National Library of Energy BETA

Sample records for bimetallic nanoparticle catalysts

  1. Structural analysis of palladium-decorated gold nanoparticles as colloidal bimetallic catalysts.

    SciTech Connect (OSTI)

    Fang, Y. L.; Miller, J. T.; Guo, N.; Heck, K. N.; Alvarez, P. J. J.; Wong, M. S. (Chemical Sciences and Engineering Division); (Rice Univ.)

    2011-02-02

    Bimetallic palladium-decorated gold nanoparticle (Pd/Au NP) catalysts are significantly more active than palladium-only catalysts, but the mechanism for enhancement is not completely clear for most reactions, like the aqueous-phase hydrodechlorination of trichloroethene. In this study, we conducted X-ray absorption spectroscopy on carbon-supported Pd/Au NPs to obtain information about the local atomic environment (i.e., oxidation states, coordination numbers, and bond distances) of the two metals under different treatment conditions. The as-synthesized NPs were confirmed to have a Pd-shell/Au-core nanostructure, in which the Pd was found as surface ensembles. Upon exposure to room temperature in air, a portion of the Pd, but not the Au, was oxidized. In comparison, nearly the entire surface of monometallic Pd NPs was oxidized, suggesting that Au in Pd/Au NPs imparts oxidation resistance to Pd atoms. The surface Pd was found randomly distributed, presumably as a PdAu surface alloy, after reduction at 300 C. X-ray absorption spectroscopy provides direct evidence for the Pd-shell/Au-core structure of Pd/Au NPs, and suggests that metallic Pd in the Pd/Au NPs is a source for higher catalytic activity for aqueous-phase trichloroethene hydrodechlorination.

  2. From First Principles Design to Realization of Bimetallic Catalysts for Ultrahigh Selectivity - Final Project Report

    SciTech Connect (OSTI)

    Richard M. Crooks

    2007-04-11

    (A) Synthesis, Characterization, and Fundamental Properties of Bimetallic DENs. AuAg alloy and core/shell bimetallic DENs were synthesized and characterized. Selective extraction was used as a structural characterization tool for these bimetallic nanoparticles. This is significant because there are few easily accessible methods for structure elucidation of bimetallic nanoparticles in this size regime. As a first step towards the synthesis of catalytically active, bimetallic heterogeneous materials we reported the incorporation of Au and Pd monometallic DENs and AuPd bimetallic DENs into amorphous titania networks. The compositional fidelity of the original DENs, and to some extent their size, is retained following dendrimer removal. Gas-phase catalytic activity for CO oxidation is higher for the bimetallic catalysts than for the corresponding Pd-only and Au-only monometallics. (B) Electrocatalysts based on dendrimer-encapsulated nanoparticles. Platinum dendrimer-encapsulated nanoparticles (DENs) were prepared within fourth-generation, hydroxyl-terminated, poly(amidoamine) dendrimers and immobilized on glassy carbon electrodes using an electrochemical immobilization strategy. X-ray photoelectron spectroscopy, electron microscopy, and electrochemical experiments confirm that the Pt DENs are about 1.4 nm in diameter and that they remain within the dendrimer following surface immobilization. The resulting Pt DEN films were electrocatalytically active for the oxygen reduction reaction (ORR). The films are also robust, surviving up to 50 consecutive cyclic voltammograms and sonication. Monometallic Pd DENs were also prepared and found to have little catalytic activity for the ORR. However, PtPd bimetallic DENs had catalytic activity nearly identical to that found for Pt-only DENs. This indicates an overall catalytic enhancement for the bimetallic electrocatalysts.

  3. Neutral bimetallic transition metal phenoxyiminato catalysts and related polymerization methods

    DOE Patents [OSTI]

    Marks, Tobin J. (Evanston, IL); Rodriguez, Brandon A. (Evanston, IL); Delferro, Massimiliano (Chicago, IL)

    2012-08-07

    A catalyst composition comprising a neutral bimetallic diphenoxydiiminate complex of group 10 metals or Ni, Pd or Pt is disclosed. The compositions can be used for the preparation of homo- and co-polymers of olefinic monomer compounds.

  4. Glycerol Hydrogenolysis on Carbon-Supported PtRu and AuRu Bimetallic Catalysts

    SciTech Connect (OSTI)

    Maris,E.; Ketchie, W.; Murayama, M.; Davis, R.

    2007-01-01

    Bimetallic PtRu and AuRu catalysts were prepared by a surface redox method in which Pt or Au was deposited onto the surface of carbon-supported Ru nanoparticles with an average diameter of 2-3 nm. Characterization by H2 chemisorption, analytical TEM, and X-ray absorption spectroscopy at the Ru K-edge, Pt LIII-edge, and Au LIII-edge confirmed that Pt and Au were successfully deposited onto Ru without disrupting the Ru particles. Depression of the ethane hydrogenolysis rate over Ru after addition of Au provided further evidence of successful deposition. The bimetallic particles were subsequently evaluated in the aqueous-phase hydrogenolysis of glycerol at 473 K and 40 bar H2 at neutral and elevated pH. Although monometallic Pt and Ru exhibited different activities and selectivities to products, the bimetallic PtRu catalyst functioned more like Ru. A similar result was obtained for the AuRu bimetallic catalyst. The PtRu catalyst appeared to be stable under the aqueous-phase reaction conditions, whereas the AuRu catalyst was altered by the harsh conditions. Gold appeared to migrate off the Ru and agglomerate on the carbon during the reaction in liquid water.

  5. Correlating Extent of Pt–Ni Bond Formation with Low-temperature Hydrogenation of Benzene and 1,3-butadiene over Supported Pt/Ni Bimetallic Catalysts

    SciTech Connect (OSTI)

    Lonergan, W.; Vlachos, D; Chen, J

    2010-01-01

    Low-temperature hydrogenation of benzene and 1,3-butadiene on supported Pt/Ni catalysts have been used as probe reactions to correlate hydrogenation activity with the extent of Pt-Ni bimetallic bond formation. Pt/Ni bimetallic and Pt and Ni monometallic catalysts were supported on {gamma}-Al{sub 2}O{sub 3} using incipient wetness impregnation. Two sets of bimetallic catalysts were synthesized: one set to study the effect of metal atomic ratio and the other to study the effect of impregnation sequence. Fourier transform infrared spectroscopy (FTIR) CO adsorption studies were performed to characterize the surface composition of the bimetallic nanoparticles, and transmission electron microscopy (TEM) was utilized to characterize the particle size distribution. Batch reactor studies with FTIR demonstrated that all bimetallic catalysts outperformed monometallic catalysts for both benzene and 1,3-butadiene hydrogenation. Within the two sets of bimetallic catalysts, it was found that catalysts with a smaller Pt:Ni ratio possessed higher hydrogenation activity and that catalysts synthesized using co-impregnation had greater activity than sequentially impregnated catalysts. Extended X-ray absorption fine structure (EXAFS) measurements were performed in order to verify the extent of Pt-Ni bimetallic bond formation, which was found to correlate with the hydrogenation activity.

  6. Low-temperature aqueous-phase reforming of ethanol on bimetallic PdZn catalysts

    SciTech Connect (OSTI)

    Xiong, Haifeng; DelaRiva, Andrew; Wang, Yong; Dayte, Abhaya

    2015-01-01

    Bimetallic PdZn catalysts supported on carbon black (CB) and carbon nanotubes (CNTs) were found to be selective for CO-free H-2 production from ethanol at low temperature (250 degrees C). On Pd, the H-2 yield was low (similar to 0.3 mol H-2/mol ethanol reacted) and the CH4/CO2 ratio was high (similar to 1.7). Addition of Zn to Pd formed the intermetallic PdZn beta phase (atomic ratio of Zn to Pd is 1) with increased H-2 yield (similar to 1.9 mol H-2/mol ethanol reacted) and CH4/CO2 ratio of <1. The higher H-2 yield and low CH4 formation was related to the improved dehydrogenation activity of the L1(0) PdZn beta phase. The TOF increased with particle size and the CNTs provided the most active and selective catalysts, which may be ascribed to pore-confinement effects. Furthermore, no significant changes in either the supports or the PdZn beta particles was found after aqueous-phase reforming (APR) indicating that the metal nanoparticles and the carbon support are hydrothermally stable in the aqueous phase at elevated temperatures and pressures (>200 degrees C, 65 bar). No CO was detected for all the catalysts performed in aqueous-phase reaction, indicating that both monometallic Pd and bimetallic PdZn catalysts have high water-gas shift activity during APR. However, the yield of H-2 is considerably lower than the theoretical value of 6 H-2 per mole ethanol which is due to the presence of oxygenated products and methane on the PdZn catalysts.

  7. Surface spectroscopic characterization of oxide thin films and bimetallic model catalysts 

    E-Print Network [OSTI]

    Wei, Tao

    2009-05-15

    Oxide thin films and bimetallic model catalysts have been studied using metastable impact electron spectroscopy (MIES), ultraviolet photoelectron spectroscopy (UPS), low energy ion scattering spectroscopy (LEISS), X – ray photoelectron spectroscopy...

  8. Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction. Final report

    SciTech Connect (OSTI)

    Chunshan Song; Schobert, H.H.; Parfitt, D.P.

    1997-11-01

    Development of new catalysts is a promising approach to more efficient coal liquefaction. It has been recognized that dispersed catalysts are superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires intimate contact between the catalyst and coal. This research is a fundamental and exploratory study on catalytic coal liquefaction, with the emphasis on exploring novel bimetallic dispersed catalysts for coal liquefaction and the effectiveness of temperature-programmed liquefaction using dispersed catalysts. The primary objective of this research was to explore novel bimetallic dispersed catalysts from organometallic molecular precursors, that could be used in low concentrations but exhibit relatively high activity for efficient hydroliquefaction of coals under temperature-programmed conditions. We have synthesized and tested various catalyst precursors in liquefaction of subbituminous and bituminous coals and in model compound studies to examine how do the composition and structure of the catalytic precursors affect their effectiveness for coal liquefaction under different reaction conditions, and how do these factors affect their catalytic functions for hydrogenation of polyaromatic hydrocarbons, for cleavage of C-C bonds in polycyclic systems such as 4-(1-naphthylmethyl)bibenzyl, for hydrogenolysis of C-O bond such as that in dinaphthylether, for hydrodeoxygenation of phenolic compounds and other oxygen-containing compounds such as xanthene, and for hydrodesulfurization of polycyclic sulfur compounds such as dibenzothiophene. The novel bimetallic and monometallic precursors synthesized and tested in this project include various Mo- and Fe-based compounds.

  9. Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products

    SciTech Connect (OSTI)

    Rangan, Meghana; Yung, Matthew M.; Medlin, J. William (NREL); (Colorado)

    2011-11-17

    A combination of density functional theory (DFT) calculations and experimental studies of supported catalysts was used to identify H{sub 2}S-resistant biomass gasification product reforming catalysts. DFT calculations were used to search for bimetallic, nickel-based (1 1 1) surfaces with lower sulfur adsorption energies and enhanced ethylene adsorption energies. These metrics were used as predictors for H{sub 2}S resistance and activity toward steam reforming of ethylene, respectively. Relative to Ni, DFT studies found that the Ni/Sn surface alloy exhibited enhanced sulfur resistance and the Ni/Ru system exhibited an improved ethylene binding energy with a small increase in sulfur binding energy. A series of supported bimetallic nickel catalysts was prepared and screened under model ethylene reforming conditions and simulated biomass tar reforming conditions. The observed experimental trends in activity were consistent with theoretical predictions, with observed reforming activities in the order Ni/Ru > Ni > Ni/Sn. Interestingly, Ni/Ru showed a high level of resistance to sulfur poisoning compared with Ni. This sulfur resistance can be partly explained by trends in sulfur versus ethylene binding energy at different types of sites across the bimetallic surface.

  10. Bimetallic Cluster Provides a Higher Activity Electrocatalyst for Methanol Oxidation*

    E-Print Network [OSTI]

    Weidner, John W.

    Bimetallic Cluster Provides a Higher Activity Electrocatalyst for Methanol Oxidation* Brenda L:Ru nanoparticles on carbon (PtRu/C) for use as an electrocatalyst for methanol oxidation. This bimetallic carbonyl support particles. Cyclic voltammo- grams of methanol oxidation from the two catalysts showed

  11. Characterization of Na+- beta-Zeolite Supported Pd and Pd Ag Bimetallic Catalysts using EXAFS, TEM and Flow Reactor

    SciTech Connect (OSTI)

    Huang,W.; Lobo, R.; Chen, J.

    2008-01-01

    Flow reactor studies of the selective hydrogenation of acetylene in the presence of ethylene have been performed on Na+ exchanged {beta}-zeolite supported Pd, Ag and PdAg catalysts, as an extension of our previous batch reactor studies [W. Huang, J.R. McCormick, R.F. Lobo, J.G. Chen, J. Catal. 246 (2007) 40-51]. Results from flow reactor studies show that the PdAg/Na+-{beta}-zeolite bimetallic catalyst has lower activity than Pd/Na+-{beta}-zeolite monometallic catalyst, while Ag/Na+-{beta}-zeolite does not show any activity for acetylene hydrogenation. However, the selectivity for the PdAg bimetallic catalyst is much higher than that for either the Pd catalyst or Ag catalyst. The selectivity to byproduct (ethane) is greatly inhibited on the PdAg bimetallic catalyst as well. The results from the current flow reactor studies confirmed the pervious results from batch reactor studies [W. Huang, J.R. McCormick, R.F. Lobo, J.G. Chen, J. Catal. 246 (2007) 40-51]. In addition, we used transmission electron microscope (TEM), extended X-ray absorption fine structure (EXAFS), and FTIR of CO adsorption to confirm the formation of Pd-Ag bimetallic alloy in the PdAg/Na+-{beta}-zeolite catalyst.

  12. Spectroscopic characterization of monometallic and bimetallic model catalysts 

    E-Print Network [OSTI]

    Luo, Kai

    2009-06-02

    is the characterization of the surface composition, morphology, and electronic/geometric structure of the following catalysts: Au/TiOx, Au-Pd/Mo(110), Au- Pd/SiO2, Cu-Pd/Mo(110), and Sn/Pd(100). Structure-reactivity correlations during surface-alloy formation...

  13. Model hydrocracking reactions over monometallic and bimetallic dispersed catalysts

    SciTech Connect (OSTI)

    Schmidt, E.; Song, C. [Penn State Univ., University Park, PA (United States)

    1994-12-31

    Coal liquefaction involves the cleavage of methylene and dimethylene bridges connecting polycyclic aromatic units. The selected compound for model reactions is 4-(1-naphthylmethyl)bibenzyl (NMBB). This work describes the synthesis and screening of several metallic complex precursors as dispersed catalysts for hydrocracking of NMBB.

  14. Record activity and stability of dealloyed bimetallic catalysts for proton exchange membrane fuel cells

    E-Print Network [OSTI]

    Han, Binghong

    We demonstrate the unprecedented proton exchange membrane fuel cell (PEMFC) performance durability of a family of dealloyed Pt–Ni nanoparticle catalysts for the oxygen reduction reaction (ORR), exceeding scientific and ...

  15. 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.

  16. Ordered Nanoparticle Catalysts article is an Energy Focus > Archived...

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

    Ordered Nanoparticle Catalysts article is an Energy Focus January 24th, 2013 A Nature Materials paper on ordered nanoparticle catalysts has been highlighted as an "Energy...

  17. Controllable Deposition of Alloy Clusters or Nanoparticles Catalysts on Carbon Surfaces

    SciTech Connect (OSTI)

    Sasaki, K.; Ando, Y.; Su, D.; Adzic, R.

    2011-08-15

    We describe a simple method for controllably depositing Pt-Ru alloy nanoparticles on carbon surfaces that is mediated by Pb or Cu adlayers undergoing underpotential deposition and stripping during Pt and Ru codeposition at diffusion-limiting currents. The amount of surface Pt atoms deposited largely reflects the number of potential cycles causing the deposition and stripping of the metal adlayer at underpotentials, the metal species used as a mediator, and the scan rate of the potential cycles. We employed electrochemical methanol oxidation to gain information on the catalyst's activities. The catalysts with large amounts of surface Pt atoms have relatively high methanol-oxidation activity. Catalysts prepared using this method enhance methanol-oxidation activity per electrode surface area, while maintaining catalytic activity per surface Pt atom; thus, the amount of Pt is reduced in comparison with conventional methanol-oxidation catalysts. The method is suitable for efficient synthesizing various bimetallic catalysts.

  18. NiW and NiRu Bimetallic Catalysts for Ethylene Steam Reforming: Alternative Mechanisms for Sulfur Resistance

    SciTech Connect (OSTI)

    Rangan, M.; Yung, M. M.; Medlin, J. W.

    2012-06-01

    Previous investigations of Ni-based catalysts for the steam reforming of hydrocarbons have indicated that the addition of a second metal can reduce the effects of sulfur poisoning. Two systems that have previously shown promise for such applications, NiW and NiRu, are considered here for the steam reforming of ethylene, a key component of biomass derived tars. Monometallic and bimetallic Al{sub 2}O{sub 3}-supported Ni and W catalysts were employed for ethylene steam reforming in the presence and absence of sulfur. The NiW catalysts were less active than Ni in the absence of sulfur, but were more active in the presence of 50 ppm H{sub 2}S. The mechanism for the W-induced improvements in sulfur resistance appears to be different from that for Ru in NiRu. To probe reasons for the sulfur resistance of NiRu, the adsorption of S and C{sub 2}H{sub 4} on several bimetallic NiRu alloy surfaces ranging from 11 to 33 % Ru was studied using density functional theory (DFT). The DFT studies reveal that sulfur adsorption is generally favored on hollow sites containing Ru. Ethylene preferentially adsorbs atop the Ru atom in all the NiRu (111) alloys investigated. By comparing trends across the various bimetallic models considered, sulfur adsorption was observed to be correlated with the density of occupied states near the Fermi level while C{sub 2}H{sub 4} adsorption was correlated with the number of unoccupied states in the d-band. The diverging mechanisms for S and C{sub 2}H{sub 4} adsorption allow for bimetallic surfaces such as NiRu that enhance ethylene binding without accompanying increases in sulfur binding energy. In contrast, bimetallics such as NiSn and NiW appear to decrease the affinity of the surface for both the reagent and the poison.

  19. Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction. Technical progress report, October--December 1993

    SciTech Connect (OSTI)

    Schmidt, E.; Kirby, S.; Song, Chunshan; Schobert, H.H.

    1994-04-01

    Development of new catalysts is a promising approach to more, efficient coal liquefaction. It has been recognized that dispersed catalysts can be superior to supported catalysts for primary liquefaction of coals, because the control of initial coal dissolution or depolymerization requires infinite contact between the catalyst and coal. The primary objective of this research is to explore the potential of bimetallic dispersed catalysts from heterometallic molecular precursors in their use in model compound liquefaction reactions. This quarterly report describes the use of three precursors in model compound reactions. The first catalyst is a heterometallic complex consisting of two transition metals, Mo and Ni, and sulfur in a single molecule. The second is a thiocubane type complex consisting of cobalt, molybdenum and sulfur. The third is a thiocubane type cluster consisting of iron and sulfur and the fourth, the pure inorganic salt ammonium tetrathiomolybdate (ATM). It was found that the structure and the ligands in the model complexes affect the activity of the resulting catalyst significantly. The optimum reaction at a pressure of 6.9 MPa hydrogen gas varied for different catalysts. The bimetallic catalysts generated in situ from the organometallic precursor are more active than monometallic catalysts like ATTM and the thiocubane type cluster Fe{sub 4}. Main products are hydrogenated phenanthrene derivatives, like DBP, THP, sym-OHP, cis- and trans-unsym-OHP with minor isomerization products such as sym-OHA. Our results indicate that other transition metal and ligand combinations in the organometallic precursors and the use of another model compound could result in substantially higher conversion activity.

  20. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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

    of Rh and Pd under alternating oxidizing and catalytic conditions. Measurements for each system began with as-prepared samples at room temperature in ultrahigh vacuum and...

  1. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  2. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  3. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  4. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  5. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  6. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  7. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  8. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  9. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  10. Reaction-Driven Restructuring of Bimetallic Nanoparticle Catalysts

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  11. The Phase of Iron Catalyst Nanoparticles during Carbon Nanotube Growth

    E-Print Network [OSTI]

    Wirth, Christoph T.; Bayer, Bernhard C.; Gamalski, Andrew D.; Esconjauregui, Santiago; Weatherup, Robert S.; Ducati, Caterina; Baehtz, Carsten; Robertson, John; Hofmann, Stephan

    2012-11-28

    growth modes occur upon hydrocarbon exposure: For ?-rich Fe nanoparticle distributions, metallic Fe is the active catalyst phase, implying that carbide formation is not a prerequisite for nanotube growth. For ?-rich catalyst mixtures, Fe3C formation more...

  12. Structurally ordered Pt–Zn/C series nanoparticles as efficient anode catalysts for formic acid electrooxidation

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

    Zhu, Jing; Zheng, Xin; Wang, Jie; Wu, Zexing; Han, Lili; Lin, Ruoqian; Xin, Huolin L.; Wang, Deli

    2015-09-15

    Controlling the size, composition, and structure of bimetallic nanoparticles is of particular interest in the field of electrocatalysts for fuel cells. In the present work, structurally ordered nanoparticles with intermetallic phases of Pt3Zn and PtZn have been successfully synthesized via an impregnation reduction method, followed by post heat-treatment. The Pt3Zn and PtZn ordered intermetallic nanoparticles are well dispersed on a carbon support with ultrasmall mean particle sizes of ~5 nm and ~3 nm in diameter, respectively, which are credited to the evaporation of the zinc element at high temperature. These catalysts are less susceptible to CO poisoning relative to Pt/Cmore »and exhibited enhanced catalytic activity and stability toward formic acid electrooxidation. The mass activities of the as-prepared catalysts were approximately 2 to 3 times that of commercial Pt at 0.5 V (vs. RHE). As a result, this facile synthetic strategy is scalable for mass production of catalytic materials.« less

  13. Supported catalysts using nanoparticles as the support material

    DOE Patents [OSTI]

    Wong, Michael S. (Houston, TX); Wachs, Israel E. (Bethlehem, PA); Knowles, William V. (Pearland, TX)

    2010-11-02

    A process for making a porous catalyst, comprises a) providing an aqueous solution containing a nanoparticle precursor, b) forming a composition containing nanoparticles, c) adding a first catalytic component or precursor thereof and a pore-forming agent to the composition containing nanoparticles and allowing the first catalytic component, the pore-forming agent, and the nanoparticles form an organic-inorganic structure, d) removing water from the organic-inorganic structure; and e) removing the pore-forming agent from the organic-inorganic structure so as to yield a porous catalyst.

  14. 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.

  15. Carbon-Supported bimetallic Pd-Fe catalysts for vapor-phase hydrodeoxygenation of guaiacol

    SciTech Connect (OSTI)

    Sun, Junming; Karim, Ayman M.; Zhang, He; Kovarik, Libor; Li, Xiaohong S.; Hensley, Alyssa; McEwen, Jean-Sabin; Wang, Yong

    2013-10-01

    Abstract Carbon supported metal catalysts (Cu/C, Fe/C, Pd/C, Pt/C, PdFe/C and Ru/C) have been prepared, characterized and tested for vapor-phase hydrodeoxygenation (HDO) of guaiacol (GUA) at atmospheric pressure. Phenol was the major intermediate on all catalysts. Over the noble metal catalysts saturation of the aromatic ring was the major pathway observed at low temperature (250 °C), forming predominantly cyclohexanone and cyclohexanol. Substantial ring opening reaction was observed on Pt/C and Ru/C at higher reaction temperatures (e.g., 350 °C). Base metal catalysts, especially Fe/C, were found to exhibit high HDO activity without ring-saturation or ring-opening with the main products being benzene, phenol along with small amounts of cresol, toluene and trimethylbenzene (TMB). A substantial enhancement in HDO activity was observed on the PdFe/C catalysts. Compared with Fe/C, the yield to oxygen-free aromatic products (i.e., benzene/toluene/TMB) on PdFe/C increased by a factor of four at 350 °C, and by approximately a factor of two (83.2% versus 43.3%) at 450 °C. The enhanced activity of PdFe/C is attributed to the formation of PdFe alloy as evidenced by STEM, EDS and TPR.

  16. From First Principles Design to Realization of Bimetallic Catalysts for Enhanced Selectivity

    SciTech Connect (OSTI)

    Lobo, Raul F.; Crooks, Richard M.; Mavrikakis, Manos

    2014-04-08

    “Catalysis by design” has been a dream for decades. To specify the composition and structure of matter to effect a desired catalytic transformation with desired and predicted rate and selectivity remains a monumental challenge, especially in heterogeneous catalysis. Our research thrusts have been chosen not only for their practical and scientific relevance, e.g. for more efficient and sustainable chemicals and fuels production, but also because they provide a foundation for developing and exploring broadly applicable principles and strategies for catalyst design.

  17. PUBLISHED ONLINE: 20 FEBRUARY 2014 | DOI: 10.1038/NMAT3872 Platinumcobalt bimetallic nanoparticles in hollow

    E-Print Network [OSTI]

    Cai, Long

    of intermetallic phases generally needs high temperatures, which easily leads to the aggregation of bimetallic-exchange with the abundant carboxylate groups (Pt@HPS-Co2+ ). In the third step, the polymer product of Pt@HPS-Co2 and Ferdi Schüth* The synthesis of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) is a highly

  18. Bimetallic Ni-Rh catalysts with low amounts of Rh for the steam and autothermal reforming of n-butane for fuel-cell applications.

    SciTech Connect (OSTI)

    Ferrandon, M.; Kropf, A. J.; Krause, T.; Chemical Sciences and Engineering Division

    2010-05-15

    Mono-metallic nickel and rhodium catalysts and bimetallic Ni-Rh catalysts supported on La-Al{sub 2}O{sub 3}, CeZrO{sub 2} and CeMgOx were prepared and evaluated for catalyzing the steam and autothermal reforming of n-butane. The binary Ni-Rh supported on La-Al{sub 2}O{sub 3} catalysts with low weight loading of rhodium exhibited higher H{sub 2} yields than Ni or Rh alone. The Ni-Rh/CeZrO{sub 2} catalyst exhibited higher performance and no coke formation, compared to the same metals on other supports. A NiAl{sub 2}O{sub 4} spinel phase was obtained on all Ni and Ni-Rh catalysts supported on La-Al{sub 2}O{sub 3}. The presence of rhodium stabilized the spinel phase as well as NiOx species upon reforming while Ni alone was mostly reduced into metallic species. Extended X-ray absorption fine-structure analysis showed evidence of Ni-Rh alloy during preparation and even further after an accelerated aging at 900C in a H{sub 2}/H{sub 2}O atmosphere.

  19. Graphdiyne as a Promising Substrate for Stabilizing Pt Nanoparticle Catalyst

    E-Print Network [OSTI]

    Lin, Zheng-Zhe

    2015-01-01

    At present, Pt nanoparticle catalysts in fuel cells suffer from aggregation and loss of chemical activity. In this work, graphdiyne, which has natural porous structure, was proposed as substrate with high adsorption ability to stabilize Pt nanoparticles. Using multiscale calculations by ab initio method and the ReaxFF potential, geometry optimizations, molecular dynamics simulations, Metropolis Monte Carlo simulations and minimum energy paths calculations were performed to investigate the adsorption energy and the rates of desorption and migration of Pt nanoparticles on graphdiyne and graphene. According to the comparison between graphdiyne and graphene, it was found that the high adsorption ability of graphdiyne can avoid Pt nanoparticle migration and aggregation on substrate. Then, simulations indicated the potential catalytic ability of graphdiyne-Pt-nanoparticle system to the oxygen reduction reaction in fuel cells. In summary, graphdiyne should be an excellent material to replace graphite or amorphous ca...

  20. Metal nanoparticles as a conductive catalyst

    DOE Patents [OSTI]

    Coker, Eric N. (Albuquerque, NM)

    2010-08-03

    A metal nanocluster composite material for use as a conductive catalyst. The metal nanocluster composite material has metal nanoclusters on a carbon substrate formed within a porous zeolitic material, forming stable metal nanoclusters with a size distribution between 0.6-10 nm and, more particularly, nanoclusters with a size distribution in a range as low as 0.6-0.9 nm.

  1. Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction. Quarterly technical progress report, July--September 1995

    SciTech Connect (OSTI)

    Song, Chunshan; Schmidt, E.; Schobert, H.H.

    1996-01-01

    Coal liquefaction involves cleavage of methylene, dimethylene and ether bridges connecting polycyclic aromatic units and the reactions of various oxygen functional groups. Here in this quarterly, we report on the hydrocracking of 4-(l-naphthylmethyl)bibenzyl in the presence of iron (Fe) catalysts and sulfur and residual wall catalytic effect. Catalytic hydrocracking of 4-(1-naphthylmethyl)bibenzyl (NMBB) predominantly yielded naphthalene and 4-methylbibenzyl. Various iron compounds were examined as catalyst precursors. Sulfur addition to most catalyst precursors led to substantially higher catalyst activity and higher conversion. NMBB was also treated with sulfur in the absence of iron compounds, in concentrations of 1.2-3.4 wt%, corresponding to the conditions present in reactions with added iron compounds. Increasing sulfur concentrations led to higher NMBB conversions. Furthermore, sulfur had a permanent effect on the reactor walls. A black sulfide layer formed on the surface which could not be removed mechanically. The supposed non-catalytic reactions done in the same reactor but after experiments with added sulfur showed higher conversions than comparable experiments done in new reactors. This wall catalytic effect can be reduced by treating the sulfided reactors with hydrochloric acid. The results of this work demonstrate the significant effect of sulfur addition and sulfur-induced residual wall effects on carbon-carbon bond cleavage and hydrogenation of aromatics.

  2. AuRu/AC as an effective catalyst for hydrogenation reactions

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

    Villa, Alberto; Chan-Thaw, Carine E.; Campisi, Sebastiano; Bianchi, Claudia L.; Wang, Di; Kotula, Paul G.; Kübel, Christian; Prati, Laura

    2015-03-23

    AuRu bimetallic catalysts have been prepared by sequential deposition of Au on Ru or vice versa obtaining different nanostructures: when Ru has been deposited on Au, a Aucore–Rushell has been observed, whereas the deposition of Au on Ru leads to a bimetallic phase with Ru enrichment on the surface. In the latter case, the unexpected Ru enrichment could be attributed to the weak adhesion of Ru on the carbon support, thus allowing Ru particles to diffuse on Au particles. Both structures result very active in catalysing the liquid phase hydrogenolysis of glycerol and levulinic acid but the activity, the selectivitymore »and the stability depend on the structure of the bimetallic nanoparticles. Ru@Au/AC core–shell structure mostly behaved as the monometallic Ru, whereas the presence of bimetallic AuRu phase in Au@Ru/AC provides a great beneficial effect on both activity and stability.« less

  3. Structure-function relationships in dendrimer-encapsulated metal nanoparticles 

    E-Print Network [OSTI]

    Wilson, Orla Mary

    2006-04-12

    The synthesis, characterization and structure-function relationships of mono- and bimetallic dendrimerencapsulated nanoparticles (DENs) are described. Control over the factors influencing the structure of bimetallic DENs ...

  4. Au-Pt heteroaggregate dendritic nanostructures and Au-Pt alloy nanoparticles and their use as catalysts

    DOE Patents [OSTI]

    Eichhorn, Bryan W. (University Park, MD); Zhou, Shenghu (Greenbelt, MD); Jackson, Gregory Scott (University Park, MD)

    2011-10-18

    Au--Pt heteroaggregate dendritic nanostructures and AuPt alloy nanoparticles, and their use as anodic catalysts in fuel cells.

  5. Biomimetic Catalysts of Graphene Conjugates and Palladium Nanoparticles

    E-Print Network [OSTI]

    Xue, Teng

    2014-01-01

    Stahl, S. S. Ligand-modulated palladium oxidation catalysis:BINAP-stabilized gold and palladium nanoparticles with smallsize and their palladium nanoparticle-catalyzed asymmetric

  6. BIMETALLIC NANOCATALYSTS IN MESOPOROUS SILICA FOR HYDROGEN PRODUCTION FROM COAL-DERIVED FUELS

    SciTech Connect (OSTI)

    Kuila, Debasish; Ilias, Shamsuddin

    2013-02-13

    In steam reforming reactions (SRRs) of alkanes and alcohols to produce H{sub 2}, noble metals such as platinum (Pt) and palladium (Pd) are extensively used as catalyst. These metals are expensive; so, to reduce noble-metal loading, bi-metallic nanocatalysts containing non-noble metals in MCM-41 (Mobil Composition of Material No. 41, a mesoporous material) as a support material with high-surface area were synthesized using one-pot hydrothermal procedure with a surfactant such as cetyltrimethylammonium bromide (CTAB) as a template. Bi-metallic nanocatalysts of Pd-Ni and Pd-Co with varying metal loadings in MCM-41 were characterized by x-ray diffraction (XRD), N{sub 2} adsorption, and Transmission electron microscopy (TEM) techniques. The BET surface area of MCM-41 (~1000 m{sup 2}/g) containing metal nanoparticles decreases with the increase in metal loading. The FTIR studies confirm strong interaction between Si-O-M (M = Pd, Ni, Co) units and successful inclusion of metal into the mesoporous silica matrix. The catalyst activities were examined in steam reforming of methanol (SRM) reactions to produce hydrogen. Reference tests using catalysts containing individual metals (Pd, Ni and Co) were also performed to investigate the effect of the bimetallic system on the catalytic behavior in the SRM reactions. The bimetallic system remarkably improves the hydrogen selectivity, methanol conversion and stability of the catalyst. The results are consistent with a synergistic behavior for the Pd-Ni-bimetallic system. The performance, durability and thermal stability of the Pd-Ni/MCM-41 and Pd-Co/MCM-41 suggest that these materials may be promising catalysts for hydrogen production from biofuels. A part of this work for synthesis and characterization of Pd-Ni-MCM-41 and its activity for SRM reactions has been published (“Development of Mesoporous Silica Encapsulated Pd-Ni Nanocatalyst for Hydrogen Production” in “Production and Purification of Ultraclean Transportation Fuels”; Hu, Y., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2011.)

  7. Monodisperse metal nanoparticle catalysts on silica mesoporous supports: synthesis, characterizations, and catalytic reactions

    SciTech Connect (OSTI)

    Somorjai, G.A.

    2009-09-14

    The design of high performance catalyst achieving near 100% product selectivity at maximum activity is one of the most important goals in the modern catalytic science research. To this end, the preparation of model catalysts whose catalytic performances can be predicted in a systematic and rational manner is of significant importance, which thereby allows understanding of the molecular ingredients affecting the catalytic performances. We have designed novel 3-dimensional (3D) high surface area model catalysts by the integration of colloidal metal nanoparticles and mesoporous silica supports. Monodisperse colloidal metal NPs with controllable size and shape were synthesized using dendrimers, polymers, or surfactants as the surface stabilizers. The size of Pt, and Rh nanoparticles can be varied from sub 1 nm to 15 nm, while the shape of Pt can be controlled to cube, cuboctahedron, and octahedron. The 3D model catalysts were generated by the incorporation of metal nanoparticles into the pores of mesoporous silica supports via two methods: capillary inclusion (CI) and nanoparticle encapsulation (NE). The former method relies on the sonication-induced inclusion of metal nanoparticles into the pores of mesoporous silica, whereas the latter is performed by the encapsulation of metal nanoparticles during the hydrothermal synthesis of mesoporous silica. The 3D model catalysts were comprehensively characterized by a variety of physical and chemical methods. These catalysts were found to show structure sensitivity in hydrocarbon conversion reactions. The Pt NPs supported on mesoporous SBA-15 silica (Pt/SBA-15) displayed significant particle size sensitivity in ethane hydrogenolysis over the size range of 1-7 nm. The Pt/SBA-15 catalysts also exhibited particle size dependent product selectivity in cyclohexene hydrogenation, crotonaldehyde hydrogenation, and pyrrole hydrogenation. The Rh loaded SBA-15 silica catalyst showed structure sensitivity in CO oxidation reaction. In addition, Pt-mesoporous silica core-shell structured NPs (Pt{at}mSiO{sub 2}) were prepared, where the individual Pt NP is encapsulated by the mesoporous silica layer. The Pt{at}mSiO{sub 2} catalysts showed promising catalytic activity in high temperature CO oxidation. The design of catalytic structures with tunable parameters by rational synthetic methods presents a major advance in the field of catalyst synthesis, which would lead to uncover the structure-function relationships in heterogeneous catalytic reactions.

  8. Palladium was supported on superparamagnetic nanoparticles: A magnetically recoverable catalyst for Heck reaction

    SciTech Connect (OSTI)

    Zhang, Fengwei; Niu, Jianrui; Wang, Haibo; Yang, Honglei; Jin, Jun; Liu, Na; Zhang, Yubin [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)] [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Li, Rong, E-mail: liyirong@lzu.edu.cn [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)] [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Ma, Jiantai, E-mail: majiantai@lzu.edu.cn [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)] [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)

    2012-02-15

    Highlights: Black-Right-Pointing-Pointer Palladium-based heterogeneous catalyst was prepared facilely via the co-precipitation method. Black-Right-Pointing-Pointer The particles are nearly spherical in shape with an average size of 20 {+-} 1.0 nm. Black-Right-Pointing-Pointer The developed magnetic catalyst showed high activity for Heck reaction. Black-Right-Pointing-Pointer The catalyst was easily recovered from the reaction mixture with external magnetic field. Black-Right-Pointing-Pointer The catalytic efficiency for Heck reaction remains unaltered even after 6 repeated cycles. -- Abstract: A novel and high-performance palladium-based catalyst for Heck reaction was prepared easily by the co-precipitation method. The catalyst was characterized by transmission electron microscopy (TEM), X-ray powder diffraction (XRD), vibrating sample magnetometry (VSM), X-ray photoelectron spectroscopy (XPS) and atomic absorption spectrophotometry (AAS). The catalyst afforded a fast conversion of the 4-bromonitrobenzene to 4-nitrostilbene at a catalyst loading of 5 mol%, and the efficiency of the catalyst remains unaltered even after 6 repeated cycles. The excellent catalytic performance of the Pd/Fe{sub 3}O{sub 4} catalyst might be attributed to the enhanced synergistic effect between Pd nanoparticles and magnetite.

  9. Dendrimer-Encapsulated Ruthenium Nanoparticles as Catalysts for Lithium-O2 Batteries

    SciTech Connect (OSTI)

    Bhattacharya, Priyanka; Nasybulin, Eduard N.; Engelhard, Mark H.; Kovarik, Libor; Bowden, Mark E.; Li, Shari; Gaspar, Daniel J.; Xu, Wu; Zhang, Jiguang

    2014-12-01

    Dendrimer-encapsulated ruthenium nanoparticles (DEN-Ru) have been used as catalysts in lithium-O2 batteries for the first time. Results obtained from UV-vis spectroscopy, electron microscopy and X-ray photoelectron spectroscopy show that the nanoparticles synthesized by the dendrimer template method are ruthenium oxide instead of metallic ruthenium reported earlier by other groups. The DEN-Ru significantly improve the cycling stability of lithium (Li)-O2 batteries with carbon black electrodes and decrease the charging potential even at low catalyst loading. The monodispersity, porosity and large number of surface functionalities of the dendrimer template prevent the aggregation of the ruthenium nanoparticles making their entire surface area available for catalysis. The potential of using DEN-Ru as stand-alone cathode materials for Li-O2 batteries is also explored.

  10. NOVEL PREPARATION AND MAGNETO CHEMICAL CHARACTERIZATION OF NANOPARTICLE MIXED ALCOHOL CATALYSTS

    SciTech Connect (OSTI)

    Seetala V. Naidu; Upali Siriwardane

    2005-05-24

    We have developed and streamlined the experimental systems: (a) Laser-induced solution deposition (LISD) photosynthesis, ball-milling, and chemical synthesis of Fe, Co, and Cu nanoparticle catalysts; (b) Sol-gel method for mesoporous {gamma}-Al{sub 2}O{sub 3}, SiO{sub 2}, hybrid alumina/silica granular supports; (c) Three sol-gel/oil-drop catalyst preparation methods to incorporate metal nanoparticles into mesoporous 1 mm granular supports; (d) Low-cost GC-TCD system with hydrogen as carrier gas for the determination of wide spectrum of alkanes produced during the F-T reactions; and (e) Gas-flow reactor and microchannel reactor for fast screening of catalysts. The LISD method could produce Co, Cu, and Fe (5 nm) nanoparticles, but in milligram quantities. We could produce nanoparticles in gram quantities using high-energy ball milling and chemical synthesis methods. Ball milling gave wide particle size distribution compared to the chemical synthesis method that gave almost uniform size ({approx}5 nm) particles. Metal nanoparticles Cu, Co, Fe, Cu/Co, Cu/Fe and Co/Fe were loaded (2-12 wt%) uniformly into {gamma}-Al{sub 2}O{sub 3}, SiO{sub 2}, or alumina/silica hybrid supports by combined sol-gel/oil-drop methods followed by calcination and hydrogenation steps, prior to syngas FT reaction studies. The properties of metal loaded {gamma}-Al{sub 2}O{sub 3} granules were compared for the two precursors: aluminum tri-sec-butoxide (ALTSB) and aluminum tri-iso-propoxide (ALTIP). The effect of solgel supports alumina, silica, and alumina/silica hybrid were examined on catalytic properties. Metal loading efficiencies for pure metal catalysts increased in the order Co, Cu and Fe in agreement with solubility of metal hydroxides. In case of mixed metals, Co and Cu seams to interfere and reduce Fe metal loading when metal nitrate solutions are used. The solubility differences of metal hydroxides would not allow precise control of metal loading. We have overcome this problem by introducing a novel method of nanoparticle metal oxide co-entrapped sol-gel that gave the highest metal loading with precise control and reproducibility, and greater mechanical strength of granules than the metal nitrate solution co-entrapping and wet impregnation methods. Both, slurry-phase-batch and gas-phase-continuous-flow, reactors were used for syngas conversion reactions. Our investigations of Co and Fe thin film deposited micro-reactors showed higher CO/H{sub 2} conversion for Fe compared to Co. The catalytic activity for CO/H{sub 2} conversion was observed in the increasing order for the nanocatalysts Cu, Co, Fe, Co/Fe, Cu/Co and Cu/Fe in alumina sol-gel support, and Co/Fe showed the highest yield for methane. The optimization of CO/H{sub 2} ratio indicated that 1:1 ratio gave more alkanes distribution in F-T process with Co/Fe (6% each) impregnated on alumina. We could estimate the activity of catalysts (involving Co, Fe) during hydrogenation and after catalytic reaction using magnetization studies. In summary our accomplishments are: (1) Novel chemical methods for the synthesis of (5 nm) Fe, Co, Cu nanoparticles with narrow size distribution. (2) Developing a method of metal oxide nanoparticles addition to alumina/silica sol-gel to control metal loading of pure and mixed metal catalysts compositions in high yields. (3) A low-cost GC-TCD system to analyze wide spectrum of alkanes (F-T reaction products). (4) Fe/Co mixed metal alumina/silica mesoporous catalysts with higher FT activity. (5) Characterizing nanoparticle catalysts and supports for detail understanding of FT-process.

  11. Improved Catalysts for Heavy Oil Upgrading Based on Zeolite Y Nanoparticles Encapsulated Stable Nanoporous Host

    SciTech Connect (OSTI)

    Conrad Ingram; Mark Mitchell

    2007-09-30

    The objective of this project is to synthesize nanocrystals of highly acidic zeolite Y nanoclusters, encapsulate them within the channels of mesoporous (nanoporous) silicates or nanoporous organosilicates, and evaluate the 'zeolite Y/Nanoporous host' composites as catalysts for the upgrading of heavy petroleum feedstocks. In comparison to conventionally-used zeolite Y catalysts of micron size particles, the nanocrystals (< 100 nm particle size) which contain shorter path lengths, are expected to allow faster diffusion of large hydrocarbon substrates and the catalysis products within and out of the zeolite's channels and cages (<1 nm size). This is expected to significantly reduce deactivation of the catalyst and to prolong their period of reactivity. Encapsulating zeolite Y nanocrystals within the nanoporous materials is expected to protect its external surfaces and pore entrances from being blocked by large hydrocarbon substrates, since these substrates will initially be converted to small molecules by the nanoporous host (a catalyst in its own right). The project consisted of four major tasks as follows: (1) synthesis of the nanoparticles of zeolite Y (of various chemical compositions) using various techniques such as the addition of organic additives to conventional zeolite Y synthesis mixtures to suppress zeolite Y crystal growth; (2) synthesis of nanoporous silicate host materials of up to 30 nm pore diameter, using poly (alkylene oxide) copolymers which when removed will yield a mesoporous material; (3) synthesis of zeolite Y/Nanoporous Host composite materials as potential catalysts; and (4) evaluation of the catalyst for the upgrading of heavy petroleum feedstocks.

  12. Dispersion enhanced metal/zeolite catalysts

    DOE Patents [OSTI]

    Sachtler, W.M.H.; Tzou, M.S.; Jiang, H.J.

    1987-03-31

    Dispersion stabilized zeolite supported metal catalysts are provided as bimetallic catalyst combinations. The catalyst metal is in a reduced zero valent form while the dispersion stabilizer metal is in an unreduced ionic form. Representative catalysts are prepared from platinum or nickel as the catalyst metal and iron or chromium dispersion stabilizer.

  13. Structure-Property Relationship in Metal Carbides and Bimetallic Alloys

    SciTech Connect (OSTI)

    Chen, Jingguan

    2014-03-04

    The primary objective of our DOE/BES sponsored research is to use carbide and bimetallic catalysts as model systems to demonstrate the feasibility of tuning the catalytic activity, selectivity and stability. Our efforts involve three parallel approaches, with the aim at studying single crystal model surfaces and bridging the “materials gap” and “pressure gap” between fundamental surface science studies and real world catalysis. The utilization of the three parallel approaches has led to the discovery of many intriguing catalytic properties of carbide and bimetallic surfaces and catalysts. During the past funding period we have utilized these combined research approaches to explore the possibility of predicting and verifying bimetallic and carbide combinations with enhanced catalytic activity, selectivity and stability.

  14. NOVEL PREPARATION AND MAGNETO CHEMICAL CHARACTERIZATION OF NANO-PARTICLE MIXED ALCOHOL CATALYSTS

    SciTech Connect (OSTI)

    Setala V. Naidu

    2003-01-01

    We have produced Co, Cu, and Fe nano-particles by Laser-induced solution deposition (LISD) as evidenced by TEM investigations. Sizes of the nano-particles created are in the order of 5 nm. The LISD system could generate nano-particles in quantities only in the order of a milligram. This may be mainly due to the limited photo induced reactions taking place on the surface of the solutions. We have designed experiments to use drop flow technique with LISD for nano-particle deposition on microreactors. Preliminary work has been done on Co and Fe thin film deposited microreactors. We are also investigating the catalytic properties of nano-particles of FeO and CoO prepared by ball milling and dispersed into sol-gel prepared alumina granules. We have continued our investigation of catalytic reactions of Cu, Co, Fe, Cu/Co, Cu/Fe and Co/Fe on alumina support. The metal oxides were first reduced with hydrogen and used for the conversion of CO/H{sub 2}. The surface area of the catalysts has been determined by nitrogen disorption. They are in the range of 200-300 m{sup 2}/g. Cu, Co, Fe, Co/Fe, Cu/Co and Cu/Fe showed increasing order of catalytic activity for CO/H{sub 2} conversion. We are also studying catalytic conversion rates for CO{sub 2}/H{sub 2} and CO/CO{sub 2}/H{sub 2} mixtures using these catalysts. Our investigations of Co and Fe thin film deposited microreactors showed higher CO/H{sub 2} conversion for Fe compared to Co. We have used vibrating sample magnetometer (VSM) to study the magnetic characteristics of as prepared, reduced, post-reaction catalysts. Comparative study of the ferromagnetic component of these samples gives the reduction efficiency and the changes in metal centers during catalytic reactions. Magnetic studies of post-reaction Co and Fe micro-reactors show that more carbide formation occurs for iron compared to cobalt.

  15. On the nature of the deactivation of supported palladium nanoparticle catalysts in the decarboxylation of fatty acids.

    SciTech Connect (OSTI)

    Ping, E. W.; Pierson, J.; Wallace, R.; Miller, J. T.; Fuller, T. F.; Jones, C. W.

    2011-04-15

    Supported palladium catalysts are effective catalysts for the hydrogen-free decarboxylation of fatty acids. However, the catalysts deactivate severely after one use. Here, the recyclability of a well-defined, mesoporous silica-supported palladium nanoparticle catalyst is evaluated in the batch decarboxylation of stearic acid at 300 C under inert atmosphere, producing n-heptadecane. The nature of the catalyst deactivation is examined in detail via an array of characterization techniques. X-ray photoelectron spectroscopy (XPS) demonstrates that little palladium surface oxidation occurs over the course of the reaction, and a combination of X-ray absorption spectroscopy and transmission electron microscopy (TEM) suggests negligible particle sintering or agglomeration. Physisorption and chemisorption measurements demonstrate substantial loss in total surface area and porosity as well as accessible palladium surface area with these losses attributed to significant organic deposition on the catalyst, as verified via thermogravimetric analysis. High temperature calcination is applied to combust and remove these residues, but resultant nanoparticle agglomeration is significant. Solid state nuclear magnetic resonance spectroscopy (NMR), Fourier transform infrared spectroscopy (FT-IR) and solid dissolution followed by organic extraction methodologies demonstrate that the carbonaceous deposits are not coke but rather strongly adsorbed reactants and products. Detrimental coke formation, as suggested by prior literature, is verified to be absent, as extraction of the surface-deposited organic species yields nearly complete recovery of the total surface area, pore volume, and active palladium surface area. Furthermore, the regenerated catalyst exhibits a corresponding significant recovery of decarboxylation activity.

  16. Palladium nanoparticles produced by fermentatively cultivated bacteria as catalyst for diatrizoate removal with biogenic hydrogen

    SciTech Connect (OSTI)

    Hennebel, T.; Fitts, J.; Nevel, S. V.; Verschuere, S.; De Corte, S.; De Gusseme, B.; Cuvelier, C.; van der Lelie, D.; Boon, N.; Verstraete, W.

    2011-05-17

    A new biological inspired method to produce nanopalladium is the precipitation of Pd on a bacterium, i.e., bio-Pd. This bio-Pd can be applied as catalyst in dehalogenation reactions. However, large amounts of hydrogen are required as electron donor in these reactions resulting in considerable costs. This study demonstrates how bacteria, cultivated under fermentative conditions, can be used to reductively precipitate bio-Pd catalysts and generate the electron donor hydrogen. In this way, one could avoid the costs coupled to hydrogen supply. The catalytic activities of Pd(0) nanoparticles produced by different strains of bacteria (bio-Pd) cultivated under fermentative conditions were compared in terms of their ability to dehalogenate the recalcitrant aqueous pollutants diatrizoate and trichloroethylene. While all of the fermentative bio-Pd preparations followed first order kinetics in the dehalogenation of diatrizoate, the catalytic activity differed systematically according to hydrogen production and starting Pd(II) concentration in solution. Batch reactors with nanoparticles formed by Citrobacter braakii showed the highest diatrizoate dehalogenation activity with first order constants of 0.45 {+-} 0.02 h{sup -1} and 5.58 {+-} 0.6 h{sup -1} in batches with initial concentrations of 10 and 50 mg L{sup -1} Pd, respectively. Nanoparticles on C. braakii, used in a membrane bioreactor treating influent containing 20 mg L{sup -1} diatrizoate, were capable of dehalogenating 22 mg diatrizoate mg{sup -1} Pd over a period of 19 days before bio-Pd catalytic activity was exhausted. This study demonstrates the possibility to use the combination of Pd(II), a carbon source and bacteria under fermentative conditions for the abatement of environmental halogenated contaminants.

  17. Hydrodechlorination of 1,2-Dichloroethane Catalyzedby Dendrimer-Derived Pt-Cu/SiO2 Catalysts

    SciTech Connect (OSTI)

    Xie, Hong; Howe, Jane Y; Schwartz, Viviane; Monnier, J. R.; Williams, Christopher T.; Ploehn, Harry J.

    2008-01-01

    Dendrimer-metal-nanocomposites (DMNs) were used as precursors to prepare SiO2 supported monometallic Pt, Cu and bimetallic Pt-Cu catalysts with Pt/Cu atomic ratios of 1:1 (Pt50Cu50) and 1:3 (Pt25Cu75). After impregnation of these DMNs onto the support, the catalysts were thermally treated and activated following an optimized protocol. Scanning transmission electron microscopy (STEM) shows that the metal nanoparticles in dendrimer-derived SiO2-supported catalysts are smaller and have a more narrow size distribution than those in conventional catalysts prepared using corresponding metal salts via the wet impregnation method. Slow deactivation was observed for hydrodechlorination of 1,2-dichloroethane over monometallic Cu catalysts, which showed an activity about one to two orders of magnitude lower than that of the Pt-containing catalysts. Hydrodechlorination of 1,2-dichloroethane over Pt and Pt50Cu50 catalysts mainly produces ethane and the selectivity towards ethane increases with temperature. For Pt25Cu75 catalyst, the selectivity towards ethane decreases in favor of ethylene. The overall activity decreases with increasing Cu loading in the catalysts. Activity based on surface Pt sites suggests the formation of bi-functional surfaces in Pt25Cu75 catalyst favoring C-Cl bond scission on Cu sites and hydrogenation of intermediate .CH2CH2. on Pt sites. Furthermore, kinetic analyses suggest different reaction mechanisms for hydrodechlorination of 1,2-dichloroethane over Pt and Cu-enriched surfaces in the Pt-Cu bimetallic catalysts.

  18. Displacement of Hexanol by the Hexanoic Acid Overoxidation Product in Alcohol Oxidation on a Model Supported Palladium Nanoparticle Catalyst

    SciTech Connect (OSTI)

    Buchbinder, Avram M. [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Inst. for Catalysis in Energy Processes; Ray, Natalie A. [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Lu, Junling [Argonne National Lab. (ANL), Argonne, IL (United States). Energy System Division; Van Duyne, Richard P. [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Inst. for Catalysis in Energy Processes; Stair, Peter C. [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Inst. for Catalysis in Energy Processes; Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Weitz, Eric [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Inst. for Catalysis in Energy Processes; Geiger, Franz M. [Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry; Center for Catalysis and Surface Science; Inst. for Catalysis in Energy Processes

    2011-11-09

    This work characterizes the adsorption, structure, and binding mechanism of oxygenated organic species from cyclohexane solution at the liquid/solid interface of optically flat alumina-supported palladium nanoparticle surfaces prepared by atomic layer deposition (ALD). The surface-specific nonlinear optical vibrational spectroscopy, sum-frequency generation (SFG), was used as a probe for adsorption and interfacial molecular structure. 1-Hexanoic acid is an overoxidation product and possible catalyst poison for the aerobic heterogeneous oxidation of 1-hexanol at the liquid/solid interface of Pd/Al?O? catalysts. Single component and competitive adsorption experiments show that 1-hexanoic acid adsorbs to both ALD-prepared alumina surfaces and alumina surfaces with palladium nanoparticles, that were also prepared by ALD, more strongly than does 1-hexanol. Furthermore, 1-hexanoic acid adsorbs with conformational order on ALD-prepared alumina surfaces, but on surfaces with palladium particles the adsorbates exhibit relative disorder at low surface coverage and become more ordered, on average, at higher surface coverage. Although significant differences in binding constant were not observed between surfaces with and without palladium nanoparticles, the palladium particles play an apparent role in controlling adsorbate structures. The disordered adsorption of 1-hexanoic acid most likely occurs on the alumina support, and probably results from modification of binding sites on the alumina, adjacent to the particles. In addition to providing insight on the possibility of catalyst poisoning by the overoxidation product and characterizing changes in its structure that result in only small adsorption energy changes, this work represents a step toward using surface science techniques that bridge the complexity gap between fundamental studies and realistic catalyst models.

  19. Rhodium Catalysts in the Oxidation of CO by O2 and NO: Shape, Composition, and Hot Electron Generation

    SciTech Connect (OSTI)

    Renzas, James R.

    2010-03-08

    It is well known that the activity, selectivity, and deactivation behavior of heterogeneous catalysts are strongly affected by a wide variety of parameters, including but not limited to nanoparticle size, shape, composition, support, pretreatment conditions, oxidation state, and electronic state. Enormous effort has been expended in an attempt to understand the role of these factors on catalytic behavior, but much still remains to be discovered. In this work, we have focused on deepening the present understanding of the role of nanoparticle shape, nanoparticle composition, and hot electrons on heterogeneous catalysis in the oxidation of carbon monoxide by molecular oxygen and nitric oxide. These reactions were chosen because they are important for environmental applications, such as in the catalytic converter, and because there is a wide range of experimental and theoretical insight from previous single crystal work as well as experimental data on nanoparticles obtained using new state-of-the-art techniques that aid greatly in the interpretation of results on complex nanoparticle systems. In particular, the studies presented in this work involve three types of samples: {approx} 6.5 nm Rh nanoparticles of different shapes, {approx} 15 nm Rh1-xPdx core-shell bimetallic polyhedra nanoparticles, and Rh ultra-thin film ({approx} 5 nm) catalytic nanodiodes. The colloidal nanoparticle samples were synthesized using a co-reduction of metal salts in alcohol and supported on silicon wafers using the Langmuir-Blodgett technique. This synthetic strategy enables tremendous control of nanoparticle size, shape, and composition. Nanoparticle shape was controlled through the use of different organic polymer capping layers. Bimetallic core-shell nanoparticles were synthesized by careful choice of metal salt precursors. Rh/TiO{sub x} and Rh/GaN catalytic nanodiodes were fabricated using a variety of thin film device fabrication techniques, including reactive DC magnetron sputtering, electron beam evaporation, and rapid thermal annealing. The combination of these techniques enabled control of catalytic nanodiode morphology, geometry, and electrical properties.

  20. An inorganic capping strategy for the seeded growth of versatile bimetallic nanostructures

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

    Pei, Yuchen; Maligal-Ganesh, Raghu V.; Xiao, Chaoxian; Goh, Tian -Wei; Brashler, Kyle; Gustafson, Jeffrey A.; Huang, Wenyu

    2015-09-11

    Metal nanostructures have attracted great attention in various fields due to their tunable properties through precisely tailored sizes, compositions and structures. Using mesoporous silica (mSiO2) as the inorganic capping agent and encapsulated Pt nanoparticles as the seeds, we developed a robust seeded growth method to prepare uniform bimetallic nanoparticles encapsulated in mesoporous silica shells (PtM@mSiO2, M = Pd, Rh, Ni and Cu). Unexpectedly, we found that the inorganic silica shell is able to accommodate an eight-fold volume increase in the metallic core by reducing its thickness. The bimetallic nanoparticles encapsulated in mesoporous silica shells showed enhanced catalytic properties and thermalmore »stabilities compared with those prepared with organic capping agents. As a result, this inorganic capping strategy could find a broad application in the synthesis of versatile bimetallic nanostructures with exceptional structural control and enhanced catalytic properties.« less

  1. FT-ICR reaction study of bimetallic clusters with alcohol and hydrocarbon

    E-Print Network [OSTI]

    Maruyama, Shigeo

    FT-ICR reaction study of bimetallic clusters with alcohol and hydrocarbon Satoshi Yoshinaga beam source [1]. In order to investigate the initial reaction of alcohol or hydrocarbon with a metal reaction of catalysts with carbon containing molecules, such as alcohol and hydrocarbon. Fig. 1 shows mass

  2. Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: Structure-activity relationship

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

    Guo, Yu; Senanayake, Sanjaya; Gu, Dong; Jin, Zhao; Du, Pei -Pei; Si, Rui; Xu, Wen -Qian; Huang, Yu -Ying; Tao, Jing; Song, Qi -Sheng; et al

    2015-01-12

    Uniform Au nanoparticles (~2 nm) with narrow size-distribution (standard deviation: 0.5–0.6 nm) supported on both hydroxylated (Fe_OH) and dehydrated iron oxide (Fe_O) have been prepared by either deposition-precipitation (DP) or colloidal-deposition (CD) methods. Different structural and textural characterizations were applied to the dried, calcined and used gold-iron oxide samples. The transmission electron microscopy (TEM) and high-resolution TEM (HRTEM) described the high homogeneity in the supported Au nanoparticles. The ex-situ and in-situ X-ray absorption fine structure (XAFS) characterization monitored the electronic and short-range local structure of active gold species. The synchrotron-based in-situ X-ray diffraction (XRD), together with the corresponding temperature-programmed reductionmore »by hydrogen (H?-TPR), indicated a structural evolution of the iron-oxide supports, correlating to their reducibility. An inverse order of catalytic activity between DP (Au/Fe_OH Au/Fe_O) was observed. Effective gold-support interaction results in a high activity for gold nanoparticles, locally generated by the sintering of dispersed Au atoms on the oxide support in the DP synthesis, while a hydroxylated surface favors the reactivity of externally introduced Au nanoparticles on Fe_OH support for the CD approach. This work reveals why differences in the synthetic protocol translate to differences in the catalytic performance of Au/FeOx catalysts with very similar structural characteristics in CO oxidation.« less

  3. Mass-selected Nanoparticles of PtxY as Model Catalysts for Oxygen...

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

    catalysts, due to a mildly weaker bond between the platinum surface atoms and the hydroxyl reaction intermediates. The EXAFS experiments were performed under grazing incidence...

  4. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    membrane fuel cell (PEMFC) and direct methanol fuel cell (operation and performance of PEMFC and DMFC depend largelyused electro-catalysts for PEMFC and DMFC are Pt-based noble

  5. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    materials are capable of serving as electro-catalysts in PEMFC andMaterials Science and Engineering University of California, Los Angeles, 2012 Professor Yu Huang, Chair Today, proton electrolyte membrane fuel cell (PEMFC) and

  6. Surface Structures of Cubo-octahedral Pt-Mo Catalyst Nanoparticles from Monte Carlo Simulations

    SciTech Connect (OSTI)

    Wang, Guofeng; Van Hove, M.A.; Ross, P.N.; Baskes, M.I.

    2005-03-31

    The surface structures of cubo-octahedral Pt-Mo nanoparticles have been investigated using the Monte Carlo method and modified embedded atom method potentials that we developed for Pt-Mo alloys. The cubo-octahedral Pt-Mo nanoparticles are constructed with disordered fcc configurations, with sizes from 2.5 to 5.0 nm, and with Pt concentrations from 60 to 90 at. percent. The equilibrium Pt-Mo nanoparticle configurations were generated through Monte Carlo simulations allowing both atomic displacements and element exchanges at 600 K. We predict that the Pt atoms weakly segregate to the surfaces of such nanoparticles. The Pt concentrations in the surface are calculated to be 5 to 14 at. percent higher than the Pt concentrations of the nanoparticles. Moreover, the Pt atoms preferentially segregate to the facet sites of the surface, while the Pt and Mo atoms tend to alternate along the edges and vertices of these nanoparticles. We found that decreasing the size or increasing the Pt concentration leads to higher Pt concentrations but fewer Pt-Mo pairs in the Pt-Mo nanoparticle surfaces.

  7. Controlled Anisotropic Growth of Co-Fe-P from Co-Fe-O Nanoparticles

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

    Mendoza-Garcia, Adriana; Zhu, Huiyuan; Yu, Yongsheng; Li, Qing; Zhou, Lin; Su, Dong; Kramer, Matthew J.; Sun, Shouheng

    2015-06-26

    Presented here is a facile approach to bimetallic phosphides, Co-Fe-P, via high-temperature (300°C) reaction between Co-Fe-O nanoparticles and trioctylphosphine. The growth of Co-Fe-P from the Co-Fe-O is anisotropic. As a result, Co-Fe-P nanorods (from the polyhedral Co-Fe-O nanoparticles) and sea-urchin-like Co-Fe-P (from the cubic Co-Fe-O nanoparticles) are synthesized with both nanorod and the sea-urchin-arm dimensions controlled by Co/Fe ratios. The Co-Fe-P structure, especially the sea-urchin-like (Co0.54Fe0.46)2P, shows enhanced catalysis for oxygen evolution reaction in KOH with its catalytic efficiency surpassing Ir catalyst. Our synthesis is simple and may be readily extended to the preparation of other multimetallic phosphides for importantmore »catalysis and energy storage applications.« less

  8. ZnO nanoparticle catalysts for use in biodiesel production and method of making

    DOE Patents [OSTI]

    Yan, Shuli; Salley, Steven O; Ng, K. Y. Simon

    2014-11-25

    A method of forming a biodiesel product and a heterogeneous catalyst system used to form said product that has a high tolerance for the presence of water and free fatty acids (FFA) in the oil feedstock is disclosed. This catalyst system may simultaneously catalyze both the esterification of FAA and the transesterification of triglycerides present in the oil feedstock. The catalyst system is comprised of a mixture of zinc oxide and a second metal oxide. The zinc oxide includes a mixture of amorphous zinc oxide and zinc oxide nanocrystals, the zinc nanocrystals having a mean grain size between about 20 and 80 nanometers with at least one of the nanocrystals including a mesopore having a diameter of about 5 to 15 nanometers. Preferably, the second metal oxide is a lanthanum oxide, the lanthanum oxide being selected as one from the group of La.sub.2CO.sub.5, LaOOH, and combinations or mixtures thereof.

  9. Monodisperse metal nanoparticle catalysts on silica mesoporous supports: synthesis, characterizations, and catalytic reactions

    E-Print Network [OSTI]

    Somorjai, G.A.

    2010-01-01

    by Rh/SBA-15 The catalytic oxidation of CO to CO 2 has beencatalytic activity in high temperature CO oxidation. Thecatalytic activity as high as bare Pt nanoparticles in CO oxidation,

  10. A pathway for the growth of core-shell Pt-Pd nanoparticles

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

    Narula, Chaitanya Kumar; Yang, Xiaofan; Li, Chen; Pennycook, Stephen J; Lupini, Andrew R

    2015-10-12

    In this study, the aging of both Pt-Pd nanoparticles and core-shell Pt-Pd nanoparticles has been reported to result in alloying of Pt with Pd. In comparison to monometallic Pt catalysts, the growth of Pd-Pt bimetallics is slower; however, the mechanism of growth of particles and the mechanism by which Pd improves the hydrothermal durability of bimetallic Pd-Pt particles remains uncertain. In our work on hydrothermal aging of core-shell Pt-Pd nanoparticles, synthesized by solution methods, with varying Pd:Pt ratio of 1:4, 1:1, and 4:1, we compare the growth of core-shell Pt-Pd nanoparticles and find that particles grow by migrating and joiningmore »together. The unique feature of the observed growth is that Pd shells from both particles open up and join, allowing the cores to merge. At high temperatures, alloying occurs in good agreement with reports by other workers.« less

  11. Controlling bimetallic nanostructures by the microemulsion method with subnanometer resolution using a prediction model

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

    Buceta, David; Tojo, Concha; Vukmirovic, Miomir B.; Deepak, F. Leonard; Lopez-Quintela, M. Arturo

    2015-06-02

    In this study, we present a theoretical model to predict the atomic structure of Au/Pt nanoparticles synthesized in microemulsions. Excellent concordance with the experimental results shows that the structure of the nanoparticles can be controlled at sub-nanometer resolution simply by changing the reactants concentration. The results of this study not only offer a better understanding of the complex mechanisms governing reactions in microemulsions, but open up a simple new way to synthesize bimetallic nanoparticles with ad-hoc controlled nanostructures.

  12. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED IN STABLE NANOPOROUS HOSTS

    SciTech Connect (OSTI)

    Conrad Ingram

    2003-09-03

    The focus of this project is to improve the catalytic performance of zeolite Y for petroleum hydrocracking by synthesizing nanoparticles of the zeolite ({approx}20-25 nm) inside nanoporous silicate or aluminosilicate hosts. The encapsulated zeolite nanoparticles are expected to possess reduced diffusional path lengths, hence hydrocarbon substrates will diffuse in, are converted and the products quickly diffused out. This is expected to prevent over-reaction and the blocking of the zeolite pores and active sites will be minimized. In this phase of the project, procedures for the synthesis of ordered nanoporous silica, such as SBA-15, using block copolymers and nonionic surfactant were successful reproduced. Expansion of the pores sizes of the nanoporous silica using trimethylbenzene is suggested based on shift in the major X-Ray Diffraction peak in the products to lower 2 angles compared with the parent SBA-15 material. The synthesis of ordered nanoporous materials with aluminum incorporated in the predominantly silicate framework was attempted but is not yet successful, and the procedures needs will be repeated and modified as necessary. Nanoparticles of zeolite Y of particle sizes in the range 40 nm to 120 nm were synthesized in the presence of TMAOH as the particle size controlling additive.

  13. IMPROVED CATALYSTS FOR HEAVY OIL UPGRADING BASED ON ZEOLITE Y NANOPARTICLES ENCAPSULATED IN STABLE NANOPOROUS HOSTS

    SciTech Connect (OSTI)

    Conrad Ingram; Mark Mitchell

    2004-06-30

    The focus of this project is to improve the catalytic performance of zeolite Y for heavy petroleum hydrocracking by synthesizing nanoparticles of the zeolite ({approx}20-30 nm) inside nanoporous silicate or aluminosilicate hosts of similar pore diameters. The encapsulated zeolite nanoparticles are expected to possess pores of reduced diffusional path lengths, hence hydrocarbon substrates will diffuse in, are converted and the products quickly diffused out. This is expected to prevent over-reaction, hence minimizing pore blockage and active sites deactivation. In this phase of the project, research activities were focused on refining procedures to: (a) improve the synthesis of ordered, high surface area nanoporous silica, such as SBA-15, with expanded pore size using trimethylbenzene as additive to the parent SBA-15 synthesis mixture; and (b) reduce the particle size of zeolite Y such that they can be effectively incorporated into the nanoporous silicas. The synthesis of high surface ordered nanoporous silica containing enlarged pores of diameter of 25 nm (larger than the standard size of 8.4 nm) using trimethylbenzene as a pore size expander was accomplished. The synthesis of zeolite Y nanoparticles with median pore size of approximately 50 nm (smaller than the 80 nm typically obtained with TMAOH) using combined TMABr/TMAOH as organic additives was also accomplished.

  14. Preparation of silver nanoparticles/graphene nanosheets as a catalyst for electrochemical oxidation of methanol

    SciTech Connect (OSTI)

    Han, Kun; Miao, Peng; Tang, Yuguo, E-mail: tangyg@sibet.ac.cn [Suzhou Institute of Biomedical Engineering and Technology, Chinese Academy of Sciences, Suzhou 215163 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Tong, Hui; Zhu, Xiaoli [Laboratory of Biosensing Technology, School of Life Sciences, Shanghai University, Shanghai 200444 (China); Liu, Tao; Cheng, Wenbo [Suzhou Institute of Biomedical Engineering and Technology, Chinese Academy of Sciences, Suzhou 215163 (China)

    2014-02-03

    In this report, silver nanoparticles (AgNPs) decorated graphene nanosheets have been prepared based on the reduction of Ag ions by hydroquinone, and their catalytic performance towards the electrochemical oxidation of methanol is investigated. The synthesis of the nano-composite is confirmed by transmission electron microscope measurements and UV-vis absorption spectra. Excellent electrocatalytic performance of the material is demonstrated by cyclic voltammograms. This material also contributes to the low peak potential of methanol oxidation compared with most of the other materials.

  15. Investigation into the molar feeding ratio and temperature dependence on the replacement reaction between platinum ions and silver nanoparticles

    E-Print Network [OSTI]

    Stuk, Archimedes

    2010-01-01

    The deliberate structuring of bimetallic nanoparticles has useful applications in both fuel cell applications and biomedical research. This thesis studies the replacement reaction between platinum ions and silver nanoparticles, ...

  16. Novel Pt/Mg(In)(Al)O catalysts for ethane and propane dehydrogenation

    SciTech Connect (OSTI)

    Sun, Pingping; Siddiqi, Georges; Vining, William C.; Chi, Miaofang; Bell, Alexis T.

    2011-10-28

    Catalysts for the dehydrogenation of light alkanes were prepared by dispersing Pt on the surface of a calcined hydrotalcite-like support containing indium, Mg(In)(Al)O. Upon reduction in H{sub 2} at temperatures above 673 K, bimetallic particles of PtIn are observed by TEM, which have an average diameter of 1 nm. Analysis of Pt LIII-edge extended X-ray absorption fine structure (EXAFS) data shows that the In content of the bimetallic particles increases with increasing bulk In/Pt ratio and reduction temperature. Pt LIII-edge X-ray absorption near edge structure (XANES) indicates that an increasing donation of electronic charge from In to Pt occurs with increasing In content in the PtIn particles. The activity and selectivity of the Pt/Mg(In)(Al)O catalysts for ethane and propane dehydrogenation reactions are strongly dependent on the bulk In/Pt ratio. For both reactants, maximum activity was achieved for a bulk In/Pt ratio of 0.48, and at this In/Pt ratio, the selectivity to alkene was nearly 100%. Coke deposition was observed after catalyst use for either ethane or propane dehydrogenation, and it was observed that the alloying of Pt with In greatly reduced the amount of coke deposited. Characterization of the deposit by Raman spectroscopy indicates that the coke is present as highly disordered graphite particles <30 nm in diameter. While the amount of coke deposited during ethane and propane dehydrogenation are comparable, the effects on activity are dependent on reactant composition. Coke deposition had no effect on ethane dehydrogenation activity, but caused a loss in propane dehydrogenation activity. This difference is attributed to the greater ease with which coke produced on the surface of PtIn nanoparticles migrates to the support during ethane dehydrogenation versus propane dehydrogenation.

  17. Stability and Aggregation of Metal Oxide Nanoparticles in Natural

    E-Print Network [OSTI]

    Cardinale, Bradley J.

    .g., sunscreens, paints, coatings, catalysts). A simplified con- ceptual model of a typical nanoparticle life

  18. ORIGINAL ARTICLES Silica-Supported AuNi Catalysts for the Dehydrogenation

    E-Print Network [OSTI]

    Goodman, Wayne

    Introduction Gold­nickel bimetallic catalysts have shown enhanced catalytic properties for a number of reactions [1­9], such as steaming reforming of hydrocarbons [1, 2], the water­gas shift reaction [3 reforming of n-butane, whereas a monometallic Ni catalyst deactivated rapidly [1]. For the water­gas shift

  19. Surface spectroscopic studies of mono- and bimetallic model catalysts 

    E-Print Network [OSTI]

    Yi, Cheol-Woo

    2007-04-25

    by physical vapor deposition (PVD) onto well-characterized metal substrates. Subsequent characterization was performed using an arsenal of modern surface science tools: low energy ion scattering spectroscopy (LEISS), infrared absorption spectroscopy (IRAS...

  20. Catalytic studies of supported Pd-Au catalysts 

    E-Print Network [OSTI]

    Boopalachandran, Praveenkumar

    2006-08-16

    -Au Bimetallic Supported Catalysts Palladium (Pd) is a well known catalyst for many reactions which are of industrial and environmental importance [7]. A major drawback of using Pd-only catalysts is the formation of carbides, i.e. PdCx, as shown in the Fig. 1... reveal that the addition of gold to palladium catalysts has pronounced catalytic effect [3, 6]. It is plausible that the electronic and geometric properties are tuned by the addition of Au with highly optimized sites [3, 6, 11]. Also, model catalytic...

  1. Bimetallic Cathode Materials for Lithium Based Batteries

    E-Print Network [OSTI]

    Bimetallic Cathode Materials for Lithium Based Batteries Frontiers in Materials Science Seminar / Chemistryg g g g g y University at Buffalo ­ The State University of New York (SUNY) Abstract Batteries/SVO batteries. A case study highlighting the rich chemistry and electrochemistry of the Li/SVO system providing

  2. Oxidation catalyst

    DOE Patents [OSTI]

    Ceyer, Sylvia T. (Cambridge, MA); Lahr, David L. (Cambridge, MA)

    2010-11-09

    The present invention generally relates to catalyst systems and methods for oxidation of carbon monoxide. The invention involves catalyst compositions which may be advantageously altered by, for example, modification of the catalyst surface to enhance catalyst performance. Catalyst systems of the present invention may be capable of performing the oxidation of carbon monoxide at relatively lower temperatures (e.g., 200 K and below) and at relatively higher reaction rates than known catalysts. Additionally, catalyst systems disclosed herein may be substantially lower in cost than current commercial catalysts. Such catalyst systems may be useful in, for example, catalytic converters, fuel cells, sensors, and the like.

  3. Hydrocracking catalysts

    SciTech Connect (OSTI)

    Parrott, S.P.; Myers, J.W.

    1984-05-08

    The activity and deactivation rate of hydrocracking catalysts are improved by making them via a particular production sequence.

  4. Enhanced electrocatalytic activity and stability of Pd3V/C nanoparticles with a trace amount of Pt decoration for the oxygen reduction reaction

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

    Liu, Sufen; Han, Lili; Zhu, Jing; Xiao, Weiping; Wang, Jie; Liu, Hongfang; Xin, Huolin; Wang, Deli

    2015-09-14

    In this study, carbon supported Pd3V bimetallic alloy nanoparticles (Pd3V/C) have been successfully synthesized via a simple impregnation–reduction method, followed by high temperature treatment under a H2 atmosphere. Electrochemical tests reveal that the half-wave potential of Pd3V/C-500 shifts positively 40 mV compared with Pd/C. However, the catalytic activity of Pd3V/C-500 suffers from serious degradation after 1k cycles. By a spontaneous displacement reaction or co-reduction method, a trace amount of Pt was decorated on the surface or inside of the Pd3V/C nanoparticles. The catalytic activity and stability of the Pd3V@Pt/C and Pt-Pd3V/C catalysts for the oxygen reduction reaction (ORR) are enhancedmore »significantly, and are comparable to commercial Pt/C. In addition, the Pt mass activity of Pd3V@Pt/C and Pt-Pd3V/C improves by factors of 10.9 and 6.5 at 0.80 V relative to Pt/C. Moreover, Pt-decorated Pd3V/C nanoparticles show almost no obvious morphology change after durability tests, because the Pt-rich shell plays an important role in preventing degradation.« less

  5. Selective Hydrogenation of Acetylene in the Presence of Ethylene on K+ -beta-Zeolite Supported Pd and PdAg Catalysts

    SciTech Connect (OSTI)

    Huang,W.; Pyrz, W.; Lobo, R.; Chen, J.

    2007-01-01

    The selective hydrogenation of acetylene in the presence of ethylene has been studied on K+ exchanged {beta}-zeolite supported Pd and PdAg catalysts. Results from batch reactor studies with Fourier transform infrared spectroscopy (FTIR) have shown that the K+-{beta}-zeolite support is more selective than the Al2O3 or Na+-{beta}-zeolite supports toward the hydrogenation of acetylene. The rate and equilibrium constants for Pd/K+-{beta}-zeolite and PdAg/K+-{beta}-zeolite were determined using a Langmuir-Hinshelwood model. The selectivity of the PdAg bimetallic catalyst is twice of that of the Pd catalyst. Results from flow reactor studies show that the PdAg/K+-{beta}-zeolite catalyst has higher selectivity but lower activity toward acetylene hydrogenation than the Pd/K+-{beta}-zeolite catalyst. The selectivity to the undesirable ethane by-product is inhibited on the bimetallic catalyst. Extended X-ray absorption fine structure (EXAFS) studies and transmission electron microscope (TEM) analysis confirm the formation of Pd-Ag bimetallic bonds in the PdAg/K+-{beta}-zeolite catalyst.

  6. Characterization and Reaction Studies of Silica Supported Platinum and Rhodium Model Catalysts 

    E-Print Network [OSTI]

    Lundwall, Matthew James

    2012-02-14

    by dispersing nanoparticles leading to inhibition of catalytic pathways. Moreover, the relationships between high index single crystals, oxide supported nanoparticles, and high surface area technical catalysts are established. Overall, the results demonstrate...

  7. Hydrocracking catalyst

    SciTech Connect (OSTI)

    Welsh, W.A.

    1984-06-26

    A stable, highly active hydrocracking catalyst which contains a rare earth/noble metal exchanged ultrastable type Y zeolite dispersed in an inorganic oxide matrix. The catalyst is hydrated to a moisture level of from about 5 to 30 percent by weight H/sub 2/O prior to activation and use in a hydrocracking process.

  8. Oxyhydrochlorination catalyst

    DOE Patents [OSTI]

    Taylor, Charles E. (Pittsburgh, PA); Noceti, Richard P. (Pittsburgh, PA)

    1992-01-01

    An improved catalyst and method for the oxyhydrochlorination of methane is disclosed. The catalyst includes a pyrogenic porous support on which is layered as active material, cobalt chloride in major proportion, and minor proportions of an alkali metal chloride and of a rare earth chloride. On contact of the catalyst with a gas flow of methane, HCl and oxygen, more than 60% of the methane is converted and of that converted more than 40% occurs as monochloromethane. Advantageously, the monochloromethane can be used to produce gasoline boiling range hydrocarbons with the recycle of HCl for further reaction. This catalyst is also of value for the production of formic acid as are analogous catalysts with lead, silver or nickel chlorides substituted for the cobalt chloride.

  9. Chemical and Physical Properties of Nanomaterials for Model Catalytic Systems and Smart Polymer Membranes 

    E-Print Network [OSTI]

    Skiles, Stephanie Lyn

    2014-10-24

    . These systems can be developed and tested using model catalyst systems. Herein, two model systems were investigated: a supported cobalt nanoparticle catalyst and a bimetallic palladium-copper system. In the cobalt system, the smallest particles are oxidized...

  10. Perovskite Sr0.95Ce0.05CoO3d loaded with copper nanoparticles as a bifunctional catalyst for lithium-air batteries

    E-Print Network [OSTI]

    for lithium-air batteries Wei Yang,ab Jason Salim,c Shuai Li,ab Chunwen Sun,*ab Liquan Chen,ab John B could be used in a metal/air battery or a PEM fuel cell as an efficient and stable bifunctional catalyst electrolyte. More challenging is the requirement for the Li/air rechargeable battery, viz. an inexpensive

  11. Photo-oxidation catalysts

    DOE Patents [OSTI]

    Pitts, J. Roland (Lakewood, CO); Liu, Ping (Irvine, CA); Smith, R. Davis (Golden, CO)

    2009-07-14

    Photo-oxidation catalysts and methods for cleaning a metal-based catalyst are disclosed. An exemplary catalyst system implementing a photo-oxidation catalyst may comprise a metal-based catalyst, and a photo-oxidation catalyst for cleaning the metal-based catalyst in the presence of light. The exposure to light enables the photo-oxidation catalyst to substantially oxidize absorbed contaminants and reduce accumulation of the contaminants on the metal-based catalyst. Applications are also disclosed.

  12. Correlation of Theory and Function in Well-Defined Bimetallic Electrocatalysts - Final Report

    SciTech Connect (OSTI)

    Crooks, Richard M.

    2014-06-05

    The objective of this research proposal was to correlate the structure of nanoparticles that are comprised of ~100-200 atoms to their electrocatalytic function. This objective was based on the growing body of evidence suggesting that catalytic properties can be tailored through controlled synthesis of nanoparticles. What has been missing from many of these studies, and what we are contributing, is a model catalyst that is sufficiently small, structurally well-defined, and well-characterized that its function can be directly predicted by theory. Specifically, our work seeks to develop a fundamental and detailed understanding of the relationship between the structure of nanoscopic oxygen-reduction catalysts and their function. We assembled a team with expertise in theory, synthesis, and advanced characterization methods to address the primary objective of this project. We anticipated the outcomes of the study to be: (1) a better theoretical understanding of how nanoparticle structure affects catalytic properties; (2) the development of advanced, in-situ and ex-situ, atomic-scale characterization methods that are appropriate for particles containing about 100 atoms; and (3) improved synthetic methods that produce unique nanoparticle structures that can be used to test theoretical predictions. During the project period, we have made excellent progress on all three fronts.

  13. In-situ Studies of the Reactions of Bifunctional and Heterocyclic Molecules over Noble Metal Single Crystal and Nanoparticle Catalysts Studied with Kinetics and Sum-Frequency Generation Vibrational Spectroscopy

    SciTech Connect (OSTI)

    Kliewer, Christopher J.

    2009-06-30

    Sum frequency generation surface vibrational spectroscopy (SFG-VS) in combination with gas chromatography (GC) was used in-situ to monitor surface bound reaction intermediates and reaction selectivities for the hydrogenation reactions of pyrrole, furan, pyridine, acrolein, crotonaldehyde, and prenal over Pt(111), Pt(100), Rh(111), and platinum nanoparticles under Torr reactant pressures and temperatures of 300K to 450K. The focus of this work is the correlation between the SFG-VS observed surface bound reaction intermediates and adsorption modes with the reaction selectivity, and how this is affected by catalyst structure and temperature. Pyrrole hydrogenation was investigated over Pt(111) and Rh(111) single crystals at Torr pressures. It was found that pyrrole adsorbs to Pt(111) perpendicularly by cleaving the N-H bond and binding through the nitrogen. However, over Rh(111) pyrrole adsorbs in a tilted geometry binding through the {pi}-aromatic orbitals. A surface-bound pyrroline reaction intermediate was detected over both surfaces with SFG-VS. It was found that the ring-cracking product butylamine is a reaction poison over both surfaces studied. Furan hydrogenation was studied over Pt(111), Pt(100), 10 nm cubic platinum nanoparticles and 1 nm platinum nanoparticles. The product distribution was observed to be highly structure sensitive and the acquired SFG-VS spectra reflected this sensitivity. Pt(100) exhibited more ring-cracking to form butanol than Pt(111), while the nanoparticles yielded higher selectivities for the partially saturated ring dihydrofuran. Pyridine hydrogenation was investigated over Pt(111) and Pt(100). The {alpha}-pyridyl surface adsorption mode was observed with SFG-VS over both surfaces. 1,4-dihydropyridine was seen as a surface intermediate over Pt(100) but not Pt(111). Upon heating the surfaces to 350K, the adsorbed pyridine changes to a flat-lying adsorption mode. No evidence was found for the pyridinium cation. The hydrogenation of the {alpha},{beta}-unsaturated aldehydes acrolein, crotonaldehyde, and prenal were investigated over Pt(111) and Pt(100). The selectivity for the hydrogenation of the C=C bond was found to depend on the number of methyl groups added to the bond. The adsorption modes of the three aldehydes were determined. The hydrogenation of crotonaldehyde was found to be nearly structure insensitive as the TOF and selectivity were very close to the same over Pt(111) and Pt(100). SFG-VS indicated identical surface intermediates over the two crystal faces during crotonaldehyde hydrogenation.

  14. Non-Platinum Bimetallic Cathode Electrocatalysts | Department of Energy

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Home Page on Google Bookmark EERE: Alternative Fuels Data Center Home Page on Delicious RankADVANCED MANUFACTURINGEnergy Bills and Reduce CarbonEnergy Fuel Effects onPlatinum Bimetallic Cathode

  15. High-throughput metal nanoparticle catalysis by pulsed laser ablation Selim Senkan a,*, Michael Kahn a

    E-Print Network [OSTI]

    Senkan, Selim M.

    -PLA were also screened for their catalytic activities and selectivities for the partial oxidation for catalytic applications. Catalytic materials containing Rh, bimetallic Rh/Pt and trimetallic Rh of propylene. In less than a day, over 40 different catalytic materials of nanoparticles supported on g-Al2O3

  16. Computational Chemistry-Based Identification of Ultra-Low Temperature Water-Gas-Shift Catalysts

    SciTech Connect (OSTI)

    Manos Mavrikakis

    2008-08-31

    The current work seeks to identify novel, catalytically-active, stable, poison-resistant LWGS catalysts that retain the superior activity typical of conventional Cu catalysts but can be operated at similar or lower temperatures. A database for the Binding Energies (BEs) of the LWGS relevant species, namely CO, O and OH on the most-stable, close-packed facets of a set of 17 catalytically relevant transition metals was established. This BE data and a database of previously established segregation energies was utilized to predict the stability of bimetallic NSAs that could be synthesized by combinations of the 17 parent transition metals. NSAs that were potentially stable both in vacuo and under the influence of strong-binding WGS intermediates were then selected for adsorption studies. A set of 40 NSAs were identified that satisfied all three screener criteria and the binding energies of CO, O and OH were calculated on a set of 66, 43 and 79 NSA candidates respectively. Several NSAs were found that bound intermediates weaker than the monometallic catalysts and were thus potentially poison-resistant. Finally, kinetic studies were performed and resulted in the discovery of a specific NSA-based bimetallic catalyst Cu/Pt that is potentially a promising LWGS catalyst. This stable Cu/Pt subsurface alloy is expected to provide facile H{sub 2}O activation and remain relatively resistant from the poisoning by CO, S and formate intermediates.

  17. 6PA40 6PA41 Sputtering ofW-Pd Bimetallic System under Nitrogen

    E-Print Network [OSTI]

    Harilal, S. S.

    (bimetallic) diffusion sys- tems, which comprise of rather thick palladium substrate and erosion rcsistant coating, e.g., tungsten on the plasma facing surface, for ac tive control of hydrogen recycling process in thermonuclear fusion de- vices. In order to choose theoptimal performances of tungsten-palladium bimetallic

  18. Catalyst suppliers consolidate further, offer more catalysts

    SciTech Connect (OSTI)

    Rhodes, A.K.

    1995-10-02

    The list of suppliers of catalysts to the petroleum refining industry has decreased by five since Oil and Gas Journal`s survey of refining catalysts and catalytic additives was last published. Despite the consolidation, the list of catalyst designations has grown to about 950 in this latest survey, compared to 820 listed in 1993. The table divides the catalysts by use and gives data on their primary differentiating characteristics, feedstock, products, form, bulk density,catalyst support, active agents, availability, and manufactures.

  19. Method of making chalcogen catalysts for polymer electrolyte fuel cells

    DOE Patents [OSTI]

    Choi, Jong-Ho (Los Alamos, NM); Zelenay, Piotr (Los Alamos, NM); Wieckowski, Andrzej (Champaign, IL); Cao, Dianxue (Harabin, CN)

    2010-12-14

    A method of making an electrode catalyst material using aqueous solutions. The electrode catalyst material includes a support comprising at least one transition metal and at least one chalcogen disposed on a surface of the transition metal. The method includes reducing a metal powder, mixing the metal powder with an aqueous solution containing at least one inorganic compound of the chalcogen to form a mixture, and providing a reducing agent to the mixture to form nanoparticles of the electrode catalyst. The electrode catalyst may be used in a membrane electrode assembly for a fuel cell.

  20. Thermally stable nanoparticles on supports

    DOE Patents [OSTI]

    Roldan Cuenya, Beatriz; Naitabdi, Ahmed R.; Behafarid, Farzad

    2012-11-13

    An inverse micelle-based method for forming nanoparticles on supports includes dissolving a polymeric material in a solvent to provide a micelle solution. A nanoparticle source is dissolved in the micelle solution. A plurality of micelles having a nanoparticle in their core and an outer polymeric coating layer are formed in the micelle solution. The micelles are applied to a support. The polymeric coating layer is then removed from the micelles to expose the nanoparticles. A supported catalyst includes a nanocrystalline powder, thin film, or single crystal support. Metal nanoparticles having a median size from 0.5 nm to 25 nm, a size distribution having a standard deviation .ltoreq.0.1 of their median size are on or embedded in the support. The plurality of metal nanoparticles are dispersed and in a periodic arrangement. The metal nanoparticles maintain their periodic arrangement and size distribution following heat treatments of at least 1,000.degree. C.

  1. Rare earth oxide fluoride nanoparticles and hydrothermal method for forming nanoparticles

    DOE Patents [OSTI]

    Fulton, John L. (Richland, WA) [Richland, WA; Hoffmann, Markus M. (Richland, WA) [Richland, WA

    2001-11-13

    A hydrothermal method for forming nanoparticles of a rare earth element, oxygen and fluorine has been discovered. Nanoparticles comprising a rare earth element, oxygen and fluorine are also described. These nanoparticles can exhibit excellent refractory properties as well as remarkable stability in hydrothermal conditions. The nanoparticles can exhibit excellent properties for numerous applications including fiber reinforcement of ceramic composites, catalyst supports, and corrosion resistant coatings for high-temperature aqueous solutions.

  2. Rare Earth Oxide Fluoride Nanoparticles And Hydrothermal Method For Forming Nanoparticles

    DOE Patents [OSTI]

    Fulton, John L. (Richland, WA); Hoffmann, Markus M. (Richland, WA)

    2003-12-23

    A hydrothermal method for forming nanoparticles of a rare earth element, oxygen and fluorine has been discovered. Nanoparticles comprising a rare earth element, oxygen and fluorine are also described. These nanoparticles can exhibit excellent refractory properties as well as remarkable stability in hydrothermal conditions. The nanoparticles can exhibit excellent properties for numerous applications including fiber reinforcement of ceramic composites, catalyst supports, and corrosion resistant coatings for high-temperature aqueous solutions.

  3. EFFECT OF PRETREATMENT ON PT-CO/C CATHODE CATALYSTS FOR THE OXYGEN-REDUCTION REACTION

    SciTech Connect (OSTI)

    Fox, E.

    2009-05-13

    In order to reduce the precious metal loading without sacrificing activity and stability, a new method for the preparation of bimetallic catalysts is proposed. Currently, Pt-alloy particles, with 2 to 3 nm in diameter, are loaded on high surface area carbon supports. Of the Pt loaded, only the surface atoms interact with the reactants. In order to increase the Pt utilization per metal particle the new process for catalyst preparation will incorporate a non-noble transition metal core coated with a skin layer of Pt deposited on high surface area carbon. The effect of reducing agent strength during synthesis was also explored. It was determined that the Co addition has a higher impact on catalyst when used with NaBH4 as reducing agent as compared to NaCOOH.

  4. Catalytic Nonoxidation Dehydrogenation of Ethane Over Fe-Ni Catalysts Supported on Mg (Al)O to Produce Hydrogen and Easily Purified Carbon Nanotubes

    SciTech Connect (OSTI)

    Shen,W.; Wang, Y.; Shi, X.; Shah, N.; Huggins, F.; Bollineni, S.; Seehra, M.; Huffman, G.

    2007-01-01

    Nonoxidative decomposition of ethane was conducted over monometallic Ni and bimetallic Fe-Ni catalysts on basic Mg(Al)O support to produce H2 free of CO and CO2 and easily purified carbon nanotubes, a potentially valuable byproduct. The Mg(Al)O support was prepared by calcination of synthetic MgAl-hydrotalcite with a Mg to Al ratio of 5. The catalysts were prepared by incipient wetness with total metal loadings of 5 wt %. The dehydrogenation of undiluted ethane was conducted at temperatures of 500, 650, and 700 C. At 500 C, the Ni/Mg(Al)O catalyst was highly active and very stable with 100% conversion of ethane to 20 vol % H2 and 80 vol % CH4. However, the bimetallic Fe-Ni/Mg(Al)O exhibited its best performance at 650 C, yielding 65 vol % H2, 10 vol % CH4, and 25 vol % unreacted ethane. The product carbon was in the form of carbon nanotubes (CNT) at all three reaction temperatures, but the morphology of the CNT depended on both the catalyst composition and reaction temperature. The CNTs were formed by a tip-growth mechanism over the Mg(Al)O supported catalysts and were easily purified by a one-step dilute nitric acid treatment. Mossbauer spectroscopy, X-ray absorption fine structure spectroscopy, N2 adsorption-desorption isotherms, TEM, STEM, TGA, and XRD were used to characterize the catalysts and the CNT, revealing the catalytic mechanisms.

  5. Electrochemical catalyst recovery method

    DOE Patents [OSTI]

    Silva, L.J.; Bray, L.A.

    1995-05-30

    A method of recovering catalyst material from latent catalyst material solids includes: (a) combining latent catalyst material solids with a liquid acid anolyte solution and a redox material which is soluble in the acid anolyte solution to form a mixture; (b) electrochemically oxidizing the redox material within the mixture into a dissolved oxidant, the oxidant having a potential for oxidation which is effectively higher than that of the latent catalyst material; (c) reacting the oxidant with the latent catalyst material to oxidize the latent catalyst material into at least one oxidized catalyst species which is soluble within the mixture and to reduce the oxidant back into dissolved redox material; and (d) recovering catalyst material from the oxidized catalyst species of the mixture. The invention is expected to be particularly useful in recovering spent catalyst material from petroleum hydroprocessing reaction waste products having adhered sulfides, carbon, hydrocarbons, and undesired metals, and as well as in other industrial applications. 3 figs.

  6. DOI: 10.1002/cvde.200506446 Aerosol Catalyst Particles for Substrate CVD Synthesis

    E-Print Network [OSTI]

    on thin SiO2 films using iron and car- bon monoxide as the catalyst material and the carbon source of surfactants that can cause particle contamination.[14­16] Another common way of producing nanoparticles

  7. Polyhedral Shapes of CeO2 Nanoparticles Zhong Lin Wang*, and Xiangdong Feng

    E-Print Network [OSTI]

    Wang, Zhong L.

    Ceria nanoparticles are a widely used nanomaterial for applications in catalysts, fuel cell are one of the most important nanoma- terials for a wide range of applications in catalysts,1,2 fuel cell are likely to affect their performance in technological applications. 1. Introduction Ceria nanoparticles

  8. Catalyst Dynamics during Carbon Nanotube and Si Nanowire CVD S. Hofmann,*

    E-Print Network [OSTI]

    Dunin-Borkowski, Rafal E.

    with the substrate. This allows us to grow gas-flow aligned, mm-long lateral nanotube arrays. Microsc Microanal 14]. In both cases, Si nuclei form by phase separation before expanding and pushing the catalyst onto the tip. Appl. Phys. 94, 6005 (2003) Fig. 1 ETEM images of Ni catalyst nanoparticles on SiOx membrane at 615°C

  9. Single-walled carbon nanotube growth from ion implanted Fe catalyst Yongho Choi

    E-Print Network [OSTI]

    Ural, Ant

    the growth of carbon nanotubes. Typically, transition metal nanoparticles, such as nickel Ni , iron FeSingle-walled carbon nanotube growth from ion implanted Fe catalyst Yongho Choi Department-walled carbon nanotubes can be grown by chemical vapor deposition from ion implanted iron catalyst

  10. Size and alloying induced shift in core and valence bands of Pd-Ag and Pd-Cu nanoparticles

    SciTech Connect (OSTI)

    Sengar, Saurabh K.; Mehta, B. R.; Govind

    2014-03-28

    In this report, X-ray photoelectron spectroscopy studies have been carried out on Pd, Ag, Cu, Pd-Ag, and Pd-Cu nanoparticles having identical sizes corresponding to mobility equivalent diameters of 60, 40, and 20?nm. The nanoparticles were prepared by the gas phase synthesis method. The effect of size on valence and core levels in metal and alloy nanoparticles has been studied by comparing the values to those with the 60?nm nanoparticles. The effect of alloying has been investigated by comparing the valence and core level binding energies of Pd-Cu and Pd-Ag alloy nanoparticles with the corresponding values for Pd, Ag, and Cu nanoparticles of identical sizes. These effects have been explained in terms of size induced lattice contractions, alloying induced charge transfer, and hybridization effects. The observation of alloying and size induced binding energy shifts in bimetallic nanoparticles is important from the point of view of hydrogen reactivity.

  11. Hydrocarbon in Catalyst in

    E-Print Network [OSTI]

    Ladkin, Peter B.

    #12;Hydrocarbon in Steam in Catalyst in Vent 1 Vent 2 Product out Tank Pressure controller Computer;#12;Vent 1 Vent 2 Product outHydrocarbon in Steam in Catalyst in light Warning Computer controller Tank

  12. Hydrocarbon in Catalyst in

    E-Print Network [OSTI]

    Ladkin, Peter B.

    Hydrocarbon in Steam in Catalyst in Vent 1 Vent 2 Product out Tank Pressure #12;#12;#12;#12;#12;#12;#12;#12;Hydrocarbon in Steam in Catalyst in Vent 1 Vent 2 Product out Tank Pressure controller Computer operator

  13. Vibrational spectroscopic studies of adsorbates on bimetallic surfaces. Doctoral thesis

    SciTech Connect (OSTI)

    Kuhn, W.K.

    1992-12-01

    In this work, well-defined bimetallic surfaces have been studied using carbon monoxide adsorption in conjunction with infrared reflection absorption spectroscopy (IRAS). These studies have indicated that for CO adsorbed on Cu overlayers, the bond between the CO and the Cu adatoms is comprised of both pi-back-donation and polarization interaction components. The sum of the contributions from these effects determines the observed bond strength with the observed CO stretching frequency being determined by the relative contributions of the components. In addition, it was determined that IR spectra of adsorbed CO show a remarkable sensitivity to surface structure. Three-dimensional Cu clusters, well-ordered two dimensional Cu islands and isolated Cu atoms are distinctively characterized by their CO IR peaks. In addition, both disorder-order and order-order transitions are observed for the metal overlayers on the single crystal metal substrates. It was also observed that localized segregation and ordering of mixed Co and S overlayers on a Mo(110) substrate occurs upon annealing.

  14. Lattice-Strain Control of Exceptional Activity in Dealloyed Core-Shell Fuel Cell Catalysts

    SciTech Connect (OSTI)

    Strasser, Peter

    2011-08-19

    We present a combined experimental and theoretical approach to demonstrate how lattice strain can be used to continuously tune the catalytic activity of the oxygen reduction reaction (ORR) on bimetallic nanoparticles that have been dealloyed. The sluggish kinetics of the ORR is a key barrier to the adaptation of fuel cells and currently limits their widespread use. Dealloyed Pt-Cu bimetallic nanoparticles, however, have been shown to exhibit uniquely high reactivity for this reaction. We first present evidence for the formation of a core-shell structure during dealloying, which involves removal of Cu from the surface and subsurface of the precursor nanoparticles. We then show that the resulting Pt-rich surface shell exhibits compressive strain that depends on the composition of the precursor alloy. We next demonstrate the existence of a downward shift of the Pt d-band, resulting in weakening of the bond strength of intermediate oxygenated species due to strain. Finally, we combine synthesis, strain, and catalytic reactivity in an experimental/theoretical reactivity-strain relationship which provides guidelines for the rational design of strained oxygen reduction electrocatalysts. The stoichiometry of the precursor, together with the dealloying conditions, provides experimental control over the resulting surface strain and thereby allows continuous tuning of the surface electrocatalytic reactivity - a concept that can be generalized to other catalytic reactions.

  15. Multimetallic nanoparticle catalysts with enhanced electrooxidation...

    Office of Scientific and Technical Information (OSTI)

    mAmg Pt, and retain greater than 90% activity after a 13 hour stability test. Authors: Sun, Shouheng ; Zhang, Sen ; Zhu, Huiyuan ; Guo, Shaojun Publication Date: 2015-07-28 OSTI...

  16. Multimetallic nanoparticle catalysts with enhanced electrooxidation

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfate Reducing(JournalspectroscopyReport)Fermentativea

  17. Multimetallic nanoparticle catalysts with enhanced electrooxidation

    Office of Scientific and Technical Information (OSTI)

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantity of NaturalDukeWakefieldSulfate Reducing(JournalspectroscopyReport)Fermentativea(Patent) | SciTech Connect Patent:

  18. Strategies for Probing Nanometer-Scale Electrocatalysts: From Single Particles to Catalyst-Membrane Architectures

    SciTech Connect (OSTI)

    Korzeniewski, Carol

    2014-01-20

    The project primary objectives are to prepare and elucidate the promoting properties of materials that possess high activity for the conversion of hydrogen and related small molecules (water, oxygen, carbon monoxide and methanol) in polymer electrolyte fuel cells. One area of research has focused on the study of catalyst materials. Protocols were developed for probing the structure and benchmarking the activity of Pt and Pt bimetallic nanometer-scale catalyst against Pt single crystal electrode standards. A second area has targeted fuel cell membrane and the advancement of simple methods mainly based on vibrational spectroscopy that can be applied broadly in the study of membrane structure and transport properties. Infrared and Raman methods combined with least-squares data modeling were applied to investigate and assist the design of robust, proton conductive membranes, which resist reactant crossover.

  19. System for reactivating catalysts

    DOE Patents [OSTI]

    Ginosar, Daniel M. (Idaho Falls, ID); Thompson, David N. (Idaho Falls, ID); Anderson, Raymond P. (Idaho Falls, ID)

    2010-03-02

    A method of reactivating a catalyst, such as a solid catalyst or a liquid catalyst is provided. The method comprises providing a catalyst that is at least partially deactivated by fouling agents. The catalyst is contacted with a fluid reactivating agent that is at or above a critical point of the fluid reactivating agent and is of sufficient density to dissolve impurities. The fluid reactivating agent reacts with at least one fouling agent, releasing the at least one fouling agent from the catalyst. The at least one fouling agent becomes dissolved in the fluid reactivating agent and is subsequently separated or removed from the fluid reactivating agent so that the fluid reactivating agent may be reused. A system for reactivating a catalyst is also disclosed.

  20. Textured catalysts and methods of making textured catalysts

    DOE Patents [OSTI]

    Werpy, Todd (West Richland, WA); Frye, Jr., John G. (Richland, WA); Wang, Yong (Richland, WA); Zacher, Alan H. (Kennewick, WA)

    2007-03-06

    A textured catalyst having a hydrothermally-stable support, a metal oxide and a catalyst component is described. Methods of conducting aqueous phase reactions that are catalyzed by a textured catalyst are also described. The invention also provides methods of making textured catalysts and methods of making chemical products using a textured catalyst.

  1. Real-Time Optical Characterization of Laser Oxidation Process in Bimetallic Direct Write Gray Scale Photomasks

    E-Print Network [OSTI]

    Chapman, Glenn H.

    density (OD), changes smoothly with increasing laser power, from ~3.0OD (unexposed) to developed capable of providing real time optical density and exposure power changes for the bimetallic thin) are exposed to laser light with power greater than its conversion threshold power, the thin film oxidizes

  2. Plasma/ion-controlled metal catalyst saturation: Enabling simultaneous growth of carbon nanotube/nanocone arrays

    SciTech Connect (OSTI)

    Levchenko, I.; Ostrikov, K.

    2008-02-11

    It is shown that the simultaneous saturation of Ni nanoparticles used as catalyst for vertically aligned carbon nanotube and nanocone arrays can be improved in low-temperature plasma- or ion-assisted processes compared with neutral gas-based routes. The results of hybrid multiscale numerical simulations of the catalyst nanoarrays (particle sizes of 2 and 10 nm) saturation with carbon show the possibility of reducing the difference in catalyst incubation times for smallest and largest catalyst particles by up to a factor of 2. This approach is generic and provides process conditions for simultaneous nucleation and growth of uniform arrays of vertically aligned nanostructures.

  3. Methods of making textured catalysts

    DOE Patents [OSTI]

    Werpy, Todd (West Richland, WA); Frye, Jr., John G. (Richland, WA); Wang, Yong (Richland, WA); Zacher, Alan H. (Kennewick, WA)

    2010-08-17

    A textured catalyst having a hydrothermally-stable support, a metal oxide and a catalyst component is described. Methods of conducting aqueous phase reactions that are catalyzed by a textured catalyst are also described. The invention also provides methods of making textured catalysts and methods of making chemical products using a textured catalyst.

  4. Ferroplasmons: Intense Localized Surface Plasmons in Metal-Ferromagnetic Nanoparticles

    SciTech Connect (OSTI)

    Sachan, Ritesh [University of Tennessee, Knoxville (UTK); Malasi, Abhinav [ORNL; Ge, Jingxuan [Materials Science and Engineering Department, University of Tennessee, Knoxville, TN, USA; Yadavali, Sagar P [ORNL; Gangopadhyay, Anup [Washington University, St. Louis; Krishna, Dr. Hare [Washington University, St. Louis; Garcia, Hernando [Southern Illinois University; Duscher, Gerd J M [ORNL; Kalyanaraman, Ramki [University of Tennessee, Knoxville (UTK)

    2014-01-01

    Interaction of photons with matter at length scales far below their wavelengths has given rise to many novel phenomena, including localized surface plasmon resonance (LSPR). However, LSPR with narrow bandwidth (BW) is observed only in a select few noble metals, and ferromagnets are not among them. Here, we report the discovery of LSPR in ferromagnetic Co and CoFe alloy (8% Fe) in contact with Ag in the form of bimetallic nanoparticles prepared by pulsed laser dewetting. These plasmons in metal-erromagnetic nanostructures, or ferroplasmons (FP) for short, are in the visible spectrum with comparable intensity and BW to those of the LSPRs from the Ag regions. This finding was enabled by electron energy-loss mapping across individual nanoparticles in a monochromated scanning transmission electron microscope. The appearance of the FP is likely due to plasmonic interaction between the contacting Ag and Co nanoparticles. Since there is no previous evidence for materials that simultaneously show ferromagnetism and such intense LSPRs, this discovery may lead to the design of improved plasmonic materials and applications. It also demonstrates that materials with interesting plasmonic properties can be synthesized using bimetallic nanostructures in contact with each other.

  5. Molecularly engineering homogenous catalysts 

    E-Print Network [OSTI]

    Hughes, Reagan Rebekah

    2013-02-22

    quickly. To attempt to 1G overcome this problem, Bergbreiter's group began work on synthesis of palladacycles in an attempt to find a more robust catalyst. The group was spurred to do this by the success of Denmark using chiral bis (oxazoline) palladium... useful in a Heck-type vinylation of aryl halides. As Bergbreiter and coworkers discovered, new tridentate SCS-type palladium (II) complexes are effective catalysts for Heck reactions between aryl iodides and alkene acceptors. The catalyst...

  6. Catalyst deposition by spin-coating for synthesis of vertically-aligned single-walled carbon nanotubes

    E-Print Network [OSTI]

    Maruyama, Shigeo

    Catalyst deposition by spin-coating for synthesis of vertically-aligned single-walled carbon-SWNTs) are synthesized from catalyst nanoparticles deposited onto Si or quartz substrates by a dip-coating process [3]. Here we present a spin-coating method as an alternative to dip-coating, where cobalt and molybdenum

  7. Numerical simulation of carbon arc discharge for nanoparticle synthesis

    SciTech Connect (OSTI)

    Kundrapu, M.; Keidar, M.

    2012-07-15

    Arc discharge with catalyst-filled carbon anode in helium background was used for the synthesis of carbon nanoparticles. In this paper, we present the results of numerical simulation of carbon arc discharges with arc current varying from 10 A to 100 A in a background gas pressure of 68 kPa. Anode sublimation rate and current voltage characteristics are compared with experiments. Distribution of temperature and species density, which is important for the estimation of the growth of nanoparticles, is obtained. The probable location of nanoparticle growth region is identified based on the temperature range for the formation of catalyst clusters.

  8. DNA-guided nanoparticle assemblies

    DOE Patents [OSTI]

    Gang, Oleg; Nykypanchuk, Dmytro; Maye, Mathew; van der Lelie, Daniel

    2013-07-16

    In some embodiments, DNA-capped nanoparticles are used to define a degree of crystalline order in assemblies thereof. In some embodiments, thermodynamically reversible and stable body-centered cubic (bcc) structures, with particles occupying <.about.10% of the unit cell, are formed. Designs and pathways amenable to the crystallization of particle assemblies are identified. In some embodiments, a plasmonic crystal is provided. In some aspects, a method for controlling the properties of particle assemblages is provided. In some embodiments a catalyst is formed from nanoparticles linked by nucleic acid sequences and forming an open crystal structure with catalytically active agents attached to the crystal on its surface or in interstices.

  9. Nanostructured catalyst supports

    DOE Patents [OSTI]

    Zhu, Yimin; Goldman, Jay L.; Qian, Baixin; Stefan, Ionel C.

    2012-10-02

    The present invention relates to SiC nanostructures, including SiC nanopowder, SiC nanowires, and composites of SiC nanopowder and nanowires, which can be used as catalyst supports in membrane electrode assemblies and in fuel cells. The present invention also relates to composite catalyst supports comprising nanopowder and one or more inorganic nanowires for a membrane electrode assembly.

  10. Hydrocracking of n-decane over zeolite-supported metal sulfide catalysts. 2: Zeolite Y-supported Ni and Ni-Mo sulfides

    SciTech Connect (OSTI)

    Welters, W.J.J.; Waerden, O.H. van der; Beer, V.H.J. de; Santen, R.A. van [Eindhoven Univ. of Technology (Netherlands). Schuit Inst. of Catalysis

    1995-04-01

    For zeolite Y-supported nickel sulfide catalysts the influence of the metal sulfide dispersion on the hydrocracking properties for n-decane is examined. In order to obtain different nickel sulfide distributions (inside or outside the zeolite structure) and dispersions, the preparation method (impregnation of CaY or ion exchange of NaY), sulfidation procedure (direct sulfidation or sulfidation after drying), and metal loading are varied. A higher nickel sulfide surface (as measured by dynamic oxygen chemisorption) results in a strong increase of the n-decane conversion, but this is not accompanied by an improvement of the catalytic properties toward ideal hydrocracking. Additionally, some zeolite Y-supported Ni-Mo sulfide catalysts (varying in preparation method and sulfidation procedure) are tested for the hydroconversion of it-decane. However, no promoter effect could be observed. The activity of the bimetallic sulfide catalysts is always almost equal to that of the most active monometallic sulfide constituent.

  11. MgO-Supported Cluster Catalysts with Pt-Ru Interactions Prepared from Pt3Ru6(CO)21(u3-H)(u-H)3

    SciTech Connect (OSTI)

    Chotisuwan,S.; Wittapyakun, J.; Lobo-Lapidus, R.; Gates, B.

    2007-01-01

    Bimetallic MgO-supported catalysts were prepared by adsorption of Pt{sub 3}Ru{sub 6}(CO){sub 21}({mu}{sub 3}-H)({mu}-H){sub 3} on porous MgO. Characterization of the supported clusters by infrared (IR) spectroscopy showed that the adsorbed species were still in the form of metal carbonyls. The supported clusters were decarbonylated by treatment in flowing helium at 300 C, as shown by IR and extended X-ray absorption fine structure (EXAFS) data, and the resulting supported PtRu clusters were shown by EXAFS spectroscopy to have metal frames that retained Pt-Ru bonds but were slightly restructured relative to those of the precursor; the average cluster size was almost unchanged as a result of the decarbonylation. These are among the smallest reported bimetallic clusters of group-8 metals. The decarbonylated sample catalyzed ethylene hydrogenation with an activity similar to that reported previously for {gamma}-Al{sub 2}O{sub 3}-supported clusters prepared in nearly the same way and having nearly the same structure. Both samples were also active for n-butane hydrogenolysis, with the MgO-supported catalyst being more active than the {gamma}-Al{sub 2}O{sub 3}-supported catalyst.

  12. Electrodeposition of Au/Ag bimetallic dendrites assisted by Faradaic AC-electroosmosis flow

    SciTech Connect (OSTI)

    Ji, Jianlong; Li, Pengwei; Sang, Shengbo, E-mail: sbsang@tyut.edu.cn; Zhang, Wendong, E-mail: wdzhang@tyut.edu.cn; Li, Gang; Hu, Jie [Micro and Nano-system Research Centre, College of Information Engineering, Taiyuan University of Technology, 030024, Taiyuan (China)] [Micro and Nano-system Research Centre, College of Information Engineering, Taiyuan University of Technology, 030024, Taiyuan (China); Zhou, Zhaoying, E-mail: zhouzy@mail.tsinghua.edu.cn; Yang, Xing; Dong, Hualai [MEMS Laboratory, Department of Precision Instruments, Tsinghua University, 100084, Beijing (China)] [MEMS Laboratory, Department of Precision Instruments, Tsinghua University, 100084, Beijing (China)

    2014-03-15

    Au/Ag bimetallic dendrites were synthesized successfully from the corresponding aqueous solution via the AC electrodeposition method. Both of the morphologies and compositions could be tuned by the electrolyte concentration and AC frequency. The prepared bimetallic dendrites were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectrometer (EDS), transmission electron microscopy (TEM) and UV–vis spectroscopy. The underlying dendrite growth mechanism was then proposed in the context of the Directed Electrochemical Nanowires Assembly (DENA) models. Owing to the unscreened voltage dropping in the electrolyte bulk, electromigration dominates the species flux process, and cations tend to accumulate in areas with strong electric field intensity, such as electrode edges. Moreover, Faradaic AC-electro-osmosis (ACEO) flow could increase the effective diffusion layer thickness in these areas during the electrochemical reaction, and leads to dendrite growth. Further Micro-Raman observations illustrated that the Au/Ag bimetallic dendrites exhibited pronounced surface-enhanced Raman scattering (SERS) activity, using 4-mercaptopyridine (4-MP) as model molecules.

  13. Catalyst for microelectromechanical systems microreactors

    DOE Patents [OSTI]

    Morse, Jeffrey D. (Martinez, CA); Sopchak, David A. (Livermore, CA); Upadhye, Ravindra S. (Pleasanton, CA); Reynolds, John G. (San Ramon, CA); Satcher, Joseph H. (Patterson, CA); Gash, Alex E. (Brentwood, CA)

    2010-06-29

    A microreactor comprising a silicon wafer, a multiplicity of microchannels in the silicon wafer, and a catalyst coating the microchannels. In one embodiment the catalyst coating the microchannels comprises a nanostructured material. In another embodiment the catalyst coating the microchannels comprises an aerogel. In another embodiment the catalyst coating the microchannels comprises a solgel. In another embodiment the catalyst coating the microchannels comprises carbon nanotubes.

  14. Catalyst for microelectromechanical systems microreactors

    DOE Patents [OSTI]

    Morse, Jeffrey D. (Martinez, CA); Sopchak, David A. (Livermore, CA); Upadhye, Ravindra S. (Pleasanton, CA); Reynolds, John G. (San Ramon, CA); Satcher, Joseph H. (Patterson, CA); Gash, Alex E. (Brentwood, CA)

    2011-11-15

    A microreactor comprising a silicon wafer, a multiplicity of microchannels in the silicon wafer, and a catalyst coating the microchannels. In one embodiment the catalyst coating the microchannels comprises a nanostructured material. In another embodiment the catalyst coating the microchannels comprises an aerogel. In another embodiment the catalyst coating the microchannels comprises a solgel. In another embodiment the catalyst coating the microchannels comprises carbon nanotubes.

  15. Transition metal carbides, nitrides and borides, and their oxygen containing analogs useful as water gas shift catalysts

    DOE Patents [OSTI]

    Thompson, Levi T.; Patt, Jeremy; Moon, Dong Ju; Phillips, Cory

    2003-09-23

    Mono- and bimetallic transition metal carbides, nitrides and borides, and their oxygen containing analogs (e.g. oxycarbides) for use as water gas shift catalysts are described. In a preferred embodiment, the catalysts have the general formula of M1.sub.A M2.sub.B Z.sub.C O.sub.D, wherein M1 is selected from the group consisting of Mo, W, and combinations thereof; M2 is selected from the group consisting of Fe, Ni, Cu, Co, and combinations thereof; Z is selected from the group consisting of carbon, nitrogen, boron, and combinations thereof; A is an integer; B is 0 or an integer greater than 0; C is an integer; O is oxygen; and D is 0 or an integer greater than 0. The catalysts exhibit good reactivity, stability, and sulfur tolerance, as compared to conventional water shift gas catalysts. These catalysts hold promise for use in conjunction with proton exchange membrane fuel cell powered systems.

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

    DOE Patents [OSTI]

    Angelici, Robert J. (Ames, IA); Gao, Hanrong (Ames, IA)

    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.

  17. 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.

  18. Epoxidation catalyst and process

    DOE Patents [OSTI]

    Linic, Suljo (Ann Arbor, MI); Christopher, Phillip (Ann Arbor, MI)

    2010-10-26

    Disclosed herein is a catalytic method of converting alkenes to epoxides. This method generally includes reacting alkenes with oxygen in the presence of a specific silver catalyst under conditions suitable to produce a yield of the epoxides. The specific silver catalyst is a silver nanocrystal having a plurality of surface planes, a substantial portion of which is defined by Miller indices of (100). The reaction is performed by charging a suitable reactor with this silver catalyst and then feeding the reactants to the reactor under conditions to carry out the reaction. The reaction may be performed in batch, or as a continuous process that employs a recycle of any unreacted alkenes. The specific silver catalyst has unexpectedly high selectivity for epoxide products. Consequently, this general method (and its various embodiments) will result in extraordinarily high epoxide yields heretofore unattainable.

  19. Hydrocracking catalysts and processes

    SciTech Connect (OSTI)

    Dolbear, G.E. [G.E. Dolbear and Associates, Diamond Bar, CA (United States)

    1995-12-31

    Hydrocracking processes convert aromatic gas oils into high quality gasoline, diesel, and turbine stocks. They operate at high hydrogen pressures, typically greater than 1500 psig. Operating temperatures range from 600-700{degrees}F (315-382{degrees}C). Commercial catalysts vary in activity and selectivity, allowing process designers to emphasize middle distillates, naphtha, or both. Catalysts are quite stable in use, with two year unit run lengths typical. A pretreatment step to remove nitrogen compounds is usually part of the same process unit. These HDN units operate integrally with the hydrocracking. The hydrogenation reactions are strongly exothermic, while the cracking is roughly thermal neutral. This combination can lead to temperature runaways. To avoid this, cold hydrogen is injected at several points in hydrocracking reactors. The mechanics of mixing this hydrogen with the oil and redistributing the mixture over the catalyst bed are very important in controlling process operation and ensuring long catalyst life.

  20. Catalysts and method

    DOE Patents [OSTI]

    Taylor, Charles E. (Pittsburgh, PA); Noceti, Richard P. (Pittsburgh, PA)

    1991-01-01

    An improved catlayst and method for the oxyhydrochlorination of methane is disclosed. The catalyst includes a pyrogenic porous support on which is layered as active material, cobalt chloride in major proportion, and minor proportions of an alkali metal chloride and of a rare earth chloride. On contact of the catalyst with a gas flow of methane, HC1 and oxygen, more than 60% of the methane is converted and of that converted more than 40% occurs as monochloromethane. Advantageously, the monochloromethane can be used to produce gasoline boiling range hydrocarbons with the recycle of HCl for further reaction. This catalyst is also of value for the production of formic acid as are analogous catalysts with lead, silver or nickel chlorides substituted for the cobalt chloride.

  1. Plasmatron-catalyst system

    DOE Patents [OSTI]

    Bromberg, Leslie (Sharon, MA); Cohn, Daniel R. (Chestnut Hill, MA); Rabinovich, Alexander (Swampscott, MA); Alexeev, Nikolai (Moscow, RU)

    2007-10-09

    A plasmatron-catalyst system. The system generates hydrogen-rich gas and comprises a plasmatron and at least one catalyst for receiving an output from the plasmatron to produce hydrogen-rich gas. In a preferred embodiment, the plasmatron receives as an input air, fuel and water/steam for use in the reforming process. The system increases the hydrogen yield and decreases the amount of carbon monoxide.

  2. Crystalline titanate catalyst supports

    DOE Patents [OSTI]

    Anthony, R.G.; Dosch, R.G.

    1993-01-05

    A series of new crystalline titanates (CT) are shown to have considerable potential as catalyst supports. For Pd supported catalyst, the catalytic activity for pyrene hydrogenation was substantially different depending on the type of CT, and one was substantially more active than Pd on hydrous titanium oxide (HTO). For 1-hexene hydrogenation the activities of the new CTs were approximately the same as for the hydrous metal oxide supports.

  3. Catalyst by Design - Theoretical, Nanostructural, and Experimental...

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

    Emission Treatment Catalyst Catalyst by Design - Theoretical, Nanostructural, and Experimental Studies of Emission Treatment Catalyst Poster presented at the 16th Directions in...

  4. Catalyst by Design - Theoretical, Nanostructural, and Experimental...

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

    Oxidation Catalyst for Diesel Engine Emission Treatment Catalyst by Design - Theoretical, Nanostructural, and Experimental Studies of Oxidation Catalyst for Diesel Engine Emission...

  5. Nanoscale Chemical Imaging of a Working Catalyst

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

    Nanoscale Chemical Imaging of a Working Catalyst Nanoscale Chemical Imaging of a Working Catalyst Print Wednesday, 28 January 2009 00:00 The heterogeneous catalysts used in most...

  6. Reaction selectivity studies on nanolithographically-fabricated platinum model catalyst arrays

    SciTech Connect (OSTI)

    Grunes, Jeffrey Benjamin

    2004-05-15

    In an effort to understand the molecular ingredients of catalytic activity and selectivity toward the end of tuning a catalyst for 100% selectivity, advanced nanolithography techniques were developed and utilized to fabricate well-ordered two-dimensional model catalyst arrays of metal nanostructures on an oxide support for the investigation of reaction selectivity. In-situ and ex-situ surface science techniques were coupled with catalytic reaction data to characterize the molecular structure of the catalyst systems and gain insight into hydrocarbon conversion in heterogeneous catalysis. Through systematic variation of catalyst parameters (size, spacing, structure, and oxide support) and catalytic reaction conditions (hydrocarbon chain length, temperature, pressures, and gas composition), the data presented in this dissertation demonstrate the ability to direct a reaction by rationally adjusting, through precise control, the design of the catalyst system. Electron beam lithography (EBL) was employed to create platinum nanoparticles on an alumina (Al{sub 2}O{sub 3}) support. The Pt nanoparticle spacing (100-150-nm interparticle distance) was varied in these samples, and they were characterized using x-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and atomic force microscopy (AFM), both before and after reactions. The TEM studies showed the 28-nm Pt nanoparticles with 100 and 150-nm interparticle spacing on alumina to be polycrystalline in nature, with crystalline sizes of 3-5 nm. The nanoparticle crystallites increased significantly after heat treatment. The nanoparticles were still mostly polycrystalline in nature, with 2-3 domains. The 28-nm Pt nanoparticles deposited on alumina were removed by the AFM tip in contact mode with a normal force of approximately 30 nN. After heat treatment at 500 C in vacuum for 3 hours, the AFM tip, even at 4000 nN, could not remove the platinum nanoparticles. The increase of adhesion upon heat treatment indicates stronger bonding between the Pt and the support at the metal-oxide interface.

  7. Hydrazine Fuels for Bimetallic Catalytic Microfluidic Pumping Michael E. Ibele, Yang Wang, Timothy R. Kline, Thomas E. Mallouk,* and Ayusman Sen*

    E-Print Network [OSTI]

    by the asymmetric catalytic decomposition of hydrogen peroxide over bimetallic surfaces.1-7 Movement on larger the proper choice of fuel. The novel bimetallic fluid pumping system consists of spatially defined palladium the palladium features along the gold surface (Figure 1). Surfaces were prepared by using an electron beam

  8. Carbon nanotube forests growth using catalysts from atomic layer deposition

    SciTech Connect (OSTI)

    Chen, Bingan; Zhang, Can; Esconjauregui, Santiago; Xie, Rongsi; Zhong, Guofang; Robertson, John; Bhardwaj, Sunil; Cepek, Cinzia

    2014-04-14

    We have grown carbon nanotubes using Fe and Ni catalyst films deposited by atomic layer deposition. Both metals lead to catalytically active nanoparticles for growing vertically aligned nanotube forests or carbon fibres, depending on the growth conditions and whether the substrate is alumina or silica. The resulting nanotubes have narrow diameter and wall number distributions that are as narrow as those grown from sputtered catalysts. The state of the catalyst is studied by in-situ and ex-situ X-ray photoemission spectroscopy. We demonstrate multi-directional nanotube growth on a porous alumina foam coated with Fe prepared by atomic layer deposition. This deposition technique can be useful for nanotube applications in microelectronics, filter technology, and energy storage.

  9. Final Technical Report on DE-SC00002460 [Bimetallic or trimetallic materials with structural metal centers based on Mn, Fe or V

    SciTech Connect (OSTI)

    Takeuchi, Esther Sans; Takeuchi, Kenneth James; Marschilok, Amy Catherine

    2013-07-26

    Bimetallic or trimetallic materials with structural metal centers based on Mn, Fe or V were investigated under this project. These metal centers are the focus of this research as they have high earth abundance and have each shown success as cathode materials in lithium batteries. Silver ion, Ag{sup +}, was initially selected as the displacement material as reduction of this center should result in increased conductivity as Ag{sup 0} metal particles are formed in-situ upon electrochemical reduction. The in-situ formation of metal nanoparticles upon electrochemical reduction has been previously noted, and more recently, we have investigated the resulting increase in conductivity. Layered materials as well as materials with tunnel or channel type structures were selected. Layered materials are of interest as they can provide 2-dimensional ion mobility. Tunnel or channel structures are also of interest as they provide a rigid framework that should remain stable over many discharge/charge cycles. We describe some examples of materials we have synthesized that demonstrate promising electrochemistry.

  10. Method for forming thermally stable nanoparticles on supports

    DOE Patents [OSTI]

    Roldan Cuenya, Beatriz; Naitabdi, Ahmed R.; Behafarid, Farzad

    2013-08-20

    An inverse micelle-based method for forming nanoparticles on supports includes dissolving a polymeric material in a solvent to provide a micelle solution. A nanoparticle source is dissolved in the micelle solution. A plurality of micelles having a nanoparticle in their core and an outer polymeric coating layer are formed in the micelle solution. The micelles are applied to a support. The polymeric coating layer is then removed from the micelles to expose the nanoparticles. A supported catalyst includes a nanocrystalline powder, thin film, or single crystal support. Metal nanoparticles having a median size from 0.5 nm to 25 nm, a size distribution having a standard deviation .ltoreq.0.1 of their median size are on or embedded in the support. The plurality of metal nanoparticles are dispersed and in a periodic arrangement. The metal nanoparticles maintain their periodic arrangement and size distribution following heat treatments of at least 1,000.degree. C.

  11. Supported organoiridium catalysts for alkane dehydrogenation

    DOE Patents [OSTI]

    Baker, R. Thomas; Sattelberger, Alfred P.; Li, Hongbo

    2013-09-03

    Solid supported organoiridium catalysts, a process for preparing such solid supported organoiridium catalysts, and the use of such solid supported organoiridium catalysts in dehydrogenation reactions of alkanes is provided. The catalysts can be easily recovered and recycled.

  12. Degradation of Bimetallic Model Electrocatalysts ___ an in situ XAS Study

    SciTech Connect (OSTI)

    Friebel, Daniel

    2011-06-22

    One of the major challenges in the development of clean energy fuel cells is the performance degradation of the electrocatalyst, which, apart from poisoning effects, can suffer from corrosion due to its exposure to a harsh environment under high potentials. In this communication, we demonstrate how interactions of Pt with a transition metal support affect not only, as commonly intended, the catalytic activity, but also the reactivity of Pt towards oxide formation or dissolution. We use two well-defined single-crystal model systems, Pt/Rh(111) and Pt/Au(111) and a unique x-ray spectroscopy technique with enhanced energy resolution to monitor the potential-dependent oxidation state of Pt, and find two markedly different oxidation mechanisms on the two different substrates. This information can be of great significance for future design of more active and more stable catalysts. We have studied the potential-induced degradation of Pt monolayer model electrocatalysts on Rh(111) and Au(111) single-crystal substrates. The anodic formation of Pt oxides was monitored using in situ high energy resolution fluorescence detection x-ray absorption spectroscopy (HERFD XAS). Although Pt was deposited on both substrates in a three-dimensional island growth mode, we observed remarkable differences during oxide formation that can only be understood in terms of strong Pt-substrate interactions throughout the Pt islands. Anodic polarization of Pt/Rh(111) up to +1.6 V vs. RHE (reversible hydrogen electrode) leads to formation an incompletely oxidized passive layer, whereas formation of PtO2 and partial Pt dissolution is observed for Pt/Au(111).

  13. Reforming using erionite catalysts

    SciTech Connect (OSTI)

    Liers, J.; Meusinger, J.; Moesch, A. (Univ. of Leipzig (Germany)); Reschetilowski, W. (Karl Winnacker Inst. of DECHEMA, Frankfurt (Germany))

    1993-08-01

    The advantage of reforming on erionite catalysts is a product with high octane numbers and low amounts of aromatics. This advantage seems to be slight at reaction pressures lower than 25 bar. But it is possible to compensate for the influence of pressure by varying the erionite content within the catalyst and the reaction temperature. When reforming on Pt/Al[sub 2]O[sub 3] catalysts, the following reactions take place: dehydrocyclization of paraffins to naphthenes, dehydrogenation of naphthenes to aromatics, isomerication of normal paraffins remains in the product, lowering its octane number. By using a Ni/H-erionite catalyst, the octane rating can be increased by 3 to 7 numbers through selective hydrocracking of n-alkanes in the reformate. Erionite catalysts favor shape-selective hydrocracking of normal paraffins and the formation of cyclopentane derivatives lowering the content of aromatics during reforming reactions. Reducing the reaction pressure decreases hydrocracking activity and cyclopentane formation. These results can be interpreted in terms of thermodynamic restrictions and deactivation.

  14. Catalysts available from East Germany

    SciTech Connect (OSTI)

    Not Available

    1990-10-01

    This paper reports that a company in East Germany manufactures catalytic reforming, hydrocracking, mild hydrocracking, hydrotreating, and hydrorefining catalysts, among others. The company offers almost 50 catalysts for these processing categories.

  15. Hydroprocessing catalyst and process

    SciTech Connect (OSTI)

    Chen, N.Y.; Huang, T.J.

    1988-07-12

    In a hydrocracking process for converting a hydrocarbon feed, at least 70% of which boils within the range of 650/sup 0/ to about 1050/sup 0/F, to liquid products boiling in the rane of C/sub 5/+ to 700/sup 0/F. This patent describes a process which comprises contacting the feed and gaseous hydrogen at elevated pressure with a hydrocracking catalyst under hydrocracking conditions. The improvement comprises: contacting the feed with a hydrocracking catalyst composition comprising a hydrogenation component, a crystalline aluminosilicate cracking component having the essential X-ray diffraction pattern of Zeolite Beta, the crystalline aluminosilicate being further characterized by the presence of 0.5 wt % to about 4.0 wt % of framework boron and a silica to alumina ratio of at least about 35, and a solid source of alumina, whereby the catalyst life is extended.

  16. Partial oxidation catalyst

    DOE Patents [OSTI]

    Krumpelt, Michael (Naperville, IL); Ahmed, Shabbir (Bolingbrook, IL); Kumar, Romesh (Naperville, IL); Doshi, Rajiv (Downers Grove, IL)

    2000-01-01

    A two-part catalyst comprising a dehydrogenation portion and an oxide-ion conducting portion. The dehydrogenation portion is a group VIII metal and the oxide-ion conducting portion is selected from a ceramic oxide crystallizing in the fluorite or perovskite structure. There is also disclosed a method of forming a hydrogen rich gas from a source of hydrocarbon fuel in which the hydrocarbon fuel contacts a two-part catalyst comprising a dehydrogenation portion and an oxide-ion conducting portion at a temperature not less than about 400.degree. C. for a time sufficient to generate the hydrogen rich gas while maintaining CO content less than about 5 volume percent. There is also disclosed a method of forming partially oxidized hydrocarbons from ethanes in which ethane gas contacts a two-part catalyst comprising a dehydrogenation portion and an oxide-ion conducting portion for a time and at a temperature sufficient to form an oxide.

  17. Thermal plasma synthesis of Fe{sub 1?x}Ni{sub x} alloy nanoparticles

    SciTech Connect (OSTI)

    Raut, Suyog A.; Kanhe, Nilesh S.; Bhoraskar, S. V.; Mathe, V. L.; Das, A. K.

    2014-04-24

    Fe-Ni alloy nanoparticles are of great interest because of diverse practical applications in the fields such as magnetic fluids, high density recording media, catalysis and medicine. We report the synthesis of Fe-Ni nanoparticles via thermal plasma route. Thermal plasma assisted synthesis is a high temperature process and gives high yields of production. Here, we have used direct arc thermal plasma plume of 6kw as a source of energy at operating pressure 500 Torr. The mixture of Fe-Ni powder in required proportion (Fe{sub 1?x}Ni{sub x}; x=0.30, 0.32, 0.34, 0.36, 0.38 and 0.40) was made to evaporate simultaneously from the graphite anode in thermal plasma reactor to form Fe-Ni bimetallic nanoparticles. The as synthesized particles were characterized by X-Ray Diffraction (XRD), Thermo-Gravimetric Analysis/Differential Scanning Calorimtry (TGA/DSC)

  18. Aerogel derived catalysts

    SciTech Connect (OSTI)

    Reynolds, J. G., LLNL

    1996-12-11

    Aerogels area class of colloidal materials which have high surface areas and abundant mesoporous structure. SiO{sub 2} aerogels show unique physical, optical and structural properties. When catalytic metals are incorporated in the aerogel framework, the potential exists for new and very effective catalysts for industrial processes. Three applications of these metal-containing SiO{sub 2} aerogels as catalysts are briefly reviewed in this paper--NO{sub x} reduction, volatile organic compound destruction, and partial oxidation of methane.

  19. Zinc sulfide liquefaction catalyst

    DOE Patents [OSTI]

    Garg, Diwakar (Macungie, PA)

    1984-01-01

    A process for the liquefaction of carbonaceous material, such as coal, is set forth wherein coal is liquefied in a catalytic solvent refining reaction wherein an activated zinc sulfide catalyst is utilized which is activated by hydrogenation in a coal derived process solvent in the absence of coal.

  20. Catalysts get concentrated attention

    SciTech Connect (OSTI)

    Bruch, H.W.

    1989-02-27

    At the most recent National Petroleum Refiners Association annual question and answer session on refining and petrochemical technology, refiners concentrated heavily on questions pertaining to modern catalyst technology and its applications and operating experiences, including: fluid catalytic cracking, hydrocracking, hydrotreating, and catalytic reforming.

  1. Molybdenum sulfide/carbide catalysts

    DOE Patents [OSTI]

    Alonso, Gabriel (Chihuahua, MX); Chianelli, Russell R. (El Paso, TX); Fuentes, Sergio (Ensenada, MX); Torres, Brenda (El Paso, TX)

    2007-05-29

    The present invention provides methods of synthesizing molybdenum disulfide (MoS.sub.2) and carbon-containing molybdenum disulfide (MoS.sub.2-xC.sub.x) catalysts that exhibit improved catalytic activity for hydrotreating reactions involving hydrodesulfurization, hydrodenitrogenation, and hydrogenation. The present invention also concerns the resulting catalysts. Furthermore, the invention concerns the promotion of these catalysts with Co, Ni, Fe, and/or Ru sulfides to create catalysts with greater activity, for hydrotreating reactions, than conventional catalysts such as cobalt molybdate on alumina support.

  2. Dye-sensitised semiconductors modified with molecular catalysts for light-driven H? production

    E-Print Network [OSTI]

    Willkomm, Janina; Orchard, Katherine L.; Reynal, Anna; Pastor, Ernest; Durrant, James R.; Reisner, Erwin

    2015-01-01

    ’. Dye-sensitised photocatalysis (DSP) with molecular catalysts is a relatively new approach to convert sunlight into a fuel such as H? and is based on the self-assembly of a molecular dye and electrocatalyst on a semiconductor nanoparticle. DSP systems...

  3. SHAPE SELECTIVE NANO-CATALYSTS: TOWARD DIRECT METHANOL FUEL CELLS APPLICATIONS

    SciTech Connect (OSTI)

    Murph, S.

    2010-06-16

    A series of bimetallic core-shell-alloy type Au-Pt nanomaterials with various morphologies, aspect ratios and compositions, were produced in a heterogenous epitaxial fashion. Gold nanoparticles with well-controlled particle size and shape, e.g. spheres, rods and cubes, were used as 'seeds' for platinum growth in the presence of a mild reducing agent, ascorbic acid and a cationic surfactant cethyltrimethyl ammonium bromide (CTAB). The reactions take place in air and water, and are quick, economical and amenable for scaling up. The synthesized nanocatalysts were characterized by electron microscopy techniques and energy dispersive X-ray analysis. Nafion membranes were embedded with the Au-Pt nanomaterials and analyzed by atomic force microscopy (AFM) and scanning electron microscopy (SEM) for their potential in direct methanol fuel cells applications.

  4. Size Effect of Ruthenium Nanoparticles in Catalytic Carbon Monoxide Oxidation

    SciTech Connect (OSTI)

    Joo, Sang Hoon; Park, Jeong Y.; Renzas, J. Russell; Butcher, Derek R.; Huang, Wenyu; Somorjai, Gabor A.

    2010-04-04

    Carbon monoxide oxidation over ruthenium catalysts has shown an unusual catalytic behavior. Here we report a particle size effect on CO oxidation over Ru nanoparticle (NP) catalysts. Uniform Ru NPs with a tunable particle size from 2 to 6 nm were synthesized by a polyol reduction of Ru(acac){sub 3} precursor in the presence of poly(vinylpyrrolidone) stabilizer. The measurement of catalytic activity of CO oxidation over two-dimensional Ru NPs arrays under oxidizing reaction conditions (40 Torr CO and 100 Torr O{sub 2}) showed an activity dependence on the Ru NP size. The CO oxidation activity increases with NP size, and the 6 nm Ru NP catalyst shows 8-fold higher activity than the 2 nm catalysts. The results gained from this study will provide the scientific basis for future design of Ru-based oxidation catalysts.

  5. Gold–promoted structurally ordered intermetallic palladium cobalt nanoparticles for the oxygen reduction reaction

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

    Kuttiyiel, Kurian A.; Sasaki, Kotaro; Su, Dong; Wu, Lijun; Zhu, Yimei; Adzic, Radoslav R.

    2014-11-06

    Considerable efforts to make palladium and palladium alloys active catalysts and a possible replacement for platinum have had a marginal success. Here, we report on a structurally ordered Au??Pd??Co?? catalyst that exhibits comparable activity to conventional platinum catalysts in both acid and alkaline media. Electron microscopic techniques demonstrate that via addition of gold atoms PdCo nanoparticles undergo at elevated temperatures an atomic structural transition from core-shell to a rare intermetallic ordered structure with twin boundaries forming stable {111}, {110} and {100} facets. The superior stability of this catalyst compared to platinum after 10,000 potential cycles in alkaline media is attributedmore »to the atomic structural order of PdCo nanoparticles along with protective effect of clusters of gold atoms on the surface. This strategy of making ordered palladium intermetallic alloy nanoparticles can be used in diverse heterogeneous catalysis where particle size and structural stability matters.« less

  6. Gold–promoted structurally ordered intermetallic palladium cobalt nanoparticles for the oxygen reduction reaction

    SciTech Connect (OSTI)

    Kuttiyiel, Kurian A.; Sasaki, Kotaro; Su, Dong; Wu, Lijun; Zhu, Yimei; Adzic, Radoslav R.

    2014-11-06

    Considerable efforts to make palladium and palladium alloys active catalysts and a possible replacement for platinum have had a marginal success. Here, we report on a structurally ordered Au??Pd??Co?? catalyst that exhibits comparable activity to conventional platinum catalysts in both acid and alkaline media. Electron microscopic techniques demonstrate that via addition of gold atoms PdCo nanoparticles undergo at elevated temperatures an atomic structural transition from core-shell to a rare intermetallic ordered structure with twin boundaries forming stable {111}, {110} and {100} facets. The superior stability of this catalyst compared to platinum after 10,000 potential cycles in alkaline media is attributed to the atomic structural order of PdCo nanoparticles along with protective effect of clusters of gold atoms on the surface. This strategy of making ordered palladium intermetallic alloy nanoparticles can be used in diverse heterogeneous catalysis where particle size and structural stability matters.

  7. ?-Fe{sub 2}O{sub 3} nanoparticles: An easily recoverable effective photo-catalyst for the degradation of rose bengal and methylene blue dyes in the waste-water treatment plant

    SciTech Connect (OSTI)

    Dutta, Amit Kumar; Maji, Swarup Kumar; Adhikary, Bibhutosh

    2014-01-01

    Graphical abstract: - Highlights: • ?-Fe{sub 2}O{sub 3} NPs from a single-source precursor and characterized by XRD, TEM, UV–vis spectra. • The NPs were tested as effective photocatalyst toward degradation of RB and MB dyes. • The possible pathway of the photocatalytic decomposition process has been discussed. • The active species, OH·, was detected by TA photoluminescence probing techniques. - Abstract: ?-Fe{sub 2}O{sub 3} nanoparticles (NPs) were synthesized from a single-source precursor complex [Fe{sub 3}O(C{sub 6}H{sub 5}COO){sub 6}(H{sub 2}O){sub 3}]NO{sub 3} by a simple thermal decomposition process and have been characterized by X-ray diffraction analysis (XRD), transmission electron microscopy (TEM) and UV–vis spectroscopic techniques. The NPs were highly pure and well crystallized having hexagonal morphology with an average particle size of 35 nm. The prepared ?-Fe{sub 2}O{sub 3} (maghemite) NPs show effective photo-catalytic activity toward the degradation of rose bengal (RB) and methylene blue (MB) dyes under visible light irradiation and can easily be recoverable in the presence of magnetic field for successive re-uses. The possible photo-catalytic decomposition mechanism is discussed through the detection of hydroxyl radical (OH·) by terephthalic acid photo-luminescence probing technique.

  8. Fluorination process using catalyst

    DOE Patents [OSTI]

    Hochel, Robert C. (Aiken, SC); Saturday, Kathy A. (Aiken, SC)

    1985-01-01

    A process for converting an actinide compound selected from the group consisting of uranium oxides, plutonium oxides, uranium tetrafluorides, plutonium tetrafluorides and mixtures of said oxides and tetrafluorides, to the corresponding volatile actinide hexafluoride by fluorination with a stoichiometric excess of fluorine gas. The improvement involves conducting the fluorination of the plutonium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF.sub.3, AgF.sub.2 and NiF.sub.2, whereby the fluorination is significantly enhanced. The improvement also involves conducting the fluorination of one of the uranium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF.sub.3 and AgF.sub.2, whereby the fluorination is significantly enhanced.

  9. Fluorination process using catalysts

    DOE Patents [OSTI]

    Hochel, R.C.; Saturday, K.A.

    1983-08-25

    A process is given for converting an actinide compound selected from the group consisting of uranium oxides, plutonium oxides, uranium tetrafluorides, plutonium tetrafluorides and mixtures of said oxides and tetrafluorides, to the corresponding volatile actinide hexafluoride by fluorination with a stoichiometric excess of fluorine gas. The improvement involves conducting the fluorination of the plutonium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF/sub 3/, AgF/sub 2/ and NiF/sub 2/, whereby the fluorination is significantly enhanced. The improvement also involves conducting the fluorination of one of the uranium compounds in the presence of a fluoride catalyst selected from the group consisting of CoF/sub 3/ and AgF/sub 2/, whereby the fluorination is significantly enhanced.

  10. Binary ferrihydrite catalysts

    DOE Patents [OSTI]

    Huffman, G.P.; Zhao, J.; Feng, Z.

    1996-12-03

    A method of preparing a catalyst precursor comprises dissolving an iron salt and a salt of an oxoanion forming agent, in water so that a solution of the iron salt and oxoanion forming agent salt has a ratio of oxoanion/Fe of between 0.0001:1 to 0.5:1. Next is increasing the pH of the solution to 10 by adding a strong base followed by collecting of precipitate having a binary ferrihydrite structure. A binary ferrihydrite catalyst precursor is also prepared by dissolving an iron salt in water. The solution is brought to a pH of substantially 10 to obtain ferrihydrite precipitate. The precipitate is then filtered and washed with distilled water and subsequently admixed with a hydroxy carboxylic acid solution. The admixture is mixed/agitated and the binary ferrihydrite precipitate is then filtered and recovered. 3 figs.

  11. Steam reforming catalyst

    DOE Patents [OSTI]

    Kramarz, Kurt W. (Murrysville, PA); Bloom, Ira D. (Bolingbrook, IL); Kumar, Romesh (Naperville, IL); Ahmed, Shabbir (Bolingbrook, IL); Wilkenhoener, Rolf (Oakbrook Terrace, IL); Krumpelt, Michael (Naperville, IL)

    2001-01-01

    A method of forming a hydrogen rich gas from a source of hydrocarbon fuel. A vapor of the hydrocarbon fuel and steam is brought in contact with a two-part catalyst having a dehydrogenation powder portion and an oxide-ion conducting powder portion at a temperature not less than about 770.degree.C. for a time sufficient to generate the hydrogen rich. The H.sub.2 content of the hydrogen gas is greater than about 70 percent by volume. The dehydrogenation portion of the catalyst includes a group VIII metal, and the oxide-ion conducting portion is selected from a ceramic oxide from the group crystallizing in the fluorite or perovskite structure and mixtures thereof. The oxide-ion conducting portion of the catalyst is a ceramic powder of one or more of ZrO.sub.2, CeO.sub.2, Bi.sub.2 O.sub.3, (BiVO).sub.4, and LaGaO.sub.3.

  12. Intermetallic nanoparticles

    SciTech Connect (OSTI)

    Singh, Dileep; Yusufoglu, Yusuf; Timofeeva, Elena; Routbort, Jules L.

    2015-11-20

    A process for preparing intermetallic nanoparticles of two or more metals is provided. In particular, the process includes the steps: a) dispersing nanoparticles of a first metal in a solvent to prepare a first metal solution, b) forming a reaction mixture with the first metal solution and a reducing agent, c) heating the reaction mixture to a reaction temperature; and d) adding a second metal solution containing a salt of a second metal to the reaction mixture. During this process, intermetallic nanoparticles, which contain a compound with the first and second metals are formed. The intermetallic nanoparticles with uniform size and a narrow size distribution is also provided. An electrochemical device such as a battery with the intermetallic nanoparticles is also provided.

  13. Intermetallic nanoparticles

    DOE Patents [OSTI]

    Singh, Dileep; Yusufoglu, Yusuf; Timofeeva, Elena; Routbort, Jules

    2015-07-14

    A process for preparing intermetallic nanoparticles of two or more metals is provided. In particular, the process includes the steps: a) dispersing nanoparticles of a first metal in a solvent to prepare a first metal solution, b) forming a reaction mixture with the first metal solution and a reducing agent, c) heating the reaction mixture to a reaction temperature; and d) adding a second metal solution containing a salt of a second metal to the reaction mixture. During this process, intermetallic nanoparticles, which contain a compound with the first and second metals are formed. The intermetallic nanoparticles with uniform size and a narrow size distribution is also provided. An electrochemical device such as a battery with the intermetallic nanoparticles is also provided.

  14. Development of GREET Catalyst Module

    SciTech Connect (OSTI)

    Wang, Zhichao; Benavides, Pahola T.; Dunn, Jennifer B.; Cronauer, Donald C.

    2015-09-01

    In this report, we develop energy and material flows for the production of five different catalysts (tar reforming, alcohol synthesis, Zeolite Socony Mobil-5 [ZSM-5], Mo/Co/ ?-Al2O3, and Pt/ ?-Al2O3) and two chemicals (olivine, dimethyl ether of polyethylene glycol [DEPG]). These compounds and catalysts are now included in the Greenhouse Gases, Regulated Emissions and Energy Use in Transportation (GREET™) catalyst module.

  15. Oxygen-reducing catalyst layer

    DOE Patents [OSTI]

    O'Brien, Dennis P. (Maplewood, MN); Schmoeckel, Alison K. (Stillwater, MN); Vernstrom, George D. (Cottage Grove, MN); Atanasoski, Radoslav (Edina, MN); Wood, Thomas E. (Stillwater, MN); Yang, Ruizhi (Halifax, CA); Easton, E. Bradley (Halifax, CA); Dahn, Jeffrey R. (Hubley, CA); O'Neill, David G. (Lake Elmo, MN)

    2011-03-22

    An oxygen-reducing catalyst layer, and a method of making the oxygen-reducing catalyst layer, where the oxygen-reducing catalyst layer includes a catalytic material film disposed on a substrate with the use of physical vapor deposition and thermal treatment. The catalytic material film includes a transition metal that is substantially free of platinum. At least one of the physical vapor deposition and the thermal treatment is performed in a processing environment comprising a nitrogen-containing gas.

  16. Catalyst systems and uses thereof

    DOE Patents [OSTI]

    Ozkan, Umit S. (Worthington, OH); Holmgreen, Erik M. (Columbus, OH); Yung, Matthew M. (Columbus, OH)

    2012-07-24

    A method of carbon monoxide (CO) removal comprises providing an oxidation catalyst comprising cobalt supported on an inorganic oxide. The method further comprises feeding a gaseous stream comprising CO, and oxygen (O.sub.2) to the catalyst system, and removing CO from the gaseous stream by oxidizing the CO to carbon dioxide (CO.sub.2) in the presence of the oxidation catalyst at a temperature between about 20 to about 200.degree. C.

  17. High Impact Technology (HIT) Catalyst

    Energy Savers [EERE]

    Impact Technology (HIT) Catalyst Images courtesy CREE, True Manufacturing, A.O. Smith, Bernstein Associates, Cambridge Engineering, Alliance Laundry Systems, NREL Commercial...

  18. Mixed Alcohol Synthesis Catalyst Screening

    SciTech Connect (OSTI)

    Gerber, Mark A.; White, James F.; Stevens, Don J.

    2007-09-03

    National Renewable Energy Laboratory (NREL) and Pacific Northwest National Laboratory (PNNL) are conducting research to investigate the feasibility of producing mixed alcohols from biomass-derived synthesis gas (syngas). PNNL is tasked with obtaining commercially available or preparing promising mixed-alcohol catalysts and screening them in a laboratory-scale reactor system. Commercially available catalysts and the most promising experimental catalysts are provided to NREL for testing using a slipstream from a pilot-scale biomass gasifier. From the standpoint of producing C2+ alcohols as the major product, it appears that the rhodium catalyst is the best choice in terms of both selectivity and space-time yield (STY). However, unless the rhodium catalyst can be improved to provide minimally acceptable STYs for commercial operation, mixed alcohol synthesis will involve significant production of other liquid coproducts. The modified Fischer-Tropsch catalyst shows the most promise for providing both an acceptable selectivity to C2+ alcohols and total liquid STY. However, further optimization of the Fischer-Tropsch catalysts to improve selectivity to higher alcohols is highly desired. Selection of a preferred catalyst will likely entail a decision on the preferred coproduct slate. No other catalysts tested appear amenable to the significant improvements needed for acceptable STYs.

  19. Nanoparticles are generated on behalf of the manufacturing

    E-Print Network [OSTI]

    Langendoen, Koen

    batteries, solar cells, fuel cells, catalysts and hydrogen storage materials. Nanoparticles have been. Optimization A team of TU Delft scientists succeeded in developing an optimized spark discharge based method this optimized spark discharge based method is unique concerning purity of the particles produced and its

  20. Oxygen Reduction at Very Low Overpotential on Nanoporous Ag Catalysts

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

    Zhou, Yang; Lu, Qi; Zhuang, Zhongbin; Hutchings, Gregory S.; Kattel, Shyam; Yan, Yushan; Chen, Jingguang G.; Xiao, John Q.; Jiao, Feng

    2015-05-07

    Here we report a monolithic nanoporous Ag (np-Ag) material, synthesized using the dealloying method, as high-performance catalysts for ORR in alkaline media. As shown in Scheme 1, when there is insufficient potential input, the O2 molecules are more likely to rebound off from a planar electrode surface (i.e. bulk polycrystalline metal, films made from nanoparticles or nanowires) before they could be reduced. In contrast, they are more likely to be trapped inside the monolithic nanoporous structure, contacting with catalytic surface for multiple time, which greatly enhances the chance for them to be fully reduced. As a result, the np-Ag catalystmore »is able to achieve an equivalent or better ORR performance than the state-of the-art Pt/C catalyst at low overpotentials, which is most desired in electrochemical energy applications for maximizing efficiency.« less

  1. Bimetallic iron and cobalt incorporated MFI/MCM-41 composite and its catalytic properties

    SciTech Connect (OSTI)

    Li, Baoshan, E-mail: bsli@mail.buct.edu.cn [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China)] [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China); Xu, Junqing [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China)] [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China); Li, Xiao [Shandong Institute of Scientific and Technical Information, Jinan, Shandong 250101 (China)] [Shandong Institute of Scientific and Technical Information, Jinan, Shandong 250101 (China); Liu, Jianjun; Zuo, Shengli [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China)] [State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029 (China); Pan, Zhiyun; Wu, Ziyu [National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029 (China)] [National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029 (China)

    2012-05-15

    Graphical abstract: The formation of FeCo-MFI/MCM-41 composite is based on two steps, the first step of synthesizing the MFI-type proto-zeolite unites under hydrothermal conditions. The second step of assembling these zeolite fragment together new silica and heteroatom source on the CTAB surfactant micelle to synthesize the mesoporous product with hexagonal structure. Highlights: Black-Right-Pointing-Pointer Bimetallic iron and cobalt incorporated MFI/MCM-41 composite was prepared using templating method. Black-Right-Pointing-Pointer FeCo-MFI/MCM-41 composite simultaneously possessed two kinds of meso- and micro-porous structures. Black-Right-Pointing-Pointer Iron and cobalt ions incorporated into the silica framework with tetrahedral coordination. -- Abstract: The MFI/MCM-41 composite material with bimetallic Fe and Co incorporation was prepared using templating method via a two-step hydrothermal crystallization procedure. The obtained products were characterized by a series of techniques including powder X-ray diffraction, N{sub 2} sorption, transmission electron microscopy, scanning electron microscope, H{sub 2} temperature programmed reduction, thermal analyses, and X-ray absorption fine structure spectroscopy of the Fe and Co K-edge. The catalytic properties of the products were investigated by residual oil hydrocracking reactions. Characterization results showed that the FeCo-MFI/MCM-41 composite simultaneously possessed two kinds of stable meso- and micro-porous structures. Iron and cobalt ions were incorporated into the silicon framework, which was confirmed by H{sub 2} temperature programmed reduction and X-ray absorption fine structure spectroscopy. This composite presented excellent activities in hydrocracking of residual oil, which was superior to the pure materials of silicate-1/MCM-41.

  2. 1 Core/Shell Au/CuPt Nanoparticles and Their Dual Electrocatalysis for 2 Both Reduction and Oxidation Reactions

    E-Print Network [OSTI]

    Wang, Zhong L.

    1 Core/Shell Au/CuPt Nanoparticles and Their Dual Electrocatalysis for 2 Both Reduction usage but also improves the 15 stability of the Au/CuPt catalyst for fuel cell reactions. The results nanoparticle catalysis for many different chemical reactions. 18 INTRODUCTION 19 Coupling fuel oxidation

  3. Refiners Increasingly Employing Catalyst Regeneration as Alternative...

    Open Energy Info (EERE)

    million by the end of 2019. Refiners Benefit from Catalyst Regeneration Technology via Price Reductions and Lower Maintenance Costs The catalyst regeneration technology is the...

  4. High Impact Technology Catalyst: Technology Deployment Strategies...

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

    High Impact Technology Catalyst: Technology Deployment Strategies High Impact Technology Catalyst: Technology Deployment Strategies The Energy Department released the High Impact...

  5. Nanoscale Chemical Imaging of a Working Catalyst

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

    of chemical processes. Watching Catalysts at Work Catalysts-substances that speed up chemical reactions without themselves being consumed-are essential to the production of...

  6. Bifunctional Catalysts for the Selective Catalytic Reduction...

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

    as Reductants Bifunctional Catalysts for the Selective Catalytic Reduction of NO by Hydrocarbons Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx...

  7. Nanoscale Chemical Imaging of a Working Catalyst

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

    Nanoscale Chemical Imaging of a Working Catalyst Print The heterogeneous catalysts used in most chemical processes typically consist of nanoscale metal or metal oxide particles...

  8. Characterization of Catalysts for Aftertreatment and Biomass...

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

    Catalysts for Aftertreatment and Biomass-derived Fuels: Success Stories from the High Temperature Materials Laboratory (HTML) User Program Characterization of Catalysts for...

  9. Transition metal sulfide loaded catalyst

    DOE Patents [OSTI]

    Maroni, V.A.; Iton, L.E.; Pasterczyk, J.W.; Winterer, M.; Krause, T.R.

    1994-04-26

    A zeolite-based catalyst is described for activation and conversion of methane. A zeolite support includes a transition metal (Mo, Cr or W) sulfide disposed within the micropores of the zeolite. The catalyst allows activation and conversion of methane to C[sub 2]+ hydrocarbons in a reducing atmosphere, thereby avoiding formation of oxides of carbon.

  10. Transition metal sulfide loaded catalyst

    DOE Patents [OSTI]

    Maroni, Victor A. (Naperville, IL); Iton, Lennox E. (Downers Grove, IL); Pasterczyk, James W. (Westmont, IL); Winterer, Markus (Westmont, IL); Krause, Theodore R. (Lisle, IL)

    1994-01-01

    A zeolite based catalyst for activation and conversion of methane. A zeolite support includes a transition metal (Mo, Cr or W) sulfide disposed within the micropores of the zeolite. The catalyst allows activation and conversion of methane to C.sub.2 + hydrocarbons in a reducing atmosphere, thereby avoiding formation of oxides of carbon.

  11. Doped palladium containing oxidation catalysts

    DOE Patents [OSTI]

    Mohajeri, Nahid

    2014-02-18

    A supported oxidation catalyst includes a support having a metal oxide or metal salt, and mixed metal particles thereon. The mixed metal particles include first particles including a palladium compound, and second particles including a precious metal group (PMG) metal or PMG metal compound, wherein the PMG metal is not palladium. The oxidation catalyst may also be used as a gas sensor.

  12. Hydroprocessing catalysts see tough service

    SciTech Connect (OSTI)

    Not Available

    1985-03-25

    Hydrotreating catalysts are the refining industry's major weapon in making good products from marginal oils. The employment and regeneration of these catalysts are the primary topics of this second abstract taken from the transcript of the National Petroleum Refiners Association's most recent question and answer session.

  13. Precision Nanoparticles

    ScienceCinema (OSTI)

    John Hemminger

    2010-01-08

    A revolutionary technology that efficiently produces nanoparticles in uniform and prescribed sizes (1-100 nanometers) using supercritical fluids. INL researcher Robert Fox was joined by Idaho State University researchers Rene Rodriquez and Joshua Pak in d

  14. Deactivation of methanol synthesis catalysts

    SciTech Connect (OSTI)

    Roberts, G.W.; Brown, D.M.; Hsiung, T.H.; Lewnard, J.J. (Air Products and Chemicals, Inc., Allentown, PA (United States))

    1993-08-01

    A novel methanol synthesis process, the liquid-phase methanol (LPMEOH) process, has been developed and scaled up to a nominal 380 kg/h (10 ton/day) pilot plant. The process is based on a gas-sparged slurry reactor instead of a conventional, fixed-bed reactor. The use of slurry reactors, which are essentially gradientless, greatly facilitated the interpretation and quantification of catalyst deactivation phenomena. With a poison-free, CO-rich feedstream, the rate of deactivation of the Cu/ZnO catalyst increased rapidly with temperature. At constant temperature, in the absence of poisons, the decline with time in the rate constant for methanol synthesis correlated with the loss of BET surface area. Iron carbonyl, nickel carbonyl, and carbonyl sulfide are severe and highly specific poisons for methanol-synthesis catalyst. There was a linear relationship between the catalyst activity loss and the concentration of metal or sulfur on the catalyst.

  15. Supported molten-metal catalysts

    DOE Patents [OSTI]

    Datta, Ravindra (Iowa City, IA); Singh, Ajeet (Iowa City, IA); Halasz, Istvan (Iowa City, IA); Serban, Manuela (Iowa City, IA)

    2001-01-01

    An entirely new class of catalysts called supported molten-metal catalysts, SMMC, which can replace some of the existing precious metal catalysts used in the production of fuels, commodity chemicals, and fine chemicals, as well as in combating pollution. SMMC are based on supporting ultra-thin films or micro-droplets of the relatively low-melting (<600.degree. C.), inexpensive, and abundant metals and semimetals from groups 1, 12, 13, 14, 15 and 16, of the periodic table, or their alloys and intermetallic compounds, on porous refractory supports, much like supported microcrystallites of the traditional solid metal catalysts. It thus provides orders of magnitude higher surface area than is obtainable in conventional reactors containing molten metals in pool form and also avoids corrosion. These have so far been the chief stumbling blocks in the application of molten metal catalysts.

  16. Dynamic Monte Carlo Simulations of the Oxygen Electroreduction Reaction on a Bimetallic Surface 

    E-Print Network [OSTI]

    Wood, Adam; Balbuena, Perla

    2006-07-11

    Platinum and platinum alloy surfaces are used as catalysts to promote the reduction of oxygen, one of the reactions used to generate electrical energy in low temperature fuel cells, which are sought as promissory clean power sources...

  17. X-ray Photoelectron Spectroscopy and Kinetic Study: Pt-Group Metals and Bimetallic Surfaces 

    E-Print Network [OSTI]

    Gath, Kerrie K.

    2010-01-14

    Pt-group metals were some of the first metals to be studied as catalysts for industrial use. The goal of these studies was to ascertain a fundamental understanding of CO oxidation and acetylene cyclotrimerization reactions ...

  18. Hydrocracking catalysts from coals

    SciTech Connect (OSTI)

    Farcasiu, M.; Petrosius, S.C.; Pladner, E. [USDOE Pittsburgh Energy Technology Center, PA (United States); Derbyshire, F.; Jagtoyen, M. [Univ. of Kentucky, Lexington, KY (United States). Center for Applied Energy Research

    1994-12-31

    In previous work at PETC it was shown that carbon blacks and carbonized polymers could be active and selective catalysts in hydrocracking reactions of interest for fossil fuels processing. Work at CAER for the production of various activated carbons from coals have shown that the properties of the materials could be varied if they are produced under different conditions. The authors will report work to optimize the catalytic properties of some coal based carbon materials prepared at CAER. One of the most promising materials for this purpose is obtained from an Illinois bituminous coal. The procedure hydroxide solution with coal and reacting in two stages; (1) heat treatment of the solution at 75 C under nitrogen for one hour followed by drying and (2) heat treatment at 400--1,100 C followed by leaching to remove KOH. The product was extensively characterized and its catalytic activity was measured. The catalytic activity of some of the materials is comparable with other, more expensive carbon materials. The catalysts have potential use in upgrading petroleum heavy ends and coal liquefaction.

  19. Stereospecific olefin polymerization catalysts

    DOE Patents [OSTI]

    Bercaw, J.E.; Herzog, T.A.

    1998-01-13

    A metallocene catalyst system is described for the polymerization of {alpha}-olefins to yield stereospecific polymers including syndiotactic, and isotactic polymers. The catalyst system includes a metal and a ligand of the formula shown wherein: R{sup 1}, R{sup 2}, and R{sup 3} are independently selected from the group consisting of hydrogen, C{sub 1} to C{sub 10} alkyl, 5 to 7 membered cycloalkyl, which in turn may have from 1 to 3 C{sub 1} to C{sub 10} alkyls as a substituent, C{sub 6} to C{sub 15} aryl or arylalkyl in which two adjacent radicals may together stand for cyclic groups having 4 to 15 carbon atoms which in turn may be substituted, or Si(R{sup 8}){sub 3} where R{sup 8} is selected from the group consisting of C{sub 1} to C{sub 10} alkyl, C{sub 6} to C{sub 15} aryl or C{sub 3} to C{sub 10} cycloalkyl; R{sup 4} and R{sup 6} are substituents both having van der Waals radii larger than the van der Waals radii of groups R{sup 1} and R{sup 3}; R{sup 5} is a substituent having a van der Waals radius less than about the van der Waals radius of a methyl group; E{sup 1}, E{sup 2} are independently selected from the group consisting of Si(R{sup 9}){sub 2}, Si(R{sup 9}){sub 2}--Si(R{sup 9}){sub 2}, Ge(R{sup 9}){sub 2}, Sn(R{sup 9}){sub 2}, C(R{sup 9}){sub 2}, C(R{sup 9}){sub 2}--C(R{sup 9}){sub 2}, where R{sup 9} is C{sub 1} to C{sub 10} alkyl, C{sub 6} to C{sub 15} aryl or C{sub 3} to C{sub 10} cycloalkyl; and the ligand may have C{sub S} or C{sub 1}-symmetry. Preferred metals are selected from the group consisting of group III, group IV, group V or lanthanide group elements. The catalysts are used to prepare stereoregular polymers including polypropylene from {alpha}-olefin monomers.

  20. Stereospecific olefin polymerization catalysts

    DOE Patents [OSTI]

    Bercaw, John E. (Pasadena, CA); Herzog, Timothy A. (Pasadena, CA)

    1998-01-01

    A metallocene catalyst system for the polymerization of .alpha.-olefins to yield stereospecific polymers including syndiotactic, and isotactic polymers. The catalyst system includes a metal and a ligand of the formula ##STR1## wherein: R.sup.1, R.sup.2, and R.sup.3 are independently selected from the group consisting of hydrogen, C.sub.1 to C.sub.10 alkyl, 5 to 7 membered cycloalkyl, which in turn may have from 1 to 3 C.sub.1 to C.sub.10 alkyls as a substituent, C.sub.6 to C.sub.15 aryl or arylalkyl in which two adjacent radicals may together stand for cyclic groups having 4 to 15 carbon atoms which in turn may be substituted, or Si(R.sup.8).sub.3 where R.sup.8 is selected from the group consisting of C.sub.1 to C.sub.10 alkyl, C.sub.6 to C.sub.15 aryl or C.sub.3 to C.sub.10 cycloalkyl; R.sup.4 and R.sup.6 are substituents both having van der Waals radii larger than the van der Waals radii of groups R.sup.1 and R.sup.3 ; R.sup.5 is a substituent having a van der Waals radius less than about the van der Waals radius of a methyl group; E.sup.1, E.sup.2 are independently selected from the group consisting of Si(R.sup.9).sub.2, Si(R.sup.9).sub.2 --Si(R.sup.9).sub.2, Ge(R.sup.9).sub.2, Sn(R.sup.9).sub.2, C(R.sup.9).sub.2, C(R.sup.9).sub.2 --C(R.sup.9).sub.2, where R.sup.9 is C.sub.1 to C.sub.10 alkyl, C.sub.6 to C.sub.15 aryl or C.sub.3 to C.sub.10 cycloalkyl; and the ligand may have C.sub.S or C.sub.1 -symmetry. Preferred metals are selected from the group consisting of group III, group IV, group V or lanthanide group elements. The catalysts are used to prepare stereoregular polymers including polypropylene from .alpha.-olefin monomers.

  1. Catalyst deactivation in residue hydrocracking

    SciTech Connect (OSTI)

    Oballa, M.C.; Wong, C.; Krzywicki, A. [Novacor Research and Technology Corp., Calgary, Alberta (Canada)

    1994-12-31

    The existence of a computer-controlled bench scale hydrocracking units at the authors site has made cheaper the non-stop running of experiments for long periods of time. It was, therefore possible to show, at minimal costs, when three hydrocracking catalysts in service reach their maximum lifetime. Different parameters which are helpful for catalyst life and activity predictions were calculated, e.g., relative catalyst age and the effectiveness factor. Experimental results compared well with model, giving them the minimum and maximum catalyst lifetime, as well as the deactivation profile with regard to sulfur and metals removal. Reaction rate constants for demetallization and desulfurization were also determined. Six commercial catalysts were evaluated at short term runs and the three most active were used for long term runs. Out of three catalysts tested for deactivation at long term runs, it was possible to choose one whose useful life was higher than the others. All runs were carried out in a Robinson-Mahoney continuous flow stirred tank reactor, using 50/50 volumetric mixture of Cold Lake/Lloydminster atmospheric residue and NiMo/Al{sub 2}O{sub 3} catalyst.

  2. Textured catalysts, methods of making textured catalysts, and methods of catalyzing reactions conducted in hydrothermal conditions

    DOE Patents [OSTI]

    Werpy, Todd [West Richland, WA; Wang, Yong [Richland, WA

    2003-12-30

    A textured catalyst having a hydrothermally-stable support, a metal oxide and a catalyst component is described. Methods of conducting aqueous phase reactions that are catalyzed by a textured catalyst are also described. The invention also provides methods of making textured catalysts and methods of making chemical products using a textured catalyst.

  3. Chalcogen catalysts for polymer electrolyte fuel cell

    DOE Patents [OSTI]

    Alonso-Vante, Nicolas (Buxerolles, FR); Zelenay, Piotr (Los Alamos, NM); Choi, Jong-Ho (Los Alamos, NM); Wieckowski, Andrzej (Champaign, IL); Cao, Dianxue (Urbana, IL)

    2009-09-15

    A methanol-tolerant cathode catalyst and a membrane electrode assembly for fuel cells that includes such a cathode catalyst. The cathode catalyst includes a support having at least one transition metal in elemental form and a chalcogen disposed on the support. Methods of making the cathode catalyst and membrane electrode assembly are also described.

  4. Chalcogen catalysts for polymer electrolyte fuel cell

    DOE Patents [OSTI]

    Zelenay, Piotr (Los Alamos, NM); Choi, Jong-Ho (Los Alamos, NM); Alonso-Vante, Nicolas (France, FR); Wieckowski, Andrzej (Champaign, IL); Cao, Dianxue (Urbana, IL)

    2010-08-24

    A methanol-tolerant cathode catalyst and a membrane electrode assembly for fuel cells that includes such a cathode catalyst. The cathode catalyst includes a support having at least one transition metal in elemental form and a chalcogen disposed on the support. Methods of making the cathode catalyst and membrane electrode assembly are also described.

  5. New hydrocracking catalysts increase throughput, run length

    SciTech Connect (OSTI)

    Huizinga, T. [Shell Internationale Petroleum Mij., The Hague (Netherlands); Theunissen, J.M.H. [Rayong Refinery Co. Ltd., Rayong (Thailand); Minderhoud, H.; Veen, R. van [Koninklijke/Shell-Lab., Amsterdam (Netherlands)

    1995-06-26

    An improved, second-stage hydrocracking catalyst has been developed by combining stabilized Y zeolites with amorphous silica alumina cracking components. A commercial application of this catalyst, along with a new, first-stage zeolitic hydrocracking catalyst, resulted in increased unit throughput and cycle length. The paper discusses the hydrocracking process, first-stage catalysts, second-stage catalysts, hydrogenation process, commercial results, and product properties.

  6. Secret Lives of Catalysts Revealed

    ScienceCinema (OSTI)

    Miquel Salmeron and Gabor Somorjai

    2010-01-08

    Miquel Salmeron and Gabor Somorjai of Berkeley Lab's Materials Sciences Division discuss the first-ever glimpse of nanoscale catalysts in action. More information: http://newscenter.lbl.gov/press-relea...

  7. SunShot Catalyst Program

    Broader source: Energy.gov [DOE]

    The SunShot Catalyst program is actively reaching out to communities of software and business innovators across the country to find individuals with startup ideas to make solar faster, more...

  8. Rh-Based Mixed Alcohol Synthesis Catalysts: Characterization and Computational Report

    SciTech Connect (OSTI)

    Albrecht, Karl O.; Glezakou, Vassiliki Alexandra; Rousseau, Roger J.; Engelhard, Mark H.; Varga, Tamas; Colby, Robert J.; Jaffe, John E.; Li, Xiaohong S.; Mei, Donghai; Windisch, Charles F.; Kathmann, Shawn M.; Lemmon, Teresa L.; Gray, Michel J.; Hart, Todd R.; Thompson, Becky L.; Gerber, Mark A.

    2013-08-01

    The U.S. Department of Energy is conducting a program focused on developing a process for the conversion of biomass to bio-based fuels and co-products. Biomass-derived syngas is converted thermochemically within a temperature range of 240 to 330°C and at elevated pressure (e.g., 1200 psig) over a catalyst. Ethanol is the desired reaction product, although other side compounds are produced, including C3 to C5 alcohols; higher (i.e., greater than C1) oxygenates such as methyl acetate, ethyl acetate, acetic acid and acetaldehyde; and higher hydrocarbon gases such as methane, ethane/ethene, propane/propene, etc. Saturated hydrocarbon gases (especially methane) are undesirable because they represent a diminished yield of carbon to the desired ethanol product and represent compounds that must be steam reformed at high energy cost to reproduce CO and H2. Ethanol produced by the thermochemical reaction of syngas could be separated and blended directly with gasoline to produce a liquid transportation fuel. Additionally, higher oxygenates and unsaturated hydrocarbon side products such as olefins also could be further processed to liquid fuels. The goal of the current project is the development of a Rh-based catalyst with high activity and selectivity to C2+ oxygenates. This report chronicles an effort to characterize numerous supports and catalysts to identify particular traits that could be correlated with the most active and/or selective catalysts. Carbon and silica supports and catalysts were analyzed. Generally, analyses provided guidance in the selection of acceptable catalyst supports. For example, supports with high surface areas due to a high number of micropores were generally found to be poor at producing oxygenates, possibly because of mass transfer limitations of the products formed out of the micropores. To probe fundamental aspects of the complicated reaction network of CO with H2, a computational/ theoretical investigation using quantum mechanical and ab initio molecular dynamics calculations was initiated in 2009. Computational investigations were performed first to elucidate understanding of the nature of the catalytically active site. Thermodynamic calculations revealed that Mn likely exists as a metallic alloy with Rh in Rh-rich environments under reducing conditions at the temperatures of interest. After determining that reduced Rh-Mn alloy metal clusters were in a reduced state, the activation energy barriers of numerous transition state species on the catalytically active metal particles were calculated to compute the activation barriers of several reaction pathways that are possible on the catalyst surface. Comparison of calculations with a Rh nanoparticle versus a Rh-Mn nanoparticle revealed that the presence of Mn enabled the reaction pathway of CH with CO to form an adsorbed CHCO species, which was a precursor to C2+ oxygenates. The presence of Mn did not have a significant effect on the rate of CH4 production. Ir was observed during empirical catalyst screening experiments to improve the activity and selectivity of Rh-Mn catalysts. Thus, the addition of Ir to the Rh-Mn nanoparticles also was probed computationally. Simulations of Rh-Mn-Ir nanoparticles revealed that, with sufficient Ir concentrations, the Rh, Mn and Ir presumably would be well mixed within a nanoparticle. Activation barriers were calculated for Rh-Mn-Ir nanoparticles for several C-, H-, and O-containing transitional species on the nanoparticle surface. It was found that the presence of Ir opened yet another reactive pathway whereby HCO is formed and may undergo insertion with CHx surface moieties. The reaction pathway opened by the presence of Ir is in addition to the CO + CH pathway opened by the presence of Mn. Similar to Mn, the presence of Ir was not found to not affect the rate of CH4 production.

  9. Ultra-High Resolution Electron Microscopy for Catalyst Characterizatio...

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

    Documents & Publications Ultra-High Resolution Electron Microscopy for Catalyst Characterization Ultra-high Resolution Electron Microscopy for Catalyst Characterization Catalyst...

  10. Rational Catalyst Design Applied to Development of Advanced Oxidation...

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

    Rational Catalyst Design Applied to Development of Advanced Oxidation Catalysts for Diesel Emission Control Rational Catalyst Design Applied to Development of Advanced Oxidation...

  11. Overcoming Hydrocarbon Inhibition on Pd-based Diesel Oxidation Catalysts with Rational Catalyst Design Approach

    Broader source: Energy.gov [DOE]

    Discusses results of a project focused on overcoming hydrocarbon inhibition on Pd-based diesel oxidation catalysts by using a rational catalyst design approach.

  12. Monodisperse Platinum and Rhodium Nanoparticles as Model Heterogeneous Catalysts

    E-Print Network [OSTI]

    Coble, Inger M

    2008-01-01

    respectively. 7.2.2 CO Oxidation Catalytic reactions weresurface for CO oxidation under catalytic conditions for1 . 8.2.3 CO Oxidation Measurements Catalytic measurements

  13. Biomimetic Catalysts of Graphene Conjugates and Palladium Nanoparticles

    E-Print Network [OSTI]

    Xue, Teng

    2014-01-01

    long- lasting antithrombotic coating for blood contactingto develop an antithrombotic coating on biomedical deviceslong-lasting antithrombotic coating for blood contacting

  14. Hollow Nanoparticles as Active and Durable Catalysts - Energy Innovation

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration would likeUniverse (JournalvivoHigh energyHighland View school4-TP59.01vacuumEnergy

  15. Catalyst suppliers further consolidate business units

    SciTech Connect (OSTI)

    Rhodes, A.K.

    1993-10-11

    The petroleum-refining catalyst industry sustained significant reorganization in 1993. A joint venture between two previous competitors and the consolidated of two sister companies reflect general trends in the global market-place. The Journal's latest survey lists more than 820 unique catalysts. This reduction of some 220 catalysts since the last complete catalyst compilation is partially the result of the deletion of some of the more specialized catalysts from this year's survey. Other factors contributing to this decrease include industry rationalization and the listing of catalyst families instead of individual products--especially in the fluid catalytic cracking category. The Journal's international refining-catalyst compilation lists catalysts manufactured for all major catalytic refinery processes by essentially all the world's petroleum catalyst producers and suppliers. The objective of the survey is two-fold: first, to list each catalyst by its specific designation or supplier identification in its process application category (for instance, hydrocracking); and second, to differentiate each catalyst from the others in that category. These differentiations can be made in terms of either the catalyst's application (for example, feedstock characteristics) or its physical characteristics (for instance, particle size or activity). The compilation is designed to provide a ready reference for both refiners and catalyst manufacturers. In the process, it may also help sort out the sometimes confusing nomenclature used to describe these catalysts.

  16. Multilayered and complex nanoparticle architectures through plasma synthesis

    SciTech Connect (OSTI)

    Phillips, Jonathan; Wakeland, Stephen; Cui, Yuehua; Knapp, Angela; Richard, Monique; Luhrs, Claudia

    2009-01-01

    Using the Aerosol Through Plasma (ATP) method in conjunction with simple chemical techniques a variety of complex and novel nanoparticle architectures were created. A TP was used to make metal-core/carbon shell nanoparticles (ca. 50 nm diameter) of SnlCarbon and AI/Carbon. These have, respectively, potential for application as battery anode (for hybrid and electric vehicles) and high energy fuel In one example of post processing, the Sn-core/carbon-shell material is treated in acidic solution and yields a true nano-sized hollow carbon shell. These shells have potential application as catalyst supports, gas storage, a neutral buoyancy material for applications as varied as proppants, and slow release capsules for pharmaceutical or agricultural applications. A different set of post-A-T-P processes were used to make three layer nanoparticles with a metal core, graphite inner shell and ceramic outer shell. This method extends the range of achievable nanoparticles architectures, hence enabling new applications.

  17. Catalyst for coal liquefaction process

    DOE Patents [OSTI]

    Huibers, Derk T. A. (Pennington, NJ); Kang, Chia-Chen C. (Princeton, NJ)

    1984-01-01

    An improved catalyst for a coal liquefaction process; e.g., the H-Coal Process, for converting coal into liquid fuels, and where the conversion is carried out in an ebullated-catalyst-bed reactor wherein the coal contacts catalyst particles and is converted, in addition to liquid fuels, to gas and residual oil which includes preasphaltenes and asphaltenes. The improvement comprises a catalyst selected from the group consisting of the oxides of nickel molybdenum, cobalt molybdenum, cobalt tungsten, and nickel tungsten on a carrier of alumina, silica, or a combination of alumina and silica. The catalyst has a total pore volume of about 0.500 to about 0.900 cc/g and the pore volume comprises micropores, intermediate pores and macropores, the surface of the intermediate pores being sufficiently large to convert the preasphaltenes to asphaltenes and lighter molecules. The conversion of the asphaltenes takes place on the surface of micropores. The macropores are for metal deposition and to prevent catalyst agglomeration. The micropores have diameters between about 50 and about 200 angstroms (.ANG.) and comprise from about 50 to about 80% of the pore volume, whereas the intermediate pores have diameters between about 200 and 2000 angstroms (.ANG.) and comprise from about 10 to about 25% of the pore volume, and the macropores have diameters between about 2000 and about 10,000 angstroms (.ANG.) and comprise from about 10 to about 25% of the pore volume. The catalysts are further improved where they contain promoters. Such promoters include the oxides of vanadium, tungsten, copper, iron and barium, tin chloride, tin fluoride and rare earth metals.

  18. Material property evaluations of bimetallic welds, stainless steel saw fusion lines, and materials affected by dynamic strain aging

    SciTech Connect (OSTI)

    Rudland, D.; Scott, P.; Marschall, C.; Wilkowski, G. [Battelle Memorial Institute, Columbus, OH (United States)

    1997-04-01

    Pipe fracture analyses can often reasonably predict the behavior of flawed piping. However, there are material applications with uncertainties in fracture behavior. This paper summarizes work on three such cases. First, the fracture behavior of bimetallic welds are discussed. The purpose of the study was to determine if current fracture analyses can predict the response of pipe with flaws in bimetallic welds. The weld joined sections of A516 Grade 70 carbon steel to F316 stainless steel. The crack was along the carbon steel base metal to Inconel 182 weld metal fusion line. Material properties from tensile and C(T) specimens were used to predict large pipe response. The major conclusion from the work is that fracture behavior of the weld could be evaluated with reasonable accuracy using properties of the carbon steel pipe and conventional J-estimation analyses. However, results may not be generally true for all bimetallic welds. Second, the toughness of austenitic steel submerged-arc weld (SAW) fusion lines is discussed. During large-scale pipe tests with flaws in the center of the SAW, the crack tended to grow into the fusion line. The fracture toughness of the base metal, the SAW, and the fusion line were determined and compared. The major conclusion reached is that although the fusion line had a higher initiation toughness than the weld metal, the fusion-line J-R curve reached a steady-state value while the SAW J-R curve increased. Last, carbon steel fracture experiments containing circumferential flaws with periods of unstable crack jumps during steady ductile tearing are discussed. These instabilities are believed to be due to dynamic strain aging (DSA). The paper discusses DSA, a screening criteria developed to predict DSA, and the ability of the current J-based methodologies to assess the effect of these crack instabilities. The effect of loading rate on the strength and toughness of several different carbon steel pipes at LWR temperatures is also discussed.

  19. Regeneration of Hydrotreating and FCC Catalysts

    SciTech Connect (OSTI)

    CM Wai; JG Frye; JL Fulton; LE Bowman; LJ Silva; MA Gerber

    1999-09-30

    Hydrotreating, hydrocracking, and fluid catalytic cracking (FCC) catalysts are important components of petroleum refining processes. Hydrotreating and hydrocracking catalysts are used to improve the yield of high-quality light oil fractions from heavier crude oil and petroleum feedstocks containing high levels of impurities. FCC catalysts improve the yield of higher octane gasoline from crude oil. Residuum hydrotreating and cracking catalysts are susceptible to irreversible deactivation caused by adsorption of sulfur and by metals impurities, such as vanadium and nickel. The gradual buildup of these impurities in a hydrotreating catalyst eventually plugs the pores and deactivates it. Nickel and vanadium adversely affect the behavior of cracking catalysts, reducing product yield and quality. Replacing deactivated catalysts represents a significant cost in petroleum refining. Equally important are the costs and potential liabilities associated with treating and disposing spent catalysts. For example, recent US Environmental Protection Agency rulings have listed spent hydrotreating and hydrorefining catalysts as hazardous wastes. FCC catalysts, though more easily disposed of as road-base or as filler in asphalt and cement, are still an economic concern mainly because of the large volumes of spent catalysts generated. New processes are being considered to increase the useful life of catalysts or for meeting more stringent disposal requirements for spent catalysts containing metals. This report discusses a collaborative effort between Pacific Northwest National Laboratory (PNNL) and Phillips Petroleum, Inc., to identify promising chemical processes for removing metals adhered to spent hydrodesulfurization (HDS, a type of hydrotreating catalyst) and FCC catalysts. This study, conducted by PNNL, was funded by the US Department of Energy's Bartlesville Project Office. Fresh and spent catalysts were provided by Phillips Petroleum. The FCC catalyst was a rare-earth exchanged Y zeolite in a silica-alumina matrix. X-ray fluorescence analyses showed that the rare earths used in preparing the catalysts were a mixture of lanthanum and cerium. Antimony found in the spent catalyst was added during operation of the FCC unit as a way to suppress the adverse effects of deposited nickel. The fresh HDS samples consisted of sulfided nickel and molybdenum on an alumina support. The spent catalyst showed nearly 10% vanadium on the catalyst and a modest increase in nickel and sulfur on the catalyst as a result of operations. Hydrocracking catalysts were not available for this study.

  20. Ultra-High Resolution Electron Microscopy for Catalyst Characterizatio...

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

    Documents & Publications Ultra-High Resolution Electron Microscopy for Catalyst Characterization Ultra-high Resolution Electron Microscopy for Catalyst Characterization...

  1. Catalysts for carbon and coal gasification

    DOE Patents [OSTI]

    McKee, Douglas W. (Burnt Hills, NY); Spiro, Clifford L. (Scotia, NY); Kosky, Philip G. (Schenectady, NY)

    1985-01-01

    Catalyst for the production of methane from carbon and/or coal by means of catalytic gasification. The catalyst compostion containing at least two alkali metal salts. A particulate carbonaceous substrate or carrier is used.

  2. Catalyst containing oxygen transport membrane

    DOE Patents [OSTI]

    Christie, Gervase Maxwell; Wilson, Jamie Robyn; van Hassel, Bart Antonie

    2012-12-04

    A composite oxygen transport membrane having a dense layer, a porous support layer and an intermediate porous layer located between the dense layer and the porous support layer. Both the dense layer and the intermediate porous layer are formed from an ionic conductive material to conduct oxygen ions and an electrically conductive material to conduct electrons. The porous support layer has a high permeability, high porosity, and a high average pore diameter and the intermediate porous layer has a lower permeability and lower pore diameter than the porous support layer. Catalyst particles selected to promote oxidation of a combustible substance are located in the intermediate porous layer and in the porous support adjacent to the intermediate porous layer. The catalyst particles can be formed by wicking a solution of catalyst precursors through the porous support toward the intermediate porous layer.

  3. Biomass Catalyst Characterization Laboratory (Fact Sheet)

    SciTech Connect (OSTI)

    Not Available

    2011-07-01

    This fact sheet provides information about Biomass Catalyst Characterization Laboratory (BCCL) capabilities and applications at NREL's National Bioenergy Center.

  4. Water Uptake in PEMFC Catalyst Layers

    E-Print Network [OSTI]

    Gunterman, Haluna P.

    2013-01-01

    of California. Water Uptake in PEMFC Catalyst Layers H. P.membrane fuel cells (PEMFC) is rife with challenges.

  5. Attrition resistant catalysts and sorbents based on heavy metal poisoned FCC catalysts

    DOE Patents [OSTI]

    Gangwal, S.; Jothimurugesan, K.

    1999-07-27

    A heavy metal poisoned, spent FCC catalyst is treated by chemically impregnating the poisoned catalyst with a new catalytic metal or metal salt to provide an attrition resistant catalyst or sorbent for a different catalytic or absorption process, such as catalysts for Fischer-Tropsh Synthesis, and sorbents for removal of sulfur gases from fuel gases and flue-gases. The heavy metal contaminated FCC catalyst is directly used as a support for preparing catalysts having new catalytic properties and sorbents having new sorbent properties, without removing or passivating the heavy metals on the spent FCC catalyst as an intermediate step.

  6. Two-catalyst hydrocracking process

    SciTech Connect (OSTI)

    Kukes, S.G.; Gutberlet, L.C.; Hensley, A.L.

    1990-09-25

    This patent describes a process for hydrocracking a hydrocarbon feedstock with hydrogen at hydrocracking conversion conditions in reaction zones in series. It comprises: contacting the feedstock in a first reaction zone with a first reaction zone catalyst comprising a nickel component and tungsten component deposed on a support component consisting essentially of an alumina component and a y zeolite and contacting the effluent from the first reaction zone in a second reaction zone with a second reaction zone catalyst comprising a cobalt component and a molybdenum component deposed on a support component consisting essentially of an alumina component and a y zeolite.

  7. Regeneration of Hydrotreating and FCC Catalysts

    SciTech Connect (OSTI)

    Gerber, Mark A.; Frye, John G.; Bowman, Lawrence E.; Fulton, John L.; Silva, Laura J.; Wai, Chien M.

    1999-09-30

    Hydrotreating, hydrocracking, and fluid catalytic cracking (FCC) catalysts are important components of petroleum refining processes. Hydrotreating and hydrocracking catalysts are used to improve the yield of high-quality light oil fractions from heavier crude oil and petroleum feedstocks containing high levels of impurities. FCC catalysts improve the yield of higher octane gasoline from crude oil.

  8. Middle distillate hydrocracking catalyst and process

    SciTech Connect (OSTI)

    Occelli, M.L.

    1991-06-11

    This patent describes a catalyst composition. It comprises at least one hydrogenation metal component; a layered magnesium silicate; an intercalated clay; and a zeolitic molecular sieve. This patent also describes a catalyst composition wherein the catalyst composition contains a hydrogenation component. It comprises tungsten and a hydrogenation component comprising nickel.

  9. Silver doped catalysts for treatment of exhaust

    DOE Patents [OSTI]

    Park, Paul Worn (Peoria, IL); Hester, Virgil Raymond (Edelstein, IL); Ragle, Christie Susan (Havana, IL); Boyer, Carrie L. (Shiloh, IL)

    2009-06-02

    A method of making an exhaust treatment element includes washcoating a substrate with a slurry that includes a catalyst support material. At least some of the catalyst support material from the slurry may be transferred to the substrate, and silver metal (Ag) is dispersed within the catalyst support material.

  10. Perovskite catalysts for oxidative coupling

    DOE Patents [OSTI]

    Campbell, Kenneth D. (Charleston, WV)

    1991-01-01

    Perovskites of the structure A.sub.2 B.sub.2 C.sub.3 O.sub.10 are useful as catalysts for the oxidative coupling of lower alkane to heavier hydrocarbons. A is alkali metal; B is lanthanide or lanthanum, cerium, neodymium, samarium, praseodymium, gadolinium or dysprosium; and C is titanium.

  11. Perovskite catalysts for oxidative coupling

    DOE Patents [OSTI]

    Campbell, K.D.

    1991-06-25

    Perovskites of the structure A[sub 2]B[sub 2]C[sub 3]O[sub 10] are useful as catalysts for the oxidative coupling of lower alkane to heavier hydrocarbons. A is alkali metal; B is lanthanide or lanthanum, cerium, neodymium, samarium, praseodymium, gadolinium or dysprosium; and C is titanium.

  12. Hydrocracking process using disparate catalyst particle sizes

    SciTech Connect (OSTI)

    Kukes, S.G.; Miller, J.T.; Gutberlet, L.C.; Kelterboro, J.C

    1989-05-30

    This patent describes a process for the hydrocracking of a hydrocarbon feedstock which comprises reacting the feedstock with hydrogen at hydrocracking conversion conditions in a plurality of reaction zones in series containing hydrocracking catalyst wherein at least one of the reaction zones contains a small nominal size hydrocracking catalyst wherein the small nominal size catalyst has a U.S. sieve mesh size ranging from about 10 to about 16, and wherein at least one reaction zone upstream of the reaction zone containing the small nominal size hydrocracking catalyst having a particle size greater than the small nominal size hydrocracking catalyst.

  13. Redox Catalytic Properties of Palladium Nanoparticles: Surfactant and Electron Donor-Acceptor Effects

    E-Print Network [OSTI]

    Wang, Zhong L.

    Redox Catalytic Properties of Palladium Nanoparticles: Surfactant and Electron Donor-0245 Received April 27, 1999. In Final Form: November 10, 1999 Dye reduction catalyzed by palladium catalysts,21-24 and shown that the redox catalytic property of still growing and fully grown palladium

  14. Periodic Inclusion of Room-Temperature-Ferromagnetic Metal Phosphide Nanoparticles in Carbon Nanotubes

    E-Print Network [OSTI]

    Dunin-Borkowski, Rafal E.

    Nanotubes Vincent Jourdain,*,, Edward T. Simpson,§ Matthieu Paillet, Takeshi Kasama,§,| Rafal E. Dunin Form: April 22, 2006 We demonstrate the use of sequential catalytic growth to encapsulate iron, nickel-iron, and iron-cobalt phosphide catalyst nanoparticles periodically along the entire lengths of carbon nanotubes

  15. Magnetron sputtering of gold nanoparticles onto WO3 and activated carbon

    E-Print Network [OSTI]

    Pennycook, Steve

    Magnetron sputtering of gold nanoparticles onto WO3 and activated carbon Gabriel M. Veith a and investigation of two supported gold catalyst systems prepared by magnetron sputtering: Au on WO3 and Au, such as WO3 and carbon, which are generally not accessible using the ubiquitous deposition

  16. Hydrocracking catalyst of improved activity

    SciTech Connect (OSTI)

    Clark, D.E.

    1987-08-25

    A process is described for refining a hydrocarbon feedstock containing organonitrogen components, organosulfur components or a mixture thereof comprising: (a) contacting the feedstock with a hydrogen-containing gas in a hydrotreating zone under hydrotreating conditions in the presence of a hydrotreating catalyst comprising a Group VIB metal component and a Group VIII metal component such that a substantial proportion of the organonitrogen components, organosulfur components or mixture thereof is converted to ammonia, hydrogen sulfide or a mixture thereof; (b) contacting substantially all of the effluent from the hydrotreating zone with molecular hydrogen in a first hydrocracking zone in the presence of a first hydrocracking catalyst comprising a zeolite and a hydrogenation component to produce a hydrocracking product of substantially lower boiling point; (c) separating the hydrocracking product into a higher boiling fraction and a lower boiling fraction; (d) contacting the higher boiling fraction with molecular hydrogen in a second hydrocracking zone under hydrocracking conditions in the presence of a second hydrocracking catalyst to convert the higher boiling fraction into lower boiling products, wherein the second hydrocracking catalyst comprises: (1) a crystalline aluminosilicate Y zeolite having a silica-to-alumina mode ratio of about 6.2 or above, the zeolite having been ion-exchanged with rare earth-containing cations and Group VIII noble metal-containing cations; (2) a porous, inorganic refractory oxide intimately mixed with the zeolite; and (3) between about 4.5 weight percent and about 6.0 weight percent water based on the total weight of the second hydrocracking catalyst.

  17. Catalyst deactivation model for residual oil hydrodesulfurization

    SciTech Connect (OSTI)

    Takatsuka, T.; Higasino, S.; Hirohama, S. [Chiyoda Corporation, Yokohama (Japan)] [and others

    1995-12-31

    Hydrodesulfurization process plays a dominant role in the modern refineries to upgrade residual oil either by removing heterogeneous atoms or by hydrocracking the bottom to distillates products. The practical model is proposed to predict a catalyst life which is the most concern in the process. The catalyst is deactivated in the early stage of the operation by coke deposition on the catalyst active site. The ultimate catalyst life is determined by pore mouth plugging depending on its metal capacity. The phenomena are mathematically described by losses of catalyst surface area and effective diffusivity of feedstock molecules in catalyst pore. The model parameters were collected through the pilot plant tests with different types of catalysts and feedstocks.

  18. Autothermal reforming catalyst having perovskite structure

    DOE Patents [OSTI]

    Krumpel, Michael (Naperville, IL); Liu, Di-Jia (Naperville, IL)

    2009-03-24

    The invention addressed two critical issues in fuel processing for fuel cell application, i.e. catalyst cost and operating stability. The existing state-of-the-art fuel reforming catalyst uses Rh and platinum supported over refractory oxide which add significant cost to the fuel cell system. Supported metals agglomerate under elevated temperature during reforming and decrease the catalyst activity. The catalyst is a perovskite oxide or a Ruddlesden-Popper type oxide containing rare-earth elements, catalytically active firs row transition metal elements, and stabilizing elements, such that the catalyst is a single phase in high temperature oxidizing conditions and maintains a primarily perovskite or Ruddlesden-Popper structure under high temperature reducing conditions. The catalyst can also contain alkaline earth dopants, which enhance the catalytic activity of the catalyst, but do not compromise the stability of the perovskite structure.

  19. Co-generation of electricity and chemicals from propane fuel in solid oxide fuel cells with anode containing nano-bimetallic catalyst

    E-Print Network [OSTI]

    Frenkel, Anatoly

    as an anode in direct propane fueled solid oxide fuel cells (SOFCs). After exposure of the initial single systems. Ó 2014 Elsevier B.V. All rights reserved. 1. Introduction Solid oxide fuel cells (SOFCsCo-generation of electricity and chemicals from propane fuel in solid oxide fuel cells with anode

  20. Ultra-high-performance core–shell structured Ru@Pt/C catalyst prepared by a facile pulse electrochemical deposition method

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

    Chen, Dan; Li, Yuexia; Liao, Shijun; Su, Dong; Song, Huiyu; Li, Yingwei; Yang, Lijun; Li, Can

    2015-08-03

    Core–shell structured catalysts, made by placing either a monolayer or a thin layer of a noble metal on relatively cheap core-metal nanoparticles, are fascinating and promising fuel cell catalysts due to their high utilization of noble metals. Here, we report our development of a core–shell structured catalyst, Ru@Pt/C, generated by a novel and facile pulse electrochemical deposition (PED) approach. We demonstrate that compared with a commercial Pt/C catalyst, this novel catalyst achieves over four times higher mass activity towards the anodic oxidation of methanol, and 3.6 times higher mass activity towards the cathodic reduction of oxygen. Importantly, we find thatmore »the intrinsic activity of Pt in this Ru@Pt/C catalyst is doubled due to the formation of the core–shell structure. The catalyst also shows superior stability: even after 2000 scans, it still retains up to 90% of the peak current. As a result, our findings demonstrate that this novel PED approach is a promising method for preparing high-performance core–shell catalysts for fuel cell applications.« less

  1. In situ XANES Spectroscopic Investigation of the Pre-Reduction of Iron-Based Catalysts for Non-Oxidative Alkane Dehydrogenation

    SciTech Connect (OSTI)

    Huggins, F.; Shen, W; Cprek, N; Shah, N; Marinkovic, N; Huffman, G

    2008-01-01

    The reduction in a methane atmosphere of two as-prepared ferric oxide catalysts for the non-oxidative dehydrogenation of alkanes has been investigated by in situ X-ray absorption near-edge structure (XANES) spectroscopy using a novel X-ray transmission reaction cell. The two catalysts were prepared by different synthesis methods (incipient wetness and nanoparticle impregnation) and were supported on Al-substituted magnesium oxide obtained by decomposition of a synthetic hydrotalcite. The reduction of the ferric oxides by methane was followed by iron XANES spectroscopy at temperatures up to 650 C complemented by a residual gas analyzer (RGA) used to track changes in the product gas. Results showed that the ferric oxides in the two catalysts underwent a stepwise reduction to first ferrous oxide, releasing mainly H{sub 2}O in the case of the nanoparticle catalyst but H{sub 2} and CO in the case of the incipient wetness formulation at temperatures between 200 and 550 C, and then more slowly to metallic iron at higher temperatures. Reaction of the ferrous oxide with the support to form magnesiowstite also occurred in conjunction with the reduction. This in situ investigation confirms that metallic iron is the active catalytic phase for alkane dehydrogenation and that observations of ferric iron in samples investigated at room temperature after reduction and reaction are most likely due to re-oxidation of the iron in the catalyst upon exposure to air rather than incomplete reduction of the original ferric iron in the catalyst.

  2. Airbrushed Nickel Nanoparticles for Large-Area

    SciTech Connect (OSTI)

    Sarac, Mehmet; ANDERSON, BRYAN; Pearce, Ryan; Railsback, Justin; Oni, Adedapo; White, Ryan M.; Hensley, Dale K; Lebeau, James M; Melechko, Anatoli; Tracy, Joseph B

    2013-01-01

    Vertically aligned carbon nanofibers (VACNFs) were grown by plasma-enhanced chemical vapor deposition (PECVD) using Ni nanoparticle (NP) catalysts that were deposited by airbrushing onto Si, Al, Cu, and Ti substrates. Airbrushing is a simple method for depositing catalyst NPs over large areas that is compatible with roll-to-roll processing. The distribution and morphology of VACNFs are affected by the airbrushing parameters and the composition of the metal foil. Highly concentrated Ni NPs in heptane give more uniform distributions than pentane and hexanes, resulting in more uniform coverage of VACNFs. For VACNF growth on metal foils, Si micropowder was added as a precursor for Si-enriched coatings formed in situ on the VACNFs that impart mechanical rigidity. Interactions between the catalyst NPs and the metal substrates impart control over the VACNF morphology. Growth of carbon nanostructures on Cu is particularly noteworthy because the miscibility of Ni with Cu poses challenges for VACNF growth, and carbon nanostructures anchored to Cu substrates are desired as anode materials for Li-ion batteries and for thermal interface materials.

  3. Supercritical/Solid Catalyst (SSC)

    ScienceCinema (OSTI)

    None

    2013-05-28

    INL's patented, continuous-flow Supercritical/Solid Catalyst (SSC) produces the highest ASTM-quality B-100 biodiesel from waste fats, oils, and greases at the site of waste generation. SSC delivers low-cost transportation fuel, avoids significant landfill costs for municipalities, and reduces potent methane and other emissions produced in landfills from these wastes. You can learn more about INL's energy research programs at http://www.facebook.com/idahonationallaboratory.

  4. Copper-containing zeolite catalysts

    DOE Patents [OSTI]

    Price, G.L.; Kanazirev, V.

    1996-12-10

    A catalyst useful in the conversion of nitrogen oxides or in the synthesis of nitriles or imines from amines, is formed by preparing an intimate mechanical mixture of a copper (II)-containing species, such as CuO or CuCl{sub 2}, or elemental copper, with a zeolite having a pore mouth comprising 10 oxygen atoms, such as ZSM-5, converting the elemental copper or copper (II) to copper (I), and driving the copper (I) into the zeolite.

  5. Copper-containing zeolite catalysts

    DOE Patents [OSTI]

    Price, Geoffrey L. (Baton Rouge, LA); Kanazirev, Vladislav (Sofia, BG)

    1996-01-01

    A catalyst useful in the conversion of nitrogen oxides or in the synthesis of nitriles or imines from amines, formed by preparing an intimate mechanical mixture of a copper (II)-containing species, such as CuO or CuCl.sub.2, or elemental copper, with a zeolite having a pore mouth comprising 10 oxygen atoms, such as ZSM-5, converting the elemental copper or copper (II) to copper (I), and driving the copper (I) into the zeolite.

  6. Catalysts for Fischer-Tropsch

    SciTech Connect (OSTI)

    Srivastava, R.D. ); Rao, V.U.S.; Cinquegrane, G.; Stiegel, G.J. )

    1990-02-01

    The slurry-phase Fischer-Tropsch (F-T) process has attracted considerable attention recently. The process can make liquid fuels by reacting hydrogen-lean synthesis gas produced from modern energy-efficient gasifiers. continuing assessment of Fischer-Tropsch Synthesis (FTS) has a high priority within an indirect liquefaction program, a part of the liquid fuels program sponsored by the U.S. Department of Energy (DOE) and executed by the Pittsburgh Energy Technology Center (PETC). Funding for the indirect liquefaction program in 1990:0090 is anticipated to be about $8.5 million compared to $6.6 million in 1989 and a like amount in the year before. The studies within the program are conducted by industry, universities, national laboratories and in-house PETC research and development. This article reviews preparation and properties of iron-based catalysts, including recent patent activities and in-depth process analysis of slurry-phase FTS. The review provides an analysis of Fischer-Tropsch catalyst research and development trends and describes options to increase selectivity for iron-based catalysts in a slurry phase.

  7. Tungsten carbide/porous carbon composite as superior support for platinum catalyst toward methanol electro-oxidation

    SciTech Connect (OSTI)

    Jiang, Liming; Fu, Honggang; Wang, Lei; Mu, Guang; Jiang, Baojiang; Zhou, Wei; Wang, Ruihong

    2014-01-01

    Graphical abstract: The WC nanoparticles are well dispersed in the carbon matrix. The size of WC nanoparticles is about 30 nm. It can be concluded that tungsten carbide and carbon composite was successfully prepared by the present synthesis conditions. - Highlights: • The WC/PC composite with high specific surface area was prepared by a simple way. • The Pt/WC/PC catalyst has superior performance toward methanol electro-oxidation. • The current density for methanol electro-oxidation is as high as 595.93 A g{sup ?1} Pt. • The Pt/WC/PC catalyst shows better durability and stronger CO electro-oxidation. • The performance of Pt/WC/PC is superior to the commercial Pt/C (JM) catalyst. - Abstract: Tungsten carbide/porous carbon (WC/PC) composites have been successfully synthesized through a surfactant assisted evaporation-induced-assembly method, followed by a thermal treatment process. In particular, WC/PC-35-1000 composite with tungsten content of 35% synthesized at the carbonized temperature of 1000 °C, exhibited a specific surface area (S{sub BET}) of 457.92 m{sup 2} g{sup ?1}. After loading Pt nanoparticles (NPs), the obtained Pt/WC/PC-35-1000 catalyst exhibits the highest unit mass electroactivity (595.93 A g{sup ?1} Pt) toward methanol electro-oxidation, which is about 2.6 times as that of the commercial Pt/C (JM) catalyst. Furthermore, the Pt/WC/PC-35-1000 catalyst displays much stronger resistance to CO poisoning and better durability toward methanol electrooxidation compared with the commercial Pt/C (JM) catalyst. The high electrocatalytic activity, strong poison-resistivity and good stability of Pt/WC/PC-35-1000 catalyst are attributed to the porous structures and high specific surface area of WC/PC support could facilitate the rapid mass transportation. Moreover, synergistic effect between WC and Pt NPs is favorable to the higher catalytic performance.

  8. Low temperature catalysts for methanol production

    DOE Patents [OSTI]

    Sapienza, R.S.; Slegeir, W.A.; O'Hare, T.E.; Mahajan, D.

    1986-09-30

    A catalyst and process useful at low temperatures (below about 160 C) and preferably in the range 80--120 C used in the production of methanol from carbon monoxide and hydrogen are disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa-M(OAc)[sub 2] where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1--6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M = Ni and R = tertiary amyl). Mo(CO)[sub 6] is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  9. Ethanol oxidation on metal oxide-supported platinum catalysts

    SciTech Connect (OSTI)

    L. M. Petkovic 090468; Sergey N. Rashkeev; D. M. Ginosar

    2009-09-01

    Ethanol is a renewable fuel that can be used as an additive to gasoline (or its substitute) with the advantage of octane enhancement and reduced carbon monoxide exhaust emissions. However, on Ethanol is a renewable fuel that can be used as an additive to gasoline (or its substitute) with the advantage of octane enhancement and reduced carbon monoxide exhaust emissions. However, on the standard three-way catalysts, the conversion of unburned ethanol is low because both ethanol and some of its partially oxidized derivatives are highly resistant to oxidation. A combination of first-principles density-functional theory (DFT) based calculations and in-situ diffuse reflectance infrared spectroscopy (DRIFTS) analysis was applied to uncover some of the fundamental phenomena associated with ethanol oxidation on Pt containing catalysts. In particular, the objective was to analyze the role of the oxide (i.e., ?-Al2O3 or SiO2) substrate on the ethanol oxidation activity. The results showed that Pt nanoparticles trap and accumulate oxygen at their surface and perimeter sites and play the role of “stoves” that burn ethanol molecules and their partially oxidized derivatives to the “final” products. The ?-Al2O3 surfaces provided higher mobility of the fragments of ethanol molecules than the SiO2 surface and hence increased the supply rate of these objects to the Pt particles. This will in turn produce a higher conversion rate of unburned ethanol.and some of its partially oxidized derivatives are highly resistant to oxidation. A combination of first-principles density-functional theory (DFT) based calculations and in-situ diffuse reflectance infrared spectroscopy (DRIFTS) analysis was applied to uncover some of the fundamental phenomena associated with ethanol oxidation on Pt containing catalysts. In particular, the objective was to analyze the role of the oxide (i.e., ?-Al2O3 or SiO2) substrate on the ethanol oxidation activity. The results showed that Pt nanoparticles trap and accumulate oxygen at their surface and perimeter sites and play the role of “stoves” that burn ethanol molecules and their partially oxidized derivatives to the “final” products. The ?-Al2O3 surfaces provided higher mobility of the fragments of ethanol molecules than the SiO2 surface and hence increased the supply rate of these objects to the Pt particles. This will in turn produce a higher conversion rate of unburned ethanol.

  10. Environmental Transmission Electron Microscopy Study of the Origins of Anomalous Particle Size Distributions in Supported Metal Catalysts

    SciTech Connect (OSTI)

    Benavidez, Angelica D.; Kovarik, Libor; Genc, Arda; Agrawal, Nitin; Larsson, Elin M.; Hansen, Thomas W.; Karim, Ayman M.; Datye, Abhaya K.

    2012-10-31

    In this Environmental TEM (ETEM) study of supported Pt and Pd model catalysts, individual nanoparticles were tracked during heat treatments at temperatures up to 600°C in H2, O2, and vacuum. We found anomalous growth of nanoparticles occurred during the early stages of catalyst sintering wherein some particles started to grow significantly larger than the mean, resulting in a broadening of the particle size distribution. We can rule out sample non-uniformity as a cause for the growth of these large particles, since images were recorded prior to heat treatments. The anomalous growth of these particles may help explain particle size distributions in heterogeneous catalysts which often show particles that are significantly larger than the mean, resulting in a long tail to the right. It has been suggested that particle migration and coalescence could be the likely cause for the broad size distributions. This study shows that anomalous growth of nanoparticles can occur under conditions where Ostwald ripening is the primary sintering mechanism.

  11. Catalysts for Dehydrogenation of ammonia boranes

    SciTech Connect (OSTI)

    Heinekey, Dennis M.

    2014-12-19

    Several effective homogeneous catalysts for the dehydrogenation of amine boranes have been developed. The best catalyst uses an iridium complex, and is capable of dehydrogenating H3NBH3 (AB) and CH3NH2BH3 (MeAB) at comparable rates. Thermodynamic measurements using this catalyst demonstrate that the dehydrogenation of AB and MeAB is substantially exothermic, which has important implications for regeneration.

  12. CLEERS Coordination & Development of Catalyst Process Kinetic...

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

    Maryland. merit08choi.pdf More Documents & Publications Functionality of Commercial NOx Storage-Reduction Catalysts and the Development of a Representative Model CLEERS...

  13. Process for coal liquefaction using electrodeposited catalyst

    DOE Patents [OSTI]

    Moore, Raymond H. (Richland, WA)

    1978-01-01

    A process for the liquefaction of solid hydrocarbonaceous materials is disclosed. Particles of such materials are electroplated with a metal catalyst and are then suspended in a hydrocarbon oil and subjected to hydrogenolysis to liquefy the solid hydrocarbonaceous material. A liquid product oil is separated from residue solid material containing char and the catalyst metal. The catalyst is recovered from the solid material by electrolysis for reuse. A portion of the product oil can be employed as the hydrocarbon oil for suspending additional particles of catalyst coated solid carbonaceous material for hydrogenolysis.

  14. Nitrogen oxides storage catalysts containing cobalt

    DOE Patents [OSTI]

    Lauterbach, Jochen (Newark, DE); Snively, Christopher M. (Clarks Summit, PA); Vijay, Rohit (Annandale, NJ); Hendershot, Reed (Breinigsville, PA); Feist, Ben (Newark, DE)

    2010-10-12

    Nitrogen oxides (NO.sub.x) storage catalysts comprising cobalt and barium with a lean NO.sub.x storage ratio of 1.3 or greater. The NO.sub.x storage catalysts can be used to reduce NO.sub.x emissions from diesel or gas combustion engines by contacting the catalysts with the exhaust gas from the engines. The NO.sub.x storage catalysts can be one of the active components of a catalytic converter, which is used to treat exhaust gas from such engines.

  15. Polyfunctional catalyst for processiing benzene fractions

    SciTech Connect (OSTI)

    G. Byakov; B.D. Zubitskii; B.G. Tryasunov; I.Ya. Petrov

    2009-05-15

    A by-product of the coke industry is a raw benzene fraction benzene- 1 which may serve as for catalytic processes. The paper reports a study on the influence of the composition and temperatures on the activity and selectivity of NiO-V{sub 2}O{sub 6}-MoO{sub 3}/{gamma}-Al{sub 2}O{sub 3} catalysts and the corresponding binary and tertiary subsystems are studied by a pulse method in model reactions; the hydrodealkylating of toluene and the hydrodesulfurizing of thioprhene. The optimal catalyst composition is established. The new catalyst is compared with industrial catalysts.

  16. Deactivation and performance testing of hydroconversion catalysts

    SciTech Connect (OSTI)

    Stork, W.H.J. [Koninklijke/Shell-Laboratorium, Amsterdam (Netherlands)

    1995-12-31

    This paper focuses on distillate hydrocracking and hydrodesulfurization with respect to catalyst deactivation. The role of testing with the aid of model compounds is described.

  17. Gold catalyst Styrene Benzaldehyde Styrene oxide Acetophenone

    E-Print Network [OSTI]

    Rouyer, Francois

    O O O + + O2 Gold catalyst Styrene Benzaldehyde Styrene oxide Acetophenone studies. However styrene. The reaction chiefly yielded benzaldehyde, with smaller amounts of styrene oxide and acetophenone

  18. Catalyst Support Interactions | Argonne Leadership Computing...

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

    on the reactivity of metal catalyst particles. The research team will also study the adhesion properties by simulating the interactions between metal particles of different sizes...

  19. Low Temperature Catalyst for Fuel Injection System

    Broader source: Energy.gov [DOE]

    A low temperature oxidation catalyst applied to a DOC and DPF combined with a unique fuel injection system remove soot from a diesel exhaust system.

  20. Developing Intermetallic Catalysts | The Ames Laboratory

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

    1: Precious metals and metal alloys are important heterogeneous catalysts for renewable energies and materials. However, both of them have their limitations. Precious metals have...

  1. Hydrocarbon synthesis catalyst and method of preparation

    DOE Patents [OSTI]

    Sapienza, Richard S. (Shoreham, NY); Sansone, Michael J. (Summit, NJ); Slegeir, William A. R. (Hampton Bays, NY)

    1983-08-02

    A catalyst for the synthesis of hydrocarbons from carbon monoxide and hydrogen composed of palladium or platinum and cobalt supported on a solid phase is disclosed. The catalyst is prepared by heating a heterogeneous component of the palladium or platinum deposited on the solid support in a solution of cobalt carbonyl or precursors thereof. The catalyst exhibits excellent activity, stability in air, and produces highly desirable product fractions even with dilute gaseous reactants. The catalyst is preferably used in dilute slurry form, which is desirable from a heat transfer standpoint.

  2. Hydrocarbon synthesis catalyst and method of preparation

    DOE Patents [OSTI]

    Sapienza, R.S.; Sansone, M.J.; Slegeir, W.A.R.

    1983-08-02

    A catalyst for the synthesis of hydrocarbons from carbon monoxide and hydrogen composed of palladium or platinum and cobalt supported on a solid phase is disclosed. The catalyst is prepared by heating a heterogeneous component of the palladium or platinum deposited on the solid support in a solution of cobalt carbonyl or precursors thereof. The catalyst exhibits excellent activity, stability in air, and produces highly desirable product fractions even with dilute gaseous reactants. The catalyst is preferably used in dilute slurry form, which is desirable from a heat transfer standpoint. 9 figs.

  3. Bifunctional Catalysts for the Selective Catalytic Reduction...

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

    Publications Bifunctional Catalysts for the Selective Catalytic Reduction of NO by Hydrocarbons Selectlive Catalytic Reducution of NOx wilth Diesel-Based Fuels as Reductants...

  4. Lean NOx Reduction with Dual Layer LNT/SCR Catalysts

    Broader source: Energy.gov [DOE]

    Results show that a series of dual layer catalysts with a bottom layer of LNT catalyst and a top layer of SCR catalyst can carry out coupled ammonia generation and NOx reduction, achieving high NOx conversion with minimal ammonia slip

  5. A general method for multimetallic platinum alloy nanowires as highly active and stable oxygen reduction catalysts

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

    Bu, Lingzheng; Ding, Jiabao; Yao, Jianlin; Huang, Xiaoqing; Guo, Shaojun; Zhang, Xu; Lu, Gang; Su, Dong; Zhu, Xing; Guo, Jun

    2015-10-13

    The production of inorganic nanoparticles (NPs) with precise control over structures has always been a central target in various fields of chemistry and physics because the properties of NPs can be desirably manipulated by their structure.[1-4] There has been an intense search for high-performance noble metal NP catalysts particular for Pt.[5-9] Precious platinum (Pt) NPs are active catalysts for various heterogeneous reactions and show particularly superior performance in both the anodic oxidation reaction and the cathodic ORR in the fuel cells, but their rare content and high cost largely impede the practical application.[10-12] A potential strategy to address this tremendousmore »challenge is alloying Pt NPs with the transition metals (TM).[13-16]« less

  6. Modeling carbon nanotube growth on the catalyst-substrate surface subjected to reactive plasma [

    SciTech Connect (OSTI)

    Tewari, Aarti; Sharma, Suresh C.

    2014-06-15

    The paper presents a theoretical model to study the growth of the carbon nanotube (CNT) on the catalyst substrate surface subjected to reactive plasma. The charging rate of the CNT, kinetics of electron, ions and neutral atoms, the growth rate of the CNT because of diffusion and accretion of ions on the catalyst nanoparticle inclusion of the issue of the plasma sheath is undertaken in the present model. Numerical calculations on the effect of ion density and temperature and the substrate bias on the growth of the CNT have been carried out for typical glow discharge plasma parameters. It is found that the height of CNT increases with the ion density of carbon ions and radius of CNT decreases with hydrogen ion density. The substrate bias also affects the growth rate of the CNT. The field emission characteristics from the CNTs can be analyzed from the results obtained.

  7. Thermally Stable Nanocatalyst for High Temperature Reactions: Pt-Mesoporous Silica Core-Shell Nanoparticles

    SciTech Connect (OSTI)

    Joo, Sang Hoon; Park, J.Y.; Tsung, C.-K.; Yamada, Y.; Yang, P.; Somorjai, G.A.

    2008-10-25

    Recent advances in colloidal synthesis enabled the precise control of size, shape and composition of catalytic metal nanoparticles, allowing their use as model catalysts for systematic investigations of the atomic-scale properties affecting catalytic activity and selectivity. The organic capping agents stabilizing colloidal nanoparticles, however, often limit their application in high-temperature catalytic reactions. Here we report the design of a high-temperature stable model catalytic system that consists of Pt metal core coated with a mesoporous silica shell (Pt{at}mSiO{sub 2}). While inorganic silica shells encaged the Pt cores up to 750 C in air, the mesopores directly accessible to Pt cores made the Pt{at}mSiO{sub 2} nanoparticles as catalytically active as bare Pt metal for ethylene hydrogenation and CO oxidation. The high thermal stability of Pt{at}mSiO{sub 2} nanoparticles permitted high-temperature CO oxidation studies, including ignition behavior, which was not possible for bare Pt nanoparticles because of their deformation or aggregation. The results suggest that the Pt{at}mSiO{sub 2} nanoparticles are excellent nanocatalytic systems for high-temperature catalytic reactions or surface chemical processes, and the design concept employed in the Pt{at}mSiO{sub 2} core-shell catalyst can be extended to other metal-metal oxide compositions.

  8. Late transition metal bimetallics for photocatalytic hydrogen production, M-X and C-H bond activation

    E-Print Network [OSTI]

    Esswein, Arthur J

    2007-01-01

    Broadly defined this thesis has focused on the design and study of molecular catalysts that engender multi-electron reactions and photoreactions on small molecule substrates relevant to solar energy conversion. Specifically ...

  9. Development of Optimal Catalyst Designs and Operating Strategies...

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

    Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx...

  10. Development of Optimal Catalyst Designs and Operating Strategies...

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

    Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems Development of Optimal Catalyst Designs and Operating Strategies for Coupled LNT...

  11. Ultra-high Resolution Electron Microscopy for Catalyst Characterizatio...

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

    high Resolution Electron Microscopy for Catalyst Characterization Ultra-high Resolution Electron Microscopy for Catalyst Characterization 2009 DOE Hydrogen Program and Vehicle...

  12. Functionality of Commercial NOx Storage-Reduction Catalysts and...

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

    Functionality of Commercial NOx Storage-Reduction Catalysts and the Development of a Representative Model Functionality of Commercial NOx Storage-Reduction Catalysts and the...

  13. Dynamometer Evaluation of Plasma-Catalyst for Diesel NOx Reduction...

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

    Evaluation of Plasma-Catalyst for Diesel NOx Reduction Dynamometer Evaluation of Plasma-Catalyst for Diesel NOx Reduction 2003 DEER Conference Presentation: Ford Motor Company...

  14. Unique Catalyst System for NOx Reduction in Diesel Exhaust |...

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

    Catalyst System for NOx Reduction in Diesel Exhaust Unique Catalyst System for NOx Reduction in Diesel Exhaust Poster presentation at the 2007 Diesel Engine-Efficiency & Emissions...

  15. Cobalt discovery replaces precious metals as industrial catalyst

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

    Discovery Replaces Precious Metals Cobalt discovery replaces precious metals as industrial catalyst Cobalt holds promise as an industrial catalyst with potential applications...

  16. Nanosegregated Cathode Catalysts with Ultra-Low Platinum Loading...

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

    Nanosegregated Cathode Catalysts with Ultra-Low Platinum Loading Nanosegregated Cathode Catalysts with Ultra-Low Platinum Loading Presented at the Department of Energy Fuel Cell...

  17. Controlled catalystic and thermal sequential pyrolysis and hydrolysis...

    Office of Scientific and Technical Information (OSTI)

    catalystic and thermal sequential pyrolysis and hydrolysis of polycarbonate and plastic waste to recover monomers Citation Details In-Document Search Title: Controlled catalystic...

  18. Single Step Manufacturing of Low Catalyst Loading Electrolyzer...

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

    Gen Process) Direct Coat onto Membrane Manufacture MEA through Single-step Catalyst Pyrolysis and Membrane Deposition. Synthesize Catalyst Ink Transfer Ink to Substrate Drive-off...

  19. Impact of Fuel Metal Impurities on Diesel Exhaust Catalysts ...

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

    Diesel Exhaust Catalysts Investigates impact of metal impurities in biodiesel on full useful life durability of catalysts in diesel exhaust aftertreatment systems...

  20. Novel Approach to Advanced Direct Methanol Fuel Cell Anode Catalysts...

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

    Approach to Advanced Direct Methanol Fuel Cell Anode Catalysts Novel Approach to Advanced Direct Methanol Fuel Cell Anode Catalysts Presented at the Department of Energy Fuel Cell...

  1. Novel Vertimass Catalyst for Conversion of Ethanol and Other...

    Office of Environmental Management (EM)

    Novel Vertimass Catalyst for Conversion of Ethanol and Other Alcohols into Fungible Gasoline, Jet, and Diesel Fuel Blend Stocks Novel Vertimass Catalyst for Conversion of Ethanol...

  2. Reaction Rates and Catalysts in Ethanol Production (1 Activity...

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

    Reaction Rates and Catalysts in Ethanol Production (1 Activity) Reaction Rates and Catalysts in Ethanol Production (1 Activity) Below is information about the student activity...

  3. Table I: Technical Targets for Catalyst Coated Membranes (CCMs...

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

    I: Technical Targets for Catalyst Coated Membranes (CCMs): Automotive Table I: Technical Targets for Catalyst Coated Membranes (CCMs): Automotive Technical targets for fuel cell...

  4. Catalyst-Assisted Production of Olefins from Natural Gas Liquids...

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

    Catalyst-Assisted Production of Olefins from Natural Gas Liquids: Prototype Development and Full-Scale Testing, April 2013 Catalyst-Assisted Production of Olefins from Natural Gas...

  5. Global kinetics for a commercial diesel oxidation catalyst with...

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

    kinetics for a commercial diesel oxidation catalyst with two exhaust hydrocarbons Global kinetics for a commercial diesel oxidation catalyst with two exhaust hydrocarbons...

  6. Hydrocracking process and catalyst therefor

    SciTech Connect (OSTI)

    Ward, J. W.; Carlson, T. L.

    1985-05-14

    A hydrocracking process, of especial use in the production of a relatively high yield of middle distillate products along with a smaller but still significant yield of gasoline from high boiling gas oils and the like, comprises contacting a gas oil or other hydrocarbon feedstock under hydrocracking conditions with a novel catalyst comprising one or more hydrogenation components on a support material comprising, in combination, a dispersion of silica-alumina in alumina and a zeolite to the Y crystalline structure but having a silica-to-alumina ratio above 6.0.

  7. Attrition resistant fluidizable reforming catalyst

    DOE Patents [OSTI]

    Parent, Yves O. (Golden, CO); Magrini, Kim (Golden, CO); Landin, Steven M. (Conifer, CO); Ritland, Marcus A. (Palm Beach Shores, FL)

    2011-03-29

    A method of preparing a steam reforming catalyst characterized by improved resistance to attrition loss when used for cracking, reforming, water gas shift and gasification reactions on feedstock in a fluidized bed reactor, comprising: fabricating the ceramic support particle, coating a ceramic support by adding an aqueous solution of a precursor salt of a metal selected from the group consisting of Ni, Pt, Pd, Ru, Rh, Cr, Co, Mn, Mg, K, La and Fe and mixtures thereof to the ceramic support and calcining the coated ceramic in air to convert the metal salts to metal oxides.

  8. Thermodynamic Properties of Supported Catalysts

    SciTech Connect (OSTI)

    Gorte, Raymond J.

    2014-03-26

    The goals of this work were to develop Coulometric Titration as a method for characterizing the thermodynamic redox properties of oxides and to apply this technique to the characterization of ceria- and vanadia-based catalysts. The redox properties of ceria and vanadia are a major part of what makes these materials catalytically active but their properties are also dependent on their structure and the presence of other oxides. Quantifying these properties through the measurement of oxidation energetics was the goal of this work.

  9. SISGR-Fundamental Experimental and Theoretical Studies on a Novel Family of Oxide Catalyst Supports for Water Electrolysis

    SciTech Connect (OSTI)

    Kumta, Prashant

    2014-10-03

    Identification and development of non-noble metal based electro-catalysts or electro-catalysts with significant reduction of expensive noble metal contents (E.g. IrO2, Pt) with comparable electrochemical performance as the standard noble metal/metal oxide for proton exchange membrane (PEM) based water electrolysis would constitute a major breakthrough in the generation of hydrogen by water electrolysis. Accomplishing such a system would not only result reduction of the overall capital costs of PEM based water electrolyzers, but also help attain the targeted hydrogen production cost [< $ 3.0 / gallon gasoline equivalent (gge)] comparable to conventional liquid fuels. In line with these goals, it was demonstrated that fluorine doped IrO2 thin films and nanostructured high surface area powders display remarkably higher electrochemical activity, and comparable durability as pure IrO2 electro-catalyst for the oxygen evolution reaction (OER) in PEM based water electrolysis. Furthermore, corrosion resistant SnO2 and NbO2 support has been doped with F and coupled with IrO2 or RuO2 for use as an OER electro-catalyst. A solid solution of SnO2:F or NbO2:F with only 20 - 30 mol.% IrO2 or RuO2 yielding a rutile structure in the form of thin films and bulk nanoparticles displays similar electrochemical activity and stability as pure IrO2/RuO2. This would lead to more than 70 mol.% reduction in the noble metal oxide content. Novel nanostructured ternary (Ir,Sn,Nb)O2 thin films of different compositions FUNDAMENTAL STUDY OF NANOSTRUCTURED ELECTRO-CATALYSTS WITH REDUCED NOBLE METAL CONTENT FOR PEM BASED WATER ELECTROLYSIS 4 have also been studied. It has been shown that (Ir0.40Sn0.30Nb0.30)O2 shows similar electrochemical activity and enhanced chemical robustness as compared to pure IrO2. F doping of the ternary (Ir,Sn,Nb)O2 catalyst helps in further decreasing the noble metal oxide content of the catalyst. As a result, these reduced noble metal oxide catalyst systems would potentially be preferred as OER electro-catalysts for PEM electrolysis. The excellent performance of the catalysts coupled with its robustness would make them great candidates for contributing to significant reduction in the overall capital costs of PEM based water electrolyzers. This s.thesis provides a detailed fundamental study of the synthesis, materials, characterization, theoretical studies and detailed electrochemical response and potential mechanisms of these novel electro-catalysts for OER processes.

  10. Sulfur-mediated palladium catalyst immobilized on a GaAs surface

    SciTech Connect (OSTI)

    Shimoda, M. [Surface Physics and Structure Unit, Surface Physics Group, National Institute for Materials Science, 1-2-1, Sengen, Tsukuba, Ibaraki 305-0047 (Japan); Konishi, T. [Anan National College of Technology, 265 Aoki, Minobayashi-cho, Anan, Tokushima 774-0017 (Japan); Nishiwaki, N. [School of Environmental and Engineering, Kochi University of Technology, Tosayamada, Kami, Kochi 782-8502 (Japan); Yamashita, Y.; Yoshikawa, H. [Synchrotron X-ray Station at SPring-8, National Institute for Materials Science, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148 (Japan)

    2012-06-15

    We present a hard x-ray photoelectron spectroscopy study on the preparation process of palladium catalyst immobilized on an S-terminated GaAs(100) surface. It is revealed that Pd(II) species are reduced on the GaAs surface and yield Pd nanoparticles during the process of Pd immobilization and the subsequent heat treatment. A comparison with the results on GaAs without S-termination suggests that the reduction of Pd is promoted by hydroxy groups during the Pd immobilization and by S during the heat treatment.

  11. Enhancing H2 evolution performance of an immobilised cobalt catalyst by rational ligand design

    E-Print Network [OSTI]

    Willkomm, Janina; Muresan, Nicoleta M.; Reisner, Erwin

    2015-02-02

    l P catalyst on ruthenium-dye sensitised TiO2 nanoparticles in aqueous solutions in the presence of a hole Introduction Solar fuels generation through ar a well-balanced combination o separation with proton reduction preferentially in a photoelectroc... (Fig. 2A). When scanning towards more cathodic potential, a third reduction wave is observed which is attributed to catalytic proton reduction by the complex.3d Comparable electrochemical responses were obtained when a pH 7 triethanolamine (TEOA)/Na2SO4...

  12. Method for reactivating catalysts and a method for recycling supercritical fluids used to reactivate the catalysts

    DOE Patents [OSTI]

    Ginosar, Daniel M. (Idaho Falls, ID); Thompson, David N. (Idaho Falls, ID); Anderson, Raymond P. (Idaho Falls, ID)

    2008-08-05

    A method of reactivating a catalyst, such as a solid catalyst or a liquid catalyst. The method comprises providing a catalyst that is at least partially deactivated by fouling agents. The catalyst is contacted with a fluid reactivating agent that is at or above a critical point of the fluid reactivating agent and is of sufficient density to dissolve impurities. The fluid reactivating agent reacts with at least one fouling agent, releasing the at least one fouling agent from the catalyst. The at least one fouling agent becomes dissolved in the fluid reactivating agent and is subsequently separated or removed from the fluid reactivating agent so that the fluid reactivating agent may be reused. A system for reactivating a catalyst is also disclosed.

  13. Improved catalysts for carbon and coal gasification

    DOE Patents [OSTI]

    McKee, D.W.; Spiro, C.L.; Kosky, P.G.

    1984-05-25

    This invention relates to improved catalysts for carbon and coal gasification and improved processes for catalytic coal gasification for the production of methane. The catalyst is composed of at least two alkali metal salts and a particulate carbonaceous substrate or carrier is used. 10 figures, 2 tables.

  14. Improved catalyst can clear the air

    SciTech Connect (OSTI)

    Pritchard, S. [Cormetech Inc. (United States)

    2006-05-15

    Catalyst technology can make clean coal plants look as clean as they are. This article examines the need and available methods for SO{sub 2} control with a specific focus on a catalyst technology developed by Cormetech. It also presents the results of commercial operating experience. 1 fig., 2 tabs.

  15. Catalyst and method for production of methylamines

    DOE Patents [OSTI]

    Klier, Kamil (Bethlehem, PA); Herman, Richard G. (Whitehall, PA); Vedage, Gamini A. (Bethlehem, PA)

    1987-01-01

    This invention relates to an improved catalyst and method for the selective production of methylamines. More particularly, it is concerned with the preparation of stable highly active catalysts for producing methylamines by a catalytic reaction of ammonia or substituted amines and binary synthesis gas (CO+H.sub.2).

  16. Thin film hydrous metal oxide catalysts

    DOE Patents [OSTI]

    Dosch, Robert G. (Albuquerque, NM); Stephens, Howard P. (Albuquerque, NM)

    1995-01-01

    Thin film (<100 nm) hydrous metal oxide catalysts are prepared by 1) synthesis of a hydrous metal oxide, 2) deposition of the hydrous metal oxide upon an inert support surface, 3) ion exchange with catalytically active metals, and 4) activating the hydrous metal oxide catalysts.

  17. Integrated current collector and catalyst support

    DOE Patents [OSTI]

    Bregoli, Lawrence J. (Southwick, MA)

    1985-10-22

    An integrated current collecting electrode for a molten carbonate fuel cell includes a corrugated metal conductive strip positioned in contact with a catalyst layer. The corrugations of the metal strip form a plurality of gas channels immediately adjacent the surface of the catalyst through which a reactant gas flows. Each channel is filled with a particulate material to maintain separation between the metal strip and the catalyst in ensuring gas channel integrity. The catalyst may be in the form of a compacted, particulate material provided the particle size of the material within the gas channels is larger than that of the catalyst particles to prevent catalyst migration to the metal conductor and provide reactant gas access to the catalyst layer. The gas channels formed by the corrugations of the metal strip are arranged in an offset pattern along the direction of gas flow for improved reactant gas distribution to the catalyst layer. The particulate material positioned within the gas flow channels may be a ceramic conductor such as a perovskite or a spinel for enhanced current collection.

  18. Integrated current collector and catalyst support

    DOE Patents [OSTI]

    Bregoli, L.J.

    1984-10-17

    An integrated current collecting electrode for a molten carbonate fuel cell includes a corrugated metal conductive strip positioned in contact with a catalyst layer. The corrugations of the metal strip form a plurality of gas channels immediately adjacent the surface of the catalyst through which a reactant gas flows. Each channel is filled with a particulate material to maintain separation between the metal strip and the catalyst in ensuring gas channel integrity. The catalyst may be in the form of a compacted, particulate material provided the particle size of the material within the gas channels is larger than that of the catalyst particles to prevent catalyst migration to the metal conductor and provide reactant gas access to the catalyst layer. The gas channels formed by the corrugations of the metal strip are arranged in an offset pattern along the direction of gas flow for improved reactant gas distribution to the catalyst layer. The particulate material positioned within the gas flow channels may be a ceramic conductor such as a perovskite or a spinel for enhanced current collection.

  19. Membrane catalyst layer for fuel cells

    DOE Patents [OSTI]

    Wilson, Mahlon S. (Los Alamos, NM)

    1993-01-01

    A gas reaction fuel cell incorporates a thin catalyst layer between a solid polymer electrolyte (SPE) membrane and a porous electrode backing. The catalyst layer is preferably less than about 10 .mu.m in thickness with a carbon supported platinum catalyst loading less than about 0.35 mgPt/cm.sup.2. The film is formed as an ink that is spread and cured on a film release blank. The cured film is then transferred to the SPE membrane and hot pressed into the surface to form a catalyst layer having a controlled thickness and catalyst distribution. Alternatively, the catalyst layer is formed by applying a Na.sup.+ form of a perfluorosulfonate ionomer directly to the membrane, drying the film at a high temperature, and then converting the film back to the protonated form of the ionomer. The layer has adequate gas permeability so that cell performance is not affected and has a density and particle distribution effective to optimize proton access to the catalyst and electronic continuity for electron flow from the half-cell reaction occurring at the catalyst.

  20. Process for magnetic beneficiating petroleum cracking catalyst

    DOE Patents [OSTI]

    Doctor, R.D.

    1993-10-05

    A process is described for beneficiating a particulate zeolite petroleum cracking catalyst having metal values in excess of 1000 ppm nickel equivalents. The particulate catalyst is passed through a magnetic field in the range of from about 2 Tesla to about 5 Tesla generated by a superconducting quadrupole open-gradient magnetic system for a time sufficient to effect separation of said catalyst into a plurality of zones having different nickel equivalent concentrations. A first zone has nickel equivalents of about 6,000 ppm and greater, a second zone has nickel equivalents in the range of from about 2000 ppm to about 6000 ppm, and a third zone has nickel equivalents of about 2000 ppm and less. The zones of catalyst are separated and the second zone material is recycled to a fluidized bed of zeolite petroleum cracking catalyst. The low nickel equivalent zone is treated while the high nickel equivalent zone is discarded. 1 figures.

  1. Nanostructured Basic Catalysts: Opportunities for Renewable Fuels

    SciTech Connect (OSTI)

    Conner, William C; Huber, George; Auerbach, Scott

    2009-06-30

    This research studied and developed novel basic catalysts for production of renewable chemicals and fuels from biomass. We focused on the development of unique porous structural-base catalysts zeolites. These catalysts were compared to conventional solid base materials for aldol condensation, that were being commercialized for production of fuels from biomass and would be pivotal in future biomass conversion to fuels and chemicals. Specifically, we had studied the aldolpyrolysis over zeolites and the trans-esterification of vegetable oil with methanol over mixed oxide catalysts. Our research has indicated that the base strength of framework nitrogen in nitrogen substituted zeolites (NH-zeolites) is nearly twice as strong as in standard zeolites. Nitrogen substituted catalysts have been synthesized from several zeolites (including FAU, MFI, BEA, and LTL) using NH3 treatment.

  2. Process for magnetic beneficiating petroleum cracking catalyst

    DOE Patents [OSTI]

    Doctor, Richard D. (Lisle, IL)

    1993-01-01

    A process for beneficiating a particulate zeolite petroleum cracking catalyst having metal values in excess of 1000 ppm nickel equivalents. The particulate catalyst is passed through a magnetic field in the range of from about 2 Tesla to about 5 Tesla generated by a superconducting quadrupole open-gradient magnetic system for a time sufficient to effect separation of said catalyst into a plurality of zones having different nickel equivalent concentrations. A first zone has nickel equivalents of about 6,000 ppm and greater, a second zone has nickel equivalents in the range of from about 2000 ppm to about 6000 ppm, and a third zone has nickel equivalents of about 2000 ppm and less. The zones of catalyst are separated and the second zone material is recycled to a fluidized bed of zeolite petroleum cracking catalyst. The low nickel equivalent zone is treated while the high nickel equivalent zone is discarded.

  3. Rejuvenation and reuse of spent fluid cracking catalysts

    SciTech Connect (OSTI)

    Elvin, F.J. (ChemCat Corp., New Orleans, LA (US))

    1988-01-01

    Refineries processing heavy, high metals feedstocks have reused other refineries' spent cracking catalyst for the past ten years without observing any yield debits. ChemCat has developed a process whereby a refinery can reuse its own spent catalyst without suffering any yield debits. The new DEMET process is being demonstrated in the world's first commercial fluid cracking catalyst rejuvenation and demetallization plant. The plant is located in Meraux, Louisiana and processes 20 tons/day of spent cracking catalyst for local refineries. The plant removes contaminant metals from zeolite catalysts, while simultaneously increasingly the zeolite and matrix surface areas. The demetallized catalyst has a higher activity and better selectivity than the undemetallized spent catalyst. The demetallized catalyst is also more hydrothermally stable than the spent catalyst. ChemCat's DEMET process enables refiners to eliminate the high cost of spent FCCU catalyst disposal and to significantly reduce their consumption and cost of fresh catalyst.

  4. Oxygen and CO Adsorption on Au/SiO2 Catalysts Prepared by Magnetron Sputtering: The Role of Gold Subsurface

    SciTech Connect (OSTI)

    Zheng, Xiaolin [Washington University, St. Louis; Veith, Gabriel M [ORNL; Redekop, Evgeniy [Washington University, St. Louis; Lo, Cynthia [Washington University, St. Louis; Yablonsky, Gregory [Washington University, St. Louis; Madix, Robert J [Harvard University; Friend, Cynthia [Harvard University; Gleaves, John t [Washington University, St. Louis

    2010-01-01

    Temporal Analysis of Products (TAP) reactor system is used to investigate CO oxidation behavior on Au/SiO2 catalysts prepared via the physical vapor deposition method magnetron sputtering. Au/SiO2 catalysts are a valuable model system for studying the reactivity of Au nanoparticles, since the SiO2 support plays little role in the reaction. The adsorption of CO on the catalyst was studied under TAP vacuum conditions and at different temperatures. The heat of CO adsorption estimated from TAP results by moment analysis is -23.9 kJ/mol which is high compared to heat of CO adsorption reported by other TAP groups studying Au/TiO2 catalysts [29]. The reaction over the catalyst pretreated with oxygen under different pretreatment pressures (vacuum pressures to 33.66 psia) was studied under TAP vacuum conditions via CO titration. It was found that the amount of oxygen available on the surface for CO oxidation is proportional to the pretreatment pressure.

  5. Synthesis and characterization of model MgO supported catalyst with Pt-Mo interactions.

    SciTech Connect (OSTI)

    Alexeev, O.; Kawi, S.; Gates, B.C. [Univ. of California, Davis, CA (United States)] [Univ. of California, Davis, CA (United States); Shelef, M. [Ford Motor Co., Dearborn, MI (United States)] [Ford Motor Co., Dearborn, MI (United States)

    1996-01-04

    MgO supported platinum and platinum-molybdenum catalysts were prepared from organometallic precursors and charaterized structurally to determine how the nature of the bimetallic precursors and the treatment conditions affected the interaction between the two metals. Samples were prepared from [PtCl{sub 2}(PhCN){sub 2}], [PtCl{sub 2}(PhCN){sub 2}] + [Mo(CO){sub 6}], and [C@Pt[Mo(CO){sub 3}(C{sub 5}H{sub 5})]{sub 2}(PhCN){sub 2}] BC@ characterized by infrared and extended X-ray absorption fine structure (EXAFS) spectroscopies, tranmission electron microscopy, and chemisorption of H{sub 2}, CO, and O{sub 2}. The samples were treated in H{sub 2} at 400{degree}C prior to most of the characterizatons. Incorporation of Mo reduced the chemisorption of CO and of H{sub 2}. EXAFS spectra measured at the Pt L{sub III} edge and at the Mo K edge showed substantial Pt-Mo contributions with a Pt-Mo cordination number of about 2 and an average distance of 2.63 A for the sample prepared from [C@Pt[Mo(CO){sub 3}(C{sub 5}H{sub 5})]{sub 2}(PhCN){sub 2}] BC@. In constract, no significant Pt-Mo contribution was observed for the sample prepared from [PtCl{sub 2}(PhCN){sub 2}]+ [Mo(CO){sub 6}]. Electron micrographs and EXAFS results show that interaction between Pt and Mo ions in the former sample helped to maintain the platinum in a highly dispersed form, with supported platinum clusters being smaller than about 10 A. 53 refs., 9 figs., 9 tabs.

  6. New hydroprocessing catalysts prepared from molecular complexes

    SciTech Connect (OSTI)

    Ho, T.C.

    1994-12-31

    Current commercial hydroprocessing catalysts are transition metal sulfides (TMS) based on Group 8 and 11 metals. They are prepared by dispersing MoO{sub 3} and a promoter metal oxide, either CoO or NiO, on {gamma}-Al{sub 2}O{sub 3} or SiO{sub 2}-modified Al{sub 2}O{sub 3}. This is followed by sulfiding with a sulfur-bearing stream such as H{sub 2}S at high temperatures. The thus formed MoS{sub 2} crystallites are the backbone of the working catalysts. A potentially fruitful approach to new catalysts would be to molecularly incorporate promoter metals into the structure of MoS{sub 2} edge planes. As a first step, it would seem reasonable to exploit the use of heterometallic metal sulfur complexes as hydroprocessing catalyst precursors. The authors have developed several families of new catalysts along this line. In this paper the authors restrict themselves to the metal amine thiomolybdate-derived catalysts. Specifically, they give an overview of the performance of the bulk (unsupported) FeMo sulfide prepared from MAT. This low-surface-area catalyst shows a high HDN-to-HDS volumetric activity ratio and is also active for HDA. While most of the results are taken from their previous publications, some new results are reported here.

  7. Templated synthesis of nickel nanoparticles: Toward heterostructured nanocomposites for efficient hydrogen storage

    SciTech Connect (OSTI)

    Nelson, Nicholas Cole

    2013-05-07

    The world is currently facing an energy and environmental crisis for which new technologies are needed. Development of cost-competitive materials for catalysis and hydrogen storage on-board motor vehicles is crucial to lead subsequent generations into a more sustainable and energy independent future. This thesis presents work toward the scalable synthesis of bimetallic heterostructures that can enable hydrogen to compete with carbonaceous fuels by meeting the necessary gravimetric and volumetric energy densities and by enhancing hydrogen sorption/desorption kinetics near ambient temperatures and pressures. Utilizing the well-known phenomenon of hydrogen spillover, these bimetallic heterostructures could work by lowering the activation energy for hydrogenation and dehydrogenation of metals. Herein, we report a novel method for the scalable synthesis of silica templated zero-valent nickel particles (Ni?SiO{sub 2}) that hold promise for the synthesis of nickel nanorods for use in bimetallic heterostructures for hydrogen storage. Our synthesis proceeds by chemical reduction of a nickel-hydrazine complex with sodium borohydride followed by calcination under hydrogen gas to yield silica encapsulated nickel particles. Transmission electron microscopy and powder X-ray diffraction were used to characterize the general morphology of the resultant nanocapsules as well as the crystalline phases of the incorporated Ni{sup 0} nanocrystals. The structures display strong magnetic behavior at room temperature and preliminary data suggests nickel particle size can be controlled by varying the amount of nickel precursor used in the synthesis. Calcination under different environments and TEM analysis provides evidence for an atomic migration mechanism of particle formation. Ni?SiO{sub 2} nanocapsules were used as seeds to induce heterogeneous nucleation and subsequent growth within the nanocapsule via electroless nickel plating. Nickel nanoparticle growth occurs under high temperature alkaline conditions, however silica nanocapsule integrity is not maintained due to the incompatibility of silica with the growth conditions. Silica nanocapsule integrity is maintained under low temperature neutral conditions, but nickel particle growth is not observed. Through FTIR and UV/Vis analysis, we show the degree of crosslinking and condensation increases in calcined silica compared to as-synthesized silica. We propose the increased density of the silica nanocapsule hinders mass transfer of the bulky nickel precursor complex from solution and onto the surface of the “catalytic” zero-valent nickel seed within the nanocapsule cavity. Decreasing the density of the silica nanocapsule can be achieved through co-condensation of tetraethylorthosilicate with an alkyl functionalized silane followed by calcination to remove the organic component or by chemical etching in alkaline solution, but will not be addressed in this thesis.

  8. EXPERIMENTAL RESULTS ON DUAL-UEGO ACTIVE CATALYST CONTROL

    E-Print Network [OSTI]

    Grizzle, Jessy W.

    EXPERIMENTAL RESULTS ON DUAL-UEGO ACTIVE CATALYST CONTROL Giovanni Fiengo Jessy W. Grizzle hydrocarbons. Linear exhaust gas oxygen sensors are used to measure pre- and post-catalyst air-fuel ratio- and post-catalyst air-fuel ratio measurements to compensate for the bias corrupting the pre-catalyst air-fuel

  9. Catalyst for producing lower alcohols

    DOE Patents [OSTI]

    Rathke, Jerome W. (Bolingbrook, IL); Klingler, Robert J. (Woodridge, IL); Heiberger, John J. (Glen Ellyn, IL)

    1987-01-01

    A process and system for the production of the lower alcohols such as methanol, ethanol and propanol involves the reaction of carbon monoxide and water in the presence of a lead salt and an alkali metal formate catalyst combination. The lead salt is present as solid particles such as lead titanate, lead molybdate, lead vanadate, lead zirconate, lead tantalate and lead silicates coated or in slurry within molten alkali metal formate. The reactants, carbon monoxide and steam are provided in gas form at relatively low pressures below 100 atmospheres and at temperatures of 200-400.degree. C. The resulted lower alcohols can be separated into boiling point fractions and recovered from the excess reactants by distillation.

  10. Palladium catalysts synthesized by atomic layer deposition for methanol decomposition.

    SciTech Connect (OSTI)

    Elam, J. W.; Feng, H.; Stair, P. C.; Libera, J. A.; Setthapun, W.; Northwestern Univ.

    2010-05-25

    Atomic layer deposition (ALD) palladium films were deposited at 200 C on various ALD metal oxide surfaces using sequential exposures to Pd(II) hexafluoroacetylacetonate (Pd(hfac)2) and formalin. In situ quartz crystal microbalance measurements as well as ex situ measurements performed on planar substrates revealed that the Pd growth begins with a relatively slow nucleation process and accelerates once an adequate amount of Pd has deposited on the surface. Furthermore, the Pd nucleation is faster on ALD ZnO surfaces compared to ALD Al2O3 surfaces. ALD was utilized to synthesize highly dispersed, uniform Pd nanoparticles (1 to 2 nm in diameter) on ALD ZnO and Al2O3 coated mesoporous silica gel, and the catalytic performances of these samples were compared in the methanol decomposition reaction. The ALD Pd-Al2O3 showed high activity and hydrogen selectivity at relatively low temperatures while the ALD Pd-ZnO showed very low activity as well as quick deactivation. In situ extended X-ray absorption fine structure (EXAFS) measurement revealed that the Pd supported on ZnO 'dissolves' into the substrate during the methanol decomposition reaction which accounts for the gradual disappearance of its catalytic activity. By applying one cycle of ALD Al2O3 on top of the Pd-ZnO catalyst, the activity was enhanced and the catalyst deactivation was mitigated. This Al2O3 overcoating method stabilizes the Pd-ZnO and effectively prevents the dissolution of Pd into the ZnO substrate.

  11. Automated Morphology Analysis of Nanoparticles 

    E-Print Network [OSTI]

    Park, Chiwoo

    2012-10-19

    The functional properties of nanoparticles highly depend on the surface morphology of the particles, so precise measurements of a particle's morphology enable reliable characterizing of the nanoparticle's properties. ...

  12. Commercial experience with new-generation Unicracking catalysts

    SciTech Connect (OSTI)

    Abdo, S.F. (Unocal Process Technology and Licensing, Brea, CA (United States)); Penning, R.T. (UOP, Des Plaines, IL (United States))

    1994-01-01

    In response to today's refining needs, Unocal and UOP have developed a new generation of hydrocracking catalysts, which have been installed in hydrocrackers worldwide. This paper discusses some of the critical elements in hydrocracking catalyst design, with emphasis on showing how knowledge of the interplay between catalyst components, feed types and operating conditions can lead to catalyst products which better fit the needs of the refiners. Also presented are commercial examples of (a) new applications for recently introduced Unicracking catalysts and (b) first-time applications for new catalysts. Data from commercial units show how changes in hydrocracker operating mode, coupled with a judicious choice of catalyst, can lead to significant economic benefits.

  13. Synthesis of iron based hydrocracking catalysts

    DOE Patents [OSTI]

    Farcasiu, Malvina (Pittsburgh, PA); Eldredge, Patricia A. (Barboursville, VA); Ladner, Edward P. (Pittsburgh, PA)

    1993-01-01

    A method of preparing a fine particle iron based hydrocracking catalyst and the catalyst prepared thereby. An iron (III) oxide powder and elemental sulfur are reacted with a liquid hydrogen donor having a hydroaromatic structure present in the range of from about 5 to about 50 times the weight of iron (III) oxide at a temperature in the range of from about 180.degree. C. to about 240.degree. C. for a time in the range of from about 0 to about 8 hours. Various specific hydrogen donors are disclosed. The catalysts are active at low temperature (<350.degree. C.) and low pressure.

  14. Formic acid fuel cells and catalysts

    DOE Patents [OSTI]

    Masel, Richard I.; Larsen, Robert; Ha, Su Yun

    2010-06-22

    An exemplary fuel cell of the invention includes a formic acid fuel solution in communication with an anode (12, 134), an oxidizer in communication with a cathode (16, 135) electrically linked to the anode, and an anode catalyst that includes Pd. An exemplary formic acid fuel cell membrane electrode assembly (130) includes a proton-conducting membrane (131) having opposing first (132) and second surfaces (133), a cathode catalyst on the second membrane surface, and an anode catalyst including Pd on the first surface.

  15. Method for making nanotubes and nanoparticles

    DOE Patents [OSTI]

    Zettl, Alexander Karlwalter (Kensington, CA); Cohen, Marvin Lou (Piedmont, CA)

    2000-01-01

    The present invention is an apparatus and method for producing nano-scale tubes and particles. The apparatus comprises novel electrodes for use in arc discharge techniques. The electrodes have interior conduits for delivery and withdrawal of material from the arc region where product is formed. In one embodiment, the anode is optionally made from more than one material and is termed a compound anode. The materials used in the compound anode assist in the reaction that forms product in the arc region of the apparatus. The materials assist either by providing reaction ingredients, catalyst, or affecting the reaction kinetics. Among other uses, the inventive apparatus is used to produce nanotubes and nanoparticles having a variety of electrical and mechanical properties.

  16. Diesel Oxidation Catalyst Combined to Non-Thermal Plasma: Effect on Activation Catalyst Temperature and by-products formation

    E-Print Network [OSTI]

    Paris-Sud XI, Université de

    Diesel Oxidation Catalyst Combined to Non-Thermal Plasma: Effect on Activation Catalyst Temperature efficiency together with the catalyst activation temperature when a Diesel Oxidation Catalyst (DOC) is placed downstream to a multi-plans Dielectric Barrier Discharge (DBD) reactor. In order to simulate Diesel engine

  17. Enhanced catalyst for conversion of syngas to liquid motor fuels

    DOE Patents [OSTI]

    Coughlin, Peter K. (Yorktown Heights, NY); Rabo, Jule A. (Armonk, NY)

    1985-01-01

    Synthesis gas comprising carbon monoxide and hydrogen is converted to C.sub.5.sup.+ hydrocarbons suitable for use as liquid motor fuels by contact with a dual catalyst system capable of enhancing the selectivity of said conversion to motor fuel range hydrocarbons and the quality of the resulting motor fuel product. The catalyst composition employs a Fischer-Tropsch catalyst, together with a co-catalyst/support component comprising SAPO silicoaluminophosphate, non-zeolitic molecular sieve catalyst.

  18. Enhanced catalyst for conversion of syngas to liquid motor fuels

    DOE Patents [OSTI]

    Coughlin, P.K.; Rabo, J.A.

    1985-12-03

    Synthesis gas comprising carbon monoxide and hydrogen is converted to C[sub 5][sup +] hydrocarbons suitable for use as liquid motor fuels by contact with a dual catalyst system capable of enhancing the selectivity of said conversion to motor fuel range hydrocarbons and the quality of the resulting motor fuel product. The catalyst composition employs a Fischer-Tropsch catalyst, together with a co-catalyst/support component comprising a SAPO silicoaluminophosphate, non-zeolitic molecular sieve catalyst.

  19. Water Uptake in PEMFC Catalyst Layers

    E-Print Network [OSTI]

    Gunterman, Haluna P.

    2013-01-01

    of proton-exchange-membrane fuel-cell catalyst layers arein proton-exchange-membrane fuel cells (PEMFC) is rife withRenewable Energy, Office of Fuel Cell Technologies, of the

  20. Pf/Zeolite Catalyst for Tritium Stripping

    SciTech Connect (OSTI)

    Hsu, R.H.

    2001-03-26

    This report described promising hydrogen (protium and tritium) stripping results obtained with a Pd/zeolite catalyst at ambient temperature. Preliminary results show 90-99+ percent tritium stripping efficiency may be obtained, with even better performance expected as bed configuration and operating conditions are optimized. These results suggest that portable units with single beds of the Pd/zeolite catalyst may be utilized as ''catalytic absorbers'' to clean up both tritium gas and tritiated water. A cart-mounted prototype stripper utilizing this catalyst has been constructed for testing. This portable stripper has potential applications in maintenance-type jobs such as tritium line breaks. This catalyst can also potentially be utilized in an emergency stripper for the Replacement Tritium Facility.

  1. Synthesis and Understanding of Novel Catalysts

    SciTech Connect (OSTI)

    Stair, Peter C. [Northwestern University] [Northwestern University

    2013-07-09

    The research took advantage of our capabilities to perform in-situ and operando Raman spectroscopy on complex systems along with our developing expertise in the synthesis of uniform, supported metal oxide materials to investigate relationships between the catalytically active oxide composition, atomic structure, and support and the corresponding chemical and catalytic properties. The project was organized into two efforts: 1) Synthesis of novel catalyst materials by atomic layer deposition (ALD). 2) Spectroscopic and chemical investigations of coke formation and catalyst deactivation. ALD synthesis was combined with conventional physical characterization, Raman spectroscopy, and probe molecule chemisorption to study the effect of supported metal oxide composition and atomic structure on acid-base and catalytic properties. Operando Raman spectroscopy studies of olefin polymerization leading to coke formation and catalyst deactivation clarified the mechanism of coke formation by acid catalysts.

  2. Water Uptake in PEMFC Catalyst Layers

    E-Print Network [OSTI]

    Gunterman, Haluna P.

    2013-01-01

    the University of California. Water Uptake in PEMFC CatalystUniversity, Montreal, QC, CAN Water uptake profiles of80 kPa to eject imbibed water. Comparison of materials made

  3. Combustion Catalysts in Industry- An Update 

    E-Print Network [OSTI]

    Merrell, G. A.; Knight, R. S.

    1985-01-01

    combustibles in the refuse and help a plant attain emissions compliance requirements that are not always achieved with pollution-control equipment. Combustion catalysts promote the combustion process by lowering the ignition temperature of the fuel, allowing...

  4. Extended Platinum Nanotubes as Fuel Cell Catalysts

    SciTech Connect (OSTI)

    Alia, S.; Pivovar, B. S.; Yan, Y.

    2012-01-01

    Energy consumption has relied principally on fossil fuels as an energy source; fuel cells, however, can provide a clean and sustainable alternative, an answer to the depletion and climate change concerns of fossil fuels. Within proton exchange membrane fuel cells, high catalyst cost and poor durability limit the commercial viability of the device. Recently, platinum nanotubes (PtNTs) were studied as durable, active catalysts, providing a platform to meet US Department of Energy vehicular activity targets.[1] Porous PtNTs were developed to increase nanotube surface area, improving mass activity for oxygen reduction without sacrificing durability.[2] Subsurface platinum was then replaced with palladium, forming platinum-coated palladium nanotubes.[3] By forming a core shell structure, platinum utilization was increased, reducing catalyst cost. Alternative substrates have also been examined, modifying platinum surface facets and increasing oxygen reduction specific activity. Through modification of the PtNT platform, catalyst limitations can be reduced, ensuring a commercially viable device.

  5. 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.

  6. Single-layer transition metal sulfide catalysts

    DOE Patents [OSTI]

    Thoma, Steven G. (Albuquerque, NM)

    2011-05-31

    Transition Metal Sulfides (TMS), such as molybdenum disulfide (MoS.sub.2), are the petroleum industry's "workhorse" catalysts for upgrading heavy petroleum feedstocks and removing sulfur, nitrogen and other pollutants from fuels. We have developed an improved synthesis technique to produce SLTMS catalysts, such as molybdenum disulfide, with potentially greater activity and specificity than those currently available. Applications for this technology include heavy feed upgrading, in-situ catalysis, bio-fuel conversion and coal liquefaction.

  7. Hydrocarbon zeolite catalyst employed in hydrocracking process

    SciTech Connect (OSTI)

    Ward, J.W.

    1987-05-12

    A hydrocracking process is described which comprises contacting a hydrocarbon feedstock under hydrocracking conditions with hydrogen in the presence of a catalyst comprising at least one hydrogenation component, a crystalline aluminosilicate zeolite having catalytic activity for cracking hydrocarbons, and a dispersion of silica-alumina in a matrix consisting essentially of alumina, wherein the catalyst comprises particles in the shape of a three-leaf clover.

  8. Catalyst and method for aqueous phase reactions

    DOE Patents [OSTI]

    Elliott, Douglas C. (Richland, WA); Hart, Todd R. (Kennewick, WA)

    1999-01-01

    The present invention is a catalyst in the form of a plurality of porous particles wherein each particle is a support having nickel metal catalytic phase or reduced nickel deposited thereon in a first dispersed phase and an additional metal deposited onto the support in a second dispersed phase. The additional metal is effective in retarding or reducing agglomeration or sintering of the nickel metal catalytic phase without substantially affecting the catalytic activity, thereby increasing the life time of the catalyst.

  9. Cationic Ruthenium Catalysts for Olefin Hydrovinylation 

    E-Print Network [OSTI]

    Sanchez, Richard P., Jr

    2010-01-14

    of the Hydrovinylation Reaction ................................. 1 1.2 Mechanism of the Hydrovinylation Reaction........................... 4 1.3 Nickel and Palladium Catalyzed Reactions.............................. 6 1.4 Ruthenium Catalyzed Reactions... to form followed by isomerization to give the observed product. Ph Ph Me Ph Me Me RhCl3?3H2O 1000 atm ethylene MeOH, 50 ?C (6) Few catalysts had been used in early studies, but typically nickel and palladium catalysts were used due to their higher...

  10. Nanoparticle growth Controlled Growth of Platinum Nanoparticles on Strontium

    E-Print Network [OSTI]

    Poeppelmeier, Kenneth R.

    on complex support geometries, such as aerogels, porous structures, and other nanoparticles. Efficient

  11. Beam-deposited platinum as versatile catalyst for bottom-up silicon nanowire synthesis

    SciTech Connect (OSTI)

    Hibst, N.; Strehle, S. [Institute of Electron Devices and Circuits, Ulm University, Albert-Einstein-Allee 45, 89081 Ulm (Germany); Knittel, P.; Kranz, C.; Mizaikoff, B. [Institute of Analytical and Bioanalytical Chemistry, Ulm University, Albert-Einstein-Allee 11, 89081 Ulm (Germany)

    2014-10-13

    The controlled localized bottom-up synthesis of silicon nanowires on arbitrarily shaped surfaces is still a persisting challenge for functional device assembly. In order to address this issue, electron beam and focused ion beam-assisted catalyst deposition have been investigated with respect to platinum expected to form a PtSi alloy catalyst for a subsequent bottom-up nanowire synthesis. The effective implementation of pure platinum nanoparticles or thin films for silicon nanowire growth has been demonstrated recently. Beam-deposited platinum contains significant quantities of amorphous carbon due to the organic precursor and gallium ions for a focused ion beam-based deposition process. Nevertheless, silicon nanowires could be grown on various substrates regardless of the platinum purity. Additionally, p-type doping could be realized with diborane whereas n-type doping suppressed a nanowire growth. The rational utilization of this beam-assisted approach enables us to control the localized synthesis of single silicon nanowires at planar surfaces but succeeded also in single nanowire growth at the three-dimensional apex of an atomic force microscopy tip. Therefore, this catalyst deposition method appears to be a unique extension of current technologies to assemble complex nanowire-based devices.

  12. Low temperature catalysts for methanol production

    DOE Patents [OSTI]

    Sapienza, Richard S. (1 Miller Ave., Shoreham, NY 11786); Slegeir, William A. (7 Florence Rd., Hampton Bays, NY 11946); O'Hare, Thomas E. (11 Geiger Pl., Huntington Station, NY 11746); Mahajan, Devinder (14 Locust Ct., Selden, NY 11784)

    1986-01-01

    A catalyst and process useful at low temperatures (below about 160.degree. C.) and preferably in the range 80.degree.-120.degree. C. used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa--M(OAc).sub.2 where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M=Ni and R=tertiary amyl). Mo(CO).sub.6 is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  13. Low temperature catalysts for methanol production

    DOE Patents [OSTI]

    Sapienza, R.S.; Slegeir, W.A.; O'Hare, T.E.; Mahajan, D.

    1985-03-12

    A catalyst and process useful at low temperatures (below about 160/sup 0/C) and preferably in the range 80 to 120/sup 0/C used in the production of methanol from carbon monoxide and hydrogen is disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH-RONa-M(OAc)/sub 2/ where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1 to 6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is Nic (where M = Ni and R = tertiary amyl). Mo(CO)/sub 6/ is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  14. Low temperature catalysts for methanol production

    DOE Patents [OSTI]

    Sapienza, R.S.; Slegeir, W.A.; O'Hare, T.E.; Mahajan, D.

    1986-10-28

    A catalyst and process useful at low temperatures (below about 160 C) and preferably in the range 80--120 C used in the production of methanol from carbon monoxide and hydrogen are disclosed. The catalyst is used in slurry form and comprises a complex reducing agent derived from the component structure NaH--RONa-M(OAc)[sub 2] where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1-6 carbon atoms. This catalyst is preferably used alone but is also effective in combination with a metal carbonyl of a group VI (Mo, Cr, W) metal. The preferred catalyst precursor is NiC (where M = Ni and R = tertiary amyl). Mo(CO)[sub 6] is the preferred metal carbonyl if such component is used. The catalyst is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  15. 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 PI’s 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 PI’s 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.

  16. New applications of noble metal catalysts in hydrocracking

    SciTech Connect (OSTI)

    Mitchell, D.H.G.; Bertram, R.V. [UOP, Des Plaines, IL (United States); Dencker, G.D. [Marathon Oil Co., Robinson, IL (United States). Illinois Refining Div.

    1995-09-01

    The paper explores how a noble metal hydrocracking catalyst functions stably in a hydrogen sulfide and ammonia environment and, in particular, how the physical positioning of the noble metal molecules affects catalyst performance. A commercial example, HC-28 catalyst in the Unicracking unit at Marathon Oil Refinery in Robinson, Illinois, demonstrates the success of the noble metal catalyst approach for naphtha production. In addition, a new Unicracking catalyst, HC-35, which uses a noble metal component to produce high-quality middle distillates, is introduced. The paper also shows how refiners may derive increased economic and operational benefits from their catalyst investment by using the latest developments in reactor internals design.

  17. 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.

  18. Dispersed metal cluster catalysts by design. Synthesis, characterization, structure, and performance

    SciTech Connect (OSTI)

    Arslan, Ilke; Dixon, David A.; Gates, Bruce C.; Katz, Alexander

    2015-09-30

    To understand the class of metal cluster catalysts better and to lay a foundation for the prediction of properties leading to improved catalysts, we have synthesized metal catalysts with well-defined structures and varied the cluster structures and compositions systematically—including the ligands bonded to the metals. These ligands include supports and bulky organics that are being tuned to control both the electron transfer to or from the metal and the accessibility of reactants to influence catalytic properties. We have developed novel syntheses to prepare these well-defined catalysts with atomic-scale control the environment by choice and placement of ligands and applied state-of-the art spectroscopic, microscopic, and computational methods to determine their structures, reactivities, and catalytic properties. The ligands range from nearly flat MgO surfaces to enveloping zeolites to bulky calixarenes to provide controlled coverages of the metal clusters, while also enforcing unprecedented degrees of coordinative unsaturation at the metal site—thereby facilitating bonding and catalysis events at exposed metal atoms. With this wide range of ligand properties and our arsenal of characterization tools, we worked to achieve a deep, fundamental understanding of how to synthesize robust supported and ligand-modified metal clusters with controlled catalytic properties, thereby bridging the gap between active site structure and function in unsupported and supported metal catalysts. We used methods of organometallic and inorganic chemistry combined with surface chemistry for the precise synthesis of metal clusters and nanoparticles, characterizing them at various stages of preparation and under various conditions (including catalytic reaction conditions) and determining their structures and reactivities and how their catalytic properties depend on their compositions and structures. Key characterization methods included IR, NMR, and EXAFS spectroscopies to identify ligands on the metals and their reactions; EXAFS spectroscopy and high-resolution STEM to determine cluster framework structures and changes resulting from reactant treatment and locations of metal atoms on support surfaces; X-ray diffraction crystallography to determine full structures of cluster-ligand combinations in the absence of a support, and TEM with tomographic methods to observe individual metal atoms and determine three-dimensional structures of catalysts. Electronic structure calculations were used to verify and interpret spectra and extend the understanding of reactivity beyond what is measurable experimentally.

  19. Nanoparticle Emissions from Internal Combustion Engines | Department...

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

    Nanoparticle Emissions from Internal Combustion Engines Nanoparticle Emissions from Internal Combustion Engines 2004 Diesel Engine Emissions Reduction (DEER) Conference...

  20. Development of Ultra-low Platinum Alloy Cathode Catalyst for...

    Energy Savers [EERE]

    Development of Ultra-low Platinum Alloy Cathode Catalyst for PEM Fuel Cells Development of Ultra-low Platinum Alloy Cathode Catalyst for PEM Fuel Cells These slides were presented...

  1. Atomic-Scale Observations Aid Mesoscale Catalyst Design | ornl...

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

    Materials Characterization Atomic-Scale Observations Aid Mesoscale Catalyst Design April 08, 2015 Fig.1. Z-contrast STEM image shows the Mo-V-Te-Ta oxide catalyst. (a) "M1-like"...

  2. Modified zeolite-based catalyst for effective extinction hydrocracking

    SciTech Connect (OSTI)

    Yan, T.Y. (Mobil Research and Development Corp., Princeton, NJ (USA))

    1989-10-01

    The shape selectivity of zeolites makes them generally ineffective for extinction hydrocracking of polycyclic aromatic feeds. To overcome this problem, the zeolite can be modified with an amorphous cracking component to form a composite catalyst. This composite catalyst will be effective for extinction hydrocracking and retain the superior performance characteristics of a zeolite catalyst at the same time because the zeolite and the amorphous components of the catalyst operate complementarily. To illustrate this principle, NiW/REX-NiW/SiO/sub 2/Al/sub 2/O/sub 3/ composite catalyst was tested in the pilot plant. It was active, low in aging rate, resistant to nitrogen poisoning and high in selectivities for naphthas. The aged catalyst could be oxidatively regenerated to fully recover the activity and the product selectivities. This composite catalyst was superior to both individual (zeolite and amorphous) components for extinction hydrocracking. Catalysts similar to this have been used commercially for many years.

  3. Enhancement of alkylation catalysts for improved supercritical fluid regeneration

    DOE Patents [OSTI]

    Ginosar, Daniel M. (Idaho Falls, ID); Petkovic, Lucia M. (Idaho Falls, ID)

    2010-12-28

    A method of modifying an alkylation catalyst to reduce the formation of condensed hydrocarbon species thereon. The method comprises providing an alkylation catalyst comprising a plurality of active sites. The plurality of active sites on the alkylation catalyst may include a plurality of weakly acidic active sites, intermediate acidity active sites, and strongly acidic active sites. A base is adsorbed to a portion of the plurality of active sites, such as the strongly acidic active sites, selectively poisoning the strongly acidic active sites. A method of modifying the alkylation catalyst by providing an alkylation catalyst comprising a pore size distribution that sterically constrains formation of the condensed hydrocarbon species on the alkylation catalyst or by synthesizing the alkylation catalyst to comprise a decreased number of strongly acidic active sites is also disclosed, as is a method of improving a regeneration efficiency of the alkylation catalyst.

  4. Enhancement of alkylation catalysts for improved supercritical fluid regeneration

    DOE Patents [OSTI]

    Ginosar, Daniel M. (Idaho Falls, ID); Petkovic, Lucia (Idaho Falls, ID)

    2009-09-22

    A method of modifying an alkylation catalyst to reduce the formation of condensed hydrocarbon species thereon. The method comprises providing an alkylation catalyst comprising a plurality of active sites. The plurality of active sites on the alkylation catalyst may include a plurality of weakly acidic active sites, intermediate acidity active sites, and strongly acidic active sites. A base is adsorbed to a portion of the plurality of active sites, such as the strongly acidic active sites, selectively poisoning the strongly acidic active sites. A method of modifying the alkylation catalyst by providing an alkylation catalyst comprising a pore size distribution that sterically constrains formation of the condensed hydrocarbon species on the alkylation catalyst or by synthesizing the alkylation catalyst to comprise a decreased number of strongly acidic active sites is also disclosed, as is a method of improving a regeneration efficiency of the alkylation catalyst.

  5. Los Alamos catalyst could jumpstart e-cars, green energy

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

    Catalyst could jumpstart e-cars, green energy Los Alamos catalyst could jumpstart e-cars, green energy The new material has the highest oxygen reduction reaction (ORR) activity in...

  6. Catalysts for oxidation of mercury in flue gas

    DOE Patents [OSTI]

    Granite, Evan J. (Wexford, PA); Pennline, Henry W. (Bethel Park, PA)

    2010-08-17

    Two new classes of catalysts for the removal of heavy metal contaminants, especially mercury (Hg) from effluent gases. Both of these classes of catalysts are excellent absorbers of HCl and Cl.sub.2 present in effluent gases. This adsorption of oxidizing agents aids in the oxidation of heavy metal contaminants. The catalysts remove mercury by oxidizing the Hg into mercury (II) moieties. For one class of catalysts, the active component is selected from the group consisting of iridium (Ir) and iridum-platinum (Ir/Pt) alloys. The Ir and Ir/Pt alloy catalysts are especially corrosion resistant. For the other class of catalyst, the active component is partially combusted coal or "Thief" carbon impregnated with Cl.sub.2. Untreated Thief carbon catalyst can be self-activating in the presence of effluent gas streams. The Thief carbon catalyst is disposable by means of capture from the effluent gas stream in a particulate collection device (PCD).

  7. Long term experiences with HDD SCR Catalysts | Department of...

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

    HDD SCR Catalysts Test bench results and on-road experiences of more than 1 million km offer comparisons of fresh and used catalyst activity and NOx conversion capability using...

  8. Applications of hydrogenation and dehydrogenation on noble metal catalysts 

    E-Print Network [OSTI]

    Wang, Bo

    2009-05-15

    Hydrogenation and dehydrogenation on Pd- and Pt- catalysts are encountered in many industrial hydrocarbon processes. The present work considers the development of catalysts and their kinetic modeling along a general and rigorous approach. The first...

  9. Volatility of Vanadia from Vanadia-Based SCR Catalysts under...

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

    Vanadia from Vanadia-Based SCR Catalysts under Accelerated Aging Conditions Volatility of Vanadia from Vanadia-Based SCR Catalysts under Accelerated Aging Conditions TiO2-supported...

  10. Understanding the Deactivation Mechanisms of Cu/Zeolite SCR Catalysts...

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

    of CuZeolite urea-SCR catalysts in diesel applications, the effects of engine and lab aging on catalyst reactivity and material properties were investigated. deer08cheng.pdf...

  11. The Effects of Hydrothermal Agingon a Commercial Cu SCR Catalyst...

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

    Hydrothermal Agingon a Commercial Cu SCR Catalyst Examines the effect of hydrothermal aging on the Nox reduction over a commercial Cu-zeolite SCR catalyst. deer11lee.pdf More...

  12. Ship-in-a-bottle catalysts

    DOE Patents [OSTI]

    Haw, James F.; Song, Weiguo

    2006-07-18

    In accordance with the present invention there is provided a novel catalyst system in which the catalytic structure is tailormade at the nanometer scale using the invention's novel ship-in-a-bottle synthesis techniques. The invention describes modified forms of solid catalysts for use in heterogeneous catalysis that have a microporous structure defined by nanocages. Examples include zeolites, SAPOs, and analogous materials that have the controlled pore dimensions and hydrothermal stability required for many industrial processes. The invention provides for modification of these catalysts using reagents that are small enough to pass through the windows used to access the cages. The small reagents are then reacted to form larger molecules in the cages.

  13. Homogeneous catalyst formulations for methanol production

    DOE Patents [OSTI]

    Mahajan, Devinder (Port Jefferson, NY); Sapienza, Richard S. (Shoreham, NY); Slegeir, William A. (Hampton Bays, NY); O'Hare, Thomas E. (Huntington Station, NY)

    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.

  14. Homogeneous catalyst formulations for methanol production

    DOE Patents [OSTI]

    Mahajan, Devinder (Port Jefferson, NY); Sapienza, Richard S. (Shoreham, NY); Slegeir, William A. (Hampton Bays, NY); O'Hare, Thomas E. (Huntington Station, NY)

    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.

  15. Method for producing catalysts from coal

    DOE Patents [OSTI]

    Farcasiu, M.; Derbyshire, F.; Kaufman, P.B.; Jagtoyen, M.

    1998-02-24

    A method for producing catalysts from coal is provided comprising mixing an aqueous alkali solution with the coal, heating the aqueous mixture to treat the coal, drying the now-heated aqueous mixture, reheating the mixture to form carbonized material, cooling the mixture, removing excess alkali from the carbonized material, and recovering the carbonized material, wherein the entire process is carried out in controlled atmospheres, and the carbonized material is a hydrocracking or hydrodehalogenation catalyst for liquid phase reactions. The invention also provides for a one-step method for producing catalysts from coal comprising mixing an aqueous alkali solution with the coal to create a mixture, heating the aqueous mixture from an ambient temperature to a predetermined temperature at a predetermined rate, cooling the mixture, and washing the mixture to remove excess alkali from the treated and carbonized material, wherein the entire process is carried out in a controlled atmosphere. 1 fig.

  16. Protein Scaffolding for Small Molecule Catalysts

    SciTech Connect (OSTI)

    Baker, David [Univ. of Washington, Seattle, WA (United States)

    2014-09-14

    We aim to design hybrid catalysts for energy production and storage that combine the high specificity, affinity, and tunability of proteins with the potent chemical reactivities of small organometallic molecules. The widely used Rosetta and RosettaDesign methodologies will be extended to model novel protein / small molecule catalysts in which one or many small molecule active centers are supported and coordinated by protein scaffolding. The promise of such hybrid molecular systems will be demonstrated with the nickel-phosphine hydrogenase of DuBois et. al.We will enhance the hydrogenase activity of the catalyst by designing protein scaffolds that incorporate proton relays and systematically modulate the local environment of the catalyticcenter. In collaboration with DuBois and Shaw, the designs will be experimentally synthesized and characterized.

  17. Low temperature catalyst system for methanol production

    DOE Patents [OSTI]

    Sapienza, R.S.; Slegeir, W.A.; O'Hare, T.E.

    1984-04-20

    This patent discloses a catalyst and process useful at low temperatures (150/sup 0/C) and preferably in the range 80 to 120/sup 0/C used in the production of methanol from carbon monoxide and hydrogen. The catalyst components are used in slurry form and comprise (1) a complex reducing agent derived from the component structure NaH-ROH-M(OAc)/sub 2/ where M is selected from the group consisting of Ni, Pd, and Co and R is a lower alkyl group containing 1 to 6 carbon atoms and (2) a metal carbonyl of a group VI (Mo, Cr, W) metal. For the first component, Nic is preferred (where M = Ni and R = tertiary amyl). For the second component, Mo(CO)/sub 6/ is preferred. The mixture is subjected to a conditioning or activating step under temperature and pressure, similar to the parameters given above, to afford the active catalyst.

  18. Method for dispersing catalyst onto particulate material

    DOE Patents [OSTI]

    Utz, Bruce R. (Pittsburgh, PA); Cugini, Anthony V. (Pittsburgh, PA)

    1992-01-01

    A method for dispersing finely divided catalyst precursors onto the surface of coal or other particulate material includes the steps of forming a wet paste mixture of the particulate material and a liquid solution containing a dissolved transition metal salt, for instance a solution of ferric nitrate. The wet paste mixture is in a state of incipient wetness with all of this solution adsorbed onto the surfaces of the particulate material without the presence of free moisture. On adding a precipitating agent such as ammonia, a catalyst precursor such as hydrated iron oxide is deposited on the surfaces of the coal. The catalyst is activated by converting it to the sulfide form for the hydrogenation or direct liquefaction of the coal.

  19. Pyrochlore catalysts for hydrocarbon fuel reforming

    DOE Patents [OSTI]

    Berry, David A.; Shekhawat, Dushyant; Haynes, Daniel; Smith, Mark; Spivey, James J.

    2012-08-14

    A method of catalytically reforming a reactant gas mixture using a pyrochlore catalyst material comprised of one or more pyrochlores having the composition A2B2-y-zB'yB"zO7-.DELTA., where y>0 and z.gtoreq.0. Distribution of catalytically active metals throughout the structure at the B site creates an active and well dispersed metal locked into place in the crystal structure. This greatly reduces the metal sintering that typically occurs on supported catalysts used in reforming reactions, and reduces deactivation by sulfur and carbon. Further, oxygen mobility may also be enhanced by elemental exchange of promoters at sites in the pyrochlore. The pyrochlore catalyst material may be utilized in catalytic reforming reactions for the conversion of hydrocarbon fuels into synthesis gas (H2+CO) for fuel cells, among other uses.

  20. Colloidal synthesis and characterization of carbon-supported Pd-Cu nanoparticle oxygen reduction electrocatalysts.

    SciTech Connect (OSTI)

    Kariuki, N. N.; Wang, X.; Mawdsley, J. R.; Ferrandon, M. S.; Niyogi, S. G.; Vaughey, J. T.; Myers, D. J.; Chemical Sciences and Engineering Division

    2010-07-27

    The ability to control the size and composition of metal or alloys nanoparticles is important in preparing catalysts. This paper reports a colloidal synthesis methodology for the preparation of monodisperse palladium-copper (Pd-Cu) alloy nanoparticles with an average diameter of 3 nm for the as-prepared particles and 5-10 nm upon removal of the capping agents. Our approach involves the use of metal precursors, capping agents, and reducing agents in controlled ratios for nanoparticle formation in a single organic phase, followed by deposition of the capped nanoparticles on high surface area carbon and removal of the capping agents via heat treatment in either oxidizing or reducing atmosphere. The results of characterizations using transmission electron microscopy-energy dispersive X-ray analysis (TEM-EDX), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), temperature programmed oxidation and reduction combined with mass spectrometry (TPO/TPR-MS), powder X-ray diffraction (XRD), and cyclic voltammetry (CV) are discussed. The resulting high-surface-area-carbon-supported Pd-Cu catalysts (PdCu/C) showed high activity for the oxygen reduction reaction (ORR) in acidic electrolyte. Our study revealed composition and heat-treatment dependent ORR activity.

  1. Thief carbon catalyst for oxidation of mercury in effluent stream

    DOE Patents [OSTI]

    Granite, Evan J. (Wexford, PA); Pennline, Henry W. (Bethel Park, PA)

    2011-12-06

    A catalyst for the oxidation of heavy metal contaminants, especially mercury (Hg), in an effluent stream is presented. The catalyst facilitates removal of mercury through the oxidation of elemental Hg into mercury (II) moieties. The active component of the catalyst is partially combusted coal, or "Thief" carbon, which can be pre-treated with a halogen. An untreated Thief carbon catalyst can be self-promoting in the presence of an effluent gas streams entrained with a halogen.

  2. Numerical study of reaction in porous catalysts under composition modulation

    E-Print Network [OSTI]

    Hsiao, Hsu-Wen

    2010-01-01

    in monolithic NOx storage and reduction catalyst." Topics in2007). "Model for NOx storage/reduction in the presence of

  3. Catalyst structure and method of fischer-tropsch synthesis

    DOE Patents [OSTI]

    Wang, Yong [Richland, WA; Vanderwiel, David P [Richland, WA; Tonkovich, Anna Lee Y [Pasco, WA; Gao, Yufei [Kennewick, WA; Baker, Eddie G [Pasco, WA

    2002-12-10

    The present invention includes Fischer-Tropsch catalysts, reactions using Fischer-Tropsch catalysts, methods of making Fischer-Tropsch catalysts, processes of hydrogenating carbon monoxide, and fuels made using these processes. The invention provides the ability to hydrogenate carbon monoxide with low contact times, good conversion rates and low methane selectivities. In a preferred method, the catalyst is made using a metal foam support.

  4. Catalyst structure and method of Fischer-Tropsch synthesis

    DOE Patents [OSTI]

    Wang, Yong; Vanderwiel, David P.; Tonkovich, Anna Lee Y.; Gao, Yufei; Baker, Eddie G.

    2004-06-15

    The present invention includes Fischer-Tropsch catalysts, reactions using Fischer-Tropsch catalysts, methods of making Fischer-Tropsch catalysts, processes of hydrogenating carbon monoxide, and fuels made using these processes. The invention provides the ability to hydrogenate carbon monoxide with low contact times, good conversion rates and low methane selectivities. In a preferred method, the catalyst is made using a metal foam support.

  5. Substituted pyridine ligands and related water-soluble catalysts

    DOE Patents [OSTI]

    Emrick, Todd S. (Deerfield, MA)

    2011-06-14

    Versatile Group VIII metathesis catalysts, as can be used in a range of polymerization reactions and other chemical methodologies.

  6. 90 Seconds of Discovery: Biofuel Catalyst Life and Plugs

    ScienceCinema (OSTI)

    Zacher, Alan; Olarte, Mariefel

    2014-06-12

    Scientist at PNNL are working to extend the life of the catalysts used in the production of biomass fuels.

  7. 90 Seconds of Discovery: Biofuel Catalyst Life and Plugs

    SciTech Connect (OSTI)

    Zacher, Alan; Olarte, Mariefel

    2014-06-11

    Scientist at PNNL are working to extend the life of the catalysts used in the production of biomass fuels.

  8. Tethered catalysts for the hydration of carbon dioxide

    SciTech Connect (OSTI)

    Valdez, Carlos A; Satcher, Jr., Joe H; Aines, Roger D; Wong, Sergio E; Baker, Sarah E; Lightstone, Felice C; Stolaroff, Joshuah K

    2014-11-04

    A system is provided that substantially increases the efficiency of CO.sub.2 capture and removal by positioning a catalyst within an optimal distance from the air-liquid interface. The catalyst is positioned within the layer determined to be the highest concentration of carbon dioxide. A hydrophobic tether is attached to the catalyst and the hydrophobic tether modulates the position of the catalyst within the liquid layer containing the highest concentration of carbon dioxide.

  9. Catalyst for converting synthesis gas to liquid motor fuels

    DOE Patents [OSTI]

    Coughlin, Peter K. (Yorktown Heights, NY)

    1986-01-01

    The addition of an inert metal component, such as gold, silver or copper, to a Fischer-Tropsch catalyst comprising cobalt enables said catalyst to convert synthesis gas to liquid motor fuels at about 240.degree.-370.degree. C. with advantageously reduced selectivity of said cobalt for methane in said conversion. The catalyst composition can advantageously include a support component, such as a molecular sieve, co-catalyst/support component or a combination of such support components.

  10. The Challenges for PEMFC Catalysts in Automotive Applications

    Broader source: Energy.gov [DOE]

    Presentation by Stephen Campbell for the 2013 DOE Catalysis Working Group Meeting on PEMFC catalysts in automotive applications.

  11. Thermally Polymerized Rylene Nanoparticles

    E-Print Network [OSTI]

    Andrew, Trisha Lionel

    Rylene dyes functionalized with varying numbers of phenyl trifluorovinyl ether (TFVE) moieties were subjected to a thermal emulsion polymerization to yield shape-persistent, water-soluble chromophore nanoparticles. Perylene ...

  12. Magnetic nanoparticle temperature estimation

    SciTech Connect (OSTI)

    Weaver, John B.; Rauwerdink, Adam M.; Hansen, Eric W.

    2009-05-15

    The authors present a method of measuring the temperature of magnetic nanoparticles that can be adapted to provide in vivo temperature maps. Many of the minimally invasive therapies that promise to reduce health care costs and improve patient outcomes heat tissue to very specific temperatures to be effective. Measurements are required because physiological cooling, primarily blood flow, makes the temperature difficult to predict a priori. The ratio of the fifth and third harmonics of the magnetization generated by magnetic nanoparticles in a sinusoidal field is used to generate a calibration curve and to subsequently estimate the temperature. The calibration curve is obtained by varying the amplitude of the sinusoidal field. The temperature can then be estimated from any subsequent measurement of the ratio. The accuracy was 0.3 deg. K between 20 and 50 deg. C using the current apparatus and half-second measurements. The method is independent of nanoparticle concentration and nanoparticle size distribution.

  13. Divalent metal nanoparticles

    E-Print Network [OSTI]

    DeVries, Gretchen Anne

    2008-01-01

    Metal nanoparticles hold promise for many scientific and technological applications, such as chemical and biological sensors, vehicles for drug delivery, and subdiffraction limit waveguides. To fabricate such devices, a ...

  14. CdO-CdS nano-composites as improved photo-catalysts for the generation of hydrogen from water

    SciTech Connect (OSTI)

    Kahane, Shital V.; Mahamuni, Shailaja; Sasikala, R.; Sudarsan, V.

    2014-04-24

    CdO-CdS nanocomposites were prepared by polyol method followed by heating at 300°C. XRD study confirmed the atomic scale mixing of CdO and CdS nanoparticles, leading to the formation of CdSO{sub 3} phase at the interfacial region between CdO and CdS. The enhancement in photo-catalytic activity for hydrogen generation from water is observed in case of CdO-CdS nanocomposites compared to individual CdS and CdO nanoparticles. Based on XRD, steady state and time resolved luminescence studies and surface area measurements, it is determined that, the fine mixing of CdS and CdO, higher surface area of the composite sample and increase in lifetime of the charge carriers are responsible for the observed increase in hydrogen yield from water when composite sample was used as the photo-catalyst compared to individual components.

  15. Method for producing iron-based catalysts

    DOE Patents [OSTI]

    Farcasiu, Malvina (Pittsburgh, PA); Kaufman, Phillip B. (Library, PA); Diehl, J. Rodney (Pittsburgh, PA); Kathrein, Hendrik (McMurray, PA)

    1999-01-01

    A method for preparing an acid catalyst having a long shelf-life is provided comprising doping crystalline iron oxides with lattice-compatible metals and heating the now-doped oxide with halogen compounds at elevated temperatures. The invention also provides for a catalyst comprising an iron oxide particle having a predetermined lattice structure, one or more metal dopants for said iron oxide, said dopants having an ionic radius compatible with said lattice structure; and a halogen bound with the iron and the metal dopants on the surface of the particle.

  16. Catalysts for lean burn engine exhaust abatement

    DOE Patents [OSTI]

    Ott, Kevin C. (Los Alamos, NM); Clark, Noline C. (Jemez Springs, NM); Paffett, Mark T. (Los Alamos, NM)

    2003-01-01

    The present invention provides a process for catalytically reducing nitrogen oxides in an exhaust gas stream containing nitrogen oxides and a reductant material by contacting the gas stream under conditions effective to catalytically reduce the nitrogen oxides with a catalyst comprising a aluminum-silicate type material and a minor amount of a metal, the catalyst characterized as having sufficient catalytic activity so as to reduce the nitrogen oxides by at least 60 percent under temperatures within the range of from about 200.degree. C. to about 400.degree. C.

  17. The Chemical Composition and Structure of Supported Sulfated Zirconia with Regulated Size Nanoparticles

    SciTech Connect (OSTI)

    Kanazhevskiy, V. V.; Shmachkova, V. P.; Kotsarenko, N. S.; Kochubey, D. I.; Vedrine, J. C.

    2007-02-02

    A set of model skeletal isomerization catalysts - sulfated zirconia nanoparticles of controlled thickness anchored on different supports - was prepared using colloidal solutions of Zr salt on titania as support. The nanoparticles of zirconia (1-5 nm) are epitaxially connected to the support surface, with S/Zr ratio equals to 1.3-1.5. It was shown by EXAFS that nanoparticles of non-stoichiometric zirconium sulfate Zr(SO4)1+x, where x<0.5, are formed on the support surface. Its structure looks like half-period shifted counterdirected chains built-up by zirconium atoms linked by triangle pyramids of sulfate groups. Considering catalytic data of skeletal n-butane isomerisation at 150 deg. C, one can suggest that these species behave as the active component of sulfated zirconia. They are formed in subsurface layers as zirconium hydroxide undergoes sulfation followed by thermal treatment.

  18. Engineering Pharmaceutical Nanoparticles

    E-Print Network [OSTI]

    Berkland, Cory

    2006-10-26

    Engineering Pharmaceutical Nanoparticles Cory Berkland Assistant Professor Department of Pharmaceutical Chemistry Assistant Professor Department of Chemical and Petroleum Engineering The University of Kansas 2 Acknowledgements Postdocs: David Shi... Technology #0;z Supercritical Fluids #0;z Polymer Nanoparticles #0;z Molecular Technology/Polyplexes #0;z Block copolymers ? micelles #0;z Liposomes/Polymersomes #0;z Polymer/Drug conjugates #0;z Berkland Lab 14 Milling/Spraying Technology 15 Wet milling...

  19. Decorating multi-walled carbon nanotubes with nickel nanoparticles for selective hydrogenation of citral

    SciTech Connect (OSTI)

    Tang Yuechao; Yang Dong; Qin Feng; Hu Jianhua; Wang Changchun; Xu Hualong

    2009-08-15

    The nanocomposites of multi-walled carbon nanotubes (MWNTs) decorated with nickel nanoparticles were conveniently prepared by a chemical reduction of nickel salt in the present of poly(acrylic acid) grafted MWNTs (PAA-g-MWNTs). Due to the strong interaction between Ni{sup 2+} and -COOH, PAA-g-MWNTs became an excellent supporting material for Ni nanoparticles. The morphology and distribution of Ni nanoparticles on the surface of MWNTs were greatly influenced by the reduction temperatures, the experimental results also showed that the distribution of Ni nanoparticles was greatly improved while the MWNTs were modified by poly(acrylic acid) (PAA). The hydrogenation activity and selectivity of MWNTs decorated with Ni nanoparticles (Ni-MWNTs) for alpha, beta-unsaturated aldehyde (citral) were also studied, and the experimental results showed that the citronellal, an important raw material for flavoring and perfumery industries, is the favorable product with a percentage as high as 86.9%, which is 7 times higher than that of catalyst by Ni-supported active carbon (Ni-AC). - Abstract: Nickel nanoparticles decorated multi-walled carbon nanotubes (Ni-MWNTs) nanocomposites were conveniently prepared by a chemical reduction of nickel salt in the present of poly(acrylic acid) grafted MWNTs (PAA-g-MWNTs). These nanocomposites possessed excellent catalytic activity and selectivity for hydrogenation of citral.

  20. Cobalt Fischer-Tropsch catalysts having improved selectivity

    DOE Patents [OSTI]

    Miller, James G. (Pearl River, NY); Rabo, Jule A. (Armonk, NY)

    1989-01-01

    The promoter(s) Mn oxide or Mn oxide and Zr oxide are added to a cobalt Fischer-Tropsch catalyst combined with the molecular sieve TC-103 or TC-123 such that the resultant catalyst demonstrates improved product selectivity, stability and catalyst life. The improved selectivity is evidenced by lower methane production, higher C5+ yield and increased olefin production.

  1. Supported metal catalysts for alcohol/sugar alcohol steam reforming

    SciTech Connect (OSTI)

    Davidson, Stephen; Zhang, He; Sun, Junming; Wang, Yong

    2014-08-21

    Despite extensive studies on hydrogen production via steam reforming of alcohols and sugar alcohols, catalysts typically suffer a variety of issues from poor hydrogen selectivity to rapid deactivation. Here, we summarize recent advances in fundamental understanding of functionality and structure of catalysts for alcohol/sugar alcohol steam reforming, and provide perspectives on further development required to design highly efficient steam reforming catalysts.

  2. Reaction Rates and Catalysts in Ethanol Production (1 Activity)

    K-12 Energy Lesson Plans and Activities Web site (EERE)

    Students will have the opportunity to investigate alternative catalysts for the degradation of hydrogen peroxide, which will be used as a model system for the breaking down of cellulose into sugar. After identifying other potential catalysts, students will develop their own research question about catalysts and conduct an additional experiment of their own design to investigate their question.

  3. SOLUBLE POLYMER-SUPPORTED CATALYSTS AND INITIATORS A Dissertation Presented

    E-Print Network [OSTI]

    Venkataraman, Dhandapani "DV"

    SOLUBLE POLYMER-SUPPORTED CATALYSTS AND INITIATORS A Dissertation Presented by UCHE K. ANYANWU. Anyanwu 2005 All Rights Reserved #12;SOLUBLE POLYMER-SUPPORTED CATALYSTS AND INITIATORS A Dissertation it without you guys. Yes Oooh! #12;vi ABSTRACT SOLUBLE POLYMER-SUPPORTED CATALYSTS AND INITIATORS MAY 2005

  4. Nano Catalysts for Diesel Engine Emission Remediation

    SciTech Connect (OSTI)

    Narula, Chaitanya Kumar; Yang, Xiaofan; Debusk, Melanie Moses; Mullins, David R; Mahurin, Shannon Mark; Wu, Zili

    2012-06-01

    The objective of this project was to develop durable zeolite nanocatalysts with broader operating temperature windows to treat diesel engine emissions to enable diesel engine based equipment and vehicles to meet future regulatory requirements. A second objective was to improve hydrothermal durability of zeolite catalysts to at least 675 C. The results presented in this report show that we have successfully achieved both objectives. Since it is accepted that the first step in NO{sub x} conversion under SCR (selective catalytic reduction) conditions involves NO oxidation to NO{sub 2}, we reasoned that catalyst modification that can enhance NO oxidation at low-temperatures should facilitate NO{sub x} reduction at low temperatures. Considering that Cu-ZSM-5 is a more efficient catalyst than Fe-ZSM-5 at low-temperature, we chose to modify Cu-ZSM-5. It is important to point out that the poor low-temperature efficiency of Fe-ZSM-5 has been shown to be due to selective absorption of NH{sub 3} at low-temperatures rather than poor NO oxidation activity. In view of this, we also reasoned that an increased electron density on copper in Cu-ZSM-5 would inhibit any bonding with NH{sub 3} at low-temperatures. In addition to modified Cu-ZSM-5, we synthesized a series of new heterobimetallic zeolites, by incorporating a secondary metal cation M (Sc{sup 3+}, Fe{sup 3+}, In{sup 3+}, and La{sup 3+}) in Cu exchanged ZSM-5, zeolite-beta, and SSZ-13 zeolites under carefully controlled experimental conditions. Characterization by diffuse-reflectance ultra-violet-visible spectroscopy (UV-Vis), X-ray powder diffraction (XRD), extended X-ray absorption fine structure spectroscopy (EXAFS) and electron paramagnetic resonance spectroscopy (EPR) does not permit conclusive structural determination but supports the proposal that M{sup 3+} has been incorporated in the vicinity of Cu(II). The protocols for degreening catalysts, testing under various operating conditions, and accelerated aging conditions were provided by our collaborators at John Deere Power Systems. Among various zeolites reported here, CuFe-SSZ-13 offers the best NO{sub x} conversion activity in 150-650 C range and is hydrothermally stable when tested under accelerated aging conditions. It is important to note that Cu-SSZ-13 is now a commercial catalyst for NO{sub x} treatment on diesel passenger vehicles. Thus, our catalyst performs better than the commercial catalyst under fast SCR conditions. We initially focused on fast SCR tests to enable us to screen catalysts rapidly. Only the catalysts that exhibit high NO{sub x} conversion at low temperatures are selected for screening under varying NO{sub 2}:NO{sub x} ratio. The detailed tests of CuFe-SSZ-13 show that CuFe-SSZ-13 is more effective than commercial Cu-SSZ-13 even at NO{sub 2}:NO{sub x} ratio of 0.1. The mechanistic studies, employing stop-flow diffuse reflectance FTIR spectroscopy (DRIFTS), suggest that high concentration of NO{sup +}, generated by heterobimetallic zeolites, is probably responsible for their superior low temperature NO{sub x} activity. The results described in this report clearly show that we have successfully completed the first step in a new emission treatment catalyst which is synthesis and laboratory testing employing simulated exhaust. The next step in the catalyst development is engine testing. Efforts are in progress to obtain follow-on funding to carry out scale-up and engine testing to facilitate commercialization of this technology.

  5. Nanoparticles synthesis of tungsten disulfide via AOT-based microemulsions

    SciTech Connect (OSTI)

    Ghoreishi, S.M.; Meshkat, S.S.; Department of Chemical Engineering, Urmia University of Technology, Urmia 57155-419 ; Ghiaci, M.; Dadkhah, A.A.

    2012-06-15

    Graphical abstract: A controlled synthesis of WS2 nanoparticles (most probably inorganic fullerene (IF)) via microemulsion was applied for the first time to prepare WS2 (7–12 nm) by acidification of the water cores of the AOT reverse microemulsion. Highlights: ? An innovative reverse microemulsion technique was developed for WS{sub 2} synthesis. ? WS{sub 2} nanoparticles were obtained with narrow size distribution in range of 7–12 nm. ? Operating cost of microemulsion was lower in contrast to quartz reactor method. ? WS{sub 2} morphology could be controlled to obtain highly active and selective catalysts. ? Lower size of WS{sub 2} in this study overcomes the shortcoming of quartz reactor method. -- Abstract: The tungsten disulfide (WS{sub 2}) nanoparticles (most probably inorganic fullerene (IF)) with a narrow size distribution were synthesized by a reverse micelle technique for the first time. The particle size was controlled by varying water-to-surfactant molar ratio (W{sub 0}), aging time and reagent concentration. The synthesized WS{sub 2} nanoparticles were characterized by zetasizer, UV–visible spectrophotometers and transmission electron microscopy (TEM). The WS{sub 2} nanoparticles with particle diameter size of 7–12 nm were obtained via 24 h aging time. The particle size was controlled by changing the aging time and molar ratio of water/surfactant. Doubling W{sub 0} increased the amount and particle size of WS{sub 2} by 22 and 26%, respectively. The effect of aging time in the range of 6–24 h was investigated and the complete disappearance of yellowish color at 24 h resulted in an optically clear solution, which was the indication of WS{sub 2} formation with 100% conversion of reactant ((NH{sub 4}){sub 2}WS{sub 4}) in the batch reactor.

  6. Synthesis and characterization of NiFe{sub 2}O{sub 4}–Pd magnetically recyclable catalyst for hydrogenation reaction

    SciTech Connect (OSTI)

    Karao?lu, E.; Özel, U.; Caner, C.; Baykal, A.; Summak, M.M.; Sözeri, H.

    2012-12-15

    Graphical abstract: Display Omitted Highlights: ? Novel superparamagnetic NiFe{sub 2}O{sub 4}–Pd magnetically recyclable catalyst was fabricated through co-precipitation. ? It could be reused several times without significant loss in catalytic activity for hydrogenation reaction. ? No further modification of the NiFe{sub 2}O{sub 4}–Pd magnetically recyclable catalyst is necessary for utilization as catalyst. -- Abstract: Herein we report the fabrication and characterization magnetically recyclable catalysts of NiFe{sub 2}O{sub 4}–Pd nanocomposite as highly effective catalysts for reduction reactions in liquid phase. The reduction Pd{sup 2+} was accomplished with polyethylene glycol 400 (PEG-400) instead of sodium borohydride (NaBH{sub 4}) and NiFe{sub 2}O{sub 4} nanoparticles was prepared by sonochemically using FeCI{sub 3}·6H{sub 2}O and NiCl{sub 2}. The chemical characterization of the product was done with X-ray diffractometry, Infrared spectroscopy, transmission electron microscopy, UV–Vis spectroscopy, thermal gravimetry and inductively coupled plasma. Thus formed NiFe{sub 2}O{sub 4}–Pd MRCs showed a very high activity in reduction reactions of 4-nitro aniline and 1,3-dinitrobenzene in liquid phase. It was found out that the catalytic activity of NiFe{sub 2}O{sub 4}–Pd MRCs on the reduction of 4-nitro aniline and 1,3-dinitrobenzene in liquid phase are between 99–93% and 98–93%, respectively. Magnetic character of this system allowed recovery and multiple use without significant loss of its catalytic activity. It is found that NiFe{sub 2}O{sub 4}–Pd MRCs showed very efficient catalytic activity and multiple usability.

  7. Direct hierarchical assembly of nanoparticles

    SciTech Connect (OSTI)

    Xu, Ting; Zhao, Yue; Thorkelsson, Kari

    2014-07-22

    The present invention provides hierarchical assemblies of a block copolymer, a bifunctional linking compound and a nanoparticle. The block copolymers form one micro-domain and the nanoparticles another micro-domain.

  8. Catalysts compositions for use in fuel cells

    DOE Patents [OSTI]

    Chuang, Steven S.C.

    2015-12-01

    The present invention generally relates to the generation of electrical energy from a solid-state fuel. In one embodiment, the present invention relates to a solid-oxide fuel cell for generating electrical energy from a carbon-based fuel, and to catalysts for use in a solid-oxide fuel cell.

  9. Catalysts compositions for use in fuel cells

    DOE Patents [OSTI]

    Chuang, Steven S.C.

    2015-12-02

    The present invention generally relates to the generation of electrical energy from a solid-state fuel. In one embodiment, the present invention relates to a solid-oxide fuel cell for generating electrical energy from a carbon-based fuel, and to catalysts for use in a solid-oxide fuel cell.

  10. Supported metal catalysts: Preparation, characterization, and function

    SciTech Connect (OSTI)

    Jackson, S.D.; Leeming, P. [ICI Katalco, Cleveland (United Kingdom)] [ICI Katalco, Cleveland (United Kingdom); Webb, G. [Univ. of Glasgow (United Kingdom)] [Univ. of Glasgow (United Kingdom)

    1996-05-01

    The sorptive properties of supported platinum catalysts has been studied for the adsorption of carbonyl sulfide and hydrogen sulfide. It was observed that hydrogen sulfide adsorption disallowed carbon monoxide adsorption. Dissociation chemistry was probed using labelled compounds. 32 refs., 8 tabs.

  11. Fuel cells and fuel cell catalysts

    DOE Patents [OSTI]

    Masel, Richard I.; Rice, Cynthia A.; Waszczuk, Piotr; Wieckowski, Andrzej

    2006-11-07

    A direct organic fuel cell includes a formic acid fuel solution having between about 10% and about 95% formic acid. The formic acid is oxidized at an anode. The anode may include a Pt/Pd catalyst that promotes the direct oxidation of the formic acid via a direct reaction path that does not include formation of a CO intermediate.

  12. the Catalyst Yellow is the New Green

    E-Print Network [OSTI]

    Ziurys, Lucy M.

    the Catalyst Yellow is the New Green: Dr. Jeff Pyun turns waste sulfur into plastics Chemistry? . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 Going Yellow! From Garbage to Plastics and Beyond . 8 Giving Back: New Tools Using the Graphical Madden BS Chemistry 1970 I am currently working with career and technology education (CTE) teachers

  13. Naphthene upgrading with pillared synthetic clay catalysts

    SciTech Connect (OSTI)

    Sharma, R.K.; Olson, E.S. [Univ. of North Dakota, Grand Forks, ND (United States)

    1995-12-31

    Catalytic hydrotreatment of methylcyclohexane was investigated to model upgrading of coal-derived naphthenes. Nickel-substituted synthetic mica montmorillonite (NiSMM), alumina-pillared NiSMM and Zirconia-pillared NiSMM were prepared and tested for hydrocracking and hydroisomerization of methylcyclohexane. Infrared and thermal desorption studies of the pyridine-adsorbed catalysts indicated the presence of Lewis and Bronsted acid sites. Total acidity and surface area increased with pillaring of NiSMM with polyoxy aluminum and polyoxy zirconium cations. Methylcyclohexane was reacted with these catalysts under a variety of conditions. Pillared clays gave higher gas yields and higher hydrocracking but lower hydroisomerization activity than nonpillared clay. The majority of the products were branched alkanes (isoparaffinic). These catalysts effectively use hydrogen as indicated by the minimal formation of aromatic hydrocarbons, coke, or other oligomeric materials. The effect of various operating conditions, i.e., reaction temperature, contact time, H{sub 2} pressure, and catalyst, on the product distribution will be described.

  14. Multifunctional Catalysts for Singlewall Carbon Nanotube

    E-Print Network [OSTI]

    Guo, Ting

    because the two metals in the bi- MNPs can enhance certain functions by playing complementary catalytic.1,2 For example, bi-MNPs are preferred heterogeneous catalysts in petroleum reforming processes.3 Bi, cleanness, and lengths. Previous studies on bi-MNPs have revealed that their superior catalytic abilities

  15. Catalyst Activity Comparison of Alcohols over Zeolites

    SciTech Connect (OSTI)

    Ramasamy, Karthikeyan K.; Wang, Yong

    2013-01-01

    Alcohol transformation to transportation fuel range hydrocarbon on HZSM-5 (SiO2 / Al2O3 = 30) catalyst was studied at 360oC and 300psig. Product distributions and catalyst life were compared using methanol, ethanol, 1-propanol or 1-butanol as a feed. The catalyst life for 1-propanol and 1-butanol was more than double compared to that for methanol and ethanol. For all the alcohols studied, the product distributions (classified to paraffin, olefin, napthene, aromatic and naphthalene compounds) varied with time on stream (TOS). At 24 hours TOS, liquid product from 1-propanol and 1-butanol transformation primarily contains higher olefin compounds. The alcohol transformation process to higher hydrocarbon involves a complex set of reaction pathways such as dehydration, oligomerization, dehydrocyclization, and hydrogenation. Compared to ethylene generated from methanol and ethanol, oligomerization of propylene and butylene has a lower activation energy and can readily take place on weaker acidic sites. On the other hand, dehydrocyclization of propylene and butylene to form the cyclic compounds requires the sits with stronger acid strength. Combination of the above mentioned reasons are the primary reasons for olefin rich product generated in the later stage of the time on stream and for the extended catalyst life time for 1 propanol and 1 butanol compared to methanol and ethanol conversion over HZSM-5.

  16. Nitrated metalloporphyrins as catalysts for alkane oxidation

    DOE Patents [OSTI]

    Ellis, P.E. Jr.; Lyons, J.E.

    1994-01-18

    Compositions of matter comprising nitro-substituted metal complexes of porphyrins are catalysts for the oxidation of alkanes. The metal is iron, chromium, manganese, ruthenium, copper or cobalt. The porphyrin ring has nitro groups attached thereto in meso and/or [beta]-pyrrolic positions.

  17. Nitrated metalloporphyrins as catalysts for alkane oxidation

    DOE Patents [OSTI]

    Ellis, Jr., Paul E. (Downingtown, PA); Lyons, James E. (Wallingford, PA)

    1992-01-01

    Alkanes are oxidized by contact with oxygen-containing gas in the presence as catalyst of a metalloporphyrin in which hydrogen atoms in the porphyrin ring have been replaced with one or more nitro groups. Hydrogen atoms in the porphyrin ring may also be substituted with halogen atoms.

  18. Nitrated metalloporphyrins as catalysts for alkane oxidation

    DOE Patents [OSTI]

    Ellis, Jr., Paul E. (Downingtown, PA); Lyons, James E. (Wallingford, PA)

    1994-01-01

    Compositions of matter comprising nitro-substituted metal complexes of porphyrins are catalysts for the oxidation of alkanes. The metal is iron, chromium, manganese, ruthenium, copper or cobalt. The porphyrin ring has nitro groups attached thereto in meso and/or .beta.-pyrrolic positions.

  19. Nanotube/Nanowire Based ORR Catalyst

    Broader source: Energy.gov [DOE]

    Presentation about nanotube or nanowire-based oxygen reduction reaction (ORR) catalysts, presented by Yushan Yan, University of Delaware, at 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.

  20. Catalysts for conversion of syngas to liquid motor fuels

    DOE Patents [OSTI]

    Rabo, Jule A. (Armonk, NY); Coughlin, Peter K. (Yorktown Heights, NY)

    1987-01-01

    Synthesis gas comprising carbon monoxide and hydrogen is converted to C.sub.5.sup.+ hydrocarbons suitable for use as liquid motor fuels by contact with a dual catalyst composition capable of ensuring the production of only relatively minor amounts of heavy products boiling beyond the diesel oil range. The catalyst composition, having desirable stability during continuous production operation, employs a Fischer-Tropsch catalyst, together with a co-catalyst/support component. The latter component is a steam-stabilized zeolite Y catalyst of hydrophobic character, desirably in acid-extracted form.

  1. Process of activation of a palladium catalyst system

    DOE Patents [OSTI]

    Sobolevskiy, Anatoly (Orlando, FL); Rossin, Joseph A. (Columbus, OH); Knapke, Michael J. (Columbus, OH)

    2011-08-02

    Improved processes for activating a catalyst system used for the reduction of nitrogen oxides are provided. In one embodiment, the catalyst system is activated by passing an activation gas stream having an amount of each of oxygen, water vapor, nitrogen oxides, and hydrogen over the catalyst system and increasing a temperature of the catalyst system to a temperature of at least 180.degree. C. at a heating rate of from 1-20.degree./min. Use of activation processes described herein leads to a catalyst system with superior NOx reduction capabilities.

  2. Mercury Detection with Gold Nanoparticles

    E-Print Network [OSTI]

    Crosby, Jeffrey

    2013-01-01

    also examined similar palladium-hydrogen catalytic surfacedtransistors. The palladium, a hydrogen catalyst, converts Hof the palladium device acted as a sink for hydrogen. There

  3. Hydrocarbon reforming catalyst material and configuration of the same

    DOE Patents [OSTI]

    Singh, Prabhakar (Export, PA); Shockling, Larry A. (Plum Borough, PA); George, Raymond A. (Pittsburgh, PA); Basel, Richard A. (Plub Borough, PA)

    1996-01-01

    A hydrocarbon reforming catalyst material comprising a catalyst support impregnated with catalyst is provided for reforming hydrocarbon fuel gases in an electrochemical generator. Elongated electrochemical cells convert the fuel to electrical power in the presence of an oxidant, after which the spent fuel is recirculated and combined with a fresh hydrocarbon feed fuel forming the reformable gas mixture which is fed to a reforming chamber containing a reforming catalyst material, where the reforming catalyst material includes discrete passageways integrally formed along the length of the catalyst support in the direction of reformable gas flow. The spent fuel and/or combusted exhaust gases discharged from the generator chamber transfer heat to the catalyst support, which in turn transfers heat to the reformable gas and to the catalyst, preferably via a number of discrete passageways disposed adjacent one another in the reforming catalyst support. The passageways can be slots extending inwardly from an outer surface of the support body, which slots are partly defined by an exterior confining wall. According to a preferred embodiment, the catalyst support is non-rigid, porous, fibrous alumina, wherein the fibers are substantially unsintered and compressible, and the reforming catalyst support is impregnated, at least in the discrete passageways with Ni and MgO, and has a number of internal slot passageways for reformable gas, the slot passageways being partly closed by a containing outer wall.

  4. Hydrocarbon reforming catalyst material and configuration of the same

    DOE Patents [OSTI]

    Singh, P.; Shockling, L.A.; George, R.A.; Basel, R.A.

    1996-06-18

    A hydrocarbon reforming catalyst material comprising a catalyst support impregnated with catalyst is provided for reforming hydrocarbon fuel gases in an electrochemical generator. Elongated electrochemical cells convert the fuel to electrical power in the presence of an oxidant, after which the spent fuel is recirculated and combined with a fresh hydrocarbon feed fuel forming the reformable gas mixture which is fed to a reforming chamber containing a reforming catalyst material, where the reforming catalyst material includes discrete passageways integrally formed along the length of the catalyst support in the direction of reformable gas flow. The spent fuel and/or combusted exhaust gases discharged from the generator chamber transfer heat to the catalyst support, which in turn transfers heat to the reformable gas and to the catalyst, preferably via a number of discrete passageways disposed adjacent one another in the reforming catalyst support. The passageways can be slots extending inwardly from an outer surface of the support body, which slots are partly defined by an exterior confining wall. According to a preferred embodiment, the catalyst support is non-rigid, porous, fibrous alumina, wherein the fibers are substantially unsintered and compressible, and the reforming catalyst support is impregnated, at least in the discrete passageways with Ni and MgO, and has a number of internal slot passageways for reformable gas, the slot passageways being partly closed by a containing outer wall. 5 figs.

  5. Catalyst Additives to Enhance Mercury Oxidation and Capture

    SciTech Connect (OSTI)

    Jared W. Cannon; Thomas K. Gale

    2004-12-31

    Preliminary research has shown that SCR catalysts employed for nitrogen-oxide reduction can effectively oxidize mercury. This report discusses initial results from fundamental investigations into the behavior of mercury species in the presence of SCR catalysts at Southern Research Institute. Three different SCR catalysts are being studied. These are honeycomb-type, plate-type, and a hybrid-type catalyst. The catalysts are manufactured and supplied by Cormetech Inc., Hitachi America Ltd., and Haldor-Topsoe Inc., respectively. Test methods and experimental procedures were developed for current and future testing. The methods and procedures equalize factors influencing mercury adsorption and oxidation (surface area, catalyst activity, and pore structure) that normally differ for each catalyst type. Initial testing was performed to determine the time necessary for each catalyst to reach surface-adsorption equilibrium. In addition, the fraction of Hg oxidized by each of the SCR catalyst types is being investigated, for a given amount of catalyst and flow rate of mercury and flue gas. The next major effort will be to examine the kinetics of mercury oxidation across the SCR catalysts with respect to changes in mercury concentration and with respect to HCl concentration. Hg-sorption equilibrium times will also be investigated with respect to ammonia concentration in the simulated flue gas.

  6. Novel Attrition-Resistant Fischer Tropsch Catalyst

    SciTech Connect (OSTI)

    Weast, Logan, E.; Staats, William, R.

    2009-05-01

    There is a strong national interest in the Fischer-Tropsch synthesis process because it offers the possibility of making liquid hydrocarbon fuels from reformed natural gas or coal and biomass gasification products. This project explored a new approach that had been developed to produce active, attrition-resistant Fischer-Tropsch catalysts that are based on glass-ceramic materials and technology. This novel approach represented a promising solution to the problem of reducing or eliminating catalyst attrition and maximizing catalytic activity, thus reducing costs. The technical objective of the Phase I work was to demonstrate that glass-ceramic based catalytic materials for Fischer-Tropsch synthesis have resistance to catalytic deactivation and reduction of particle size superior to traditional supported Fischer-Tropsch catalyst materials. Additionally, these novel glass-ceramic-based materials were expected to exhibit catalytic activity similar to the traditional materials. If successfully developed, the attrition-resistant Fischer-Tropsch catalyst materials would be expected to result in significant technical, economic, and social benefits for both producers and public consumers of Fischer-Tropsch products such as liquid fuels from coal or biomass gasification. This program demonstrated the anticipated high attrition resistance of the glass-ceramic materials. However, the observed catalytic activity of the materials was not sufficient to justify further development at this time. Additional testing documented that a lack of pore volume in the glass-ceramic materials limited the amount of surface area available for catalysis and consequently limited catalytic activity. However, previous work on glass-ceramic catalysts to promote other reactions demonstrated that commercial levels of activity can be achieved, at least for those reactions. Therefore, we recommend that glass-ceramic materials be considered again as potential Fischer-Tropsch catalysts if it can be demonstrated that materials with adequate pore volume can be produced. During the attrition resistance tests, it was learned that the glass-ceramic materials are very abrasive. Attention should be paid in any further developmental efforts to the potential for these hard, abrasive materials to damage reactors.

  7. One-Dimensional Ceria as Catalyst for the Low-Temperature Water-Gas Shift Reaction

    SciTech Connect (OSTI)

    Han, W.; Wen, W; Hanson, J; Teng, X; Marinkovic, N; Rodriguez, J

    2009-01-01

    Synchrotron-based in situ time-resolved X-ray diffraction and X-ray absorption spectroscopy were used to study pure ceria and Pd-loaded ceria nanotubes and nanorods (1D-ceria) as catalysts for the water-gas shift (WGS) reaction. While bulk ceria is very poor as WGS catalysts, pure 1D-ceria displayed catalytic activity at a temperature as low as 300 C. The reduction of the pure 1D-ceria in pure hydrogen started at 150 C, which is a much lower temperature than those previously reported for the reduction of 3D ceria nanoparticles. This low reduction temperature reflects the novel morphology of the oxide systems and may be responsible for the low-temperature WGS catalytic activity seen for the 1D-ceria. Pd-loaded 1D ceria displayed significant WGS activity starting at 200 C. During pretreatment in H{sub 2}, the ceria lattice parameter increased significantly around 60 C, which indicates that Pd-oxygen interactions may facilitate the reduction of Pd-loaded 1D-ceria. Pd and ceria both participate in the formation of the active sites for the catalytic reactions. The low-temperature hydrogen pretreatment results in higher WGS activity for Pd-loaded 1D-ceria.

  8. Simultaneous catalyst deposition and growth of aligned carbon nanotubes on SiO{sub 2}/Si substrates by radio frequency magnetron sputtering

    SciTech Connect (OSTI)

    Scalese, S.; Scuderi, V.; Privitera, V.; Pennisi, A.; Simone, F.

    2007-12-01

    Radio frequency magnetron sputtering has been used for the synthesis of aligned carbon nanotubes (CNTs) on a SiO{sub 2}/Si substrate, with simultaneous in situ catalyst deposition. This method allows the use of substrates without the need of a surface predeposition of catalytic particles. In particular, among the metals considered, we observed the formation of CNTs using W or Ni as catalysts. Only in the case of Ni did we find that the CNTs are aligned along the target-substrate direction, unlike the randomly oriented CNTs observed when W was used as catalyst. Scanning and transmission electron microscopies show that the catalytic Ni nanoparticle is found mostly on the tip of the obtained bamboolike CNTs, while W nanoparticles are encapsulated inside hollow nanotubes, at different points along their length. We ascribe not only the observed structural differences to the size of the W and Ni particles but also to a different diffusion behavior of C in the two kinds of metallic clusters.

  9. Hydroprocessing of solvent-refined coal: catalyst-screening results

    SciTech Connect (OSTI)

    Stiegel, G.J.; Tischer, R.E.; Polinski, L.M.

    1982-03-01

    This report presents the results of screening four catalysts for hydroprocessing a 50 wt% mixture of SRC-I in a prehydrogenated creosote oil using a continuous flow unit. All catalysts employed were nickel-molybdates with varying properties. Reaction conditions were 2000 psi, 8 SCFH of hydrogen, volume hourly space velocity of 0.6 to 1.0 cc of SRC-I/hr/cc of catalyst, and 48 hours at 750/sup 0/F followed by 72 hours at 780/sup 0/F. The results indicate that the Shell 324 catalyst is best for hydrogenation of the feedstock but only marginally better than CB 81-44 for denitrogenation. The CB 81-44 catalyst may be slightly better than Shell 324 for the conversion of the +850/sup 0/F fraction of the feedstock. Desulfurization was uniformly high for all catalysts. Catalysts with a bimodal pore size distribution (i.e., SMR7-6137(1)) appear to be better for denitrogenation than unimodal catalysts (i.e., SMR7-6137(4)) containing the same metals loading. Unimodal catalysts (i.e., Shell 324) with higher metals loadings are comparable to bimodal catalysts (i.e., CB 81-44) containing less metals. The results indicate that pore size distribution and metals loading are important parameters for high activity. Catalysts with a unimodal pore volume distribution are capable of being restored to their original state, while bimodal ones experience a loss in surface area and pore volume and an increase in pellet density. This is attributed to the more efficient use of the interior surface area of the catalyst, which results in higher accumulation of coke and metals. Since coke can be removed via controlled oxidation, the irreversible loss is due to the higher concentrations of metals in the catalyst.

  10. Nanoparticle-Based Biosensors and Bioassays

    SciTech Connect (OSTI)

    Liu, Guodong; Wang, Jun; Lin, Yuehe; Wang, Joseph

    2007-10-11

    In this book chapter, we review the recent advances in nanoparticles based bioassay. The nanoparticles include quantum dots, silica nanoparticles and apoferritin nanoparticles. The new nanoparticles-based labels hold great promise for multiplex protein and DNA detection and for enhancing the sensitivity of other bioassays.

  11. Interactions of Copper Nanoparticles with the Microalgae, Chlamydomonas reinhardtii

    E-Print Network [OSTI]

    Spitzmiller, Melissa Rae

    2012-01-01

    Nanoparticles with the Microalgae, Chlamydomonas reinhardtiiNanoparticles with the Microalgae, Chlamydomonas reinhardtiifor Microalgae . 4 2.

  12. Exploring the activity of a novel Au/TiC(001) model catalyst towards CO and CO2 hydrogenation

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

    Asara, Gian Giacomo; Ricart, Josep M.; Rodriguez, Jose A.; Illas, Francesc

    2015-02-02

    Small metallic nanoparticles supported on transition metal carbides exhibit an unexpected high activity towards a series of chemical reactions. In particular, the Au/TiC system has proven to be an excellent catalyst for SO2 decomposition, thiophene hydrodesulfurization, O2 and H2 dissociation and the water gas shift reaction. Recent studies have shown that Au/TiC is a very good catalyst for the reverse water–gas shift (CO2 + H2 ? CO + H2O) and CO2 hydrogenation to methanol. The present work further expands the range of applicability of this novel type of systems by exploring the catalytic activity of Au/TiC towards the hydrogenation ofmore »CO or CO2 with periodic density functional theory (DFT) calculations on model systems. Hydrogen dissociates easily on Au/TiC but direct hydrogenation of CO to methanol is hindered by very high activation barriers implying that, on this model catalyst, methanol production from CO2 involves the hydrogenation of a HOCO-like intermediate. Thus, when dealing with mixtures of syngas (CO/CO2/H2/H2O), CO could be transformed into CO2 through the water gas shift reaction with subsequent hydrogenation of CO2 to methanol.« less

  13. Predict carbonation rate on iron catalyst

    SciTech Connect (OSTI)

    Dry, M.E.

    1980-02-01

    On solely thermodynamic grounds, the main hydrocarbon product of the Fischer-Tropsch reaction should be methane; in practice, however, carbon is frequently produced as well and deposited on the iron catalyst, fouling the active surface sites. South African Coal, Oil and Gas Corp., Ltd.'s experiments with a fluidized Fischer-Tropsch catalyst bed demonstrate that the rate of carbon deposition is strongly dependent on the hydrogen partial pressure in the reactor, much less dependent on the CO pressure, and not affected at all by the pressure of CO/sub 2/. A suggested reaction scheme for the Fischer-Tropsch synthesis explains these observations and provides a basis for a correlation useful in predicting carbon-deposition rates.

  14. Oxidation of propylene over copper oxide catalysts 

    E-Print Network [OSTI]

    Billingsley, David Stuart

    1958-01-01

    are to be found in the patent literature which is often not particularly informative. Discussion of this material has, therefore been reserved for a subsequent section of this survey. If view of the considerable activity in most phases of the petro- chemicals... to have a bearing on this work and which provided sufficient information to be helpful in determining roughly what could be expected of different catalysts. In many of the patents surveyed, observed conversions of olefins to various products were...

  15. Synthesis of iron based hydrocracking catalysts

    SciTech Connect (OSTI)

    Farcasiu, M.; Eldredge, P.A.; Ladner, E.P.

    1993-05-25

    A method of preparing an iron based hydrocracking catalyst is described, comprising reacting iron (111) oxide powders and elemental sulfur with a liquid hydrogen donor having a hydroaromatic structure present in the range of from about 5 to about 50 times the weight of iron (111) oxide at a temperature in the range of from about 180 C to about 240 C for a time in the range of from about 0 to about 8 hours.

  16. Autothermal hydrodesulfurizing reforming method and catalyst

    DOE Patents [OSTI]

    Krumpelt, Michael; Kopasz, John P.; Ahmed, Shabbir; Kao, Richard Li-chih; Randhava, Sarabjit Singh

    2005-11-22

    A method for reforming a sulfur-containing carbonaceous fuel in which the sulfur-containing carbonaceous fuel is mixed with H.sub.2 O and an oxidant, forming a fuel/H.sub.2 O/oxidant mixture. The fuel H.sub.2 O/oxidant mixture is brought into contact with a catalyst composition comprising a dehydrogenation portion, an oxidation portion and a hydrodesulfurization portion, resulting in formation of a hydrogen-containing gas stream.

  17. Intermediate Ethanol Blends Catalyst Durability Program

    SciTech Connect (OSTI)

    West, Brian H; Sluder, Scott; Knoll, Keith; Orban, John; Feng, Jingyu

    2012-02-01

    In the summer of 2007, the U.S. Department of Energy (DOE) initiated a test program to evaluate the potential impacts of intermediate ethanol blends (also known as mid-level blends) on legacy vehicles and other engines. The purpose of the test program was to develop information important to assessing the viability of using intermediate blends as a contributor to meeting national goals for the use of renewable fuels. Through a wide range of experimental activities, DOE is evaluating the effects of E15 and E20 - gasoline blended with 15% and 20% ethanol - on tailpipe and evaporative emissions, catalyst and engine durability, vehicle driveability, engine operability, and vehicle and engine materials. This report provides the results of the catalyst durability study, a substantial part of the overall test program. Results from additional projects will be reported separately. The principal purpose of the catalyst durability study was to investigate the effects of adding up to 20% ethanol to gasoline on the durability of catalysts and other aspects of the emissions control systems of vehicles. Section 1 provides further information about the purpose and context of the study. Section 2 describes the experimental approach for the test program, including vehicle selection, aging and emissions test cycle, fuel selection, and data handling and analysis. Section 3 summarizes the effects of the ethanol blends on emissions and fuel economy of the test vehicles. Section 4 summarizes notable unscheduled maintenance and testing issues experienced during the program. The appendixes provide additional detail about the statistical models used in the analysis, detailed statistical analyses, and detailed vehicle specifications.

  18. Highly Dispersed Alloy Catalyst for Durability

    SciTech Connect (OSTI)

    Vivek S. Murthi , Elise Izzo, Wu Bi, Sandra Guerrero and Lesia Protsailo

    2013-01-08

    Achieving DOE�¢����s stated 5000-hr durability goal for light-duty vehicles by 2015 will require MEAs with characteristics that are beyond the current state of the art. Significant effort was placed on developing advanced durable cathode catalysts to arrive at the best possible electrode for high performance and durability, as well as developing manufacturing processes that yield significant cost benefit. Accordingly, the overall goal of this project was to develop and construct advanced MEAs that will improve performance and durability while reducing the cost of PEMFC stacks. The project, led by UTC Power, focused on developing new catalysts/supports and integrating them with existing materials (membranes and gas diffusion layers (GDLs)) using state-of-the-art fabrication methods capable of meeting the durability requirements essential for automotive applications. Specifically, the project work aimed to lower platinum group metals (PGM) loading while increasing performance and durability. Appropriate catalysts and MEA configuration were down-selected that protects the membrane, and the layers were tailored to optimize the movements of reactants and product water through the cell to maximize performance while maintaining durability.

  19. Method for regeneration and activity improvement of syngas conversion catalyst

    DOE Patents [OSTI]

    Lucki, Stanley J. (Runnemede, NJ); Brennan, James A. (Cherry Hill, NJ)

    1980-01-01

    A method is disclosed for the treatment of single particle iron-containing syngas (synthes.s gas) conversion catalysts comprising iron, a crystalline acidic aluminosilicate zeolite having a silica to alumina ratio of at least 12, a pore size greater than about 5 Angstrom units and a constraint index of about 1-12 and a matrix. The catalyst does not contain promoters and the treatment is applicable to either the regeneration of said spent single particle iron-containing catalyst or for the initial activation of fresh catalyst. The treatment involves air oxidation, hydrogen reduction, followed by a second air oxidation and contact of the iron-containing single particle catalyst with syngas prior to its use for the catalytic conversion of said syngas. The single particle iron-containing catalysts are prepared from a water insoluble organic iron compound.

  20. Increasing the hydrogenation activity of commercial catalysts for selective hydrocracking

    SciTech Connect (OSTI)

    Khashagul`gova, N.S.; Freiman, L.L.; Zelentsov, Yu.N. [and others

    1994-07-01

    The catalysts generally used in hydrodewaxing or selective hydrocracking of n-paraffins are zeolites with the pentasil structure: TsVK, TsVM, TsVN, and Ultrasil. For use in the production of high-quality transformer oils from paraffinic feedstocks, these catalysts have not only a high cracking activity but also an adequate hydrogenating activity. Catalysts containing a nickel-molybdenum complex (or nickel molybdate synthesized by a specific method) are higher in hydrogenating activity in comparison with catalysts in which the metals are introduced by coextrusion or impregnation. Precipitation of a nickel-molybdenum complex on a solid support (aluminosilicate or zeolite) tends to increase its hydrogenating activity, so that the content of the hydrogenating metals in the catalyst can be reduced. This report describes studies on catalysts based on TsVM and TsVN high-silica zeolites.

  1. TECHNOLOGY DEVELOPMENT FOR IRON FISCHER-TROPSCH CATALYSTS

    SciTech Connect (OSTI)

    Davis, B.H.

    1998-07-22

    The goal of the proposed work described in this Final Report was the development of iron-based Fischer-Tropsch catalysts that combined high activity, selectivity and life with physical robustness for slurry phase reactors that will produce either low-alpha or high-alpha products. The work described here has optimized the catalyst composition and pretreatment operation for a low-alpha catalyst. In parallel, work has been conducted to design a high-alpha iron catalyst that is suitable for slurry phase synthesis. Studies have been conducted to define the chemical phases present at various stages of the pretreatment and synthesis stages and to define the course of these changes. The oxidation/reduction cycles that are anticipated to occur in large, commercial reactors have been studied at the laboratory scale. Catalyst performance has been determined for catalysts synthesized in this program for activity, selectivity and aging characteristics.

  2. Catalyst Additives to Enhance Mercury Oxidation and Capture

    SciTech Connect (OSTI)

    Thomas K. Gale

    2005-12-31

    Preliminary research has shown that SCR catalysts employed for nitrogen-oxide reduction can effectively oxidize mercury. Three different SCR catalysts are currently being studied in this project--honeycomb-type, plate-type, and a hybrid-type catalyst. The catalysts were manufactured and supplied by Cormetech Inc., Hitachi America Ltd., and Haldor-Topsoe Inc., respectively. Parametric testing was performed to investigate the contribution of flue-gas chemistry on mercury oxidation via SCR catalysts. Future work to characterize flue gas simulations typically derived from low and high sulfur bituminous coal are being performed in a stepwise manner, to avoid the constant interruptions in testing that occur when leaks in the system are generated during temperature transitions. Specifically, chlorine concentration vs. mercury oxidation correlations will be developed for each catalyst. The contributions of temperature are also being investigated. SO2 oxidation is also being investigated for each test condition.

  3. Activation of catalysts for synthesizing methanol from synthesis gas

    DOE Patents [OSTI]

    Blum, David B. (108 Tall Oaks Dr., Wayne, NJ 07470); Gelbein, Abraham P. (45 Headley Rd., Morristown, NJ 07960)

    1985-01-01

    A method for activating a methanol synthesis catalyst is disclosed. In this method, the catalyst is slurried in an inert liquid and is activated by a reducing gas stream. The activation step occurs in-situ. That is, it is conducted in the same reactor as is the subsequent step of synthesizing methanol from a methanol gas stream catalyzed by the activated catalyst still dispersed in a slurry.

  4. Enhanced catalyst for converting synthesis gas to liquid motor fuels

    DOE Patents [OSTI]

    Coughlin, Peter K. (Yorktown Heights, NY)

    1986-01-01

    The conversion of synthesis gas to liquid molar fuels by means of a cobalt Fischer-Tropsch catalyst composition is enhanced by the addition of molybdenum, tungsten or a combination thereof as an additional component of said composition. The presence of the additive component increases the olefinic content of the hydrocarbon products produced. The catalyst composition can advantageously include a support component, such as a molecular sieve, co-catalyst/support component or a combination of such support components.

  5. Mapping Metals Incorporation of a Single Catalyst Particle Using...

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

    Mapping Metals Incorporation of a Single Catalyst Particle Using Element Specific X-ray Nanotomography Tuesday, March 31, 2015 Fluid catalytic cracking (FCC) is the refining...

  6. Activation of molecular catalysts using semiconductor quantum dots

    DOE Patents [OSTI]

    Meyer, Thomas J. (Chapel Hill, NC); Sykora, Milan (Los Alamos, NM); Klimov, Victor I. (Los Alamos, NM)

    2011-10-04

    Photocatalytic materials based on coupling of semiconductor nanocrystalline quantum dots (NQD) and molecular catalysts. These materials have capability to drive or catalyze non-spontaneous chemical reactions in the presence of visible radiation, ultraviolet radiation, or both. The NQD functions in these materials as a light absorber and charge generator. Following light absorption, the NQD activates a molecular catalyst adsorbed on the surface of the NQD via transfer of one or more charges (either electrons or electron-holes) from the NQD to the molecular catalyst. The activated molecular catalyst can then drive a chemical reaction. A photoelectrolytic device that includes such photocatalytic materials is also described.

  7. In situ structural characterization of metal catalysts and materials...

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

    In situ structural characterization of metal catalysts and materials using XAFS spectroscopy in combination with complementary techniques. Wednesday, October 17, 2012 - 1:00pm SSRL...

  8. Catalyst for Improving the Combustion Efficiency of Petroleum...

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

    for Improving the Combustion Efficiency of Petroleum Fuels in Diesel Engines Catalyst for Improving the Combustion Efficiency of Petroleum Fuels in Diesel Engines 2005 Diesel...

  9. Toward Catalyst Design from Theoretical Calculations (464th Brookhaven Lecture)

    SciTech Connect (OSTI)

    Liu, Ping

    2010-12-15

    Catalysts have been used to speed up chemical reactions as long as yeast has been used to make bread rise. Today, catalysts are used everywhere from home kitchens to industrial chemical factories. In the near future, new catalysts being developed at Brookhaven Lab may be used to speed us along our roads and highways as they play a major role in solving the world’s energy challenges. During the lecture, Liu will discuss how theorists and experimentalists at BNL are working together to formulate and test new catalysts that could be used in real-life applications, such as hydrogen-fuel cells that may one day power our cars and trucks.

  10. Multimetal Nanoframes Improve Catalyst Performance | U.S. DOE...

    Office of Science (SC) Website

    of Science, Basic Energy Sciences and Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Program (catalyst mass activity and durability). King Abdulaziz...

  11. Lean-NOx Catalyst Development for Diesel Engine Applications...

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

    More Documents & Publications Lean NOx Catalysis Research and Development Selective reduction of NOx in oxygen rich environments with plasma-assisted catalysis: Catalyst...

  12. Pyrochem Catalysts for Diesel Fuel Reforming - Energy Innovation...

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

    Vehicles and Fuels Vehicles and Fuels Hydrogen and Fuel Cell Hydrogen and Fuel Cell Return to Search Pyrochem Catalysts for Diesel Fuel Reforming National Energy Technology...

  13. Combined catalysts for the combustion of fuel in gas turbines

    DOE Patents [OSTI]

    Anoshkina, Elvira V.; Laster, Walter R.

    2012-11-13

    A catalytic oxidation module for a catalytic combustor of a gas turbine engine is provided. The catalytic oxidation module comprises a plurality of spaced apart catalytic elements for receiving a fuel-air mixture over a surface of the catalytic elements. The plurality of catalytic elements includes at least one primary catalytic element comprising a monometallic catalyst and secondary catalytic elements adjacent the primary catalytic element comprising a multi-component catalyst. Ignition of the monometallic catalyst of the primary catalytic element is effective to rapidly increase a temperature within the catalytic oxidation module to a degree sufficient to ignite the multi-component catalyst.

  14. Small Catalyst Finding Could Lead to Big Breakthrough for Fuel...

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

    Labs -- could make fuel cells cost-competitive with other power generators. Using nanotechnology (science at very small scales), researchers have created a nanoframe catalyst that...

  15. Selective zeolite catalyst for preparing ethylbenzene from toluene and methanol

    SciTech Connect (OSTI)

    Vasil`ev, A.N.; Galinskii, A.A.

    1995-10-10

    A selective catalyst for methylation of toluene in the side chain has been prepared by modification of Cs{sub 0.85}NaX zeolite. Highly active catalysts for alkylation of toluene with methanol in the side chain are prepared by hydrothermal modification of zeolites. Previously it was found that with a high cesium content in catalysts, which was reached by ion exchange, their selectivity with respect to styrene considerably increases. In this paper the authors proposed a procedure for preparing a highly selective catalyst for synthesis of ethylbenzene.

  16. Catalysts and process for liquid hydrocarbon fuel production

    DOE Patents [OSTI]

    White, Mark G; Liu, Shetian

    2014-12-09

    The present invention provides a novel process and system in which a mixture of carbon monoxide and hydrogen synthesis gas, or syngas, is converted into hydrocarbon mixtures composed of high quality gasoline components, aromatic compounds, and lower molecular weight gaseous olefins in one reactor or step. The invention utilizes a novel molybdenum-zeolite catalyst in high pressure hydrogen for conversion, as well as a novel rhenium-zeolite catalyst in place of the molybdenum-zeolite catalyst, and provides for use of the novel catalysts in the process and system of the invention.

  17. Los Alamos catalyst could jumpstart e-cars, green energy

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

    materials and alkaline fuel cells, metal-air batteries and certain electrolyzers. Economical non-precious-metal catalyst capitalizes on carbon nanotubes LOS...

  18. Ceramatec NOx Sensor and NOx Catalyst Technologies | Department...

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

    & Publications Enhanced High Temperature Performance of NOx StorageReduction (NSR) Materials Pt-free, Perovskite-based Lean NOx Trap Catalysts Active Soot Filter Regeneration...

  19. Attrition Resistant Fischer-Tropsch Catalysts Based on FCC Supports

    SciTech Connect (OSTI)

    Adeyinka Adeyiga

    2010-02-05

    Commercial spent fluid catalytic cracking (FCC) catalysts provided by Engelhard and Albemarle were used as supports for Fe-based catalysts with the goal of improving the attrition resistance of typical F-T catalysts. Catalysts with the Ruhrchemie composition (100 Fe/5 Cu/4.2 K/25 spent FCC on mass basis) were prepared by wet impregnation. XRD and XANES analysis showed the presence of Fe{sub 2}O{sub 3} in calcined catalysts. FeC{sub x} and Fe{sub 3}O{sub 4} were present in the activated catalysts. The metal composition of the catalysts was analyzed by ICP-MS. F-T activity of the catalysts activated in situ in CO at the same conditions as used prior to the attrition tests was measured using a fixed bed reactor at T = 573 K, P = 1.38 MPa and H{sub 2}:CO ratio of 0.67. Cu and K promoted Fe supported over Engelhard provided spent FCC catalyst shows relatively good attrition resistance (8.2 wt% fines lost), high CO conversion (81%) and C{sub 5}+ hydrocarbons selectivity (18.3%).

  20. Selective ammonia slip catalyst enabling highly efficient NOx...

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

    enabling highly efficient NOx removal requirements of the future A low precious metal loading ammonia-slip catalyst was developed that is able to oxidize the ammonia that...

  1. Low temperature catalysts and process for methanol production

    DOE Patents [OSTI]

    Sapienza, R.S.

    1984-02-21

    This patent discloses a catalyst and process useful in low temperatures (=1500/sup 0/C) and preferably in the range 80 to 120/sup 0/C us

  2. New Developments in Titania-Based Catalysts for Selective Catalytic...

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

    SCR Application Volatility of Vanadia from Vanadia-Based SCR Catalysts under Accelerated Aging Conditions Progress on Acidic Zirconia Mixed Oxides for Efficient NH3-SCR Catalysis...

  3. Understanding the Distributed Intra-Catalyst Impact of Sulfation...

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

    Lean NOx Trap catalyst is an aftertreatment technology for abatement of nitrogen-oxide emissions from lean-burn vehicle engines. deer10partridge.pdf More Documents &...

  4. Multi-stage catalyst systems and uses thereof

    DOE Patents [OSTI]

    Ozkan, Umit S. (Worthington, OH); Holmgreen, Erik M. (Columbus, OH); Yung, Matthew M. (Columbus, OH)

    2009-02-10

    Catalyst systems and methods provide benefits in reducing the content of nitrogen oxides in a gaseous stream containing nitric oxide (NO), hydrocarbons, carbon monoxide (CO), and oxygen (O.sub.2). The catalyst system comprises an oxidation catalyst comprising a first metal supported on a first inorganic oxide for catalyzing the oxidation of NO to nitrogen dioxide (NO.sub.2), and a reduction catalyst comprising a second metal supported on a second inorganic oxide for catalyzing the reduction of NO.sub.2 to nitrogen (N.sub.2).

  5. VEHICLES - New catalyst looms big ... | ornl.gov

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

    overcomes the problem of inhibition, in which nitrogen oxides, copper oxide and hydrocarbons effectively clog the catalyst designed to cleanse a vehicle's exhaust stream. This...

  6. Stabilization of Pt monolayer catalysts under harsh conditions...

    Office of Scientific and Technical Information (OSTI)

    Stabilization of Pt monolayer catalysts under harsh conditions of fuel cells Citation Details In-Document Search This content will become publicly available on May 21, 2016 Title:...

  7. Electroless preparation and characterization of Ni-B nanoparticles supported on multi-walled carbon nanotubes and their catalytic activity towards hydrogenation of styrene

    SciTech Connect (OSTI)

    Liu, Zheng; Li, Zhilin; Institute of Carbon Fibers and Composites, Beijing University of Chemical Technology, Beijing 100029 ; Wang, Feng; Institute of Carbon Fibers and Composites, Beijing University of Chemical Technology, Beijing 100029 ; Liu, Jingjun; Ji, Jing; Institute of Carbon Fibers and Composites, Beijing University of Chemical Technology, Beijing 100029 ; Park, Ki Chul; Endo, Morinobu

    2012-02-15

    Graphical abstract: The MWCNT/Ni-B catalyst has been successfully prepared by an electroless deposition process. The Ni-B nanoparticles on the supporter are amorphous and are well-distributed. The catalytic conversion towards hydrogenation of styrene shows excellent catalytic activity of the obtained materials. Highlights: Black-Right-Pointing-Pointer A two-step treatment of MWCNTs enabled the homogeneous growth of Ni-B nanoparticles. Black-Right-Pointing-Pointer Ni-B nanoparticles were amorphous with an average size of 60 nm. Black-Right-Pointing-Pointer There were electron transfer between Ni and B. Black-Right-Pointing-Pointer The catalyst had excellent catalytic activity towards hydrogenation of styrene. -- Abstract: Nickel-boron (Ni-B) nanoparticles supported on multi-walled carbon nanotubes (MWCNTs) were successfully synthesized through an electroless deposition process using the plating bath with sodium borohydride as a reducing agent. The structural and morphological analyses using field-emission scanning electron microscopy, X-ray diffractometry and high-resolution transmission electron microscopy have shown that the Ni-B nanoparticles deposited on the sidewalls of MWCNTs are fine spheres comprised of amorphous structure with the morphologically unique fine-structure like flowers, and homogenously dispersed with a narrow particle size distribution centered at around 60 nm diameter. The catalytic activity of MWCNT/Ni-B nanoparticles was evaluated with respect to hydrogenation of styrene. The hydrogenation catalyzed by MWCNT-supported Ni-B nanoparticles has been found to make styrene selectively converted into ethylbenzene. The highest conversion reaches 99.8% under proper reaction conditions, which demonstrates the high catalytic activity of MWCNT/Ni-B nanoparticles.

  8. A Multi-Ligand Based Pd Catalyst for C–N Cross-Coupling Reactions

    E-Print Network [OSTI]

    Fors, Brett P.

    An alternative approach to catalyst development, which led to a Pd catalyst based on two biarylphosphine ligands for C?N cross-coupling reactions, is reported. By effectively being able to take the form of multiple catalysts ...

  9. Pt-free, Perovskite-based Lean NOx Trap Catalysts | Department...

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

    Pt-free, Perovskite-based Lean NOx Trap Catalysts Pt-free, Perovskite-based Lean NOx Trap Catalysts Perovskite-based lean NOx catalysts shown to achieve comparable NOx reduction...

  10. Estimation of the distributed temperature of a SI engine catalyst for light-off strategy

    E-Print Network [OSTI]

    at a virtual entry point inside the catalyst. This new input has a static gain depending on the state, speed-up of the catalyst warm-up is a point of critical importance. When the catalyst is cold, heat

  11. Evaluation of monolayer protected metal nanoparticle technology

    E-Print Network [OSTI]

    Wu, Diana J

    2005-01-01

    Self assembling nanostructured nanoparticles represent a new class of synthesized materials with unique functionality. Such monolayer protected metal nanoparticles are capable of resisting protein adsorption, and if utilized ...

  12. Understanding the Distributed Intra-Catalyst Impact of Sulfation on Water Gas Shift in a Lean NOx Trap Catalyst

    Broader source: Energy.gov [DOE]

    The Lean NOx Trap catalyst is an aftertreatment technology for abatement of nitrogen-oxide emissions from lean-burn vehicle engines.

  13. CATALYSTS NHI Thermochemical Systems FY 2009 Year-End Report

    SciTech Connect (OSTI)

    Daniel M. Ginosar

    2009-09-01

    Fiscal Year 2009 work in the Catalysts project focused on advanced catalysts for the decomposition of sulfuric acid, a reaction common to both the Sulfur-Iodine (S-I) cycle and the Hybrid Sulfur cycle. Prior years’ effort in this project has found that although platinum supported on titanium oxide will be an acceptable catalyst for sulfuric acid decomposition in the integrated laboratory scale (ILS) project, the material has short comings, including significant cost and high deactivation rates due to sintering and platinum evaporation. For pilot and larger scale systems, the catalyst stability needs to be improved significantly. In Fiscal Year 2008 it was found that at atmospheric pressure, deactivation rates of a 1 wt% platinum catalyst could be reduced by 300% by adding either 0.3 wt% iridium (Ir) or 0.3 wt% ruthenium (Ru) to the catalyst. In Fiscal Year 2009, work focused on examining the platinum group metal catalysts activity and stability at elevated pressures. In addition, simple and complex metal oxides are known to catalyze the sulfuric acid decomposition reaction. These metal oxides could offer activities comparable to platinum but at significantly reduced cost. Thus a second focus for Fiscal Year 2009 was to explore metal oxide catalysts for the sulfuric acid decomposition reaction. In Fiscal Year 2007 several commercial activated carbons had been identified for the HI decomposition reaction; a reaction specific to the S-I cycle. Those materials should be acceptable for the pilot scale project. The activated carbon catalysts have some disadvantages including low activity at the lower range of reactor operating temperature (350 to 400°C) and a propensity to generate carbon monoxide in the presence of water that could contaminate the hydrogen product, but due to limited funding, this area had low priority in Fiscal Year 2009. Fiscal Year 2009 catalyst work included five tasks: development, and testing of stabilized platinum based H2SO4 catalysts, development and testing of metal oxide based H2SO4 catalysts, support of the ILS for catalyst studies, conducting a long term catalyst stability test at anticipated operating temperatures and pressures, and developing capabilities for conducting pressurized catalyst tests.

  14. Attrition Resistant Iron-Based Fischer-Tropsch Catalysts.

    SciTech Connect (OSTI)

    Jothimurugesan, K.; Goodwin, J.S.; Spivey, J.J.; Gangwal, S.K.

    1997-09-22

    The Fischer-Tropsch (F-T) reaction provides a way of converting coal-derived synthesis gas (CO and H{sub 2}) to liquid fuels. Since the reaction is highly exothermic, one of the major problems in control of the reaction is heat removal. Recent work has shown that the use of slurry bubble column reactors (SBCRs) can largely solve this problem. Iron-based (Fe) catalysts are preferred catalysts for F-T when using low CO/H{sub 2} ratio synthesis gases derived from modern coal gasifiers. This is because in addition to reasonable F-T activity, the F-T catalysts also possess high water gas shift (WGS) activity. However, a serious problem with the use of Fe catalysts in a SBCR is their tendency to undergo attrition. This can cause fouling/plugging of downstream filters and equipment, making the separation of catalyst from the oil/wax product very difficult if not impossible, and results in a steady loss of catalyst from the reactor. The objectives of this research are to develop a better understanding of the parameters affecting attrition resistance of Fe F-T catalysts suitable for use in SBCRs and to incorporate this understanding into the design of novel Fe catalysts having superior attrition resistance. Catalyst preparations will be based on the use of spray drying and will be scalable using commercially available equipment. The research will employ among other measurements, attrition testing and F-T synthesis, including long duration slurry reactor runs in order to ascertain the degree of success of the various preparations. The goal is to develop an Fe catalyst which can be used in a SBCR having only an internal filter for separation of the catalyst from the liquid product, without sacrificing F-T activity and selectivity.

  15. Subnanometer and nanometer catalysts, method for preparing size-selected catalysts

    DOE Patents [OSTI]

    Vajda, Stefan (Lisle, IL); Pellin, Michael J. (Naperville, IL); Elam, Jeffrey W. (Elmhurst, IL); Marshall, Christopher L. (Naperville, IL); Winans, Randall A. (Downers Grove, IL); Meiwes-Broer, Karl-Heinz (Roggentin, GR)

    2012-03-27

    Highly uniform cluster based nanocatalysts supported on technologically relevant supports were synthesized for reactions of top industrial relevance. The Pt-cluster based catalysts outperformed the very best reported ODHP catalyst in both activity (by up to two orders of magnitude higher turn-over frequencies) and in selectivity. The results clearly demonstrate that highly dispersed ultra-small Pt clusters precisely localized on high-surface area supports can lead to affordable new catalysts for highly efficient and economic propene production, including considerably simplified separation of the final product. The combined GISAXS-mass spectrometry provides an excellent tool to monitor the evolution of size and shape of nanocatalyst at action under realistic conditions. Also provided are sub-nanometer gold and sub-nanometer to few nm size-selected silver catalysts which possess size dependent tunable catalytic properties in the epoxidation of alkenes. Invented size-selected cluster deposition provides a unique tool to tune material properties by atom-by-atom fashion, which can be stabilized by protective overcoats.

  16. Subnanometer and nanometer catalysts, method for preparing size-selected catalysts

    DOE Patents [OSTI]

    Vajda, Stefan (Lisle, IL), Pellin, Michael J. (Naperville, IL); Elam, Jeffrey W. (Elmhurst, IL); Marshall, Christopher L. (Naperville, IL); Winans, Randall A. (Downers Grove, IL); Meiwes-Broer, Karl-Heinz (Roggentin, GR)

    2012-04-03

    Highly uniform cluster based nanocatalysts supported on technologically relevant supports were synthesized for reactions of top industrial relevance. The Pt-cluster based catalysts outperformed the very best reported ODHP catalyst in both activity (by up to two orders of magnitude higher turn-over frequencies) and in selectivity. The results clearly demonstrate that highly dispersed ultra-small Pt clusters precisely localized on high-surface area supports can lead to affordable new catalysts for highly efficient and economic propene production, including considerably simplified separation of the final product. The combined GISAXS-mass spectrometry provides an excellent tool to monitor the evolution of size and shape of nanocatalyst at action under realistic conditions. Also provided are sub-nanometer gold and sub-nanometer to few nm size-selected silver catalysts which possess size dependent tunable catalytic properties in the epoxidation of alkenes. Invented size-selected cluster deposition provides a unique tool to tune material properties by atom-by-atom fashion, which can be stabilized by protective overcoats.

  17. High-Throughput Program for the Discovery of NOx Reduction Catalysts...

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

    High-Throughput Program for the Discovery of NOx Reduction Catalysts High-Throughput Program for the Discovery of NOx Reduction Catalysts 2004 Diesel Engine Emissions Reduction...

  18. Selective ammonia slip catalyst enabling highly efficient NOx removal requirements of the future

    Broader source: Energy.gov [DOE]

    A low precious metal loading ammonia-slip catalyst was developed that is able to oxidize the ammonia that slips past the SCR catalyst to nitrogen.

  19. Deactivation Mechanism of Cu/Zeolite SCR Catalyst Due to Reductive...

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

    Mechanism of CuZeolite SCR Catalyst Due to Reductive Hydrothermal Aging Deactivation Mechanism of CuZeolite SCR Catalyst Due to Reductive Hydrothermal Aging Better control for...

  20. Selective catalyst reduction light-off strategy

    DOE Patents [OSTI]

    Gonze, Eugene V [Pinckney, MI

    2011-10-18

    An emissions control system includes a temperature determination module and an emissions control module. The temperature determination module determines a first temperature of a heater element of a diesel particulate filter (DPF) assembly in an exhaust system and determines a second temperature of a catalyst of the DPF assembly. The emissions control module selectively activates the heater element, selectively initiates a predefined combustion process in an engine based upon the first temperature, and selectively starts a reductant injection process based upon the second temperature.

  1. Electrically heated particulate filter using catalyst striping

    DOE Patents [OSTI]

    Gonze, Eugene V; Paratore, Jr., Michael J; Ament, Frank

    2013-07-16

    An exhaust system that processes exhaust generated by an engine is provided. The system generally includes a particulate filter (PF) that filters particulates from the exhaust wherein an upstream end of the PF receives exhaust from the engine. A grid of electrically resistive material is applied to an exterior upstream surface of the PF and selectively heats exhaust passing through the grid to initiate combustion of particulates within the PF. A catalyst coating is applied to the PF that increases a temperature of the combustion of the particulates within the PF.

  2. Hydrogen recombiner catalyst test supporting data

    SciTech Connect (OSTI)

    Britton, M.D.

    1995-01-19

    This is a data package supporting the Hydrogen Recombiner Catalyst Performance and Carbon Monoxide Sorption Capacity Test Report, WHC-SD-WM-TRP-211, Rev 0. This report contains 10 appendices which consist of the following: Mass spectrometer analysis reports: HRC samples 93-001 through 93-157; Gas spectrometry analysis reports: HRC samples 93-141 through 93-658; Mass spectrometer procedure PNL-MA-299 ALO-284; Alternate analytical method for ammonia and water vapor; Sample log sheets; Job Safety analysis; Certificate of mixture analysis for feed gases; Flow controller calibration check; Westinghouse Standards Laboratory report on Bois flow calibrator; and Sorption capacity test data, tables, and graphs.

  3. Catalyst for elemental sulfur recovery process

    DOE Patents [OSTI]

    Flytzani-Stephanopoulos, M.; Liu, W.

    1995-01-24

    A catalytic reduction process is described for the direct recovery of elemental sulfur from various SO[sub 2]-containing industrial gas streams. The catalytic process provides high activity and selectivity, as well as stability in the reaction atmosphere, for the reduction of SO[sub 2] to elemental sulfur product with carbon monoxide or other reducing gases. The reaction of sulfur dioxide and reducing gas takes place over a metal oxide composite catalyst having one of the following empirical formulas: [(FO[sub 2])[sub 1[minus]n](RO)[sub n

  4. Effects of oxygen and catalyst on tetraphenylborate decomposition rate

    SciTech Connect (OSTI)

    Walker, D.D.

    1999-12-15

    Previous studies indicate that palladium catalyzes rapid decomposition of alkaline tetraphenylborate slurries. Oxygen inhibits the reaction at low temperature (25 C), presumably by preventing activation of the catalyst. The present study investigated oxygen's inhibiting effectiveness at higher temperature (45 C) and catalyst concentrations.

  5. Cobalt Fischer-Tropsch catalysts having improved selectivity

    DOE Patents [OSTI]

    Miller, James G. (Pearl River, NY); Rabo, Jule A. (Armonk, NY)

    1989-01-01

    A cobalt Fischer-Tropsch catalyst having an improved steam treated, acid extracted LZ-210 support is taught. The new catalyst system demonstrates improved product selectivity at Fischer-Tropsch reaction conditions evidenced by lower methane production, higher C.sub.5.sup.+ yield and increased olefin production.

  6. Silica-Supported Tantalum Clusters: Catalyst for Alkane Conversion

    SciTech Connect (OSTI)

    Nemana ,S.; Gates, B.

    2006-01-01

    Silica-supported tantalum clusters (on average, approximately tritantalum) were formed by the treatment, in either H{sub 2} or ethane, of adsorbed Ta(CH{sub 2}Ph){sub 5}; the supported catalyst is active for ethane conversion to methane and propane at 523 K, with the used catalyst containing clusters of the same average nuclearity as the precursor.

  7. The Use of Catalysts in Near-Critical Water Processing

    SciTech Connect (OSTI)

    Elliott, Douglas C.

    2005-06-26

    The use of heterogeneous catalysts in near-critical water processing provides many challenges of material stability in addition to the normal questions of chemical activity. Conventional catalyst materials developed in traditional organic chemistry or petroleum chemistry applications provide a source of information of materials with the required activities but often without the required stability when used in hot liquid water. The importance of the use of catalysts in near-critical water processing plays a particularly crucial role for the development of renewable fuels and chemicals based on biomass feedstocks. Stability issues include both those related to the catalytic metal and also to the catalyst support material. In fact, the stability of the support is the most likely concern when using conventional catalyst formulations in near-critical water processing. Processing test results are used to show important design parameters for catalyst formulations for use in wet biomass gasification in high-pressure water and in catalytic hydrogenations in water for production of value-added chemical products from biomass in the biorefinery concept. Analytical methods including powder x-ray diffraction for crystallite size and composition determination, surface area and porosity measurements, and elemental analysis have all been used to quantify differences in catalyst materials before and after use. By these methods both the chemical and physical stability of heterogeneous catalysts can be verified.

  8. Development of Highly Selective Oxidation Catalysts by Atomic Layer Deposition

    Broader source: Energy.gov [DOE]

    This factsheet describes a research project whose goal is to use Atomic Layer Deposition to construct nanostructured catalysts to improve the effectiveness of oxidative dehydrogenation of alkanes. More effective catalysts could enable higher specific conversion rates and result in drastic energy savings - up to 25 trillion Btu per year by 2020.

  9. Effects of catalyst pretreatment for carbon nanotube growth

    E-Print Network [OSTI]

    Morgan, Caitlin D

    2007-01-01

    The effects of pretreatment of iron catalyst for carbon nanotube (CNT) growth was studied. CNTs were grown on Fe/A1203 (1/10 nm) thin-film catalyst deposited on silicon substrates via exposure to C2H4 in a thermal chemical ...

  10. NOVEL SLURRY PHASE DIESEL CATALYSTS FOR COAL-DERIVED SYNGAS

    SciTech Connect (OSTI)

    Dr. Dragomir B. Bukur; Dr. Ketil Hanssen; Alec Klinghoffer; Dr. Lech Nowicki; Patricia O'Dowd; Dr. Hien Pham; Jian Xu

    2001-01-07

    This report describes research conducted to support the DOE program in novel slurry phase catalysts for converting coal-derived synthesis gas to diesel fuels. The primary objective of this research program is to develop attrition resistant catalysts that exhibit high activities for conversion of coal-derived syngas.

  11. A New Instrument For Characterizing Solid Oxide Fuel Cell Catalysts

    E-Print Network [OSTI]

    RESEARCH HIGHLIGHTS A New Instrument For Characterizing Solid Oxide Fuel Cell Catalysts From fuels to renewable energy sources. Solid oxide fuel cells (SOFCs) have enormous potential in this area A New Instrument For Characterizing Solid Oxide Fuel Cell Catalysts Rob Usiskin In partnership

  12. Supported organometallic catalysts for hydrogenation and Olefin Polymerization

    DOE Patents [OSTI]

    Marks, Tobin J. (Evanston, IL); Ahn, Hongsang (Evanston, IL)

    2001-01-01

    Novel heterogeneous catalysts for the which hydrogenation of olefins and arenes with high conversion rates under ambient conditions and the polymerization of olefins have been developed. The catalysts are synthesized from Ziegler-type precatalysts by supporting them on sulfate-modified zirconia.

  13. ATTRITION RESISTANT IRON-BASED FISCHER-TROPSCH CATALYSTS

    SciTech Connect (OSTI)

    James G. Goodwin, Jr.; James J. Spivey; K. Jothimurugesan; Santosh K. Gangwal

    1999-03-29

    The Fischer-Tropsch (F-T) reaction provides a way of converting coal-derived synthesis gas (CO+H{sub 2}) to liquid fuels. Since the reaction is highly exothermic, one of the major problems in control of the reaction is heat removal. Recent work has shown that the use of slurry bubble column reactors (SBCRs) can largely solve this problem. Iron-based (Fe) catalysts are preferred catalysts for F-T when using low CO/H2 ratio synthesis gases derived from modern coal gasifiers. This is because in addition to reasonable F-T activity, the F-T catalysts also possess high water gas shift (WGS) activity. However, a serious problem with the use of Fe catalysts in a SBCR is their tendency to undergo attrition. This can cause fouling/plugging of downstream filters and equipment, making the separation of catalyst from the oil/wax product very difficult if not impossible, and results in a steady loss of catalyst from the reactor. The objectives of this research are to develop a better understanding of the parameters affecting attrition resistance of Fe F-T catalysts suitable for use in SBCRs and to incorporate this understanding into the design of novel Fe catalysts having superior attrition resistance. Catalyst preparations will be based on the use of spray drying and will be scalable using commercially available equipment. The research will employ among other measurements, attrition testing and F-T synthesis, including long duration slurry reactor runs in order to ascertain the degree of success of the various preparations. The goal is to develop an Fe catalyst which can be used in a SBCR having only an internal filter for separation of the catalyst from the liquid product, without sacrificing F-T activity and selectivity. The effect of silica addition via coprecipitation and as a binder to a doubly promoted Fischer-Tropsch synthesis iron catalyst (100 Fe/5 Cu/4.2 K) was studied. The catalysts were prepared by coprecipitation, followed by binder addition and drying in a 1 m diameter, 2 m tall spray dryer. The binder silica content was varied from 0 to 20 wt %. A catalyst with 12 wt % binder silica was found to have the highest attrition resistance. F-T reaction studies over 100 hours in a fixed-bed reactor showed that this catalyst maintained around 95 % CO conversion with a methane selectivity of less than 7 wt % and a C5 + selectivity of greater than 73 wt %. The effect of adding precipitated silica from 0 to 20 parts by weight to this catalyst (containing 12 wt % binder silica) was also studied. Addition of precipitated silica was found to be detrimental to attrition resistance and resulted in increased methane and reduced wax formation. An HPR series of proprietary catalysts was prepared to further improve the attrition resistance. Based on the experience gained, a proprietary HPR-43 catalyst has been successfully spray dried in 500 g quantity. This catalyst showed 95 % CO conversion over 125 h and had less than 4 % methane selectivity. Its attrition resistance was one of the highest among the catalyst tested.

  14. Ceramic wash-coat for catalyst support

    DOE Patents [OSTI]

    Kulkarni, Anand A.; Subramanian, Ramesh; Sabol, Stephen M.

    2012-08-14

    Abstract A wash-coat (16) for use as a support for an active catalyst species (18) and a catalytic combustor component (10) incorporating such wash-coat. The wash-coat is a solid solution of alumina or alumina-based material (Al.sub.2O.sub.3-0-3 wt % La.sub.2O.sub.3) and a further oxide exhibiting a coefficient of thermal expansion that is lower than that exhibited by alumina. The further oxide may be silicon dioxide (2-30 wt % SiO.sub.2), zirconia silicate (2-30 wt % ZrSiO.sub.4), neodymium oxide (0-4 wt %), titania (Al.sub.2O.sub.3-3-40% TiO.sub.2) or alumina-based magnesium aluminate spinel (Al.sub.2O.sub.3-25 wt % MgO) in various embodiments. The active catalyst species may be palladium and a second metal in a concentration of 10-50% of the concentration of the palladium.

  15. Catalyst Additives to Enhance Mercury Oxidation and Capture

    SciTech Connect (OSTI)

    Alex J. Berry; Thomas K. Gale

    2005-09-30

    Preliminary research has shown that SCR catalysts employed for nitrogen-oxide reduction can effectively oxidize mercury. This report discusses initial results from fundamental investigations into the behavior of mercury species in the presence of SCR catalysts at Southern Research Institute. The testing was performed at Southern Research's Catalyst Test Facility, a bench-scale reactor capable of simulating gas-phase reactions occurring in coal-fired utility pollution-control equipment. Three different SCR catalysts are currently being studied in this project - honeycomb-type, plate-type, and a hybrid-type catalyst. The catalysts were manufactured and supplied by Cormetech Inc., Hitachi America Ltd., and Haldor-Topsoe Inc., respectively. Parametric testing was performed to investigate the contribution of flue-gas chemistry on mercury oxidation via SCR catalysts. Methods and procedures for experimental testing continue to be developed to produce the highest quality mercury-oxidation data. Most experiments so far have focused on testing the catalysts in a simulated Powder River Basin (PRB) flue-gas environment, which contains lower sulfur and chlorine than produced by other coals. Future work to characterize flue gas simulations typically derived from low and high sulfur bituminous coal will be performed in a stepwise manner, to avoid the constant interruptions in testing that occur when leaks in the system are generated during temperature transitions. Specifically, chlorine concentration vs. mercury oxidation graph will be developed for each catalyst. The contributions of temperature and later sulfur will be investigated after this is complete. Also, last quarter's tests showed a potential linear relationship between SO3 conversion and mercury oxidation. As a result, SO3 samples will be taken more frequently to investigate each catalyst's ability to selectively oxidize mercury.

  16. Nanoparticle "theranostic" platforms for applications in cancer

    E-Print Network [OSTI]

    Steiner, Jason Michael

    2011-01-01

    addressed by oscillating magnetic fields and produce aa rapidly oscillating external magnetic field, nanoparticles

  17. Novel, Low-Cost Nanoparticle Production

    SciTech Connect (OSTI)

    2011-05-31

    Fact sheet describing a modular hybrid plasma reactor and process to manufacture low-cost nanoparticles

  18. Morphology Control of Noble Metal Nanoparticle Catalysts Using Strategic Organic Capping Agents in Colloidal Phase Synthesis

    E-Print Network [OSTI]

    Roeser, Kayla Mae

    2014-01-01

    A Selective Review. Fuel Cells 1, 105-116, doi:10.1002/1615-and challenges for automotive fuel cells. Nature 486, 43-51,Coversion for Hydrogen-Fuel-Cell-Driven Vehicles. Catalysis

  19. Hidden features of the catalyst nanoparticles favorable for single-walled carbon nanotube growth

    E-Print Network [OSTI]

    Curtarolo, Stefano

    nanotube growth by using chemical vapor deposition synthesis augmented by an attached mass spectrometer MS,16 Fig. 1 a , a widely debated issue in the literature.7­10 Based on the cal- culated Fe­C liquidus lines to mention that in our studies we use methane gas. Unlike methane, the dehydrogenation reactions of other

  20. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    polymer electrolyte fuel cell (PEFC), (2) alkaline fuel cell (AFC), (3) phosphoric acid fuel cell (PAFC),(4) molten carbonate

  1. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    GRAPHENE OXIDE (RGO)/CARBON BLACK (CB) COMPOSITE .. 139 Introduction .. 139 Experimental 140 7.2.1 Synthesis of Pt NCs 140 7.2.2 Preparation

  2. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    interest as electrocatalysts for fuel cell applications. 1-3molecules for the fuel cell applications. 13 The synthesiscatalysts for fuel cell applications. The biomimetic

  3. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    Stamenkovic, V. ; Ross, P. N. Fuel Cells Min, M. K. ; Cho,Stamenkovic, V. ; Ross, P. N. Fuel Cell B643. Dillon, R. ;Hormes, J. ; Behm, R. J. Fuel Cells 2006 , 6 , 190. Wang, H.

  4. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    as better catalytic performance in oxidation of methanol,as better catalytic performance in oxidation of methanol,as CO oxidation, which enhanced their catalytic activity and

  5. Nanoparticle Silver Catalysts That Show Enhanced Activity for Carbon Dioxide Electrolysis

    E-Print Network [OSTI]

    Kenis, Paul J. A.

    Information ABSTRACT: Electrochemical conversion of CO2 has been proposed both as a way to reduce CO2 emissions and as a source of renewable fuels and chemicals, but conversion rates need improvement before the process will be practical. In this article, we show that the rate of CO2 conversion per unit surface area

  6. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    Y. , Biomimetic Synthesis of Inorganic Materials and Theirsynthesis of inorganic materials .NPs. 1.2 Biomimetic synthesis of inorganic materials Through

  7. Deactivation resistance of Pd/Au nanoparticle catalysts for water-phase hydrodechlorination

    E-Print Network [OSTI]

    Alvarez, Pedro J.

    and Biomolecular Engineering, Rice University, 6100 S. Main Street, Houston, TX 77005, United States b Department States c Department of Chemistry, Rice University, 6100 S. Main Street, Houston, TX 77005, United States, Houston, TX 77005, United States a r t i c l e i n f o Article history: Received 6 May 2009 Revised 24

  8. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    electrolyte fuel cell (PEFC), (2) alkaline fuel cell (with different electrolyte. PEFC Electrolyte AFC PAFC MCFCDEFC), which can be used with PEFC configuration, and direct

  9. Biomimetic Synthesis of Noble Metal Nanoparticles and Their Applications as Electro-catalysts in Fuel Cells

    E-Print Network [OSTI]

    Li, Yujing

    2012-01-01

    and (5) solid oxide fuel cell (SOFC). The characteristics ofPEFC Electrolyte AFC PAFC MCFC SOFC Hydrated Polymeric Iondeveloped with AFC, MCFC, and SOFC configurations. The

  10. Ordered Nanoparticle Catalysts article is an Energy Focus > Archived News

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration wouldMass mapSpeeding access toOctober 1996TechnologiesDistribution,Oracle

  11. Mass-selected Nanoparticles of PtxY as Model Catalysts for Oxygen

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

    AFDC Printable Version Share this resource Send a link to EERE: Alternative Fuels Data Center Home Page to someone by E-mail Share EERE: Alternative Fuels Data Center Home Page on Facebook Tweet about EERE: Alternative Fuels Data Center Home Page on Twitter Bookmark EERE: Alternative Fuels Data Center Homesum_a_epg0_fpd_mmcf_m.xls" ,"Available from WebQuantityBonneville Power Administration wouldMass map shines light on dark matter By Sarah Schlieder * July 9, 2015 Tweet

  12. Methane ignition catalyzed by in situ generated palladium nanoparticles

    SciTech Connect (OSTI)

    Shimizu, T.; Abid, A.D.; Poskrebyshev, G.; Wang, H. [Department of Aerospace and Mechanical Engineering, University of Southern California, Los Angeles, CA 90089 (United States); Nabity, J.; Engel, J.; Yu, J. [TDA Research, Inc., 12345 W. 52nd Ave, Wheat Ridge, CO 80033 (United States); Wickham, D. [Reaction Systems, LLC, 19039 E. Plaza Drive, Suite 290, Parker, CO 80134 (United States); Van Devener, B.; Anderson, S.L. [Department of Chemistry, University of Utah, Salt Lake City, UT 84112 (United States); Williams, S. [Air Force Research Laboratory, Mail Stop RZA, 1950 Fifth Street, WPAFB, OH 45433 (United States)

    2010-03-15

    Catalytic ignition of methane over the surfaces of freely-suspended and in situ generated palladium nanoparticles was investigated experimentally and numerically. The experiments were conducted in a laminar flow reactor. The palladium precursor was a compound (Pd(THD){sub 2}, THD: 2,2,6,6-tetramethyl-3,5-heptanedione) dissolved in toluene and injected into the flow reactor as a fine aerosol, along with a methane-oxygen-nitrogen mixture. For experimental conditions chosen in this study, non-catalytic, homogeneous ignition was observed at a furnace temperature of {proportional_to}1123 K, whereas ignition of the same mixture with the precursor was found to be {proportional_to}973 K. In situ production of Pd/PdO nanoparticles was confirmed by scanning mobility, transmission electron microscopy and X-ray photoelectron spectroscopy analyses of particles collected at the reactor exit. The catalyst particle size distribution was log-normal. Depending on the precursor loading, the median diameter ranged from 10 to 30 nm. The mechanism behind catalytic ignition was examined using a combined gas-phase and gas-surface reaction model. Simulation results match the experiments closely and suggest that palladium nanocatalyst significantly shortens the ignition delay times of methane-air mixtures over a wide range of conditions. (author)

  13. DEVELOPMENT OF PRECIPITATED IRON FISCHER-TROPSCH CATALYSTS

    SciTech Connect (OSTI)

    Dr. Dragomir B. Bukur; Dr. X. Lang; Dr. S. Chokkaram; Dr. L. Nowicki; G. Wei; Dr. Y. Ding; Dr. B. Reddy; Dr. S. Xiao

    1999-07-22

    Despite the current worldwide oil glut, the US will ultimately require large-scale production of liquid (transportation) fuels from coal. Slurry phase Fischer-Tropsch (F-T) technology, with its versatile product slate, may be expected to play a major role in production of transportation fuels via indirect coal liquefaction. Some of the F-T catalysts synthesized and tested at Texas A and M University under DOE Contract No. DE-AC22-89PC89868 were more active than any other known catalysts developed for maximizing production of high molecular weight hydrocarbons (waxes). The objectives of the present contract were to demonstrate repeatability of catalyst performance and reproducibility of preparation procedures of two of these catalysts on a laboratory scale. Improvements in the catalyst performance were attempted through the use of: (a) higher reaction pressure and gas space velocity to maximize the reactor productivity; (b) modifications in catalyst preparation steps; and (c) different pretreatment procedures. Repeatability of catalyst performance and reproducibility of catalyst synthesis procedure have been successfully demonstrated in stirred tank slurry reactor tests. Reactor space-time-yield was increased up to 48% by increasing reaction pressure from 1.48 MPa to 2.17 MPa, while maintaining the gas contact time and synthesis gas conversion at a constant value. Use of calcination temperatures above 300 C, additional CaO promoter, and/or potassium silicate as the source of potassium promoter, instead of potassium bicarbonate, did not result in improved catalyst performance. By using different catalyst activation procedures they were able to increase substantially the catalyst activity, while maintaining low methane and gaseous hydrocarbon selectivities. Catalyst productivity in runs SA-0946 and SA-2186 was 0.71 and 0.86 gHC/g-Fe/h, respectively, and this represents 45-75% improvement in productivity relative to that achieved in Rheinpreussen's demonstration plant unit (the most successful bubble column slurry reactor performance to date), and sets new standards of performance for ''high alpha'' iron catalysts.

  14. Carbon-Supported IrNi Core-Shell Nanoparticles: Synthesis Characterization and Catalytic Activity

    SciTech Connect (OSTI)

    K Sasaki; K Kuttiyiel; L Barrio; D Su; A Frenkel; N Marinkovic; D Mahajan; R Adzic

    2011-12-31

    We synthesized carbon-supported IrNi core-shell nanoparticles by chemical reduction and subsequent thermal annealing in H{sub 2}, and verified the formation of Ir shells on IrNi solid solution alloy cores by various experimental methods. The EXAFS analysis is consistent with the model wherein the IrNi nanoparticles are composed of two-layer Ir shells and IrNi alloy cores. In situ XAS revealed that the Ir shells completely protect Ni atoms in the cores from oxidation or dissolution in an acid electrolyte under elevated potentials. The formation of Ir shell during annealing due to thermal segregation is monitored by time-resolved synchrotron XRD measurements, coupled with Rietveld refinement analyses. The H{sub 2} oxidation activity of the IrNi nanoparticles was found to be higher than that of a commercial Pt/C catalyst. This is predominantly due to Ni-core-induced Ir shell contraction that makes the surface less reactive for IrOH formation, and the resulting more metallic Ir surface becomes more active for H{sub 2} oxidation. This new class of core-shell nanoparticles appears promising for application as hydrogen anode fuel cell electrocatalysts.

  15. Nanoparticle enhanced ionic liquid heat transfer fluids

    DOE Patents [OSTI]

    Fox, Elise B.; Visser, Ann E.; Bridges, Nicholas J.; Gray, Joshua R.; Garcia-Diaz, Brenda L.

    2014-08-12

    A heat transfer fluid created from nanoparticles that are dispersed into an ionic liquid is provided. Small volumes of nanoparticles are created from e.g., metals or metal oxides and/or alloys of such materials are dispersed into ionic liquids to create a heat transfer fluid. The nanoparticles can be dispersed directly into the ionic liquid during nanoparticle formation or the nanoparticles can be formed and then, in a subsequent step, dispersed into the ionic liquid using e.g., agitation.

  16. Catalyst Additives to Enhance Mercury Oxidation and Capture

    SciTech Connect (OSTI)

    Thomas K. Gale

    2006-06-30

    Catalysis is the key fundamental ingredient to convert elemental mercury in coal-fired power stations into its oxidized forms that are more easily captured by sorbents, ESPs, baghouses, and wet scrubbers, whether the catalyst be unburned carbon (UBC) in the ash or vanadium pentoxide in SCR catalysts. This project has investigated several different types of catalysts that enhance mercury oxidation in several different ways. The stated objective of this project in the Statement of Objectives included testing duct-injection catalysts, catalyst-sorbent hybrids, and coated low-pressure-drop screens. Several different types of catalysts were considered for duct injection, including different forms of iron and carbon. Duct-injection catalysts would have to be inexpensive catalysts, as they would not be recycled. Iron and calcium had been shown to catalyze mercury oxidation in published bench-scale tests. However, as determined from results of an on-going EPRI/EPA project at Southern Research, while iron and calcium did catalyze mercury oxidation, the activity of these catalysts was orders of magnitude below that of carbon and had little impact in the short residence times available for duct-injected catalysts or catalyst-sorbent hybrids. In fact, the only catalyst found to be effective enough for duct injection was carbon, which is also used to capture mercury and remove it from the flue gas. It was discovered that carbon itself is an effective catalyst-sorbent hybrid. Bench-scale carbon-catalyst tests were conducted, to obtain kinetic rates of mercury adsorption (a key step in the catalytic oxidation of mercury by carbon) for different forms of carbon. All carbon types investigated behaved in a similar manner with respect to mercury sorption, including the effect of temperature and chlorine concentration. Activated carbon was more effective at adsorbing mercury than carbon black and unburned carbon (UBC), because their internal surface area of activated carbon was greater. Catalyst coating of low-pressure-drop screens was of particular interest as this project was being developed. However, it was discovered that URS was already heavily involved in the pursuit of this same technology, being funded by DOE, and reporting significant success. Hence, testing of SCR catalysts became a major focus of the project. Three different commercial SCR catalysts were examined for their ability to oxidize mercury in simulated flue-gas. Similar performance was observed from each of the three commercial catalysts, both in terms of mercury oxidation and SO{sub 3} generation. Ammonia injection hindered mercury oxidation at low HCl concentrations (i.e., {approx}2 ppmv), yet had little impact on mercury oxidation at higher HCl concentrations. On the other hand, SO{sub 2} oxidation was significantly reduced by the presence of ammonia at both low and high concentrations of HCl.

  17. ATTRITION RESISTANT IRON-BASED FISCHER-TROPSCH CATALYSTS

    SciTech Connect (OSTI)

    K. Jothimurugesan; James G. Goodwin, Jr.; Santosh K. Gangwal

    1999-10-01

    Fischer-Tropsch (FT) synthesis to convert syngas (CO + H{sub 2}) derived from natural gas or coal to liquid fuels and wax is a well-established technology. For low H{sub 2} to CO ratio syngas produced from CO{sub 2} reforming of natural gas or from gasification of coal, the use of Fe catalysts is attractive because of their high water gas shift activity in addition to their high FT activity. Fe catalysts are also attractive due to their low cost and low methane selectivity. Because of the highly exothermic nature of the FT reaction, there has been a recent move away from fixed-bed reactors toward the development of slurry bubble column reactors (SBCRs) that employ 30 to 90 {micro}m catalyst particles suspended in a waxy liquid for efficient heat removal. However, the use of FeFT catalysts in an SBCR has been problematic due to severe catalyst attrition resulting in fines that plug the filter employed to separate the catalyst from the waxy product. Fe catalysts can undergo attrition in SBCRs not only due to vigorous movement and collisions but also due to phase changes that occur during activation and reaction.

  18. Deactivation by carbon of iron catalysts for indirect liquefaction

    SciTech Connect (OSTI)

    Bartholomew, C.H.

    1991-01-10

    Although promoted cobalt and iron catalysts for Fischer-Tropsch (FT) synthesis of gasoline feedstock were first developed more than three decades ago, a major technical problem still limiting the commercial use of these catalysts today is carbon deactivation. This report describes recent progress in a fundamental, three-year investigation of carbon formation and its effects on the activity and selectivity of promoted iron catalysts for FT synthesis, the objectives of which are to: determine rates and mechanisms of carbon deactivation of unsupported Fe and Fe/K catalysts during CO hydrogenation over a range of CO concentrations, CO:H{sub 2} ratios, and temperatures; and model the rates of deactivation of the same catalysts in fixed-bed reactors. To accomplish the above objectives, the project is divided into the following tasks: (1) determine the kinetics of reaction and of carbon deactivation during CO hydrogenation on Fe and Fe/K catalysts coated on monolith bodies. (2) Determine the reactivities and types of carbon deposited during reaction on the same catalysts from temperature-programmed-surface-reaction spectroscopy (TPSR) and transmission electron microscopy (TEM). Determine the types of iron carbides formed at various temperatures and H{sub 2}/CO ratios using x-ray diffraction and Moessbauer spectroscopy. (3) Develop mathematical deactivation models which include heat and mass transport contributions for FT synthesis is packed-bed reactors. Progress to date is described. 48 refs., 3 figs., 1 tab.

  19. 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.

  20. Catalysts for the selective oxidation of hydrogen sulfide to sulfur

    DOE Patents [OSTI]

    Srinivas, Girish (Thornton, CO); Bai, Chuansheng (Baton Rouge, LA)

    2000-08-08

    This invention provides catalysts for the oxidation of hydrogen sulfide. In particular, the invention provides catalysts for the partial oxidation of hydrogen sulfide to elemental sulfur and water. The catalytically active component of the catalyst comprises a mixture of metal oxides containing titanium oxide and one or more metal oxides which can be selected from the group of metal oxides or mixtures of metal oxides of transition metals or lanthanide metals. Preferred metal oxides for combination with TiO.sub.2 in the catalysts of this invention include oxides of V, Cr, Mn, Fe, Co, Ni, Cu, Nb, Mo, Tc, Ru, Rh, Hf, Ta, W, Au, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu. Catalysts which comprise a homogeneous mixture of titanium oxide and niobium (Nb) oxide are also provided. A preferred method for preparing the precursor homogenous mixture of metal hydroxides is by coprecipitation of titanium hydroxide with one or more other selected metal hydroxides. Catalysts of this invention have improved activity and/or selectivity for elemental sulfur production. Further improvements of activity and/or selectivity can be obtained by introducing relatively low amounts (up to about 5 mol %)of a promoter metal oxide (preferably of metals other than titanium and that of the selected second metal oxide) into the homogeneous metal/titanium oxide catalysts of this invention.