurization or extinguishing of hot combustion gases. The evaporation of a water drop into a ternary gaseous mixture of air, steam, and naphthalene vapor was investigated. The experimental results were compared with a theoretical prediction based on a numerical solution of coupled boundary layer equations for heat and mass transfer from a drop moving in ternary gas. In the experiments the naphthalene vapor condensed on the water drop as a supercooled liquid even at temperatures far below the melting point of naphthalene. The condensation on drop surface is discussed in terms of classical theory of heterogeneous nucleation on smooth surfaces.

  1. Ganglion dynamics of Supercritical CO2 in heterogeneous media

    Office of Scientific and Technical Information (OSTI)

    Ganglion dynamics of Supercritical CO2 in heterogeneous media SAND2015-2548C \ 1.E+01 Mobile 1.E+00 Trapped £ 1.E-01 1.E-02 1.0E-05 1.0E-04 1.0E-03 1.0E-02 Pore diameter (2rp) (m) 1.0 1.E+00 0.9 0.8 0.7 1.E-01 / / 1.E-02 £ 40 0.3 0.2 Ganglion size (cm) 0.1 0.0 1.E-03 1.E-04 1.E-03 1.E-02 Water Flow Velocity (Vw°) (m/s) Trapping efficiency Injectivity Permeability or porosity Research Team Y Wang, MJ Martinez & K Chojnicki Objectives of Research - Develop observationaNy-constrained models

  2. On fluid flow in a heterogeneous medium under nonisothermal conditions

    SciTech Connect (OSTI)

    D.W., Vasco

    2010-11-01

    An asymptotic technique, valid in the presence of smoothly-varying heterogeneity, provides explicit expressions for the velocity of a propagating pressure and temperature disturbance. The governing equations contain nonlinear terms due to the presence of temperature-dependent coefficients and due to the advection of fluids with differing temperatures. Two cases give well-defined expressions in terms of the parameters of the porous medium: the uncoupled propagation of a pressure disturbance and the propagation of a fully coupled temperature and pressure disturbance. The velocity of the coupled disturbance or front, depends upon the medium parameters and upon the change in temperature and pressure across the front. For uncoupled flow, the semi-analytic expression for the front velocity reduces to that associated with a linear diffusion equation. A comparison of the asymptotic travel time estimates with calculations from a numerical simulator indicates reasonably good agreement for both uncoupled and coupled disturbances.

  3. Multiscale Universal Interface: A concurrent framework for coupling heterogeneous solvers

    SciTech Connect (OSTI)

    Tang, Yu-Hang; Kudo, Shuhei; Bian, Xin; Li, Zhen; Karniadakis, George Em

    2015-09-15

    Graphical abstract: - Abstract: Concurrently coupled numerical simulations using heterogeneous solvers are powerful tools for modeling multiscale phenomena. However, major modifications to existing codes are often required to enable such simulations, posing significant difficulties in practice. In this paper we present a C++ library, i.e. the Multiscale Universal Interface (MUI), which is capable of facilitating the coupling effort for a wide range of multiscale simulations. The library adopts a header-only form with minimal external dependency and hence can be easily dropped into existing codes. A data sampler concept is introduced, combined with a hybrid dynamic/static typing mechanism, to create an easily customizable framework for solver-independent data interpretation. The library integrates MPI MPMD support and an asynchronous communication protocol to handle inter-solver information exchange irrespective of the solvers' own MPI awareness. Template metaprogramming is heavily employed to simultaneously improve runtime performance and code flexibility. We validated the library by solving three different multiscale problems, which also serve to demonstrate the flexibility of the framework in handling heterogeneous models and solvers. In the first example, a Couette flow was simulated using two concurrently coupled Smoothed Particle Hydrodynamics (SPH) simulations of different spatial resolutions. In the second example, we coupled the deterministic SPH method with the stochastic Dissipative Particle Dynamics (DPD) method to study the effect of surface grafting on the hydrodynamics properties on the surface. In the third example, we consider conjugate heat transfer between a solid domain and a fluid domain by coupling the particle-based energy-conserving DPD (eDPD) method with the Finite Element Method (FEM)

  4. Impact of heterogeneous chemistry on model predictions of ozone changes

    SciTech Connect (OSTI)

    Granier, C.; Brasseur, G. )

    1992-11-20

    A two-dimensional chemical/transport model of the middle atmosphere is used to assess the importance of chemical heterogeneous processes in the polar regions (on polar stratospheric clouds (PSCs)) and at other latitudes (on sulfate aerosols). When conversion on type I and type II PSCs of N[sub 2]O[sub 5] into HNO[sub 3] and of CIONO[sub 2] into reactive forms of chlorine is taken into account, enhanced CIO concentrations lead to the formation of a springtime ozone hole over the Antarctic continent; no such major reduction in the ozone column is found in the Arctic region. When conversion of nitrogen and chlorine compounds is assumed to occur on sulfate particles in the lower stratosphere, significant perturbations in the chemistry are also found. For background aerosol conditions, the concentration of nitric acid is enhanced and agrees with observed values, while that of nitrogen oxides is reduced and agrees less than if heterogeneous processes are ignored in the calculations. The concentration of the OH radical is significantly increased. Ozone number density appears to become larger between 16 and 30 km but smaller below 16 km, especially at high latitudes. The ozone column is only slightly modified, except at high latitudes where it is substantially reduced if the CIONO[sub 2] conversion into reactive chlorine is considered. After a large volcanic eruption these changes are further exacerbated. The ozone budget in the lower stratrosphere becomes less affected by nitrogen oxides but is largely controlled by the CIO[sub x] and HO[sub x] chemistries. A substantial decrease in the ozone column is predicted as a result of the Pinatubo volcanic eruption, mostly in winter at middle and high latitudes. 62 refs., 18 figs., 3 tabs.

  5. X-ray micro-diffraction studies of heterogeneous interfaces between...

    Office of Scientific and Technical Information (OSTI)

    Article: X-ray micro-diffraction studies of heterogeneous interfaces between cementitious materials and geological formations Citation Details In-Document Search Title: X-ray ...

  6. Effective properties of a fly ash geopolymer: Synergistic application of X-ray synchrotron tomography, nanoindentation, and homogenization models

    SciTech Connect (OSTI)

    Das, Sumanta; Yang, Pu; Singh, Sudhanshu S.; Mertens, James C. E.; Xiao, Xianghui; Chawla, Nikhilesh; Neithalath, Narayanan

    2015-09-02

    Microstructural and micromechanical investigation of a fly ash-based geopolymer using: (i) synchrotron x-ray tomography (XRT) to determine the volume fraction and tortuosity of pores that are influential in fluid transport, (ii) mercury intrusion porosimetry (MIP) to capture the volume fraction of smaller pores, (iii) scanning electron microscopy (SEM) combined with multi-label thresholding to identify and characterize the solid phases in the microstructure, and (iv) nanoindentation to determine the component phase elastic properties using statistical deconvolution, is reported in this paper. The phase volume fractions and elastic properties are used in multi-step mean field homogenization (Mori- Tanaka and double inclusion) models to determine the homogenized macroscale elastic modulus of the composite. The homogenized elastic moduli are in good agreement with the flexural elastic modulus determined on macroscale paste beams. As a result, the combined use of microstructural and micromechanical characterization tools at multiple scales provides valuable information towards the material design of fly ash geopolymers.

  7. Towards graphyne molecular electronics (Journal Article) | SciTech...

    Office of Scientific and Technical Information (OSTI)

    of Publication: United States Language: English Subject: catalysis (heterogeneous), solar (photovoltaic), energy storage (including batteries and capacitors), hydrogen and...

  8. High-pressure phases of a hydrogen-rich compound: Tetramethylgermane...

    Office of Scientific and Technical Information (OSTI)

    of Publication: United States Language: English Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and...

  9. Constraint on the potassium content for the superconductivity...

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  10. Vibrational and structural properties of tetramethyltin under...

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    of Publication: United States Language: English Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and...

  11. Formation of Nanofoam carbon and re-emergence of Superconductivity...

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    of Publication: United States Language: English Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and...

  12. First-principles investigations on the magnetic property in tripotassi...

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    of Publication: United States Language: English Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and...

  13. Pressure induced superconductivity in CaC2 (Journal Article)...

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  14. Search for: All records | SciTech Connect

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    catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, charge ...

  15. Pressure-Driven Quantum Criticality in An Iron-Selenide Superconductor...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, ...

  16. Structural properties of BaFe1.8Ni0.2As2 under pressure (Journal...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, ...

  17. Pressure-induced phase coexistence in BaFe1.8Co0.2As2 (Journal...

    Office of Scientific and Technical Information (OSTI)

    Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, ...

  18. Structural feature controlling superconductivity in compressed...

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    Subject: catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy storage (including batteries and capacitors), hydrogen and fuel cells, superconductivity, ...

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  5. Thermal equation of state and spin transition of magnesiosiderite...

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  9. HeteroFoaM | U.S. DOE Office of Science (SC)

    Office of Science (SC) Website

    as fuel cells, batteries, supercapacitors, electrolyzers, and solid membranes. Research Topics: catalysis (heterogeneous), energy storage (including batteries and capacitors), ...

  10. Fluid Interface Reactions, Structures and Transport Center (FIRST...

    Office of Science (SC) Website

    Research Topics catalysis (heterogeneous), energy storage (including batteries and capacitors), charge transport, mesostructured materials, materials and chemistry by design, ...

  11. A quasi-Bohmian approach for a homogeneous spherical solid body based on its geometric structure

    SciTech Connect (OSTI)

    Koupaei, Jalaledin Yousefi; Institutes for Theoretical Physics and Mathematics , Tehran ; Golshani, Mehdi; Department of Physics, Sharif University of Technology, Tehran

    2013-12-15

    In this paper we express the space of rotation as a Riemannian space and try to generalize the classical equations of motion of a homogeneous spherical solid body in the domain of quantum mechanics. This is done within Bohm's view of quantum mechanics, but we do not use the Schrdinger equation. Instead, we assume that in addition to the classical potential there is an extra potential and try to obtain it. In doing this, we start from a classical picture based on Hamilton-Jacobi formalism and statistical mechanics but we use an interpretation which is different from the classical one. Then, we introduce a proper action and extremize it. This procedure gives us a mathematical identity for the extra potential that limits its form. The classical mechanics is a trivial solution of this method. In the simplest cases where the extra potential is not a constant, a mathematical identity determines it uniquely. In fact the first nontrivial potential, apart from some constant coefficients which are determined by experiment, is the usual Bohmian quantum potential.

  12. Structure transitions induced by the Hall term in homogeneous and isotropic magnetohydrodynamic turbulence

    SciTech Connect (OSTI)

    Miura, H., E-mail: miura.hideaki@nifs.ac.jp [Department of Helical Plasma Research, National Institute for Fusion Science, 322-6 Oroshi, Toki, Gifu 509-5292 (Japan); Araki, K. [Faculty of Engineering, Okayama University of Science, 1-1 Ridai-cho, Okayama 700-0005 (Japan)

    2014-07-15

    Hall effects on local structures in homogeneous, isotropic, and incompressible magnetohydrodynamic turbulence are studied numerically. The transition of vortices from sheet-like to tubular structures induced by the Hall term is found, while the kinetic energy spectrum does not distinguish the two types of structures. It is shown by the use of the sharp low-pass filter that the transition occurs not only in the scales smaller than the ion skin depth but also in a larger scale. The transition is related with the forward energy transfer in the spectral space. Analyses by the use of the sharp low-pass filter show that the nonlinear energy transfer associated with the Hall term is dominated by the forward transfer and relatively local in the wave number space. A projection of the simulation data to a Smagorinsky-type sub-grid-scale model shows that the high wave number component of the Hall term may possibly be replaced by the model effectively.

  13. Particle dispersion in homogeneous turbulence using the one-dimensional turbulence model

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

    Sun, Guangyuan; Lignell, David O.; Hewson, John C.; Gin, Craig R.

    2014-10-09

    Lagrangian particle dispersion is studied using the one-dimensional turbulence (ODT) model in homogeneous decaying turbulence configurations. The ODT model has been widely and successfully applied to a number of reacting and nonreacting flow configurations, but only limited application has been made to multiphase flows. We present a version of the particle implementation and interaction with the stochastic and instantaneous ODT eddy events. The model is characterized by comparison to experimental data of particle dispersion for a range of intrinsic particle time scales and body forces. Particle dispersion, velocity, and integral time scale results are presented. Moreover, the particle implementation introducesmore » a single model parameter β p , and sensitivity to this parameter and behavior of the model are discussed. Good agreement is found with experimental data and the ODT model is able to capture the particle inertial and trajectory crossing effects. Our results serve as a validation case of the multiphase implementations of ODT for extensions to other flow configurations.« less

  14. MOX recycling in GEN 3 + EPR Reactor homogeneous and stable full MOX core

    SciTech Connect (OSTI)

    Arslan, M.; Villele, E. de; Gauthier, J.C.; Marincic, A.

    2013-07-01

    In the case of the EPR (European Pressurized Reactor) reactor, 100% MOX core management is possible with simple design adaptations which are not significantly costly. 100% MOX core management offers several highly attractive advantages. First, it is possible to have the same plutonium content in all the rods of a fuel assembly instead of having rods with 3 different plutonium contents, as in MOX assemblies in current PWRs. Secondly, the full MOX core is more homogeneous. Thirdly, the stability of the core is significantly increased due to a large reduction in the Xe effect. Fourthly, there is a potential for the performance of the MOX fuel to match that of new high performance UO{sub 2} fuel (enrichment up to 4.95 %) in terms of increased burn up and cycle length. Fifthly, since there is only one plutonium content, the manufacturing costs are reduced. Sixthly, there is an increase in the operating margins of the reactor, and in the safety margins in accident conditions. The use of 100% MOX core will improve both utilisation of natural uranium resources and reductions in high level radioactive waste inventory.

  15. Localizing multiple X chromosome-linked retinitis pigmentosa loci using multilocus homogeneity tests

    SciTech Connect (OSTI)

    Ott, J.; Terwilliger, J.D. ); Bhattacharya, S. ); Chen, J.D.; Denton, J.; Donald, J. ); Dubay, C.; Litt, M.; Weleber, R.G. ); Farrar, G.J.; Humphries, P. ); Fishman, G.A.; Wong, F. ); Frey, D.; Maechler, M. )

    1990-01-01

    Multilocus linkage analysis of 62 family pedigrees with X chromosome-linked retinitis pigmentosa (XLRP) was undertaken to determine the presence of possible multiple disease loci and to reliability estimate their map location. Multilocus homogeneity tests furnish convincing evidence for the presence of two XLRP loci, the likelihood ratio being 6.4 {times} 10{sup 9}:1 in a favor of two versus a single XLRP locus and gave accurate estimates for their map location. In 60-75% of the families, location of an XLRP gene was estimated at 1 centimorgan distal to OTC, and in 25-40% of the families, an XLRP locus was located halfway between DXS14 (p58-1) and DXZ1 (Xcen), with an estimated recombination fraction of 25% between the two XLRP loci. There is also good evidence for third XLRP locus, midway between DXS28 (C7) and DXS164 (pERT87), supported by a likelihood ratio of 293:1 for three versus two XLRP loci.

  16. High Compositional Homogeneity of CdTexSe1-x Crystals Grown by the Bridgman Method

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

    Roy, U. N.; Bolotnikov, A. E.; Camarda, G. S.; Cui, Y.; Hossain, A.; Lee, K.; Lee, W.; Tappero, R.; Yang, G.; Gul, R.; et al

    2015-02-03

    We obtained high-quality CdTexSe1-x (CdTeSe) crystals from ingots grown by the vertical Bridgman technique. The compositional uniformity of the ingots was evaluated by X-ray fluorescence at BNL’s National Synchrotron Light Source X27A beam line. The resulting compositional homogeneity was highly uniform throughout the ingot, and the effective segregation coefficient of Se was ~1.0. This uniformity offers potential opportunity to enhance the yield of the materials for both infrared substrate and radiation-detector applications, so greatly lowering the cost of production and also offering us the prospect to grow large-diameter ingots for use as large-area substrates and for producing higher efficiency gamma-raymore » detectors. The concentration of secondary phases was found to be much lower, by eight- to ten fold compared to that of conventional CdxZn1-xTe (CdZnTe or CZT).« less

  17. Adapting SAFT-? perturbation theory to site-based molecular dynamics simulation. I. Homogeneous fluids

    SciTech Connect (OSTI)

    Ghobadi, Ahmadreza F.; Elliott, J. Richard

    2013-12-21

    In this work, we aim to develop a version of the Statistical Associating Fluid Theory (SAFT)-? equation of state (EOS) that is compatible with united-atom force fields, rather than experimental data. We rely on the accuracy of the force fields to provide the relation to experimental data. Although, our objective is a transferable theory of interfacial properties for soft and fused heteronuclear chains, we first clarify the details of the SAFT-? approach in terms of site-based simulations for homogeneous fluids. We show that a direct comparison of Helmholtz free energy to molecular simulation, in the framework of a third order Weeks-Chandler-Andersen perturbation theory, leads to an EOS that takes force field parameters as input and reproduces simulation results for Vapor-Liquid Equilibria (VLE) calculations. For example, saturated liquid density and vapor pressure of n-alkanes ranging from methane to dodecane deviate from those of the Transferable Potential for Phase Equilibria (TraPPE) force field by about 0.8% and 4%, respectively. Similar agreement between simulation and theory is obtained for critical properties and second virial coefficient. The EOS also reproduces simulation data of mixtures with about 5% deviation in bubble point pressure. Extension to inhomogeneous systems and united-atom site types beyond those used in description of n-alkanes will be addressed in succeeding papers.

  18. Analysis of Homogeneous Charge Compression Ignition (HCCI) Engines for Cogeneration Applications

    SciTech Connect (OSTI)

    Aceves, S; Martinez-Frias, J; Reistad, G

    2004-04-30

    This paper presents an evaluation of the applicability of Homogeneous Charge Compression Ignition Engines (HCCI) for small-scale cogeneration (less than 1 MWe) in comparison to five previously analyzed prime movers. The five comparator prime movers include stoichiometric spark-ignited (SI) engines, lean burn SI engines, diesel engines, microturbines and fuel cells. The investigated option, HCCI engines, is a relatively new type of engine that has some fundamental differences with respect to other prime movers. Here, the prime movers are compared by calculating electric and heating efficiency, fuel consumption, nitrogen oxide (NOx) emissions and capital and fuel cost. Two cases are analyzed. In Case 1, the cogeneration facility requires combined power and heating. In Case 2, the requirement is for power and chilling. The results show that the HCCI engines closely approach the very high fuel utilization efficiency of diesel engines without the high emissions of NOx and the expensive diesel fuel. HCCI engines offer a new alternative for cogeneration that provides a unique combination of low cost, high efficiency, low emissions and flexibility in operating temperatures that can be optimally tuned for cogeneration systems. HCCI engines are the most efficient technology that meets the oncoming 2007 CARB NOx standards for cogeneration engines. The HCCI engine appears to be a good option for cogeneration systems and merits more detailed analysis and experimental demonstration.

  19. Utilizing interfaces: One-step forward for rational design of heterogeneous catalysts

    SciTech Connect (OSTI)

    Kim H. Y.

    2013-06-20

    As far as heterogeneous catalysts are a composite material, physicochemical properties of the interfaces between individual components should be extensively studied for rational design of catalysts with desired properties. Here, I will present recent computational achievements in following three heterogeneous catalysts where the interface between composing materials plays a critical role

  20. A comparison of unburned fuel and aldehyde emissions from a methanol-fueled stratified charge and homogeneous charge engine

    SciTech Connect (OSTI)

    Foster, D.E.; Kim, C.; Scull, N.

    1987-03-01

    This paper presents the results of an experimental program in which a Texaco L-163S engine was fueled with methanol and operated in its traditional stratified charge mode and then modified to run as a homogeneous charge spark ignited engine. The primary data taken were the aldehyde and unburned fuel emissions (UBF). Those data were taken using a continuous time-averaging sampling probe at the exhaust tank and at the exhaust port and with a rotary time-resolving sampling valve located at the exhaust port. The data are for two loads, 138.1 kPa (20 psi) and 207.1 kPa (30 psi) BMEP and three speeds, 1000, 1400 and 1800 rpm. The data indicate that both the stratified charge and the homogeneous charge modes of operation formaldehyde was the only aldehyde detected in the exhaust and it primarily originated in the exhaust and it primarily originated in the cylinder. Over the load and speed ranges tested, the unburned fuel emission were higher and the formaldehyde emission lower when comparing the stratified charge to the homogeneous charge operation. Time resolved data at the exhaust port for the two modes of operation are compared. The homogeneous charge operation had a uniform concentration of both unburned fuel and formaldehyde over the exhaust stroke. The stratified charge data shows large changes in the unburned fuel and moderate changes in the aldehyde concentrations during the exhaust stroke.

  1. Cavitation in a metallic liquid: Homogeneous nucleation and growth of nanovoids

    SciTech Connect (OSTI)

    Cai, Y.; Wu, H. A.; Luo, S. N.

    2014-06-07

    Large-scale molecular dynamics (MD) simulations are performed to investigate homogeneous nucleation and growth of nanovoids during cavitation in liquid Cu. We characterize in detail the atomistic cavitation processes by following the temporal evolution of cavities or voids, analyze the nucleation behavior with the mean first-passage time (MFPT) and survival probability (SP) methods, and discuss the results against classical nucleation theory (CNT), the Tolman equation for surface energy, independent calculation of surface tension via integrating the stress profiles, the Johnson-Mehl-Avrami (JMA) growth law, and the power law for nucleus size distributions. Cavitation in this representative metallic liquid is a high energy barrier Poisson processes, and the steady-state nucleation rates obtained from statistical runs with the MFPT and SP methods are in agreement. The MFPT method also yields the critical nucleus size and the Zeldovich factor. Fitting with the Tolman's equation to the MD simulations yields the surface energy of a planar interface (∼0.9 J m{sup −2}) and the Tolman length (0.4–0.5 Å), and those values are in accord with those from integrating the stress profiles of a planar interface. Independent CNT predictions of the nucleation rate (10{sup 33−34} s{sup −1} m{sup −3}) and critical size (3–4 Å in radius) are in agreement with the MFPT and SP results. The JMA law can reasonably describe the nucleation and growth process. The size distribution of subcritical nuclei appears to follow a power law with an exponent decreasing with increasing tension owing to coupled nucleation and growth, and that of the supercritical nuclei becomes flattened during further stress relaxation due to void coalescence.

  2. Tidal dissipation in a homogeneous spherical body. II. Three examples: Mercury, Io, and Kepler-10 b

    SciTech Connect (OSTI)

    Makarov, Valeri V.; Efroimsky, Michael E-mail: michael.efroimsky@usno.navy.mil

    2014-11-01

    In Efroimsky and Makarov (Paper I), we derived from the first principles a formula for the tidal heating rate in a homogeneous sphere, compared it with the previously used formulae, and noted the differences. Now we present case studies: Mercury, Kepler-10 b, and a triaxial Io. A sharp frequency dependence of k {sub 2}/Q near spin-orbit resonances yields a sharp dependence of k {sub 2}/Q (and, therefore, of tidal heating) upon the spin rate. Thereby physical libration plays a major role in tidal heating of synchronously rotating planets. The magnitude of libration in the spin rate being defined by the planet's triaxiality, the latter becomes a factor determining the dissipation rate. Other parameters equal, a strongly triaxial synchronized body generates more heat than a similar body of a more symmetrical shape. After an initially triaxial object melts and loses its triaxiality, dissipation becomes less intensive; the body can solidify, with the tidal bulge becoming a new figure with triaxiality lower than the original. We derive approximate expressions for the dissipation rate in a Maxwell planet with the Maxwell time longer than the inverse tidal frequency. The expressions derived pertain to the 1:1 and 3:2 resonances and a nonresonant case; so they are applicable to most close-in super-Earths detected. In these planets, the heating outside synchronism is weakly dependent on the eccentricity and obliquity, provided both these parameters's values are moderate. According to our calculation, Kepler-10 b could hardly survive the intensive tidal heating without being synchronized, circularized, and reshaped through a complete or partial melt-down.

  3. Heterogeneity and dynamics in villin headpiece crystal structures

    SciTech Connect (OSTI)

    Meng, Jianmin; McKnight, Christopher James, E-mail: cjmck@bu.edu [Boston University School of Medicine (United States)

    2009-05-01

    New crystal structures of the well studied protein-folding model system villin headpiece in a new space group provide insights into the conformations available in the folded state. The villin headpiece domain (HP67) is the C-terminal F-actin-binding motif that confers F-actin-bundling activity to villin, a component of the actin bundles that support the brush-border microvilli. It has been investigated extensively by both experimental and theoretical measurements. Our laboratory, for example, has determined both its NMR and its crystal structures. This study presents the structures of HP67 and its pH-stabilized mutant (H41Y) in a different crystal form and space group. For both constructs, two molecules are found in each asymmetric unit in the new space group P6{sub 1}. While one of the two structures (Mol A) is structurally similar to our previously determined structure (Mol X), the other (Mol B) has significant deviations, especially in the N-terminal subdomain, where lattice contacts do not appear to contribute to the difference. In addition, the structurally most different crystal structure, Mol B, is actually closer to the averaged NMR structure. Harmonic motions, as suggested by the B-factor profiles, differ between these crystal structures; crystal structures from the same space group share a similar pattern. Thus, heterogeneity and dynamics are observed in different crystal structures of the same protein even for a protein as small as villin headpiece.

  4. A Method for Correcting IMRT Optimizer Heterogeneity Dose Calculations

    SciTech Connect (OSTI)

    Zacarias, Albert S.; Brown, Mellonie F. Mills, Michael D.

    2010-04-01

    Radiation therapy treatment planning for volumes close to the patient's surface, in lung tissue and in the head and neck region, can be challenging for the planning system optimizer because of the complexity of the treatment and protected volumes, as well as striking heterogeneity corrections. Because it is often the goal of the planner to produce an isodose plan with uniform dose throughout the planning target volume (PTV), there is a need for improved planning optimization procedures for PTVs located in these anatomical regions. To illustrate such an improved procedure, we present a treatment planning case of a patient with a lung lesion located in the posterior right lung. The intensity-modulated radiation therapy (IMRT) plan generated using standard optimization procedures produced substantial dose nonuniformity across the tumor caused by the effect of lung tissue surrounding the tumor. We demonstrate a novel iterative method of dose correction performed on the initial IMRT plan to produce a more uniform dose distribution within the PTV. This optimization method corrected for the dose missing on the periphery of the PTV and reduced the maximum dose on the PTV to 106% from 120% on the representative IMRT plan.

  5. Inverse problems in heterogeneous and fractured media using peridynamics

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

    Turner, Daniel Z.; van Bloemen Waanders, Bart G.; Parks, Michael L.

    2015-12-10

    The following work presents an adjoint-based methodology for solving inverse problems in heterogeneous and fractured media using state-based peridynamics. We show that the inner product involving the peridynamic operators is self-adjoint. The proposed method is illustrated for several numerical examples with constant and spatially varying material parameters as well as in the context of fractures. We also present a framework for obtaining material parameters by integrating digital image correlation (DIC) with inverse analysis. This framework is demonstrated by evaluating the bulk and shear moduli for a sample of nuclear graphite using digital photographs taken during the experiment. The resulting measuredmore » values correspond well with other results reported in the literature. Lastly, we show that this framework can be used to determine the load state given observed measurements of a crack opening. Furthermore, this type of analysis has many applications in characterizing subsurface stress-state conditions given fracture patterns in cores of geologic material.« less

  6. Aggregate Model for Heterogeneous Thermostatically Controlled Loads with Demand Response

    SciTech Connect (OSTI)

    Zhang, Wei; Kalsi, Karanjit; Fuller, Jason C.; Elizondo, Marcelo A.; Chassin, David P.

    2012-07-22

    Due to the potentially large number of Distributed Energy Resources (DERs) demand response, distributed generation, distributed storage - that are expected to be deployed, it is impractical to use detailed models of these resources when integrated with the transmission system. Being able to accurately estimate the fast transients caused by demand response is especially important to analyze the stability of the system under different demand response strategies. On the other hand, a less complex model is more amenable to design feedback control strategies for the population of devices to provide ancillary services. The main contribution of this paper is to develop aggregated models for a heterogeneous population of Thermostatic Controlled Loads (TCLs) to accurately capture their collective behavior under demand response and other time varying effects of the system. The aggregated model efficiently includes statistical information of the population and accounts for a second order effect necessary to accurately capture the collective dynamic behavior. The developed aggregated models are validated against simulations of thousands of detailed building models using GridLAB-D (an open source distribution simulation software) under both steady state and severe dynamic conditions caused due to temperature set point changes.

  7. Supporting Dynamic Spectrum Access in Heterogeneous LTE+ Networks

    SciTech Connect (OSTI)

    Luiz A. DaSilva; Ryan E. Irwin; Mike Benonis

    2012-08-01

    As early as 2014, mobile network operators’ spectral capac- ity is expected to be overwhelmed by the demand brought on by new devices and applications. With Long Term Evo- lution Advanced (LTE+) networks likely as the future one world 4G standard, network operators may need to deploy a Dynamic Spectrum Access (DSA) overlay in Heterogeneous Networks (HetNets) to extend coverage, increase spectrum efficiency, and increase the capacity of these networks. In this paper, we propose three new management frameworks for DSA in an LTE+ HetNet: Spectrum Accountability Client, Cell Spectrum Management, and Domain Spectrum Man- agement. For these spectrum management frameworks, we define protocol interfaces and operational signaling scenar- ios to support cooperative sensing, spectrum lease manage- ment, and alarm scenarios for rule adjustment. We also quan- tify, through integer programs, the benefits of using DSA in an LTE+ HetNet, that can opportunistically reuse vacant TV and GSM spectrum. Using integer programs, we consider a topology using Geographic Information System data from the Blacksburg, VA metro area to assess the realistic benefits of DSA in an LTE+ HetNet.

  8. Comparison of unburned fuel and aldehyde emissions from a methanol-fueled stratified charge and homogeneous charge engine

    SciTech Connect (OSTI)

    Scull, N.; Kim, C.; Foster, D.E.

    1986-01-01

    This paper presents the results of an experimental program in which a Texaco L-163S engine was fueled with methanol and operated in its traditional stratified charge mode and then modified to run as a homogenous charge spark ignited engine. The primary data taken were the aldehyde and unburned fuel emissions (UBF). These data were taken using a continuous time-averaging sampling probe at the exhaust tank and at the exhaust port and with a rotary time-resolving sampling valve located at the exhaust port. The data indicate that for both the stratified charge and the homogeneous charge modes of operation formaldehyde was the only aldehyde detected in the exhaust and it primarily originated in the cylinder.

  9. Effective properties of a fly ash geopolymer: Synergistic application of X-ray synchrotron tomography, nanoindentation, and homogenization models

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

    Das, Sumanta; Yang, Pu; Singh, Sudhanshu S.; Mertens, James C. E.; Xiao, Xianghui; Chawla, Nikhilesh; Neithalath, Narayanan

    2015-09-02

    Microstructural and micromechanical investigation of a fly ash-based geopolymer using: (i) synchrotron x-ray tomography (XRT) to determine the volume fraction and tortuosity of pores that are influential in fluid transport, (ii) mercury intrusion porosimetry (MIP) to capture the volume fraction of smaller pores, (iii) scanning electron microscopy (SEM) combined with multi-label thresholding to identify and characterize the solid phases in the microstructure, and (iv) nanoindentation to determine the component phase elastic properties using statistical deconvolution, is reported in this paper. The phase volume fractions and elastic properties are used in multi-step mean field homogenization (Mori- Tanaka and double inclusion) modelsmore » to determine the homogenized macroscale elastic modulus of the composite. The homogenized elastic moduli are in good agreement with the flexural elastic modulus determined on macroscale paste beams. As a result, the combined use of microstructural and micromechanical characterization tools at multiple scales provides valuable information towards the material design of fly ash geopolymers.« less

  10. New Homogeneous Standards by Atomic Layer Deposition for Synchrotron X-ray Fluorescence and Absorption Spectroscopies.

    SciTech Connect (OSTI)

    Butterworth, A.L.; Becker, N.; Gainsforth, Z.; Lanzirotti, A.; Newville, M.; Proslier, T.; Stodolna, J.; Sutton, S.; Tyliszczak, T.; Westphal, A.J.; Zasadzinski, J. (UCB)

    2012-03-13

    Quantification of synchrotron XRF analyses is typically done through comparisons with measurements on the NIST SRM 1832/1833 thin film standards. Unfortunately, these standards are inhomogeneous on small scales at the tens of percent level. We are synthesizing new homogeneous multilayer standards using the Atomic Layer Deposition technique and characterizing them using multiple analytical methods, including ellipsometry, Rutherford Back Scattering at Evans Analytical, Synchrotron X-ray Fluorescence (SXRF) at Advanced Photon Source (APS) Beamline 13-ID, Synchrotron X-ray Absorption Spectroscopy (XAS) at Advanced Light Source (ALS) Beamlines 11.0.2 and 5.3.2.1 and by electron microscopy techniques. Our motivation for developing much-needed cross-calibration of synchrotron techniques is borne from coordinated analyses of particles captured in the aerogel of the NASA Stardust Interstellar Dust Collector (SIDC). The Stardust Interstellar Dust Preliminary Examination (ISPE) team have characterized three sub-nanogram, {approx}1{micro}m-sized fragments considered as candidates to be the first contemporary interstellar dust ever collected, based on their chemistries and trajectories. The candidates were analyzed in small wedges of aerogel in which they were extracted from the larger collector, using high sensitivity, high spatial resolution >3 keV synchrotron x-ray fluorescence spectroscopy (SXRF) and <2 keV synchrotron x-ray transmission microscopy (STXM) during Stardust ISPE. The ISPE synchrotron techniques have complementary capabilities. Hard X-ray SXRF is sensitive to sub-fg mass of elements Z {ge} 20 (calcium) and has a spatial resolution as low as 90nm. X-ray Diffraction data were collected simultaneously with SXRF data. Soft X-ray STXM at ALS beamline 11.0.2 can detect fg-mass of most elements, including cosmochemically important oxygen, magnesium, aluminum and silicon, which are invisible to SXRF in this application. ALS beamline 11.0.2 has spatial resolution better than 25 nm. Limiting factors for Stardust STXM analyses were self-imposed limits of photon dose due to radiation damage concerns, and significant attenuation of <1500 eV X-rays by {approx}80{micro}m thick, {approx}25 mg/cm{sup 3} density silica aerogel capture medium. In practice, the ISPE team characterized the major, light elements using STXM (O, Mg, Al, Si) and the heavier minor and trace elements using SXRF. The two data sets overlapped only with minor Fe and Ni ({approx}1% mass abundance), providing few quantitative cross-checks. New improved standards for cross calibration are essential for consortium-based analyses of Stardust interstellar and cometary particles, IDPs. Indeed, they have far reaching application across the whole synchrotron-based analytical community. We have synthesized three ALD multilayers simultaneously on silicon nitride membranes and silicon and characterized them using RBS (on Si), XRF (on Si{sub 3}N{sub 4}) and STXM/XAS (holey Si{sub 3}N{sub 4}). The systems we have started to work with are Al-Zn-Fe and Y-Mg-Er. We have found these ALD multi-layers to be uniform at {micro}m- to nm scales, and have found excellent consistency between four analytical techniques so far. The ALD films can also be used as a standard for e-beam instruments, eg., TEM EELS or EDX. After some early issues with the consistency of coatings to the back-side of the membrane windows, we are confident to be able to show multi-analytical agreement to within 10%. As the precision improves, we can use the new standards to verify or improve the tabulated cross-sections.

  11. Complexity analysis of pipeline mapping problems in distributed heterogeneous networks

    SciTech Connect (OSTI)

    Lin, Ying; Wu, Qishi; Zhu, Mengxia; Rao, Nageswara S

    2009-04-01

    Largescale scientific applications require using various system resources to execute complex computing pipelines in distributed networks to support collaborative research. System resources are typically shared in the Internet or over dedicated connections based on their location, availability, capability, and capacity. Optimizing the network performance of computing pipelines in such distributed environments is critical to the success of these applications. We consider two types of largescale distributed applications: (1) interactive applications where a single dataset is sequentially processed along a pipeline; and (2) streaming applications where a series of datasets continuously flow through a pipeline. The computing pipelines of these applications consist of a number of modules executed in a linear order in network environments with heterogeneous resources under different constraints. Our goal is to find an efficient mapping scheme that allocates the modules of a pipeline to network nodes for minimum endtoend delay or maximum frame rate. We formulate the pipeline mappings in distributed environments as optimization problems and categorize them into six classes with different optimization goals and mapping constraints: (1) Minimum Endtoend Delay with No Node Reuse (MEDNNR), (2) Minimum Endtoend Delay with Contiguous Node Reuse (MEDCNR), (3) Minimum Endtoend Delay with Arbitrary Node Reuse (MEDANR), (4) Maximum Frame Rate with No Node Reuse or Share (MFRNNRS), (5) Maximum Frame Rate with Contiguous Node Reuse and Share (MFRCNRS), and (6) Maximum Frame Rate with Arbitrary Node Reuse and Share (MFRANRS). Here, 'contiguous node reuse' means that multiple contiguous modules along the pipeline may run on the same node and 'arbitrary node reuse' imposes no restriction on node reuse. Note that in interactive applications, a node can be reused but its resource is not shared. We prove that MEDANR is polynomially solvable and the rest are NP-complete. MEDANR, where either contiguous or noncontiguous modules in the pipeline can be mapped onto the same node, is essentially the Maximum n-hop Shortest Path problem, and can be solved using a dynamic programming method. In MEDNNR and MFRNNRS, any network node can be used only once, which requires selecting the same number of nodes for onetoone onto mapping. We show its NP-completeness by reducing from the Hamiltonian Path problem. Node reuse is allowed in MEDCNR, MFRCNRS and MFRANRS, which are similar to the Maximum n-hop Shortest Path problem that considers resource sharing. We prove their NP-completeness by reducing from the Disjoint-Connecting-Path Problem and Widest path with the Linear Capacity Constraints problem, respectively.

  12. Isotoxic Dose Escalation in the Treatment of Lung Cancer by Means of Heterogeneous Dose Distributions in the Presence of Respiratory Motion

    SciTech Connect (OSTI)

    Baker, Mariwan; Nielsen, Morten [Laboratory of Radiation Physics, Odense University Hospital, Odense (Denmark); Hansen, Olfred [Department of Oncology, Odense University Hospital, Odense (Denmark); Jahn, Jonas Westberg [Laboratory of Radiation Physics, Odense University Hospital, Odense (Denmark); Korreman, Stine [Department of Radiation Oncology, Copenhagen University Hospital, Copenhagen (Denmark); Brink, Carsten, E-mail: carsten.brink@ouh.regionsyddanmark.dk [Laboratory of Radiation Physics, Odense University Hospital, Odense (Denmark); Institute of Clinical Research, University of Southern Denmark, Odense (Denmark)

    2011-11-01

    Purpose: To test, in the presence of intrafractional respiration movement, a margin recipe valid for a homogeneous and conformal dose distribution and to test whether the use of smaller margins combined with heterogeneous dose distributions allows an isotoxic dose escalation when respiratory motion is considered. Methods and Materials: Twenty-three Stage II-III non-small-cell lung cancer patients underwent four-dimensional computed tomography scanning. The gross tumor volume and clinical target volume (CTV) were outlined in the mid-ventilation phase. The CTV-to-planning target volume (PTV) margin was calculated by use of a standard margin recipe and the patient-specific respiration pattern. Standard three-dimensional treatment plans were generated and recalculated on the remaining respiration phases. The planning was repeated for a CTV-to-PTV margin decreased by 2.5 and 5 mm relative to the initial margin in all directions. Time-averaged dose-volume histograms (four-dimensional dose-volume histograms) were calculated to evaluate the CTV-to-PTV margin. Finally, the dose was escalated in the plans with decreased PTV such that the mean lung dose (predictor of radiation-induced pneumonitis) was equal to mean lung dose in the plan by use of the initially calculated margin. Results: A reduction of the standard margin by 2.5 mm compared with the recipe resulted in too low of a minimum dose for some patients. A combination of dose escalation and use of heterogeneous dose distribution was able to increase the minimum dose to the target by approximately 10% and 20% for a CTV-to-PTV margin reduction of 2.5 mm and 5.0 mm, respectively. Conclusion: The margin recipe is valid for intrafractional respiration-induced tumor motions. It is possible to increase the dose to the target without increased mean lung dose with an inhomogeneous dose distribution.

  13. Influence of heterogeneity on second-kind self-similar solutions...

    Office of Scientific and Technical Information (OSTI)

    a heterogeneous porous medium whose permeability and porosity have power-law variations. ... that propagate away from the origin (a point of zero permeability); (b) a second-kind ...

  14. Resolving Cancer Heterogeneity by Single Cell Sequencing (7th Annual SFAF Meeting, 2012)

    ScienceCinema (OSTI)

    Xu, Xun [BGI

    2013-02-11

    Xun Xu on "Resolving Cancer Heterogeneity by Single Cell Sequencing" at the 2012 Sequencing, Finishing, Analysis in the Future Meeting held June 5-7, 2012 in Santa Fe, New Mexico.

  15. New Helical Foldamers: Heterogeneous Backbones with 1:2 and 2...

    Office of Scientific and Technical Information (OSTI)

    New Helical Foldamers: Heterogeneous Backbones with 1:2 and 2:1 alpha:superscript beta-Amino Acid Residue Patterns Citation Details In-Document Search Title: New Helical ...

  16. X-ray micro-diffraction studies of heterogeneous interfaces between

    Office of Scientific and Technical Information (OSTI)

    cementitious materials and geological formations (Journal Article) | SciTech Connect SciTech Connect Search Results Journal Article: X-ray micro-diffraction studies of heterogeneous interfaces between cementitious materials and geological formations Citation Details In-Document Search Title: X-ray micro-diffraction studies of heterogeneous interfaces between cementitious materials and geological formations Authors: Dähn, R. ; Popov, D. ; Schaub, Ph. ; Pattison, P. ; Grolimund, D. ; Mäder,

  17. EFFECTS OF PORE STRUCTURE CHANGE AND MULTI-SCALE HETEROGENEITY ON

    Office of Scientific and Technical Information (OSTI)

    CONTAMINANT TRANSPORT AND REACTION RATE UPSCALING (Technical Report) | SciTech Connect Technical Report: EFFECTS OF PORE STRUCTURE CHANGE AND MULTI-SCALE HETEROGENEITY ON CONTAMINANT TRANSPORT AND REACTION RATE UPSCALING Citation Details In-Document Search Title: EFFECTS OF PORE STRUCTURE CHANGE AND MULTI-SCALE HETEROGENEITY ON CONTAMINANT TRANSPORT AND REACTION RATE UPSCALING This project addressed the scaling of geochemical reactions to core and field scales, and the interrelationship

  18. The scale dependence of dispersivity in multi-faces heterogeneous sediments

    Office of Scientific and Technical Information (OSTI)

    (Journal Article) | SciTech Connect The scale dependence of dispersivity in multi-faces heterogeneous sediments Citation Details In-Document Search Title: The scale dependence of dispersivity in multi-faces heterogeneous sediments Early work on stochastic modeling of the transport of inert solutes in porous media assumed that log conductivity could be characterized by a single, finite integral scale representing the spatial correlation of log conductivity. In this study, we focused on

  19. Design, Synthesis, and Mechanistic Evaluation of Iron-Based Catalysis for Synthesis Gas Conversion to Fuels and Chemicals

    SciTech Connect (OSTI)

    Enrique Iglesia; Akio Ishikawa; Manual Ojeda; Nan Yao

    2007-09-30

    A detailed study of the catalyst composition, preparation and activation protocol of Fe-based catalysts for the Fischer-Tropsch Synthesis (FTS) have been carried out in this project. We have studied the effects of different promoters on the catalytic performance of Fe-based catalysts. Specifically, we have focused on how their sequence of addition dramatically influences the performance of these materials in the Fischer-Tropsch synthesis. The resulting procedures have been optimized to improve further upon the already unprecedented rates and C{sub 5+} selectivities of the Fe-based catalysts that we have developed as part of this project. Selectivity to C{sub 5+} hydrocarbon was close to 90 % (CO{sub 2}-free basis) and CO conversion rate was about 6.7 mol h{sup -1} g-at Fe{sup -1} at 2.14 MPa, 508 K and with substoichiometric synthesis gas; these rates were larger than any reported previously for Fe-based FTS catalysts at these conditions. We also tested the stability of Fe-based catalysts during FTS reaction (10 days); as a result, the high hydrocarbon formation rates were maintained during 10 days, though the gradual deactivation was observed. Our investigation has also focused on the evaluation of Fe-based catalysts with hydrogen-poor synthesis gas streams (H{sub 2}/CO=1). We have observed that the Fe-based catalysts prepared in this project display also a high hydrocarbon synthesis rate with substoichiometric synthesis gas (H{sub 2}/CO=1) stream, which is a less desirable reactant mixture than stoichiometric synthesis gas (H{sub 2}/CO=2). We have improved the catalyst preparation protocols and achieved the highest FTS reaction rates and selectivities so far reported at the low temperatures required for selectivity and stability. Also, we have characterized the catalyst structural change and active phases formed, and their catalytic behavior during the activation process to evaluate their influences on FTS reaction. The efforts of this project led to (i) structural evolution of Fe-Zn oxide promoted with K and Cu, and (ii) evaluation of hydrocarbon and CH{sub 4} formation rates during activation procedures at various temperature and H{sub 2}/CO ratios. On the basis of the obtained results, we suggest that lower reactor temperature can be sufficient to activate catalysts and lead to the high FTS performance. In this project, we have also carried out a detailed kinetic and mechanistic study of the Fischer-Tropsch Synthesis with Fe-based catalysts. We have proposed a reaction mechanism with two CO activation pathways: unassisted and H-assisted. Both routes lead to the formation of the same surface monomers (CH{sub 2}). However, the oxygen removal mechanism is different. In the H-assisted route, oxygen is removed exclusively as water, while oxygen is rejected as carbon dioxide in the unassisted CO dissociation. The validity of the mechanism here proposed has been found to be in agreement with the experimental observation and with theoretical calculations over a Fe(110) surface. Also, we have studied the validity of the mechanism that we propose by analyzing the H{sub 2}/D{sub 2} kinetic isotope effect (r{sub H}/r{sub D}) over a conventional iron-based Fischer-Tropsch catalyst Fe-Zn-K-Cu. We have observed experimentally that the use of D{sub 2} instead of H{sub 2} leads to higher hydrocarbons formation rates (inverse kinetic isotopic effect). On the contrary, primary carbon dioxide formation is not influenced. These experimental observations can be explained by two CO activation pathways. We have also explored the catalytic performance of Co-based catalysts prepared by using inverse micelles techniques. We have studied several methods in order to terminate the silanol groups on SiO{sub 2} support including impregnation, urea homogeneous deposition-precipitation, or zirconium (IV) ethoxide titration. Although hydroxyl groups on the SiO{sub 2} surface are difficult to be stoichiometrically titrated by ZrO{sub 2}, a requirement to prevent the formation of strongly-interacting Co oxide species on SiO{sub 2}, modification of ZrO{sub 2} on SiO{sub 2} surface can improve the Co clusters dispersion leading to a marked increase in the number of accessible Co sites. Inverse micelle method allowed the synthesis of small Co clusters on SiO{sub 2}, but the required surfactant removal steps led to the re-oxidation of Co metal clusters and to the formation of difficult to reduce CoO{sub x} species.

  20. IMPROVING CO2 EFFICIENCY FOR RECOVERING OIL IN HETEROGENEOUS RESERVOIRS

    SciTech Connect (OSTI)

    Reid B. Grigg; Robert K. Svec

    2002-12-20

    This document is the First Annual Report for the U.S. Department of Energy under contract No., a three-year contract entitled: ''Improving CO{sub 2} Efficiency for Recovering Oil in Heterogeneous Reservoirs.'' The research improved our knowledge and understanding of CO{sub 2} flooding and includes work in the areas of injectivity and mobility control. The bulk of this work has been performed by the New Mexico Petroleum Recovery Research Center, a research division of New Mexico Institute of Mining and Technology. This report covers the reporting period of September 28, 2001 and September 27, 2002. Injectivity continues to be a concern to the industry. During this period we have contacted most of the CO{sub 2} operators in the Permian Basin and talked again about their problems in this area. This report has a summary of what we found. It is a given that carbonate mineral dissolution and deposition occur in a formation in geologic time and are expected to some degree in carbon dioxide (CO{sub 2}) floods. Water-alternating-gas (WAG) core flood experiments conducted on limestone and dolomite core plugs confirm that these processes can occur over relatively short time periods (hours to days) and in close proximity to each other. Results from laboratory CO{sub 2}-brine flow experiments performed in rock core were used to calibrate a reactive transport simulator. The calibrated model is being used to estimate in situ effects of a range of possible sequestration options in depleted oil/gas reservoirs. The code applied in this study is a combination of the well known TOUGH2 simulator, for coupled groundwater/brine and heat flow, with the chemistry code TRANS for chemically reactive transport. Variability in response among rock types suggests that CO{sub 2} injection will induce ranges of transient and spatially dependent changes in intrinsic rock permeability and porosity. Determining the effect of matrix changes on CO{sub 2} mobility is crucial in evaluating the efficacy and potential environmental implications of storing CO{sub 2} in the subsurface. Chemical cost reductions are identified that are derived from the synergistic effects of cosurfactant systems using a good foaming agent and a less expensive poor foaming agent. The required good foaming agent is reduced by at least 75%. Also the effect on injectivity is reduced by as much as 50% using the cosurfactant system, compared to a previously used surfactant system. Mobility control of injected CO{sub 2} for improved oil recovery can be achieved with significant reduction in the chemical cost of SAG, improved injectivity of SAG, and improved economics of CO{sub 2} injection project when compared to reported systems. Our past work has identified a number of mobility control agents to use for CO{sub 2}-foam flooding. In particular the combination of the good foaming agent CD 1045 and a sacrificial agent and cosurfactant lignosulfonate. This work scrutinizes the methods that we are using to determine the efficiency of the sacrificial agents and cosurfactant systems. These have required concentration determinations and reusing core samples. Here, we report some of the problems that have been found and some interesting effects that must be considered.

  1. Significant enhancement of compositional and superconducting homogeneity in Ti rather than Ta-doped Nb3Sn

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

    Tarantini, C.; Sung, Z. -H.; Lee, P. J.; Ghosh, A. K.; Larbalestier, D. C.

    2016-01-25

    Nb3Sn wires are now very close to their final optimization but despite its classical nature, detailed understanding of the role of Ta and Ti doping in the A15 is not fully understood. Long thought to be essentially equivalent in their influence on Hc2, they were interchangeably applied. Here we show that Ti produces significantly more homogeneous chemical and superconducting properties. Despite Ta-doped samples having a slightly higher Tc onset in zero-field, they always have a wider Tc-distribution. In particular, whereas the Ta-doped A15 has a Tc-distribution extending from 18 down to 5-6 K (the lowest expected Tc for the binarymore » A15 phase), the Ti-doped samples have no A15 phase with Tc below ~12 K. The much narrower Tc distribution in the Ti-doped samples has a positive effect on their in-field Tc-distribution too, leading to an extrapolated μ0Hc2(0) 2 Tesla larger than the Ta-doped one. Ti-doping also appears to be very homogeneous even when the Sn content is reduced in order to inhibit breakdown of the diffusion barriers in very high Jc conductors. As a result, the enhanced homogeneity of the Ti-doped samples appears to result from its assistance of rapid diffusion of Sn into the filaments and by its incorporation into the A15 phase interchangeably with Sn on the Sn sites of the A15 phase.« less

  2. Scaling Effects of Cr(VI) Reduction Kinetics. The Role of Geochemical Heterogeneity

    SciTech Connect (OSTI)

    Wang, Li; Li, Li

    2015-10-22

    The natural subsurface is highly heterogeneous with minerals distributed in different spatial patterns. Fundamental understanding of how mineral spatial distribution patterns regulate sorption process is important for predicting the transport and fate of chemicals. Existing studies about the sorption was carried out in well-mixed batch reactors or uniformly packed columns, with few data available on the effects of spatial heterogeneities. As a result, there is a lack of data and understanding on how spatial heterogeneities control sorption processes. In this project, we aim to understand and develop modeling capabilities to predict the sorption of Cr(VI), an omnipresent contaminant in natural systems due to its natural occurrence and industrial utilization. We systematically examine the role of spatial patterns of illite, a common clay, in determining the extent of transport limitation and scaling effects associated with Cr(VI) sorption capacity and kinetics using column experiments and reactive transport modeling. Our results showed that the sorbed mass and rates can differ by an order of magnitude due to of the illite spatial heterogeneities and transport limitation. With constraints from data, we also developed the capabilities of modeling Cr(VI) in heterogeneous media. The developed model is then utilized to understand the general principles that govern the relationship between sorption and connectivity, a key measure of the spatial pattern characteristics. This correlation can be used to estimate Cr(VI) sorption characteristics in heterogeneous porous media. Insights gained here bridge gaps between laboratory and field application in hydrogeology and geochemical field, and advance predictive understanding of reactive transport processes in the natural heterogeneous subsurface. We believe that these findings will be of interest to a large number of environmental geochemists and engineers, hydrogeologists, and those interested in contaminant fate and transport, water quality and water composition, and natural attenuation processes in natural systems.

  3. Visible-Light Photoredox Catalysis: Selective Reduction of Carbon Dioxide to Carbon Monoxide by a Nickel N-Heterocyclic Carbene-Isoquinoline Complex

    SciTech Connect (OSTI)

    Thoi, VanSara; Kornienko, Nick; Margarit, C; Yang, Peidong; Chang, Christopher

    2013-06-07

    The solar-driven reduction of carbon dioxide to value-added chemical fuels is a longstanding challenge in the fields of catalysis, energy science, and green chemistry. In order to develop effective CO2 fixation, several key considerations must be balanced, including (1) catalyst selectivity for promoting CO2 reduction over competing hydrogen generation from proton reduction, (2) visible-light harvesting that matches the solar spectrum, and (3) the use of cheap and earth-abundant catalytic components. In this report, we present the synthesis and characterization of a new family of earth-abundant nickel complexes supported by N-heterocyclic carbene amine ligands that exhibit high selectivity and activity for the electrocatalytic and photocatalytic conversion of CO2 to CO. Systematic changes in the carbene and amine donors of the ligand have been surveyed, and [Ni(Prbimiq1)]2+ (1c, where Prbimiq1 = bis(3-(imidazolyl)isoquinolinyl)propane) emerges as a catalyst for electrochemical reduction of CO2 with the lowest cathodic onset potential (Ecat = 1.2 V vs SCE). Using this earth-abundant catalyst with Ir(ppy)3 (where ppy = 2-phenylpyridine) and an electron donor, we have developed a visible-light photoredox system for the catalytic conversion of CO2 to CO that proceeds with high selectivity and activity and achieves turnover numbers and turnover frequencies reaching 98,000 and 3.9 s1, respectively. Further studies reveal that the overall efficiency of this solar-to-fuel cycle may be limited by the formation of the active Ni catalyst and/or the chemical reduction of CO2 to CO at the reduced nickel center and provide a starting point for improved photoredox systems for sustainable carbon-neutral energy conversion.

  4. In situ measurements of heterogeneous reactions on ambient aerosol particles: Impacts on atmospheric chemistry and climate

    SciTech Connect (OSTI)

    Bertram, Timothy

    2015-02-11

    Aerosol particles play a critical role in the Earth’s energy budget through the absorption and scattering of radiation, and/or through their ability to form clouds and alter cloud lifetime. Heterogeneous and multi-phase reactions alter the climate-relevant properties of aerosol particles and catalyze reaction pathways that are energetically unfavorable in the gas phase. The chemical composition of aerosol particles dictates the kinetics of heterogeneous and multi-phase reactions. At present, the vast majority of the molecular level information on these processes has been determined in laboratory investigations on model aerosol systems. The work described here provides a comprehensive investigation into the reactivity of complex, ambient aerosol particles is proposed to determine: 1) how representative laboratory investigations of heterogeneous and multi-phase processes conducted on model, simple systems are of the real atmosphere, and 2) the impact of heterogeneous and multi-phase processes on ambient particle optical properties and their ability to nucleate clouds. This work has focused on the uptake kinetics for ammonia (NH3) and dinitrogen pentoxide (N2O5). The results of these investigations will be used to directly improve the representation of heterogeneous and multi-phase processes in global climate models, by identifying the key mechanistic drivers that control the variability in the observed kinetics.

  5. Heterogeneity-corrected vs -uncorrected critical structure maximum point doses in breast balloon brachytherapy

    SciTech Connect (OSTI)

    Kim, Leonard; Narra, Venkat; Yue, Ning

    2013-07-01

    Recent studies have reported potentially clinically meaningful dose differences when heterogeneity correction is used in breast balloon brachytherapy. In this study, we report on the relationship between heterogeneity-corrected and -uncorrected doses for 2 commonly used plan evaluation metrics: maximum point dose to skin surface and maximum point dose to ribs. Maximum point doses to skin surface and ribs were calculated using TG-43 and Varian Acuros for 20 patients treated with breast balloon brachytherapy. The results were plotted against each other and fit with a zero-intercept line. Max skin dose (Acuros) = max skin dose (TG-43) ? 0.930 (R{sup 2} = 0.995). The average magnitude of difference from this relationship was 1.1% (max 2.8%). Max rib dose (Acuros) = max rib dose (TG-43) ? 0.955 (R{sup 2} = 0.9995). The average magnitude of difference from this relationship was 0.7% (max 1.6%). Heterogeneity-corrected maximum point doses to the skin surface and ribs were proportional to TG-43-calculated doses. The average deviation from proportionality was 1%. The proportional relationship suggests that a different metric other than maximum point dose may be needed to obtain a clinical advantage from heterogeneity correction. Alternatively, if maximum point dose continues to be used in recommended limits while incorporating heterogeneity correction, institutions without this capability may be able to accurately estimate these doses by use of a scaling factor.

  6. Displacement Fields and Self-Energies of Circular and Polygonal Dislocation Loops in Homogeneous and Layered Anisotropic Solids

    SciTech Connect (OSTI)

    Gao, Yanfei; Larson, Ben C.

    2015-06-19

    There are large classes of materials problems that involve the solutions of stress, displacement, and strain energy of dislocation loops in elastically anisotropic solids, including increasingly detailed investigations of the generation and evolution of irradiation induced defect clusters ranging in sizes from the micro- to meso-scopic length scales. Based on a two-dimensional Fourier transform and Stroh formalism that are ideal for homogeneous and layered anisotropic solids, we have developed robust and computationally efficient methods to calculate the displacement fields for circular and polygonal dislocation loops. Using the homogeneous nature of the Green tensor of order -1, we have shown that the displacement and stress fields of dislocation loops can be obtained by numerical quadrature of a line integral. In addition, it is shown that the sextuple integrals associated with the strain energy of loops can be represented by the product of a pre-factor containing elastic anisotropy effects and a universal term that is singular and equal to that for elastic isotropic case. Furthermore, we have found that the self-energy pre-factor of prismatic loops is identical to the effective modulus of normal contact, and the pre-factor of shear loops differs from the effective indentation modulus in shear by only a few percent. These results provide a convenient method for examining dislocation reaction energetic and efficient procedures for numerical computation of local displacements and stresses of dislocation loops, both of which play integral roles in quantitative defect analyses within combined experimental–theoretical investigations.

  7. THREE DISCRETE GROUPS WITH HOMOGENEOUS CHEMISTRY ALONG THE RED GIANT BRANCH IN THE GLOBULAR CLUSTER NGC2808

    SciTech Connect (OSTI)

    Carretta, E.

    2014-11-10

    We present the homogeneous reanalysis of Mg and Al abundances from high resolution UVES/FLAMES spectra for 31 red giants in the globular cluster NGC2808. We found a well defined Mg-Al anticorrelation reaching a regime of subsolar Mg abundance ratios, with a spread of about 1.4dex in [Al/Fe]. The main result from the improved statistics of our sample is that the distribution of stars is not continuous along the anticorrelation because they are neatly clustered into three distinct clumps, each with different chemical compositions. One group (P) shows a primordial composition of field stars of similar metallicity, and the other two (I and E) have increasing abundances of Al and decreasing abundances of Mg. The fraction of stars we found in the three components (P: 68%, I: 19%, E: 13%) is in excellent agreement with the ratios computed for the three distinct main sequences in NGC2808: for the first time there is a clear correspondence between discrete photometric sequences of dwarfs and distinct groups of giants with homogeneous chemistry. The composition of the I group cannot be reproduced by mixing of matter with extreme processing in hot H-burning and gas with pristine, unprocessed composition, as also found in the recent analysis of three discrete groups in NGC6752. This finding suggests that different classes of polluters were probably at work in NGC2808 as well.

  8. Thermomechanical process optimization of U-10wt% Mo Part 2: The effect of homogenization on the mechanical properties and microstructure

    SciTech Connect (OSTI)

    Joshi, Vineet V.; Nyberg, Eric A.; Lavender, Curt A.; Paxton, Dean M.; Burkes, Douglas E.

    2015-07-09

    Low-enriched uranium alloyed with 10 wt% molybdenum (U-10Mo) is currently being investigated as an alternative fuel for the highly enriched uranium used in several of the United States high performance research reactors. Development of the methods to fabricate the U-10Mo fuel plates is currently underway and requires fundamental understanding of the mechanical properties at the expected processing temperatures. In the first part of this series, it was determined that the as-cast U-10Mo had a dendritic microstructure with chemical inhomogeneity and underwent eutectoid transformation during hot compression testing. In the present (second) part of the work, the as-cast samples were heat treated at several temperatures and times to homogenize the Mo content. Like the previous as-cast material, the homogenized materials were then tested under compression between 500 and 800C. The as-cast samples and those treated at 800C for 24 hours had grain sizes of 25-30 ?m, whereas those treated at 1000C for 16 hours had grain sizes around 250 ?m before testing. Upon compression testing, it was determined that the heat treatment had effects on the mechanical properties and the precipitation of the lamellar phase at sub-eutectoid temperatures.

  9. EVOLUTION OF THE SOLAR NEBULA. IX. GRADIENTS IN THE SPATIAL HETEROGENEITY OF THE SHORT-LIVED RADIOISOTOPES {sup 60}Fe AND {sup 26}Al AND THE STABLE OXYGEN ISOTOPES

    SciTech Connect (OSTI)

    Boss, Alan P.

    2011-10-01

    Short-lived radioisotopes (SLRIs) such as {sup 60}Fe and {sup 26}Al were likely injected into the solar nebula in a spatially and temporally heterogeneous manner. Marginally gravitationally unstable (MGU) disks, of the type required to form gas giant planets, are capable of rapid homogenization of isotopic heterogeneity as well as of rapid radial transport of dust grains and gases throughout a protoplanetary disk. Two different types of new models of an MGU disk in orbit around a solar-mass protostar are presented. The first set has variations in the number of terms in the spherical harmonic solution for the gravitational potential, effectively studying the effect of varying the spatial resolution of the gravitational torques responsible for MGU disk evolution. The second set explores the effects of varying the initial minimum value of the Toomre Q stability parameter, from values of 1.4 to 2.5, i.e., toward increasingly less unstable disks. The new models show that the basic results are largely independent of both sets of variations. MGU disk models robustly result in rapid mixing of initially highly heterogeneous distributions of SLRIs to levels of {approx}10% in both the inner (<5 AU) and outer (>10 AU) disk regions, and to even lower levels ({approx}2%) in intermediate regions, where gravitational torques are most effective at mixing. These gradients should have cosmochemical implications for the distribution of SLRIs and stable oxygen isotopes contained in planetesimals (e.g., comets) formed in the giant planet region ({approx}5 to {approx}10 AU) compared to those formed elsewhere.

  10. Characterization of trapped gas saturation and heterogeneity in core sampling using miscible-displacement experiments

    SciTech Connect (OSTI)

    Smith, D.H.; Jikich, S.A.

    1994-12-31

    Trapped gas saturation and permeability heterogeneity were evaluated in Berea cores at reservoir conditions, using standard miscible displacement experiments, with and without surfactants. Pressure and production history were influenced by core heterogeneity and foam lamellae formation when aqueous surfactant was present in the core. The objective of the dispersion-capacitance model was to estimate trapped gas saturations; however longitudinal dispersion and mass transfer also were examined. The results show that the dispersion-capacitance model accurately fits trapped gas saturation controlled by rock heterogeneities and foam lamellae for lamella generating mechanisms that allow a continuous gas phase (leave-behind lamellae). The practical applications resulting from this study can aid in core sample selection and scaling short laboratory corefloods to field dimensions for applications to foam stimulation and underground storage of natural gas.

  11. New Helical Foldamers: Heterogeneous Backbones with 1:2 and 2:1

    Office of Scientific and Technical Information (OSTI)

    [alpha]:[superscript beta]-Amino Acid Residue Patterns (Journal Article) | SciTech Connect New Helical Foldamers: Heterogeneous Backbones with 1:2 and 2:1 [alpha]:[superscript beta]-Amino Acid Residue Patterns Citation Details In-Document Search Title: New Helical Foldamers: Heterogeneous Backbones with 1:2 and 2:1 [alpha]:[superscript beta]-Amino Acid Residue Patterns Authors: Schmitt, Margaret A. ; Choi, SooHyuk ; Guzei, Ilia A. ; Gellman, Samuel H. [1] + Show Author Affiliations (UW)

  12. Chemical Heterogeneity of a Large Cluster CP IDP: Clues to its Formation

    Office of Scientific and Technical Information (OSTI)

    History Using X-ray Fluoresence Mapping and Cr and Fe XANES Spectroscopy (Conference) | SciTech Connect SciTech Connect Search Results Conference: Chemical Heterogeneity of a Large Cluster CP IDP: Clues to its Formation History Using X-ray Fluoresence Mapping and Cr and Fe XANES Spectroscopy Citation Details In-Document Search Title: Chemical Heterogeneity of a Large Cluster CP IDP: Clues to its Formation History Using X-ray Fluoresence Mapping and Cr and Fe XANES Spectroscopy Authors:

  13. Displacement Fields and Self-Energies of Circular and Polygonal Dislocation Loops in Homogeneous and Layered Anisotropic Solids

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

    Gao, Yanfei; Larson, Ben C.

    2015-06-19

    There are large classes of materials problems that involve the solutions of stress, displacement, and strain energy of dislocation loops in elastically anisotropic solids, including increasingly detailed investigations of the generation and evolution of irradiation induced defect clusters ranging in sizes from the micro- to meso-scopic length scales. Based on a two-dimensional Fourier transform and Stroh formalism that are ideal for homogeneous and layered anisotropic solids, we have developed robust and computationally efficient methods to calculate the displacement fields for circular and polygonal dislocation loops. Using the homogeneous nature of the Green tensor of order -1, we have shown thatmore » the displacement and stress fields of dislocation loops can be obtained by numerical quadrature of a line integral. In addition, it is shown that the sextuple integrals associated with the strain energy of loops can be represented by the product of a pre-factor containing elastic anisotropy effects and a universal term that is singular and equal to that for elastic isotropic case. Furthermore, we have found that the self-energy pre-factor of prismatic loops is identical to the effective modulus of normal contact, and the pre-factor of shear loops differs from the effective indentation modulus in shear by only a few percent. These results provide a convenient method for examining dislocation reaction energetic and efficient procedures for numerical computation of local displacements and stresses of dislocation loops, both of which play integral roles in quantitative defect analyses within combined experimental–theoretical investigations.« less

  14. Predicting the influence of long-range molecular interactions on macroscopic-scale diffusion by homogenization of the Smoluchowski equation

    SciTech Connect (OSTI)

    Kekenes-Huskey, P. M.; Gillette, A. K.; McCammon, J. A.; Department of Chemistry, Howard Hughes Medical Institute, University of California San Diego, La Jolla, California 92093-0636

    2014-05-07

    The macroscopic diffusion constant for a charged diffuser is in part dependent on (1) the volume excluded by solute obstacles and (2) long-range interactions between those obstacles and the diffuser. Increasing excluded volume reduces transport of the diffuser, while long-range interactions can either increase or decrease diffusivity, depending on the nature of the potential. We previously demonstrated [P. M. Kekenes-Huskey et al., Biophys. J. 105, 2130 (2013)] using homogenization theory that the configuration of molecular-scale obstacles can both hinder diffusion and induce diffusional anisotropy for small ions. As the density of molecular obstacles increases, van der Waals (vdW) and electrostatic interactions between obstacle and a diffuser become significant and can strongly influence the latter's diffusivity, which was neglected in our original model. Here, we extend this methodology to include a fixed (time-independent) potential of mean force, through homogenization of the Smoluchowski equation. We consider the diffusion of ions in crowded, hydrophilic environments at physiological ionic strengths and find that electrostatic and vdW interactions can enhance or depress effective diffusion rates for attractive or repulsive forces, respectively. Additionally, we show that the observed diffusion rate may be reduced independent of non-specific electrostatic and vdW interactions by treating obstacles that exhibit specific binding interactions as buffers that absorb free diffusers. Finally, we demonstrate that effective diffusion rates are sensitive to distribution of surface charge on a globular protein, Troponin C, suggesting that the use of molecular structures with atomistic-scale resolution can account for electrostatic influences on substrate transport. This approach offers new insight into the influence of molecular-scale, long-range interactions on transport of charged species, particularly for diffusion-influenced signaling events occurring in crowded cellular environments.

  15. A New Equivalence Theory Method for Treating Doubly Heterogeneous Fuel - II. Verifications

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

    Choi, Sooyoung; Kong, Chidong; Lee, Deokjung; Williams, Mark L.

    2015-03-09

    A new methodology has been developed recently to treat resonance self-shielding in systems for which the fuel compact region of a reactor lattice consists of small fuel grains dispersed in a graphite matrix. The theoretical development adopts equivalence theory in both micro- and macro-level heterogeneities to provide approximate analytical expressions for the shielded cross sections, which may be interpolated from a table of resonance integrals or Bondarenko factors using a modified background cross section as the interpolation parameter. This paper describes the first implementation of the theoretical equations in a reactor analysis code. In order to reduce discrepancies caused bymore » use of the rational approximation for collision probabilities in the original derivation, a new formulation for a doubly heterogeneous Bell factor is developed in this paper to improve the accuracy of doubly heterogeneous expressions. This methodology is applied to a wide range of pin cell and assembly test problems with varying geometry parameters, material compositions, and temperatures, and the results are compared with continuous-energy Monte Carlo simulations to establish the accuracy and range of applicability of the new approach. It is shown that the new doubly heterogeneous self-shielding method including the Bell factor correction gives good agreement with reference Monte Carlo results.« less

  16. High-throughput imaging of heterogeneous cell organelles with an X-ray laser

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

    Hantke, Max, F.

    2014-11-17

    Preprocessed detector images that were used for the paper "High-throughput imaging of heterogeneous cell organelles with an X-ray laser". The CXI file contains the entire recorded data - including both hits and blanks. It also includes down-sampled images and LCLS machine parameters. Additionally, the Cheetah configuration file is attached that was used to create the pre-processed data.

  17. Physics of DNAPL migration and remediation in the presence of heterogeneities. 1997 annual progress report

    SciTech Connect (OSTI)

    Conrad, S.; Glass, R.

    1997-01-01

    'The authors are in the process of conducting well-controlled laboratory experiments to better understand the physics of DNAPL migration and remediation in the presence of heterogeneities. These experiments are being used to develop and test an upscaled percolation model, a new approach for modeling DNAPL migration. In addition, numerical simulators under current use in evaluating remediation techniques will be compared against the remediation experiments. They are making use of their unique experimental capabilities in the Subsurface Flow and Transport Processes Laboratory at Sandia to conduct controlled, systematic, repeatable experiments that first consider the physics of DNAPL migration in initially water-saturated, heterogeneous porous media and then evaluate the efficacy of a suite of promising remediation techniques for remediating DNAPLs from heterogeneous aquifers. The results of the migration experiments are being used to test and continue development of new modeling approaches based on upscaled percolation theory developed by us. The remediation experiments include visual and quantitative measures of each remediation technique''s performance. The results of the remediation experiments will be used to test, for the first time, within heterogeneous media, the quantitative performance of remediation design codes (two-phase flow codes that incorporate compositional models).'

  18. A New Equivalence Theory Method for Treating Doubly Heterogeneous Fuel - II. Verifications

    SciTech Connect (OSTI)

    Choi, Sooyoung; Kong, Chidong; Lee, Deokjung; Williams, Mark L.

    2015-03-09

    A new methodology has been developed recently to treat resonance self-shielding in systems for which the fuel compact region of a reactor lattice consists of small fuel grains dispersed in a graphite matrix. The theoretical development adopts equivalence theory in both micro- and macro-level heterogeneities to provide approximate analytical expressions for the shielded cross sections, which may be interpolated from a table of resonance integrals or Bondarenko factors using a modified background cross section as the interpolation parameter. This paper describes the first implementation of the theoretical equations in a reactor analysis code. In order to reduce discrepancies caused by use of the rational approximation for collision probabilities in the original derivation, a new formulation for a doubly heterogeneous Bell factor is developed in this paper to improve the accuracy of doubly heterogeneous expressions. This methodology is applied to a wide range of pin cell and assembly test problems with varying geometry parameters, material compositions, and temperatures, and the results are compared with continuous-energy Monte Carlo simulations to establish the accuracy and range of applicability of the new approach. It is shown that the new doubly heterogeneous self-shielding method including the Bell factor correction gives good agreement with reference Monte Carlo results.

  19. Characterization of trapped gas saturation and heterogeneity in core samples using miscible-displacement experiments

    SciTech Connect (OSTI)

    Smith, D.H.; Jikich, S.A.

    1994-12-31

    Trapped gas saturation and permeability heterogeneity were evaluated in Berea cores at reservoir conditions, using standard miscible displacement experiments, with and without surfactants. Pressure and production history were influenced by core heterogeneity and foam lamellae formation when aqueous surfactant was present in the core. A simple dispersion model and a three-coefficient dispersion-capacitance model (Coates-Smith) were fit to the experimental data. The dispersion-capacitance model successfully matched the experiments in which foam lamella formed, while the simple dispersion model was used only for determining initial core flow heterogeneity. The objective of the dispersion-capacitance model was to estimate trapped gas saturations; however longitudinal dispersion and mass transfer also were examined. The results show that the dispersion-capacitance model accurately fits trapped gas saturation controlled by rock heterogeneities and foam lamellae for lamella generating mechanisms that allow a continuous gas phase (leave-behind lamellae). The practical applications resulting from this study can aid in core sample selection and scaling short laboratory corefloods to field dimensions for applications to foam stimulation and underground storage of natural gas.

  20. Long-term Differences in Tillage and Land Use Affect Intra-aggregate Pore Heterogeneity

    SciTech Connect (OSTI)

    Kravchenko, A.N.; Wang, A.N.W.; Smucker, A.J.M.; Rivers, M.L.

    2012-10-25

    Recent advances in computed tomography provide measurement tools to study internal structures of soil aggregates at micrometer resolutions and to improve our understanding of specific mechanisms of various soil processes. Fractal analysis is one of the data analysis tools that can be helpful in evaluating heterogeneity of the intra-aggregate internal structures. The goal of this study was to examine how long-term tillage and land use differences affect intra-aggregate pore heterogeneity. The specific objectives were: (i) to develop an approach to enhance utility of box-counting fractal dimension in characterizing intra-aggregate pore heterogeneity; (ii) to examine intra-aggregate pores in macro-aggregates (4-6 mm in size) using the computed tomography scanning and fractal analysis, and (iii) to compare heterogeneity of intra-aggregate pore space in aggregates from loamy Alfisol soil subjected to 20 yr of contrasting management practices, namely, conventional tillage (chisel plow) (CT), no-till (NT), and native succession vegetation (NS). Three-dimensional images of the intact aggregates were obtained with a resolution of 14.6 {micro}m at the Advanced Photon Source, Argonne National Laboratory, Argonne, IL. Proposed box-counting fractal dimension normalization was successfully implemented to estimate heterogeneity of pore voxel distributions without bias associated with different porosities in soil aggregates. The aggregates from all three studied treatments had higher porosity associated with large (>100 {micro}m) pores present in their centers than in their exteriors. Pores 15 to 60 {micro}m were equally abundant throughout entire aggregates but their distributions were more heterogeneous in aggregate interiors. The CT aggregates had greater numbers of pores 15 to 60 {micro}m than NT and NS. Distribution of pore voxels belonging to large pores was most heterogeneous in the aggregates from NS, followed by NT and by CT. This result was consistent with presence of very large pores associated with former root channels in NT and NS aggregates. Our findings indicate that mechanisms of macro-aggregate formation might differ in their importance in different land use and management practices.

  1. Characterization of fundamental catalytic properties of MoS2/WS2 nanotubes and nanoclusters for desulfurization catalysis - a surface temperature study

    SciTech Connect (OSTI)

    U. Burghaus

    2012-07-05

    The prior project consisted of two main project lines. First, characterization of novel nanomaterials for hydrodesulfurization (HDS) applications. Second, studying more traditional model systems for HDS such as vapor-deposited silica-supported Mo and MoSx clusters. In the first subproject, we studied WS2 and MoS2 fullerene-like nanoparticles as well as WS2 nanotubes. Thiophene (C4H4S) was used as the probe molecule. Interestingly, metallic and sulfur-like adsorption sites could be identified on the silica-supported fullerene-particles system. Similar structures are seen for the traditional system (vapor-deposited clusters). Thus, this may be a kinetics fingerprint feature of modern HDS model systems. In addition, kinetics data allowed characterization of the different adsorption sites for thiophene on and inside WS2 nanotube bundles. The latter is a unique feature of nanotubes that has not been reported before for any inorganic nanotube system; however, examples are known for carbon nanotubes, including prior work of the PI. Although HDS has been studied for decades, utilizing nanotubes as nanosized HDS reactors has never been tried before, as far as we know. This is of interest from a fundamental perspective. Unfortunately, the HDS activity of the nanocatalysts at ultra-high vacuum (UHV) conditions was close to the detection limit of our techniques. Therefore, we propose to run experiments at ambient pressure on related nanopowder samples as part of the renewal application utilizing a now-available GC (gas chromatograph) setup. In addition, Ni and Co doped nanocatalyts are proposed for study. These dopants will boost the catalytic activity. In the second subproject of the prior grant, we studied HDS-related chemistry on more traditional supported cluster catalysts. Mo clusters supported by physical vapor deposition (PVD) on silica have been characterized. Two reaction pathways are evident when adsorbing thiophene on Mo and MoSx clusters: molecular adsorption and dissociation. PVD Mo clusters turned out to be very reactive toward thiophene bond activation. Sulfur and carbon residuals form, which poison the catalyst and sulfide the Mo clusters. Sulfided silica-supported MoSx samples are not reactive toward thiophene bond activation. In addition to S and C deposits, H2, H2S, and small organic molecules were detected in the gas phase. Catalyst reactivation procedures, including O2 and atomic hydrogen treatments, have been tested. Cluster size effects have been seen: thiophene adsorbs molecularly with larger binding energies on smaller clusters. However, larger clusters have smaller activation energy for C4H4S bond activation than smaller clusters. The latter is consistent with early catalysis studies. Kinetics and dynamics parameters have been determined quantitatively. We spent a significant amount of time on upgrades of our equipment. A 2nd-hand refurbished X-ray photoelectron spectrometer (XPS) has been integrated into the existing molecular beam scattering system and is already operational (supported by the DoE supplemental grant available in October 2009). We also added a time of flight (TOF) system to the beam scattering apparatus and improved on the accessible impact energy range (new nozzle heater and gas mixing manifold) for the beam scattering experiments. In addition, a GC-based powder atmospheric flow reactor for studies on powder samples is now operational. Furthermore, a 2nd UHV kinetics system has been upgraded as well. In summary, mostly single crystal systems have so far been considered in basic science studies about HDS. Industrial catalysts, however, can be better approximated with the supported cluster systems that we studied in this project. Furthermore, an entirely new class of HDS systems, namely fullerene-like particles and inorganic nanotubes, has been included. Studying new materials and systems has the potential to impact science and technology. The systems investigated are closely related to energy and environmental-related surface science/catalysis. This prior project, conducted at NDSU by a sma

  2. Catalysis Center for Energy Innovation

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

    I: Analytical Characterization Instructors: Professor Paul Dauenhauer (University of Minnesota) Jeff Everhart (University of Delaware) 322 ISE Lab 10:45-11:00 Break 11:00-12:30 ...

  3. Electrochemistry: Catalysis at the boundaries

    SciTech Connect (OSTI)

    Appel, Aaron M.

    2014-04-09

    Renewable energy provides an opportunity to power society without the potential impacts from the use of fossil fuels, but a major limitation of sources such as solar and wind is their intermittent availability. Efficient storage of energy from these renewable sources is critical in developing their widespread utilization. One approach to the storage of renewable energy is the production of fuels, such as ethanol, from water and carbon dioxide. Unlike traditional centralized fuel production, electrochemical systems can operate under mild pressures and temperatures in dispersed, small-scale reactors. Renewable sources of energy are inherently dispersed, and therefore are well matched with the production of fuels electrochemically. However, the development of efficient catalysts is essential for the intended chemical transformations.

  4. Differential homogeneous immunosensor device

    DOE Patents [OSTI]

    Malmros, M.K.; Gulbinski, J. III.

    1990-04-10

    There is provided a novel method of testing for the presence of an analyte in a fluid suspected of containing the same. In this method, in the presence of the analyte, a substance capable of modifying certain characteristics of the substrate is bound to the substrate and the change in these qualities is measured. While the method may be modified for carrying out quantitative differential analyses, it eliminates the need for washing the analyte from the substrate which is characteristic of prior art methods. 12 figs.

  5. homogeneous charge compression ignition

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

    Home Office Equipment Tables (Million U.S. Households; 12 pages, 123 kb) Contents Pages HC7-1a. Home Office Equipment by Climate Zone, Million U.S. Households, 2001 1 HC7-2a. Home Office Equipment by Year of Construction, Million U.S. Households, 2001 1 HC7-3a. Home Office Equipment by Household Income, Million U.S. Households, 2001 1 HC7-4a. Home Office Equipment by Type of Housing Unit, Million U.S. Households, 2001 1 HC7-5a. Home Office Equipment by Type of Owner-Occupied Housing Unit,

  6. Differential homogeneous immunosensor device

    DOE Patents [OSTI]

    Malmros, Mark K.; Gulbinski, III, Julian

    1990-04-10

    There is provided a novel method of testing for the presence of an analyte in a fluid suspected of containing the same. In this method, in the presence of the analyte, a substance capable of modifying certain characteristics of the substrate is bound to the substrate and the change in these qualities is measured. While the method may be modified for carrying out quantitative differential analyses, it eliminates the need for washing analyte from the substrate which is characteristic of prior art methods.

  7. Multiple current peaks in room-temperature atmospheric pressure homogenous dielectric barrier discharge plasma excited by high-voltage tunable nanosecond pulse in air

    SciTech Connect (OSTI)

    Yang, De-Zheng; Wang, Wen-Chun; Zhang, Shuai; Tang, Kai; Liu, Zhi-jie; Wang, Sen

    2013-05-13

    Room temperature homogenous dielectric barrier discharge plasma with high instantaneous energy efficiency is acquired by using nanosecond pulse voltage with 20-200 ns tunable pulse width. Increasing the voltage pulse width can lead to the generation of regular and stable multiple current peaks in each discharge sequence. When the voltage pulse width is 200 ns, more than 5 organized current peaks can be observed under 26 kV peak voltage. Investigation also shows that the organized multiple current peaks only appear in homogenous discharge mode. When the discharge is filament mode, organized multiple current peaks are replaced by chaotic filament current peaks.

  8. Role of the laser pulse-length in producing high-quality electron beams in a homogenous plasma

    SciTech Connect (OSTI)

    Upadhyay, Ajay K.; Arun Samant, Sushil; Krishnagopal, Srinivas

    2012-07-15

    In laser wakefield acceleration, the pulse-length of the laser is an important parameter that affects the laser evolution and electron beam injection and acceleration in the bubble regime. Here, we use three-dimensional simulations to find, for a given plasma density, the optimal pulse-length that gives the best quality electron beam. For three different pulse lengths, we study the evolution dynamics of the laser spot-size and quality of the injected electron beam. We find that a pulse-length that is less than the theoretical optimum, {tau}{sub L} = {lambda}{sub p}/{radical}2{pi}c, derived from linear theory, gives the best beam quality. Conversely, our simulations suggest that for a given laser system, with a fixed pulse-length, there is an optimal value of the plasma density that will give the best quality accelerated beams in experiments. For an rms pulse-length of 10 fs (around 24 fs FWHM), this corresponds to a plasma density of around 3.4 Multiplication-Sign 10{sup 18}/cm{sup 3}. For these parameters, we obtain, in a homogenous plasma and with a single laser, an electron beam with an energy of around 700 MeV, an energy-spread less than 2%, and rms normalized emittance of a few {pi} mm-mrad.

  9. A Comprehensive Parameterization of Heterogeneous Ice Nucleation of Dust Surrogate: Laboratory Study with Hematite Particles and Its Application to Atmospheric Models

    SciTech Connect (OSTI)

    Hiranuma, Naruki; Paukert, Marco; Steinke, Isabelle; Zhang, Kai; Kulkarni, Gourihar R.; Hoose, Corinna; Schnaiter, Martin; Saathoff, Harald; Mohler, Ottmar

    2014-12-10

    A new heterogeneous ice nucleation parameterization that covers a wide temperature range (-36 ?C to -78 ?C) is presented. Developing and testing such an ice nucleation parameterization, which is constrained through identical experimental conditions, is critical in order to accurately simulate the ice nucleation processes in cirrus clouds. The surface-scaled ice nucleation efficiencies of hematite particles, inferred by ns, were derived from AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber measurements under water subsaturated conditions that were realized by continuously changing temperature (T) and relative humidity with respect to ice (RHice) in the chamber. Our measurements showed several different pathways to nucleate ice depending on T and RHice conditions. For instance, almost independent freezing was observed at -60 ?C < T < -50 ?C, where RHice explicitly controlled ice nucleation efficiency, while both T and RHice played roles in other two T regimes: -78 ?C < T < -60 ?C and -50 ?C < T < -36 ?C. More specifically, observations at T colder than -60 ?C revealed that higher RHice was necessary to maintain constant ns, whereas T may have played a significant role in ice nucleation at T warmer than -50 ?C. We implemented new ns parameterizations into two cloud models to investigate its sensitivity and compare with the existing ice nucleation schemes towards simulating cirrus cloud properties. Our results show that the new AIDA-based parameterizations lead to an order of magnitude higher ice crystal concentrations and inhibition of homogeneous nucleation in colder temperature regions. Our cloud simulation results suggest that atmospheric dust particles that form ice nuclei at lower temperatures, below -36 ?C, can potentially have stronger influence on cloud properties such as cloud longevity and initiation when compared to previous parameterizations.

  10. Long-term desorption behavior of uranium and neptunium in heterogeneous volcanic tuff materials /

    SciTech Connect (OSTI)

    Dean, Cynthia A.

    2010-05-01

    Uranium and neptunium desorption were studied in long-term laboratory experiments using four well-characterized volcanic tuff cores collected from southeast of Yucca Mountain, Nevada. The objectives of the experiments were to 1. Demonstrate a methodology aimed at characterizing distributions of sorption parameters (attributes of multiple sorption sites) that can be applied to moderately-sorbing species in heterogeneous systems to provide more realistic reactive transport parameters and a more realistic approach to modeling transport in heterogeneous systems. 2. Focus on uranium and neptunium because of their high solubility, relatively weak sorption, and high contributions to predicted dose in Yucca Mountain performance assessments. Also, uranium is a contaminant of concern at many DOE legacy sites and uranium mining sites.

  11. Theory of ultrafast heterogeneous electron transfer: Contributions of direct charge transfer excitations to the absorbance

    SciTech Connect (OSTI)

    Wang, Luxia; Willig, Frank; May, Volkhard

    2007-04-07

    Absorption spectra related to heterogeneous electron transfer are analyzed with the focus on direct charge transfer transition from the surface attached molecule into the semiconductor band states. The computations are based on a model of reduced dimensionality with a single intramolecular vibrational coordinate but a complete account for the continuum of conduction band states. The applicability of this model to perylene on TiO{sub 2} has been demonstrated in a series of earlier papers. Here, based on a time-dependent formulation, the absorbance is calculated with the inclusion of charge transfer excitations. A broad parameter set inspired by the perylene TiO{sub 2} systems is considered. In particular, the description generalizes the Fano effect to heterogeneous electron transfer reactions. Preliminary simulations of measured spectra are presented for perylene-catechol attached to TiO{sub 2}.

  12. Thermal Design and Characterization of Heterogeneously Integrated InGaP/GaAs HBTs

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

    Choi, Sukwon; Peake, Gregory M.; Keeler, Gordon A.; Geib, Kent M.; Briggs, Ronald D.; Beechem, Thomas E.; Shaffer, Ryan A.; Clevenger, Jascinda; Patrizi, Gary A.; Klem, John F.; et al

    2016-04-21

    Flip-chip heterogeneously integrated n-p-n InGaP/GaAs heterojunction bipolar transistors (HBTs) with integrated thermal management on wide-bandgap AlN substrates followed by GaAs substrate removal are demonstrated. Without thermal management, substrate removal after integration significantly aggravates self-heating effects, causing poor I–V characteristics due to excessive device self-heating. An electrothermal codesign scheme is demonstrated that involves simulation (design), thermal characterization, fabrication, and evaluation. Thermoreflectance thermal imaging, electrical-temperature sensitive parameter-based thermometry, and infrared thermography were utilized to assess the junction temperature rise in HBTs under diverse configurations. In order to reduce the thermal resistance of integrated devices, passive cooling schemes assisted by structural modification, i.e.,more » positioning indium bump heat sinks between the devices and the carrier, were employed. By implementing thermal heat sinks in close proximity to the active region of flip-chip integrated HBTs, the junction-to-baseplate thermal resistance was reduced over a factor of two, as revealed by junction temperature measurements and improvement of electrical performance. In conclusion, the suggested heterogeneous integration method accounts for not only electrical but also thermal requirements providing insight into realization of advanced and robust III–V/Si heterogeneously integrated electronics.« less

  13. Reservoir heterogeneity in carboniferous sandstone of the Black Warrior basin. Final report

    SciTech Connect (OSTI)

    Kugler, R.L.; Pashin, J.C.; Carroll, R.E.; Irvin, G.D.; Moore, H.E.

    1994-06-01

    Although oil production in the Black Warrior basin of Alabama is declining, additional oil may be produced through improved recovery strategies, such as waterflooding, chemical injection, strategic well placement, and infill drilling. High-quality characterization of reservoirs in the Black Warrior basin is necessary to utilize advanced technology to recover additional oil and to avoid premature abandonment of fields. This report documents controls on the distribution and producibility of oil from heterogeneous Carboniferous reservoirs in the Black Warrior basin of Alabama. The first part of the report summarizes the structural and depositional evolution of the Black Warrior basin and establishes the geochemical characteristics of hydrocarbon source rocks and oil in the basin. This second part characterizes facies heterogeneity and petrologic and petrophysical properties of Carter and Millerella sandstone reservoirs. This is followed by a summary of oil production in the Black Warrior basin and an evaluation of seven improved-recovery projects in Alabama. In the final part, controls on the producibility of oil from sandstone reservoirs are discussed in terms of a scale-dependent heterogeneity classification.

  14. Dynamics and heterogeneity of a fate determinant during transition towards cell differentiation

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

    Peláez, Nicolás; Gavalda-Miralles, Arnau; Wang, Bao; Navarro, Heliodoro Tejedor; Gudjonson, Herman; Rebay, Ilaria; Dinner, Aaron R.; Katsaggelos, Aggelos K.; Amaral, Luís AN; Carthew, Richard W.

    2015-11-19

    Yan is an ETS-domain transcription factor responsible for maintaining Drosophila eye cells in a multipotent state. Yan is at the core of a regulatory network that determines the time and place in which cells transit from multipotency to one of several differentiated lineages. Using a fluorescent reporter for Yan expression, we observed a biphasic distribution of Yan in multipotent cells, with a rapid inductive phase and slow decay phase. Transitions to various differentiated states occurred over the course of this dynamic process, suggesting that Yan expression level does not strongly determine cell potential. Consistent with this conclusion, perturbing Yan expressionmore » by varying gene dosage had no effect on cell fate transitions. However, we observed that as cells transited to differentiation, Yan expression became highly heterogeneous and this heterogeneity was transient. Signals received via the EGF Receptor were necessary for the transience in Yan noise since genetic loss caused sustained noise. Since these signals are essential for eye cells to differentiate, we suggest that dynamic heterogeneity of Yan is a necessary element of the transition process, and cell states are stabilized through noise reduction.« less

  15. Reservoir heterogeneity in Carboniferous sandstone of the Black Warrior basin. Final report

    SciTech Connect (OSTI)

    Kugler, R.L.; Pashin, J.C.; Carroll, R.E.; Irvin, G.D.; Moore, H.E.

    1994-04-01

    Although oil production in the Black Warrior basin of Alabama is declining, additional oil may be produced through improved recovery strategies, such as waterflooding, chemical injection, strategic well placement, and infill drilling. High-quality characterization of reservoirs in the Black Warrior basin is necessary to utilize advanced technology to recover additional oil and to avoid premature abandonment of fields. This report documents controls on the distribution and producibility of oil from heterogeneous Carboniferous reservoirs in the Black Warrior basin of Alabama. The first part of the report summarizes the structural and depositional evolution of the Black Warrior basin and establishes the geochemical characteristics of hydrocarbon source rocks and oil in the basin. This second part characterizes facies heterogeneity and petrologic and petrophysical properties of Carter and Millerella sandstone reservoirs. This is followed by a summary of oil production in the Black Warrior basin and an evaluation of seven improved-recovery projects in Alabama. In the final part, controls on the producibility of oil from sandstone reservoirs are discussed in terms of a scale-dependent heterogeneity classification.

  16. Influence of heterogeneity on second-kind self-similar solutions for viscous gravity currents

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

    Zheng, Zhong; Christov, Ivan  C.; Stone, Howard  A.

    2014-04-16

    We report experimental, theoretical and numerical results on the effects of horizontal heterogeneities on the propagation of viscous gravity currents. We use two geometries to highlight these effects: (a) a horizontal channel (or crack) whose gap thickness varies as a power-law function of the streamwise coordinate; (b) a heterogeneous porous medium whose permeability and porosity have power-law variations. We demonstrate that two types of self-similar behaviours emerge as a result of horizontal heterogeneity: (a) a first-kind self-similar solution is found using dimensional analysis (scaling) for viscous gravity currents that propagate away from the origin (a point of zero permeability); (b)more » a second-kind self-similar solution is found using a phase-plane analysis for viscous gravity currents that propagate toward the origin. These theoretical predictions, obtained using the ideas of self-similar intermediate asymptotics, are compared with experimental results and numerical solutions of the governing partial differential equation developed under the lubrication approximation. All three results are found to be in good agreement.« less

  17. Tests of a Prototype for Assessing the Field Homogeneity of the Iseult/Inumac 11.7T Whole Body MRI Magnet

    SciTech Connect (OSTI)

    Quettier, Lionel

    2010-06-01

    A neuroscience research center with very high field MRI equipments has been opened in November 2006 by the CEA life science division. One of the imaging systems will require a 11.75 T magnet with a 900 mm warm bore, the so-call Iseult/Inumac magnet. Regarding the large aperture and field strength, this magnet is a challenge as compared to the largest MRI systems ever built, and is then developed within an ambitious R&D program. With the objective of demonstrating the possibility of achieving field homogeneity better than 1 ppm using double pancake windings, a 24 double pancakes model coil, working at 1.5 T has been designed. This model magnet has been manufactured by Alstom MSA and tested at CEA. It has been measured with a very high precision, in order to fully characterize the field homogeneity, and then to investigate and discriminate the parameters that influence the field map. This magnet has reached the bare magnet field homogeneity specification expected for Iseult and thus successfully demonstrated the feasibility of building a homogenous magnet with the double pancake winding technique.

  18. Chemical Sciences Division annual report 1994

    SciTech Connect (OSTI)

    1995-06-01

    The division is one of ten LBL research divisions. It is composed of individual research groups organized into 5 scientific areas: chemical physics, inorganic/organometallic chemistry, actinide chemistry, atomic physics, and chemical engineering. Studies include structure and reactivity of critical reaction intermediates, transients and dynamics of elementary chemical reactions, and heterogeneous and homogeneous catalysis. Work for others included studies of superconducting properties of high-{Tc} oxides. In FY 1994, the division neared completion of two end-stations and a beamline for the Advanced Light Source, which will be used for combustion and other studies. This document presents summaries of the studies.

  19. Scaling impacts on environmental controls and spatial heterogeneity of soil organic carbon stocks

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

    Mishra, U.; Riley, W. J.

    2015-01-27

    The spatial heterogeneity of land surfaces affects energy, moisture, and greenhouse gas exchanges with the atmosphere. However, representing heterogeneity of terrestrial hydrological and biogeochemical processes in earth system models (ESMs) remains a critical scientific challenge. We report the impact of spatial scaling on environmental controls, spatial structure, and statistical properties of soil organic carbon (SOC) stocks across the US state of Alaska. We used soil profile observations and environmental factors such as topography, climate, land cover types, and surficial geology to predict the SOC stocks at a 50 m spatial scale. These spatially heterogeneous estimates provide a dataset with reasonablemore » fidelity to the observations at a sufficiently high resolution to examine the environmental controls on the spatial structure of SOC stocks. We upscaled both the predicted SOC stocks and environmental variables from finer to coarser spatial scales (s = 100, 200, 500 m, 1, 2, 5, 10 km) and generated various statistical properties of SOC stock estimates. We found different environmental factors to be statistically significant predictors at different spatial scales. Only elevation, temperature, potential evapotranspiration, and scrub land cover types were significant predictors at all scales. The strengths of control (the median value of geographically weighted regression coefficients) of these four environmental variables on SOC stocks decreased with increasing scale and were accurately represented using mathematical functions (R2 = 0.83–0.97). The spatial structure of SOC stocks across Alaska changed with spatial scale. Although the variance (sill) and unstructured variability (nugget) of the calculated variograms of SOC stocks decreased exponentially with scale, the correlation length (range) remained relatively constant across scale. The variance of predicted SOC stocks decreased with spatial scale over the range of 50 to ~ 500 m, and remained constant beyond this scale. The fitted exponential function accounted for 98% of variability in the variance of SOC stocks. We found moderately-accurate linear relationships between mean and higher-order moments of predicted SOC stocks (R2 ~ 0.55–0.63). Current ESMs operate at coarse spatial scales (50–100 km), and are therefore unable to represent environmental controllers and spatial heterogeneity of high-latitude SOC stocks consistent with observations. We conclude that improved understanding of the scaling behavior of environmental controls and statistical properties of SOC stocks can improve ESM land model benchmarking and perhaps allow representation of spatial heterogeneity of biogeochemistry at scales finer than those currently resolved by ESMs.« less

  20. Scaling impacts on environmental controls and spatial heterogeneity of soil organic carbon stocks

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

    Mishra, U.; Riley, W. J.

    2015-07-02

    The spatial heterogeneity of land surfaces affects energy, moisture, and greenhouse gas exchanges with the atmosphere. However, representing the heterogeneity of terrestrial hydrological and biogeochemical processes in Earth system models (ESMs) remains a critical scientific challenge. We report the impact of spatial scaling on environmental controls, spatial structure, and statistical properties of soil organic carbon (SOC) stocks across the US state of Alaska. We used soil profile observations and environmental factors such as topography, climate, land cover types, and surficial geology to predict the SOC stocks at a 50 m spatial scale. These spatially heterogeneous estimates provide a data setmore » with reasonable fidelity to the observations at a sufficiently high resolution to examine the environmental controls on the spatial structure of SOC stocks. We upscaled both the predicted SOC stocks and environmental variables from finer to coarser spatial scales (s = 100, 200, and 500 m and 1, 2, 5, and 10 km) and generated various statistical properties of SOC stock estimates. We found different environmental factors to be statistically significant predictors at different spatial scales. Only elevation, temperature, potential evapotranspiration, and scrub land cover types were significant predictors at all scales. The strengths of control (the median value of geographically weighted regression coefficients) of these four environmental variables on SOC stocks decreased with increasing scale and were accurately represented using mathematical functions (R2 = 0.83–0.97). The spatial structure of SOC stocks across Alaska changed with spatial scale. Although the variance (sill) and unstructured variability (nugget) of the calculated variograms of SOC stocks decreased exponentially with scale, the correlation length (range) remained relatively constant across scale. The variance of predicted SOC stocks decreased with spatial scale over the range of 50 m to ~ 500 m, and remained constant beyond this scale. The fitted exponential function accounted for 98 % of variability in the variance of SOC stocks. We found moderately accurate linear relationships between mean and higher-order moments of predicted SOC stocks (R2 ∼ 0.55–0.63). Current ESMs operate at coarse spatial scales (50–100 km), and are therefore unable to represent environmental controllers and spatial heterogeneity of high-latitude SOC stocks consistent with observations. We conclude that improved understanding of the scaling behavior of environmental controls and statistical properties of SOC stocks could improve ESM land model benchmarking and perhaps allow representation of spatial heterogeneity of biogeochemistry at scales finer than those currently resolved by ESMs.« less

  1. Assessment of Molecular Modeling & Simulation

    SciTech Connect (OSTI)

    2002-01-03

    This report reviews the development and applications of molecular and materials modeling in Europe and Japan in comparison to those in the United States. Topics covered include computational quantum chemistry, molecular simulations by molecular dynamics and Monte Carlo methods, mesoscale modeling of material domains, molecular-structure/macroscale property correlations like QSARs and QSPRs, and related information technologies like informatics and special-purpose molecular-modeling computers. The panel's findings include the following: The United States leads this field in many scientific areas. However, Canada has particular strengths in DFT methods and homogeneous catalysis; Europe in heterogeneous catalysis, mesoscale, and materials modeling; and Japan in materials modeling and special-purpose computing. Major government-industry initiatives are underway in Europe and Japan, notably in multi-scale materials modeling and in development of chemistry-capable ab-initio molecular dynamics codes.

  2. Covariance statistics of turbulence velocity components for wind-energy-conversion system design-homogeneous, isotropic case

    SciTech Connect (OSTI)

    Fichtl, G.H.

    1983-09-01

    When designing a wind energy converison system (WECS), it may be necessary to take into account the distribution of wind across the disc of rotation. The specific engineering applications include structural strength, fatigue, and control. This wind distribution consists of two parts, namely that associated with the mean wind profile and that associated with the turbulence velocity fluctuation field. The work reported herein is aimed at the latter, namely the distribution of turbulence velocity fluctuations across the WECS disk of rotation. A theory is developed for the two-time covariance matrix for turbulence velocity vector components for wind energy conversion system (WECS) design. The theory is developed for homogeneous and iotropic turbulance with the assumption that Taylor's hypothesis is valid. The Eulerian turbulence velocity vector field is expanded about the hub of the WECS. Formulae are developed for the turbulence velocity vector component covariance matrix following the WECS blade elements. It is shown that upon specification of the turbulence energy spectrum function and the WECS rotation rate, the two-point, two-time covariance matrix of the turbulent flow relative to the WECS bladed elements is determined. This covariance matrix is represented as the sum of nonstationary and stationary contributions. Generalized power spectral methods are used to obtain two-point, double frequency power spectral density functions for the turbulent flow following the blade elements. The Dryden turbulence model is used to demonstrate the theory. A discussion of linear system response analysis is provided to show how the double frequency turbulence spectra might be used to calculate response spectra of a WECS to turbulent flow. Finally the spectrum of the component of turbulence normal to the WECS disc of rotation, following the blade elements, is compared with experimental results.

  3. Mammalian. cap alpha. -polymerase: cloning of partial complementary DNA and immunobinding of catalytic subunit in crude homogenate protein blots

    SciTech Connect (OSTI)

    SenGupta, D.N.; Kumar, P.; Zmudzka, B.Z.; Coughlin, S.; Vishwanatha, J.K.; Robey, F.A.; Parrott, C.; Wilson, S.H.

    1987-02-10

    A new polyclonal antibody against the ..cap alpha..-polymerase catalytic polypeptide was prepared by using homogeneous HeLa cell..cap alpha..-polymerase. The antibody neutralized ..cap alpha..-polymerase activity and was strong and specific for the ..cap alpha..-polymerase catalytic polypeptide (M/sub r/ 183,000) in Western blot analysis of crude extracts of HeLa cells. The antibody was used to screen a cDNA library of newborn rat brain poly(A+) RNA in lambdagt11. A positive phage was identified and plaque purified. This phage, designated lambdapol..cap alpha..1.2, also was found to be positive with an antibody against Drosophila ..cap alpha..-polymerase. The insert in lambdapol..cap alpha..1.2 (1183 base pairs) contained a poly(A) sequence at the 3' terminus and a short in-phase open reading frame at the 5' terminus. A synthetic oligopeptide (eight amino acids) corresponding to the open reading frame was used to raise antiserum in rabbits. Antibody affinity purified from this serum was found to be immunoreactive against purified ..cap alpha..-polymerase by enzyme-linked immunosorbent assay and was capable of immunoprecipitating ..cap alpha..-polymerase. This indicated the lambdapol..cap alpha..1.2 insert encoded an ..cap alpha..-polymerase epitope and suggested that the cDNA corresponded to an ..cap alpha..-polymerase mRNA. This was confirmed in hybrid selection experiments using pUC9 containing the cDNA insert and poly(A+) RNA from newborn rat brain; the insert hybridized to mRNA capable of encoding ..cap alpha..-polymerase catalytic polypeptides. Northern blot analysis of rat brain poly(A+) RNA revealed that this mRNA is approx.5.4 kilobases.

  4. Steps towards verification and validation of the Fetch code for Level 2 analysis, design, and optimization of aqueous homogeneous reactors

    SciTech Connect (OSTI)

    Nygaard, E. T.; Pain, C. C.; Eaton, M. D.; Gomes, J. L. M. A.; Goddard, A. J. H.; Gorman, G.; Tollit, B.; Buchan, A. G.; Cooling, C. M.; Angelo, P. L.

    2012-07-01

    Babcock and Wilcox Technical Services Group (B and W) has identified aqueous homogeneous reactors (AHRs) as a technology well suited to produce the medical isotope molybdenum 99 (Mo-99). AHRs have never been specifically designed or built for this specialized purpose. However, AHRs have a proven history of being safe research reactors. In fact, in 1958, AHRs had 'a longer history of operation than any other type of research reactor using enriched fuel' and had 'experimentally demonstrated to be among the safest of all various type of research reactor now in use [1].' While AHRs have been modeled effectively using simplified 'Level 1' tools, the complex interactions between fluids, neutronics, and solid structures are important (but not necessarily safety significant). These interactions require a 'Level 2' modeling tool. Imperial College London (ICL) has developed such a tool: Finite Element Transient Criticality (FETCH). FETCH couples the radiation transport code EVENT with the computational fluid dynamics code (Fluidity), the result is a code capable of modeling sub-critical, critical, and super-critical solutions in both two-and three-dimensions. Using FETCH, ICL researchers and B and W engineers have studied many fissioning solution systems include the Tokaimura criticality accident, the Y12 accident, SILENE, TRACY, and SUPO. These modeling efforts will ultimately be incorporated into FETCH'S extensive automated verification and validation (V and V) test suite expanding FETCH'S area of applicability to include all relevant physics associated with AHRs. These efforts parallel B and W's engineering effort to design and optimize an AHR to produce Mo99. (authors)

  5. Experimental study and chemical analysis of n-heptane homogeneous charge compression ignition combustion with port injection of reaction inhibitors

    SciTech Connect (OSTI)

    Lue, Xingcai; Ji, Libin; Zu, Linlin; Hou, Yuchun; Huang, Cheng; Huang, Zhen

    2007-05-15

    The control of ignition timing in the homogeneous charge compression ignition (HCCI) of n-heptane by port injection of reaction inhibitors was studied in a single-cylinder engine. Four suppression additives, methanol, ethanol, isopropanol, and methyl tert-butyl ether (MTBE), were used in the experiments. The effectiveness of inhibition of HCCI combustion with various additives was compared under the same equivalence ratio of total fuel and partial equivalence ratio of n-heptane. The experimental results show that the suppression effectiveness increases in the order MTBE < isopropanol << ethanol < methanol. But ethanol is the best additive when the operating ranges, indicated thermal efficiency, and emissions are considered. For ethanol/n-heptane HCCI combustion, partial combustion may be observed when the mole ratio of ethanol to that of total fuel is larger than 0.20; misfires occur when the mole ratio of ethanol to that of total fuel larger than 0.25. Moreover, CO emissions strongly depend on the maximum combustion temperature, while HC emissions are mainly dominated by the mole ratio of ethanol to that of total fuel. To obtain chemical mechanistic informations relevant to the ignition behavior, detailed chemical kinetic analysis was conducted. The simulated results also confirmed the retarding of the ignition timing by ethanol addition. In addition, it can be found from the simulation that HCHO, CO, and C{sub 2}H{sub 5}OH could not be oxidized completely and are maintained at high levels if the partial combustion or misfire occurs (for example, for leaner fuel/air mixture). (author)

  6. Karma Sawyer | Department of Energy

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

    at Berkeley in 2008, focusing on spin-crossover dynamics and homogeneous catalysis reactions using ultrafast infrared spectroscopy and density functional theory (DFT) calculations. ...

  7. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    (3) atomic force microscopy (2) brookhaven rhic (2) catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, mesostructured materials, materials and chemistry ...

  8. Automated treatment planning for a dedicated multi-source intra-cranial radiosurgery treatment unit accounting for overlapping structures and dose homogeneity

    SciTech Connect (OSTI)

    Ghobadi, Kimia; Ghaffari, Hamid R.; Aleman, Dionne M.; Institute of Health Policy, Management and Evaluation, University of Toronto, Ontario M5T 3M6; Techna Institute, University Health Network, Ontario M5G 1P5 ; Jaffray, David A.; Department of Radiation Oncology, University of Toronto, Ontario M5S 3E2; Department of Medical Biophysics, University of Toronto, Ontario M5G 2M9; Institute of Biomaterial and Biomedical Engineering, University of Toronto, Ontario M5S 2J7; Techna Institute, University Health Network, Ontario M5G 1P5; Ontario Cancer Institute, Ontario M5G 0A3 ; Ruschin, Mark; Department of Radiation Oncology, University of Toronto, Toronto, Ontario M5S 3E2

    2013-09-15

    Purpose: The purpose of this work is to advance the two-step approach for Gamma Knife{sup } Perfexion (PFX) optimization to account for dose homogeneity and overlap between the planning target volume (PTV) and organs-at-risk (OARs).Methods: In the first step, a geometry-based algorithm is used to quickly select isocentre locations while explicitly accounting for PTV-OARs overlaps. In this approach, the PTV is divided into subvolumes based on the PTV-OARs overlaps and the distance of voxels to the overlaps. Only a few isocentres are selected in the overlap volume, and a higher number of isocentres are carefully selected among voxels that are immediately close to the overlap volume. In the second step, a convex optimization is solved to find the optimal combination of collimator sizes and their radiation duration for each isocentre location.Results: This two-step approach is tested on seven clinical cases (comprising 11 targets) for which the authors assess coverage, OARs dose, and homogeneity index and relate these parameters to the overlap fraction for each case. In terms of coverage, the mean V{sub 99} for the gross target volume (GTV) was 99.8% while the V{sub 95} for the PTV averaged at 94.6%, thus satisfying the clinical objectives of 99% for GTV and 95% for PTV, respectively. The mean relative dose to the brainstem was 87.7% of the prescription dose (with maximum 108%), while on average, 11.3% of the PTV overlapped with the brainstem. The mean beam-on time per fraction per dose was 8.6 min with calibration dose rate of 3.5 Gy/min, and the computational time averaged at 205 min. Compared with previous work involving single-fraction radiosurgery, the resulting plans were more homogeneous with average homogeneity index of 1.18 compared to 1.47.Conclusions: PFX treatment plans with homogeneous dose distribution can be achieved by inverse planning using geometric isocentre selection and mathematical modeling and optimization techniques. The quality of the obtained treatment plans are clinically satisfactory while the homogeneity index is improved compared to conventional PFX plans.

  9. Scale-up of miscible flood processes for heterogeneous reservoirs. Final report

    SciTech Connect (OSTI)

    Orr, F.M. Jr.

    1996-04-01

    Results of a wide-ranging investigation of the scaling of gas injection processes are reported. The research examines how the physical mechanisms at work during a gas injection project interact to determine process performance. In particular, the authors examine: the interactions of equilibrium phase behavior and two-phase flow that determine local displacement efficiency and minimum miscibility pressure, the combined effects of viscous fingering, gravity segregation and heterogeneity that control sweep efficiency in 2- and 3-dimensional porous media, the use of streamtube/streamline methods to create very efficient simulation technique for multiphase compositional displacements, the scaling of viscous, capillary and gravity forces for heterogeneous reservoirs, and the effects of the thin films and spreading behavior on three-phase flow. The following key results are documented: rigorous procedures for determination of minimum miscibility pressure (MMP) or minimum miscibility enrichment (MME) for miscibility have been developed for multicomponent systems; the complex dependence of MMP`s for nitrogen/methane floods on oil and injection gas composition observed experimentally is explained for the first time; the presence of layer-like heterogeneities strongly influences the interplay of gravity segregation and viscous fingering, as viscous fingers adapt to preferential flow paths and low permeability layers restrict vertical flow; streamtube/streamline simulation techniques are demonstrated for a variety of injection processes in 2 and 3 dimensions; quantitative scaling estimates for the transitions from capillary-dominated to gravity-dominated to viscous-dominated flows are reported; experimental results are given that demonstrate that high pressure CO{sub 2} can be used to generate low IFT gravity drainage in fractured reservoirs if fractures are suitably connected; and the effect of wetting and spreading behavior on three-phase flow is described. 209 refs.

  10. Search for: All records | SciTech Connect

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    Everything24 Electronic Full Text0 Citations24 Multimedia0 Datasets0 Software0 Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ...

  11. Search for: All records | SciTech Connect

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    Everything34 Electronic Full Text3 Citations31 Multimedia0 Datasets0 Software0 Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ...

  12. Search for: All records | SciTech Connect

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    Everything8 Electronic Full Text0 Citations8 Multimedia0 Datasets0 Software0 Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ...

  13. Search for: All records | SciTech Connect

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    Filter Results Filter by Subject materials science (14) synchrotrons (10) x-ray diffraction (10) catalysis (heterogeneous), solar (photovoltaic), phonons, thermoelectric, energy ...

  14. Surface-structure sensitivity of CeO2 nanocrystals in photocatalysis...

    Office of Scientific and Technical Information (OSTI)

    heterogeneous (photo)catalysis. In this study, using aberration-corrected scanning transmission electron microscopy (STEM), the atomic surface structures of well-defined...

  15. Compositional Variation Within Hybrid Nanostructures

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

    Within Hybrid Nanostructures Print The inherently high surface area of bimetallic nanoparticles makes them especially attractive materials for heterogeneous catalysis. The...

  16. Search for: All records | SciTech Connect

    Office of Scientific and Technical Information (OSTI)

    ... Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ... Pressure, stress, and strain distribution in the double-stage diamond anvil cell Lobanov, ...

  17. Search for: All records | SciTech Connect

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    ... Filter Results Filter by Subject catalysis (heterogeneous), solar (photovoltaic), phonons, ... and powder diffraction studies using synchrotron radiation and a diamond-anvil cell. ...

  18. Role of Surface Structure on Li-ion Energy Storage Capacity of...

    Office of Scientific and Technical Information (OSTI)

    (FIRST) Sponsoring Org: USDOE SC Office of Basic Energy Sciences (SC-22) Country of Publication: United States Language: English Subject: catalysis (heterogeneous), solar ...

  19. Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

    SciTech Connect (OSTI)

    Quan, Jiannong; Liu, Yangang; Liu, Quan; Li, Xia; Gao, Yang; Jia, Xingcan; Sheng, Jiujiang

    2015-09-30

    In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO2 and NOx, accelerated the formation of secondary inorganic aerosols, and led to rapid increase of the PM2.5 concentration.

  20. Heterogeneous catalyst for the production of ethylidene diacetate from acetic anhydride

    DOE Patents [OSTI]

    Ramprasad, D.; Waller, F.J.

    1998-06-16

    This invention relates to a process for producing ethylidene diacetate by the reaction of acetic anhydride, acetic acid, hydrogen and carbon monoxide at elevated temperatures and pressures in the presence of an alkyl halide and a heterogeneous, bifunctional catalyst that is stable to hydrogenation and comprises an insoluble polymer having pendant quaternized heteroatoms, some of which heteroatoms are ionically bonded to anionic Group VIII metal complexes, the remainder of the heteroatoms being bonded to iodide. In contrast to prior art processes, no accelerator (promoter) is necessary to achieve the catalytic reaction and the products are easily separated from the catalyst by filtration. The catalyst can be recycled without loss in activity.

  1. Directing Self-Assembly of Heterogeneous NanoSystems | MIT-Harvard Center

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

    for Excitonics Directing Self-Assembly of Heterogeneous NanoSystems December 5, 2013 at 3pm/36-428 Alfredo Alexander-Katz Department of Material Science and Engineering, Massachusetts Institute of Technology alexander-katz_004 Abstract: Directed self-assembly of block copolymers is a route to obtain tailored 2D patterns on the 10nm scale that have a high degree of order. These patterns are promising for applications in multiple areas, including sub 10nm lithography, light harvesting, and

  2. Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

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

    Quan, Jiannong; Liu, Yangang; Liu, Quan; Li, Xia; Gao, Yang; Jia, Xingcan; Sheng, Jiujiang

    2015-09-30

    In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM2.5), nitrate (NO3), sulfate (SO4), ammonium (NH4)], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO2), and ozone (O3)], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (Nratio) and S from SO2 to sulfate (Sratio) bothmore » significantly increased in haze events, suggesting enhanced conversions from NOx and SO2 to their corresponding particle phases in the late haze period. Further analysis shows that Nratio and Sratio increased with increasing RH, with Nratio and Sratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of Nratio and Sratio to O3: the conversion ratios increase with decreasing O3 concentration when O3 concentration is lower than <15 ppb but increased with increasing O3 when O3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO2 and NOx, accelerated the formation of secondary inorganic aerosols, and led to rapid increase of the PM2.5 concentration.« less

  3. Heterogeneous catalyst for the production of ethylidene diacetate from acetic anhydride

    DOE Patents [OSTI]

    Ramprasad, Dorai (Allentown, PA); Waller, Francis Joseph (Allentown, PA)

    1998-01-01

    This invention relates to a process for producing ethylidene diacetate by the reaction of acetic anhydride, acetic acid, hydrogen and carbon monoxide at elevated temperatures and pressures in the presence of an alkyl halide and a heterogeneous, bifunctional catalyst that is stable to hydrogenation and comprises an insoluble polymer having pendant quaternized heteroatoms, some of which heteroatoms are ionically bonded to anionic Group VIII metal complexes, the remainder of the heteroatoms being bonded to iodide. In contrast to prior art processes, no accelerator (promoter) is necessary to achieve the catalytic reaction and the products are easily separated from the catalyst by filtration. The catalyst can be recycled without loss in activity.

  4. Characterization and Analysis Methods for the Examination of the Heterogeneous Solid Oxide Fuel Cell Electrode Microstructure, Part 1: Volumetric Measurements of the Heterogeneous Structure

    SciTech Connect (OSTI)

    Grew, Kyle N.; Peracchio, Aldo A.; Joshi, Abhijit S.; Izzo, Jr., John R.; Chiu, W. K. S.

    2010-12-15

    Advanced imaging and characterization methods have permitted the 3-D and phase-specific reconstruction of dense and opaque samples with features that have a length scale on the order of tens of nanometers and comprised of materials with large X-ray mass absorption coefficients. Engineered materials, like those found in solid oxide fuel cell (SOFC) electrodes, use complex materials that have often limited opportunities to perform 3-D characterization and analysis. Still, characterization and analysis methods are needed to better understand these structures and their functional impact. The development, verification, and validation of methods used by the authors for the characterization and analysis of the heterogeneous SOFC anode are discussed in this work. These methods include the measurement of the volume fractions of the individual phases, contiguity or volumetric connectivity, tortuosity, and interfacial properties. A second and complementary part of this work will examine quantitative methods that provide detailed descriptions of the structure and its relations to the transport processes that it must support. These efforts are intended to describe the formulation of methods developed to provide insight into the SOFC anode nano/microstructure.

  5. Improving the homogeneity of alternating current-drive atmospheric pressure dielectric barrier discharges in helium with an additional low-amplitude radio frequency power source: A numerical study

    SciTech Connect (OSTI)

    Wang Qi [Dalian Institute of Semiconductor Technology, School of Electronics Science and Technology, Dalian University of Technology, Dalian 116023 (China); Sun Jizhong; Zhang Jianhong; Wang Dezhen [School of Physics and Optoelectronic Technology, Dalian University of Technology, Dalian 116023 (China); Liu Liying [Department of Electrical Engineering, Shenyang Institute of Engineering, Shenyang 110136 (China)

    2013-04-15

    It was proposed in this paper that the homogeneity of the atmospheric pressure discharge driven by an ac power source could be improved by applying an auxiliary low-amplitude rf power source. To verify the idea, a two-dimensional fluid model then was applied to study the atmospheric discharges in helium driven by ac power, low-amplitude rf power, and combined ac and low-amplitude rf power, respectively. Simulation results confirmed that an auxiliary rf power could improve the homogeneity of a discharge driven by an ac power source. It was further found that there existed a threshold voltage of the rf power source leading to the transition from inhomogeneous to homogeneous discharge. As the frequency of the rf power source increased from 2 to 22 MHz, the magnitude of the threshold voltage dropped first rapidly and then to a constant value. When the frequency was over 13.56 MHz, the magnitude of the threshold voltage was smaller than one-sixth of the ac voltage amplitude under the simulated discharge parameters.

  6. Optimization of a heterogeneous fast breeder reactor core with improved behavior during unprotected transients

    SciTech Connect (OSTI)

    Poumerouly, S.; Schmitt, D.; Massara, S.; Maliverney, B.

    2012-07-01

    Innovative Sodium-cooled Fast Reactors (SFRs) are currently being investigated by CEA, AREVA and EDF in the framework of a joint French collaboration, and the construction of a GEN IV prototype, ASTRID (Advanced Sodium Technical Reactor for Industrial Demonstration), is scheduled in the years 2020. Significant improvements are expected so as to improve the reactor safety: the goal is to achieve a robust safety demonstration of the mastering of the consequences of a Core Disruptive Accident (CDA), whether by means of prevention or mitigation features. In this framework, an innovative design was proposed by CEA in 2010. It aims at strongly reducing the sodium void effect, thereby improving the core behavior during unprotected loss of coolant transients. This design is strongly heterogeneous and includes, amongst others, a fertile plate, a sodium plenum associated with a B{sub 4}C upper blanket and a stepwise modulation of the fissile height of the core (onwards referred to as the 'diabolo shape'). In this paper, studies which were entirely carried out at EDF are presented: the full potential of this heterogeneous concept is thoroughly investigated using the SDDS methodology. (authors)

  7. On the correlation between microscopic structural heterogeneity and embrittlement behavior in metallic glasses

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

    Li, Weidong; Gao, Yanfei; Bei, Hongbin

    2015-10-05

    To establish a relationship between microstructure and mechanical properties, we systematically annealed a Zr-based bulk metallic glass (BMG) at 100 ~ 300°C and measured their mechanical and thermal properties. The as-cast BMG exhibits some ductility, while the increase of annealing temperature and time leads to the transition to a brittle behavior that can reach nearly-zero fracture energy. The differential scanning calorimetry did not find any significant changes in crystallization temperature and enthalpy, indicating that the materials still remained fully amorphous. Elastic constants measured by ultrasonic technique vary only slightly with respect to annealing temperature and time, which does obey themore » empirical relationship between Poisson’s ratio and fracture behavior. Nanoindentation pop-in tests were conducted, from which the pop-in strength mapping provides a “mechanical probe” of the microscopic structural heterogeneities in these metallic glasses. Based on stochastically statistic defect model, we found that the defect density decreases with increasing annealing temperature and annealing time and is exponentially related to the fracture energy. A ductile-versus-brittle behavior (DBB) model based on the structural heterogeneity is developed to identify the physical origins of the embrittlement behavior through the interactions between these defects and crack tip.« less

  8. On the correlation between microscopic structural heterogeneity and embrittlement behavior in metallic glasses

    SciTech Connect (OSTI)

    Li, Weidong; Gao, Yanfei; Bei, Hongbin

    2015-10-05

    To establish a relationship between microstructure and mechanical properties, we systematically annealed a Zr-based bulk metallic glass (BMG) at 100 ~ 300°C and measured their mechanical and thermal properties. The as-cast BMG exhibits some ductility, while the increase of annealing temperature and time leads to the transition to a brittle behavior that can reach nearly-zero fracture energy. The differential scanning calorimetry did not find any significant changes in crystallization temperature and enthalpy, indicating that the materials still remained fully amorphous. Elastic constants measured by ultrasonic technique vary only slightly with respect to annealing temperature and time, which does obey the empirical relationship between Poisson’s ratio and fracture behavior. Nanoindentation pop-in tests were conducted, from which the pop-in strength mapping provides a “mechanical probe” of the microscopic structural heterogeneities in these metallic glasses. Based on stochastically statistic defect model, we found that the defect density decreases with increasing annealing temperature and annealing time and is exponentially related to the fracture energy. A ductile-versus-brittle behavior (DBB) model based on the structural heterogeneity is developed to identify the physical origins of the embrittlement behavior through the interactions between these defects and crack tip.

  9. Evaluation of Technical Feasibility of Homogeneous Charge Compression Ignition (HCCI) Engine Fueled with Hydrogen, Natural Gas, and DME

    SciTech Connect (OSTI)

    Pratapas, John; Mather, Daniel; Kozlovsky, Anton

    2013-03-31

    The objective of the proposed project was to confirm the feasibility of using blends of hydrogen and natural gas to improve the performance, efficiency, controllability and emissions of a homogeneous charge compression ignition (HCCI) engine. The project team utilized both engine simulation and laboratory testing to evaluate and optimize how blends of hydrogen and natural gas fuel might improve control of HCCI combustion. GTI utilized a state-of-the art single-cylinder engine test platform for the experimental work in the project. The testing was designed to evaluate the feasibility of extending the limits of HCCI engine performance (i.e., stable combustion, high efficiency and low emissions) on natural gas by using blends of natural gas and hydrogen. Early in the project Ricardo provided technical support to GTI as we applied their engine performance simulation program, WAVE, to our HCCI research engine. Modeling support was later provided by Digital Engines, LLC to use their proprietary model to predict peak pressures and temperatures for varying operating parameters included in the Design of Experiments test plan. Digital Engines also provided testing support for the hydrogen and natural gas blends. Prof. David Foster of University of Wisconsin-Madison participated early in the project by providing technical guidance on HCCI engine test plans and modeling requirements. The main purpose of the testing was to quantify the effects of hydrogen addition to natural gas HCCI. Directly comparing straight natural gas with the hydrogen enhanced test points is difficult due to the complexity of HCCI combustion. With the same air flow rate and lambda, the hydrogen enriched fuel mass flow rate is lower than the straight natural gas mass flow rate. However, the energy flow rate is higher for the hydrogen enriched fuel due to hydrogen’s significantly greater lower heating value, 120 mJ/kg for hydrogen compared to 45 mJ/kg for natural gas. With these caveats in mind, an analysis of test results indicates that hydrogen enhanced natural gas HCCI (versus neat natural gas HCCI at comparable stoichiometry) had the following characteristics: • Substantially lower intake temperature needed for stable HCCI combustion • Inconclusive impact on engine BMEP and power produced, • Small reduction in the thermal efficiency of the engine, • Moderate reduction in the unburned hydrocarbons in the exhaust, • Slight increase in NOx emissions in the exhaust, • Slight reduction in CO2 in the exhaust. • Increased knocking at rich stoichiometry The major accomplishments and findings from the project can be summarized as follows: 1. A model was calibrated for accurately predicting heat release rate and peak pressures for HCCI combustion when operating on hydrogen and natural gas blends. 2. A single cylinder research engine was thoroughly mapped to compare performance and emissions for micro-pilot natural gas compression ignition, and HCCI combustion for neat natural gas versus blends of natural gas and hydrogen.

  10. Evaluation of Technical Feasibility of Homogeneous Charge Compression Ignition (HCCI) Engine Fueled with Hydrogen, Natural Gas, and DME

    SciTech Connect (OSTI)

    John Pratapas; Daniel Mather; Anton Kozlovsky

    2007-03-31

    The objective of the proposed project was to confirm the feasibility of using blends of hydrogen and natural gas to improve the performance, efficiency, controllability and emissions of a homogeneous charge compression ignition (HCCI) engine. The project team utilized both engine simulation and laboratory testing to evaluate and optimize how blends of hydrogen and natural gas fuel might improve control of HCCI combustion. GTI utilized a state-of-the art single-cylinder engine test platform for the experimental work in the project. The testing was designed to evaluate the feasibility of extending the limits of HCCI engine performance (i.e., stable combustion, high efficiency and low emissions) on natural gas by using blends of natural gas and hydrogen. Early in the project Ricardo provided technical support to GTI as we applied their engine performance simulation program, WAVE, to our HCCI research engine. Modeling support was later provided by Digital Engines, LLC to use their proprietary model to predict peak pressures and temperatures for varying operating parameters included in the Design of Experiments test plan. Digital Engines also provided testing support for the hydrogen and natural gas blends. Prof. David Foster of University of Wisconsin-Madison participated early in the project by providing technical guidance on HCCI engine test plans and modeling requirements. The main purpose of the testing was to quantify the effects of hydrogen addition to natural gas HCCI. Directly comparing straight natural gas with the hydrogen enhanced test points is difficult due to the complexity of HCCI combustion. With the same air flow rate and lambda, the hydrogen enriched fuel mass flow rate is lower than the straight natural gas mass flow rate. However, the energy flow rate is higher for the hydrogen enriched fuel due to hydrogen's significantly greater lower heating value, 120 mJ/kg for hydrogen compared to 45 mJ/kg for natural gas. With these caveats in mind, an analysis of test results indicates that hydrogen enhanced natural gas HCCI (versus neat natural gas HCCI at comparable stoichiometry) had the following characteristics: (1) Substantially lower intake temperature needed for stable HCCI combustion; (2) Inconclusive impact on engine BMEP and power produced; (3) Small reduction in the thermal efficiency of the engine; (4) Moderate reduction in the unburned hydrocarbons in the exhaust; (5) Slight increase in NOx emissions in the exhaust; (6) Slight reduction in CO2 in the exhaust; and (7) Increased knocking at rich stoichiometry. The major accomplishments and findings from the project can be summarized as follows: (1) A model was calibrated for accurately predicting heat release rate and peak pressures for HCCI combustion when operating on hydrogen and natural gas blends. (2) A single cylinder research engine was thoroughly mapped to compare performance and emissions for micro-pilot natural gas compression ignition, and HCCI combustion for neat natural gas versus blends of natural gas and hydrogen. (3) The benefits of using hydrogen to extend, up to a limit, the stable operating window for HCCI combustion of natural gas at higher intake pressures, leaner air to fuel ratios or lower inlet temperatures was documented.

  11. Pore and Continuum Scale Study of the Effect of Subgrid Transport Heterogeneity on Redox Reaction Rates

    SciTech Connect (OSTI)

    Liu, Yuanyuan; Liu, Chongxuan; Zhang, Changyong; Yang, Xiaofan; Zachara, John M.

    2015-08-01

    A micromodel system with a pore structure for heterogeneous flow and transport was used to investigate the effect of subgrid transport heterogeneity on redox reaction rates. Hematite reductive dissolution by injecting a reduced form of flavin mononucleotide (FMNH2) at variable flow rates was used as an example to probe the variations of redox reaction rates in different subgrid transport domains. Experiments, pore-scale simulations, and macroscopic modeling were performed to measure and simulate in-situ hematite reduction and to evaluate the scaling behavior of the redox reaction rates from the pore to macroscopic scales. The results indicated that the measured pore-scale rates of hematite reduction were consistent with the predictions from a pore scale reactive transport model. A general trend is that hematite reduction followed reductant transport pathways, starting from the advection-dominated pores toward the interior of diffusion-dominated domains. Two types of diffusion domains were considered in the micromodel: a micropore diffusion domain, which locates inside solid grains or aggregates where reactant transport is limited by diffusion; and a macropore diffusion domain, which locates at wedged, dead-end pore spaces created by the grain-grain contacts. The rate of hematite reduction in the advection-dominated domain was faster than those in the diffusion-controlled domains, and the rate in the macropore diffusion domain was faster than that in the micropore domain. The reduction rates in the advection and macropore diffusion domains increased with increasing flow rate, but were affected by different mechanisms. The rate increase in the advection domain was controlled by the mass action effect as a faster flow supplied more reactants, and the rate increase in the macropore domain was more affected by the rate of mass exchange with the advection domain, which increased with increasing flow rate. The hematite reduction rate in the micropore domain was, however, not affected by the flow rate because molecular diffusion limits reductant supply to the micropore domain interior. Domain-based macroscopic models were evaluated to scale redox reaction rates from the pore to macroscopic scales. A single domain model, which ignores subgrid transport heterogeneity deviated significantly from the pore-scale results. Further analysis revealed that the rate expression for hematite reduction was not scalable from the pore to porous media using the single domain model. A three-domain model, which effectively considers subgrid reactive diffusion in the micropore and macropore domains, significantly improved model description. Overall this study revealed the importance of subgrid transport heterogeneity in the manifestation of redox reaction rates in porous media and in scaling reactions from the pore to porous media. The research also supported that the domain-based scaling approach can be used to directly scale redox reactions in porous media with subgrid transport heterogeneity.

  12. Thomas Jaramillo - JCAP

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

    thomas jaramillo Principal Investigator and Research Thrust Coordinator Email: jaramillo@stanford.edu Dr. Jaramillo's research interests center around: energy and catalysis, engineering surface and bulk materials chemistry in relation to energy conversion reactions-production, utilization, and storage. General themes include nano-scale effects in heterogeneous catalysis and electro-catalysis. Topics include water electrolysis, fuel cell electrocatalysis (oxygen reduction, fuel oxidation,

  13. Model Catalysis of Ammonia Synthesis ad Iron-Water Interfaces - ASum Frequency Generation Vibrational Spectroscopic Study of Solid-GasInterfaces and Anion Photoelectron Spectroscopic Study of Selected Anionclusters

    SciTech Connect (OSTI)

    Ferguson, Michael James

    2005-12-15

    The ammonia synthesis reaction has been studied using single crystal model catalysis combined with sum frequency generation (SFG) vibrational spectroscopy. The adsorption of gases N{sub 2}, H{sub 2}, O{sub 2} and NH{sub 3} that play a role in ammonia synthesis have been studied on the Fe(111) crystal surface by sum frequency generation vibrational spectroscopy using an integrated Ultra-High Vacuum (UHV)/high-pressure system. SFG spectra are presented for the dissociation intermediates, NH{sub 2} ({approx}3325 cm{sup -1}) and NH ({approx}3235 cm{sup -1}) under high pressure of ammonia or equilibrium concentrations of reactants and products on Fe(111) surfaces. Special attention was paid to understand how potassium promotion of the iron catalyst affects the intermediates of ammonia synthesis. An Fe(111) surface promoted with 0.2 monolayers of potassium red shifts the vibrational frequencies of the reactive surface intermediates, NH and NH{sub 2}, providing evidence for weakened the nitrogen-hydrogen bonds relative to clean Fe(111). Spectral features of these surface intermediates persisted to higher temperatures for promoted iron surfaces than for clean Fe(111) surfaces implying that nitrogen-iron bonds are stronger for the promoted surface. The ratio of the NH to NH{sub 2} signal changed for promoted surfaces in the presence of equilibrium concentrations of reactants and products. The order of adding oxygen and potassium to promoted surfaces does not alter the spectra indicating that ammonia induces surface reconstruction of the catalyst to produce the same surface morphology. When oxygen is co-adsorbed with nitrogen, hydrogen, ammonia or potassium on Fe(111), a relative phase shift of the spectra occurs as compared to the presence of adsorbates on clean iron surfaces. Water adsorption on iron was also probed using SFG vibrational spectroscopy. For both H{sub 2}O and D{sub 2}O, the only spectral feature was in the range of the free OH or free OD. From the absence of SFG spectra of ice-like structure we conclude that surface hydroxides are formed and no liquid water is present on the surface. Other than model catalysis, gas phase anion photoelectron spectroscopy of the Cl + H{sub 2} van der Waals well, silicon clusters, germanium clusters, aluminum oxide clusters and indium phosphide clusters were studied. The spectra help to map out the neutral potential energy surfaces of the clusters. For aluminum oxide, the structures of the anions and neutrals were explored and for silicon, germanium and indium phosphide the electronic structure of larger clusters was mapped out.

  14. DOE SBIR Phase II Final Report: Distributed Relevance Ranking in Heterogeneous Document Collections

    SciTech Connect (OSTI)

    Abe Lederman

    2007-01-08

    This report contains the comprehensive summary of the work performed on the SBIR Phase II project (Distributed Relevance Ranking in Heterogeneous Document Collections) at Deep Web Technologies (http://www.deepwebtech.com). We have successfully completed all of the tasks defined in our SBIR Proposal work plan (See Table 1 - Phase II Tasks Status). The project was completed on schedule and we have successfully deployed an initial production release of the software architecture at DOE-OSTI for the Science.gov Alliance's search portal (http://www.science.gov). We have implemented a set of grid services that supports the extraction, filtering, aggregation, and presentation of search results from numerous heterogeneous document collections. Illustration 3 depicts the services required to perform QuickRank filtering of content as defined in our architecture documentation. Functionality that has been implemented is indicated by the services highlighted in green. We have successfully tested our implementation in a multi-node grid deployment both within the Deep Web Technologies offices, and in a heterogeneous geographically distributed grid environment. We have performed a series of load tests in which we successfully simulated 100 concurrent users submitting search requests to the system. This testing was performed on deployments of one, two, and three node grids with services distributed in a number of different configurations. The preliminary results from these tests indicate that our architecture will scale well across multi-node grid deployments, but more work will be needed, beyond the scope of this project, to perform testing and experimentation to determine scalability and resiliency requirements. We are pleased to report that a production quality version (1.4) of the science.gov Alliance's search portal based on our grid architecture was released in June of 2006. This demonstration portal is currently available at http://science.gov/search30 . The portal allows the user to select from a number of collections grouped by category and enter a query expression (See Illustration 1 - Science.gov 3.0 Search Page). After the user clicks search a results page is displayed that provides a list of results from the selected collections ordered by relevance based on the query expression the user provided. Our grid based solution to deep web search and document ranking has already gained attention within DOE, other Government Agencies and a fortune 50 company. We are committed to the continued development of grid based solutions to large scale data access, filtering, and presentation problems within the domain of Information Retrieval and the more general categories of content management, data mining and data analysis.

  15. Influence of hot spot features on the initiation characteristics of heterogeneous nitromethane

    SciTech Connect (OSTI)

    Dattelbaum, Dana M; Sheffield, Stephen A; Stahl, David B; Dattelbaum, Andrew M; Engelke, Ray

    2010-01-01

    To gain insights into the critical hot spot features influencing energetic materials initiation characteristics, well-defined micron-scale particles have been intentionally introduced into the homogeneous explosive nitromethane (NM). Two types of potential hot spot origins have been examined - shock impedance mismatches using solid silica beads, and porosity using hollow microballoons - as well as their sizes and inter-particle separations. Here, we present the results of several series of gas gun-driven plate impact experiments on NM/particle mixtures with well-controlled shock inputs. Detailed insights into the nature of the reactive flow during the build-up to detonation have been obtained from the response of in-situ electromagnetic gauges, and the data have been used to establish Pop-plots (run-distance-to-detonation vs. shock input pressure) for the mixtures. Comparisons of sensitization effects and energy release characteristics relative to the initial shock front between the solid and hollow beads are presented.

  16. System of and method for transparent management of data objects in containers across distributed heterogenous resources

    DOE Patents [OSTI]

    Moore, Reagan W.; Rajasekar, Arcot; Wan, Michael Y.

    2010-09-21

    A system of and method for maintaining data objects in containers across a network of distributed heterogeneous resources in a manner which is transparent to a client. A client request pertaining to containers is resolved by querying meta data for the container, processing the request through one or more copies of the container maintained on the system, updating the meta data for the container to reflect any changes made to the container as a result processing the request, and, if a copy of the container has changed, changing the status of the copy to indicate dirty status or synchronizing the copy to one or more other copies that may be present on the system.

  17. System of and method for transparent management of data objects in containers across distributed heterogenous resources

    DOE Patents [OSTI]

    Moore, Reagan W.; Rajasekar, Arcot; Wan, Michael Y.

    2004-01-13

    A system of and method for maintaining data objects in containers across a network of distributed heterogeneous resources in a manner which is transparent to a client. A client request pertaining to containers is resolved by querying meta data for the container, processing the request through one or more copies of the container maintained on the system, updating the meta data for the container to reflect any changes made to the container as a result processing the request, and, if a copy of the container has changed, changing the status of the copy to indicate dirty status or synchronizing the copy to one or more other copies that may be present on the system.

  18. System of and method for transparent management of data objects in containers across distributed heterogenous resources

    DOE Patents [OSTI]

    Moore, Reagan W.; Rajasekar, Arcot; Wan, Michael Y.

    2007-09-11

    A system of and method for maintaining data objects in containers across a network of distributed heterogeneous resources in a manner which is transparent to a client. A client request pertaining to containers is resolved by querying meta data for the container, processing the request through one or more copies of the container maintained on the system, updating the meta data for the container to reflect any changes made to the container as a result processing the re quest, and, if a copy of the container has changed, changing the status of the copy to indicate dirty status or synchronizing the copy to one or more other copies that may be present on the system.

  19. Geostatistical Simulation of Hydrofacies Heterogeneity of the West Thessaly Aquifer Systems in Greece

    SciTech Connect (OSTI)

    Modis, K. Sideri, D.

    2013-06-15

    Integrating geological properties, such as relative positions and proportions of different hydrofacies, is of highest importance in order to render realistic geological patterns. Sequential indicator simulation (SIS) and Plurigaussian simulation (PS) are alternative methods for conceptual and deterministic modeling for the characterization of hydrofacies distribution. In this work, we studied the spatial differentiation of hydrofacies in the alluvial aquifer system of West Thessaly basin in Greece. For this, we applied both SIS and PS techniques to an extensive set of borehole data from that basin. Histograms of model versus experimental hydrofacies proportions and indicative cross sections were plotted in order to validate the results. The PS technique was shown to be more effective in reproducing the spatial characteristics of the different hydrofacies and their distribution across the study area. In addition, the permeability differentiations reflected in the PS model are in accordance to known heterogeneities of the aquifer capacity.

  20. Heterogeneous catalyst for the production of acetic anhydride from methyl acetate

    DOE Patents [OSTI]

    Ramprasad, D.; Waller, F.J.

    1999-04-06

    This invention relates to a process for producing acetic anhydride by the reaction of methyl acetate, carbon monoxide, and hydrogen at elevated temperatures and pressures in the presence of an alkyl halide and a heterogeneous, bifunctional catalyst that contains an insoluble polymer having pendant quaternized phosphine groups, some of which phosphine groups are ionically bonded to anionic Group VIII metal complexes, the remainder of the phosphine groups being bonded to iodide. In contrast to prior art processes, no accelerator (promoter) is necessary to achieve the catalytic reaction and the products are easily separated from the catalyst by filtration. The catalyst can be recycled for consecutive runs without loss in activity. Bifunctional catalysts for use in carbonylating dimethyl ether are also provided.