WorldWideScience

Sample records for bimetallic dispersed catalysts

  1. Novel bimetallic dispersed catalysts for temperature-programmed coal liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Chunshan, Song; Kirby, S.; Schmidt, E. [Pennsylvania State Univ., University Park, PA (United States)] [and others

    1995-12-31

    The objective of this project is to explore bimetallic dispersed catalysts for more efficient coal liquefaction. Coal liquefaction involves cleavage of methylene, dimethylene and ether bridges connecting various aromatic units and the reactions of various oxygen functional groups. This paper describes recent results on (1) hydrodeoxygenation of O-containing polycyclic model compounds using novel organometallic catalyst precursors; and (2) activity and selectivity of dispersed Fe catalysts from organometallic and inorganic precursors for hydrocracking of 4-(1-naphthylmethyl) bibenzyl. The results showed that some iron containing catalysts have higher activity in the sulfur-free form, contrary to conventional wisdom. Adding sulfur to Fe precursors with Cp-ligands decreased the activity of the resulting catalyst. This is in distinct contrast to the cases with iron pentacarbonyl and superfine Fe{sub 2}O{sub 3}, where S addition increased their catalytic activity substantially. A positive correlation between sulfur addition and increased activity can be seen, but a reversed trend between Fe cluster size and hydrocracking conversion could be observed, for carbonyl-type Fe precursors. It is apparent that the activity and selectivity of Fe catalysts for NMBB conversion depends strongly on both the type of ligand environment, the oxidation state and the number of intermetal bonds in the molecular precursor.

  2. Bimetallic Catalysts.

    Science.gov (United States)

    Sinfelt, John H.

    1985-01-01

    Chemical reaction rates can be controlled by varying composition of miniscule clusters of metal atoms. These bimetallic catalysts have had major impact on petroleum refining, where work has involved heterogeneous catalysis (reacting molecules in a phase separate from catalyst.) Experimentation involving hydrocarbon reactions, catalytic…

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

    Energy Technology Data Exchange (ETDEWEB)

    Chunshan Song; Schobert, H.H.; Parfitt, D.P. [and others

    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.

  4. Preparation and catalytic performance of monolayer-dispersed Pd/Ni bimetallic catalysts for hydrogenation

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    Pd/Ni bimetallic catalysts were prepared by replacement reactions,characterized by X-ray diffraction,CO chemisorption and H2 temperature-programmed desorption,and evaluated for hydrogenation of cyclohexene,styrene and acetone.The results show that Pd atoms are monolayer-dispersed on the Ni surface in these Pd/Ni catalysts.Consequently,Pd/Ni catalysts are much more active than Pd/Ni and Pd/γ-Al2O3 with the same Pd loading prepared by the conventional impregnation method.

  5. Preparation of highly dispersed Ru-Sn bimetallic supported catalysts from the single source precursors Cp(PPh32Ru-SnX3 (X = Cl or Br

    Directory of Open Access Journals (Sweden)

    Ana Cláudia Bernardes Silva

    2003-06-01

    Full Text Available In this work highly dispersed Ru-Sn bimetallic catalysts have been prepared from organobimetallic Cp(PPh32Ru-SnX3 (X = Cl or Br complexes. These single source precursors can be easily impregnated in high surface area supports, such as activated carbon and sol-gel SiO2, and upon controlled thermal treatment the ligands are released as volatile products resulting in the formation of the bimetallic system Ru-Sn. Catalytic reactions, such as hydrodechlorination of CCl4 and chlorobenzene and TPR (Temperature Programmed Reduction experiments carried out with these RuSn catalysts suggested a strong interaction between Ruthenium and Tin. Mössbauer measurements showed that these materials when exposed to air are immediately oxidized to form Sn (IV. It was shown that upon controlled reduction conditions with H2 it is possible to reduce selectively Sn to different oxidation states and different phases. The Sn oxidation state showed significant effect on the catalytic hydrogenation of 1,5-cyclooctadiene. The use of these single source precursors with a controlled decomposition/reduction procedure allows the preparation of unique catalysts with an intimate interaction between the components ruthenium and tin and the possibility of varying the Sn oxidation state around the Ru metal.

  6. Preparation of highly dispersed Ru-Sn bimetallic supported catalysts from the single source precursors Cp(PPh3)2Ru-SnX3 (X = Cl or Br)

    OpenAIRE

    Ana Cláudia Bernardes Silva; Ana Paula Guimarães de Sousa; José Domingos Ardisson; Helmuth Guido Luna Siebald; Edmilson Moura; Eduardo Nicolau dos Santos; Nelcy Della Santina Mohallem; Rochel Montero Lago

    2003-01-01

    In this work highly dispersed Ru-Sn bimetallic catalysts have been prepared from organobimetallic Cp(PPh3)2Ru-SnX3 (X = Cl or Br) complexes. These single source precursors can be easily impregnated in high surface area supports, such as activated carbon and sol-gel SiO2, and upon controlled thermal treatment the ligands are released as volatile products resulting in the formation of the bimetallic system Ru-Sn. Catalytic reactions, such as hydrodechlorination of CCl4 and chlorobenzene and TPR...

  7. Direct decomposition of methane over SBA-15 supported Ni, Co and Fe based bimetallic catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Pudukudy, Manoj, E-mail: manojpudukudy@gmail.com [Fuel Cell Institute, Universiti Kebangsaan Malaysia, UKM, Bangi 43600, Selangor (Malaysia); Department of Chemical and Process Engineering, Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, UKM, Bangi 43600, Selangor (Malaysia); Yaakob, Zahira, E-mail: zahirayaakob65@gmail.com [Department of Chemical and Process Engineering, Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, UKM, Bangi 43600, Selangor (Malaysia); Akmal, Zubair Shamsul [Department of Chemical and Process Engineering, Faculty of Engineering and Built Environment, Universiti Kebangsaan Malaysia, UKM, Bangi 43600, Selangor (Malaysia)

    2015-03-01

    Graphical abstract: - Highlights: • Synthesis and characterization of Ni, Co and Fe based bimetallic catalysts supported over SBA-15. • Thermocatalytic decomposition of methane over the SBA-15 supported bimetallic catalysts. • Enhanced catalytic efficiency of the bimetallic catalysts for the production of CO{sub x} free hydrogen and nanocarbon. • Production of value added open tip hollow multi-walled carbon nanotubes. • Crystalline characterization of carbon nanotubes by XRD, Raman and thermogravimetric analysis. - Abstract: Thermocatalytic decomposition of methane is an alternative route for the production of CO{sub x}-free hydrogen and carbon nanomaterials. In this work, a set of novel Ni, Co and Fe based bimetallic catalysts supported over mesoporous SBA-15 was synthesized by a facile wet impregnation route, characterized for their structural, textural and reduction properties and were successfully used for the methane decomposition. The fine dispersion of metal oxide particles on the surface of SBA-15, without affecting its mesoporous texture was clearly shown in the low angle X-ray diffraction patterns and the transmission electron microscopy (TEM) images. The nitrogen sorption analysis showed the reduced specific surface area and pore volume of SBA-15, after metal loading due to the partial filling of hexagonal mesopores by metal species. The results of methane decomposition experiments indicated that all of the bimetallic catalysts were highly active and stable for the reaction at 700 °C even after 300 min of time on stream (TOS). However, a maximum hydrogen yield of ∼56% was observed for the NiCo/SBA-15 catalyst within 30 min of TOS. A high catalytic stability was shown by the CoFe/SBA-15 catalyst with 51% of hydrogen yield during the course of reaction. The catalytic stability of the bimetallic catalysts was attributed to the formation of bimetallic alloys. Moreover, the deposited carbons were found to be in the form of a new set of hollow

  8. Platinum-Bismuth Bimetallic Catalysts: Synthesis, Characterization and Applications

    OpenAIRE

    Saucedo, Jose A, Jr; Xiao, Yang; Varma, Arvind

    2015-01-01

    Bimetallic catalysts have been explored and shown to exhibit unique characteristics which are not present in monometallic catalysts. Platinum is well known as an effective catalyst for oxidation and reduction reactions, and it can be made more effective when bismuth is introduced as a promotor. Thus, the effectiveness of the Pt-Bi catalyst was demonstrated in prior work. What is not clear, however, is the mechanism behind the catalyst function; why addition of bismuth to platinum decreases de...

  9. Controlled surface segregation leads to efficient coke-resistant nickel/platinum bimetallic catalysts for the dry reforming of methane

    KAUST Repository

    Li, Lidong

    2015-02-03

    Surface composition and structure are of vital importance for heterogeneous catalysts, especially for bimetallic catalysts, which often vary as a function of reaction conditions (known as surface segregation). The preparation of bimetallic catalysts with controlled metal surface composition and structure is very challenging. In this study, we synthesize a series of Ni/Pt bimetallic catalysts with controlled metal surface composition and structure using a method derived from surface organometallic chemistry. The evolution of the surface composition and structure of the obtained bimetallic catalysts under simulated reaction conditions is investigated by various techniques, which include CO-probe IR spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near-edge structure analysis, XRD, and X-ray photoelectron spectroscopy. It is demonstrated that the structure of the bimetallic catalyst is evolved from Pt monolayer island-modified Ni nanoparticles to core-shell bimetallic nanoparticles composed of a Ni-rich core and a Ni/Pt alloy shell upon thermal treatment. These catalysts are active for the dry reforming of methane, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure. The reform of reforming: A series of alumina-supported Ni/Pt bimetallic nanoparticles (NPs) with controlled surface composition and structure are prepared. Remarkable surface segregation for these bimetallic NPs is observed upon thermal treatment. These bimetallic NPs are active catalysts for CO2 reforming of CH4, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure.

  10. Controlled Surface Segregation Leads to Efficient Coke-Resistant Nickel/Platinum Bimetallic Catalysts for the Dry Reforming of Methane

    Energy Technology Data Exchange (ETDEWEB)

    Li, Lidong [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Zhou, Lu [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Ould-Chikh, Samy [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Anjum, Dalaver H. [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Kanoun, Mohammed B. [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Scaranto, Jessica [SABIC Corporate Research and Innovation Center, Thuwal (Saudi Arabia); Hedhili, Mohamed N. [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Khalid, Syed [Brookhaven National Lab. (BNL), Upton, NY (United States); Laveille, Paco V. [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); D' Souza, Lawrence [SABIC Corporate Research and Innovation Center, Thuwal (Saudi Arabia); Clo, Alain [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia); Basset, Jean-Marie [King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)

    2015-02-03

    The surface composition and structure are of vital importance for heterogeneous catalysts, especially for bimetallic catalysts, which often vary as a function of reaction conditions (known as surface segregation). The preparation of bimetallic catalysts with controlled metal surface composition and structure is very challenging. In this study, we synthesize a series of Ni/Pt bimetallic catalysts with controlled metal surface composition and structure using a method derived from surface organometallic chemistry. Moreover, the evolution of the surface composition and structure of the obtained bimetallic catalysts under simulated reaction conditions is investigated by various techniques, which include CO-probe IR spectroscopy, high-angle annular dark-field scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, extended X-ray absorption fine structure analysis, X-ray absorption near-edge structure analysis, XRD, and X-ray photoelectron spectroscopy. It is demonstrated that the structure of the bimetallic catalyst is evolved from Pt monolayer island-modified Ni nanoparticles to core–shell bimetallic nanoparticles composed of a Ni-rich core and a Ni/Pt alloy shell upon thermal treatment. The catalysts are active for the dry reforming of methane, and their catalytic activities, stabilities, and carbon formation vary with their surface composition and structure.

  11. The synergistic effect in the Fe-Co bimetallic catalyst system for the growth of carbon nanotube forests

    Energy Technology Data Exchange (ETDEWEB)

    Hardeman, D.; Esconjauregui, S., E-mail: cse28@cam.ac.uk; Cartwright, R.; D' Arsié, L.; Robertson, J. [Department of Engineering, University of Cambridge, Cambridge CB3 0FA (United Kingdom); Bhardwaj, S.; Cepek, C. [Istituto Officina dei Materiali-CNR, Laboratorio TASC, Trieste I-34149 (Italy); Oakes, D.; Clark, J. [Johnson Matthey Technology Centre, Sonning Common RG4 9NH (United Kingdom); Ducati, C. [Department of Materials Science and Metallurgy, University of Cambridge, Cambridge CB3 0FS (United Kingdom)

    2015-01-28

    We report the growth of multi-walled carbon nanotube forests employing an active-active bimetallic Fe-Co catalyst. Using this catalyst system, we observe a synergistic effect by which—in comparison to pure Fe or Co—the height of the forests increases significantly. The homogeneity in the as-grown nanotubes is also improved. By both energy dispersive spectroscopy and in-situ x-ray photoelectron spectroscopy, we show that the catalyst particles consist of Fe and Co, and this dramatically increases the growth rate of the tubes. Bimetallic catalysts are thus potentially useful for synthesising nanotube forests more efficiently.

  12. Improvements in NOx reduction by carbon using bimetallic catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Illan-Gomez, M.J.; Brandan, S.; Salinas-Martinez de Lecea, C.; Linares-Solano, A. [Universidad de Alicante, Alicante (Spain). Departamento de Quimica Inorganica

    2001-11-30

    A catalysis of the C-NOx reaction has been studied to optimize the composition of the catalysts in order to decrease the carbon consumption by oxygen. Both the metal content and the composition of the catalysts have been investigated. The activity of bimetallic (KNi, NiCo and NiCu) catalysts for NOx reduction by carbon has been studied using both isothermal reactions at 300{sup o}C and temperature programmed reaction up to 500{sup o}C. It has been found that the experimental variables (i.e. amount of catalysts and nature of the bimetallic catalysts) determine the selectivity against carbon combustion by oxygen. Thus, it has been observed that the amount of catalyst greatly affects the C-O{sub 2} reaction but only lightly the C-NOx reaction and, consequently, modifies the selectivity of the catalyst for NOx reduction. Among the bimetallic catalysts tested, NiCu catalyst presents the best performance, at a temperature as low as 250{sup o}C, a high de-NOx activity and a high NOx selectivity due to a low carbon burn-off, with the additional advantage of the absence of N{sub 2}O and CO in the reaction products. Thus, the results obtained in this study show, in comparison with our previous results, that better selectivities are achieved. 20 refs., 3 figs., 2 tabs.

  13. PROPERTIES OF POLYMER SUPPORTED Ni-Cu BIMETALLIC CATALYSTS PREPARED BY SOLVATED METAL ATOM IMPREGNATION

    Institute of Scientific and Technical Information of China (English)

    WU Shihua; ZHU Changying; HUANG Wenqiang

    1996-01-01

    D-72 resin supported nickel-copper catalysts prepared by solvated metal atom impregnation (SMAI) were studied by magnetic measurements and X-ray photoelectron spectroscopy (XPS). The Ni particles on the catalysts are very highly dispersed and display superparamagnetic behaviour. Ni-Cu alloy clusters were found to be formed. The surface compositions are different from the bulk concentrations. In contrast with the surface enrichment in copper generally observed on conventional Ni-Cu catalysts, the surfaces of these catalysts are enriched in nickel. The nickel is in both zero and valent states, while copper is mainly in metallic state. Catalytic data show that the formation of Ni-Cu alloy clusters has a profound effect on the catalytic activities of the catalysts in the hydrogenation of furfural. The activity of the Ni:Cu ratio of one bimetallic catalysts is much higher than that of the Ni or Cu monometallic catalyst.

  14. High pressure CO hydrogenation over bimetallic Pt-Co catalysts

    DEFF Research Database (Denmark)

    Christensen, Jakob Munkholt; Medford, Andrew James; Studt, Felix;

    2014-01-01

    The potential of bimetallic Pt-Co catalysts for production of higher alcohols in high pressure CO hydrogenation has been assessed. Two catalysts (Pt3Co/SiO2 and PtCo/SiO2) were tested, and the existing literature on CO hydrogenation over Pt-Co catalysts was reviewed. It is found that the catalysts...... produce mainly methanol in the Pt-rich composition range andmainly hydrocarbons (and to a modest extent higher alcohols) in the Co-rich composition range. The transition between the two types of behavior occurs in a narrow composition range around a molar Pt:Co ratio of 1:1....

  15. Bimetallic Pt-Ni catalysts supported on usy zeolite for n-hexane isomerization

    Directory of Open Access Journals (Sweden)

    F. V. Barsi

    2009-06-01

    Full Text Available Isomerization of linear alkanes has had considerable importance for the refining industry because the isomers formed in this reaction have high octane number. Most works reported in the literature studied the use of bifunctional catalysts, i.e., ones that have acid sites and metallic sites. In this study, bifunctional monometallic (Ni or Pt and bimetallic catalysts (Pt-Ni, using HUSY zeolite as the support, were prepared in order to verify the role of the metal content and composition on the catalytic properties for n-hexane isomerization. The method used for metal dispersion in the zeolite was competitive ion exchange using ammine complexes [Ni(NH36]Cl2 and [Pt(NH34]Cl2 as precursors. Four series of catalysts with constant atomic metal content had total metal amounts between 130 and 280 µmol M/g cat. Catalysts were characterized by temperature programmed reduction (TPR and subjected to catalytic evaluation for n-hexane isomerization at 250 ºC and 1 atm using H2/C6 = 9 molar ratio. TPR results show an easier reducibility of Ni+2 cations in the presence of Pt, which was evidenced by the displacement of the reduction peak of those cations towards lower temperatures in bimetallic catalysts. The bimetallic catalysts presented a higher activity in the isomerization of n-hexane when compared to the monometallic ones, as well better stability as the Pt content in the solid increases. The results of the activity as a function of the Pt content in the bimetallic catalysts show a maximum value around 50% of Pt. An addition of Pt above this critical value leads to a small decrease of the catalytic activity.

  16. CO methanation over supported bimetallic Ni-Fe catalysts: From computational studies towards catalyst optimization

    DEFF Research Database (Denmark)

    Kustov, Arkadii; Frey, Anne Mette; Larsen, Kasper Emil;

    2007-01-01

    , we report a more detailed catalytic study aimed at optimizing the catalyst performance. For this purpose, two series of mono and bimetallic Ni-Fe catalysts supported on MgAl2O4 and Al2O3, respectively, were prepared. All catalysts were tested in the CO methanation reaction in the temperature interval...

  17. Bimetallic catalysts for upgrading of biomass to fuels and chemicals.

    Science.gov (United States)

    Alonso, David Martin; Wettstein, Stephanie G; Dumesic, James A

    2012-12-21

    Research interest in biomass conversion to fuels and chemicals has increased significantly in the last decade as the necessity for a renewable source of carbon has become more evident. Accordingly, many different reactions and processes to convert biomass into high-value products and fuels have been proposed in the literature. Special attention has been given to the conversion of lignocellulosic biomass, which does not compete with food sources and is widely available as a low cost feedstock. In this review, we start with a brief introduction on lignocellulose and the different chemical structures of its components: cellulose, hemicellulose, and lignin. These three components allow for the production of different chemicals after fractionation. After a brief overview of the main reactions involved in biomass conversion, we focus on those where bimetallic catalysts are playing an important role. Although the reactions are similar for cellulose and hemicellulose, which contain C(6) and C(5) sugars, respectively, different products are obtained, and therefore, they have been reviewed separately. The third major fraction of lignocellulose that we address is lignin, which has significant challenges to overcome, as its structure makes catalytic processing more challenging. Bimetallic catalysts offer the possibility of enabling lignocellulosic processing to become a larger part of the biofuels and renewable chemical industry. This review summarizes recent results published in the literature for biomass upgrading reactions using bimetallic catalysts. PMID:22872312

  18. Bimetallic Catalysts Containing Gold and Palladium for Environmentally Important Reactions

    Directory of Open Access Journals (Sweden)

    Ahmad Alshammari

    2016-07-01

    Full Text Available Supported bimetallic nanoparticles (SBN are extensively used as efficient redox catalysts. This kind of catalysis particularly using SBN has attracted immense research interest compared to their parent metals due to their unique physico-chemical properties. The primary objective of this contribution is to provide comprehensive overview about SBN and their application as promising catalysts. The present review contains four sections in total. Section 1 starts with a general introduction, recent progress, and brief summary of the application of SBN as promising catalysts for different applications. Section 2 reviews the preparation and characterization methods of SBN for a wide range of catalytic reactions. Section 3 concentrates on our own results related to the application of SBN in heterogeneous catalysis. In this section, the oxidation of cyclohexane to adipic acid (an eco-friendly and novel approach will be discussed. In addition, the application of bimetallic Pd catalysts for vapor phase toluene acetoxylation in a fixed bed reactor will also be highlighted. Acetoxylation of toluene to benzyl acetate is another green route to synthesize benzyl acetate in one step. Finally, Section 4 describes the summary of the main points and also presents an outlook on the application of SBN as promising catalysts for the production of valuable products.

  19. The selective hydrogenation of crotonaldehyde over bimetallic catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Schoeb, A.M.

    1997-02-01

    The selective hydrogenation of crotonaldehyde has been investigated over a monometallic Pt/SiO{sub 2} catalyst and platinum bimetallic catalysts where the second metal was either silver, copper, or tin. The effects of addition of a second metal to the Pt/SiO{sub 2} system on the selectivity to crotyl alcohol were investigated. The Pt-Sn bimetallic catalysts were characterized by hydrogen chemisorption, {sup 1}H NMR and microcalorimetry. The Pt-Ag/SiO{sub 2} and Pt-Cu/SiO{sub 2} catalysts were characterized by hydrogen chemisorption. Pt-Sn/SiO{sub 2} catalysts selectively hydrogenated crotonaldehyde to crotyl alcohol and the method of preparation of these catalysts affected the selectivity. The most selective Pt-Sn/SiO{sub 2} catalysts for the hydrogenation of crotonaldehyde to crotyl alcohol were those in which the Sn precursor was dissolved in a HCl solution. Sn increased both the rate of formation of butyraldehyde and the rate of formation of crotyl alcohol. The Pt/SiO{sub 2}, Pt-Ag/SiO{sub 2} and Pt-Cu/SiO{sub 2} catalysts produced only butyraldehyde. Initial heats of adsorption ({approximately}90 kJ/mol) measured using microcalorimetry were not affected by the presence of Sn on Pt. We can conclude that there is no through metal electronic interaction between Pt and Sn at least with respect to hydrogen surface bonds since the Pt and Pt-Sn at least with respect to hydrogen surface bonds since the Pt and Pt-Sn had similar initial heats of adsorption coupled with the invariance of the {sup 1}H NMR Knight shift.

  20. Exploration of Nanotube Structure Selectivity Using Bimetallic Catalysts

    Science.gov (United States)

    Pfefferle, Lisa

    2007-10-01

    Achieving selectivity for nanotube chirality is one of the holy grails for single-walled carbon nanotube research. One approach we are following is based on the ability to engineer the size and state of the initiating metal particle to constrain the type of cap formed. The chirality/structure of a nanotube is controlled by carbon cap formation on the metal particle during the nucleation step. It has been proposed that varying the carbon-metal catalyst binding energy could help lead to structure selectivity. One reason theoretically proposed for the favoring of armchair nanotubes, for example, is the proximity of low energy binding locations for two carbon atoms. Thus blocking sites or perturbing the binding energy on adjacent sites could in theory affect the structure of the carbon cap formed in the nucleation step. Our goal is to demonstrate structure selectivity in the growth of single wall carbon nanotubes (SWNT) using a bimetallic catalyst. The catalyst used was a bimetallic CoCr-MCM 41 and the effect of different molecular ratios between the two metals on the SWNT diameter distribution was studied. We have found that by adding Cr to the Co-MCM 41 monometallic catalyst the diameter distribution shifted in a systematic manner correlated to the development of a bimetallic phase as characterized by X-Ray absorption spectroscopy (XAS). We have also found that the shift is accompanied by suppression of metallic SWNT, particularly those with diameter over 0.9 nm. We are also currently exploring the possibility of a further narrowing of the distribution by lowering the reaction temperatures.

  1. High-performance PdRu bimetallic catalyst supported on mesoporous silica nanoparticles for phenol hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Chao [The Key Laboratory of Fuel Cell Technology of Guangdong Province and The Key Laboratory for New Energy of Guangdong Universities, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou (China); Yang, Xu [Key Laboratory of Renewable Energy, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou (China); Yang, Hui; Huang, Peiyan; Song, Huiyu [The Key Laboratory of Fuel Cell Technology of Guangdong Province and The Key Laboratory for New Energy of Guangdong Universities, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou (China); Liao, Shijun, E-mail: chsjliao@scut.edu.cn [The Key Laboratory of Fuel Cell Technology of Guangdong Province and The Key Laboratory for New Energy of Guangdong Universities, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou (China)

    2014-10-01

    Graphical abstract: The addition of Ru could significantly improve the performance of the mesoporous silica nanoparticles supported PdRu/MSN catalyst, which showed over 5 times higher mass activity than the mono-Pd/MSN towards the liquid-phase hydrogenation of phenol. The improved dispersion and the electronic interaction contributed to the enhanced catalytic activity for the catalyst towards phenol hydrogenation. - Highlights: • PdRu bimetal catalyst supported on mesoporous silica nanoparticles was prepared. • The average sizeof PdRu alloy is smaller than that of mono-Pd. • The addition of Ru to Pd modulates the electronic properties between Pd and Ru. • PdRu/MSN catalyst shows superior activity on phenol hydrogenation than Pd/MSN. • PdRu/MSN catalyst shows good selectivity for cyclohexanol to some extent. - Abstract: A high-performance PdRu bimetallic catalyst supported on mesoporous silica nanoparticles (MSN), PdRu/MSN, was prepared by a facile impregnation–hydrogen reduction method. It was found that PdRu/MSN showed 5 times higher activity than that of Pd/MSN towards the liquid-phase hydrogenation of phenol. The catalysts were characterized comprehensively by multiple techniques, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and hydrogen temperature program reduction (TPR). It was revealed that adding Ru could effectively improve the Pd dispersion and promote the electronic interaction between the Pd and Ru, both of which contribute to enhancing the catalytic activity.

  2. Nanocrystalline MgO supported nickel-based bimetallic catalysts for carbon dioxide reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Meshkani, Fereshteh [Catalyst and Advanced Materials Research Laboratory, Chemical Engineering Department, Faculty of Engineering, University of Kashan, Kashan (Iran); Rezaei, Mehran [Catalyst and Advanced Materials Research Laboratory, Chemical Engineering Department, Faculty of Engineering, University of Kashan, Kashan (Iran); Institute of Nanoscience and Nanotechnology, University of Kashan, Kashan (Iran)

    2010-10-15

    Nanocrystalline magnesium oxide with high surface area and plate-like shape was employed as catalyst support for preparation of nickel-based bimetallic catalysts in methane reforming with carbon dioxide. The prepared samples were characterized by X-ray diffraction (XRD), N{sub 2} adsorption (BET), Temperature programmed oxidation and desorption (TPO-TPD), Thermal gravimetric and differential thermal gravimetric (TGA-DTG), H{sub 2} chemisorption and Transmission and electron microscopies (TEM and SEM) analyses. CO{sub 2}-TPD data showed the high CO{sub 2} adsorption capacity of catalysts which improves the resistance of catalysts against the carbon formation. The H{sub 2} chemisorption results also indicated that the addition of Pt to nickel catalyst improved the nickel dispersion. The obtained results revealed that the prepared catalysts showed a high activity and stability during the reaction with a low amount of deposited carbon. Addition of Pt to nickel catalyst improved both the activity and resistivity against carbon formation. (author)

  3. High-performance PdRu bimetallic catalyst supported on mesoporous silica nanoparticles for phenol hydrogenation

    Science.gov (United States)

    Huang, Chao; Yang, Xu; Yang, Hui; Huang, Peiyan; Song, Huiyu; Liao, Shijun

    2014-10-01

    A high-performance PdRu bimetallic catalyst supported on mesoporous silica nanoparticles (MSN), PdRu/MSN, was prepared by a facile impregnation-hydrogen reduction method. It was found that PdRu/MSN showed 5 times higher activity than that of Pd/MSN towards the liquid-phase hydrogenation of phenol. The catalysts were characterized comprehensively by multiple techniques, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and hydrogen temperature program reduction (TPR). It was revealed that adding Ru could effectively improve the Pd dispersion and promote the electronic interaction between the Pd and Ru, both of which contribute to enhancing the catalytic activity.

  4. thesis of high-purity carbon nanotubes over alumina and silica supported bimetallic catalysts

    Directory of Open Access Journals (Sweden)

    Sanja Ratković

    2009-10-01

    Full Text Available Carbon nanotubes (CNTs were synthesized by a catalytic chemical vapor deposition method (CCVD of ethylene over alumina and silica supported bimetallic catalysts based on Fe, Co and Ni. The catalysts were prepared by a precipitation method, calcined at 600 °C and in situ reduced in hydrogen flow at 700 °C. The CNTs growth was carried out by a flow the mixture of C2H4 and nitrogen over the catalyst powder in a horizontal oven. The structure and morphology of as-synthesized CNTs were characterized using SEM. The as-synthesized nanotubes were purified by acid and basic treatments in order to remove impurities such as amorphous carbon, graphite nanoparticles and metal catalysts. XRD and DTA/TG analyses showed that the amounts of by-products in the purified CNTs samples were reduced significantly. According to the observed results, ethylene is an active carbon source for growing high-density CNTs with high yield but more on alumina-supported catalysts than on their silica- supported counterparts. The last might be explained by SMSI formed in the case of alumina-supported catalysts, resulting in higher active phase dispersion.

  5. Enantioselective Epoxide Polymerization Using a Bimetallic Cobalt Catalyst

    KAUST Repository

    Thomas, Renee M.

    2010-11-24

    A highly active enantiopure bimetallic cobalt complex was explored for the enantioselective polymerization of a variety of monosubstituted epoxides. The polymerizations were optimized for high rates and stereoselectivity, with s-factors (kfast/kslow) for most epoxides exceeding 50 and some exceeding 300, well above the threshold for preparative utility of enantiopure epoxides and isotactic polyethers. Values for mm triads of the resulting polymers are typically greater than 95%, with some even surpassing 98%. In addition, the use of a racemic catalyst allowed the preparation of isotactic polyethers in quantitative yields. The thermal properties of these isotactic polyethers are presented, with many polymers exhibiting high T m values. This is the first report of the rapid synthesis of a broad range of highly isotactic polyethers via the enantioselective polymerization of racemic epoxides. © 2010 American Chemical Society.

  6. Bimetallic Au-decorated Pd catalyst for the liquid phase hydrodechlorination of 2,4-dichlorophenol

    Science.gov (United States)

    Zhou, Juan; Chen, Huan; Chen, Quanyuan; Huang, Zhaolu

    2016-11-01

    Monometallic and bimetallic Pd-Au catalysts supported on multi-walled carbon nanotubes (CNTs) with varied Au cooperation amounts were prepared using the complexing-reduction method in the presence of tetrahydrofuran (THF). The liquid phase catalytic hydrodechlorination (HDC) of 2,4-dichlorophenol (2,4-DCP) was investigated over these bimetallic catalysts. The catalysts were characterized by N2 adsorption-desorption isotherms, X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and H2 chemisorption. Characterization results showed that the co-reduction of Pd and Au mainly formed alloy-like structure. The bimetallic catalysts had smaller metal particles and larger numbers of exposed active site than that of monometallic catalysts. In addition, compared with Pd(1.7)/CNTs and Au(0.4)/CNTs, the binding energies of Pd 3d5/2 shifted to higher positions while that of Au 4f7/2 had negative shifts in the Pd-Au bimetallic catalysts, which can be ascribed to the electrons transferred from metal Pd to Au and the cationization of Pd particles was enhanced. Accordingly, the bimetallic Pd-Au particles with different Au contents in the catalysts exhibited varied synergistic effects for the catalytic HDC of 2,4-DCP, with Pd(1.8)Au(0.4)/CNTs having the highest catalytic activity. For the bimetallic catalysts, a disproportional increase of turnover frequency (TOF) was observed with increasing Au content due to the enhanced cationization of Pd particles. Moreover, the dechlorination of 2,4-DCP over the supported monometallic and bimetallic catalysts proceeded via both the stepwise and concerted pathway, and the concerted pathway became predominant with Au decoration amount in the catalyst.

  7. An in-depth understanding of the bimetallic effects and coked carbon species on an active bimetallic Ni(Co)/Al2O3 dry reforming catalyst.

    Science.gov (United States)

    Liao, Xin; Gerdts, Rihards; Parker, Stewart F; Chi, Lina; Zhao, Yongxiang; Hill, Martyn; Guo, Junqiu; Jones, Martin O; Jiang, Zheng

    2016-06-29

    Ni/Al2O3, Co/Al2O3 and bimetallic Ni(Co)/Al2O3 catalysts were prepared using an impregnation method and employed in CO2 dry reforming of methane under coking-favored conditions. The spent catalysts were carefully characterized using typical characterization technologies and inelastic neutron scattering spectroscopy. The bimetallic catalyst exhibited a superior activity and anti-coking performance compared to Ni/Al2O3, while the most resistant to coking behavior was Co/Al2O3. The enhanced activity of the Ni(Co)/Al2O3 bimetallic catalyst is attributed to the reduced particle size of metallic species and resistance to forming stable filamentous carbon. The overall carbon deposition on the spent bimetallic catalyst is comparable to that of the spent Ni/Al2O3 catalyst, whereas the carbon deposited on the bimetallic catalyst is mainly less-stable carbonaceous species as confirmed by SEM, TPO, Raman and INS characterization. This study provides an in depth understanding of alloy effects in catalysts, the chemical nature of coked carbon on spent Ni-based catalysts and, hopefully, inspires the creative design of a new bimetallic catalyst for dry reforming reactions.

  8. Performance enhancement of bimetallic Co-Ru/CNTs nano catalysts using microemulsion technique

    Institute of Scientific and Technical Information of China (English)

    Ahmad; Tavasoli; Somayeh; Taghavi

    2013-01-01

    Bimetallic cobalt-ruthenium nano catalysts supported on carbon nanotubes(CNTs)are prepared using microemultion technique with water-to-surfactant ratios of 0.5—1.5.The nano catalysts were extensively characterized by different methods and their activity and selectivity in Fischer-Tropsch synthesis(FTS)have been assessed in a fixed-bed microreactor.The physicochemical properties and performance of the nanocatalysts were compared with the catalyst prepared by impregnation method.Very narrow particle size distribution has been produced by the microemulsion technique at relatively high loadings of active metals(15 wt%Co and 1 wt%Ru).According to TEM images,small Co particles(2—7 nm)were mostly confined inside the CNTs.Comparing with the catalyst prepared by impregnation,the use of microemulsion technique with water to surfactant ratio of 0.5 decreased the average cobalt oxide particle size to 4.8 nm,the dispersion was almost doubled and the reduction increased by 28%.Activity and selectivity were found to be dependent on the catalyst preparation method and water-to-surfactant ratio(as well as cobalt particle sizes).CO conversion increased from 59.1%to 75.1%and the FTS rate increased from 0.291 to0.372 gHC/(gcath).C5+liquid hydrocarbons selectivity decreased from 92.4%to 87.6%.

  9. Enhancement of bimetallic Fe-Mn/CNTs nano catalyst activity and product selectivity using microemulsion technique

    Institute of Scientific and Technical Information of China (English)

    Zahra; Zolfaghari; Ahmad; Tavasoli; Saber; Tabyar; Ali; Nakhaei; Pour

    2014-01-01

    Bimetallic Fe-Mn nano catalysts supported on carbon nanotubes(CNTs) were prepared using microemulsion technique with water-to-surfactant ratios of 0.4-1.6. The nano catalysts were extensively characterized by different methods and their activity and selectivity in Fischer-Tropsch synthesis(FTS) have been assessed in a fixed-bed microreactor. The physicochemical properties and performance of the nanocatalysts were compared with the catalyst prepared by impregnation method. Very narrow particle size distribution has been produced by the microemulsion technique at relatively high loading of active metal. TEM images showed that small metal nano particles in the range of 3–7 nm were not only confined inside the CNTs but also located on the outer surface of the CNTs. Using microemulsion technique with water to surfactant ratio of0.4 decreased the average iron particle sizes to 5.1 nm. The reduction percentage and dispersion percentage were almost doubled. Activity and selectivity were found to be dependent on the catalyst preparation method and average iron particle size. CO conversion and FTS rate increased from 49.1% to 71.0% and 0.144 to 0.289 gHC/(gcat h), respectively. While the WGS rate decreased from 0.097 to 0.056 gCO2/(gcat h). C5+liquid hydrocarbons selectivity decreased slightly and olefins selectivity almost doubled.

  10. Non-Precious Bimetallic Catalysts for Selective Dehydrogenation of an Organic Chemical Hydride System

    KAUST Repository

    Shaikh Ali, Anaam

    2015-07-06

    Methylcyclohexane (MCH)-Toluene (TOL) chemical hydride cycles as a hydrogen carrier system is successful with the selective dehydrogenation reaction of MCH to TOL, which has been achieved only using precious Pt-based catalysts. Herein, we report improved selectivity using non-precious metal nickel-based bimetallic catalysts, where the second metal occupies the unselective step sites.

  11. Bimetallic Catalysts and Platinum Surfaces Studied by X-ray Absorption Spectroscopy and Scanning Tunnelling Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Roenning, Magnus

    2000-07-01

    Bimetallic catalyst systems used in Fischer-Tropsch synthesis (Co-Re/Al{sub 2}O{sub 3}) and in the naphtha reforming process (Pt-Re/Al{sub 2}O{sub 3}) have been studied in situ using X-ray absorption spectroscopy (EXAFS). Additionally, the adsorption of ethene on platinum single crystal surfaces has been investigated using scanning tunnelling microscopy. In situ EXAFS at the cobalt K absorption edge have been carried out at 450{sup o}C on the hydrogen reduction of a rhenium-promoted Co{sub 3}O{sub 4}/Al{sub 2}O{sub 3} catalyst. Reductions carried out using 100% hydrogen and 5% hydrogen in helium gave different results. Whereas the reduction using dilute hydrogen leads to bulk-like metallic cobalt particles (hcp or fcc), reaction with pure hydrogen yields a more dispersed system with smaller cobalt metal particles (< 40 A). The results are rationalised in terms of different degrees of reoxidation of cobalt by the higher and lower concentrations of water generated during the reduction of cobalt oxide by 100% and 5% hydrogen, respectively. Additionally, in both reduction protocols a small fraction (3 -4 wt%) of the cobalt content is randomly dispersed over the tetrahedral vacancies of the alumina support. This dispersion occurs during reduction and not calcination. The cobalt in these sites cannot be reduced at 450 {sup o}C. The local environments about the rhenium atoms in Co-Re/{gamma}-A1{sub 2}O{sub 3} catalyst after different reduction periods have been studied by X-ray absorption spectroscopy. A bimetallic catalyst containing 4.6 wt% cobalt and 2 wt% rhenium has been compared with a corresponding monometallic sample with 2 wt% rhenium on the same support. The rhenium L{sub III} EXAFS analysis shows that bimetallic particles are formed after reduction at 450{sup o}C with the average particle size being 10-15 A. Rhenium is shown to be reduced at a later stage than cobalt. The fraction of cobalt atoms entering the support obstructs the access to the support for the

  12. Bimetallic Catalysts and Platinum Surfaces Studied by X-ray Absorption Spectroscopy and Scanning Tunnelling Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Roenning, Magnus

    2000-07-01

    Bimetallic catalyst systems used in Fischer-Tropsch synthesis (Co-Re/Al{sub 2}O{sub 3}) and in the naphtha reforming process (Pt-Re/Al{sub 2}O{sub 3}) have been studied in situ using X-ray absorption spectroscopy (EXAFS). Additionally, the adsorption of ethene on platinum single crystal surfaces has been investigated using scanning tunnelling microscopy. In situ EXAFS at the cobalt K absorption edge have been carried out at 450{sup o}C on the hydrogen reduction of a rhenium-promoted Co{sub 3}O{sub 4}/Al{sub 2}O{sub 3} catalyst. Reductions carried out using 100% hydrogen and 5% hydrogen in helium gave different results. Whereas the reduction using dilute hydrogen leads to bulk-like metallic cobalt particles (hcp or fcc), reaction with pure hydrogen yields a more dispersed system with smaller cobalt metal particles (< 40 A). The results are rationalised in terms of different degrees of reoxidation of cobalt by the higher and lower concentrations of water generated during the reduction of cobalt oxide by 100% and 5% hydrogen, respectively. Additionally, in both reduction protocols a small fraction (3 -4 wt%) of the cobalt content is randomly dispersed over the tetrahedral vacancies of the alumina support. This dispersion occurs during reduction and not calcination. The cobalt in these sites cannot be reduced at 450 {sup o}C. The local environments about the rhenium atoms in Co-Re/{gamma}-A1{sub 2}O{sub 3} catalyst after different reduction periods have been studied by X-ray absorption spectroscopy. A bimetallic catalyst containing 4.6 wt% cobalt and 2 wt% rhenium has been compared with a corresponding monometallic sample with 2 wt% rhenium on the same support. The rhenium L{sub III} EXAFS analysis shows that bimetallic particles are formed after reduction at 450{sup o}C with the average particle size being 10-15 A. Rhenium is shown to be reduced at a later stage than cobalt. The fraction of cobalt atoms entering the support obstructs the access to the support for the

  13. Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

    KAUST Repository

    Biausque, Gregory

    2015-04-28

    Methods to synthesize NiPt bimetallic nanoparticles by a reversed-phase microemulsion, deposition of NiPt bimetallic nanoparticles on a support, and application of the supported catalyst for CO.sub.2 reforming of methane

  14. Synergistic Effects in Bimetallic Palladium-Copper Catalysts Improve Selectivity in Oxygenate Coupling Reactions.

    Science.gov (United States)

    Goulas, Konstantinos A; Sreekumar, Sanil; Song, Yuying; Kharidehal, Purnima; Gunbas, Gorkem; Dietrich, Paul J; Johnson, Gregory R; Wang, Y C; Grippo, Adam M; Grabow, Lars C; Gokhale, Amit A; Toste, F Dean

    2016-06-01

    Condensation reactions such as Guerbet and aldol are important since they allow for C-C bond formation and give higher molecular weight oxygenates. An initial study identified Pd-supported on hydrotalcite as an active catalyst for the transformation, although this catalyst showed extensive undesirable decarbonylation. A catalyst containing Pd and Cu in a 3:1 ratio dramatically decreased decarbonylation, while preserving the high catalytic rates seen with Pd-based catalysts. A combination of XRD, EXAFS, TEM, and CO chemisorption and TPD revealed the formation of CuPd bimetallic nanoparticles with a Cu-enriched surface. Finally, density functional theory studies suggest that the surface segregation of Cu atoms in the bimetallic alloy catalyst produces Cu sites with increased reactivity, while the Pd sites responsible for unselective decarbonylation pathways are selectively poisoned by CO. PMID:27195582

  15. Levulinic acid hydrogenolysis on Al2O3-based Ni-Cu bimetallic catalysts

    Institute of Scientific and Technical Information of China (English)

    Iker Obregón; Eriz Corro; Urko Izquierdo; Jesus Requies; Pedro L. Arias

    2014-01-01

    Inexpensive γ-alumina-based nickel-copper bimetallic catalysts were studied for the hydrogenolysis of levulinic acid, a key platform molecule for biomass conversion to biofuels and other valued chemicals, into γ-valerolactone as a first step towards the production of 2-methyltetrahydrofurane. The activities of both monometallic and bimetallic catalysts were tested. Their textural and chemical characteristics were determined by nitrogen physisorption, elemental analysis, temperature-pro-grammed ammonia desorption, and temperature-programmed reduction. The monometallic nickel catalyst showed high activity but the highest by-product production and significant amounts of carbon deposited on the catalyst surface. The copper monometallic catalyst showed the lowest activity but the lowest carbon deposition. The incorporation of the two metals generated a bimetal-lic catalyst that displayed a similar activity to that of the Ni monometallic catalyst and significantly low by-product and carbon contents, indicating the occurrence of important synergetic effects. The influence of the preparation method was also examined by studying impregnated- and sol-gel-derived bimetallic catalysts. A strong dependency on the preparation procedure and calcina-tion temperature was observed. The highest activity per metal atom was achieved using the sol-gel-derived catalyst that was calcined at 450 °C. High reaction rates were achieved;the total levulinic acid conversion was obtained in less than 2 h of reaction time, yielding up to 96%γ-valerolactone, at operating temperature and pressure of 250 °C and 6.5 MPa hydrogen, respec-tively.

  16. Synergy between metals in bimetallic zeolite supported catalyst for NO-promoted N2O decomposition

    NARCIS (Netherlands)

    Pieterse, J.A.Z.; Mul, G.; Melian-Cabrera, I.; van den Brink, R.W.

    2005-01-01

    The detrimental effect of NO on N2O decomposition over zeolite supported noble metal catalysts can be (partly) eliminated by combining noble metal with iron or cobalt. In the presence of NO, the total conversion of N2O over these bimetallic-zeolites exceeds the sum of conversions over the monometall

  17. Nanosegregated bimetallic oxide anode catalyst for proton exchange membrane electrolyzer

    Energy Technology Data Exchange (ETDEWEB)

    Danilovic, Nemanja; Kang, Yijin; Markovic, Nenad; Stamenkovic, Vojislav; Myers, Deborah J.; Subbaraman, Ram

    2016-08-23

    A surface segregated bimetallic composition of the formula Ru.sub.1-xIr.sub.x wherein 0.1.ltoreq.x.ltoreq.0.75, wherein a surface of the material has an Ir concentration that is greater than an Ir concentration of the material as a whole is provided. The surface segregated material may be produced by a method including heating a bimetallic composition of the formula Ru.sub.1-xIr.sub.x, wherein 0.1.ltoreq.x.ltoreq.0.75, at a first temperature in a reducing environment, and heating the composition at a second temperature in an oxidizing environment. The surface segregated material may be utilized in electrochemical devices.

  18. Kinetics of oxygen-enhanced water gas shift on bimetallic catalysts and the roles of metals and support

    Science.gov (United States)

    Kugai, Junichiro

    dissociation and/or the subsequent reaction with chemisorbed CO as well as Pd keeps Cu in reduced state. Cu was found to keep Pd dispersed, suppress H2 activation on Pd, and facilitate CO 2 desorption from catalyst surface. While composition and structure of metal have large impacts on OWGS performance, CeO2 was shown to create new sites for H2O activation at metal-ceria interfacial region in concert with metal. These new sites strongly activate H2O to drive OWGS and WGS compared to the pure metallic sites which are present in majority on Al2O3-supported catalyst. The observed two regimes of turnover rate, the one dependent on catalyst surface area and the other independent of surface area, strongly suggested bifunctional reaction pathway where the reaction rate is determined by activation of H2O and by association of chemisorbed CO and H 2O. The associative route was also evidenced by pulse response study where the reaction occurs only when CO and H2O pulses are supplied together, and thus pre-adsorbed species such as formate and carbonate identified by FT-IR are proven to be spectators. No correlation between WGS rate and isotopic exchange rate of molecularly adsorbed D2O with H 2 showed H2O dissociation is necessary for WGS to occur. Long duration tests revealed CeO2-supported Pd-Cu, Pt-Cu and Cu catalysts are stable in OWGS condition compared to Pt, Pd, and Al 2O3-supported Pd-Cu catalysts which exhibited continuous deactivation during about 70 hours of test. The addition of Cu prevents agglomeration of monometallic Pd and carbonate formation on monometallic Pt during the reaction. The better activity and stability of Pd-Cu and Pt-Cu bimetallic catalysts in the realistic OWGS condition were ascribed to the unique active sites consisting of highly dispersed Pd in Cu or Pt in Cu on CeO2, which are good for H2O activation with low reaction inhibition by the product gases. Pt monometallic catalyst showed and highest activity in OWGS in the absence of product gases, but this

  19. STUDY ON POLYMER- Ru- Co BIMETALLIC COMPLEXES CATALYSTS Ⅱ. X-RAY PHOTOELECTRON SPECTROSCOPIC ANALYSIS

    Institute of Scientific and Technical Information of China (English)

    ZONG Huijuan; TANG Qi; CHEN Zonghan; JIANG Yingyan

    1991-01-01

    Polymer-Ru-Co bimetallic complexes have been examined by X-ray photoelectron spectroscopy.The catalyst is highly active only when the mole ratio of Co/Ru is 4:3. The activity of catalysts does not depend on the total Co/Ru ratio, but on the surface stoichiometry of Co and Ru. When the relative intensities of Co2p and Ru3d of XP S peaks are close to each other and both are high, the catalyst exhibits its maximum activity.The mechanism of catalytic hydroformylation has been discussed.

  20. SULFUR-RESISTANT BIMETALLIC NOBLE METAL CATALYSTS FOR AROMATIC HYDROGENATION OF DIESEL FUEL

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Y zeolite supporting noble metal catalysts, as the important industrial catalysts for aromatics hydrogenation, have received increasing attention in recent years. Pd-M/Y bimetallic catalysts, where M is non-noble metal element, were prepared to investigate the effects of the addition of a second metal. Pd-M/Y catalysts were evaluated under the following conditions: H2 pressure 4.2 MPa, MHSV 4.0 h-1, sulfur content in feed 3000 μg/g. The microreactor results indicated that the second metal remarkably affects the hydrogenation activity of Pd/Y catalysts. Among them, Cr and W improve the sulfur resistance of Pd/Y, but La, Mn, Mo and Ag make the sulfur resistance worse and the second metals have no evident influence on product selectivity and acidic properties of the catalysts.

  1. Selective hydrogenation of citral over Au-based bimetallic catalysts in supercritical carbon dioxide

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    Selective hydrogenation of citral was investigated over Au-based bimetallic catalysts in the environmentally benign supercritical carbon dioxide (scCO2) medium.The catalytic performances were different in citral hydrogenation when Pd or Ru was mixed (physically and chemically) with Au.Compared with the corresponding monometallic catalyst,the total conversion and the selectivity to citronellal (CAL) were significantly enhanced over TiO2 supported Pd and Au bimetallic catalysts (physically and chemically mixed);however,the conversion and selectivity did not change when Ru was physically mixed with Au catalyst compared to the monometallic Ru/TiO2,and the chemically mixed Ru-Au/TiO2 catalyst did not show any activity.The effect of CO2 pressure on the conversion of citral and product selectivity was significantly different over the Au/TiO2,Pd-Au/TiO2,and Pd/TiO2 catalysts.It was assumed to be ascribed to the difference in the interactions between Au,Pd nanoparticles and CO2 under different CO2 pressures.

  2. Bimetallic Palladium Catalysts for Methane Combustion in Gas Turbines

    OpenAIRE

    Persson, Katarina

    2006-01-01

    Catalytic combustion is a promising combustion technology for gas turbines, which results in ultra low emission levels of nitrogen oxides (NOx), carbon monoxide (CO) and unburned hydrocarbons (UHC). Due to the low temperature achieved in catalytic combustion almost no thermal NOx is formed. This thesis is concentrated on the first stage in a catalytic combustion chamber, i.e. the ignition catalyst. The catalyst used for this application is often a supported palladium based catalyst due to its...

  3. Exceptional methanol electro-oxidation activity by bimetallic concave and dendritic Pt-Cu nanocrystals catalysts

    Science.gov (United States)

    Wang, Ying-Xia; Zhou, Hui-Jing; Sun, Ping-Chuan; Chen, Tie-Hong

    2014-01-01

    PtCux (x = 1, 2 and 3) bimetallic nanocrystals with concave surface and dendritic morphology were prepared and used as electrocatalysts in methanol oxidation reaction (MOR) for polymer electrolyte membrane fuel cells. The bimetallic nanocrystals were synthesized via one-pot co-reduction of H2PtCl6 and Cu(acac)2 by oleylamine and polyvinyl pyrrolidone (PVP) in an autoclave at 180 °C. The concave dendritic bimetallic nanostructure consisted of a core rich in Cu and nanodendrites rich in Pt, which was formed via galvanic replacement of Cu by Pt. It was found that PVP played an important role in initiating, facilitating, and directing the replacement reaction. The electrochemical properties of the PtCux were characterized by cyclic voltammetry (CV) and chronoamperometry (CA). The concave dendritic PtCu2/C nanocrystals exhibited exceptionally high activity and strong poisoning resistance in MOR. At 0.75 V (vs. reversible hydrogen electrode, RHE) the mass activity and specific activity of PtCu2/C were 3.3 and 4.1 times higher than those of the commercial Pt/C catalysts, respectively. The enhanced catalytic activity could be attributed to the unique concave dendritic morphology of the bimetallic nanocrystals.

  4. Enantioselective polymerization of epoxides using biaryl-linked bimetallic cobalt catalysts: A mechanistic study

    KAUST Repository

    Ahmed, Syud M.

    2013-12-18

    The enantioselective polymerization of propylene oxide (PO) using biaryl-linked bimetallic salen Co catalysts was investigated experimentally and theoretically. Five key aspects of this catalytic system were examined: (1) the structural features of the catalyst, (2) the regio- and stereoselectivity of the chain-growth step, (3) the probable oxidation and electronic state of Co during the polymerization, (4) the role of the cocatalyst, and (5) the mechanism of monomer enchainment. Several important insights were revealed. First, density functional theory (DFT) calculations provided detailed structural information regarding the regio- and stereoselective chain-growth step. Specifically, the absolute stereochemistry of the binaphthol linker determines the enantiomer preference in the polymerization, and the interaction between the salen ligand and the growing polymer chain is a fundamental aspect of enantioselectivity. Second, a new bimetallic catalyst with a conformationally flexible biphenol linker was synthesized and found to enantioselectively polymerize PO, though with lower enantioselectivity than the binaphthol linked catalysts. Third, DFT calculations revealed that the active form of the catalyst has two active exo anionic ligands (chloride or carboxylate) and an endo polymer alkoxide which can ring-open an adjacent cobalt-coordinated epoxide. Fourth, calculations showed that initiation is favored by an endo chloride ligand, while propagation is favored by the presence of two exo carboxylate ligands. © 2013 American Chemical Society.

  5. STUDY ON POLYMER-Ru-Co-BIMETALLIC COMPLEXES CATALYSTS I. SYNTHESIS OF CATALYSTS AND THEIR USE FOR THE HYDROFORMYLATION

    Institute of Scientific and Technical Information of China (English)

    TANG Qi; ZONG Huijuan; CHEN Zonghan; JIANG Yingyan

    1991-01-01

    Six kinds of polymer ligands, supported on SiO2, containing coordinating atoms P, S and N respectively, have been synthesized. The Ru(Ⅲ)-Co(Ⅱ) bimetallic complexes of these polymer ligands have been obtained and examined as catalysts for the hydroformylation of cyclohexene. The effects of reaction temperature, pressure and Co/Ru ratio etc. on the activities of catalysts were investigated in detail. The catalysts are all polymer-noncarbonyl-metal complexes, easily to be prepared, active and stable. From the experimental results it can be suggested that under reaction conditions such polymer-noncarbonyl-metal complexes convert "in situ" to polymer-carbonyl-metal complexes, thus become active catalysts. The course of this conversion is supposed as a preliminary approach.

  6. Effects of bimetallic catalysts on synthesis of nitrogen-doped carbon nanotubes as nanoscale energetic materials

    Institute of Scientific and Technical Information of China (English)

    Hao Liu; Yong Zhang; Ruying Li; Xueliang Sun; Hakima Abou-Rachid

    2011-01-01

    Well aligned nitrogen-doped carbon nanotubes (CNx-NTs),as energetic materials,are synthesized on a silicon substrate by aerosol-assisted chemical vapor deposition.Tungsten (W) and molybdenum (Mo) metals are respectively introduced to combine with iron (Fe) to act as a bimetallic co-catalyst layer.Correlations between the composition and shape of the co-catalyst and morphology,size,growth rate and nitrogen doping amount of the synthesized CNx-NTs are investigated by secondary and backscattered electron imaging in a field emission scanning electron microscope (FESEM) and X-ray photoelectron spectrometer (XPS).Compared to pure iron catalyst.W-Fe co-catalyst can result in lower growth rate,larger diameter and wider size distribution of the CNx-NTs; while incorporation of molybdenum into the iron catalyst layer can reduce the diameter and size distribution of the nanotubes.Compared to the sole iron catalyst,Fe-W catalyst impedes nitrogen doping while Fe-Mo catalyst promotes the incorporation of nitrogen into the nanotubes.The present work indicates that CNx-NTs with modulated size,growth rate and nitrogen doping concentration are expected to be synthesized by tuning the size and composition of co-catalysts,which may find great potential in producing CNx-NTs with controlled structure and properties.

  7. Reverse Micelle Synthesis and Characterization of Supported Pt/Ni Bimetallic Catalysts on gamma-Al2O3

    Energy Technology Data Exchange (ETDEWEB)

    B Cheney; J Lauterbach; J Chen

    2011-12-31

    Reverse micelle synthesis was used to improve the nanoparticle size uniformity of bimetallic Pt/Ni nanoparticles supported on {gamma}-Al{sub 2}O{sub 3}. Two impregnation methods were investigated to optimize the use of the micelle method: (1) step-impregnation, where Ni nanoparticles were chemically reduced in microemulsion and then supported, followed by Pt deposition using incipient wetness impregnation, and (2) co-impregnation, where Ni and Pt were chemically reduced simultaneously in microemulsion and then supported. Transmission electron microscopy (TEM) was used to characterize the particle size distribution. Atomic absorption spectroscopy (AAS) was used to perform elemental analysis of bimetallic catalysts. Extended X-ray absorption fine structure (EXAFS) measurements were utilized to confirm the formation of the Pt-Ni bimetallic bond in the step-impregnated catalyst. CO pulse chemisorption and Fourier transform infrared spectroscopy (FTIR) studies of 1,3-butadiene hydrogenation in a batch reactor were performed to determine the catalytic activity. Step-impregnated Pt/Ni catalyst demonstrated enhanced hydrogenation activity over the parent monometallic Pt and Ni catalysts due to bimetallic bond formation. The catalyst synthesized using co-impregnation showed no enhanced activity, behaving similarly to monometallic Ni. Overall, our results indicate that reverse micelle synthesis combined with incipient wetness impregnation produced small, uniform nanoparticles with bimetallic bonds that enhanced hydrogenation activity.

  8. Strategies for designing supported gold-palladium bimetallic catalysts for the direct synthesis of hydrogen peroxide.

    Science.gov (United States)

    Edwards, Jennifer K; Freakley, Simon J; Carley, Albert F; Kiely, Christopher J; Hutchings, Graham J

    2014-03-18

    Hydrogen peroxide is a widely used chemical but is not very efficient to make in smaller than industrial scale. It is an important commodity chemical used for bleaching, disinfection, and chemical manufacture. At present, manufacturers use an indirect process in which anthraquinones are sequentially hydrogenated and oxidized in a manner that hydrogen and oxygen are never mixed. However, this process is only economic at a very large scale producing a concentrated product. For many years, the identification of a direct process has been a research goal because it could operate at the point of need, producing hydrogen peroxide at the required concentration for its applications. Research on this topic has been ongoing for about 100 years. Until the last 10 years, catalyst design was solely directed at using supported palladium nanoparticles. These catalysts require the use of bromide and acid to arrest peroxide decomposition, since palladium is a very active catalyst for hydrogen peroxide hydrogenation. Recently, chemists have shown that supported gold nanoparticles are active when gold is alloyed with palladium because this leads to a significant synergistic enhancement in activity and importantly selectivity. Crucially, bimetallic gold-based catalysts do not require the addition of bromide and acids, but with carbon dioxide as a diluent its solubility in the reaction media acts as an in situ acid promoter, which represents a greener approach for peroxide synthesis. The gold catalysts can operate under intrinsically safe conditions using dilute hydrogen and oxygen, yet these catalysts are so active that they can generate peroxide at commercially significant rates. The major problem associated with the direct synthesis of hydrogen peroxide concerns the selectivity of hydrogen usage, since in the indirect process this factor has been finely tuned over decades of operation. In this Account, we discuss how the gold-palladium bimetallic catalysts have active sites for the

  9. CuAu–ZnO–graphene nanocomposite: A novel graphene-based bimetallic alloy-semiconductor catalyst with its enhanced photocatalytic degradation performance

    Energy Technology Data Exchange (ETDEWEB)

    Xie, Hong [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Ye, Xiaoliang [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China); Duan, Kaiyue; Xue, Muyin; Du, Yongling; Ye, Weichun [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China); Wang, Chunming, E-mail: wangcm@lzu.edu.cn [College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000 (China)

    2015-07-05

    Graphical abstract: In this work, we have successfully synthesized a novel graphene-based bimetallic alloy-semiconductor catalyst: CuAu–ZnO–Gr nanocomposite, and which behaved an enhanced photocatalytic activity. - Highlights: • A bimetallic alloy-based catalyst: CuAu–ZnO–Gr is synthesized. • CuAu–ZnO–Gr behaves an enhanced photocatalytic activity. • The detailed explanation of photocatalytic mechanism of CuAu–ZnO–Gr. - Abstract: The bimetallic alloy CuAu nanoparticles (NPs) can produce more photogenerated electrons when compared with single metal Au NPs. Moreover, graphene (Gr) sheets can help the charge separation and slow down the recombination of the electron hole pairs of ZnO. Hence, a novel graphene-based bimetallic alloy-semiconductor catalyst: CuAu–ZnO–Gr nanocomposite is synthesized. Due to the synergistic effect among CuAu NPs, ZnO nanopyramids, and Gr sheets, CuAu–ZnO–Gr behaves an enhanced photocatalytic activity for the photocatalytic degradation of synthetic colorants methyl orange (MO), methylene blue (MB), indigotin (IN), sunset yellow (SY), and tartrazine (TT) under the simulated sunlight irradiation. Furthermore, the apparent rate constants (k{sub app}) of MO, MB, IN, SY, and TT degradation are estimated respectively. In addition, the as-prepared CuAu–ZnO–Gr nanocomposite is characterized by X-ray diffraction, UV–vis spectrum, transmission electron microscopy, energy dispersive X-ray analysis (EDX), and EDX mapping. As a result of the facile synthesis route and the enhanced photocatalytic activity, this new material CuAu–ZnO–Gr can be a promising photocatalyst for the degradation of dyes.

  10. Catalytic performance of dealuminated H-Y zeolite supported bimetallic nano catalysts in Hydroizomerization of n-hexane and n-heptane

    International Nuclear Information System (INIS)

    A series of dealuminated Y-zeolites impregnated by 0.5 wt % Pt catalysts promoted by different amounts of Ni, Pd or Cr (0.3 and 0.6 wt %) were prepared and characterized as hydrocracking catalysts. The physicochemical and structural characterization of the solid catalysts were investigated and reported through N2 physisorption, XRD, TGA-DSC, FT-IR and TEM techniques. Solid catalysts surface acidities were investigated through FT-IR spectroscopy aided by pyridine adsorption. The solid catalytic activities were evaluated through hydro conversion of n-hexane and n-heptane employing micro-catalytic pulse technique directly connected to a gas chromatograph analyzer. The thermal stability of the solids was also investigated up to 800 degree C. Crystallinity studies using the XRD technique of all modified samples proved analogous to the parent Y-zeolite, exhibiting nearly an amorphous and microcrystalline character of the second metal oxides. Disclosure of bimetallic catalysts crystalline characterization, through XRD, was not viable. The nitrogen adsorption-desorption isotherms for all samples concluded type I adsorption isotherms, without any hysteresis loop, indicating that the entire pore system is composed of micropores. TEM micrographs of the solid catalysts demonstrate well-dispersed Pt, Ni and Cr nanoparticles having sizes of 2-4 nm and 7-8 nm, respectively. The catalytic activity results indicate that the bimetallic (0.5 Pt-0.3 Cr)/D18 H-Y catalyst is the most active towards n-hexane and n-heptane isomerization while (0.5 Pt-0.6 Ni)/D18 H-Y catalyst can be designed as most suitable as a cracking catalyst

  11. Synergetic effects leading to coke-resistant NiCo bimetallic catalysts for dry reforming of methane

    KAUST Repository

    Li, Lidong

    2015-01-08

    A new dry reforming of methane catalyst comprised of NiCo bimetallic nanoparticles and a Mgx(Al)O support that exhibits high coke resistance and long-term on-stream stability is reported. The structural characterization by XRD, TEM, temperature-programmed reduction, and BET analysis demonstrates that the excellent performance of this catalyst is ascribed to the synergy of various parameters, including metal-nanoparticle size, metal-support interaction, catalyst structure, ensemble size, and alloy effects.

  12. Synthesis and Characterization of Cluster-Derived Supported Bimetallic Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Adams, Richard D; Amiridis, Michael D

    2008-10-10

    New procedures have been developed for synthesizing di- and tri-metallic cluster complexes. The chemical properties of the new complexes have been investigated, particularly toward the activation of molecular hydrogen. These complexes were then converted into bi- and tri-metallic nanoparticles on silica and alumina supports. These nanoparticles were characterized by electron microscopy and were then tested for their ability to produce catalytic hydrogenation of unsaturated hydrocarbons and for the preferential oxidation of CO in the presence of hydrogen. The bi- and tri-metallic nanoparticles exhibited far superior activity and selectivity as hydrogenation catalysts when compared to the individual metallic components. It was found that the addition of tin greatly improved the selectivity of the catalysts for the hydrogenation of polyolefins. The addition of iron improves the catalysts for the selective oxidation of CO by platinum in the presence of hydrogen. The observations should lead to the development of lower cost routes to molecules that can be used to produce polymers and plastics for use by the general public and for procedures to purify hydrogen for use as an alternative energy in the hydrogen economy of the future.

  13. Synthesis and Electrochemical Evaluation of Carbon Supported Pt-Co Bimetallic Catalysts Prepared by Electroless Deposition and Modified Charge Enhanced Dry Impregnation

    Directory of Open Access Journals (Sweden)

    John Meynard M. Tengco

    2016-06-01

    Full Text Available Carbon-supported bimetallic Pt-Co cathode catalysts have been previously identified as higher activity alternatives to conventional Pt/C catalysts for fuel cells. In this work, a series of Pt-Co/C catalysts were synthesized using electroless deposition (ED of Pt on a Co/C catalyst prepared by modified charge enhanced dry impregnation. X-ray diffraction (XRD and scanning transmission electron microscopy (STEM characterization of the base catalyst showed highly dispersed particles. A basic ED bath containing PtCl62− as the Pt precursor, dimethylamine borane as reducing agent, and ethylenediamine as stabilizing agent successfully targeted deposition of Pt on Co particles. Simultaneous action of galvanic displacement and ED resulted in Pt-Co alloy formation observed in XRD and energy dispersive X-ray spectroscopy (XEDS mapping. In addition, fast deposition kinetics resulted in hollow shell Pt-Co alloy particles while particles with Pt-rich shell and Co-rich cores formed with controlled Pt deposition. Electrochemical evaluation of the Pt-Co/C catalysts showed lower active surface but much higher mass and surface activities for oxygen reduction reaction compared to a commercial Pt/C fuel cell catalyst.

  14. Exploration of Cocatalyst Effects on a Bimetallic Cobalt Catalyst System: Enhanced Activity and Enantioselectivity in Epoxide Polymerization

    KAUST Repository

    Widger, Peter C. B.

    2011-07-26

    Organic ionic compounds were synthesized and investigated as cocatalysts with a bimetallic cobalt complex for enantioselective epoxide polymerization. The identities of both the cation and the anion were systematically varied, and the subsequent reactivity was studied. The nature of the ionic cocatalyst dramatically impacted the rate and enantioselectivity of the catalyst system. The ionic cocatalyst [P(N=P(N(CH2)4)3) 4 +][tBuCO2 -] in combination with a bimetallic cobalt complex produced a catalyst system that exhibited the greatest activity and selectivity for a variety of monosubstituted epoxides. © 2011 American Chemical Society.

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

    Energy Technology Data Exchange (ETDEWEB)

    MAVRIKAKIS, MANOS

    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

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  17. Surface-Bound Ligands Modulate Chemoselectivity and Activity of a Bimetallic Nanoparticle Catalyst

    KAUST Repository

    Vu, Khanh B.

    2015-04-03

    "Naked" metal nanoparticles (NPs) are thermodynamically and kinetically unstable in solution. Ligands, surfactants, or polymers, which adsorb at a particle\\'s surface, can be used to stabilize NPs; however, such a mode of stabilization is undesirable for catalytic applications because the adsorbates block the surface active sites. The catalytic activity and the stability of NPs are usually inversely correlated. Here, we describe an example of a bimetallic (PtFe) NP catalyst stabilized by carboxylate surface ligands that bind preferentially to one of the metals (Fe). NPs stabilized by fluorous ligands were found to be remarkably competent in catalyzing the hydrogenation of cinnamaldehyde; NPs stabilized by hydrocarbon ligands were significantly less active. The chain length of the fluorous ligands played a key role in determining the chemoselectivity of the FePt NP catalysts. (Chemical Presented). © 2015 American Chemical Society.

  18. Pt-Pd bimetallic nanoparticles on MWCNTs: catalyst for hydrogen peroxide electrosynthesis

    Energy Technology Data Exchange (ETDEWEB)

    Felix-Navarro, R. M., E-mail: moi6salazar@hotmail.com; Beltran-Gastelum, M.; Salazar-Gastelum, M. I.; Silva-Carrillo, C.; Reynoso-Soto, E. A.; Perez-Sicairos, S.; Lin, S. W. [Centro de Graduados e Investigacion, Instituto Tecnologico de Tijuana (Mexico); Paraguay-Delgado, F. [Centro de Investigacion en Materiales Avanzados (Mexico); Alonso-Nunez, G. [Centro de Nanociencias y Nanotecnologia (Mexico)

    2013-08-15

    Bimetallic nanoparticles of Pt-Pd were deposited by the microemulsion method on a multiwall carbon nanotube (MWCNTs) to obtain a Pt-Pd/MWCNTs for electrocatalytic reduction of O{sub 2} to H{sub 2}O{sub 2}. The activity and selectivity of the catalyst was determined qualitatively by the rotating disk electrode method in acidic medium. The catalyst was spray-coated onto a reticulated vitreous carbon substrate and quantitatively was tested in bulk electrolysis for 20 min under potentiostatic conditions (0.5 V vs Ag/AgCl) in a 0.5 M H{sub 2}SO{sub 4} electrolyte using dissolved O{sub 2}. The bulk electrolysis experiments show that the Pt-Pd/MWCNTs catalyst is more efficient for H{sub 2}O{sub 2} electrogeneration than a MWCNTs catalyst. Nitrobenzene degradation by electrogenerated H{sub 2}O{sub 2} alone and Electro-Fenton process were also tested. Our results show that both processes decompose nitrobenzene, but the Electro-Fenton process does it more efficiently. The prepared nanoparticulated catalyst shows a great potential in environmental applications.

  19. Highly selective bimetallic Pt-Cu/Mg(Al)O catalysts for the aqueous-phase reforming of glycerol

    NARCIS (Netherlands)

    Boga, D.A.; Oord, R.; Beale, A.M.; Chung, Y.M.; Bruijnincx, P.C.A.; Weckhuysen, B.M.

    2013-01-01

    Monometallic Pt and bimetallic Pt-Cu catalysts supported on Mg(Al)O mixed oxides, obtained by calcination of the corresponding layered double hydroxides (LDHs), were prepared and tested in the aqueous-phase reforming (APR) of glycerol. The effect of the Mg/Al ratio and calcination temperature of the

  20. Sn surface-enriched Pt-Sn bimetallic nanoparticles as a selective and stable catalyst for propane dehydrogenation

    KAUST Repository

    Zhu, Haibo

    2014-12-01

    A new one pot, surfactant-free, synthetic route based on the surface organometallic chemistry (SOMC) concept has been developed for the synthesis of Sn surface-enriched Pt-Sn nanoparticles. Bu3SnH selectively reacts with [Pt]-H formed in situ at the surface of Pt nanoparticles, Pt NPs, obtained by reduction of K2PtCl4 by LiB(C2H5)3H. Chemical analysis, 1H MAS and 13C CP/MAS solid-state NMR as well as two-dimensional double-quantum (DQ) and triple-quantum (TQ) experiments show that organo-tin moieties Sn(n-C4H9) are chemically linked to the surface of Pt NPs to produce, in fine, after removal of most of the n-butyl fragment, bimetallic Pt-Sn nanoparticles. The Sn(n-CH2CH2CH2CH3) groups remaining at the surface are believed to stabilize the as-synthesized Pt-Sn NPs, enabling the bimetallic NPs to be well dispersed in THF. Additionally, the Pt-Sn nanoparticles can be supported on MgAl2O4 during the synthesis of the nanoparticles. Some of the Pt-Sn/MgAl2O4 catalyst thus prepared exhibits high activity in PROX of CO and an extremely high selectivity and stability in propane dehydrogenation to propylene. The enhanced activity in propane dehydrogenation is associated with the high concentration of inactive Sn at the surface of Pt nanoparticles which ”isolates” the active Pt atoms. This conclusion is confirmed by XRD, NMR, TEM, and XPS analysis.

  1. Selective Liquid-Phase Semihydrogenation of Functionalized Acetylenes and Propargylic Alcohols with Silica-Supported Bimetallic Palladium—Copper Catalysts

    NARCIS (Netherlands)

    Koten, G. van; Spee, M.P.R.; Meijer, M.D.; Slagt, M.Q.; Geus, John W.

    2001-01-01

    Silica-supported, bimetallic palladium-copper catalysts were prepared in solution under mild conditions by reacting lithium di(4-tolyl)cuprate with palladium acetate in the presence of silica particles. Small bimetallic palladium-copper particles were deposited on the silica surface as confirmed wit

  2. Facile synthesis of ultrathin bimetallic PtSn wavy nanowires by nanoparticle attachment as enhanced hydrogenation catalysts.

    Science.gov (United States)

    Ding, Jiabao; Bu, Lingzheng; Zhang, Nan; Yao, Jianlin; Huang, Yu; Huang, Xiaoqing

    2015-03-01

    Ultrathin wavy nanowires represent an emerging class of nanostructures that exhibit unique catalytic, magnetic, and electronic properties, but the controlled production of bimetallic wavy nanowires remains a significant challenge. Ultrathin bimetallic PtSn nanowires have been prepared with high yield and featuring a highly wavy structure. Owing to the ultrathin nature and unique electronic properties of these PtSn wavy nanowires, they exhibit improved catalytic performance for the hydrogenation of nitrobenzene, as well as for the hydrogenation of styrene. These results suggest a new strategy to prepare highly active catalysts through defect engineering and can significantly impact broad practical applications. PMID:25603959

  3. Ag-Cu Bimetallic Nanoparticles Prepared by Microemulsion Method as Catalyst for Epoxidation of Styrene

    Directory of Open Access Journals (Sweden)

    Hong-Kui Wang

    2012-01-01

    Full Text Available Ag/Cu bimetallic nanocatalysts supported on reticulate-like γ-alumina were prepared by a microemulsion method using N2H4·H2O as the reducing agent. The catalysts were activated by calcination followed with hydrogen reduction at 873K, and the properties were confirmed using various characterization techniques. Compared with metal oxides particles, Ag-Cu particles exhibited smaller sizes (<5 nm after calcination in H2 at 873K. XPS results indicated that the binding energies changed with the Ag/Cu ratios, suggesting that increasing the copper content gave both metals a greater tendency to lose electrons. Furthermore, Ag-Cu bimetallic nanoparticles supported on γ-alumina showed better catalytic activity on the epoxidation of styrene as compared with the corresponding monometallic silver or copper. The styrene oxide selectivity could reach 76.6% at Ag/Cu molar ratio of 3/1, while the maximum conversion (up to 94.6% appeared at Ag/Cu molar ratio of 1/1 because of the maximum interaction between silver and copper.

  4. Desorption of Furfural from Bimetallic Pt-Fe Oxides/Alumina Catalysts

    Directory of Open Access Journals (Sweden)

    Gloria Lourdes Dimas-Rivera

    2014-01-01

    Full Text Available In this work, the desorption of furfural, which is a competitive intermediate during the production of biofuel and valuable aromatic compounds, was studied using pure alumina, as well as alumina impregnated with iron and platinum oxides both individually and in combination, using thermogravimetric analysis (TGA. The bimetallic sample exhibited the lowest desorption percentage for furfural. High-resolution transmission electron microscopy (HRTEM imaging revealed the intimate connection between the iron and platinum oxide species on the alumina support. The mechanism of furfural desorption from the Pt-Fe/Al2O3 0.5%-0.5% sample was determined using physisorbed furfural instead of chemisorbed furfural; this mechanism involved the oxidation of the C=O group on furfural by the catalyst. The oxide nanoparticles on γ-Al2O3 support helped to stabilize the furfural molecule on the surface.

  5. Design of Pd-Based Bimetallic Catalysts for ORR: A DFT Calculation Study

    Directory of Open Access Journals (Sweden)

    Lihui Ou

    2015-01-01

    Full Text Available Developing Pd-lean catalysts for oxygen reduction reaction (ORR is the key for large-scale application of proton exchange membrane fuel cells (PEMFCs. In the present paper, we have proposed a multiple-descriptor strategy for designing efficient and durable ORR Pd-based alloy catalysts. We demonstrated that an ideal Pd-based bimetallic alloy catalyst for ORR should possess simultaneously negative alloy formation energy, negative surface segregation energy of Pd, and a lower oxygen binding ability than pure Pt. By performing detailed DFT calculations on the thermodynamics, surface chemistry and electronic properties of Pd-M alloys, Pd-V, Pd-Fe, Pd-Zn, Pd-Nb, and Pd-Ta, are identified theoretically to have stable Pd segregated surface and improved ORR activity. Factors affecting these properties are analyzed. The alloy formation energy of Pd with transition metals M can be mainly determined by their electron interaction. This may be the origin of the negative alloy formation energy for Pd-M alloys. The surface segregation energy of Pd is primarily determined by the surface energy and the atomic radius of M. The metals M which have smaller atomic radius and higher surface energy would tend to favor the surface segregation of Pd in corresponding Pd-M alloys.

  6. {gamma}-Al{sub 2}O{sub 3}-supported Pt catalysts with extremely high dispersions resulting from Pt-W interactions

    Energy Technology Data Exchange (ETDEWEB)

    Alexeev, O.S.; Graham, G.W.; Shelef, M.; Gates, B.C.

    2000-02-15

    Supported bimetallic catalysts are used in large-scale applications, illustrated by naphtha reforming and simultaneous removal of CO, hydrocarbons, and NO from automobile exhaust. Conventional preparation methods give materials with relatively large metal particles and low concentrations of bimetallic structures, which are difficult to characterize structurally because of their nonuniformity. Organometallic compounds with preformed metal-metal bonds, in contrast, offer good opportunities for preparation of catalysts with maximized bimetallic interactions and well-defined, highly dispersed structures. The goal of the work described here was to investigate how supports other than MgO stabilize such highly dispersed bimetallic structures and how the nuclearity and composition of the bimetallic cluster precursor influence the catalyst structure and properties, including the Pt-W interactions. The authors report the preparation, characterization, and catalytic properties of {gamma}-Al{sub 2}O{sub 3} supported samples prepared from {l{underscore}brace}Pt[W(CO){sub 3}(C{sub 5}H{sub 5})]{sub 2}(PhCN){sub 2}{r{underscore}brace} and from {l{underscore}brace}Pt{sub 2}W{sub 2}(CO){sub 6}(C{sub 5}H{sub 5}){sub 2}(PPh{sub 3}){sub 2}{r{underscore}brace}.

  7. Pd-Au bimetallic catalysts: understanding alloy effects from planar models and (supported) nanoparticles.

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Feng; Goodman, Wayne D.

    2012-12-21

    Pd-Au bimetallic catalysts often display enhanced catalytic activities and selectivities compared with Pd-alone catalysts. This enhancement is often caused by two alloy effects, i.e., ensemble and ligand effects. The ensemble effect is dilution of surface Pd by Au. With increasing surface Au coverages, contiguous Pd ensembles disappear and isolated Pd ensembles form. For certain reactions, for example vinyl acetate synthesis, this effect is responsible for reaction rate enhancement via the formation of highly active surface sites, e.g., isolated Pd pairs. The disappearance of contiguous Pd ensembles also switches off side reactions catalyzed by these sites. This explains selectivity increase of certain reactions, for example direct H2O2 synthesis. The ligand effect is electronic perturbation of Au to Pd. By direct charge transfer or affecting bond length, the ligand effect causes the Pd d band to be more filled and the d-band center away from the Fermi level. Both changes make Pd more "atomic like" therefore binding reactants and products weaker. For certain reactions, this eliminates the so-called "self poisoning" and enhances activity/selectivity.

  8. Monolayer dispersion thresholds and threshold effect displayed by supported catalysts

    Institute of Scientific and Technical Information of China (English)

    Cun DENG

    2008-01-01

    The principle of spontaneous monolayer dis-persion holds that active components of many supported catalysts will disperse spontaneously onto the surface of the carrier. The monolayer dispersion threshold of the active component on the surface of the carrier can be measured by X-ray diffraction phase-quantitative extra-polation method, etc. By measuring the monolayer disper-sion threshold, beneficial information on the surface structure and dispersion of supported catalysts can be obtained, and the optimal preparative processing condi-tions of the catalysts can be chosen. The proportion of the active component of many supported catalysts can be optimized while its monolayer dispersion threshold is observed. Mutation values of many physicochemical properties of supported catalysts are related to monolayer dispersion thresholds; the threshold effect on catalysts is apparent, and the proposal regarding the threshold effect provides instruction for the research on catalysts.

  9. Facile Synthesis of Porous Dendritic Bimetallic Platinum-Nickel Nanocrystals as Efficient Catalysts for the Oxygen Reduction Reaction.

    Science.gov (United States)

    Eid, Kamel; Wang, Hongjing; Malgras, Victor; Alothman, Zeid Abdullah; Yamauchi, Yusuke; Wang, Liang

    2016-05-01

    Certain bimetallic nanocrystals (NCs) possess promising catalytic properties for electrochemical energy conversion. Herein, we report a facile method for the one-step synthesis of porous dendritic PtNi NCs in aqueous solution at room temperature that contrasts with the traditional multistep thermal decomposition approach. The dendritic PtNi NCs assembled by interconnected arms are efficient catalysts for the oxygen reduction reaction. This direct and efficient method is favorable for the up-scaled synthesis of active catalysts used in electrochemical applications. PMID:26879517

  10. Chemical composition dispersion in bi-metallic nanoparticles: semi-automated analysis using HAADF-STEM

    Energy Technology Data Exchange (ETDEWEB)

    Epicier, T., E-mail: thierry.epicier@insa-lyon.fr [INSA-Lyon, MATEIS CNRS UMR5510, Bat. Blaise Pascal (France); Sato, K. [Institute for Materials Research, Tohoku University, Material Processing and Characterization Division (Japan); Tournus, F. [Universite Lyon 1, LPMCN, UMR 5586 CNRS and Universite de Lyon (France); Konno, T. [Institute for Materials Research, Tohoku University, Material Processing and Characterization Division (Japan)

    2012-09-15

    We present a method using high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) to determine the chemical composition of bi-metallic nanoparticles. This method, which can be applied in a semi-automated way, allows large scale analysis with a statistical number of particles (several hundreds) in a short time. Once a calibration curve has been obtained, e.g., using energy-dispersive X-ray spectroscopy (EDX) measurements on a few particles, the HAADF integrated intensity of each particle can indeed be directly related to its chemical composition. After a theoretical description, this approach is applied to the case of iron-palladium nanoparticles (expected to be nearly stoichiometric) with a mean size of 8.3 nm. It will be shown that an accurate chemical composition histogram is obtained, i.e., the Fe content has been determined to be 49.0 at.% with a dispersion of 10.4 %. HAADF-STEM analysis represents a powerful alternative to fastidious single particle EDX measurements, for the compositional dispersion in alloy nanoparticles.

  11. Rational design of Mg-Al mixed oxide-supported bimetallic catalysts for dry reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Tsyganok, Andrey I. [Centre for Catalysis Research and Innovation, Department of Chemistry, University of Ottawa, D' Iorio Hall, 10 Marie Curie Street, Ottawa, Ont. (Canada); Inaba, Mieko [Natural Gas Technology Development Team, Teikoku Oil Co., 9-23-30 Kitakarasuyama, Setagaya-ku, Tokyo 157-0061 (Japan); Tsunoda, Tatsuo; Uchida, Kunio; Suzuki, Kunio; Hayakawa, Takashi [Institute for Materials and Chemical Process, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba 305-8565 (Japan); Takehira, Katsuomi [Department of Applied Chemistry, Faculty of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527 (Japan)

    2005-09-18

    A novel synthetic strategy for preparing bimetallic Ru-M (M=Cr, Fe, Co, Ni and Cu) catalysts, supported on Mg-Al mixed oxide, has been introduced. It was based on a 'memory effect', i.e. on the ability of Mg-Al mixed oxide to reconstruct a layered structure upon rehydration with an aqueous solution. By repeated calcinations-rehydration cycles, layered double hydroxide (LDH) precursors of catalysts containing two different metals were synthesized. Bimetallic catalysts were then generated (1) in situ from LDH under methane reforming reaction conditions and (2) from mixed metal oxides obtained by preliminary LDH calcination. Among all the LDH-derived catalysts, a Ru{sup 0.1%}-Ni{sup 5.0%}/MgAlO{sub x} sample revealed the highest activity and selectivity to syngas, a suitable durability and a low coking capacity. A promoting effect of ruthenium on catalytic function of supported nickel was demonstrated. Preliminary LDH calcination was shown to markedly affect the catalytic activity of the derived catalysts and especially their coking properties.

  12. Designing supported palladium-on-gold bimetallic nano-catalysts for controlled hydrogenation of acetylene in large excess of ethylene

    Science.gov (United States)

    Malla, Pavani

    Ethylene is used as a starting point for many chemical intermediates in the petrochemical industry. It is predominantly produced through steam cracking of higher hydrocarbons (ethane, propane, butane, naphtha, and gas oil). During the cracking process, a small amount of acetylene is produced as a side product. However, acetylene must be removed since it acts as a poison for ethylene polymerization catalysts at even ppm concentrations (>5 ppm). Thus, the selective hydrogenation of acetylene to ethylene is an important process for the purification of ethylene. Conventional, low weight loading Pd catalysts are used for this selective reaction in high concentration ethylene streams. Gold was initially considered to be catalytically inactive for a long time. This changed when gold was seen in the context of the nanometric scale, which has indeed shown it to have excellent catalytic activity as a homogeneous or a heterogeneous catalyst. Gold is proved to have high selectivity to ethylene but poor at conversion. Bimetallic Au and Pd catalysts have exhibited superior activity as compared to Pd particles in semi-hydrogenation. Hydrogenation of acetylene was tested using this bimetallic combination. The Pd-on-Au bimetallic catalyst structure provides a new synthesis approach in improving the catalytic properties of monometallic Pd materials. TiO 2 as a support material and 0.05%Pd loading on 1%Au on titania support and used different treatment methods like washing plasma and reduction between the two metal loadings and was observed under 2:1 ratio. In my study there were two set of catalysts which were prepared by a modified incipient wetness impregnation technique. Out of all the reaction condition the catalyst which was reduced after impregnating gold and then impregnating palladium which was further treated in non-thermal hydrogen plasma and then pretreated in hydrogen till 250°C for 1 hour produced the best activity of 76% yield at 225°C. Stability tests were conducted

  13. Preparation and characterization of planar Ni–Au bimetallic model catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Fan, E-mail: fan.yang@chem.tamu.edu; Yao, Yunxi; Yan, Zhen; Min, Hlaing; Goodman, D. Wayne

    2013-10-15

    Ni–Au bimetallic model catalysts were prepared as thin films on Re(0 0 0 1) or Ru(0 0 0 1) single crystal substrates. Surface compositions and electronic structures of the Ni–Au thin films were characterized by low energy ion scattering spectroscopy and X-ray photoelectron spectroscopy, respectively. Surface alloys were prepared by annealing Ni–Au thin films from 500 to 800 K, resulting in substantial surface enrichment of Au. Annealing a Ni–Au thin film with a 1:1 bulk composition ratio at 700 K for 10 min resulted in a surface alloy with 84% (atomic concentration) of Au in the outermost surface layer. The surface atomic structure was investigated using CO as probe molecules, which exclusively adsorbs on the Ni atoms rather than on the Au atoms at room temperature. Polarization modulation infrared reflection absorption spectroscopy of CO adsorption on Ni–Au surface alloys showed that CO adsorption on two-fold bridge sites decreased and finally disappeared with an increase of Au surface concentration. The absence of Ni bridge site CO adsorption indicated that Ni atoms were isolated by Au atoms on Ni–Au alloyed surface.

  14. Application of a Re-Pd bimetallic catalyst for treatment of perchlorate in waste ion-exchange regenerant brine.

    Science.gov (United States)

    Liu, Jinyong; Choe, Jong Kwon; Sasnow, Zachary; Werth, Charles J; Strathmann, Timothy J

    2013-01-01

    Concentrated sodium chloride (NaCl) brines are often used to regenerate ion-exchange (IX) resins applied to treat drinking water sources contaminated with perchlorate (ClO(4)(-)), generating large volumes of contaminated waste brine. Chemical and biological processes for ClO(4)(-) reduction are often inhibited severely by high salt levels, making it difficult to recycle waste brines. Recent work demonstrated that novel rhenium-palladium bimetallic catalysts on activated carbon support (Re-Pd/C) can efficiently reduce ClO(4)(-) to chloride (Cl(-)) under acidic conditions, and here the applicability of the process for treating waste IX brines was examined. Experiments conducted in synthetic NaCl-only brine (6-12 wt%) showed higher Re-Pd/C catalyst activity than in comparable freshwater solutions, but the rate constant for ClO(4)(-) reduction measured in a real IX waste brine was found to be 65 times lower than in the synthetic NaCl brine. Through a series of experiments, co-contamination of the IX waste brine by excess NO(3)(-) (which the catalyst reduces principally to NH(4)(+)) was found to be the primary cause for deactivation of the Re-Pd/C catalyst, most likely by altering the immobilized Re component. Pre-treatment of NO(3)(-) using a different bimetallic catalyst (In-Pd/Al(2)O(3)) improved selectivity for N(2) over NH(4)(+) and enabled facile ClO(4)(-) reduction by the Re-Pd/C catalyst. Thus, sequential catalytic treatment may be a promising strategy for enabling reuse of waste IX brine containing NO(3)(-) and ClO(4)(-).

  15. Low-temperature 1 3-butadiene Hydrogenation over Supported Pt/3d/gamma-Al2O3 Bimetallic Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    W Lonergan; X Xing; R Zheng; S Qi; B Huang; J Chen

    2011-12-31

    Low-temperature 1,3-butadiene hydrogenation is used as a probe reaction to investigate the hydrogenation activity over several {gamma}-Al{sub 2}O{sub 3} supported Pt/3d (3d = Co, Ni, Cu) bimetallic catalysts. Batch and flow reactor studies are employed to quantify the kinetic activity and steady-state conversion, respectively, of each catalyst. Transmission electron microscopy (TEM) is utilized to characterize particle sizes and extended X-ray absorption fine structure (EXAFS) measurements are performed to verify the Pt-3d bimetallic bond formation. Pulse carbon monoxide chemisorption measurements are also performed to characterize the number of active sites. Additionally, density functional theory (DFT) calculations are included to determine the binding energies of 1,3-butadiene and atomic hydrogen on the corresponding model surfaces. The binding energies of the adsorbates are found to correlate with the hydrogenation activity, allowing for use of such correlation to potentially predict hydrogenation catalysts with enhanced activity based on the binding energies of the adsorbates of interest.

  16. Hydrotreatment of wood-based pyrolysis oil using zirconia-supported mono- and bimetallic (Pt, Pd, Rh) catalysts

    OpenAIRE

    Ardiyanti, A. R.; GUTIERREZ, A.; Honkela, M. L.; Krause, A.O.I.; Heeres, H. J.

    2011-01-01

    Fast pyrolysis oil (PO), the liquid product of fast pyrolysis of lignocellulosic biomass, requires upgrading to extent its application range and for instance to allow for co-feeding in an existing oil-refinery. Catalytic hydrotreatment reactions (350 degrees C, 20 MPa total pressure, and 4h reaction time) with mono- and bimetallic metal catalysts based on Rh, Pt, Pd on a zirconia support were performed in a batch set-up. Pd/ZrO(2) showed the highest activity, followed by Rh/ZrO(2). Upgraded o...

  17. Catalytic activity of bimetallic catalysts highly sensitive to the atomic composition and phase structure at the nanoscale

    Science.gov (United States)

    Shan, Shiyao; Petkov, Valeri; Prasai, Binay; Wu, Jinfang; Joseph, Pharrah; Skeete, Zakiya; Kim, Eunjoo; Mott, Derrick; Malis, Oana; Luo, Jin; Zhong, Chuan-Jian

    2015-11-01

    The ability to determine the atomic arrangement in nanoalloy catalysts and reveal the detailed structural features responsible for the catalytically active sites is essential for understanding the correlation between the atomic structure and catalytic properties, enabling the preparation of efficient nanoalloy catalysts by design. Herein we describe a study of CO oxidation over PdCu nanoalloy catalysts focusing on gaining insights into the correlation between the atomic structures and catalytic activity of nanoalloys. PdCu nanoalloys of different bimetallic compositions are synthesized as a model system and are activated by a controlled thermochemical treatment for assessing their catalytic activity. The results show that the catalytic synergy of Pd and Cu species evolves with both the bimetallic nanoalloy composition and temperature of the thermochemical treatment reaching a maximum at a Pd : Cu ratio close to 50 : 50. The nanoalloys are characterized structurally by ex situ and in situ synchrotron X-ray diffraction, including atomic pair distribution function analysis. The structural data show that, depending on the bimetallic composition and treatment temperature, PdCu nanoalloys adopt two different structure types. One features a chemically ordered, body centered cubic (B2) type alloy consisting of two interpenetrating simple cubic lattices, each occupied with Pd or Cu species alone, and the other structure type features a chemically disordered, face-centered cubic (fcc) type of alloy wherein Pd and Cu species are intermixed at random. The catalytic activity for CO oxidation is strongly influenced by the structural features. In particular, it is revealed that the prevalence of chemical disorder in nanoalloys with a Pd : Cu ratio close to 50 : 50 makes them superior catalysts for CO oxidation in comparison with the same nanoalloys of other bimetallic compositions. However, the catalytic synergy can be diminished if the Pd50Cu50 nanoalloys undergo phase

  18. Synergy between Two Metal Catalysts: A Highly Active Silica-Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane.

    Science.gov (United States)

    Samantaray, Manoja K; Dey, Raju; Kavitake, Santosh; Abou-Hamad, Edy; Bendjeriou-Sedjerari, Anissa; Hamieh, Ali; Basset, Jean-Marie

    2016-07-13

    A well-defined, silica-supported bimetallic precatalyst [≡Si-O-W(Me)5≡Si-O-Zr(Np)3] (4) has been synthesized for the first time by successively grafting two organometallic complexes [W(Me)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple-quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON = 1436) than the monometallic W hydride (TON = 650) in the metathesis of n-decane at 150 °C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation that occurs on Zr. The produced olefin resulting from a β-H elimination undergoes easy metathesis on W. PMID:27248839

  19. Synergy between Two Metal Catalysts: A Highly Active Silica Supported Bimetallic W/Zr Catalyst for Metathesis of n-Decane

    KAUST Repository

    Samantaray, Manoja K

    2016-06-01

    A well-defined, silica supported, bimetallic precatalyst [≡Si-O-W(Me)5 ≡Si-O-Zr(Np)3](4) has been synthesized for the first time via successively grafting two organometallic complexes [W(CH3)6 (1) followed by ZrNp4 (2)] on a single silica support. Surprisingly, multiple quantum NMR characterization demonstrates that W and Zr species are in close proximity to each other. Hydrogenation of this bimetallic catalyst at room temperature showed the easy formation of Zirconium hydride, probably facilitated by tungsten hydride which was formed at this temperature. This bimetallic W/Zr hydride precatalyst proved to be more efficient (TON: 1436) than the monometallic W hydride (TON: 650) in metathesis of n-decane at 150 0C. This synergy between Zr and W suggests that the slow step of alkane metathesis is the C-H bond activation which occurs on Zr. The produced olefin resulting from a ß–H elimination undergoes easy metathesis on W.

  20. Enhanced performance of the catalytic conversion of allyl alcohol to 3-hydroxypropionic acid using bimetallic gold catalysts.

    Science.gov (United States)

    Falletta, Ermelinda; Della Pina, Cristina; Rossi, Michele; He, Qian; Kiely, Christopher J; Hutchings, Graham J

    2011-01-01

    One of the strategic building blocks in organic synthesis is 3-hydroxypropionic acid, which is particularly important for the manufacture of high performance polymers. However, to date, despite many attempts using both biological and chemical routes, no large scale effective process for manufacturing 3-hydroxypropionic acid has been developed. One potentially useful starting point is from allyl alcohol, as this can be obtained in principle from the dehydration of glycerol, thereby presenting a bio-renewable green pathway to this important building block. The catalytic transformation of allyl alcohol to 3-hydroxypropionic acid presents interesting challenges in catalyst design, particularly with respect to the control of selectivity among the products that can be expected, as acrylic acid, acrolein and glyceric acid can also be formed. In this paper, we present a novel eco-sustainable catalytic pathway leading to 3-hydroxypropionic acid, which highlights the outstanding potential of gold-based and bimetallic catalysts in the aerobic oxidation of allyl alcohol. PMID:22455056

  1. Enhanced Hydrodeoxygenation of m -Cresol over Bimetallic Pt–Mo Catalysts through an Oxophilic Metal-Induced Tautomerization Pathway

    Energy Technology Data Exchange (ETDEWEB)

    Robinson, Allison; Ferguson, Glen Allen; Gallagher, James R.; Cheah, Singfoong; Beckham, Gregg T.; Schaidle, Joshua A.; Hensley, Jesse E.; Medlin, J. Will

    2016-07-01

    Supported bimetallic catalysts consisting of a noble metal (e.g., Pt) and an oxophilic metal (e.g., Mo) have received considerable attention for the hydrodeoxygenation of oxygenated aromatic compounds produced from biomass fast pyrolysis. Here, we report that PtMo can catalyze m-cresol deoxygenation via a pathway involving an initial tautomerization step. In contrast, the dominant mechanism on monometallic Pt/Al2O3 was found to be sequential Pt-catalyzed ring hydrogenation followed by dehydration on the support. Bimetallic Pt10Mo1 and Pt1Mo1 catalysts were found to produce the completely hydrogenated and deoxygenated product, methylcyclohexane (MCH), with much higher yields than monometallic Pt catalysts with comparable metal loadings and surface areas. Over an inert carbon support, MCH formation was found to be slow over monometallic Pt catalysts, while deoxygenation was significant for PtMo catalysts even in the absence of an acidic support material. Experimental studies of m-cresol deoxygenation together with density functional theory calculations indicated that Mo sites on the PtMo bimetallic surface dramatically lower the barrier for m-cresol tautomerization and subsequent deoxygenation. The accessibility of this pathway arises from the increased interaction between the oxygen of m-cresol and the Mo sites in the Pt surface. This interaction significantly alters the configuration of the precursor and transition states for tautomerization. A suite of catalyst characterization techniques including X-ray absorption spectroscopy (XAS) and temperature-programmed reduction (TPR) indicate that Mo was present in a reduced state on the bimetallic surface under conditions relevant for reaction. Overall, these results suggest that the use of bifunctional metal catalysts can result in new reaction pathways that are unfavorable on monometallic noble metal catalysts.

  2. Suppression of carbon formation in CH4–CO2 reforming by addition of Sr into bimetallic Ni–Co/γ-Al2O3 catalyst

    Directory of Open Access Journals (Sweden)

    Ahmed Al-Fatesh

    2015-01-01

    Full Text Available Bimetallic catalysts, containing 5 wt% Ni + 5 wt% Co supported on γ-Al2O3 combined with different amounts of Sr promoter ranging from 0 to 1 wt%, for dry reforming reaction were prepared by the impregnation method. The dry reforming reaction was carried out at atmospheric pressure using CO2/CH4/N2 feed ratio of 17/17/2, F/W = 60 mL/min gcat and reaction temperature range of 500–700 °C. The performance of the developed catalyst was evaluated by estimating the CH4 and CO2 conversions, and by performing a long run stability test. The fresh and spent catalysts were characterized by BET, TGA, TPD, TPR, and TPO. The bimetallic catalysts provided higher activity than the monometallic-catalysts. When the bimetallic was promoted with Sr, the activity decreased slightly however, the stability enhanced. The best stability, estimated by the deactivation factor, and less carbon deposition, measured by TGA, were obtained when 5Ni5CoSr0.75 catalyst was used.

  3. Aqueous Phase Glycerol Reforming by PtMo Bimetallic Nano-Particle Catalyst: Product Selectivity and Structural Characterization

    Energy Technology Data Exchange (ETDEWEB)

    Stach E. A.; Dietrich, P.J.; Lobo-Lapidus, R.J.; Wu, T.; Sumer, A.; Akatay, M.C.; Fingland, B.R.; Guo, N.; Dumesic, J.A.; Marshall, C.L.; Jellinek, J.; Delgass, W.N.; Ribeiro, F.H.; Miller, J.T.

    2012-03-01

    A carbon supported PtMo aqueous phase reforming catalyst for producing hydrogen from glycerol was characterized by analysis of the reaction products and pathway, TEM, XPS and XAS spectroscopy. Operando X-ray absorption spectroscopy (XAS) indicates the catalyst consists of bimetallic nano-particles with a Pt rich core and a Mo rich surface. XAS of adsorbed CO indicates that approximately 25% of the surface atoms are Pt. X-ray photoelectron spectroscopy indicates that there is unreduced and partially reduced Mo oxide (MoO{sub 3} and MoO{sub 2}), and Pt-rich PtMo bimetallic nano-particles. The average size measured by transmission electron microscopy of the fresh PtMo nano-particles is about 2 nm, which increases in size to 5 nm after 30 days of glycerol reforming at 31 bar and 503 K. The catalyst structure differs from the most energetically stable structure predicted by density functional theory (DFT) calculations for metallic Pt and Mo atoms. However, DFT indicates that for nano-particles composed of metallic Pt and Mo oxide, the Mo oxide is at the particle surface. Subsequent reduction would lead to the experimentally observed structure. The aqueous phase reforming reaction products and intermediates are consistent with both C-C and C-OH bond cleavage to generate H{sub 2}/CO{sub 2} or the side product CH{sub 4}. While the H{sub 2} selectivity at low conversion is about 75%, cleavage of C-OH bonds leads to liquid products with saturated carbon atoms. At high conversions (to gas), these will produced additional CH{sub 4} reducing the H{sub 2} yield and selectivity.

  4. Greatly improved electrochemical performance of lithium-oxygen batteries with a bimetallic platinum-copper alloy catalyst

    Science.gov (United States)

    Lee, Minwook; Hwang, Yubin; Yun, Kyung-Han; Chung, Yong-Chae

    2015-08-01

    Research on the cathode catalysts of lithium-oxygen (Li-O2) batteries is one of the most important branches to commercialize these batteries to overcome the sluggish kinetics during both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). In this study, a high performance catalyst based on a bimetallic Pt-Cu alloy is investigated for Li-O2 batteries using first-principles calculation. The theoretical prediction shows that the Pt-Cu alloy is much more effective than the pure Pt according to the electrochemical performance. In particular, the effectiveness of the catalytic property is maximized in the case of the PtCu (111) surface which greatly reduces the large overpotentials of the original Li-O2 batteries during the OER/ORR. It is identified for the first time that the charge overpotentials are affected mainly by the inherent surface charge character of the alloy catalyst. It is observed that the more negatively charged PtCu (111) surface can act as a weakly positively charged surface for the adsorption of Li-O intermediates and thus result in weak ionic bonding of the intermediates on the surface. As a result, the dominant factor improving the catalytic performance is clearly demonstrated, providing insight into the design of an efficient catalyst for Li-O2 battery technologies.

  5. Efficiently cubic platinum-cobalt bimetallic nano-catalysts for use in low-cost dye-sensitized solar cells

    International Nuclear Information System (INIS)

    Graphical abstract: Low-platinum (Pt) alloy can be expected to substitute for the conventional Pt catalyst due to its modified Pt electronic structure with highly electrocatalytic activity and Pt-skin nano-structure with high durability. Pt3Co bimetallic nano-catalysts show high catalytic activity for the reduction of triiodide to iodide and low charge transfer resistance at the electrolyte/counter electrode interface as well as those of pure cubic Pt nano-catalysts. DSSC based on Pt3Co CE achieves an enhanced efficiency of 8.16% compared to that of thermal decomposition Pt CE (7.26%). - Highlights: • Cubic Co, Pt, PtCo, and Pt3Co nano-catalysts were synthesized in the oleylamine. • Pt-metal alloy with modified Pt electronic structure shows highly electrocatalytic activity. • Pt-metal alloy with Pt-skin nano-structure shows high durability. • The efficiency of DSSC with Pt3Co bimetallic counter electrode reaches 8.16%. - Abstract: Low-platinum (Pt) alloy can be expected to substitute for the conventional Pt catalyst due to its modified Pt electronic structure with highly electrocatalytic activity and Pt-skin nano-structure with high durability. Here we synthesize the pure cobalt (Co), pure Pt, PtCo, and Pt3Co nano-catalysts in the oleylamine and use their as the counter electrode (CE) materials for dye-sensitized solar cells (DSSCs). Cyclic voltammetry and electrochemical impedance spectroscopy measurements indicate that the cubic Pt3Co CE has a high catalytic activity for the reduction of triiodide to iodide and a low charge transfer resistance at the electrolyte/CE interface, which are close to those of the pure cubic Pt CE but superior than those of the thermal decomposition platinum (TDPt) CE due to its modified Pt electronic structure and its catalytic surfaces are composed of Pt-rich and Pt-skin nano-structure. DSSC based on Pt3Co CE achieves a photovoltaic conversion efficiency of 8.16% under full sunlight illumination (100 mW cm−2, AM1.5 G), which

  6. EXAFS Peaks and TPR Characterizing Bimetallic Interactions: Effects of Impregnation Methods on the Structure of Pt-Ru/C Catalysts

    Directory of Open Access Journals (Sweden)

    Nan-Yu Chen

    2014-01-01

    Full Text Available To investigate bimetallic interactions, Pt-Ru/C catalysts were prepared by coimpregnation (Pt-Ruco/C and successive impregnation (Ru-Ptse/C, while Pt/C, Ru/C, and reduced Pt-Rublack were used as reference. Those samples were characterized by XAS and TPR. When Pt(absorber-Ru(backscatter phase-and-amplitude correction is applied to Fourier transformed (FT EXAFS of Pt-Rublack at Pt edge, the characteristic peak of Pt-Ru interactions appears at 2.70 Å´, whereas, when Pt-Pt correction is applied, the peak appears at about 2.5 Å´. Detailed EXAFS analysis for Pt-Ruco/C and Pt-Ruse/C confirms the nature of the characteristic peak and further indicates that the interactions can semiquantitatively be determined by the relative intensity between Pt-Ru and Pt-Pt characteristic peaks. This simple method in determining bimetallic interaction can be extended to characterize Pt-Pd/γ-Al2O3. However, for Pt-Re/γ-Al2O3, Pt-Re interactions cannot be determined by the method because of the overlap of Pt-Pt and Pt-Re characteristic peaks due to similar phase functions.

  7. Remarkable effect of bimetallic nanocluster catalysts for aerobic oxidation of alcohols: combining metals changes the activities and the reaction pathways to aldehydes/carboxylic acids or esters.

    Science.gov (United States)

    Kaizuka, Kosuke; Miyamura, Hiroyuki; Kobayashi, Shū

    2010-11-01

    Selective oxidation of alcohols catalyzed by novel carbon-stabilized polymer-incarcerated bimetallic nanocluster catalysts using molecular oxygen has been developed. The reactivity and the selectivity were strongly dependent on the combination of metals and solvent systems; aldehydes and ketones were obtained by the gold/platinum catalyst in benzotrifluoride, and esters were formed by the gold/palladium catalyst in methanol. To the best of our knowledge, this is the first example that the reaction pathway has been changed dramatically in gold catalysis by combining with a second metal. The differences in the activity and the selectivity are considered to be derived from the difference in the structure of the bimetallic clusters.

  8. Bimetallic PtAu superlattice arrays: Highly electroactive and durable catalyst for oxygen reduction and methanol oxidation reactions

    Science.gov (United States)

    Feng, Jiu-Ju; He, Li-Li; Fang, Rui; Wang, Qiao-Li; Yuan, Junhua; Wang, Ai-Jun

    2016-10-01

    Superlattice arrays, an important type of nanomaterials, have wide applications in catalysis, optic/electronics and energy storage for the synergetic effects determined by both individual metals and collective interactions. Herein, a simple one-pot solvothermal coreduction approach is developed for facile preparation of bimetallic PtAu alloyed superlattice arrays (PtAu SLAs) in oleylamine, with the assistance of urea via hydrogen bonding induced self-assembly. Urea is essential in morphology-controlled process and prevents PtAu nanoparticles from the disordered aggregation. The characterization and formation mechanism of PtAu SLAs are investigated in details. The as-synthesized hybrid nanocrystals exhibit enhanced electrocatalytic performances for oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) in alkaline electrolyte in comparison with commercial Pt-C (50%, wt.%) and Pt black catalysts.

  9. Desorption of Furfural from Bimetallic Pt-Fe Oxides/Alumina Catalysts

    OpenAIRE

    Gloria Lourdes Dimas-Rivera; Javier Rivera de la Rosa; Carlos J. Lucio-Ortiz; José Antonio De los Reyes Heredia; Virgilio González González; Tomás Hernández

    2014-01-01

    In this work, the desorption of furfural, which is a competitive intermediate during the production of biofuel and valuable aromatic compounds, was studied using pure alumina, as well as alumina impregnated with iron and platinum oxides both individually and in combination, using thermogravimetric analysis (TGA). The bimetallic sample exhibited the lowest desorption percentage for furfural. High-resolution transmission electron microscopy (HRTEM) imaging revealed the intimate connection betwe...

  10. Selective hydrogenation of acetylene on SiO2 supported Ni-In bimetallic catalysts: Promotional effect of In

    Science.gov (United States)

    Chen, Yanjun; Chen, Jixiang

    2016-11-01

    Ni/SiO2 and the bimetallic NixIn/SiO2 catalysts with different Ni/In ratios were tested for the selective hydrogenation of acetylene, and their physicochemical properties before and after the reaction were characterized by means of N2-sorption, H2-TPR, XRD, TEM, XPS, H2 chemisorption, C2H4-TPD, NH3-TPD, FT-IR of adsorbed pyridine, and TG/DTA and Raman. A promotional effect of In on the performance of Ni/SiO2 was found, and NixIn/SiO2 with a suitable Ni/In ratio gave much higher acetylene conversion, ethylene selectivity and catalyst stability than Ni/SiO2. This is ascribed to the geometrical isolation of the reactive Ni atoms with the inert In ones and the charge transfer from the In atoms to Ni ones, both of which are favorable for reducing the adsorption strength of ethylene and restraining the Csbnd C hydrogenolysis and the polymerizations of acetylene and the intermediate compounds. On the whole, Ni6In/SiO2 and Ni10In/SiO2 had better performance. Nevertheless, with increasing the In content, the selectivity to the C4+ hydrocarbons tended to increase due to the enhanced catalyst acidity because of the charge transfer from the In atoms to Ni ones. As the Lewis acid ones, the In sites could promote the polymerization. The catalyst deactivation was also analyzed. We propose that the Ni/SiO2 deactivation is mainly attributed to the phase change from metallic Ni to nickel carbide. The introduction of In inhibited the formation of nickel carbide. However, as the In content increased, the carbonaceous deposit became the main reason for the NixIn/SiO2 deactivation due to the enhanced catalyst acidity.

  11. Dispersed catalysts for co-processing and coal liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Bockrath, B.; Parfitt, D.; Miller, R. [Pittsburgh Energy Technology Center, PA (United States)

    1995-12-31

    The basic goal is to improve dispersed catalysts employed in the production of clean fuels from low value hydrocarbons. The immediate objective is to determine how the properties of the catalysts may be altered to match the demands placed on them by the properties of the feedstock, the qualities of the desired end products, and the economic constraints put upon the process. Several interrelated areas of the application of dispersed catalysts to co-processing and coal conversion are under investigation. The first involves control of the selectivity of MoS{sub 2} catalysts for HDN, HDS, and hydrogenation of aromatics. A second area of research is the development and use of methods to evaluate dispersed catalysts by means of activity and selectivity tests. A micro-flow reactor has been developed for determining intrinsic reactivities using model compounds, and will be used to compare catalysts prepared in different ways. Micro-autoclaves will also be used to develop data in batch experiments at higher partial pressures of hydrogen. The third area under investigation concerns hydrogen spillover reactions between MoS{sub 2} catalysts and carbonaceous supports. Preliminary results obtained by monitoring H{sub 2}/D{sub 2} exchange reactions with a pulse-flow microreactor indicate the presence of spillover between MoS{sub 2} and a graphitic carbon. A more complete study will be made at a later stage of the project. Accomplishments and conclusions are discussed.

  12. Ni-Based Catalysts for Low Temperature Methane Steam Reforming: Recent Results on Ni-Au and Comparison with Other Bi-Metallic Systems

    Directory of Open Access Journals (Sweden)

    Anna M. Venezia

    2013-06-01

    Full Text Available Steam reforming of light hydrocarbons provides a promising method for hydrogen production. Ni-based catalysts are so far the best and the most commonly used catalysts for steam reforming because of their acceptably high activity and significantly lower cost in comparison with alternative precious metal-based catalysts. However, nickel catalysts are susceptible to deactivation from the deposition of carbon, even when operating at steam-to-carbon ratios predicted to be thermodynamically outside of the carbon-forming regime. Reactivity and deactivation by carbon formation can be tuned by modifying Ni surfaces with a second metal, such as Au through alloy formation. In the present review, we summarize the very recent progress in the design, synthesis, and characterization of supported bimetallic Ni-based catalysts for steam reforming. The progress in the modification of Ni with noble metals (such as Au and Ag is discussed in terms of preparation, characterization and pretreatment methods. Moreover, the comparison with the effects of other metals (such as Sn, Cu, Co, Mo, Fe, Gd and B is addressed. The differences of catalytic activity, thermal stability and carbon species between bimetallic and monometallic Ni-based catalysts are also briefly shown.

  13. Synthesis of supported bimetallic nanoparticles with controlled size and composition distributions for active site elucidation

    Energy Technology Data Exchange (ETDEWEB)

    Hakim, Sikander H.; Sener, Canan; Alba Rubio, Ana C.; Gostanian, Thomas M.; O' neill, Brandon J; Ribeiro, Fabio H.; Miller, Jeffrey T.; Dumesic, James A

    2015-08-01

    Elucidation of active sites in supported bimetallic catalysts is complicated by the high level of dispersity in the nanoparticle size and composition that is inherent in conventional methods of catalyst preparation. We present a synthesis strategy that leads to highly dispersed, bimetallic nanoparticles with uniform particle size and composition by means of controlled surface reactions. We demonstrate the synthesis of three systems, RhMo, PtMo, and RhRe, consisting of a highly reducible metal with an oxophilic promoter. These catalysts are characterized by FTIR, CO chemisorption, STEM/EDS, TPR, and XAS analysis. The catalytic properties of these bimetallic nanoparticles were probed for the selective CO hydrogenolysis of (hydroxymethyl)tetrahydropyran to produce 1,6 hexanediol. Based on the characterization results and reactivity trends, the active sites in the hydrogenolysis reaction are identified to be small ensembles of the more noble metal (Rh, Pt) adjacent to highly reduced moieties of the more oxophilic metal (Mo, Re).

  14. Correlating ethylene glycol reforming activity with in-situ EXAFS detection of Ni segregation in supported NiPt bimetallic catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Trupy, Sarah A.; Karim, Ayman M.; Bagia, Christtina; Deng, Weihua; Huang, Yulin; Vlachos, Dionisios G.; Chen, Jingguang

    2012-10-31

    The structural changes in supported NiPt/C and NiPt/γ-Al2O3 catalysts were investigated using in-situ extended X-ray absorption fine structure (EXAFS) under aqueous phase reforming (APR) of ethylene glycol conditions. Reverse Monte Carlo is introduced to analyze the EXAFS data. Parallel reactor studies of APR of ethylene glycol showed that NiPt catalysts were initially more active than monometallic Pt catalysts. The enhanced activity was correlated to changes in the catalyst structure. Under APR conditions, Ni segregated to the surface of the catalysts, resembling Ni-terminated bimetallic surfaces that were predicted to be more active than Pt from theoretical and experimental studies on model surfaces.

  15. A Novelγ-Alumina Supported Fe-Mo Bimetallic Catalyst for Reverse Water Gas Shift Reaction

    Institute of Scientific and Technical Information of China (English)

    Abolfazl Gharibi Kharaji; Ahmad Shariati; Mohammad Ali Takassi

    2013-01-01

    In reverse water gas shift (RWGS) reaction CO2 is converted to CO which in turn can be used to pro-duce beneficial chemicals such as methanol. In the present study, Mo/Al2O3, Fe/Al2O3 and Fe-Mo/Al2O3 catalysts were synthesised using impregnation method. The structures of catalysts were studied using X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) method, inductively coupled plasma atomic emission spectrometer (ICP-AES), temperature programmed reduction (H2-TPR), CO chemisorption, energy dispersive X-ray (EDX) and scanning electron microscopy (SEM) techniques. Kinetic properties of all catalysts were investigated in a batch re-actor for RWGS reaction. The results indicated that Mo existence in structure of Fe-Mo/Al2O3 catalyst enhances its activity as compared to Fe/Al2O3. This enhancement is probably due to better Fe dispersion and smaller particle size of Fe species. Stability test of Fe-Mo/Al2O3 catalyst was carried out in a fixed bed reactor and a high CO yield for 60 h of time on stream was demonstrated. Fe2(MoO4)3 phase was found in the structures of fresh and used catalysts. TPR results also indicate that Fe2(MoO4)3 phase has low reducibility, therefore the Fe2(MoO4)3 phase significantly inhibits the reduction of the remaining Fe oxides in the catalyst, resulted in high stability of Fe-Mo/Al2O3 catalyst. Overall, this study introduces Fe-Mo/Al2O3 as a novel catalyst with high CO yield, almost no by-products and fairly stable for RWGS reaction.

  16. Hydrogenation Conversion of Phenanthrene over Dispersed Mo-based Catalysts

    Institute of Scientific and Technical Information of China (English)

    Hu Yiwen; Da Zhijian; Wang Zijun

    2015-01-01

    With oil-soluble molybdenum compound and sublimed sulfur serving as raw materials, two dispersed Mo-based catalysts were prepared, characterized and then applied to the hydrogenation conversion of phenanthrene. The test results showed that under the conditions speciifed by this study, the catalyst prepared in a higher sulifding atmosphere was more catalytically active due to its higher content of MoS2 and stronger intrinsic catalytic activity of MoS2 unit, which demon-strated that the sulifding atmosphere for the preparation of catalysts not only could inlfuence the yield of MoS2 but also the structure of MoS2. The analysis on the selectivity of octahydrophenanthrene isomers revealed that the catalyst prepared in a lower sulifding atmosphere had a relatively higher catalytic selectivity to the hydrogenation of outer aromatic ring and the structure of catalysts could be modiifed under the speciifc reaction conditions. Moreover, the selectivity between the isomers of as-octahydrophenanthrene at different reaction time and temperature was analyzed and, based on the results, a hydroge-nation mechanism over dispersed Mo-based catalysts was suggested, with monatomic hydrogen transfer and catalytic sur-face desorption of the half-addition intermediates functioning as the key points. In addition, it is concluded that the catalyst prepared in a lower sulifding atmosphere was more capable of adsorption than the other one.

  17. Homogeneously dispersed multimetal oxygen-evolving catalysts.

    Science.gov (United States)

    Zhang, Bo; Zheng, Xueli; Voznyy, Oleksandr; Comin, Riccardo; Bajdich, Michal; García-Melchor, Max; Han, Lili; Xu, Jixian; Liu, Min; Zheng, Lirong; García de Arquer, F Pelayo; Dinh, Cao Thang; Fan, Fengjia; Yuan, Mingjian; Yassitepe, Emre; Chen, Ning; Regier, Tom; Liu, Pengfei; Li, Yuhang; De Luna, Phil; Janmohamed, Alyf; Xin, Huolin L; Yang, Huagui; Vojvodic, Aleksandra; Sargent, Edward H

    2016-04-15

    Earth-abundant first-row (3d) transition metal-based catalysts have been developed for the oxygen-evolution reaction (OER); however, they operate at overpotentials substantially above thermodynamic requirements. Density functional theory suggested that non-3d high-valency metals such as tungsten can modulate 3d metal oxides, providing near-optimal adsorption energies for OER intermediates. We developed a room-temperature synthesis to produce gelled oxyhydroxides materials with an atomically homogeneous metal distribution. These gelled FeCoW oxyhydroxides exhibit the lowest overpotential (191 millivolts) reported at 10 milliamperes per square centimeter in alkaline electrolyte. The catalyst shows no evidence of degradation after more than 500 hours of operation. X-ray absorption and computational studies reveal a synergistic interplay between tungsten, iron, and cobalt in producing a favorable local coordination environment and electronic structure that enhance the energetics for OER. PMID:27013427

  18. Bimetallic catalysts for CO.sub.2 hydrogenation and H.sub.2 generation from formic acid and/or salts thereof

    Energy Technology Data Exchange (ETDEWEB)

    Hull, Jonathan F.; Himeda, Yuichiro; Fujita, Etsuko; Muckeman, James T.

    2015-08-04

    The invention relates to a ligand that may be used to create a catalyst including a coordination complex is formed by the addition of two metals; Cp, Cp* or an unsubstituted or substituted .pi.-arene; and two coordinating solvent species or solvent molecules. The bimetallic catalyst may be used in the hydrogenation of CO.sub.2 to form formic acid and/or salts thereof, and in the dehydrogenation of formic acid and/or salts thereof to form H.sub.2 and CO.sub.2.

  19. Purification of Carbon Nanotubes Synthesized by Catalytic Decomposition of Methane using Bimetallic Fe-Co Catalysts Supported on MgO

    Energy Technology Data Exchange (ETDEWEB)

    Guan, Beh Hoe; Ramli, Irmawati [Advanced Materials and Nanotechnology Laboratory, Institute of Advanced Technology, Universiti Putra Malaysia 43400 UPM Serdang, Selangor (Malaysia); Yahya, Noorhana [Fundamental and Applied Science Department Universiti Teknologi Petronas, Bandar Seri Iskandar, 31750 Tronoh, Perak (Malaysia); Pah, Lim Kean, E-mail: irmawati@science.upm.edu.my [Physics department, Faculty of Science, Universiti Putra Malaysia 43400 UPM Serdang, Selangor (Malaysia)

    2011-02-15

    This work reports the synthesis of carbon nanotubes by catalytic decomposition of methane using bimetallic Fe-Co catalysts supported on MgO. Transmission electron microscopy (TEM) results show the as-prepared carbon nanotubes are multi-walled carbon nanotubes (MWCNTs) with diameter in the range of 15nm to 45nm. Purification of as-prepared MWCNTs was carried out by acid and heat treatment method. EDX results show the Fe, Co and MgO catalysts were successfully removed by refluxing the as-prepared MWCNTs in 3M H{sub 2}SO{sub 4}.

  20. Purification of Carbon Nanotubes Synthesized by Catalytic Decomposition of Methane using Bimetallic Fe-Co Catalysts Supported on MgO

    Science.gov (United States)

    Guan, Beh Hoe; Ramli, Irmawati; Yahya, Noorhana; Kean Pah, Lim

    2011-02-01

    This work reports the synthesis of carbon nanotubes by catalytic decomposition of methane using bimetallic Fe-Co catalysts supported on MgO. Transmission electron microscopy (TEM) results show the as-prepared carbon nanotubes are multi-walled carbon nanotubes (MWCNTs) with diameter in the range of 15nm to 45nm. Purification of as-prepared MWCNTs was carried out by acid and heat treatment method. EDX results show the Fe, Co and MgO catalysts were successfully removed by refluxing the as-prepared MWCNTs in 3M H2SO4.

  1. Highly Dispersed Alloy Catalyst for Durability

    Energy Technology Data Exchange (ETDEWEB)

    Murthi, Vivek S.; Izzo, Elise; Bi, Wu; Guerrero, Sandra; Protsailo, Lesia

    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.

  2. Cu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO

    KAUST Repository

    Sarfraz, Saad

    2016-03-23

    We report a selective and stable electrocatalyst utilizing non-noble metals consisting of Cu and Sn for the efficient and selective reduction of CO2 to CO over a wide potential range. The bimetallic electrode was prepared through the electrodeposition of Sn species on the surface of oxide-derived copper (OD-Cu). The Cu surface, when decorated with an optimal amount of Sn, resulted in a Faradaic efficiency (FE) for CO greater than 90% and a current density of −1.0 mA cm−2 at −0.6 V vs. RHE, compared to the CO FE of 63% and −2.1 mA cm−2 for OD-Cu. Excess Sn on the surface caused H2 evolution with a decreased current density. X-ray diffraction (XRD) suggests the formation of Cu-Sn alloy. Auger electron spectroscopy of the sample surface exhibits zero-valent Cu and Sn after the electrodeposition step. Density functional theory (DFT) calculations show that replacing a single Cu atom with a Sn atom leaves the d-band orbitals mostly unperturbed, signifying no dramatic shifts in the bulk electronic structure. However, the Sn atom discomposes the multi-fold sites on pure Cu, disfavoring the adsorption of H and leaving the adsorption of CO relatively unperturbed. Our catalytic results along with DFT calculations indicate that the presence of Sn on reduced OD-Cu diminishes the hydrogenation capability—i.e., the selectivity towards H2 and HCOOH—while hardly affecting the CO productivity. While the pristine monometallic surfaces (both Cu and Sn) fail to selectively reduce CO2, the Cu-Sn bimetallic electrocatalyst generates a surface that inhibits adsorbed H*, resulting in improved CO FE. This study presents a strategy to provide a low-cost non-noble metals that can be utilized as a highly selective electrocatalyst for the efficient aqueous reduction of CO2.

  3. An anodic alumina supported Ni-Pt bimetallic plate-type catalysts for multi-reforming of methane, kerosene and ethanol

    KAUST Repository

    Zhou, Lu

    2014-05-01

    An anodic alumina supported Ni-Pt bimetallic plate-type catalyst was prepared by a two-step impregnation method. The trace amount 0.08 wt% of Pt doping efficiently suppressed the nickel particle sintering and improved the nickel oxides reducibility. The prepared Ni-Pt catalyst showed excellent performance during steam reforming of methane, kerosene and ethanol under both 3000 h stationary and 500-time daily start-up and shut-down operation modes. Self-activation ability of this catalyst was evidenced, which was considered to be resulted from the hydrogen spillover effect over Ni-Pt alloy. In addition, an integrated combustion-reforming reactor was proposed in this study. However, the sintering of the alumina support is still a critical issue for the industrialization of Ni-Pt catalyst. Copyright © 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.

  4. Driving the Oxygen Evolution Reaction by Nonlinear Cooperativity in Bimetallic Coordination Catalysts.

    Science.gov (United States)

    Wurster, Benjamin; Grumelli, Doris; Hötger, Diana; Gutzler, Rico; Kern, Klaus

    2016-03-23

    Developing efficient catalysts for electrolysis, in particular for the oxygen evolution in the anodic half cell reaction, is an important challenge in energy conversion technologies. By taking inspiration from the catalytic properties of single-atom catalysts and metallo-proteins, we exploit the potential of metal-organic networks as electrocatalysts in the oxygen evolution reaction (OER). A dramatic enhancement of the catalytic activity toward the production of oxygen by nearly 2 orders of magnitude is demonstrated for novel heterobimetallic organic catalysts compared to metallo-porphyrins. Using a supramolecular approach we deliberately place single iron and cobalt atoms in either of two different coordination environments and observe a highly nonlinear increase in the catalytic activity depending on the coordination spheres of Fe and Co. Catalysis sets in at about 300 mV overpotential with high turnover frequencies that outperform other metal-organic catalysts like the prototypical hangman porphyrins. PMID:26937997

  5. Catalyst dispersion and activity under conditions of temperature- staged liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-02-01

    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation.

  6. Performance Comparison of Two Newly Developed Bimetallic (X-Mo/Al2O3, X=Fe or Co) Catalysts for Reverse Water Gas Shift Reaction

    Institute of Scientific and Technical Information of China (English)

    Abolfazl Gharibi Kharaji; Ahmad Shariati

    2016-01-01

    The performance of the two newly developed bimetallic catalysts based on the precursor, Mo/Al2O3, was com-pared for reverse water gas shift (RWGS) reaction. The structures of the precursor and the catalysts were studied using X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) analysis, inductively coupled plasma-atomic emission spec-trometry (ICP-AES), CO chemisorption, temperature programmed reduction of hydrogen (H2-TPR) and scanning electron microscopy (SEM) techniques. The activity of Fe-Mo and Co-Mo catalysts was compared in a ifxed bed reactor at different temperatures. It is shown that the Co-Mo catalyst has higher CO2 conversion at all temperature level. The time-on-stream (TOS) analysis of the activity of catalysts for the RWGS reaction was carried out over a continuous period of 60 h for both catalysts. The Fe-Mo/Al2O3 catalyst exhibits good stability within a period of 60 h, however, the Co-Mo/Al2O3 is gradually deactivated after 50 h of reaction time. Existence of Fe2(MoO4)3 phase in Fe-Mo/Al2O3 catalyst makes this catalyst more stable for RWGS reaction.

  7. XPS study of Cu-Ni bimetallic catalyst%Cu-Ni双金属催化剂的XPS研究

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    采用XPS方法研究了以不同方式引入Ni的Cu-Ni/Al2O3双金 属催化剂的表面结构及不同处理条件对催化剂表面结构的影响。发现催化剂表面存在表面铝 酸盐物种,且Ni的存在会促进表面铝酸盐物种的生成。催化剂经H2还原处理或经CO2加 氢反应后均要发生表面重构。Ni的存在会影响表面重构过程从而影响催化剂的活性和选择性 ,在所研究的含Ni催化剂上,CO2加氢反应经历了生成双齿表面吸附中间物的过程。%The surface structure of Cu-Ni bimetallic catalysts and its variation with diff erent treatment conditions were studied by XPS techique.The effect of the chemi cal state of Ni before the impregnation of Cu in catalyst preparation on the sur f ace structure and its variation were also investigated.It is found that Cu atom approaches the surface of Al2O3 when it is supported.Surface aluminates a re formed on the surface of the catalysts and the presence of Ni favorites the f ormation of surface aluminates.The surface content of Cu is increased when Ni e x isted in reduced form before the introduction of Cu,while the opposite is true w hen Ni existed in oxidized form before introduction of Cu.Surface reconstructio n is observed when the samples studied are reduced in H2 or treated under CO 2 hydrogenation condition.The hydrogenation of CO2 enriches the surface c ontenrt of Cu species comparing to reduction.After CO2 hydrogenation treat ment,Cu species is observed to migrate to the surface of the catalyst in the abs ence of Ni,while in the presence of Ni surface is remarkably decreased.Bidentat e CO2 adsorptive species with the two O of CO2 cooordinated to metal atom s is a possible intermediate in the hydrogenation of CO2 over Ni containing c atalyst studied.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  9. How to Determine the Core-Shell Nature in Bimetallic Catalyst Particles?

    Directory of Open Access Journals (Sweden)

    Emma Westsson

    2014-11-01

    Full Text Available Nanometer-sized materials have significantly different chemical and physical properties compared to bulk material. However, these properties do not only depend on the elemental composition but also on the structure, shape, size and arrangement. Hence, it is not only of great importance to develop synthesis routes that enable control over the final structure but also characterization strategies that verify the exact nature of the nanoparticles obtained. Here, we consider the verification of contemporary synthesis strategies for the preparation of bimetallic core-shell particles in particular in relation to potential particle structures, such as partial absence of core, alloying and raspberry-like surface. It is discussed what properties must be investigated in order to fully confirm a covering, pin-hole free shell and which characterization techniques can provide such information. Not uncommonly, characterization strategies of core-shell particles rely heavily on visual imaging like transmission electron microscopy. The strengths and weaknesses of various techniques based on scattering, diffraction, transmission and absorption for investigating core-shell particles are discussed and, in particular, cases where structural ambiguities still remain will be highlighted. Our main conclusion is that for particles with extremely thin or mono-layered shells—i.e., structures outside the limitation of most imaging techniques—other strategies, not involving spectroscopy or imaging, are to be employed. We will provide a specific example of Fe-Pt core-shell particles prepared in bicontinuous microemulsion and point out the difficulties that arise in the characterization process of such particles.

  10. 常压下Pt-Bi双金属催化剂上甘油选择性氧化%Glycerol Oxidation with Oxygen over Bimetallic Pt-Bi Catalysts under Atmospheric Pressure

    Institute of Scientific and Technical Information of China (English)

    梁丹; 崔世玉; 高静; 王军华; 陈平; 侯昭胤

    2011-01-01

    制备了一系列活性碳(AC)负载的Pt-Bi双金属催化剂,考察了催化剂中Bi含量对其催化甘油选择性氧化反应性能的影响.结果表明,适量Bi的添加可以改善催化剂中Pt的氧化还原性能,从而有利于催化剂活性的提高和二羟基丙酮(DIHA)产物的生成.当Bi的含量为5%时,该催化剂的活性最高,甘油转化率和DIHA选择性分别达到91.5%和49.0%.表征结果显示,Pt-Bi颗粒的平均粒径为3.8 nm,且高度分散在催化剂表面,这是该催化剂具有较高活性的主要原因.%A series of bimetallic Pt-Bi catalysts with a constant platinum content of 5.0 wt% and a varied bismuth content (3.0-7.0 wt%)supported on active carbon were prepared and used for glycerol oxidation with oxygen under atmospheric pressure.The bimetallic Pt-Bi/C was efficient for the selective oxidation of glycerol to dihydroxyacetone (DIHA) and the selectivity for DIHA reached 49.0% at a 91.5%conversion of glycerol over the 5%Pt-5%Bi/C catalyst.X-ray diffraction and transmission electron microscopy analysis revealed that the specially configured Pt-Bi nanoparticles in 5%Pt-5%Bi/C were highly dispersed (3.8 nm) over the active carbon support,which is proposed to contribute to the improved performance.

  11. Mono- and Bimetallic Ruthenium—Arene Catalysts for Olefin Metathesis: A Survey

    Science.gov (United States)

    Borguet, Yannick; Sauvage, Xavier; Demonceau, Albert; Delaude, Lionel

    In this chapter, we summarize the main achievements of our group toward the development of easily accessible, highly efficient ruthenium—arene catalyst precursors for olefin metathesis. Major advances in this field are presented chronologically, with an emphasis on catalyst design and mechanistic details. The first part of this survey focuses on monometallic complexes with the general formula RuCl2(p-cymene)(L), where L is a phosphine or N-heterocyclic carbene ancillary ligand. In the second part, we disclose recent developments in the synthesis and catalytic applications of homobimetallic ruthenium—arene complexes of generic formula (p-cymene)Ru(μ-Cl)3RuCl(η2-C2H4)(L) and their derivatives resulting from the substitution of the labile ethylene moiety with vinylidene, allenylidene, or indenylidene units

  12. Low-Temperature 1,3-Butadiene Hydrogenation over Supported Pt/3d/gamma-Al2O3 Bimetallic Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Lonergan, William W; Xing, X; Zheng, Renyang; Qi, Suitao; Huang, B; Chen, Jingguang

    2011-02-02

    Low-temperature 1,3-butadiene hydrogenation is used as a probe reaction to investigate the hydrogenation activity over several γ-Al{sub 2}O{sub 3} supported Pt/3d (3d = Co, Ni, Cu) bimetallic catalysts. Batch and flow reactor studies are employed to quantify the kinetic activity and steady-state conversion, respectively, of each catalyst. Transmission electron microscopy (TEM) is utilized to characterize particle sizes and extended X-ray absorption fine structure (EXAFS) measurements are performed to verify the Pt–3d bimetallic bond formation. Pulse carbon monoxide chemisorption measurements are also performed to characterize the number of active sites. Additionally, density functional theory (DFT) calculations are included to determine the binding energies of 1,3-butadiene and atomic hydrogen on the corresponding model surfaces. The binding energies of the adsorbates are found to correlate with the hydrogenation activity, allowing for use of such correlation to potentially predict hydrogenation catalysts with enhanced activity based on the binding energies of the adsorbates of interest.

  13. Catalyst dispersion and activity under conditions of temperature- staged liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1991-09-01

    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of the catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation. Liquefaction experiments of solvent-treated and untreated Blind Canyon (DECS-6) and Texas lignite (DECS-1) have been performed using ammonium tetrathiomolybdate (ATTM) and bis (dicarbonylcyclopentadienyl) iron (CPI) as catalyst precursors using temperature-staged conditions (275{degrees}C, 30 min; 425{degrees}C, 30 min). Solid state {sup 13}C NMR analysis was carried out for each coal and for selected residues. 12 refs., 14 figs., 9 tabs.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  15. Preparation of Pt–Ru bimetallic catalyst supported on carbon nanotubes

    Indian Academy of Sciences (India)

    B Rajesh; K Ravindranathan Thampi; J -M Bonard; B Viswanathan

    2000-10-01

    The template carbonization of polyphenyl acetylene yields hollow, uniform cylindrical carbon nanotubes with outer diameter almost equal to pore diameter of the template used. High resolution transmission electron microscopic investigation reveals that Pt–Ru nanoparticles are highly dispersed inside the tube with an average particle size of 1.7 nm.

  16. Deep Hydrodesulfurization of Diesel Fuel over Diatomite-dispersed NiMoW Sulifde Catalyst

    Institute of Scientific and Technical Information of China (English)

    Liu Di; Liu Chenguang

    2013-01-01

    Diatomite-dispersed NiMoW catalyst was prepared and characterized,and the activity of catalyst samples was tested during the HDS reaction of FCC diesel. Sulfur compounds in the feedstock and the hydrogenated products obtained over different catalysts were determined by GC-PFPD. The test results showed that the diatomite-dispersed NiMoW catalyst had high hydrodesulfurization activity for FCC diesel, which could be contributed to the excellent hydrogenation perfor-mance of the said catalyst. Characterization of catalyst by TEM and XRD indicated that the diatomite-dispersed NiMoW catalyst possessed higher layer stacking, larger curvature of MoS2 or WS2, and segregated Ni3S2 crystals relative to the sup-ported catalyst. This kind of structure leads to high hydrogenation activity of the diatomite-dispersed NiMoW catalyst.

  17. SURFACE-MODIFIED COALS FOR ENHANCED CATALYST DISPERSION AND LIQUEFACTION

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Yaw D. Yeboah

    1999-09-01

    This is the final report of the Department of Energy Sponsored project DE-FGF22-95PC95229 entitled, surface modified coals for enhanced catalyst dispersion and liquefaction. The aims of the study were to enhance catalyst loading and dispersion in coal for improved liquefaction by preadsorption of surfactants and catalysts on the coal and to train and educate minority scientists in catalysts and separation science. Illinois No. 6 Coal (DEC-24) was selected for the study. The surfactants investigated included dodecyl dimethyl ethyl ammonium bromide (DDAB), a cationic surfactant, sodium dodecyl sulfate, an anionic surfactant, and Triton x-100, a neutral surfactant. Ammonium molybdate tetrahydrate was used as the molybdenum catalyst precursor. Zeta potential, BET, FTIR, AFM, UV-Vis and luminescence intensity measurements were undertaken to assess the surface properties and the liquefaction activities of the coal. The parent coal had a net negative surface charge over the pH range 2-12. However, in the presence of DDAB the negativity of the surface charge decreased. At higher concentrations of DDAB, a positive surface charge resulted. In contrast to the effect of DDAB, the zeta potential of the coal became more negative than the parent coal in the presence of SDS. Adsorption of Triton reduced the net negative charge density of the coal samples. The measured surface area of the coal surface was about 30 m{sup 2}/g compared to 77m{sup 2}/g after being washed with deionized water. Addition of the surfactants decreased the surface area of the samples. Adsorption of the molybdenum catalyst increased the surface area of the coal sample. The adsorption of molybdenum on the coal was significantly promoted by preadsorption of DDAB and SDS. Molybdenum adsorption showed that, over a wide range of concentrations and pH values, the DDAB treated coal adsorbed a higher amount of molybdenum than the samples treated with SDS. The infrared spectroscopy (FTIR) and the atomic force

  18. Effects of the ratio of Fe to Co over Fe-Co/SiO2 bimetallic catalysts on their catalytic performance for Fischer-Tropsch synthesis

    Institute of Scientific and Technical Information of China (English)

    Xiangdong Ma; Qiwen Sun; Weiyong Ying; Dingye Fang

    2009-01-01

    The Fe-Co/SiO2 bimetallic catalysts with different ratios of Fe to Co were prepared by aqueous incipient wetness impregnation. The catalysts of 10%Fe:0%Co/SiO2, 10%Fe:6%Co/SiO2, 10%Fe:2%Co/SiO2, 10%Fe: 10%Co/SiO2, 6%Fe: 10%Co/SiO2, 2%Fe: 10%Co/SiO2 and 0%Fe: 10%Co/SiO2 by mass were tested in a fixed reactor by the Fischer-Tropsch synthesis. Activity and hydrocarbon distribution were found to be determined by the ratio of iron to cobalt of the catalysts. Higher iron content inhibited the activity, whereas higher cobalt content enhanced the activity of the Fe-Co/SiO2 catalysts. On the other hand, for the catalysts of 10%Fe:6%Co/SiO2, 10%Fe: 10%Co/SiO2, 6%Fe: 10%Co/SiO2, and 2%Fe: 10%Co/SiO2, the total C2-C4 fraction increased (from 10.65% to 26.78%) and C5+ fraction decreased (from 75.75% to 57.63%) at 523 K. Temperature programmed reduction revealed that the addition of cobalt enhanced the reducibility of the Fe-Co/SiO2 catalyst. Metal oxides were present in those catalysts as shown by XRD. The Fe-Co alloy phase was found in the 2%Fe: 10%Co/SiO2, 6%Fe: 10%Co/SiO2, 10%Fe:10%Co/SiO2, 10%Fe:6%Co/SiO2 catalysts and their crystals were perfect.

  19. A structure investigation of Pt-Co bimetallic catalysts fabricated by mechanical alloying

    Energy Technology Data Exchange (ETDEWEB)

    Lucariello, Marialaura; Penazzi, Nerino [Dipartimento di Scienza dei Materiali e Ingegneria Chimica, Politecnico di Torino, C.so Duca Abruzzi n. 24, I-10129 Torino (Italy); Arca, Elisabetta; Mulas, Gabriele [Dipartimento di Chimica, Universita di Sassari, Via Vienna n. 2, I-07100 Sassari (Italy); Enzo, Stefano [Dipartimento di Chimica, Universita di Sassari, Via Vienna n. 2, I-07100 Sassari (Italy)], E-mail: enzo@uniss.it

    2009-03-15

    Three Pt-Co mixtures of composition Pt{sub 25}Co{sub 75}, Pt{sub 50}Co{sub 50} and Pt{sub 75}Co{sub 25} respectively, were synthesized using the high-energy ball milling technique of the elemental powders with a view to prepare catalysts for fuel cells. The kinetics of phase evolution, their structure and average microstructure properties were quantitatively investigated by X-ray powder diffraction with the Rietveld method. The results show that the ball milling technique is able to produce Pt-Co solid solutions soon after few minutes of mechanical treatment. Of the two polymorphs of cobalt the fcc allotrope appears to be involved preferentially in the early stage of alloying reaction with fcc platinum. For the three compositions, a sigmoidal equation based on an interdiffusion-controlled mechanism satisfactorily accounts for the evolution of the solid solution as a function of mechanical treatment time. A characteristic reaction time of 3-6 h is observed for the solid state transformation reaction with the milling conditions adopted in our reactor. In the case of the Pt{sub 25}Co{sub 75} composition, a competitive-consecutive reaction is observed. Lattice parameters of the solid solutions after extended times of milling and related atomic volumes turn out to be slightly above the values ideally predicted on the basis of the Vegard's law. For the Pt{sub 75}Co{sub 25} composition the average crystallite size is reduced down to ca. 150 A after 12 h when the lattice microstrain is also at a maximum, but further mechanical treatment increases the average crystal size value and to decrease the strain. Similar results are found for equiatomic and Co-rich compositions. Annealing of the alloyed equiatomic powders promotes a cubic-to-tetragonal transformation which is already operative at 600 deg. C. In fact, after this treatment two tetragonal phases are observed. Further thermal treatment and annealing at 700 deg. C induces peak sharpening of the diffraction patterns

  20. Passivation of bimetallic catalysts used in water treatment: prevention and reactivation.

    Science.gov (United States)

    Chen, Jianming; Gillham, Robert W; Gui, Lai

    2013-01-01

    With respect to degradation rates and the range in contaminants treated, bimetals such as Ni-Fe or Pd-Fe generally outperform unamended granular iron. However, the catalytic enhancement is generally short-lived, lasting from a few days to months. To take advantage of the significant benefits of bimetals, this study aims at developing an effective method for the rejuvenation of passivated bimetals and alternatively, the prevention of rapid reactivity loss of bimetals. Because the most likely cause of Ni-Fe and Pd-Fe passivation is the deposition of iron oxide films over the catalyst sites, it is hypothesized that removal of the iron oxide films will restore the lost reactivity or avoiding the deposition of iron oxide films will prevent passivation. Two organic ligands (ethylenediaminetetraacetic acid (EDTA), and [s,s]-ethylenediaminedisuccinate acid ([s,s]-EDDS)) and two acids (citric acid and sulphuric acid) were tested as possible chemical reagents for both passivation rejuvenation and prevention. Trichloroethene (TCE) and Ni-Fe were chosen as probes for chlorinated solvents and bimetals respectively. The test was carried out using small glass columns packed with Ni-Fe. TCE solution containing a single reagent at various concentrations was pumped through the Ni-Fe columns with a residence time in the Ni-Fe of about 6.6 min. TCE concentrations in the influent and effluent were measured to evaluate the performance of each chemical reagent. The results show that (i) for passivated Ni-Fe, flushing with a low concentration of acid or ligand solution without mechanical mixing can fully restore the lost reactivity; and (ii) for passivation prevention, adding a small amount of a ligand or an acid to the feed solution can successfully prevent or at least substantially reduce Ni-Fe passivation. All four chemicals tested are effective in both rejuvenation and prevention, but sulphuric acid and citric acid are considered to be the most practical reagents due to their

  1. Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst

    Science.gov (United States)

    Choi, Chang Hyuck; Kim, Minho; Kwon, Han Chang; Cho, Sung June; Yun, Seongho; Kim, Hee-Tak; Mayrhofer, Karl J. J.; Kim, Hyungjun; Choi, Minkee

    2016-01-01

    Maximum atom efficiency as well as distinct chemoselectivity is expected for electrocatalysis on atomically dispersed (or single site) metal centres, but its realization remains challenging so far, because carbon, as the most widely used electrocatalyst support, cannot effectively stabilize them. Here we report that a sulfur-doped zeolite-templated carbon, simultaneously exhibiting large sulfur content (17 wt% S), as well as a unique carbon structure (that is, highly curved three-dimensional networks of graphene nanoribbons), can stabilize a relatively high loading of platinum (5 wt%) in the form of highly dispersed species including site isolated atoms. In the oxygen reduction reaction, this catalyst does not follow a conventional four-electron pathway producing H2O, but selectively produces H2O2 even over extended times without significant degradation of the activity. Thus, this approach constitutes a potentially promising route for producing important fine chemical H2O2, and also offers opportunities for tuning the selectivity of other electrochemical reactions on various metal catalysts. PMID:26952517

  2. Synthesis of coal-derived single-walled carbon nanotube from coal by varying the ratio of Zr/Ni as bimetallic catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Kumar, Rajesh, E-mail: rajeshbhu1@gmail.com [Banaras Hindu University, Nanoscience and Nanotechnology Unit, Department of Physics (India); Singh, Rajesh Kumar, E-mail: rksbhu@gmail.com [Indian Institute of Technology (Banaras Hindu University), Department of Applied Physics (India); Ghosh, A. K.; Sen, Raja; Srivastava, S. K. [Central Institute of Mining and Fuel Research (India); Tiwari, R. S.; Srivastava, O. N. [Banaras Hindu University, Nanoscience and Nanotechnology Unit, Department of Physics (India)

    2013-01-15

    In this paper coal, source has been used in place of graphite for synthesis of single-walled carbon nanotubes (SWCNTs) with new Zr/Ni bimetallic catalyst. Using coal as starting material to produce the high-value-added SWCNTs is an economically competent route. SWCNTs have been synthesized by the electric arc discharge method using the so-called heterogeneous annealed coal anode filled with Zr and Ni catalyst. SWCNTs have been synthesized using annealed coal rod. The SWCNTs bundles synthesized generally have diameters of 4-10 nm. Most of those produced with Zr/Ni as the catalyst has a diameter ranging from 2.0 to 1.0 nm. The as-synthesized SWCNTs have been characterized employing XRD, HRTEM, EDX, Raman spectroscopy, and FTIR. It has been found that the change of the ratio of Zr and Ni concentration (wt%) in the catalyst affects the yield of SWCNTs. However, the purity of SWCNTs is very sensitive to the concentration of Zr. An optimal range of Zr/Ni compositions for synthesis of SWCNTs with relatively high purity and yield is obtained at specific concentration of 3:1.

  3. Advanced liquefaction using coal swelling and catalyst dispersion techniques

    Energy Technology Data Exchange (ETDEWEB)

    Curtis, C.W. (Auburn Univ., AL (United States)); Gutterman, C. (Foster Wheeler Development Corp., Livingston, NJ (United States)); Chander, S. (Pennsylvania State Univ., University Park, PA (United States))

    1992-08-26

    Research in this project centers upon developing a new approach to the direct liquefaction of coal to produce an all-distillate product slate at a sizable cost reduction over current technology. The approach integrates all aspects of the coal liquefaction process including coal selection, pretreatment, coal swelling with catalyst impregnation, coal liquefaction experimentation, product recovery with characterization, alternate bottoms processing, and a technical assessment including an economic evaluation. The project is being carried out under contract to the United States Department of Energy. On May 28, 1992, the Department of Energy authorized starting the experimental aspects of this projects; therefore, experimentation at Amoco started late in this quarterly report period. Research contracts with Auburn University, Pennsylvania State University, and Foster Wheeler Development Corporation were signed during June, 1992, so their work was just getting underway. Their work will be summarized in future quarterly reports. A set of coal samples were sent to Hazen Research for beneficiation. The samples were received and have been analyzed. The literature search covering coal swelling has been up-dated, and preliminary coal swelling experiments were carried out. Further swelling experimentation is underway. An up-date of the literature on the liquefaction of coal using dispersed catalysts is nearing completion; it will be included in the next quarterly report.

  4. Heterogenized Bimetallic Pd-Pt-Fe3O4 Nanoflakes as Extremely Robust, Magnetically Recyclable Catalysts for Chemoselective Nitroarene Reduction.

    Science.gov (United States)

    Byun, Sangmoon; Song, Yeami; Kim, B Moon

    2016-06-15

    A very simple synthesis of bimetallic Pd-Pt-Fe3O4 nanoflake-shaped alloy nanoparticles (NPs) for cascade catalytic reactions such as dehydrogenation of ammonia-borane (AB) followed by the reduction of nitro compounds (R-NO2) to anilines or alkylamines (R-NH2) in methanol at ambient temperature is described. The Pd-Pt-Fe3O4 NPs were easily prepared via a solution phase hydrothermal method involving the simple one-pot coreduction of potassium tetrachloroplatinate (II) and palladium chloride (II) in polyvinylpyrrolidone with subsequent deposition on commercially available Fe3O4 NPs. The bimetallic Pd-Pt alloy NPs decorated on Fe3O4 NPs provide a unique synergistic effect for the catalysis of cascade dehydrogenation/reduction. Various nitroarene derivatives were reduced to anilines with very specific chemoselectivity in the presence of other reducible functional groups. The bimetallic Pd-Pt-Fe3O4 NPs provide a unique synergistic effect for the catalysis of cascade dehydrogenation/reduction. The nitro reduction proceeded in 5 min with nearly quantitative conversions and yields. Furthermore, the magnetically recyclable nanocatalysts were readily separated using an external magnet and reused up to 250 times without any loss of catalytic activity. A larger scale (10 mmol) reaction was also successfully performed with >99% yield. This efficient, recyclable Pd-Pt-Fe3O4 NPs system can therefore be repetitively utilized for the reduction of various nitro-containing compounds. PMID:27191706

  5. Dendritic Pt-Cu bimetallic nanocrystals with a high electrocatalytic activity toward methanol oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Jintao; Ma Jizhen [Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576 (Singapore); Wan Yong [Institute of Multifunctional Materials (IMM), Laboratory of New Fiber Materials and Modern Textile, Growing Base for State Key Laboratory, Qingdao University, Qingdao 266071 (China); Jiang Jianwen [Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576 (Singapore); Zhao, X.S., E-mail: george.zhao@uq.edu.au [Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore 117576 (Singapore); Institute of Multifunctional Materials (IMM), Laboratory of New Fiber Materials and Modern Textile, Growing Base for State Key Laboratory, Qingdao University, Qingdao 266071 (China)

    2012-02-15

    Highlights: Black-Right-Pointing-Pointer Dendritic Pt-Cu bimetallic nanocrystals were synthesized by one-step aqueous-phase reduction. Black-Right-Pointing-Pointer The formation process of dendritic Pt-Cu bimetallic nanocrystals can be carried out under mild conditions. Black-Right-Pointing-Pointer The dendritic Pt-Cu bimetallic nanocrystals exhibited a higher catalytic activity toward the electro-oxidation of methanol than commercial Pt/C catalysts. Black-Right-Pointing-Pointer The new findings are of fundamental importance to the development of high-performance electrocatalysts for direct methanol fuel cell. - Abstract: Dendritic Pt-Cu bimetallic nanocrystals were synthesized by one-step aqueous-phase reduction of H{sub 2}PtCl{sub 6} and CuCl{sub 2} at a mild temperature (60 Degree-Sign C). The morphology and composition of the dendritic Pt-Cu nanocrystals were characterized by means of high-resolution transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and energy dispersive X-ray spectrometer. The electrochemical properties were characterized by the cyclic voltammetry technique. It was found that the dendritic Pt-Cu bimetallic nanocrystals exhibited a higher catalytic activity toward the electro-oxidation of methanol than commercial Pt/C catalyst The enhanced catalytic activity would be contributed to the unique dendritic structure and the formation of Pt-Cu alloy nanocrystals.

  6. Comparison of P-containing {gamma}-Al{sub 2}O{sub 3} supported Ni-Mo bimetallic carbide, nitride and sulfide catalysts for HDN and HDS of gas oils derived from Athabasca bitumen

    Energy Technology Data Exchange (ETDEWEB)

    Sundaramurthy, V.; Dalai, A.K. [Catalysis and Chemical Reaction Engineering Laboratories, Department of Chemical Engineering, University of Saskatchewan, Saskatoon, SK (Canada); Adjaye, J. [Syncrude Edmonton Research Centre, Edmonton, AB (Canada)

    2006-09-01

    Phosphorus containing {gamma}-Al{sub 2}O{sub 3} supported bimetallic Ni-Mo carbide, nitride and sulfide catalysts have been synthesized from an oxide precursor containing 12.73wt.% Mo, 2.54wt.% Ni and 2.38wt.% P and characterized by elemental analysis, pulsed CO chemisorption, surface area measurements, X-ray diffraction, temperature-programmed reduction and DRIFT spectroscopy of CO adsorption. DRIFT spectroscopy of adsorbed CO on activated catalysts showed that carbide and nitride catalysts have surface exposed sites of Mo{sup o+} (0bimetallic Ni-Mo carbide, nitride and sulfide catalysts were compared against commercial Ni-Mo/Al{sub 2}O{sub 3} catalyst in a trickle bed reactor using light gas oil and heavy gas oil derived from Athabasca bitumen in the temperature range 340-370 and 375-400{sup o}C respectively at 8.8MPa. The gradual transformation of Ni-Mo carbide and nitride phases into Ni-Mo sulfide phases was observed during precoking period, and the formed Ni-Mo sulfide phases enhanced the HDN and HDS activities of carbide and nitride catalysts. The {gamma}-Al{sub 2}O{sub 3} supported Ni-Mo bimetallic sulfide catalyst was found to be more active for HDN and HDS of light gas oil and heavy gas oil than the corresponding carbide and nitride catalysts on the basis of unit weight. (author)

  7. Surface structure and reaction property of CuCl2-PdCl2 bimetallic catalyst in methanol oxycarbonylation: A DFT approach

    International Nuclear Information System (INIS)

    Surface structure of CuCl2-PdCl2 bimetallic catalyst (Wacker-type catalyst) was built employing density functional theory (DFT) calculations, and the reaction mechanism of methanol oxycarbonylation over the CuCl2-PdCl2 surfaces was also investigated. On the CuCl2-PdCl2 surface, the active site for methanol oxidation was confirmed as Cu-Cl-Cu (Pd). Comparing with pure CuCl2 surface, the introduction of Pd atom causes the electron repopulation on the surface and lowers the energy barrier for methanol oxidation, but the number of the active site decreases with the increasing of Pd doping volume. Agreed with previous experimental results, the Pd site is most favorable for the CO insertion, indicated by the lowest activation barrier for the formation of COOCH3 on Pd atom. The lowest energy barrier for the formation of DMC appears when COOCH3 species adsorbed on Pd atom and methoxyl adsorbed on Cu atoms, which is 0.42 eV. Finally, the reconstruction of the unsaturated surface is a spontaneous and exothermic process. Comparing with other surfaces, the rate-limiting step, methanol oxidation, on CuCl2-PdCl2 surface with Pd/Cu = 1:17 has the lowest energy barrier, which is agreed with the experimental observation that PdCl2-CuCl2 catalyst with Pd/Cu = 1:20 has the favorable activity. The adsorbed methoxyl will further lower the activation barrier of methanol oxidation, which is agreed with experimental observation that the Wacker-type catalysts have an induction period in the methanol oxidative carbonylation system.

  8. Facile Fabrication of Composition-Tuned Ru-Ni Bimetallics in Ordered Mesoporous Carbon for Levulinic Acid Hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Ying; Gao, Guang; Zhang, Xin; Li, Fuwei [ChinaU - Petroleum; (Chinese Aca. Sci.)

    2016-02-04

    Bimetallic catalysts are of great importance due to their unique catalytic properties. However, their conventional synthesis requires tedious multistep procedures and prolonged synthetic time, and the resulting bimetallics usually disperse unevenly and show poor stability. It is challenging to develop a facile and step-economic synthetic methodology for highly efficient bimetallic catalysts. In this study, we report an elegant metal complex-involved multicomponent assembly route to highly efficient Ru–Ni bimetallics in ordered mesoporous carbons (OMC). The fabrication of composition-tuned Ru–Ni bimetallics in OMC (RuxNi1–x–OMC, x = 0.5–0.9) was facilely realized via in situ construction of CTAB-directed cubic Ia3d chitosan-ruthenium–nickel–silica mesophase before pyrolysis and silica removal. The resulting RuxNi1–x–OMC materials are in-depth characterized with X-ray diffraction, N2 adsorption–desorption, transmission electron microscopy, infrared spectrum, and X-ray absorption fine structure. This facile fabrication method renders homogeneously dispersed Ru–Ni bimetallics embedded in the mesoporous carbonaceous framework and creates a highly active and stable Ru0.9Ni0.1–OMC catalyst for the hydrogenation of levulinic acid (LA) to prepare γ-valerolactone (GVL), a biomass-derived platform molecule with wide application in the preparation of renewable chemicals and liquid transportation fuels. A high TOF (>2000 h–1) was obtained, and the Ru0.9Ni0.1–OMC catalyst could be used at least 15 times without obvious loss of its catalytic performance.

  9. One step electrochemical synthesis of bimetallic PdAu supported on nafion–graphene ribbon film for ethanol electrooxidation

    Energy Technology Data Exchange (ETDEWEB)

    Shendage, Suresh S., E-mail: sureshsshendage@gmail.com; Singh, Abilash S.; Nagarkar, Jayashree M., E-mail: jm.nagarkar@ictmumbai.edu.in

    2015-10-15

    Highlights: • Electrochemical deposition of bimetallic PdAu NPs. • Highly loaded PdAu NPs are obtained. • Nafion–graphene supported PdAu NPs shows good activity for ethanol electrooxidation. - Abstract: A nafion–graphene ribbon (Nf–GR) supported bimetallic PdAu nanoparticles (PdAu/Nf–GR) catalyst was prepared by electrochemical codeposition of Pd and Au at constant potential. The prepared catalyst was characterized by scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDAX), transmission electron microscopy (TEM) and X-ray diffraction analysis (XRD). The average particle size of PdAu nanoparticles (NPs) determined from XRD was 3.5 nm. The electrocatalytic activity of the PdAu/Nf–GR catalyst was examined by cyclic voltametry. It was observed that the as prepared catalyst showed efficient activity and good stability for ethanol electrooxidation in alkaline medium.

  10. Fabrication of PdCo Bimetallic Nanoparticles Anchored on Three-Dimensional Ordered N-Doped Porous Carbon as an Efficient Catalyst for Oxygen Reduction Reaction.

    Science.gov (United States)

    Xue, Hairong; Tang, Jing; Gong, Hao; Guo, Hu; Fan, Xiaoli; Wang, Tao; He, Jianping; Yamauchi, Yusuke

    2016-08-17

    PdCo bimetallic nanoparticles (NPs) anchored on three-dimensional (3D) ordered N-doped porous carbon (PdCo/NPC) were fabricated by an in situ synthesis. Within this composite, N-doped porous carbon (NPC) with an ordered mesoporous structure possesses a high surface area (659.6 m(2) g(-1)), which can facilitate electrolyte infiltration. NPC also acts as a perfect 3D conductive network, guaranteeing fast electron transport. In addition, homogeneously distributed PdCo alloy NPs (∼15 nm) combined with the doping of the N element can significantly improve the electrocatalytic activity for the oxygen reduction reaction (ORR). Due to the structural and material superiority, although the weight percentage of PdCo NPs (∼8 wt%) is much smaller than that of commercial Pt/C (20 wt%), the PdCo/NPC catalyst exhibits similar excellent electrocatalytic activity; however, its superior durability and methanol-tolerance ability of the ORR are as great as those of commercial Pt/C in alkaline media. PMID:27441490

  11. Uninterrupted galvanic reaction for scalable and rapid synthesis of metallic and bimetallic sponges/dendrites as efficient catalysts for 4-nitrophenol reduction.

    Science.gov (United States)

    Barman, Barun Kumar; Nanda, Karuna Kar

    2015-03-01

    Here, we demonstrate an uninterrupted galvanic replacement reaction (GRR) for the synthesis of metallic (Ag, Cu and Sn) and bimetallic (Cu-M, M=Ag, Au, Pt and Pd) sponges/dendrites by sacrificing the low reduction potential metals (Mg in our case) in acidic medium. The acidic medium prevents the oxide formation on Mg surface and facilitates the uninterrupted reaction. The morphology of dendritic/spongy structures is controlled by the volume of acid used for this reaction. The growth mechanism of the spongy/dendritic microstructures is explained by diffusion-limited aggregate model (DLA), which is also largely affected by the volume of acid. The significance of this method is that the yield can be easily predicted, which is a major challenge for the commercialization of the products. Furthermore, the synthesis is complete in 1-2 minutes at room temperature. We show that the sponges/dendrites efficiently act as catalysts to reduce 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) using NaBH4-a widely studied conversion process. PMID:25628256

  12. Different dispersions of group II catalysts over SBA 15 and MCM-41: Effects on transesterification reactivity

    OpenAIRE

    Sullivan, James A; Sherry, Linda

    2015-01-01

    Activities of CaO catalysts on SBA-15 and MCM-41 have been compared in transesterification and SBA-15 supported samples invariably more active than those on MCM-41. Increased activity is not due to diffusional effects (as measured using substrates of differing size) but rather to increased dispersion of CaO on SBA-15 (as measured using NOx TPD). The effect, i.e. increased reactivity of SBA-15 supported catalysts being related to increased dispersion, is also noted in supported BaO catalysts w...

  13. Sulfided heterogeneous, bimetallic RuMo catalysts derived from mixtures of Ru{sub 3}(CO){sub 12} (or RuCl{sub 3}) and a molybdenum heteropolyanion. The reactions of ethanol with tetrahydroquinoline

    Energy Technology Data Exchange (ETDEWEB)

    Koo, Sang-Man; Ryan, D.; Laine, R.M.

    1992-09-01

    Efforts have been made to develop Ru/Mo bimetallic catalyst systems for hydrodenitrogenation (HDN) of tetrahydroquinoline (THQ)- In the course of these studies, it was discovered that in ethanol, under H{sub 2} and in the presence Of CS2, Precatalyst solutions containing Ru [as Ru{sub 3} (CO){sub 12} or RuCl{sub 3}] and Mo [as the H{sub 3}PMO{sub 12}0{sub 40} heteropolyanion (HPA)] decompose to form bimetallic, sulfided particles. Particle diameters run from 0.1 to 5 {mu}m depending on the rate of stirring. Catalyst particles with sizes ranging from 0.1--1 {mu}m can be prepared reproducibly. BET measured surface areas for these size particles ranged from 2 to 20 m2/g. These sulfided particles were found to catalyze, at temperatures of 200--250{degrees}C and hydrogen pressures of 200--1000 psig H{sub 2}, the N-ethylation of THQ to form NEt-THQ; rather than the formation of propylcyclohexane or propylbenzene, reaction products expected for HDN of THQ. Monometallic heterogeneous catalysts prepared from the individual precatalyst complexes, under identical conditions, show minimal activity for N-ethylation by comparison with the bimetallic catalyst. In the absence of H{sub 2}, the reaction proceeds such that THQ is converted to Q, N-EtTHQ, N-C{sub 6}H{sub 9}-THQ, and N-C{sub 6}H{sub 13}-THQ. The latter products appear to arise via acetaldehyde, formed as an intermediate by dehydrogenation of ethanol. Acetaldehyde either condenses with THQ to form N-Et-THQ, or self condenses (aldol condensation) prior to reaction with THQ thereby giving higher homolog alkylation products.

  14. Sulfided heterogeneous, bimetallic RuMo catalysts derived from mixtures of Ru sub 3 (CO) sub 12 (or RuCl sub 3 ) and a molybdenum heteropolyanion. The reactions of ethanol with tetrahydroquinoline

    Energy Technology Data Exchange (ETDEWEB)

    Koo, Sang-Man; Ryan, D.; Laine, R.M.

    1992-01-01

    Efforts have been made to develop Ru/Mo bimetallic catalyst systems for hydrodenitrogenation (HDN) of tetrahydroquinoline (THQ)- In the course of these studies, it was discovered that in ethanol, under H{sub 2} and in the presence Of CS2, Precatalyst solutions containing Ru (as Ru{sub 3} (CO){sub 12} or RuCl{sub 3}) and Mo (as the H{sub 3}PMO{sub 12}0{sub 40} heteropolyanion (HPA)) decompose to form bimetallic, sulfided particles. Particle diameters run from 0.1 to 5 {mu}m depending on the rate of stirring. Catalyst particles with sizes ranging from 0.1--1 {mu}m can be prepared reproducibly. BET measured surface areas for these size particles ranged from 2 to 20 m2/g. These sulfided particles were found to catalyze, at temperatures of 200--250{degrees}C and hydrogen pressures of 200--1000 psig H{sub 2}, the N-ethylation of THQ to form NEt-THQ; rather than the formation of propylcyclohexane or propylbenzene, reaction products expected for HDN of THQ. Monometallic heterogeneous catalysts prepared from the individual precatalyst complexes, under identical conditions, show minimal activity for N-ethylation by comparison with the bimetallic catalyst. In the absence of H{sub 2}, the reaction proceeds such that THQ is converted to Q, N-EtTHQ, N-C{sub 6}H{sub 9}-THQ, and N-C{sub 6}H{sub 13}-THQ. The latter products appear to arise via acetaldehyde, formed as an intermediate by dehydrogenation of ethanol. Acetaldehyde either condenses with THQ to form N-Et-THQ, or self condenses (aldol condensation) prior to reaction with THQ thereby giving higher homolog alkylation products.

  15. Chirality specific and spatially uniform synthesis of single-walled carbon nanotubes from a sputtered Co-W bimetallic catalyst

    Science.gov (United States)

    An, Hua; Kumamoto, Akihito; Takezaki, Hiroki; Ohyama, Shinnosuke; Qian, Yang; Inoue, Taiki; Ikuhara, Yuichi; Chiashi, Shohei; Xiang, Rong; Maruyama, Shigeo

    2016-07-01

    Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system.Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system. Electronic supplementary information (ESI) available: Raman spectroscopy (G-band) of SWNTs grown from Co and Co-W catalyst; Kataura plot for chirality

  16. Characterization of Metal Dispersion of Some Naphtha Reforming Catalysts by Methylcyclohexane Dehydrogenation Reaction

    Directory of Open Access Journals (Sweden)

    Ameel Mohammed Rahman

    2009-01-01

    Full Text Available The dispersion of supported Pt and Pt–Ir reforming catalysts have been studied, after treatment with oxidative and reducing atmosphere. Methylcyclohexane dehydrogenation reaction in the absence of hydrogen was used as a test reaction. An attempt was made to relate the behavior of the catalysts upon subject to reaction, to the dispersion of the same type of catalysts upon treatment with similar atmosphere and temperatures which appeared in literature. The total conversion of reaction can be explained by a change in metal dispersion. Thus, methylcyclohexane dehydrogenation reaction appears to be a really “structure sensitive” reaction. The toluene yield increases as the oxidation temperature increases over the studied catalyst RG-402, RG-412, RG-422 and RG-432 respectively and reached a maximum value at 550°C. Above 550 the conversion decreases due to the effect of catalyst sintering. No significant change were observed for reduction temperature range 400-600°C for the above studied catalysts.The selectivity order for the studied catalysts and for reduction treatment experiments arranged as follows:RG-422> RG-432> RG-412> RG-402

  17. Chirality specific and spatially uniform synthesis of single-walled carbon nanotubes from a sputtered Co-W bimetallic catalyst.

    Science.gov (United States)

    An, Hua; Kumamoto, Akihito; Takezaki, Hiroki; Ohyama, Shinnosuke; Qian, Yang; Inoue, Taiki; Ikuhara, Yuichi; Chiashi, Shohei; Xiang, Rong; Maruyama, Shigeo

    2016-08-14

    Synthesis of single-walled carbon nanotubes (SWNTs) with well-defined atomic arrangements has been widely recognized in the past few decades as the biggest challenge in the SWNT community, and has become a bottleneck for the application of SWNTs in nano-electronics. Here, we report a selective synthesis of (12, 6) SWNTs with an enrichment of 50%-70% by chemical vapor deposition (CVD) using sputtered Co-W as a catalyst. This is achieved under much milder reduction and growth conditions than those in the previous report using transition-metal molecule clusters as catalyst precursors (Nature, 2014, 510, 522). Meanwhile, in-plane transmission electron microscopy unambiguously identified an intermediate structure of Co6W6C, which is strongly associated with selective growth. However, most of the W atoms disappear after a 5 min CVD growth, which implies that anchoring W may be important in this puzzling Co-W system. PMID:27412697

  18. Development of a PtSn bimetallic catalyst for direct fuel cells using bio-butanol fuel

    OpenAIRE

    Puthiyapura, V.K.; Brett, D. J. L.; Russell, A E; Lin, W.F.; Hardacre, C.

    2015-01-01

    Pt and PtSn catalysts were studied for n-butanol electro-oxidation at various temperatures. PtSn showed a higher activity towards butanol electro-oxidation compared to Pt in acidic media. The onset potential for n-butanol oxidation on PtSn is similar to 520 mV lower than that found on Pt, and significantly lower activation energy was found for PtSn compared with that for Pt.

  19. Development of a PtSn bimetallic catalyst for direct fuel cells using bio-butanol fuel.

    Science.gov (United States)

    Puthiyapura, V K; Brett, D J L; Russell, A E; Lin, W F; Hardacre, C

    2015-09-01

    Pt and PtSn catalysts were studied for n-butanol electro-oxidation at various temperatures. PtSn showed a higher activity towards butanol electro-oxidation compared to Pt in acidic media. The onset potential for n-butanol oxidation on PtSn is ∼520 mV lower than that found on Pt, and significantly lower activation energy was found for PtSn compared with that for Pt. PMID:26214283

  20. The effects of cerium doping concentration on the properties and photocatalytic activity of bimetallic Mo/Ce catalyst

    Science.gov (United States)

    Allaedini, Ghazaleh; Tasirin, Siti Masrinda; Aminayi, Payam

    2016-10-01

    In this study, the characterization and photocatalytic activity of MoO3 nanoparticles doped with various doping concentrations of cerium have been investigated. The Fourier transform infrared (FT-IR) spectra of the prepared catalysts confirmed that MoO3 particles have been successfully doped by cerium. Field emission scanning electron microscopy (FESEM) was performed to visualize the surface morphology of the obtained catalysts. The XRD patterns suggested that the crystallinity of the sample with the lowest doping concentration of 15 mol % was higher in comparison with samples of higher doping concentrations. The volume-averaged crystal sizes of the obtained catalysts were calculated to be 25, 28, and 32 nm for 15, 35, and 60 mol % samples, respectively. The photocatalytic activity along with the reaction kinetics of Ce-doped MoO3 nanoparticles have also been investigated through the dye degradation of methyl orange. The synthesized Ce-doped MoO3 particles with the lowest dopant concentration of 15 mol % exhibited the highest photocatalytic activity for methyl orange dye degradation. It was observed that photo-degradation activity decreased with an increase in the doping concentration of cerium. The predicted rate constants for samples with 15, 35, and 60 mol % doping concentrations were found to be 0.0432, 0.035, and 0.029 min-1, respectively.

  1. Science Letters: Structure relationship of nitrochlorobenzene catalytic degradation process in water over palladium-iron bimetallic catalyst

    Institute of Scientific and Technical Information of China (English)

    NIU Shao-feng; ZHOU Hong-yi; AO Xu-ping; XU Xin-hua; LOU Zhang-hua

    2006-01-01

    Two isomers of nitrochlorobenzene (o-, and p-NCB) were treated by a Pd/Fe catalyst in aqueous solutions through catalytic amination and dechlorination. Nitrochlorobenzenes are rapidly converted to form chloroanilines (CAN) first through an amination process, and then rapidly dechlorinated to become aniline (AN) and Cl-, without the involvement of any other intermediate reaction products. The amination and dechlorination reaction are believed to take place predominantly on the surface site of the Pd/Fe catalysts. The dechlorination rate of the reductive degradation of the two isomers of nitrochlorobenzene (o-, and p-NCB) in the presence of Pd/Fe as a catalyst was measured experimentally. In all cases, the reaction rate constants were found to increase with the decrease in the Gibbs free energy (correlation with the activation energy) of NCBs formation; the activation energy of each dechlorination reaction was measured to be 95.83 and 77.05 kJ/mol, respectively for o- and p-NCB. The results demonstrated that p-NCBs were reduced more easily than o-NCBs.

  2. PROPERTIES OF HIGHLY DISPERSED PALLADIUM CATALYSTS ON POLY N—VINYL—2—PYRROLIDONE

    Institute of Scientific and Technical Information of China (English)

    SUNJuntan; CHENChunfu; 等

    1992-01-01

    Four kinds of palladium catalysts dispersed on poly-N-vinyl-2-pyrrolidone were prepared by using CH3OH-NaOH,NaBH4,H2O or CH3OH-H2O as the reducing agent in the process of catalyst preparation. The catalysts were characterized by XPS,TEM,XRD and used for the hydrogenation of methyl acrylate.It was found that the valence state of palladium and distribution of palladium particles as well as the hydrogenation rate were greatly affected by the reducing agent.The best evenly dispersed palladium catalyst showing high hydrogenation activity was prepared using CH3OH-NaOH as the reducing agent.

  3. Dispersed catalysts for transforming extra heavy crude oil into transportable upgraded crude: phase identification

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, S.; Canizales, E.; Machin, I. [Gerencia Depttal de Investigacion Estrategica en Refinacion PDVSA Intevep (Venezuela); Segovia, X.; Rivas, A.; Lopez, E.; Pena, J.P.; Rojas, J.D.; Sardella, R. [Gerencia Depttal de Infraestructura y Mejoramiento en Faja Petrolifera PDVSA Intevep (Venezuela)

    2011-07-01

    A new technology to convert extra heavy crude oil into transportable upgraded crude has been developed. A water/oil emulsion composed of steam and catalyst precursors is introduced in the feed which then generates unsupported dispersed catalyst in situ under thermal decomposition. The aim of this paper is to characterize the particles. The study was conducted in a laboratory and on a pilot scale on three different vacuum residues using high resolution transmission electron microscopy and a transmission electron microscope. Results showed that the particles were formed by oxides and inorganic sulphur based in transition metals and their sizes ranged between 5 and 120 nm; in addition, good dispersion was observed. This study demonstrated that the process involved in the generation of dispersed catalyst is extremely complex and showed that further work with heavy crude oils and its residua is required to understand the mechanisms involved.

  4. Investigation on Dispersed Catalyst for Slurry Bed Hydroprocessing of Heavy Oil

    Institute of Scientific and Technical Information of China (English)

    Liu Dong; Guo Aijun; Ma Kuiju; Que Guohe

    2006-01-01

    The slurry-bed hydrocracking of Karamay VGO with water-soluble dispersed catalyst was studied and the catalyst after being separated from the reaction products was analyzed by using LRS, XRD and XPS to identify the crystal structure of the catalyst. In this paper, the catalytic functions of molybdenum, nickel and iron were studied respectively during the slurry-phase hydrocracking while using diphenylmethane as the model compound and VGO from Karamay crude as the feedstock. The test results showed that, during the slurry-phase hydrocracking of heavy oil, the metal sulfides entered into chemical reactions with the free radical intermediate H· formed on the catalyst surface. The free-radical intermediate H· formed on the catalyst surface could react with the free-radicals of big molecules and could suppress coke deposition.

  5. Catalyst dispersion and activity under conditions of temperature-staged liquefaction. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1993-02-01

    This research program involves the investigation of the use of highly dispersed catalyst precursors for the pretreatment of coals by mild hydrogenation. During the course of this effort solvent preswelling of the coal was evaluated as a means of deeply impregnating catalysts into coal, active phases of catalysts under reaction conditions were studied and the impact of these techniques were evaluated during pretreatment and temperature-staged liquefaction. Two coals, a Texas subbituminous and a Utah high volatile A bituminous, were used to examine the effects of solvent swelling pretreatment and catalyst impregnation on conversion behavior at 275{degrees}C, representative of the first, low-temperature stage in a temperature-staged liquefaction reaction. Ferrous sulfate, iron pentacarbonyl, ammonium tetrathiomolybdate, and molybdenum hexacarbonyl were used as catalyst precursors. Without swelling pretreatment, impregnation of both coals increased conversion, mainly through increased yields of preasphaltenes.

  6. Catalyst dispersion and activity under conditions of temperature-staged liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1993-02-01

    This research program involves the investigation of the use of highly dispersed catalyst precursors for the pretreatment of coals by mild hydrogenation. During the course of this effort solvent preswelling of the coal was evaluated as a means of deeply impregnating catalysts into coal, active phases of catalysts under reaction conditions were studied and the impact of these techniques were evaluated during pretreatment and temperature-staged liquefaction. Two coals, a Texas subbituminous and a Utah high volatile A bituminous, were used to examine the effects of solvent swelling pretreatment and catalyst impregnation on conversion behavior at 275[degrees]C, representative of the first, low-temperature stage in a temperature-staged liquefaction reaction. Ferrous sulfate, iron pentacarbonyl, ammonium tetrathiomolybdate, and molybdenum hexacarbonyl were used as catalyst precursors. Without swelling pretreatment, impregnation of both coals increased conversion, mainly through increased yields of preasphaltenes.

  7. Catalyst for Ammonia Oxidation

    DEFF Research Database (Denmark)

    2015-01-01

    The present invention relates to a bimetallic catalyst for ammonia oxidation, a method for producing a bimetallic catalyst for ammonia oxidation and a method for tuning the catalytic activity of a transition metal. By depositing an overlayer of less catalytic active metal onto a more catalytic...

  8. The Simple, Effective Synthesis of Highly Dispersed Pd/C and CoPd/C Heterogeneous Catalysts via Charge-Enhanced Dry Impregnation

    Directory of Open Access Journals (Sweden)

    Lawrence D’Souza

    2016-05-01

    Full Text Available Pd/C and CoPd/C heterogeneous catalysts have been synthesized by adopting Charge Enhanced Dry Impregnation (CEDI. The particles size distribution, their high metal surface-to-bulk ratios, and synthesis feasibility are unmatchable to any known noble metal bimetallic heterogeneous catalyst preparation techniques. Next generation Fuel Cells and Fischer-Tropsch catalytic processes economy will be benefited from the proposed methodology.

  9. A photoactive bimetallic framework for direct aminoformylation of nitroarenes

    Data.gov (United States)

    U.S. Environmental Protection Agency — A bimetallic catalyst, AgPd@g-C3N4, synthesized by reducing silver and palladium salts over graphitic carbon nitride (g-C3N4), enables the concerted reductive...

  10. The role of the catalysts with highly dispersed and isolated active sites in the selective oxidation of light hydrocarbons

    Institute of Scientific and Technical Information of China (English)

    WANG Hongxuan; ZHAO Zhen

    2005-01-01

    This review summarizes the role of catalysts with highly dispersed and isolated active sites (active sites: supported atoms f≤0.5 % ) in the selective oxidation of light hydrocarbons, such as methane, ethane and propane, into oxygenatesand the epoxidation of olefins. The plausible structures of the highly dispersed and isolated active species, as well as their effects on the catalytic performances are discussed. The special physico-chemical properties and the functional mechanism of the catalysts with highly dispersed and isolated active sites, as well as the preparation, characterization of the catalysts with highly dispersed and isolated active sites and their applications in other types of reactions of lower hydrocarbons are summarized.

  11. Catalyst dispersion and activity under conditions of temperature-staged liquefaction

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-02-01

    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of the catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation.

  12. Catalytic selectivity and H-transfer in the hydroconversion of a petroleum residue using dispersed catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Cebolla, V.L.; Membrado, L.; Vela, J.; Bacaud, R.; Rouleau, L. [Instituto de Carboquimica, Zaragoza (Spain). Dept. de Procesos Quimicos

    1995-09-01

    Hydroconversion of a deasphalted vacuum residue of a crude oil has been performed in the presence of various disposable, dispersed catalysts at low concentration (450 ppm of metal) under identical conditions: a plasma-prepared nickel-carbon catalyst, an oil-soluble molybdenum naphthenate, and a commercial nickel-molybdenum supported on alumina, in order to obtain some insight into their influence upon their mechanisms of hydrogen transfer, and to evaluate their selectivities toward the production of various hydrocarbon groups. For this last purpose, a quantitative, rapid and accurate method for hydrocarbon group type analysis has been used, based on an improved system of thin-layer chromatography with flame ionization detection. The catalysts significantly affect the quantitative distribution of hydrocarbon groups without producing new chemical families. The total hydrogen consumption is only slightly increased in the presence of these kind of catalysts. However, a different distribution of the hydrogen is achieved depending on the catalyst. Molybdenum naphthenate exhibits the higher hydrogen incorporation to its derived distillates, which in turn present significantly higher number-average molecular weight and percentage of saturates than those obtained with the other catalysts. For every catalyst studied, the more the incorporation of hydrogen in distillates, the less the production of coke and gas. Throughout this paper, the agreement between the data obtained from TLC-FID and hydrogen balance is evidenced and explained. 18 refs., 5 figs., 2 tabs.

  13. Synthesis, characterization, and growth simulations of Cu–Pt bimetallic nanoclusters

    Directory of Open Access Journals (Sweden)

    Subarna Khanal

    2014-08-01

    Full Text Available Highly monodispersed Cu–Pt bimetallic nanoclusters were synthesized by a facile synthesis approach. Analysis of transmission electron microscopy (TEM and spherical aberration (Cs-corrected scanning transmission electron microscopy (STEM images shows that the average diameter of the Cu–Pt nanoclusters is 3.0 ± 1.0 nm. The high angle annular dark field (HAADF-STEM images, intensity profiles, and energy dispersive X-ray spectroscopy (EDX line scans, allowed us to study the distribution of Cu and Pt with atomistic resolution, finding that Pt is embedded randomly in the Cu lattice. A novel simulation method is applied to study the growth mechanism, which shows the formation of alloy structures in good agreement with the experimental evidence. The findings give insight into the formation mechanism of the nanosized Cu–Pt bimetallic catalysts.

  14. Microwave-assisted synthesis of high-loading, highly dispersed Pt/carbon aerogel catalyst for direct methanol fuel cell

    Indian Academy of Sciences (India)

    Zhijun Guo; Hong Zhu; Xinwei Zhang; Fanghui Wang; Yubao Guo; Yongsheng Wei

    2011-06-01

    A Pt supported on carbon aerogel catalyst has been synthesized by the microwave-assisted polyol process. The Pt supported on carbon aerogel catalyst was characterized by high resolution transmission electron microscopy and X-ray diffraction. The results show a uniform dispersion of spherical Pt nanoparticles 2.5–3.0 nm in diameter. Cyclic voltammetry and chronoamperometry were used to evaluate the electrocatalytic activity of the Pt/carbon aerogel catalyst for methanol oxidation at room temperature. The Pt/carbon aerogel catalyst shows higher electrochemical catalytic activity and stability for methanol oxidation than a commercial Pt/C catalyst of the same Pt loading.

  15. Nanocrystal and surface alloy properties of bimetallic Gold-Platinum nanoparticles

    Directory of Open Access Journals (Sweden)

    Mott Derrick

    2006-01-01

    Full Text Available AbstractWe report on the correlation between the nanocrystal and surface alloy properties with the bimetallic composition of gold-platinum(AuPt nanoparticles. The fundamental understanding of whether the AuPt nanocrystal core is alloyed or phase-segregated and how the surface binding properties are correlated with the nanoscale bimetallic properties is important not only for the exploitation of catalytic activity of the nanoscale bimetallic catalysts, but also to the general exploration of the surface or interfacial reactivities of bimetallic or multimetallic nanoparticles. The AuPt nanoparticles are shown to exhibit not only single-phase alloy character in the nanocrystal, but also bimetallic alloy property on the surface. The nanocrystal and surface alloy properties are directly correlated with the bimetallic composition. The FTIR probing of CO adsorption on the bimetallic nanoparticles supported on silica reveals that the surface binding sites are dependent on the bimetallic composition. The analysis of this dependence further led to the conclusion that the relative Au-atop and Pt-atop sites for the linear CO adsorption on the nanoparticle surface are not only correlated with the bimetallic composition, but also with the electronic effect as a result of the d-band shift of Pt in the bimetallic nanocrystals, which is the first demonstration of the nanoscale core-surface property correlation for the bimetallic nanoparticles over a wide range of bimetallic composition.

  16. Ni-Based Catalysts for Low Temperature Methane Steam Reforming: Recent Results on Ni-Au and Comparison with Other Bi-Metallic Systems

    OpenAIRE

    Anna M. Venezia; Fabrizio Puleo; Valeria La Parola; Giuseppe Pantaleo; Hongjing Wu; Leonarda F. Liotta

    2013-01-01

    Steam reforming of light hydrocarbons provides a promising method for hydrogen production. Ni-based catalysts are so far the best and the most commonly used catalysts for steam reforming because of their acceptably high activity and significantly lower cost in comparison with alternative precious metal-based catalysts. However, nickel catalysts are susceptible to deactivation from the deposition of carbon, even when operating at steam-to-carbon ratios predicted to be thermodynamically outside...

  17. Effect of Activated Carbon as a Support on Metal Dispersion and Activity of Ruthenium Catalyst for Ammonia Synthesis

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Ten kinds of activated carbon from different raw materials were used as supports to prepare ruthenium catalysts. N2 physisorption and CO chemisorption were carried out to investigate the pore size distribution and the ruthenium dispersion of the catalysts. It was found that the Ru dispersion of the catalyst was closely related to not only the texture of carbon support but also the purity of activated carbon. The activities of a series of the carbon-supported barium-promoted Ru catalysts for ammonia synthesis were measured at 425 ℃, 10.0 MPa and 10 000 h-1. The result shows that the same raw material activated carbon, with a high purity, high surface area, large pore volume and reasonable pore size distribution might disperse ruthenium and promoter sufficiently, which activated carbon as support, could be used to manufacture ruthenium catalyst with a high activity for ammonia synthesis. The different raw material activated carbon as the support would greatly influence the catalytic properties of the ruthenium catalyst for ammonia synthesis. For example, with coconut shell carbon(AC1) as the support, the ammonia concentration in the effluent was 13.17% over 4%Ru-BaO/AC1 catalyst, while with the desulfurized coal carbon(AC10) as the support, that in the effluent was only 1.37% over 4%Ru-BaO/AC10 catalyst.

  18. Catalyst dispersion and activity under conditions of temperature- staged liquefaction. [Catalyst precursors for molybdenum-based catalyst and iron-based catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-07-01

    Two coals, a Texas subbituminous C and a Utah high volatile A bituminous, were used to examine the effects of solvent swelling and catalyst impregnation on liquefaction conversion behavior in temperature staged reactions for 30 minutes each at 275{degree} and 425{degree}C in H{sub 2} and 95:5 H{sub 2}:H{sub 2}S atmospheres. Methanol, pyridine, tetrahydrofuran, and tetrabutylammonium hydroxide were used as swelling agents. Molybdenum-based catalyst precursors were ammonium tetrathiomolybdate, molybdenum trisulfide, molybdenum hexacarbonyl, and bis(tricarbonylcyclopentadienyl-molybdenum). Ferrous sulfate and bis(dicarbonylcyclo-pentadienyliron) served as iron-based catalyst precursors. In addition, ion exchange was used for loading iron onto the subbituminous coal. For most experiments, liquefaction in H{sub 2}:H{sub 2}S was superior to that in H{sub 2}, regardless of the catalyst precursor. The benefit of the H{sub 2}S was greater for the subbituminous, presumably because of its higher iron content relative to the hvab coal. Tetrabutylammonium hydroxide was the only swelling agent to enhance conversion of the hvab coal significantly; it also caused a remarkable increase in conversion of the subbituminous coal. The combined application of solvent swelling and catalyst impregnation also improves liquefaction, mainly through increased oil yields from the hvab coal and increased asphaltenes from the subbituminous. A remarkable effect from use of ammonium tetrathiomolybdate as a catalyst precursor is substantial increase in pristane and phytane yields. Our findings suggest that these compounds are, at least in part, bound to the coal matrix.

  19. A silica supported Fe-Co bimetallic catalyst prepared by the sol/gel technique: Operating conditions, catalytic properties and characterization

    Energy Technology Data Exchange (ETDEWEB)

    Mirzaei, Ali A.; Babaei, Adel Beig; Galavy, Maryam [Department of Chemistry, Faculty of Sciences, University of Sistan and Baluchestan, Zahedan 98135-674 (Iran); Youssefi, Abbas [Par-e-Taavouse Research Institute, Mashhad (Iran)

    2010-03-15

    A Co/Fe catalyst was prepared using the sol/gel technique in order to study its catalytic activity and selectivity in the Fischer-Tropsch synthesis. The effect of a range of operation variables such as pressure, temperature and H{sub 2}/CO molar feed ratio on the catalytic performance of 40%Fe/60%Co/15 wt.%SiO{sub 2}/1.5 wt.%K catalyst was investigated. It was found that the optimum operating conditions is a H{sub 2}/CO = 2/1 molar feed ratio at 350 C temperature and 3 bar pressure. Characterization of both precursor and calcined catalysts was carried out using XRD, SEM, EDS, TPR, BET surface area measurements and thermal analysis methods such as TGA and DSC. It was observed that all of the different operation variables influenced the structure, morphology and catalytic performance of the catalysts. (author)

  20. Bimetallic Wiregauze Supported Pt-Ru Nanocatalysts for Hydrogen Mitigation.

    Science.gov (United States)

    Sanap, Kiran K; Varma, S; Waghmode, S B; Sharma, P; Manoj, N; Vatsa, R K; Bharadwaj, S R

    2015-05-01

    Passive autocatalytic recombiner (PAR) is one of the most suitable devices for mitigation of hydrogen, generated in nuclear power plant under accidental conditions. For this purpose we report development of stainless steel wire gauze supported Pt-Ru nanoparticles as catalysts. Simultaneous electroless deposition has been employed for the synthesis of the catalysts. Pt-Ru based bimetallic catalysts were characterized for their rate of coating kinetics, noble metal loading, phase purity by XRD and surface morphology by SEM, TEM and elemental analysis by SIMS. Developed catalysts were found to be active for efficient recombination of hydrogen and oxygen in air as well as in presence of various prospective poisons like CO2, CH4, CO and relative humidity. Pt-Ru based bimetallic catalyst with 0.9% loading was found to be active for CO poisoning up to 400 ppm of CO. PMID:26504972

  1. Cobalt Fischer-Tropsch catalysts: influence of cobalt dispersion and titanium oxides promotion

    Energy Technology Data Exchange (ETDEWEB)

    Azib, H.

    1996-04-10

    The aim of this work is to study the effect of Sol-Gel preparation parameters which occur in silica supported cobalt catalysts synthesis. These catalysts are particularly used for the waxes production in natural gas processing. The solids have been characterized by several techniques: transmission electron microscopy (TEM), X-ray absorption near edge spectroscopy (XANES), programmed temperature reduction (TPR), infrared spectroscopy (IR), ultraviolet spectroscopy (UV), Magnetism, thermodesorption of H{sub 2} (TPD). The results indicate that the control of the cobalt dispersion and oxide phases nature is possible by modifying Sol-Gel parameters. The catalytic tests in Fischer-Tropsch synthesis were conducted on a pilot unit under pressure (20 atm) and suggested that turnover rates were independent of Co crystallite size, Co phases in the solids (Co deg., cobalt silicate) and titanium oxide promotion. On the other methane, the C{sub 3}{sup +} hydrocarbon selectivity is increased with increasing crystallite size. Inversely, the methane production is favoured by very small crystallites, cobalt silicate increase and titanium addition. However, the latter, used as a cobalt promoter, has a benefic effect on the active phase stability during the synthesis. (author). 149 refs., 102 figs., 71 tabs.

  2. Catalyst dispersion and activity under conditions of temperature-staged liquefaction. Technical progress report, October--December 1991

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-02-01

    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of the catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation.

  3. Catalyst dispersion and activity under conditions of temperature- staged liquefaction. Technical progress report, July--September 1991

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-02-01

    The general objectives of this research are (1) to investigate the use of highly dispersed catalysts for the pretreatment of coal by mild hydrogenation, (2) to identify the active forms of catalysts under reaction conditions and (3) to clarify the mechanisms of catalysis. The ultimate objective is to ascertain if mild catalytic hydrogenation resulting in very limited or no coal solubilization is an advantageous pretreatment for the transformation of coal into transportable fuels. The experimental program will focus upon the development of effective methods of impregnating coal with catalysts, evaluating the conditions under which the catalysts are most active and establishing the relative impact of improved impregnation on conversion and product distributions obtained from coal hydrogenation.

  4. Autothermal Reforming and Partial Oxidation of Methane in Fluidized Reactor over Highly Dispersed Ni Catalyst Prepared from Ni Complex

    Institute of Scientific and Technical Information of China (English)

    GAO Jing; HOU Zhao-Yin; SHEN Kai; LOU Hui; FEI Jin-Hua; ZHENG Xiao-Ming

    2006-01-01

    Highly dispersed Ni catalysts on spherical SiO2 were prepared by simple impregnation of Ni(acac)2, [Ni-(NH3)6-n(H2O)n]2+, [Ni(en)3]2+ and [Ni(EDTA)]2-. Pulse adsorption of H2 and TEM analysis results confirmed that Ni was dispersed very well on the surface of SiO2 even after calcination (4 h) and reduction (1 h) at high temperature of 800 ℃. These highly dispersed and uniquely sized Ni crystallites were more stable and more reactive for both autothermal reforming and partial oxidation of methane in fluidized reactor.

  5. Effect of the Dispersibility of Nano-CuO Catalyst on Heat Releasing of AP/HTPB Propellant

    OpenAIRE

    Yi Yang; Xinjie Yu; Jun Wang; Yaxue Wang

    2011-01-01

    Kneading time is adjusted to change the dispersibility of nano-CuO in AP/HTPB (Ammonia Perchlorate/Hydroxyl-Terminated Polybutadiene) composite propellants. Nano-CuO/AP is prepared to serve as the other dispersing method of nano-CuO, named predispersing procedure. Several kinds of heat releasing, thermal decomposition by DSC, combustion heat in oxygen environment, and explosion heat in nitrogen environment, are characterized to learn the effect of dispersibility of nano-CuO catalyst on heat r...

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

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Jingguan [University of Delaware

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-01-05

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

  8. A facile reflux procedure to increase active surface sites form highly active and durable supported palladium@platinum bimetallic nanodendrites

    Science.gov (United States)

    Wang, Qin; Li, Yingjun; Liu, Baocang; Xu, Guangran; Zhang, Geng; Zhao, Qi; Zhang, Jun

    2015-11-01

    A series of well-dispersed bimetallic Pd@Pt nanodendrites uniformly supported on XC-72 carbon black are fabricated by using different capping agents. These capping agents are essential for the branched morphology control. However, the surfactant adsorbed on the nanodendrites surface blocks the access of reactant molecules to the active surface sites, and the catalytic activities of these bimetallic nanodendrites are significantly restricted. Herein, a facile reflux procedure to effectively remove the capping agent molecules without significantly affecting their sizes is reported for activating supported nanocatalysts. More significantly, the structure and morphology of the nanodendrites can also be retained, enhancing the numbers of active surface sites, catalytic activity and stability toward methanol and ethanol electro-oxidation reactions. The as-obtained hot water reflux-treated Pd@Pt/C catalyst manifests superior catalytic activity and stability both in terms of surface and mass specific activities, as compared to the untreated catalysts and the commercial Pt/C and Pd/C catalysts. We anticipate that this effective and facile removal method has more general applicability to highly active nanocatalysts prepared with various surfactants, and should lead to improvements in environmental protection and energy production.

  9. Synthesis of higher alcohols over highly dispersed Cu-Fe based catalysts derived from layered double hydroxides.

    Science.gov (United States)

    Han, Xinyou; Fang, Kegong; Zhou, Juan; Zhao, Lu; Sun, Yuhan

    2016-05-15

    Highly dispersed Cu-Fe based catalysts with Fe/Cu molar ratios ranging from 0.2 to 1 were prepared via thermal decomposition of layered double hydroxides (LDHs) precursors and tested for higher alcohol synthesis (HAS) via CO hydrogenation. The catalysts were characterized using different techniques such as XRD, TEM, XPS, and H2-TPR. It was demonstrated that the Cu and Fe ions were highly dispersed in the brucite-like layers of the LDHs. With increased Fe/Cu atomic ratio, the tetrahedrally coordinated Cu ion content, Cu reduction temperatures, and the spacing of layers initially increase until the Fe/Cu ratio reaches 0.5 and then decrease. In addition to the catalytic evaluation for CO hydrogenation and catalyst characterization, the relationships between the physical-chemical properties of the catalysts and their catalytic performances were also investigated. It was also found that the alcohols/hydrocarbons ratios correlate linearly with the tetrahedrally coordinated Cu ion content. Moreover, higher reduction temperatures of Cu species as well as larger spacing between the layers in the catalyst are favorable for the synthesis of alcohols. The incorporation of a suitable amount of Fe is beneficial for the production of higher alcohols, with the best catalytic performance (alcohol selectivity of 20.77% and C2+ alcohol selectivity of 48.06%) obtained from a Fe/Cu atomic ratio of 0.5. PMID:26943001

  10. Effects of Cu over Pd based catalysts supported on silica or niobia

    Directory of Open Access Journals (Sweden)

    Roma M.N.S.C.

    2000-01-01

    Full Text Available Palladium and palladium-copper catalysts supported on silica and niobia were characterized by H2 chemisorption and H2-O2 titration. Systems over silica were also analyzed by transmission electron microscopy and EXAFS. The metallic dispersion decreased from 20% to 7% when the content of Pd was increased from 0.5wt.-% to 3wt.-% in monometallic catalysts. The addition of 3 wt.-% Cu to obtain Pd-Cu catalysts caused a remarkable capacity loss of hydrogen chemisorption. TPR analysis suggested an interaction between the two metals and EXAFS characterization of the catalyst supported on silica confirmed the formation of Pd-Cu alloy. Pd/Nb2O5 catalysts showed turnover numbers higher than those obtained with the Pd/SiO2 systems in the cyclohexane dehydrogenation. However, the bimetallic catalysts showed very low turnover numbers.

  11. Promotion of the electrocatalytic activity of a bimetallic platinum-ruthenium catalyst by repetitive redox treatments for direct methanol fuel cell

    Science.gov (United States)

    Huang, Sheng-Yang; Yeh, Chuin-Tih

    Pt-Ru/C catalyst (12 wt%) was prepared by the incipient wetness impregnation method followed by a redox heat-treatment. Transmission electron microscopy (TEM) results revealed uniformly distributed metallic crystallites of Pt-Ru alloy nanoparticles (d PtRu = 2.1 ± 1.0 nm). The effect of redox treatments of the impregnated catalysts on methanol oxidation reaction (MOR) was examined by cyclic voltammetry (CV). The MOR activity of the PtRu/C was significantly improved after each oxidation step of the redox treatment cycles. The enhanced catalytic activity was found to be quite stable in chronoamperometry (CA) measurements. CV, X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD) results strongly suggested that the improved catalytic activity was due to the formation of a stable c-RuO x (x = 2-3) domain during the oxidation treatments. A bifunctional based mechanism was proposed for the MOR on the oxidized PtRu/C catalysts. Formation of Ru-OH species on the surface of c-RuO x domains was suggested as stale sites for the oxidation of carbon monoxide adsorbed on the Pt catalytic sites.

  12. Biosensors Incorporating Bimetallic Nanoparticles

    Directory of Open Access Journals (Sweden)

    John Rick

    2015-12-01

    Full Text Available This article presents a review of electrochemical bio-sensing for target analytes based on the use of electrocatalytic bimetallic nanoparticles (NPs, which can improve both the sensitivity and selectivity of biosensors. The review moves quickly from an introduction to the field of bio-sensing, to the importance of biosensors in today’s society, the nature of the electrochemical methods employed and the attendant problems encountered. The role of electrocatalysts is introduced with reference to the three generations of biosensors. The contributions made by previous workers using bimetallic constructs, grouped by target analyte, are then examined in detail; following which, the synthesis and characterization of the catalytic particles is examined prior to a summary of the current state of endeavor. Finally, some perspectives for the future of bimetallic NPs in biosensors are given.

  13. Formation of Catalyst Model Dispersed of Pd on a thin MgO(100)

    Science.gov (United States)

    Baara, F.; Chemam, A.

    2016-04-01

    The nucleation kinetics or the formation of a catalyst model dispersed for the system Pd/thin MgO (100) are calculated by developing many programs using Fortran software. This simulation is based upon parameters studied in situ by transmission electron microscopy (TEM), related to the first quantitative study on the nucleation and the growth. Palladium nanoparticles deposited on thin MgO are tested in the temperature range 573-1073 K and deposition time of 1000 s. The nucleation kinetics are interpreted according to the theory of random nucleation. The general scheme is consisting of three stages namely, nucleation, growth and coalescence. The saturation density of clusters decreases when the substrate temperature increases following Arrhenius law. This behavior is in agreement with a recent AFM study for Ag/MgO and Au/MgO. The phenomenon of coalescence is explained via island migration process. It is shown that the coalescence occurs more rapidly when the substrate temperature is high.

  14. Synthesis of Supported NiPt Bimetallic Nanoparticles, Methods for Controlling the Surface Coverage of Ni Nanoparticles With Pt, Methods Of Making NiPt Multilayer Core-Shell Structures and Application of the Supported Catalysts for CO2 Reforming

    KAUST Repository

    Li, Lidong

    2015-06-25

    Embodiments of the present disclosure provide for supported Ni/Pt bimetallic nanoparticles, compositions including supported NiPt nanoparticles, methods of making supported NiPt nanoparticles, methods of using supported NiPt nanoparticles, and the like.

  15. Cu-Co bi-metal catalyst prepared by perovskite CuO/LaCoO3 used for higher alcohol synthesis from syngas

    Institute of Scientific and Technical Information of China (English)

    Yuzhen Fang; Yuan Liu; Wei Deng; Junhai Liu

    2014-01-01

    Cu-Co bi-metal catalysts derived from CuO/LaCoO3 perovskite structure were prepared by one-step citrate complexing method, and the structure evolution reaction from CuO/LaCoO3 to Cu-Co2C/La2O2CO3 under H2 pretreatment was investigated by techniques of XRD, TPR and TEM. The results suggest that a much higher dispersion of copper significantly enhanced the reduction of cobalt, and a stronger interaction between copper and cobalt ions in LaCoO3 particles led to the formation of bi-metallic Cu-Co particles in the reduced catalysts and the enrichment of Co on the surface of bimetallic particles. The prepared catalysts were highly active and selective for the alcohol synthesis from syngas due to the presence of copper-modified Co2 C species.

  16. Facile Synthesis of Worm-like Micelles by Visible Light Mediated Dispersion Polymerization Using Photoredox Catalyst.

    Science.gov (United States)

    Yeow, Jonathan; Xu, Jiangtao; Boyer, Cyrille

    2016-01-01

    Presented herein is a protocol for the facile synthesis of worm-like micelles by visible light mediated dispersion polymerization. This approach begins with the synthesis of a hydrophilic poly(oligo(ethylene glycol) methyl ether methacrylate) (POEGMA) homopolymer using reversible addition-fragmentation chain-transfer (RAFT) polymerization. Under mild visible light irradiation (λ = 460 nm, 0.7 mW/cm(2)), this macro-chain transfer agent (macro-CTA) in the presence of a ruthenium based photoredox catalyst, Ru(bpy)3Cl2 can be chain extended with a second monomer to form a well-defined block copolymer in a process known as Photoinduced Electron Transfer RAFT (PET-RAFT). When PET-RAFT is used to chain extend POEGMA with benzyl methacrylate (BzMA) in ethanol (EtOH), polymeric nanoparticles with different morphologies are formed in situ according to a polymerization-induced self-assembly (PISA) mechanism. Self-assembly into nanoparticles presenting POEGMA chains at the corona and poly(benzyl methacrylate) (PBzMA) chains in the core occurs in situ due to the growing insolubility of the PBzMA block in ethanol. Interestingly, the formation of highly pure worm-like micelles can be readily monitored by observing the onset of a highly viscous gel in situ due to nanoparticle entanglements occurring during the polymerization. This process thereby allows for a more reproducible synthesis of worm-like micelles simply by monitoring the solution viscosity during the course of the polymerization. In addition, the light stimulus can be intermittently applied in an ON/OFF manner demonstrating temporal control over the nanoparticle morphology. PMID:27340940

  17. Supported Cobalt Molybdenum Bimetallic Nitrides for Ammonia Decomposition%负载型钴铜双金属氮化物催化氨分解研究

    Institute of Scientific and Technical Information of China (English)

    项益智; 李小年

    2005-01-01

    Co and Mo bimetallic nitrides supported on Mg(Al)O, MgO and γ-Al2O3 were prepared in temperatureprogrammed reactions with NH3. The surface morphology, chemical composition and catalytic activity for NH3 decomposition on the supported Co and Mo bimetallic nitrides were studied by X-ray diffractometer (XRD), NH3 temperature-programmed desorption and mass spectrometer (NH3-TPD-MS), temperature-programmed desorption and mass spectrometer (TPD-MS), H2 temperature-programmed surface reaction (H2-TPSR) and activity test.The phases of Co3MosN and MoN could be formed on Mg(Al)O, MgO and Al2O3 during the nitridation, and they might be more uniformly dispersed on Mg(Al)O and MgO than on γ-Al2O3. Transition metallic nitrides are generally considered as potential catalysts for hydrogen-involving reactions due to the entrance of hydrogen atoms into subsurface and the lattice of metallic nitrides. The diffusion of nitrogen in the bulk and the structure transformation of Co and Mo nitride compounds occur during NH3-TPD, but the supported Co and Mo bimetallic nitrides are not easily reduced at H2 atmosphere. Co3Mo3N/Mg(Al)O catalyst exhibits the highest activity, while Co3Mo3N/Al2O3 exhibits the lowest activity for NH3 decomposition. Furthermore, the catalytic activity of Co and Mo bimetallic nitrides is not only much higher than that of supported single metallic nitride, but also highly dependent upon the surface acidity and BET surface area of support.

  18. Structural Characterization of Bimetallic Nanocrystal Electrocatalysts

    Energy Technology Data Exchange (ETDEWEB)

    Cullen, David A [ORNL

    2016-01-01

    Late transition metal nanocrystals find applications in heterogeneous catalysis such as plasmon-enhanced catalysis and as electrode materials for fuel cells, a zero-emission and sustainable energy technology. Their commercial viability for automotive transportation has steadily increased in recent years, almost exclusively due to the discovery of more efficient bimetallic nanocatalysts for the oxygen reduction reaction (ORR) at the cathode. Despite improvements to catalyst design, achieving high activity while maintaining durability is essential to further enhance their performance for this and other important applications in catalysis. Electronic effects arising from the generation of metal-metal interfaces, from plasmonic metals, and from lattice distortions, can vastly improve sorption properties at catalytic surfaces, while increasing durability.[1] Multimetallic lattice-strained nanoparticles are thus an interesting opportunity for fundamental research.[2,3] A colloidal synthesis approach is demonstrated to produce AuPd alloy and Pd@Au core-shell nanoicosahedra as catalysts for electro-oxidations. The nanoparticles are characterized using aberration-corrected scanning transmission electron microscopy (ac-STEM) and large solid angle energy dispersive X-ray spectroscopy (EDS) on an FEI Talos 4-detector STEM/EDS system. Figure 1 shows bright-field (BF) and high-angle annular dark-field (HAADF) ac-STEM images of the alloy and core-shell nanoicosahedra together with EDS line-scans and elemental maps. These structures are unique in that the presence of twin boundaries, alloying, and core-shell morphology could create highly strained surfaces and interfaces. The shell thickness of the core-shell structures observed in HAADF-STEM images is tuned by adjusting the ratio between metal precursors (Figure 2a-f) to produce shells ranging from a few to several monolayers. Specific activity was measured in ethanol electro-oxidation to examine the effect of shell thickness on

  19. XAFS studies on highly dispersed Ni 2P/SiO 2 catalysts for hydrodesulfurization of 4,6-dimethyldibenzothiophene

    Science.gov (United States)

    Cho, Kye-Sung; Lee, Yong-Kul

    2010-09-01

    The Ni 2P catalysts were prepared by a new synthetic method with the use of less oxidic phosphorus precursor in order to achieve high dispersion on silica support, and their structural properties and catalytic activity in HDS of 4,6-DMDBT were studied. Comparison was made with a conventionally prepared sample which was obtained by temperature programmed reduction method. Various characterizations were conducted by BET, CO uptake, TPR, XRD and X-ray absorption spectroscopy. The amounts of CO chemisorption uptake were 64 and 20 μmol g -1 for Ni 2P/SiO 2-LT and Ni 2P/SiO 2-HT, respectively, indicating that the low temperature reduction technique led to better dispersion of Ni 2P particles on SiO 2 support. The catalytic activity in the HDS of 4,6-DMDBT followed the order, Ni 2P/SiO 2-HT(54%)catalysts highly depend on the dispersion of the Ni 2P phase.

  20. Bimetallic redox synergy in oxidative palladium catalysis.

    Science.gov (United States)

    Powers, David C; Ritter, Tobias

    2012-06-19

    (II/IV) catalysis has guided the successful development of many reactions. Herein we discuss differences between monometallic Pd(IV) and bimetallic Pd(III) redox catalysis. We address whether appreciation of the relevance of bimetallic Pd(III) redox catalysis is of academic interest exclusively, serving to provide a more nuanced description of catalysis, or if the new insight regarding bimetallic Pd(III) chemistry can be a platform to enable future reaction development. To this end, we describe an example in which the hypothesis of bimetallic redox chemistry guided reaction development, leading to the discovery of reactivity distinct from monometallic catalysts.

  1. Chlorination of Carbon Nanotubes Obtained on the Different Metal Catalysts

    Directory of Open Access Journals (Sweden)

    Iwona Pełech

    2013-01-01

    Full Text Available In this paper, a chlorination method is proposed for simultaneous purification and functionalization of carbon nanotubes, thus increasing their ability to use. Carbon nanotubes were obtained by CVD method through ethylene decomposition on the nanocrystalline iron or cobalt or bimetallic iron-cobalt catalysts. The effects of temperature (50, 250, and 450°C in the case of carbon nanotubes obtained on the Fe-Co catalyst and type of catalyst (Fe, Co, Fe/Co on the effectiveness of the treatment and functionalization were tested. The phase composition of the samples was determined using the X-ray diffraction method. The quantitative analysis of metal impurity content was validated by means of the thermogravimetric analysis. Using X-ray Photoelectron Spectroscopy (XPS, Energy Dispersive Spectroscopy (EDS analysis, and also Mohr titration method, the presence of chlorine species on the surface of chlorinated samples was confirmed.

  2. Synthesis and characterization of niobium-promoted cobalt/iron catalysts supported on carbon nanotubes for the hydrogenation of carbon monoxide

    Institute of Scientific and Technical Information of China (English)

    Zahra Gholami; Noor Asmawati Mohd Zabidi; Fatemeh Gholami; Mohammadtaghi Vakili

    2016-01-01

    Bimetallic Co/Fe catalysts supported on carbon nanotubes ( CNTs) were prepared, and niobium ( Nb) was added as promoter to the 70Co:30Fe/CNT catalyst. The physicochemical properties of the catalysts were characterized, and the catalytic performances were analyzed at the same operation conditions (H2:CO (volume ratio)= 2:1, p = 1 MPa, and t = 260℃) in a tubular fixed-bed microreactor system. The addition of Nb to the bimetallic catalyst decreases the average size of the oxide nanoparticles and improves the reducibility of the bimetallic catalyst. Evaluation of the catalyst performance in a Fischer-Tropsch reaction shows that the catalyst results in high selectivity to methane, and the selectivity to C5+ increased slightly in the bimetallic catalyst unlike that in the monometallic catalysts. The addition of 1% Nb to the bimetallic catalyst increases CO conversion and selectivity to C5+. Meanwhile, a decrease in methane selectivity is observed.

  3. Catalytic Performance and Characterization of Pt-Co/Al2O3Catalysts for CO2 Reforming of CH4 to Synthesis Gas

    Institute of Scientific and Technical Information of China (English)

    HUANG, Chuan-Jing; ZHENG, Xiao-Ming; MO, Liu-Ye; FEI, Jin-Hua

    2001-01-01

    Pt-Co/Al2O3 catalyst has been studied for CO2 reforming of CH4 to synthesis gas. It was found that the catalytic performance of the catalyst was sensitive to calcination temperature.When Co/Al2O3 was calcined at 1473 K prior to adding a small amount of Pt to it, the resulting bimetallic catalyst showed high activity, optimal stability and excellent resistance to carbon deposition, which was more effective to the reaction than Co/Al2O3 and Pt/Al2O3 catalysts. At lower metal loading, catalyst activity decreased in the following order: Pt-Co/Al2O3 > Pt/Al2O3 》 Co/Al2O3. With 9% Co, the Co/Al2O3calcined at 923 K was also active for CO2 reforming of CH4,however, its carbon formation was much more fast than that of the Pt-Co/Al2O3 catalyst. The XRD results indicated that Pt species well dispersed over the bimetallic catalyst. Its high dispersion was related to the presence of CoAl2O4, formed during calcining of Co/Al2O3 at high temperature before Pt addition. Promoted by Pt, CoAl2O4 in the catalyst could be reduced partially even at 923 K, the temperature of pre-re-duction for the reaction, confirmed by TPR. Based on these results, it was considered that the zerovalent platinum with high dispersion over the catalyst surface and the zerovalent cobalt resulting from CoAl2O4 reduction are responsible for high activity of the Pt-Co/Al2O3 catalyst, and the remain CoAl2O4 is beneficial to suppression of carbon deposition over the catalyst.

  4. Ni-Co/Mg-Al catalyst derived from hydrotalcite-like compound prepared by plasma for dry reforming of methane

    Institute of Scientific and Technical Information of China (English)

    Huali; Long; Yan; Xu; Xiaoqing; Zhang; Shijing; Hu; Shuyong; Shang; Yongxiang; Yin; Xiaoyan; Dai

    2013-01-01

    Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.

  5. Effect of the Dispersibility of Nano-CuO Catalyst on Heat Releasing of AP/HTPB Propellant

    Directory of Open Access Journals (Sweden)

    Yi Yang

    2011-01-01

    Full Text Available Kneading time is adjusted to change the dispersibility of nano-CuO in AP/HTPB (Ammonia Perchlorate/Hydroxyl-Terminated Polybutadiene composite propellants. Nano-CuO/AP is prepared to serve as the other dispersing method of nano-CuO, named predispersing procedure. Several kinds of heat releasing, thermal decomposition by DSC, combustion heat in oxygen environment, and explosion heat in nitrogen environment, are characterized to learn the effect of dispersibility of nano-CuO catalyst on heat releasing of propellants. With pre-dispersing procedures, thermal decomposition temperature of nano-CuO/AP and its propellant are about 25∘C and 8.6∘C lower than that of AP simple mixed with nano-CuO and its propellant, respectively. Comparing propellant with simple mixed nano-CuO kneading 3 hours, combustion heat and explosion heat of propellant with nano-CuO/AP increase about 1.4% and 1.7%, respectively. However, because of the breaking of nano-CuO/AP structure during kneading procedure, combustion heat and explosion heat of all the samples are decreased with the increase of kneading time after 3 hours.

  6. Advanced liquefaction using coal swelling and catalyst dispersion techniques. Quarterly technical progress report, July--September 1992

    Energy Technology Data Exchange (ETDEWEB)

    Curtis, C.W. [Auburn Univ., AL (United States); Gutterman, C. [Foster Wheeler Development Corp., Livingston, NJ (United States); Chander, S. [Pennsylvania State Univ., University Park, PA (United States)

    1992-12-31

    The experimental study of coal swelling ratios have been determined with a wide variety of solvents. Only marginal levels of coal swelling were observed for the hydrocarbon solvents, but high levels were found with solvents having heteroatom functionality. Blends were superior to pure solvents. The activity of various catalyst precursors for pyrene hydrogenation and coal conversion was measured. Higher coal conversions were observed for the S0{sub 2}-treated coal than the raw coal, regardless of catalyst type. Coal conversions were highest for Molyvan-L, molybdenum naphthenate, and nickel octoate, respectively. Bottoms processing consists of a combination of the ASCOT process coupling solvent deasphalting with delayed coking. Initial results indicate that a blend of butane and pentane used near the critical temperature of butane is the best solvent blend for producing a yield/temperature relationship of proper sensitivity and yet retaining an asphalt phase of reasonable viscosity. The literature concerning coal swelling, both alone and in combination with coal liquefaction, and the use of dispersed or unsupported catalysts in coal liquefaction has been updated.

  7. Effect of ball-milling duration and dehydrogenation on the morphology, microstructure and catalyst dispersion in Ni-catalyzed MgH2 hydrogen storage materials

    International Nuclear Information System (INIS)

    The effects of high-energy ball-milling on catalyst morphology and dispersion as a function of milling duration and on hydrogen desorption were investigated. Samples of MgH2 doped with 0.05 Ni catalyst were examined after 1, 5 and 10 h of milling. Longer milling durations produced finer catalyst particle sizes and more uniform dispersions, but yielded higher hydrogen desorption temperatures. This behavior is attributed to the formation of Mg2NiH4 with increased milling times. Electron tomography was used to show that the Ni particles reside both inside and outside the MgH2 particles. On dehydrogenation there was a redistribution of catalyst and continued formation of Mg2Ni. The formation of this phase is proposed to explain the reported degradation of hydrogen capacity and the change in kinetics of this system with cycling

  8. Highly-dispersed Ta-oxide catalysts prepared by electrodeposition in a non-aqueous plating bath for polymer electrolyte fuel cell cathodes

    KAUST Repository

    Seo, Jeongsuk

    2012-01-01

    The Ta-oxide cathode catalysts were prepared by electrodeposition in a non-aqueous solution. These catalysts showed excellent catalytic activity and have an onset potential of 0.92 V RHE for the oxygen reduction reaction (ORR). The highly-dispersed Ta species at the nanometer scale on the carbon black was an important contributor to the high activity. © 2012 The Royal Society of Chemistry.

  9. Facile synthesis of Cu-Pd bimetallic multipods for application in cyclohexane oxidation

    Science.gov (United States)

    Zhang, Zhuo-Qun; Huang, Jianliu; Zhang, Lan; Sun, Mei; Wang, You-Cheng; Lin, Yue; Zeng, Jie

    2014-10-01

    The synergy between Cu and Pd makes Cu-Pd bimetallic nanocrystals interesting materials for investigation. The scarcity of shapes of Cu-Pd bimetallic nanocrystals motivated us to explore highly branched structures, which may promote a wide range of applications. In this communication, we report a facile synthesis of Cu-Pd bimetallic multipods (19.2 ± 1.2 nm), on branches of which some high-index facets were exposed. Modification of reaction parameters concerning capping agents and reductant led to the formation of other shapes, including sphere-like nanocrystals (SNCs). When loaded onto TiO2, the as-prepared Cu-Pd bimetallic multipods exhibited excellent catalytic activity for the oxidation of cyclohexane by hydrogen peroxide and higher selectivity towards cyclohexanone than monometallic catalysts and SNCs/TiO2.

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

    Energy Technology Data Exchange (ETDEWEB)

    Arslan, Ilke [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Dixon, David A. [Univ. of Alabama, Tuscaloosa, AL (United States); Gates, Bruce C. [Univ. of California, Davis, CA (United States); Katz, Alexander [Univ. of California, Berkeley, CA (United States)

    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

  11. Fundamental Studies of the Reforming of Oxygenated Compounds over Supported Metal Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Dumesic, James A. [Univ. of Wisconsin, Madison, WI (United States)

    2016-01-04

    microcopy (STEM) to measure size and structure, energy dispersive X-ray spectroscopy (EDS) to measure atomic composition, X-ray absorption spectroscopy (XAS) to measure oxidation state and metal coordination, Fourier transform infrared spectroscopy (FTIR) to study adsorbed species, laser Raman spectroscopy to probe metal oxide promoters, and temperature programmed reaction/desorption to study the energetics of adsorption and desorption processes. We have studied our bimetallic catalysts for the selective cleavage of carbon-oxygen bonds, and we have studied the effects of adding metal oxide promoters to supported platinum and gold catalysts for water-gas shift (i.e., the production of hydrogen by reaction of carbon monoxide with water). We anticipate that the knowledge obtained from our studies will allow us to identify promising directions for new catalysts that show high activity, selectivity, and stability for important reactions, such as the conversion of biomass-derived oxygenated hydrocarbons to fuels and chemicals.

  12. New catalysts for exhaust gas cleaning

    Energy Technology Data Exchange (ETDEWEB)

    Haerkoenen, M. [Kemira Metalkat Oy, Oulu (Finland)

    1996-12-31

    Major challenge for future catalyst systems was to develop thermally more stable washcoats for close coupled operating conditions and for engines operating under high speed and load conditions. To design these future emission systems extensive research and development was undertaken to develop methods to disperse and stabilize the key catalytic materials for operation at much higher temperatures. Second priority was to design catalysts that are more effective under low temperature exhaust conditions and have improved oxygen storage properties in the washcoats. Incorporating new materials and modified preparation technology a new generation of metallic catalyst formulations emerged, those being trimetallic K6 (Pt:Pd:Rh and bimetallic K7) (Pd+Pd:Rh). The target was to combine the best property of Pt:Rh (good NO{sub x} reduction) with that of the good HC oxidation activity of Pd and to ensure that precious metal/support interactions were positively maintained. Both K6 and K7 concepts contain special catalyst structures with optimized washcoat performance which can be brick converter configuration. Improvement in light-off, thermal stability and transient performance with these new catalyst formulations have clearly been shown in both laboratory and vehicle testing. (author) (20 refs.)

  13. Efficient Nd Promoted Rh Catalysts for Vapor Phase Methanol Carbonylation

    Institute of Scientific and Technical Information of China (English)

    Shu Feng ZHANG; Qing Li QIAN; Ping Lai PAN; Yi CHEN; Guo Qing YUAN

    2005-01-01

    A Nd promoted-Rh catalysts supported on polymer-derived carbon beads for vapor-phase methanol carbonylation was developed. Rh-Nd bimetallic catalysts obviously have higher activity than that of supported Rh catalyst under similar reaction condition. The difference between the activity of above two catalyst systems is clearly caused by the intrinsic properties generated by the introduction of Nd.

  14. CVD synthesis of carbon nanotubes using a finely dispersed cobalt catalyst and their use in double layer electrochemical capacitors

    International Nuclear Information System (INIS)

    Carbon nanotubes (CNT) were obtained by chemical vapour deposition (CVD), decomposing turpentine oil over finely dispersed Co metal as a catalyst at 675 deg. C. Scanning electron microscope (SEM) and transmission electron microscope (TEM) images reveal that the nanotubes are densely packed and of 10-50 nm in diameter. The XRD pattern of purified CNT shows that they are graphitic in nature. Resistivity measurements of these CNT indicate that they are highly conducting. Hall measurements of CNT reveal that electrons are the majority carriers with a carrier concentration of 1.35x1020 cm-3. Cyclic voltammetry (CV) and constant current charging/discharging was used to characterise the behaviour of electrochemical double layer capacitors of purified CNT with H2SO4. For CNT/2 M H2SO4/CNT, a capacitance of 12 F g-1 (based on the weight of the active material) was obtained

  15. Advanced liquefaction using coal swelling and catalyst dispersion techniques. Quarterly technical progress report, April--June 1992

    Energy Technology Data Exchange (ETDEWEB)

    Curtis, C.W. [Auburn Univ., AL (United States); Gutterman, C. [Foster Wheeler Development Corp., Livingston, NJ (United States); Chander, S. [Pennsylvania State Univ., University Park, PA (United States)

    1992-08-26

    Research in this project centers upon developing a new approach to the direct liquefaction of coal to produce an all-distillate product slate at a sizable cost reduction over current technology. The approach integrates all aspects of the coal liquefaction process including coal selection, pretreatment, coal swelling with catalyst impregnation, coal liquefaction experimentation, product recovery with characterization, alternate bottoms processing, and a technical assessment including an economic evaluation. The project is being carried out under contract to the United States Department of Energy. On May 28, 1992, the Department of Energy authorized starting the experimental aspects of this projects; therefore, experimentation at Amoco started late in this quarterly report period. Research contracts with Auburn University, Pennsylvania State University, and Foster Wheeler Development Corporation were signed during June, 1992, so their work was just getting underway. Their work will be summarized in future quarterly reports. A set of coal samples were sent to Hazen Research for beneficiation. The samples were received and have been analyzed. The literature search covering coal swelling has been up-dated, and preliminary coal swelling experiments were carried out. Further swelling experimentation is underway. An up-date of the literature on the liquefaction of coal using dispersed catalysts is nearing completion; it will be included in the next quarterly report.

  16. Study of Pd-Sn/Al{sub 2}O{sub 3} catalysts prepared by an oxide colloidal route; Etude de catalyseurs Pd-Sn/Al{sub 2}O{sub 3} prepares par voie colloidale oxyde

    Energy Technology Data Exchange (ETDEWEB)

    Verdier, St.

    2001-09-01

    The oxide colloidal route, developed in the laboratory for mono-metallic catalysts, consists in preparing a metallic oxide hydro-sol which leads to the supported catalyst after deposition onto a support and an activation stage. In this work, this method has been adapted to the preparation of alumina supported bimetallic Pd-Sn catalysts to determine its interest for the control of the properties of the bimetallic phase (size, composition and structure). In the preliminary study concerning tin oxide sols, SnO{sub 2} (size=2,3 nm) and Sn{sub 6}O{sub 4}(OH){sub 4} (size = 25 nm) nano-particles were synthesized by neutralization respectively for tin(IV) and tin(H). The control through the pH of the aggregation of the PdO and SnO{sub 2} particles revealed that increasing oxide solubility promotes integral re-dispersion of the oxide particles. To synthesize oxide bimetallic sols, three strategies were defined. Copolymerization (formation of a mixed oxide nano-sol by cross condensation of both metals) does not lead to a mixed oxide Pd-Sn phase. Surface precipitation (neutralization of the second metal in the presence of the first oxide sol) yields nano-particles of both oxides in close interaction. Adsorption (adsorption of the second metal onto the first oxide sol) significantly occurs when contacting tin with a basic PdO sol (hydrolytic adsorption). The characterization and the assessment of the catalytic properties (selective hydrogenation of buta-1,3-diene) of the catalysts prepared by deposition of oxide bimetallic sols showed that the oxide colloidal route allows the control of the properties of the supported bimetallic phase. Moreover, our results display that both Pd-Sn alloy formation and,aggregation of the metallic particles contribute to increase the selectivity for this reaction. (author)

  17. Well-dispersed Pt cubes on porous Cu foam: high-performance catalysts for the electrochemical oxidation of glucose in neutral media.

    Science.gov (United States)

    Niu, Xiangheng; Lan, Minbo; Zhao, Hongli; Chen, Chen

    2013-07-15

    The investigation of highly efficient catalysts for the electrochemical oxidation of glucose is the most critical challenge to commercialize nonenzymatic glucose sensors, which display a few attractive superiorities including the sufficient stability of their properties and the desired reproducibility of results over enzyme electrodes. Herein we propose a new and very promising catalyst: Pt cubes well-dispersed on the porous Cu foam, for the the electrochemical oxidation reaction of glucose in neutral media. The catalyst is fabricated in situ on a homemade screen-printed carbon electrode (SPCE) substrate through initially synthesizing the three-dimensional (3D) porous Cu foam using a hydrogen evolution assisted electrodeposition strategy, followed by electrochemically reducing the platinic precursor simply and conveniently. Field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM) proofs demonstrate that Pt cubes, with an average size (the distance of opposite faces) of 185.1 nm, highly dispersed on the macro/nanopore integrated Cu foam support can be reproducibly obtained. The results of electrochemical tests indicate that the cubic Pt-based catalyst exhibits significant enhancement on the catalytic activity towards the electrooxidation of glucose in the presence of chloride ions, providing a specific activity 6.7 times and a mass activity 5.3 times those of commercial Pt/C catalysts at -0.4 V (vs. Ag/AgCl). In addition, the proposed catalyst shows excellent stability of performance, with only a 2.8% loss of electrocatalytic activity after 100 repetitive measurements. PMID:23744705

  18. Effect of Copper Nanoparticles Dispersion on Catalytic Performance of Cu/SiO2 Catalyst for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

    Directory of Open Access Journals (Sweden)

    Yajing Zhang

    2013-01-01

    Full Text Available Cu/SiO2 catalysts, for the synthesis of ethylene glycol (EG from hydrogenation of dimethyl oxalate (DMO, were prepared by ammonia-evaporation and sol-gel methods, respectively. The structure, size of copper nanoparticles, copper dispersion, and the surface chemical states were investigated by X-ray diffraction (XRD, transmission electron microscopy (TEM, temperature-programmed reduction (TPR, and X-ray photoelectron spectroscopy (XPS and N2 adsorption. It is found the structures and catalytic performances of the catalysts were highly affected by the preparation method. The catalyst prepared by sol-gel method had smaller average size of copper nanoparticles (about 3-4 nm, better copper dispersion, higher Cu+/C0 ratio and larger BET surface area, and higher DMO conversion and EG selectivity under the optimized reaction conditions.

  19. Transmission electron microscopy and energy dispersive x-ray spectroscopy studies of Pt-Re/[gamma]-Al[sub 2]O[sub 3] catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Z.; Fryer, J.R.; Park, C.; Stirling, D.; Webb, G. (Univ. of Glasgow (United Kingdom))

    1994-08-01

    A series of Pt/[gamma]-Al[sub 2]O[sub 3], Re/[gamma]-Al[sub 2]O[sub 3], and Pt-Re/[gamma]-Al-O[sub 3] catalysts have been studied by transmission electron microscopy and energy dispersive X-ray spectroscopy. It has been shown that rhenium was not alloyed with platinum, but widely dispersed on the surface of alumina. Two types of platinum were found: (i) three-dimensional metallic particles, and (ii) small particles consisting of a few platinum atoms. Some aggregation of the platinum particles occurred during use of the catalysts in the reforming of octane. It is suggested that the interaction of rhenium with the alumina support and therefore the modification to the platinum play an essential role in promoting the enhanced stability and selectivity of these catalysts to cycloalkanes and aromatics in reforming reactions. 40 refs., 13 figs., 2 tabs.

  20. Effect of Copper Nanoparticles Dispersion on Catalytic Performance of Cu/SiO2 Catalyst for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

    International Nuclear Information System (INIS)

    Cu/SiO2 catalysts, for the synthesis of ethylene glycol (EG) from hydrogenation of dimethyl oxalate (DMO), were prepared by ammonia-evaporation and sol-gel methods, respectively. The structure, size of copper nanoparticles, copper dispersion, and the surface chemical states were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS) and N2 adsorption. It is found the structures and catalytic performances of the catalysts were highly affected by the preparation method. The catalyst prepared by sol-gel method had smaller average size of copper nanoparticles (about 3-4 nm), better copper dispersion, higher Cu+/C0 ratio and larger BET surface area, and higher DMO conversion and EG selectivity under the optimized reaction conditions.

  1. Atomic layer deposition-Sequential self-limiting surface reactions for advanced catalyst "bottom-up" synthesis

    Science.gov (United States)

    Lu, Junling; Elam, Jeffrey W.; Stair, Peter C.

    2016-06-01

    Catalyst synthesis with precise control over the structure of catalytic active sites at the atomic level is of essential importance for the scientific understanding of reaction mechanisms and for rational design of advanced catalysts with high performance. Such precise control is achievable using atomic layer deposition (ALD). ALD is similar to chemical vapor deposition (CVD), except that the deposition is split into a sequence of two self-limiting surface reactions between gaseous precursor molecules and a substrate. The unique self-limiting feature of ALD allows conformal deposition of catalytic materials on a high surface area catalyst support at the atomic level. The deposited catalytic materials can be precisely constructed on the support by varying the number and type of ALD cycles. As an alternative to the wet-chemistry based conventional methods, ALD provides a cycle-by-cycle "bottom-up" approach for nanostructuring supported catalysts with near atomic precision. In this review, we summarize recent attempts to synthesize supported catalysts with ALD. Nucleation and growth of metals by ALD on oxides and carbon materials for precise synthesis of supported monometallic catalyst are reviewed. The capability of achieving precise control over the particle size of monometallic nanoparticles by ALD is emphasized. The resulting metal catalysts with high dispersions and uniformity often show comparable or remarkably higher activity than those prepared by conventional methods. For supported bimetallic catalyst synthesis, we summarize the strategies for controlling the deposition of the secondary metal selectively on the primary metal nanoparticle but not on the support to exclude monometallic formation. As a review of the surface chemistry and growth behavior of metal ALD on metal surfaces, we demonstrate the ways to precisely tune size, composition and structure of bimetallic metal nanoparticles. The cycle-by-cycle "bottom up" construction of bimetallic (or multiple

  2. Production of biodiesel from sunflower oil using highly catalytic bimetallic gold–silver core–shell nanoparticle

    International Nuclear Information System (INIS)

    Bimetallic Gold–silver core–shell nanoparticles (Au@Ag NPs) were synthesized at room temperature, where gold nanoparticles (AuNPs) served as seeds for continuous deposition of silver atoms on its surface. The core–shell structure was examined by UV–vis spectroscopy, transmission electron microscopy (TEM) and energy dispersive X-ray (EDX) analysis. The catalytic activity of these nanoparticles toward biodiesel production from Sunflower oil through transesterification was studied. The confirmation for biofuel synthesis was performed using Fourier Transform Infra-Red (FTIR) spectroscopy. Fuel properties are determined by standard ASTM (American society for Testing and Materials) protocols. Our observations show that at certain catalyst concentration, temperature and reaction time, highest yield of biodiesel (86.9%) is attained. The fuel properties of the synthesized biofuel are at par with standard biofuel. Further, the catalyst showed sustained activity for 3 cycles of transesterification. - Highlights: • Gold–silver core–shell NPs were used for biofuel synthesis from sunflower oil. • At the optimized condition, biodiesel yield of 86.9% was achieved. • Fuel properties of the biofuel synthesized are at par with standard biofuel. • The catalyst showed sustained activity for 3 cycles of transesterification

  3. Gold/Iron Carbonyl Clusters for Tailored Au/FeOx Supported Catalysts

    Directory of Open Access Journals (Sweden)

    Stefania Albonetti

    2011-12-01

    Full Text Available A novel preparation method was developed for the preparation of gold/iron oxide supported catalysts using the bimetallic carbonyl cluster salts [NEt4]4[Au4Fe4(CO16] and [NEt4][AuFe4(CO16] as precursors of highly dispersed nanoparticles over different supports. A series of catalysts with different metal loadings were prepared and tested in the complete oxidation of dichlorobenzene, toluene, methanol and in the preferential oxidation of CO in the presence of H2 (PROX as model reactions. The characterization by BET, XRD, TEM, H2-TPR, ICP-AES and XPS point out the way the nature of the precursors and the thermal treatment conditions affected the dispersion of the active phase and their catalytic activity in the studied reactions.

  4. INTERACTION OF SULPHUR WITH BIMETALLIC SURFACES: EFFECTS OF STRUCTURAL, ELECTRONIC AND CHEMICAL PROPERTIES.

    Energy Technology Data Exchange (ETDEWEB)

    RODRIGUEZ,J.A.; HRBEK,J.

    2001-10-04

    In recent years, several new interesting phenomena have been discovered when studying the interaction of sulphur with bimetallic surfaces using the modern techniques of surface science. Very small amounts of sulphur can induce dramatic changes in the morphology of bimetallic surfaces. The electronic perturbations associated with the formation of a heteronuclear metal-metal bond affect the reactivity of the bonded metals toward sulphur. This can be a very important issue to consider when trying to minimize the negative effects of sulphur poisoning or dealing with the design of desulfurization catalysts.

  5. Platinum-cobalt bimetallic nanoparticles in hollow carbon nanospheres for hydrogenolysis of 5-hydroxymethylfurfural

    Science.gov (United States)

    Wang, Guang-Hui; Hilgert, Jakob; Richter, Felix Herrmann; Wang, Feng; Bongard, Hans-Josef; Spliethoff, Bernd; Weidenthaler, Claudia; Schüth, Ferdi

    2014-03-01

    The synthesis of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) is a highly attractive route to a renewable fuel. However, achieving high yields in this reaction is a substantial challenge. Here it is described how PtCo bimetallic nanoparticles with diameters of 3.6 ± 0.7 nm can solve this problem. Over PtCo catalysts the conversion of HMF was 100% within 10 min and the yield to DMF reached 98% after 2 h, which substantially exceeds the best results reported in the literature. Moreover, the synthetic method can be generalized to other bimetallic nanoparticles encapsulated in hollow carbon spheres.

  6. Controllable Catalysis with Nanoparticles: Bimetallic Alloy Systems and Surface Adsorbates

    KAUST Repository

    Chen, Tianyou

    2016-05-16

    Transition metal nanoparticles are privileged materials in catalysis due to their high specific surface areas and abundance of active catalytic sites. While many of these catalysts are quite useful, we are only beginning to understand the underlying catalytic mechanisms. Opening the “black box” of nanoparticle catalysis is essential to achieve the ultimate goal of catalysis by design. In this Perspective we highlight recent work addressing the topic of controlled catalysis with bimetallic alloy and “designer” adsorbate-stabilized metal nanoparticles.

  7. Preparation of promoted platinum catalysts of designed geometry and the role of promoters in the liquid-phase oxidation of 1-methoxy-2-propanol

    Energy Technology Data Exchange (ETDEWEB)

    Mallat, T.; Bodnar, Z.; Baiker, A. (Swiss Federal Institute of Technology, Zuerich (Switzerland)); Greis, O.; Struebig, H. (Technical Univ., Hamburg (Germany)); Reller, A. (Univ. of Hamburg (Germany))

    1993-07-01

    Alumina-supported or unsupported M/Pt-type catalysts were prepared by consecutive reduction of Bi, Pb, Sn, Ru, Au, or Ag modifiers (M) onto Pt particles. Structural and chemical properties of the bimetallics were studied by electron microscopy combined with energy dispersive X-ray analysis and an electrochemical (cyclic voltammetric) polarization method. Preferential deposition of promoter metal submonolayers on Pt was observed at moderate surface coverages ([theta][sub M]<0.5-0.8). Some bulk metal crystallite formation as [open quotes]bridges[close quotes] between small Pt particles covered partially with promoter was also observed on alumina-supported Bi/Pt and Pb/Pt catalysts. Measurement of the electrochemical potential of the catalyst slurry during the oxidation of 1-methoxy-2-propanol to methoxyacetone and the cyclic voltammetric polarization of the bimetallic catalysts revealed that the catalysts are in an oxidized state during reaction. The following order of promoting influence was observed: Bi > Pb [approximately] Sn > Au [approximately] Ru. Two major effects of promoters are suggested: (i) they suppress the initial irreversible adsorption of the reactant alcohol on Pt which results in self-poisoning, and (ii) they form new active centers that adsorb the oxidizing species (OH) better than Pt. A formal rate equation is suggested (r = f [center dot] [theta][sub org] [center dot] [theta][sub OH]) which explains the optimum in promoter/platinum ratio. The different influences of the promoters are explained by their hydrogen and oxygen sorption characteristics and by the surface geometry of the bimetallic catalysts. 51 refs., 12 figs., 1 tab.

  8. Monometallic Pd and Pt and Bimetallic Pd-Pt/Al2O3-TiO2 for the HDS of DBT: Effect of the Pd and Pt Incorporation Method

    Directory of Open Access Journals (Sweden)

    Reynaldo Martínez Guerrero

    2014-01-01

    Full Text Available The effect of the preparation method of monometallic Pd and Pt and bimetallic Pd-Pt/Al2O3-TiO2 catalysts on the hydrodesulfurization (HDS of dibenzothiophene (DBT was investigated in this study. The synthesis was accomplished using three methods: (A impregnation, (B metal organic chemical vapor deposition (MOCVD, and (C impregnation-MOCVD. The bimetallic Pd-Pt catalyst prepared by the impregnation-MOCVD method was most active for the HDS of DBT compared to those prepared by the single impregnation or MOCVD method due to the synergetic effect between both noble metals. The greater selectivity toward biphenyl indicated that this bimetallic Pd-Pt catalyst preferentially removes sulfur via the direct desulfurization mechanism. However, the bimetallic Pd-Pt catalyst prepared using the single MOCVD method did not produce any cyclohexylbenzene, which is most likely associated with the hydrogenation/dehydrogenation sites.

  9. Kinetics of Oxidation of L-Leucine by Mono-and Bimetallic Gold and Silver Nanoparticles in Hydrogen Peroxide Solution

    Institute of Scientific and Technical Information of China (English)

    P.VENKATESAN; J.SANTHANALAKSHMI

    2012-01-01

    The catalytic activity of surfactant stabilized mono- and bimetallic Au and Ag nanoparticles for the oxidation of an amino acid,L-leucine,was studied using hydrogen peroxide as the oxidant.The Au and Ag nanoparticle catalysts exhibited very good catalytic activity and the kinetics of the reaction were found to be pseudo-first order with respect to the amino acid.The effects of several factors,such as oxidant concentration,ionic strength,pH,and catalyst concentration on the reaction,were also investigated.In particular,optimal oxidant and catalyst concentrations were determined.Very high concentrations of the metal nano-catalysts or the oxidant led to a dramatic increase in reaction rate.Moreover,bimetallic Au-Ag catalysts provided higher selectivity than pure Au or Ag.

  10. Preparation and Characterization of Polymer-Stabilized Ruthenium-Platinum and Ruthenium-Palladium Bimetallic Colloids and Their Catalytic Properties for Hydrogenation of o-Chloronitrobenzene.

    Science.gov (United States)

    Liu; Yu; Liu; Zheng

    1999-06-15

    Colloidal dispersions of poly(N-vinyl-2-pyrrolidone) (PVP)-stabilized ruthenium-platinum and ruthenium-palladium bimetallic colloids were prepared by NaBH4 reduction of the corresponding mixed-metal salts at room temperature and characterized by TEM, XPS, and XRD. The resulting bimetallic colloids were used as catalysts for the selective hydrogenation of o-chloronitrobenzene (o-CNB) in methanol at 303 K under 0.1 MPa of hydrogen. It was observed that the catalytic performance of PVP-stabilized ruthenium-platinum colloids (PVP-Ru/Pt) and ruthenium-palladium colloids (PVP-Ru/Pd) was dependent on their compositions and could be remarkably affected by some added metal cations. In the presence of cobalt ion, nearly 100% selectivity to o-chloroaniline (o-CAN) was achieved over PVP-Ru/Pt colloids at 100% conversion of o-CNB, with an activity two orders of magnitude higher than that of monometallic PVP-Ru colloid. Copyright 1999 Academic Press. PMID:10339363

  11. Characterization and Preparation of Bimetallic Nanoparticles

    Institute of Scientific and Technical Information of China (English)

    Bing; Joe; Hwang; Ching; Hsiang; Chen; Loka; Subramanyam; Sarma; Din-gao; Liu; Jyh; Fu; Lee

    2007-01-01

    1 Results Bimetallic particles in the nanometer size range are of substantial interest due to their vast applications in catalysis[1].The synthesis of bimetallic nanoparticles with definite size with a well-control over their nanostructure remains a challenging problem.Thus there exists a great demand for both synthesis and atomic level characterization of nanostructure of bimetallic nanoparticles (NPs).With the recent advent of high-intensity tunable sources of X-rays,now available at synchrotron radia...

  12. Enhanced Activity of Supported Ni Catalysts Promoted by Pt for Rapid Reduction of Aromatic Nitro Compounds

    Directory of Open Access Journals (Sweden)

    Huishan Shang

    2016-06-01

    Full Text Available To improve the activities of non-noble metal catalysts is highly desirable and valuable to the reduced use of noble metal resources. In this work, the supported nickel (Ni and nickel-platinum (NiPt nanocatalysts were derived from a layered double hydroxide/carbon composite precursor. The catalysts were characterized and the role of Pt was analysed using X-ray diffraction (XRD, high-resolution transmission electron microscopy (HRTEM, energy dispersive X-ray spectroscopy (EDS mapping, and X-ray photoelectron spectroscopy (XPS techniques. The Ni2+ was reduced to metallic Ni0 via a self-reduction way utilizing the carbon as a reducing agent. The average sizes of the Ni particles in the NiPt catalysts were smaller than that in the supported Ni catalyst. The electronic structure of Ni was affected by the incorporation of Pt. The optimal NiPt catalysts exhibited remarkably improved activity toward the reduction of nitrophenol, which has an apparent rate constant (Ka of 18.82 × 10−3 s−1, 6.2 times larger than that of Ni catalyst and also larger than most of the reported values of noble-metal and bimetallic catalysts. The enhanced activity could be ascribed to the modification to the electronic structure of Ni by Pt and the effect of exposed crystal planes.

  13. The effect of lanthanum addition on the catalytic activity of ?-alumina supported bimetallic Co–Mo carbides for dry methane reforming

    OpenAIRE

    France, Liam J; Du, Xian; Almuqati, Naif; Vladimir L. Kuznetsov; Zhao, Yongxiang; Jiang, Zheng; Xiao, Tiancun; Bagabas, Abdulaziz; Almegren, Hamid; Edwards, Peter P.

    2014-01-01

    The effect of lanthanum addition to ?-alumina supported bimetallic carbides has been studied for the reaction of dry methane reforming using four different lanthanum loading levels of 1, 5, 10 and 15 wt% of lanthanum. It has been demonstrated that the addition of lanthanum to supported bimetallic carbides at low loading levels (1 wt%) results in smaller carbide crystallite sizes compared to catalysts containing either no lanthanum or higher lanthanum loading levels (5–15 wt%). Increased lanth...

  14. Electrocatalytical study of carbon supported Pt, Ru and bimetallic Pt–Ru nanoparticles for oxygen reduction reaction in alkaline media

    Energy Technology Data Exchange (ETDEWEB)

    Hosseini, M.G., E-mail: mg-hosseini@tabrizu.ac.ir; Zardari, P.

    2015-08-01

    Highlights: • Binary catalyst Pt.Ru/C is evaluated towards ORR. • Pt.Ru/C nanoparticles revealed best ORR catalytical activity. • The 120 mV/dec Tafel slope indicated that the first electron transfer is the rds. • The active number sites of Pt.Ru/C catalyst were 3 times higher than Pt/C. - Abstract: Carbon supported Pt, Ru and bimetallic Pt–Ru nanoparticles (Pt/C, Ru/C and Pt.Ru/C) have been prepared by the chemical reduction method. Particle morphology, composition and structure of nanoparticles have been investigated by scanning electron microscopy (SEM) and energy dispersive X-ray (EDX) analysis. SEM results showed a uniform dispersion of nanoparticles with rough and porous structure into carbon supports with the average particle size of 30–64 nm. EDX analysis demonstrated the presence of both Pt and Ru nanoparticles in each gas diffusion electrode. The Pt/C, Ru/C and Pt.Ru/C composites were used as electrocatalyst for oxygen reduction reaction (ORR) in alkaline media. The ORR activities of cathodes were characterized using cyclic voltammetry (CV), polarization technique, AC impedance spectroscopy (EIS) and chronoamperometry. CV and polarization curves showed significantly higher activity on Pt.Ru/C electrocatalyst than observed on Pt/C and Ru/C catalysts, which can be related to synergistic effect, which is playing a critical role in ORR activity. The Tafel slope values of 120 mV/dec showed that the first electron transfer is the rate determining step. The EIS results of cathodes under different polarization potentials indicated two different behaviours which depend on the applied dc potentials and reveal different electrochemical processes occurring on the electrodes.

  15. Pt-Rh/g Al2O3 Influence of Catalyst Preparation Methods on Metallic Particle Dispersion and Size Distribution

    Directory of Open Access Journals (Sweden)

    N.M. da Fonseca

    1998-06-01

    Full Text Available - Pt-Rh/Al2O3 catalysts were prepared by successive incipient impregnations or coimpregnation. Characterization was achieved by H2 chemisorption and transmission electron microscopy. It was verified that method of preparation, ratio of metal weights and sequence of deposition are factors that result in very distinct catalysts.

  16. Synthesis and characterization of bimetallic nanocatalysts and their application in selective hydrogenation of citral to unsaturated alcohols

    Indian Academy of Sciences (India)

    S A Ananthan; R Suresh; K Giribabu; V Narayanan

    2013-11-01

    TiO2-supported bimetallic nanocatalysts were prepared and reduced at two different temperatures, 375°C and 575°C for selective hydrogenation of citral to corresponding unsaturated alcohols (geraniol (GOL) and nerol (NOL)). The nanocatalysts were characterized by difference techniques of Fourier transform infrared spectroscopy (FT-IR), Brunauer, Emmett and Teller (BET) surface area measurement, scanning electron microscopy (SEM), Energy Dispersive X-ray Analysis (EDAX), transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The prepared nanocatalysts are uniformly dispersed with an average particle size of 50-100 nm and zero valence metallic state. Catalysts reduced at higher temperature lead to an increase in selectivity toward unsaturated alcohols (GOL and NOL). The Pt-Ru/TiO2 shows higher activity compared to Pt-Pd/TiO2 and Pt-Au/TiO2 nanocatalysts. In addition, a second metal (Ru) also leads to an increase in GOL and NOL selectivity during citral hydrogenation. Partially generated oxidized second metal species due to the difference in electronegativity, strongly binds the C=O group and also paves the way for selective activation of C=O bond.

  17. Porous Diatomite-Immobilized Cu–Ni Bimetallic Nanocatalysts for Direct Synthesis of Dimethyl Carbonate

    Directory of Open Access Journals (Sweden)

    Yong Chen

    2012-01-01

    Full Text Available A series of diatomite-immobilized Cu–Ni bimetallic nanocatalysts was prepared under ultrasonication and evaluated for the direct synthesis of dimethyl carbonate under various conditions. Upon being fully characterized by TPR, TPD, BET, SEM, XRD, and XPS methodologies, it is found that the bimetallic composite is effectively alloyed and well immobilized inside or outside the pore of diatomite. Under the optimal conditions of 1.2 MPa and 120∘C, the prepared catalyst with loading of 15% exhibited the highest methanol conversion of 6.50% with DMC selectivity of 91.2% as well as more than 10-hour lifetime. The possible reaction mechanism was proposed and discussed in detail. To our knowledge, this is the first report to use diatomite as a catalyst support for direct DMC synthesis from methanol and CO2.

  18. Development of MCM-41 based catalysts for the photo-Fenton's degradation of dye pollutants

    Science.gov (United States)

    Lam, Leung Yuk Frank

    The continuous advancement in most industries has resulted in serious water pollution problems. The industrial effluents contain a variety of highly toxic organics such as dye pollutants. Numerous processes have been demonstrated for treating such pollutants. Among them, photo-Fenton's reaction is effective for organic mineralization by hydroxyl radicals generated from the Fenton's reagents (Fe2+ and H2O2). However, there is a drawback in that it requires a separation system to recover the homogeneous ferrous ion in the treated wastewater. In this research, new heterogeneous Fenton's catalysts are developed to solve such a problem and to achieve an efficient mineralization of dye pollutants. Two methods for catalyst preparation, including sol-gel hydrothermal (SG) and metal-organic chemical vapor deposition (MOCVD) techniques, were studied in this work. For SG-prepared catalysts, the iron element was successfully doped into the MCM-41 structure. These catalysts demonstrated a good catalytic efficiency but leaching of metal ions from the developed catalyst was found. In the MOCVD technique, a rotated tubular reactor system was developed to synthesize Fe/MCM-41 catalyst with uniform metal dispersion. It was found that using oxygen as a carrier gas during metal deposition was able to increase the stability of the deposited metal. In degradation of a model dye pollutant, Orange II, a total of 85% TOC mineralization was achieved at pH 3. A disadvantage of using Fe/MCM-41 was the reduced efficiency at higher pH. Cu/MCM-41 was thus developed and showed better catalytic activities than Fe/MCM-41 at neutral pH. Having the specific catalytic properties of Fe/MCM-41 and Cu/MCM-41, bimetallic (Fe+Cu) catalysts supported on MCM-41 were developed which show better activities in the Orange II mineralization than those monometallic (Fe or Cu) catalysts. The preparation conditions of the catalysts were experimentally optimized. The effects of catalyst dosage, metal loading

  19. Advanced liquefaction using coal swelling and catalyst dispersion techniques. Volume 1, Final technical report, October 1, 1991--September 30, 1994

    Energy Technology Data Exchange (ETDEWEB)

    Curtis, C.W. [Auburn Univ., (United States); Gutterman, C. [Foster Wheeler Development Corp., Livingston, NJ (United States); Chander, S. [Pennsylvania State Univ., (United States)

    1994-12-31

    The overall objective of this project was to develop a new approach for the direct liquefaction of coal to produce an all-distillate product slate at a sizable cost reduction over current technology. The approach integrated coal selection, pretreatment, coal swelling with catalyst impregnation, liquefaction, product recovery with characterization, alternate bottoms processing, and a technical assessment including an economic evaluation. Heterofunctional solvents were the most effective in swelling coals. Also solvent blends such as isopropanol/water were more effective than pure solvents alone. Impregnating slurry catalysts simultaneously during coal swelling showed that better uptake was achieved with nonswelling solvent and higher impregnation temperature. Some enhancement in initial coal conversion was seen liquefying SO{sub 2}-treated Black Thunder coal with slurry catalysts, and also when hydrogen donor liquefaction solvents were used. Noncatalytic reactions showed no benefit from SO{sub 2} treatment. Coupling coal swelling and SO{sub 2} treatment with slurry catalysts was also not beneficial, although high conversion was seen with continuous operation and long residence time, however, similar high conversion was observed with untreated coal. SO{sub 2} treatment is not economically attractive unless it provides about 17% increase in coal reactivity. In most cases, the best results were obtained when the coal was untreated and the slurry catalyst was added directly into the reactor. Foster Wheeler`s ASCOT process had better average liquid yields than either Wilsonville`s vacuum tower/ROSE combination or delayed coking process. This liquid product also had good quality.

  20. Water-dispersable hybrid Au-Pd nanoparticles as catalysts in ethanol oxidation, aqueous phase Suzuki-Miyaura and Heck reactions

    KAUST Repository

    Song, HyonMin

    2012-01-01

    The catalytic activities of water-dispersable Au@Pd core-shell nanoparticles (NPs) and Au-Pd alloy NPs were examined. There is growing interest in Au-Pd hybridized NPs in a supported matrix or non-supported forms as catalysts in various reactions that are not limited to conventional Pd-related reactions. Four different Au@Pd core-shell NPs in this study were prepared at room temperature with help from the emulsion phase surrounding the Au core NPs. Au-Pd alloy NPs were prepared over 90 °C, and underwent phase transfer to aqueous medium for their catalytic use. Au@Pd core-shell NPs show catalytic activity in ethanol oxidation reactions as electrocatalysts, and both core-shell and alloy NPs are good to excellent catalysts in various Suzuki-Miyaura and Heck reactions as heterogeneous catalysts. Specifically, Au@Pd core-shell NPs with sharp branched arms show the highest yield in the reactions tested in this study. A relatively small amount (0.25 mol%) was used throughout the catalytic reactions. © 2012 The Royal Society of Chemistry.

  1. Catalyst dispersion and activity under conditions of temperature- staged liquefaction. Technical progress report, January--March 1992

    Energy Technology Data Exchange (ETDEWEB)

    Davis, A.; Schobert, H.H.; Mitchell, G.D.; Artok, L.

    1992-07-01

    Two coals, a Texas subbituminous C and a Utah high volatile A bituminous, were used to examine the effects of solvent swelling and catalyst impregnation on liquefaction conversion behavior in temperature staged reactions for 30 minutes each at 275{degree} and 425{degree}C in H{sub 2} and 95:5 H{sub 2}:H{sub 2}S atmospheres. Methanol, pyridine, tetrahydrofuran, and tetrabutylammonium hydroxide were used as swelling agents. Molybdenum-based catalyst precursors were ammonium tetrathiomolybdate, molybdenum trisulfide, molybdenum hexacarbonyl, and bis(tricarbonylcyclopentadienyl-molybdenum). Ferrous sulfate and bis(dicarbonylcyclo-pentadienyliron) served as iron-based catalyst precursors. In addition, ion exchange was used for loading iron onto the subbituminous coal. For most experiments, liquefaction in H{sub 2}:H{sub 2}S was superior to that in H{sub 2}, regardless of the catalyst precursor. The benefit of the H{sub 2}S was greater for the subbituminous, presumably because of its higher iron content relative to the hvab coal. Tetrabutylammonium hydroxide was the only swelling agent to enhance conversion of the hvab coal significantly; it also caused a remarkable increase in conversion of the subbituminous coal. The combined application of solvent swelling and catalyst impregnation also improves liquefaction, mainly through increased oil yields from the hvab coal and increased asphaltenes from the subbituminous. A remarkable effect from use of ammonium tetrathiomolybdate as a catalyst precursor is substantial increase in pristane and phytane yields. Our findings suggest that these compounds are, at least in part, bound to the coal matrix.

  2. Dispersion state and catalytic properties of vanadia species on the surface of V2O5/TiO2 catalysts

    Institute of Scientific and Technical Information of China (English)

    许波连; 范以宁; 刘浏; 林明; 陈懿

    2002-01-01

    The dispersion state and catalytic properties of anatase-supported vanadia species are studied by means of X-ray diffraction (XRD), laser Raman spectroscopy (LRS), H2 temperature-programmed reduction (TPR) and the selective oxidation of o-xylene to phthalic anhydride. The almost identical values of the experimental dispersion capacity of V2O5 on anatase and the surface vacant sites available on the preferentially exposed (001) plane of anatase suggest that the highly dispersed vanadium cations are bonded to the vacant sites on the surface of anatase as derived by the incorporation model. When the loading amount of V2O5 is far below its dispersion capacity, the dispersed vanadia species might mainly consist of isolated VOx species bridging to the surface through V-O-Ti bonds. With the increase of V2O5 loading the isolated vanadia species interact with their nearest neighbors (either isolated or polymerized vanadia) through bridging V-O-V at the expenses of V-O-Ti bonds, resulting in the increase of the ratio of polymerized to isolated vanadia species and the decrease of the reactivity of the associated surface oxygen anions and, consequently, although the activity increases with loading to reach a maximum value, the turn over number (TON) of the V2O5/TiO2 catalyst decreases linearly. When the loading amount of V2O5 is higher than its dispersion capacity, the turn over number decreases more rapidly with the increase of V2O5 loading due to the formation of V2O5 crystallites in which the oxygen anions associated with V-O-V bonds are less reactive and only partially exposed on the surface.

  3. Nanopore and nanoparticle catalysts.

    Science.gov (United States)

    Thomas, J M; Raja, R

    2001-01-01

    The design, atomic characterization, performance, and relevance to clean technology of two distinct categories of new nanocatalysts are described and interpreted. Exceptional molecular selectivity and high activity are exhibited by these catalysts. The first category consists of extended, crystallographically ordered inorganic solids possessing nanopores (apertures, cages, and channels), the diameters of which fall in the range of about 0.4 to about 1.5 nm, and the second of discrete bimetallic nanoparticles of diameter 1 to 2 nm, distributed more or less uniformly along the inner walls of mesoporous (ca. 3 to 10 nm diameter) silica supports. Using the principles and practices of solid-state and organometallic chemistry and advanced physico-chemical techniques for in situ and ex situ characterization, a variety of powerful new catalysts has been evolved. Apart from those that, inter alia, simulate the behavior of enzymes in their specificity, shape selectivity, regio-selectivity, and ability to function under ambient conditions, many of these new nanocatalysts are also viable as agents for effecting commercially significant processes in a clean, benign, solvent-free, single-step fashion. In particular, a bifunctional, molecular sieve nanopore catalyst is described that converts cyclohexanone in air and ammonia to its oxime and caprolactam, and a bimetallic nanoparticle catalyst that selectively converts cyclic polyenes into desirable intermediates. Nanocatalysts in the first category are especially effective in facilitating highly selective oxidations in air, and those in the second are well suited to effecting rapid and selective hydrogenations of a range of organic compounds.

  4. Bimetallic nanoparticles for arsenic detection.

    Science.gov (United States)

    Moghimi, Nafiseh; Mohapatra, Mamata; Leung, Kam Tong

    2015-06-01

    Effective and sensitive monitoring of heavy metal ions, particularly arsenic, in drinking water is very important to risk management of public health. Arsenic is one of the most serious natural pollutants in soil and water in more than 70 countries in the world. The need for very sensitive sensors to detect ultralow amounts of arsenic has attracted great research interest. Here, bimetallic FePt, FeAu, FePd, and AuPt nanoparticles (NPs) are electrochemically deposited on the Si(100) substrate, and their electrochemical properties are studied for As(III) detection. We show that trace amounts of As(III) in neutral pH could be determined by using anodic stripping voltammetry. The synergistic effect of alloying with Fe leads to better performance for Fe-noble metal NPs (Au, Pt, and Pd) than pristine noble metal NPs (without Fe alloying). Limit of detection and linear range are obtained for FePt, FeAu, and FePd NPs. The best performance is found for FePt NPs with a limit of detection of 0.8 ppb and a sensitivity of 0.42 μA ppb(-1). The selectivity of the sensor has also been tested in the presence of a large amount of Cu(II), as the most detrimental interferer ion for As detection. The bimetallic NPs therefore promise to be an effective, high-performance electrochemical sensor for the detection of ultratrace quantities of arsenic. PMID:25938763

  5. 铁铜双金属催化剂选择性催化氧化氨为氮气%Selective Catalytic Oxidation of Ammonia to Nitrogen over Iron and Copper Bimetallic Catalysts

    Institute of Scientific and Technical Information of China (English)

    孙萌萌; 曹毅; 兰丽; 邹莎; 房志涛; 陈耀强

    2014-01-01

    Iron and copper bimetal ic catalysts with fixed total contents of copper and iron were prepared by a co-impregnation method, and then used for selective catalytic oxidation of ammonia to nitrogen. The properties of the catalysts were characterized by N2 adsorption-desorption, H2 temperature-programmed reduction (H2-TPR), NH3 temperature-programmed desorption (NH3-TPD), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The iron and copper bimetal ic catalysts exhibited good activity and high selectivity of N2 at the gas hourly space velocity (GHSV) of 100000 h-1. The activity and N2 selectivity in the low temperature range increased with increasing Cu loading, whereas in the high temperature range (above 400 ° C) the selectivity of N2 was directly related to the content of iron. The highest NH3 conversion was achieved at about 350 °C for Fe0.25Cu0.75/ZSM-5, and the N2 selectivity was up to 97%at 300 °C. On the other hand, the extremely high N2 selectivity about 98%was obtained over Fe0.75Cu0.25/ZSM-5 at 500 °C. In addition, N2O as the by-product and greenhouse gas was obtained in very low amounts for al the catalysts. The characterization results showed that the activity was influenced by the acid content and the amounts of copper species. Moreover, the highly reducing capacity could improve the N2 selectivity.%固定铜铁的总质量不变,采用共浸渍法制备铜铁双金属催化剂.为了更好地了解催化剂的性质,分别用N2吸附-脱附、H2-程序升温还原(H2-TPR)、NH3-程序升温脱附(NH3-TPD)、X射线衍射(XRD)和X射线光电子能谱(XPS)方法对制备的催化剂进行表征.研究发现在100000 h-1空速下,铜铁双金属催化剂呈现出好的活性和氮气选择性.在低温区,随着铜含量的增加,活性和氮气的选择性增加,然而在高温区氮气的选择性直接和铁的含量相关.其中催化剂Fe0.25Cu0.75/ZSM-5,在350° C氨的转化率达到最高,在300° C

  6. Bimetallic Nanocatalysts in Mesoporous Silica for Hydrogen Production from Coal-Derived Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Kuila, Debasish; Ilias, Shamsuddin

    2013-02-13

    In steam reforming reactions (SRRs) of alkanes and alcohols to produce H2, 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), N2 adsorption, and Transmission electron microscopy (TEM) techniques. The BET surface area of MCM-41 (~1000 m2/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

  7. Bimetallic materials for large diameter pipelines

    International Nuclear Information System (INIS)

    The results are presented of the investigation of bimetallic pipes made of Ni-Mn-Mo-V + Cb08Kh19N10G2B steel and of 19MN5 (type 22K) + SB 08Kh19N10G2B steels, manufactured in Japan for piping nuclear power stations for service under corrosion attack by coolants at high both pressure and temperature and under heavy cyclic loads. The procedures are described for manufacturing elements of piping from bimetallic seamless large-diameter pipes. A study has been made of the variation in bimetallic microstructure of the short-time mechanical properties, of the impact strength, of the critical brittleness point in initial and aged states of the cyclic strength and of the strength of the bimetallic joint

  8. Partial oxidation of methane over bimetallic copper- and nickel-actinide oxides (Th, U)

    International Nuclear Information System (INIS)

    The study of partial oxidation of methane (POM) over bimetallic nickel- or copper-actinide oxides was undertaken. Binary intermetallic compounds of the type AnNi2 (An = Th, U) and ThCu2 were used as precursors and the products (2NiO.UO3, 2NiO.ThO2 and 2CuO.ThO2) characterized by means of X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy and temperature-programmed reduction. The catalysts were active and selective for the conversion of methane to H2 and CO and stable for a period of time of ∼18 h on stream. The nickel catalysts were more active and selective than the copper catalyst and, under the same conditions, show a catalytic behaviour comparable to that of a platinum commercial catalyst, 5 wt% Pt/Al2O3. The catalytic activity increases when uranium replaces thorium and the selectivity of this type of materials is clearly different from that of single metal oxides and/or mechanical mixtures. The good catalytic behaviour of the bimetallic copper- and nickel-actinide oxides was attributed to an unusual interaction between copper or nickel oxide and the actinide oxide phase as showed by H2-TPR, XPS and Raman analysis of the catalysts before and after reaction.

  9. Dehalogenation of Aryl Halides Catalyzed by Montmorillonite Immobilized Bimetal Catalyst in Aqueous System

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    A novel bisupported bimetal catalyst PVP-PdCl2-FeSO4/Al-Mont-PEG600 was prepared by immobilization of PVP (poly (N-vinyl-2-pyrrolidone)) supported bimetallic catalyst using alumina pillared inartificial montmorillonite as the carrier. This catalyst has good dehalogenation activity and selectivity to aryl halides-o-chlorotoluene in aqueous system in the presence of phase transfer catalyst (PEG) and sodium formate as hydrogen source. The catalyst also shows good reusability.

  10. Mechanical alloying of a hydrogenation catalyst used for the remediation of contaminated compounds

    Science.gov (United States)

    Quinn, Jacqueline W. (Inventor); Clausen, Christian A. (Inventor); Geiger, Cherie L. (Inventor); Aitken, Brian S. (Inventor)

    2012-01-01

    A hydrogenation catalyst including a base material coated with a catalytic metal is made using mechanical milling techniques. The hydrogenation catalysts are used as an excellent catalyst for the dehalogenation of contaminated compounds and the remediation of other industrial compounds. Preferably, the hydrogenation catalyst is a bimetallic particle including zero-valent metal particles coated with a catalytic material. The mechanical milling technique is simpler and cheaper than previously used methods for producing hydrogenation catalysts.

  11. Cr-free Co-Cu/SBA-15 catalysts for hydrogenation of biomass-derivedα-,β-unsaturated aldehyde to alcohol

    Institute of Scientific and Technical Information of China (English)

    Sanjay Srivastava; Pravakar Mohanty; Jigisha K. Parikh; Ajay K. Dalai; S. S. Amritphale; Anup K. Khare

    2015-01-01

    Cr-free bi-metallic SBA-15-supported Co–Cu catalysts were examined in the conversion of bio-mass-derived α-, β-unsaturated aldehyde (furfural) to value-added chemical furfuryl alcohol (FOL). Co–Cu/SBA-15 catalysts with a fixed Cu loading of 10 wt% and varying Co loadings (2.5, 5, and 10 wt%) were prepared by the impregnation method. The catalysts were characterized by X-ray dif-fraction, N2 sorption, H2 temperature-programmed reduction, scanning electron microscopy, ener-gy-dispersive X-ray spectroscopy, high-resolution transmission electron microscopy, CO chemi-sorption, and inductively coupled plasma mass spectrometry. The influence of different reaction parameters such as temperature, pressure, catalyst dosage, and furfural concentration on the cata-lyst performance was evaluated. Relative to catalysts supported on amorphous silica, the current SBA-15-supported Co–Cu catalysts displayed higher performance, attaining a furfural conversion of 99% and furfuryl alcohol selectivity of 80%. The catalytic reactions were conducted in a 100-mL autoclave at 170 °C and 2 MPa H2 pressure for 4 h.

  12. Bimetallic nanoalloys in heterogeneous catalysis of industrially important reactions: synergistic effects and structural organization of active components

    International Nuclear Information System (INIS)

    The review is concerned with correlations between the synergistic effects and structural organization of the surface of bimetallic alloys that are used as active components of catalysts for selective hydrogenation of organic compounds and for CO oxidation in hydrogen-rich mixtures. Studies on the preparation of novel highly efficient catalysts using modern theoretical approaches, computer-assisted molecular design and original synthetic procedures are considered. It is shown that introduction of the second metal into the monometallic catalyst and subsequent formation of alloy particles with modified structure of the surface and near-surface layers leads to nonadditive enhancement of catalytic activity and/or selectivity. The bibliography includes 203 references

  13. Controlling the dispersion of supported polyoxometalate heterogeneous catalysts: impact of hybridization and the role of hydrophilicity–hydrophobicity balance and supramolecularity

    Directory of Open Access Journals (Sweden)

    Gijo Raj

    2014-10-01

    Full Text Available The hybridization of polyoxometalates (POMs through an organic–inorganic association offers several processing advantages in the design of heterogeneous catalysts. A clear understanding of the organization of these hybrid materials on solid surfaces is necessary to optimise their properties. Herein, we report for the first time the organization of Keggin phosphotungstic [PW12O40]3− and Wells–Dawson (WD phosphomolybdic [P2Mo18O62]6− anions deposited on mica (hydrophilic, and highly oriented pyrolytic graphite (HOPG (hydrophobic surfaces. Next, the supramolecular organization of the organic–inorganic hybrid materials formed from the association of POM anions and dimethyldioctadecylammonium bromide (DODA is investigated as a function of the hydrophilic or hydrophobic nature of the surfaces. The height of the Keggin-POM anions, measured with tapping mode (TM-AFM is always in good agreement with the molecular dimension of symmetric Keggin-POM anions (ca. 1 nm. However, the asymmetric WD-POM anions form monolayer assemblies on the surfaces with the orientation of their long molecular axis (ca. 1.6 nm depending on the hydrophilic or hydrophobic properties of the substrate. Namely, the long axis is parallel on mica, and perpendicular on HOPG. When hybridized with DODA, the organization of the hybrid material is dictated by the interaction of the alkyl side chains of DODA with the substrate surface. On HOPG, the DODA–POM hybrid forms small domains of epitaxially arranged straight nanorod structures with their orientation parallel to each other. Conversely, randomly distributed nanospheres are formed when the hybrid material is deposited on freshly cleaved mica. Finally, a UV–ozone treatment of the hybrid material allows one to obtain highly dispersed isolated POM entities on both hydrophilic and hydrophobic surfaces. The hybridization strategy to prevent the clustering of POMs on various supports would enable to develop highly dispersed POM

  14. Catalysts and process for liquid hydrocarbon fuel production

    Energy Technology Data Exchange (ETDEWEB)

    White, Mark G.; Ranaweera, Samantha A.; Henry, William P.

    2016-08-02

    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 distillates, gasoline components, and lower molecular weight gaseous olefins in one reactor or step. The invention utilizes a novel supported bimetallic ion complex catalyst for conversion, and provides methods of preparing such novel catalysts and use of the novel catalysts in the process and system of the invention.

  15. Comparison between a Water-Based and a Solvent-Based Impregnation Method towards Dispersed CuO/SBA-15 Catalysts: Texture, Structure and Catalytic Performance in Automotive Exhaust Gas Abatement

    Directory of Open Access Journals (Sweden)

    Qi Xin

    2016-10-01

    Full Text Available Supported copper oxide nanoparticles are a potential candidate for replacing the rare and expensive precious metals within the automotive three-way catalyst. However, a well-designed dispersion method is necessary to allow a stable high loading of active material, compensating its lower intrinsic activity and stability. In this work, a CuO-loaded SBA-15 catalyst has been manufactured by two methods. The ammonia-driven deposition precipitation (ADP and the molecular designed dispersion (MDD methods are both considered as efficient deposition methods to provide well-dispersed copper oxide-based catalysts. Their morphology, copper dispersion and the chemical state of copper were characterized and compared. Due to the differences in the synthesis approach, a difference in the obtained copper oxide phases has been observed, leading to a distinct behavior in the catalytic performance. The structure-activity correlation of both catalysts has also been revealed for automotive exhaust gas abatement. Results demonstrate that various copper species can be formed depending on the precursor–support interaction, affecting selectivity and conversion during the catalytic reaction.

  16. Use of Citric Acid in Synthesizing a Highly Dispersed Copper Catalyst for Selective Hydrogenolysis%采用柠檬酸合成高分散铜催化剂用于选择氢解反应

    Institute of Scientific and Technical Information of China (English)

    Ming-Hoong LOOI; Shuk-Tong LEE; Sharifah Bee ABD-HAMID

    2008-01-01

    A highly dispersed Cu catalyst supported on silica was prepared by an incipient wetness impregnation method with citric acid. The synthesis was studied by nitrogen physisorption, X-ray diffraction, and temperature-programmed reduction by comparing with a reference prepared without citric acid. The catalyst precursor obtained after impregnation was X-ray amorphous. The precursor was readily transformed to crystalline CuO upon calcination. The CuO particles were of uniform size in a highly dispersed state and can be reduced to Cu at a lower temperature. The activity of the Cu catalyst obtained was an order of magnitude higher than that of the reference for the hydrogenolysis of methyl laurate to dodecanol.

  17. 4,6-Dimethyl-dibenzothiophene conversion over Al{sub 2}O{sub 3}-TiO{sub 2}-supported noble metal catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Nunez, Sara [Departamento de Ingenieria de Procesos e Hidraulica, Universidad Autonoma Metropolitana-Iztapalapa, San Rafael Atlixco 186, Vicentina, Iztapalapa, 09340, Mexico, D.F. (Mexico); Escobar, Jose, E-mail: jeaguila@imp.mx [Instituto Mexicano del Petroleo, Eje Central Lazaro Cardenas 152, San Bartolo Atepehuacan, Gustavo A. Madero, 07730, Mexico, D.F. (Mexico); Vazquez, Armando; Reyes, Jose Antonio de los [Departamento de Ingenieria de Procesos e Hidraulica, Universidad Autonoma Metropolitana-Iztapalapa, San Rafael Atlixco 186, Vicentina, Iztapalapa, 09340, Mexico, D.F. (Mexico); Hernandez-Barrera, Melissa [Instituto Mexicano del Petroleo, Eje Central Lazaro Cardenas 152, San Bartolo Atepehuacan, Gustavo A. Madero, 07730, Mexico, D.F. (Mexico)

    2011-03-15

    Research highlights: {yields} Al{sub 2}O{sub 3} and Al{sub 2}O{sub 3}-TiO{sub 2} (molar ratio Al/Ti = 2, AT2) mixed oxides were pore-filling impregnated to obtain Pd, Pt and Pd-Pt catalysts with {approx}1 wt% nominal metal loading. {yields} Reduced catalysts were tested in the 4,6-dimethyl-dibenzothiophene hydrodesulfurization (HDS). {yields} In Pd-containing materials, TiO{sub 2} incorporation into the alumina support was favorable to the catalytic activity of noble metal catalysts. {yields} Enhanced intrinsic activity (per exposed metallic site) was obtained in Pt-containing catalysts supported on the AT2 mixed oxide. {yields} Yield to different products over various catalysts seemed to be strongly influenced by metallic particles dispersion. - Abstract: Al{sub 2}O{sub 3} and Al{sub 2}O{sub 3}-TiO{sub 2} (molar ratio Al/Ti = 2, AT2) mixed oxides were synthesized using a low-temperature sol-gel method and were further pore-filling impregnated to obtain Pd and Pt catalysts with {approx}1 wt% nominal metal loading. Simultaneous impregnation was used to prepare bimetallic materials at Pd:Pt = 80:20. Solids characterization was carried out by N{sub 2}-physisorption, high-resolution transmission electron microscopy (HR-TEM and E-FTEM), X-ray diffraction, temperature-programmed reduction and CO-chemisorption. Reduced (350 deg. C, H{sub 2} flow) catalysts were tested in the 4,6-dimethyl-dibenzothiophene hydrodesulfurization (HDS) (in n-dodecane, at 300 deg. C and 5.5 MPa, batch reactor). In Pd-containing materials, TiO{sub 2} incorporation into the alumina support was favorable to the catalytic activity of noble metal catalysts, where bimetallic Pd-Pt with AT2 carrier had the highest organo-S compound conversion. Enhanced intrinsic activity (per exposed metallic site) was obtained in Pt-containing catalysts supported on the AT2 mixed oxide (as compared to alumina-supported ones). Yield to different products over various catalysts seemed to be strongly influenced by

  18. Catalytic Activity of Mono- and Bi-Metallic Nanoparticles Synthesized via Microemulsions

    Directory of Open Access Journals (Sweden)

    Ramona Y.G. König

    2014-07-01

    Full Text Available Water-in-oil (w/o microemulsions were used as a template for the synthesis of mono- and bi-metallic nanoparticles. For that purpose, w/o-microemulsions containing H2PtCl6, H2PtCl6 + Pb(NO32 and H2PtCl6 + Bi(NO3, respectively, were mixed with a w/o-microemulsion containing the reducing agent, NaBH4. The results revealed that it is possible to synthesize Pt, PtPb and PtBi nanoparticles of ~3–8 nm in diameter at temperatures of about 30°C. The catalytic properties of the bimetallic PtBi and PtPb nanoparticles were studied and compared with monometallic platinum nanoparticles. Firstly, the electrochemical oxidation of formic acid to carbon monoxide was investigated, and it was found that the resistance of the PtBi and PtPb nanoparticles against the catalyst-poisoning carbon monoxide was significantly higher compared to the Pt nanoparticles. Secondly, investigating the reduction of 4-nitrophenol to 4-aminophenol,we found that the bimetallic NPs are most active at 23 °C, while the order of the activity changes at higher temperatures, i.e., that the Pt nanoparticles are the most active ones at 36 and 49 °C. Furthermore, we observed a strong influence of the support, which was either a polymer or Al2O3. Thirdly, for the hydrogenation of allylbenzene to propylbenzene, the monometallic Pt NPs turned out to be the most active catalysts, followed by the PtPb and PtBi NPs. Comparing the two bimetallic nanoparticles, one sees that the PtPb NPs are significantly more active than the respective PtBi NPs.

  19. Correlation between Fischer-Tropsch catalytic activity and composition of catalysts

    Directory of Open Access Journals (Sweden)

    Subbarao Duvvuri

    2011-11-01

    Full Text Available Abstract This paper presents the synthesis and characterization of monometallic and bimetallic cobalt and iron nanoparticles supported on alumina. The catalysts were prepared by a wet impregnation method. Samples were characterized using temperature-programmed reduction (TPR, temperature-programmed oxidation (TPO, CO-chemisorption, transmission electron microscopy (TEM, field emission scanning electron microscopy (FESEM-EDX and N2-adsorption analysis. Fischer-Tropsch synthesis (FTS was carried out in a fixed-bed microreactor at 543 K and 1 atm, with H2/CO = 2 v/v and space velocity, SV = 12L/g.h. The physicochemical properties and the FTS activity of the bimetallic catalysts were analyzed and compared with those of monometallic cobalt and iron catalysts at similar operating conditions. H2-TPR analysis of cobalt catalyst indicated three temperature regions at 506°C (low, 650°C (medium and 731°C (high. The incorporation of iron up to 30% into cobalt catalysts increased the reduction, CO chemisorption and number of cobalt active sites of the catalyst while an opposite trend was observed for the iron-riched bimetallic catalysts. The CO conversion was 6.3% and 4.6%, over the monometallic cobalt and iron catalysts, respectively. Bimetallic catalysts enhanced the CO conversion. Amongst the catalysts studied, bimetallic catalyst with the composition of 70Co30Fe showed the highest CO conversion (8.1% while exhibiting the same product selectivity as that of monometallic Co catalyst. Monometallic iron catalyst showed the lowest selectivity for C5+ hydrocarbons (1.6%.

  20. Hierarchical paramecium-like hollow and solid Au/Pt bimetallic nanostructures constructed using goethite as template

    Energy Technology Data Exchange (ETDEWEB)

    Liu Wei; Repo, Eveliina; Sillanpaeae, Mika [Laboratory of Applied Environmental Chemistry, University of Eastern Finland, Patteristonkatu 1, FI-50100 Mikkeli (Finland); Heikkilae, Mikko; Leskelae, Markku, E-mail: weiliuzk@yahoo.cn, E-mail: mika.sillanpaa@uef.fi [Laboratory of Inorganic Chemistry, Department of Chemistry, University of Helsinki, PO Box 55 (A.I. Virtasen aukio 1), FI-00014, Helsinki (Finland)

    2010-10-01

    Novel hollow and solid paramecium-like hierarchical Au/Pt bimetallic nanostructures were constructed using goethite as template via a seed-mediated growth method. Transmission electron microscopy (TEM), {xi}-potential measurement, UV-vis spectroscopy, energy dispersive x-ray spectroscopy (EDS), ICP-AES measurement, x-ray powder diffraction (XRD) and x-ray photoelectron spectroscopy (XPS) were utilized to systematically characterize the bimetallic nanostructures. It is found that the core structure of the paramecium-like bimetallic nanomaterial is closely related to reducing agent. When ascorbic acid is used as reducing agent, goethite serves as in situ sacrificed template and hollow paramecium-like bimetallic structure is obtained. When NH{sub 2}OH{center_dot}HCl is used, solid nanostructure with preserved goethite core is produced. Heating the reaction solution is necessary to obtain the paramecium-like morphology with rough interconnected Pt cilia shell. The thickness of Pt cilia layer can be controlled by adjusting the molar ratio of H{sub 2}PtCl{sub 6} to Au nanoseeds. The overgrowth of the rough Pt cilia is proposed to be via an autocatalytic and three-dimensional heterogeneous nucleation process first through flower-like morphology. Both the hollow and solid hierarchical paramecium-like Au/Pt bimetallic nanostructures show good catalytic activities.

  1. Effect of titania on the characteristics of a Tin-Platinum catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Morales-Gil, P., E-mail: moralesp@imp.mx; Nava, N. [Instituto Mexicano del Petróleo (Mexico); Baggio-Saitovitch, E. [Centro Brasileiro de Pesquisas Físicas (Brazil)

    2015-06-15

    Pt-Sn bimetallic catalysts dispersed on alumina are commonly used for reforming and dehydrogenation reactions. In this research work, Pt and Sn were supported on titania. The resulting interactions between the components in the prepared samples, before and after treatment with hydrogen, were studied by Mössbauer spectroscopy, X-ray diffraction and Rietveld refinement. The results show the presence of Pt and SnO{sub 2} after calcinations. After the reduction process, metallic Pt, PtSn, and Pt{sub 3}Sn alloys were identified. The Rietveld refinement analysis shows that some Ti{sup 4+} atoms were replaced by Sn{sup 4+} atoms in the titania structure. Finally, the Mössbauer spectroscopy and X-ray diffraction results indicate that metallic platinum and SnO{sub 2} are encapsulated by a TiOx layer.

  2. Magneto-optical response in bimetallic metamaterials

    CERN Document Server

    Atmatzakis, Evangelos; Fedotov, Vassili; Vienne, Guillaume; Zheludev, Nikolay I

    2016-01-01

    We demonstrate resonant Faraday polarization rotation in plasmonic arrays of bimetallic nano-ring resonators consisting of Au and Ni sections. This metamaterial design allows to optimize the trade-off between the enhancement of magneto-optical effects and plasmonic dissipation. Although Ni sections correspond to as little as ~6% of the total surface of the metamaterial, the resulting magneto-optically induced polarization rotation is equal to that of a continuous film. Such bimetallic metamaterials can be used in compact magnetic sensors, active plasmonic components and integrated photonic circuits.

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

    Energy Technology Data Exchange (ETDEWEB)

    Sun, Pingping; Siddiqi, Georges; Vining, William C.; Chi, Miaofang; Bell, Alexis T. (UCB); (ORNL)

    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.

  4. Formic acid oxidation at platinum-bismuth catalysts

    Directory of Open Access Journals (Sweden)

    Popović Ksenija Đ.

    2015-01-01

    Full Text Available The field of heterogeneous catalysis, specifically catalysis on bimetallic surfaces, has seen many advances over the past few decades. Bimetallic catalysts, which often show electronic and chemical properties that are distinct from those of their parent metals, offer the opportunity to obtain new catalysts with enhanced selectivity, activity, and stability. The oxidation of formic acid is of permanent interest as a model reaction for the mechanistic understanding of the electrooxidation of small organic molecules and because of its technical relevance for fuel cell applications. Platinum is one of the most commonly used catalysts for this reaction, despite the fact that it shows a few significant disadvantages: high cost and extreme susceptibility to poisoning by CO. To solve this problem, several approaches have been used, but generally, they all consist in the modification of platinum with a second element. Especially, bismuth has received significant attention as Pt modifier. According to the results presented in this survey dealing with the effects influencing the formic acid oxidation it was found that two types of Pt-Bi bimetallic catalysts (bulk and low loading deposits on GC showed superior catalytic activity in terms of the lower onset potential and oxidation current density, as well as exceptional stability compared to Pt. The findings in this report are important for the understanding of mechanism of formic acid electrooxidation on a bulk alloy and decorated surface, for the development of advanced anode catalysts for direct formic acid fuel cells, as well as for the synthesis of novel low-loading bimetallic catalysts. The use of bimetallic compounds as the anode catalysts is an effective solution to overcoming the problems of the formic acid oxidation current stability for long term applications. In the future, the tolerance of both CO poisoning and electrochemical leaching should be considered as the key factors in the development

  5. Nature, density, and catalytic role of exposed species on dispersed VOx/CrOx/Al2O3 catalysts.

    Science.gov (United States)

    Yang, Shuwu; Iglesia, Enrique; Bell, Alexis T

    2006-02-16

    The structure and surface composition of binary oxides consisting of CrO(x) and VO(x) dispersed on alumina and their effects on the rate and selectivity of oxidative dehydrogenation (ODH) of propane were examined and compared with those for CrO(x) and VO(x) dispersed on alumina. VO(x) deposition on an equivalent CrO(x) monolayer on alumina and deposition of CrO(x) on an equivalent monolayer of VO(x) deposited on alumina led to CrVO(4) species during thermal treatment with concomitant reduction of Cr(6+) to Cr(3+). Autoreduction of Cr(6+) to Cr(3+) is also detected for CrO(x), even without the presence of VO(x). Infrared spectroscopy of NO adsorbed at 153 K probes the relative abundance of alumina and of V(5+), Cr(3+), and Cr(6+) at surfaces. This technique detects differences in the surface composition of VO(x)/CrO(x)()/Al(2)O(3) and CrO(x)/VO(x)/Al(2)O(3). The first of these samples is enriched in VO(x) relative to CrO(x) compared with the second sample. Consistent with this finding, VO(x)/CrO(x)/Al(2)O(3) and CrO(x)/VO(x)/Al(2)O(3) are distinguishable in their ODH activities and propene selectivities. The highest ODH activity and propene selectivity is observed for VO(x)/CrO(x)/Al(2)O(3), which exhibits a surface enriched in VO(x) and having a low surface concentration of Cr(6+). PMID:16471878

  6. Monodispersed bimetallic PdAg nanoparticles with twinned structures: Formation and enhancement for the methanol oxidation

    Science.gov (United States)

    Yin, Zhen; Zhang, Yining; Chen, Kai; Li, Jing; Li, Wenjing; Tang, Pei; Zhao, Huabo; Zhu, Qingjun; Bao, Xinhe; Ma, Ding

    2014-03-01

    Monodispersed bimetallic PdAg nanoparticles can be fabricated through the emulsion-assisted ethylene glycol (EG) ternary system. Different compositions of bimetallic PdAg nanoparticles, Pd80Ag20, Pd65Ag35 and Pd46Ag54 can be obtained via adjusting the reaction parameters. For the formation process of the bimetallic PdAg nanoparticles, there have two-stage growth processes: firstly, nucleation and growth of the primary nanoclusters; secondly, formation of the secondary nanoparticles with the size-selection and relax process via the coalescence or aggregation of the primary nanoclusters. The as-prepared PdAg can be supported on the carbon black without any post-treatment, which exhibited high electro-oxidation activity towards methanol oxidation under alkaline media. More importantly, carbon-supported Pd80Ag20 nanoparticles reveal distinctly superior activities for the methanol oxidation, even if compared with commercial Pt/C electro-catalyst. It is concluded that the enhanced activity is dependant on the unique twinning structure with heterogeneous phase due to the dominating coalescence growth in EG ternary system.

  7. The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol

    Science.gov (United States)

    Li, Molly Meng-Jung; Zheng, Jianwei; Qu, Jin; Liao, Fenglin; Raine, Elizabeth; Kuo, Winson C. H.; Su, Shei Sia; Po, Pang; Yuan, Youzhu; Tsang, Shik Chi Edman

    2016-02-01

    Incorporation of Zn atoms into a nanosize Cu lattice is known to alter the electronic properties of Cu, improving catalytic performance in a number of industrially important reactions. However the structural influence of Zn on the Cu phase is not well studied. Here, we show that Cu nano-clusters modified with increasing concentration of Zn, derived from ZnO support doped with Ga3+, can dramatically enhance their stability against metal sintering. As a result, the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol, an important reaction well known for deactivation from copper nanoparticle sintering, can show greatly enhanced activity and stability with the CuZn alloy catalysts due to no noticeable sintering. HRTEM, nano-diffraction and EXAFS characterization reveal the presence of a small beta-brass CuZn alloy phase (body-centred cubic, bcc) which appears to greatly stabilise Cu atoms from aggregation in accelerated deactivation tests. DFT calculations also indicate that the small bcc CuZn phase is more stable against Cu adatom migration than the fcc CuZn phase with the ability to maintain a higher Cu dispersion on its surface.

  8. The remarkable activity and stability of a highly dispersive beta-brass Cu-Zn catalyst for the production of ethylene glycol

    Science.gov (United States)

    Li, Molly Meng-Jung; Zheng, Jianwei; Qu, Jin; Liao, Fenglin; Raine, Elizabeth; Kuo, Winson C. H.; Su, Shei Sia; Po, Pang; Yuan, Youzhu; Tsang, Shik Chi Edman

    2016-01-01

    Incorporation of Zn atoms into a nanosize Cu lattice is known to alter the electronic properties of Cu, improving catalytic performance in a number of industrially important reactions. However the structural influence of Zn on the Cu phase is not well studied. Here, we show that Cu nano-clusters modified with increasing concentration of Zn, derived from ZnO support doped with Ga3+, can dramatically enhance their stability against metal sintering. As a result, the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol, an important reaction well known for deactivation from copper nanoparticle sintering, can show greatly enhanced activity and stability with the CuZn alloy catalysts due to no noticeable sintering. HRTEM, nano-diffraction and EXAFS characterization reveal the presence of a small beta-brass CuZn alloy phase (body-centred cubic, bcc) which appears to greatly stabilise Cu atoms from aggregation in accelerated deactivation tests. DFT calculations also indicate that the small bcc CuZn phase is more stable against Cu adatom migration than the fcc CuZn phase with the ability to maintain a higher Cu dispersion on its surface. PMID:26856760

  9. Temperature-programmed oxidation of coked noble metal catalysts after autothermal reforming of n-hexadecane

    Energy Technology Data Exchange (ETDEWEB)

    Kauppi, E.I.; Linnekoski, J.A.; Krause, A.O.I.; Veringa Niemelae, M.K. [Aalto University, School of Science and Technology, Department of Biotechnology and Chemical Technology, Research Group Industrial Chemistry, P.O. Box 16100, FI-00076 Aalto (Finland); Kaila, R.K. [VTT Technical Research Centre of Finland, Biologinkuja 7, Espoo, P.O. Box 1001, FI-02044 VTT (Finland)

    2010-08-15

    Autothermal reforming (ATR) of n-hexadecane was carried out on zirconia-supported mono- and bimetallic noble metal (Rh, Pt) catalysts at 600, 700, and 800 C. After ATR, the reactivity of coke deposits (2.8-9.9 wt%) on the catalysts was investigated by temperature-programmed oxidation (TPO). Analysis of the results obtained from ATR and TPO experiments at various temperatures and on the different catalysts gave information on the reaction conditions where the detrimental coke can be minimized and allows estimating the nature of carbon deposits. H{sub 2} production increased with temperature on the tested Rh-containing catalysts and the ZrO{sub 2} support, but decreased as a function of temperature on the Pt catalyst. The formation of coke was least at 800 C, evidently due to the intensifying reaction of carbon and steam with increasing temperature, as well as to the better activity of the catalysts. The amount of coke formed was highest at 700 C. Comparison of the TPO profiles obtained for the monometallic Rh and Pt catalysts with the bimetallic RhPt revealed differences in the nature of carbon deposits on their surface. At 600 C, the coke formed on the monometallic Rh and Pt catalysts was located mostly on the support, whereas on the bimetallic RhPt catalyst the formation of this type of coke was suppressed. The bimetallic RhPt catalyst also exhibited better tolerance toward coking at 700 C. Therefore, although the selectivity toward hydrogen was not related to the amount of coke formed, the deactivation patterns differed on the mono- and bimetallic catalysts. (author)

  10. Final Technical Report: First Principles Investigations for the Ensemble Effects of PdAu and PtAu Bimetallic Nanocatalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ruqian Wu

    2012-05-18

    Bimetallic surfaces with tunable chemical properties have attracted broad attention in recent years due to their ample potential for heterogeneous catalysis applications. The local chemical properties of constituents are strongly altered from their parent metals by 'ligand effect', a term encompassing the influences of charge transfer, orbital rehybridization and lattice strain. In comparison to the aforementioned, the 'ensemble effect' associated with particular arrangements of the active constituents have received much less attention, despite their notable importance towards the determination of reactivity and selectivity of bimetallic catalysts. We performed theoretical studies for understanding the ensemble effects on bimetallic catalysis: (i) simulations for the formation of different ensembles on PdAu and PtAu nanoclusters; (ii) studies of the size, shape, and substrate dependence of their electronic properties; and (iii) simulations for model reactions such as CO oxidation, methanol, ethylene and water dehydrogenation on PdAu and PtAu nanoclusters. In close collaboration with leading experimental groups, our theoretical research elucidated the fundamentals of Au based bimetallic nanocatalysts.

  11. Core-shell Rh-Pt nanocubes: A model for studying compressive strain effects in bimetallic nanocatalysts

    Science.gov (United States)

    Harak, Ethan William

    Shape-controlled bimetallic nanocatalysts often have increased activities and stabilities over their monometallic counterparts due to surface strain effects and electron transfer between the two metals. Here, we demonstrate that the degree of surface strain can be manipulated in shape-controlled nanocrystals through a bimetallic core shell architecture. This ability is achieved in a model core shell Rh Pt nanocube system through control of shell thickness. An increase in the Pt shell thickness leads to more compressive strain, which can increase the Pt 4f7/2 binding energy by as much as 0.13 eV. This change in electronic structure is correlated with a weakening of surface-adsorbate interactions, which we exploit to reduce catalyst poisoning by CO during formic acid electrooxidation. In fact, by precisely controlling the Pt shell thickness, the maximum current density achieved with Rh Pt nanocubes was 3.5 times greater than that achieved with similarly sized Pt nanocubes, with decreased CO generation as well. This system serves as a model for how bimetallic architectures can be used to manipulate the electronic structure of nanoparticle surfaces for efficient catalysis. The strategy employed here should enable the performance of bimetallic nanomaterials comprised of more cost-effective metals to be enhanced as well.

  12. Platinum-ruthenium bimetallic clusters on graphite: a comparison of vapor deposition and electroless deposition methods.

    Science.gov (United States)

    Galhenage, Randima P; Xie, Kangmin; Diao, Weijian; Tengco, John Meynard M; Seuser, Grant S; Monnier, John R; Chen, Donna A

    2015-11-14

    Bimetallic Pt-Ru clusters have been grown on highly ordered pyrolytic graphite (HOPG) surfaces by vapor deposition and by electroless deposition. These studies help to bridge the material gap between well-characterized vapor deposited clusters and electrolessly deposited clusters, which are better suited for industrial catalyst preparation. In the vapor deposition experiments, bimetallic clusters were formed by the sequential deposition of Pt on Ru or Ru on Pt. Seed clusters of the first metal were grown on HOPG surfaces that were sputtered with Ar(+) to introduce defects, which act as nucleation sites for Pt or Ru. On the unmodified HOPG surface, both Pt and Ru clusters preferentially nucleated at the step edges, whereas on the sputtered surface, clusters with relatively uniform sizes and spatial distributions were formed. Low energy ion scattering experiments showed that the surface compositions of the bimetallic clusters are Pt-rich, regardless of the order of deposition, indicating that the interdiffusion of metals within the clusters is facile at room temperature. Bimetallic clusters on sputtered HOPG were prepared by the electroless deposition of Pt on Ru seed clusters from a Pt(+2) solution using dimethylamine borane as the reducing agent at pH 11 and 40 °C. After exposure to the electroless deposition bath, Pt was selectively deposited on Ru, as demonstrated by the detection of Pt on the surface by XPS, and the increase in the average cluster height without an increase in the number of clusters, indicating that Pt atoms are incorporated into the Ru seed clusters. Electroless deposition of Ru on Pt seed clusters was also achieved, but it should be noted that this deposition method is extremely sensitive to the presence of other metal ions in solution that have a higher reduction potential than the metal ion targeted for deposition. PMID:26018140

  13. Influence of silver on the glycerol electro-oxidation over AuAg/C catalysts in alkaline medium: a cyclic voltammetry and in situ FTIR spectroscopy study

    International Nuclear Information System (INIS)

    In the present work, we investigated the influence of silver on the glycerol electro-oxidation over carbon-supported AuAg catalysts by cyclic voltammetry and in situ FTIR spectroscopy. We observed that the presence of Ag in the bimetallic materials provided a more efficient catalyst in terms of the ability to electro-oxidize glycerol at relatively low potentials. On the other hand, the bimetallic catalysts were found to be less promising than the Au/C catalyst with respect to the reaction rate. Ag addition influenced the mechanism of glycerol electro-oxidation, favoring the C-C-C bond breaking, as evidenced by the selective formation of formic acid on the bimetallic catalysts. The impact of Ag on the glycerol electro-oxidation over AuAg/C may be driven by electronic modifications and Ag segregation on the catalysts surface

  14. Etat actuel des recherches fondamentales sur les catalyseurs bimétalliques à base de platine, sur support alumine, comparables à ceux utilisés dans l'industrie pétrolière. Current State of Fundamental Research on Platinum-Base Bimetallic Catalysts on an Alumina Support, Comparable to the Ones Used in the Petroleum Industry

    Directory of Open Access Journals (Sweden)

    Charcosset H.

    2006-11-01

    és promoteurs diminuant l'hydrogénolyse ou (et inhibiteurs par encrassement ; 6 le fait que dans les 158 références de l'article la moitié date de 1976 et après, souligne l'intérêt croissant porté aux recherches fondamentales dans ce domaine. This article mainly concerns the pairs (Pt, Re, (Pt, Ir and (Pt,Ru dealt with in the following order - catalyst preparation (impregnation of the support, reduction by hydrogen ; - characterization of reduced catalysts ; - catalytic activities ; - scale-up tests ta industriel catalysts , - conclusions. Special emphasis is placed on I the difficulty of obtaining data on the degree of reduction which are meaningful concerning the state of the catalyst under normal working conditions, hence the need ta combine several techniques such as DTA, TGA, volumetry, catharometry, ESCA, in-frared spectroscopy, HL thermodesorption and the measuring of catalytic activities ; 21 the dference between the phase diagrams of divided and massed systems ; 3 the usefulness of the hydrogen titration of the unsorbed oxygen ta give evidence for the presence of small pure Mell particles in (Pt, Mell/AI20a catalysts; 4 the dependence of the final state of the catalyst on the activation mode. The pair (Pt, Re con be stabilized in a state of alloy particles having similar superficial and mean composition or in a state of particle mixture of (Pt, Re with an Re content of less than the rated composition and of pure and well dispersed Re. The pairs (Pt, Ir and especially (Pt, Ru are characterized by the difficulty in obtaining on alloy state with a constant composition from one metal particle to another ; 5 variations in catalytic activity due ta the addition of Mell to Pt, reflecting one or several of the following effects a increase in the dispersion of Pt with (or without a change in its intrinsic properties by weak-valence ions of W, Mo, Cr, etc. ; b formation of Mell in a metallic state, eventually producing an alloy with Pt ; c the rote of promoter carbon

  15. Preparation of Ag{sub core}/Au{sub shell} bimetallic nanoparticles from physical mixtures of Au clusters and Ag ions under dark conditions and their catalytic activity for aerobic glucose oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Haijun, E-mail: zhanghaijun@wust.edu.cn [College of Materials and Metallurgy, Wuhan University of Science and Technology, Wuhan, Hubei Province 430081 (China); Toshima, Naoki; Takasaki, Kanako [Department of Applied Chemistry, Tokyo University of Science Yamaguchi, SanyoOnoda-shi, Yamaguchi 756-0884 (Japan); Okumura, Mitsutaka [Department of Chemistry, Graduate School of Science, Osaka University, Machikaneyama, Toyonaka, Osaka 560-0043 (Japan)

    2014-02-15

    Graphical abstract: The synthesis, characterization and catalytic activities for glucose oxidation of AgAu bimetallic nanoparticles (BNPs) with size of less than 2 nm are reported. The catalytic activity of Ag{sub 10}Au{sub 90} BNPs was about two times higher than that of Au NPs, even the BNPs have a larger particle size than that of Au NPs. -- Highlights: • Ag{sub core}/Au{sub shell} BNPs with size of less than 2.0 nm were prepared. • No any reducing reagents and lights were used for the preparation of the BNPs. • The catalytic activity of the BNPs is about two times higher than that of Au NPs. -- Abstract: AgAu bimetallic nanoparticles (BNPs), one of the most extensively studied bimetallic systems in the literatures, could have various structures and compositions depending on their preparation conditions. In the present work, catalytically highly active PVP-protected Ag{sub core}/Au{sub shell} BNPs of about 2.5 nm in diameter were fabricated from physical mixtures of aqueous dispersions of Au nanoparticles and Ag{sup +} ions under dark conditions without using any reducing agents. The prepared Ag{sub core}/Au{sub shell} BNP colloidal catalysts, which possessed a high activity for aerobic glucose oxidation, were characterized by Ultraviolet–visible spectrophotometry (UV–Vis), Inductive coupled plasma emission spectrometer (ICP), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and Energy disperse spectroscopy (EDS) in High-resolution scanning transmission electron microscopy (HR-STEM). The highest activity (11,360 mol-glucose h{sup −1} mol-metal{sup −1}) was observed for the BNPs with the Ag/Au atomic ratio of 1/9, the TOF value of which is about two times higher than that of Au nanoparticles with the particle size of 1.3 nm. The enhanced catalytic activity of the prepared Ag{sub core}/Au{sub shell} BNPs compared to Au NPs can be ascribed to the presence of negatively charged Au atoms resulted from electron donations

  16. Synthesis of subnanometer-diameter vertically aligned single-walled carbon nanotubes with copper-anchored cobalt catalysts.

    Science.gov (United States)

    Cui, Kehang; Kumamoto, Akihito; Xiang, Rong; An, Hua; Wang, Benjamin; Inoue, Taiki; Chiashi, Shohei; Ikuhara, Yuichi; Maruyama, Shigeo

    2016-01-21

    We synthesize vertically aligned single-walled carbon nanotubes (VA-SWNTs) with subnanometer diameters on quartz (and SiO2/Si) substrates by alcohol CVD using Cu-anchored Co catalysts. The uniform VA-SWNTs with a nanotube diameter of 1 nm are synthesized at a CVD temperature of 800 °C and have a thickness of several tens of μm. The diameter of SWNTs was reduced to 0.75 nm at 650 °C with the G/D ratio maintained above 24. Scanning transmission electron microscopy energy-dispersive X-ray spectroscopy (EDS-STEM) and high angle annular dark field (HAADF-STEM) imaging of the Co/Cu bimetallic catalyst system showed that Co catalysts were captured and anchored by adjacent Cu nanoparticles, and thus were prevented from coalescing into a larger size, which contributed to the small diameter of SWNTs. The correlation between the catalyst size and the SWNT diameter was experimentally clarified. The subnanometer-diameter and high-quality SWNTs are expected to pave the way to replace silicon for next-generation optoelectronic and photovoltaic devices. PMID:26690843

  17. Preparation and characterization of silica-supported Ni/Pt catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Raab, C.; Lercher, J.A. (Universitaet Wien, Vienna (Austria)); Goodwin, J.G. Jr. (Univ. of Pittsburgh, PA (USA)); Shyu, J.Z. (Amoco Research Center, Naperville, IL (USA))

    1990-04-01

    The formation of a series of Ni/Pt catalysts was investigated by means of temperature programmed reduction (TPR) of the chloride precursor, hydrogen chemisorption, x-ray diffraction, scanning electron microscopy, XPS, and magnetic measurements. An alloy between Pt and Ni was formed. The minority constituent of the series of bimetallic catalysts was always found to be quantitatively alloyed or in close contact with the more abundant metal. For several samples, the stoichiometric NiPt compound was observed. With Ni-rich samples a nonstoichiometric alloy (rich in Ni) was concluded to exist. At all concentration levels the presence of Pt facilitated the reduction of Ni{sup 2+} significantly. Temperature-programmed reduction of the Ni/Pt catalyst with 50 mol% and higher concentrations of Pt did not differ from that of pure Pt. Based on XPS and magnetic measurements it is concluded that a constant fraction (approximately 10-15%) of Ni was highly dispersed and interacted strongly with the support. 30 refs.

  18. Stainless Steel to Titanium Bimetallic Transitions

    Energy Technology Data Exchange (ETDEWEB)

    Kaluzny, J. A. [Fermilab; Grimm, C. [Fermilab; Passarelli, D. [Fermilab

    2015-01-01

    In order to use stainless steel piping in an LCLS-II (Linac Coherent Light Source Upgrade) cryomodule, stainless steel to titanium bimetallic transitions are needed to connect the stainless steel piping to the titanium cavity helium vessel. Explosion bonded stainless steel to titanium transition pieces and bimetallic transition material samples have been tested. A sample transition tube was subjected to tests and x-ray examinations between tests. Samples of the bonded joint material were impact and tensile tested at room temperature as well as liquid helium temperature. The joint has been used successfully in horizontal tests of LCLS-II cavity helium vessels and is planned to be used in LCLS-II cryomodules. Results of material sample and transition tube tests will be presented.

  19. Characterization of Bimetallic Castings with an Austenitic Working Surface Layer and an Unalloyed Cast Steel Base

    Science.gov (United States)

    Wróbel, Tomasz

    2014-05-01

    The paper presents the technology of bimetallic castings based on the founding method of layer coating directly in the cast process of the so-called method of mold cavity preparation. The prepared castings consist of two fundamental parts, i.e., the base and the working surface layer. The base part of the bimetallic casting is typical foundry material, i.e., unalloyed cast steel, whereas the working layer is a plate of austenitic alloy steel sort X2CrNi 18-9. The quality of the joint between the base part and the working layer was evaluated on the basis of ultrasonic non-destructive testing and structure examinations containing metallographic macro- and microscopic studies with the use of a light microscope (LOM) with microhardness measurements and a scanning electron microscope (SEM) with microanalysis of the chemical composition (energy dispersive spectroscopy—EDS). On the basis of the obtained results it was confirmed that the decisive phenomena needed to create a permanent joint between the two components of the bimetallic casting are carbon and heat transport in the direction from the high-carbon and hot base material which was poured into the mold in the form of liquid metal to the low-carbon and cold material of the working layer which was placed in the mold cavity in the form of a monolithic insert.

  20. Synchrotron radiation studies of supported metal catalysts

    International Nuclear Information System (INIS)

    Metallic clusters supported on refractory oxides have been used extensively for several decades in the production of chemicals and petroleum derived transportation fuels. Catalysts containing more than one metal component are of particular interest since the addition of a second metal provides a method of controlling the selectivity of the catalyst. That is, the second metal can alter the rates of competing reactions in a complex reaction sequence and thus alter the final product distribution of the reaction. In this work the reactions of cyclohexane in hydrogen over silica supported ruthenium and osmium catalysts were studied. Bimetallic catalysts represent an important class of materials that are of interest both scientifically and technologically. Despite the importance and long-standing use of supported metal catalysts, detailed information on the structure of the metal clusters has been difficult to obtain. The development of x-ray absorption spectroscopy with the increasing availability of synchrotron radiation, however, has provided a powerful and versatile tool for studying the structure of these complex systems. Using the Extended X-ray Absorption Fine Structure (EXAFS) technique, it is possible to obtain information on the local atomic structure of supported monometallic catalytic metals and their interaction with the support. In the discussion that follows the authors will focus on results that have been obtained on the structure of supported bimetallic cluster catalysts

  1. SYNTHESIS OF POLYMER-STABILIZED PLATINUM/RUTHENIUM BIMETALLIC COLLOIDS AND THEIR CATALYTIC PROPERTIES FOR SELECTIVE HYDROGENATION OF CROTONALDEHYDE

    Institute of Scientific and Technical Information of China (English)

    Wei-xia Tu; Han-fan Liu

    2005-01-01

    Polymer-stabilized platinum/ruthenium bimetallic colloids (Pt/Ru) were synthesized by polyol reduction with microwave irradiation and characterized by TEM and XPS. The colloidal nanoparticles have small and narrow size distributions. Catalytic performance of the Pt/Ru colloidal catalysts was investigated on the selective hydrogenation of crontonaldehyde (CRAL). A suitable amount of the added metal ions and base can improve the selectivity of CRAL to crotylalcohol (CROL) remarkably. The catalytic activity and the selectivity are dependent on the compositions of bimetallic colloids. Thereinto, PVP-stabilized 9Pt/1Ru colloid with a molar ratio of metals Pt:Ru = 9:1 shows the highest catalytic selectivity 77.3% to CROL at 333 K under 4.0 MPa of hydrogen.

  2. Tetranuclear Zn/4f coordination clusters as highly efficient catalysts for Friedel-Crafts alkylation.

    Science.gov (United States)

    Griffiths, Kieran; Kumar, Prashant; Akien, Geoffrey R; Chilton, Nicholas F; Abdul-Sada, Alaa; Tizzard, Graham J; Coles, Simon J; Kostakis, George E

    2016-06-14

    A series of custom-designed, high yield, isoskeletal tetranuclear Zn/4f coordination clusters showing high efficiency as catalysts with low catalytic loadings in Friedel-Crafts alkylation are described for the first time. The possibility of altering the 4f centers in these catalysts without altering the core topology allows us to further confirm their stability via EPR and NMR, as well to gain insights into the plausible reaction mechanism, showcasing the usefulness of these bimetallic systems as catalysts. PMID:27248829

  3. RuCu nanoparticles supported on graphene: A highly efficient catalyst for hydrolysis of ammonia borane

    Energy Technology Data Exchange (ETDEWEB)

    Cao, Nan; Hu, Kai [College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei 430072 (China); Luo, Wei, E-mail: wluo@whu.edu.cn [College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei 430072 (China); Suzhou Institute of Wuhan University, Suzhou, Jiangsu, 215123 (China); Cheng, Gongzhen, E-mail: gzcheng@whu.edu.cn [College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei 430072 (China)

    2014-03-25

    Graphical abstract: Well dispersed RuCu/graphene nanoparticles exerted satisfied catalytic activity and recycle stability towards the hydrolysis of ammonia borane. Highlights: • One-step in situ synthesis of graphene supported RuCu NPs. • The catalysts exhibit excellent catalytic activity toward hydrolysis of AB. • Graphene supported NPs exhibit the highest catalytic activity. -- Abstract: Well dispersed RuCu nanoparticles (NPs) supported on graphene were in situ synthesized by a one-step co-reduction of aqueous solution of ruthenium (III) chloride, cupric (II) chloride, and graphite oxide (GO) with ammonia borane (AB) under ambient condition. The nature of the NPs was fully characterized by TEM, HRTEM, XRD, energy dispersive spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS). The as-synthesized NPs exhibit much higher catalytic activity for hydrolytic dehydrogenation of AB than the monometallic Ru and Cu, bimetallic RuCu/graphene reduced by NaBH{sub 4}, and graphene free RuCu counterparts. Additionally, the as-synthesized NPs supported on graphene exhibit higher catalytic activity than the catalysts with other conventional supports, such as SiO{sub 2}, γ-Al{sub 2}O{sub 3}, and carbon black. The activity of Ru{sub 1}Cu{sub 7.5}/graphene NPs in terms of turnover frequency (TOF) is 135 mol H{sub 2} min{sup −1} (mol Ru){sup −1}, which is higher than Ru/graphene, and most reported Ru-based or other noble metal-based NPs for the catalytic hydrolysis of AB. The activation energy for hydrolysis of AB in the presence of Ru{sub 1}Cu{sub 7.5}/graphene NPs was determined as 30.59 kJ mol{sup −1}, which is lower than most of the reported catalysts. Furthermore, the as-prepared NPs exert satisfied durable stability for the hydrolytic dehydrogenation of AB.

  4. Bimetallic electrocatalysts on titanium dioxide-based supports for methanol oxidation and oxygen evolution

    Science.gov (United States)

    Fuentes, Roderick Eliel

    Electrocatalysts are essential for the development of active and durable fuel cells and hydrogen production technologies. Generally, electrochemical processes of energy conversion and hydrogen generation in a Proton Exchange Membrane (PEM) utilize precious metals, such as platinum, iridium and ruthenium, as electrocatalysts. For the methanol oxidation and oxygen evolution reaction, a bimetallic structure can be used to enhance kinetics and increase stability. It is desired to support electrocatalysts to disperse nanoparticles on the surface and promote better catalyst utilization. Traditionally, carbon has been used as an electrochemical support because it has a high surface area and high electrical conductivity. The problem with carbon is that it is not a very stable material and can corrode at voltages more than 0.9 V, affecting performance of the electrochemical reaction. Therefore, it would be useful to support electrocatalysts in a stable material with suitable conductivity. Using titanium dioxide as a support can be advantageous due to its corrosion-resistant capability. TiO2 exhibit different crystalline structures, such as anatase and rutile, which can have an effect on catalytic activity. Unfortunately, it is not conductive; hence, it is not used in electrochemical applications. However, it can be doped with niobium to increase electronic conductivity; but, it usually come at the expense of surface area. In this work, TiO 2 and Nb-TiO2 were studied as platinum/ruthenium and iridium/ruthenium nanoparticles supports for the electrochemical oxidation of methanol and oxygen evolution, respectively. Even though the conductivity of our supports was very low, adding a considerable loading of nanoparticles increased conductivity of the composite material (support + catalyst) to acceptable levels. Using cyclic voltammetry (CV) and direct methanol fuel cell tests creating a membrane electrode assembly (MEA), Pt-Ru supported on Nb-TiO2 and TiO 2 showed superior

  5. Analysis of Manufacturing Bimetallic Tubes by the Cold Drawing Process

    Directory of Open Access Journals (Sweden)

    Halaczek D.

    2016-03-01

    Full Text Available Drawing processes apply to obtain the bimetallic tubes from the different metals and alloys, combined in the solid state, which significantly affects the specificity of this process. The manufacturing of bimetallic tubes by drawing process depends on many factors which include: preparation of the surface of materials joined in the solid state, the geometric parameters of the working tool, technological parameters of the drawing process (drawing speed, type of lubricant, the use of back pull etc.. Generally, the cold drawing process of producing the bimetallic tubes refers to metals which have high ductility (copper, aluminum, etc.. The tube sinking (tube drawing without a mandrel of bimetallic tubes together with joining them at the interface of the two metal in the solid-state is applied for tubes of the diameter range between 6 to 20 mm and based on of the reducing the diameter of the tube. However, a slight increase of wall thickness ca. 0.05 ÷ 0.10 mm can appear, which is not dangerous phenomenon in case of producing the bimetallic tubes by joining in the solid-state. The aim of the research was to investigate the technology of tubes drawing process from non-ferrous metal, drawing process of bimetallic tubes and the production of bimetallic tubes in layers composition: cooper Cu-ETP - brass CuZn37 and CuZn37 brass - copper Cu-ETP in the tube sinking process. The research program included: production of bimetallic tubes with a different composition (Cu- ETP-CuZn37 and CuZn37-Cu-ETP and a different percentage of the cross-section components; analysis of changes of tube wall thickness and the layer composition of the bimetallic tube, based on measurements on the workshop microscope; analysis of the material flow in the process of the bimetallic tubes production based on the measurements results of a profilograph CP-200.

  6. Controlled reduction of LaFe xMn yMo zO3/Al2O3 composites to produce highly dispersed and stable Fe0 catalysts: a Mössbauer investigation

    Directory of Open Access Journals (Sweden)

    Juliana Cristina Tristão

    2008-06-01

    Full Text Available In this work, controlled reduction of perovskites supported on Al2O3 was used to prepare thermally stable nanodispersed iron catalysts based on Fe0/La2O3/Al2O3. The perovskites composites LaFe0.90Mn0.08Mo0.02O3(25, 33 and 50 wt (% /Al2O3 and LaFe0.90Mn0.1O3(25 wt (% /Al2O3 were prepared and characterized by XRD, BET, TPR, SEM and Mössbauer spectroscopy. XRD for unsupported perovskite showed the formation of a single phase perovskite structure. The Mössbauer spectra of the perovskites were fitted with hyperfine field distribution model for the perovskite. Supported perovskites on Al2O3 showed a decrease of the hyperfine field in respect to unsupported perovskite, due to decrease of particle size and dispersion of the Fe3+ specimens on the support. Also showed broaden lines and relaxation effects due to the small particle size. To produce the Fe0 catalyst, the composite perovskite(25%/Al2O3 was reduced with H2 at 900, 1000 and 1100 °C for 1 hour. XRD data indicated the formation of Fe0 catalyst with particles sizes of ca. 35 nm. The Mössbauer spectrum showed the formation of metallic iron and doublets corresponding to species of octahedric Fe2+ and Fe3+ sites dispersed on Al2O3. These catalysts showed improved stability towards sintering even upon treatment at 1000 and 1100 °C under H2.

  7. Insight into the Catalytic Mechanism of Bimetallic Platinum–Copper Core–Shell Nanostructures for Nonaqueous Oxygen Evolution Reactions

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Lu; Luo, Xiangyi; Kropf, A. Jeremy; Wen, Jianguo; Wang, Xiaoping; Lee, Sungsik; Myers, Deborah J.; Miller, Dean; Wu, Tianpin; Lu, Jun; Amine, Khalil

    2016-01-01

    The oxygen evolution reaction (OER) plays a critical role in multiple energy conversion and storage applications. However, its sluggish kinetics usually results in large voltage polarization and unnecessary energy loss. Therefore, designing efficient catalysts that could facilitate this process has become an emerging topic. Here, we present a unique Pt–Cu core–shell nanostructure for catalyzing the nonaqueous OER. The catalysts were systematically investigated with comprehensive spectroscopic techniques, and applied in nonaqueous Li–O2 electrochemical cells, which exhibited dramatically reduced charging overpotential (<0.2 V). The superior performance is explained by the robust Cu(I) surface sites stabilized by the Pt core in the nanostructure. The insights into the catalytic mechanism of the unique Pt–Cu core–shell nanostructure gained in this work are expected to serve as a guide for future design of other nanostructured bimetallic OER catalysts.

  8. Synthesis and characterization of Fe-Co catalyst prepared via reverse microemulsion method

    Science.gov (United States)

    Mohd Zabidi, Noor Asmawati; Abdul Aziz, Muhammad Nur Azizi; Ali, Sardar; Taha, Mohd Faisal

    2012-09-01

    This paper reports the characterization of bimetallic catalyst systems comprising cobalt and iron on CNTs support prepared via reverse microemulsion method. The properties of the bimetallic catalyst were characterized using TEM, FESEM and N2 adsorption. Based on TEM analyses, the calculated average particle sizes ranged from 4.6 nm to 5.2 nm for the various catalyst compositions. The performance of the Co-based catalyst in a Fischer-Tropsch reaction was evaluated in a fixed-bed reactor at 220°C, 1 atm and H2/CO v/v ratio of 2:1 v/v and space velocity of 12 L/g.h. Amongst the catalysts tested, the 90Co10Fe/CNTs resulted in the highest CO conversion of 14.1% whereas the 100Co/CNTs resulted in the highest C5+ hydrocarbon selectivity.

  9. DNA-templated synthesis of PtAu bimetallic nanoparticle/graphene nanocomposites and their application in glucose biosensor

    OpenAIRE

    Leng, Jing; Wang, Wen-Min; Lu, Li-min; Bai, Ling; Qiu, Xin-Lan

    2014-01-01

    In this paper, single-stranded DNA (ss-DNA) is demonstrated to functionalize graphene (GR) and to further guide the growth of PtAu bimetallic nanoparticles (PtAuNPs) on GR with high densities and dispersion. The obtained nanocomposites (PtAuNPs/ss-DNA/GR) were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectrometer (EDS), and electrochemical techniques. Then, an enzyme nanoassembly was prepared by self-assembling glucose oxidase (GOD) on PtAuNP/ss-DNA/GR ...

  10. Enhanced Dry Reforming of Methane on Ni and Ni-Pt Catalysts Synthesized by Atomic Layer Deposition

    Energy Technology Data Exchange (ETDEWEB)

    Gould, Troy D.; Montemore, Matthew M.; Lubers, Alia M.; Ellis, Lucas D.; Weimer, Alan; Falconer, John L.; Medlin, James W.

    2015-02-25

    Atomic layer deposition (ALD) was used to deposit Ni and Pt on alumina supports to form monometallic and bimetallic catalysts with initial particle sizes of 1–2.4 nm. The ALD catalysts were more active (per mass of metal) than catalysts prepared by incipient wetness (IW) for dry reforming of methane (DRM), and they did not form carbon whiskers during reaction due to their sufficiently small size. Catalysts modified by Pt ALD had higher rates of reaction per mass of metal and inhibited coking, whereas NiPt catalysts synthesized by IW still formed carbon whiskers. Temperature-programmed reduction of Ni catalysts modified by Pt ALD indicated the presence of bimetallic interaction. Density functional theory calculations suggested that under reaction conditions, the NiPt surfaces form Ni-terminated surfaces that are associated with higher DRM rates (due to their C and O adsorption energies, as well as the CO formation and CH4 dissociation energies).

  11. BIMETALLIC LITHIUM BOROHYDRIDES TOWARD REVERSIBLE HYDROGEN STORAGE

    Energy Technology Data Exchange (ETDEWEB)

    Au, M.

    2010-10-21

    Borohydrides such as LiBH{sub 4} have been studied as candidates for hydrogen storage because of their high hydrogen contents (18.4 wt% for LiBH{sub 4}). Limited success has been made in reducing the dehydrogenation temperature by adding reactants such as metals, metal oxides and metal halides. However, full rehydrogenation has not been realized because of multi-step decomposition processes and the stable intermediate species produced. It is suggested that adding second cation in LiBH{sub 4} may reduce the binding energy of B-H. The second cation may also provide the pathway for full rehydrogenation. In this work, several bimetallic borohydrides were synthesized using wet chemistry, high pressure reactive ball milling and sintering processes. The investigation found that the thermodynamic stability was reduced, but the full rehydrogenation is still a challenge. Although our experiments show the partial reversibility of the bimetallic borohydrides, it was not sustainable during dehydriding-rehydriding cycles because of the accumulation of hydrogen inert species.

  12. Homogeneity and elemental distribution in self-assembled bimetallic Pd-Pt aerogels prepared by a spontaneous one-step gelation process.

    Science.gov (United States)

    Oezaslan, M; Liu, W; Nachtegaal, M; Frenkel, A I; Rutkowski, B; Werheid, M; Herrmann, A-K; Laugier-Bonnaud, C; Yilmaz, H-C; Gaponik, N; Czyrska-Filemonowicz, A; Eychmüller, A; Schmidt, T J

    2016-07-27

    a commercially available unsupported Pt black catalyst. We show that the Pd-Pt aerogels possess a high utilization of catalytically active centers for electrocatalytic applications based on the nanostructured bimetallic framework. Knowledge about the homogeneity and chemical distribution of the bimetallic aerogels can help to further optimize their preparation by the spontaneous one-step gelation process and to tune their electrocatalytic reactivity. PMID:27411594

  13. Impact of Multifunctional Bimetallic Materials on Lithium Battery Electrochemistry.

    Science.gov (United States)

    Durham, Jessica L; Poyraz, Altug S; Takeuchi, Esther S; Marschilok, Amy C; Takeuchi, Kenneth J

    2016-09-20

    Electric energy storage devices such as batteries are complex systems comprised of a variety of materials with each playing separate yet interactive roles, complicated by length scale interactions occurring from the molecular to the mesoscale. Thus, addressing specific battery issues such as functional capacity requires a comprehensive perspective initiating with atomic level concepts. For example, the electroactive materials which contribute to the functional capacity in a battery comprise approximately 30% or less of the total device mass. Thus, the design and implementation of multifunctional materials can conceptually reduce or eliminate the contribution of passive materials to the size and mass of the final system. Material multifunctionality can be achieved through appropriate material design on the atomic level resulting in bimetallic electroactive materials where one metal cation forms mesoscale conductive networks upon discharge while the other metal cations can contribute to atomic level structure and net functional secondary capacity, a device level issue. Specifically, this Account provides insight into the multimechanism electrochemical redox processes of bimetallic cathode materials based on transition metal oxides (MM'O) or phosphorus oxides (MM'PO) where M = Ag and M' = V or Fe. One discharge process can be described as reduction-displacement where Ag(+) is reduced to Ag(0) and displaced from the parent structure. This reduction-displacement reaction in silver-containing bimetallic electrodes allows for the in situ formation of a conductive network, enhancing the electrochemical performance of the electrode and reducing or eliminating the need for conductive additives. A second discharge process occurs through the reduction of the second transition metal, V or Fe, where the oxidation state of the metal center is reduced and lithium cations are inserted into the structure. As both metal centers contribute to the functional capacity, determining the

  14. Electrochemical impedance study and performance of PdNi nanoparticles as cathode catalyst in a polymer electrolyte membrane fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Ramos-Sanchez, G.; Santana-Salinas, A.; Vazquez-Huerta, G.; Solorza-Feria, O. [Inst. Politenico Nacional, Centro de Investigacion y de Estudios Avanzados, Mexico City (Mexico). Dept. de Quimica

    2010-07-15

    Polymer electrolyte membrane fuel cells (PEMFC) convert the energy stored in hydrogen and oxygen molecules directly into electricity. However, technical and economic challenges must be overcome to address cost, performance and stability issues associated with membrane electrode assemblies (MEA). The oxygen reduction reaction (ORR) which takes place in the cathode is the limiting reaction due to the slow kinetics of ORR on metals, including platinum (Pt). For that reason, much research has gone into finding catalyst materials with a similar or greater performance than Pt. Bimetallic palladium (Pd) based catalysts have been considered as alternative materials for ORR. In this study, a carbon-dispersed bimetallic PdNi was prepared by borohydride reduction using PdCl{sub 2} and NiCl{sub 2} as precursors in a tetrahydrofuran (THF) solution. The PdNi loading and weight percentage were optimized using the Simplex method. The MEA performance was evaluated at optimum conditions using the PdNi electrocatalyst as the cathode and a Pt-Etek carbon cloth as the anode. The maximum power density of 122 mW per cm{sup 2} was reached with 45 percent of PdNi wt percent at 30 psi and 80 degrees C. The catalytic activity and the mechanism of the ORR on PdNi, in 0.5M H{sub 2}SO{sub 4} was investigated using electrochemical impedance spectroscopy. The Tafel slope and the charge transfer coefficient were obtained from the impedance spectra at optimum condition of PdNi loading and PdNi wt percent. 24 refs., 2 tabs., 5 figs.

  15. Synthesis of bimetallic Pt-Pd core-shell nanocrystals and their high electrocatalytic activity modulated by Pd shell thickness

    Science.gov (United States)

    Li, Yujing; Wang, Zhi Wei; Chiu, Chin-Yi; Ruan, Lingyan; Yang, Wenbing; Yang, Yang; Palmer, Richard E.; Huang, Yu

    2012-01-01

    Bimetallic Pt-Pd core-shell nanocrystals (NCs) are synthesized through a two-step process with controlled Pd thickness from sub-monolayer to multiple atomic layers. The oxygen reduction reaction (ORR) catalytic activity and methanol oxidation reactivity of the core-shell NCs for fuel cell applications in alkaline solution are systematically studied and compared based on different Pd thickness. It is found that the Pd shell helps to reduce the over-potential of ORR by up to 50mV when compared to commercial Pd black, while generating up to 3-fold higher kinetic current density. The carbon monoxide poisoning test shows that the bimetallic NCs are more resistant to the CO poisoning than Pt NCs and Pt black. It is also demonstrated that the bimetallic Pt-Pd core-shell NCs can enhance the current density of the methanol oxidation reaction, lowering the over-potential by 35 mV with respect to the Pt core NCs. Further investigation reveals that the Pd/Pt ratio of 1/3, which corresponds to nearly monolayer Pd deposition on Pt core NCs, gives the highest oxidation current density and lowest over-potential. This study shows for the first time the systematic investigation of effects of Pd atomic shells on Pt-Pd bimetallic nanocatalysts, providing valuable guidelines for designing high-performance catalysts for fuel cell applications.Bimetallic Pt-Pd core-shell nanocrystals (NCs) are synthesized through a two-step process with controlled Pd thickness from sub-monolayer to multiple atomic layers. The oxygen reduction reaction (ORR) catalytic activity and methanol oxidation reactivity of the core-shell NCs for fuel cell applications in alkaline solution are systematically studied and compared based on different Pd thickness. It is found that the Pd shell helps to reduce the over-potential of ORR by up to 50mV when compared to commercial Pd black, while generating up to 3-fold higher kinetic current density. The carbon monoxide poisoning test shows that the bimetallic NCs are more

  16. Catalytically Active Bimetallic Nanoparticles Supported on Porous Carbon Capsules Derived From Metal-Organic Framework Composites.

    Science.gov (United States)

    Yang, Hui; Bradley, Siobhan J; Chan, Andrew; Waterhouse, Geoffrey I N; Nann, Thomas; Kruger, Paul E; Telfer, Shane G

    2016-09-14

    We report a new methodology for producing monometallic or bimetallic nanoparticles confined within hollow nitrogen-doped porous carbon capsules. The capsules are derived from metal-organic framework (MOF) crystals that are coated with a shell of a secondary material comprising either a metal-tannic acid coordination polymer or a resorcinol-formaldehyde polymer. Platinum nanoparticles are optionally sandwiched between the MOF core and the shell. Pyrolysis of the MOF-shell composites produces hollow capsules of porous nitrogen-doped carbon that bear either monometallic (Pt, Co, and Ni) or alloyed (PtCo and PtNi) metal nanoparticles. The Co and Ni components of the bimetallic nanoparticles are derived from the shell surrounding the MOF crystals. The hollow capsules prevent sintering and detachment of the nanoparticles, and their porous walls allow for efficient mass transport. Alloyed PtCo nanoparticles embedded in the capsule walls are highly active, selective, and recyclable catalysts for the hydrogenation of nitroarenes to anilines. PMID:27575666

  17. Catalytic reduction of nitrate and nitrite ions by hydrogen : investigation of the reaction mechanism over Pd and Pd-Cu catalysts

    NARCIS (Netherlands)

    Ilinitch, OM; Nosova, LV; Gorodetskii, VV; Ivanov, VP; Trukhan, SN; Gribov, EN; Bogdanov, SV; Cuperus, FP

    2000-01-01

    The catalytic behavior of mono- and bimetallic catalysts with Pd and/or Cu supported over gamma-Al2O3 in the reduction of aqueous nitrate and nitrite ions by hydrogen was investigated. The composition of the supported metal catalysts was analysed using secondary ion mass spectroscopy (SIMS) and X-ra

  18. Development of Cu and Ni catalysts supported on ZrO{sub 2} for the generation of H{sub 2} by means of the reaction of reformed methanol in atmosphere oxidizer; Desarrollo de catalizadores de Cu y Ni soportados en ZrO{sub 2} para la generacion de H{sub 2} mediante la reaccion de reformado de metanol en atmosfera oxidante

    Energy Technology Data Exchange (ETDEWEB)

    Lopez C, P.

    2012-07-01

    ZrO{sub 2} was prepared by the sol-gel method and calcined at 450 C. The prepared zirconia was impregnated with an aqueous solution of Cu(CH{sub 3}CO{sub 2}){sub 2}{center_dot}H{sub 2}O or NiNO{sub 3}{center_dot}6H{sub 2}O at an appropriate concentration to yield 3 wt % of copper or nickel, respectively, in the mono metallic catalysts. Three bimetallic samples were prepared at 80% Cu and 20% Ni respectively to obtain 3 wt % of total metallic phase. Surface area of the Cu-Ni base catalysts supported on ZrO{sub 2} oxide showed differences as a function of the metal addition. Between them, the Cu/ZrO{sub 2} catalyst had the lowest surface area than other catalysts. X-ray diffraction patterns of the bimetallic catalysts did not show diffraction peaks of the Cu, Ni or bimetallic Cu-Ni alloys. In addition, TPR profiles of the bimetallic catalysts had the lowest reduction temperature compared with the mono metallic samples. The reactivity of the catalysts in the range of 250-350 C showed that the samples prepared by successive impregnation had the highest catalytic activity than the other catalysts studied. Also the selectivity for H{sub 2} production was higher for these catalysts. This finding was associated to the presence of the bimetallic Cu-Ni nanoparticles, as was evidenced by Tem-EDX analysis. (Author)

  19. 分散型镍、铁催化剂用于重油-煤的加氢共炼研究%Study on dispersed Ni and Fe catalysts for coal-heavy oil co-processing

    Institute of Scientific and Technical Information of China (English)

    戈军; 石斌; 杨圣闯; 李慎伟; 郭龙德; 郭智慧; 张建芳

    2011-01-01

    将硝酸镍和硝酸铁分别溶于水、甲醇或N,N二甲基甲酰胺(DMF),然后通过高速剪切分散在重油中,脱除溶剂后在350℃下采用升华硫预硫化成为分散型镍、铁催化剂,用于重油-煤加氢共炼.结果表明:与水溶性镍、铁催化剂相比,有机溶剂化的镍、铁催化剂前体在重油中由于黏度较小和相容性较好而具有更好的分散性,并且DMF做溶剂的性能优于甲醇;顶硫化后甲醇化的镍、铁催化剂颗粒分别可达50和120 nm,而采用DMF相应的催化剂颗粒为10 ~40和30 ~50 nm,并且催化剂粒径均匀;在420℃、1h、冷氢压8.0 MPa和煤与重油质量比1∶3的反应条件下,与以水为溶剂相比,采用甲醇或DMF为溶剂,尤其是DMF制备的镍、铁催化剂更能明显改善轮古常压渣油、Du-84特稠油与神华烟煤以及内蒙褐煤的加氢共炼效果;有机溶剂化制备的镍、铁催化剂在硫化和共炼条件下不容易聚结失活,并且DMF作溶剂的性能优于甲醇.%The dispersed nickel or ferric sulfide catalyst were prepared from nickel or ferric nitrate by dissolving in H2O, methanol or N-N dimethyl foramide ( DMF) and then dispersing in heavy oil and presulfurizing with sulfur at 330 t. The results show that the particles sizes of the nickel and ferric sulfides from organic-soluble catalysts precursors are smaller and more symmetrical than those of the traditional water solution. The particles sizes of nickel and ferric sulfides from DMF-solu-ble catalysts precursors are about 10-40 nm and 30-50 tun, exhibiting the advantage of DMF on methanol for the corresponding particles size from methanol-soluble respectively about 50 nm and 120 nm, which resulted from the lower viscosity and good compatibility of the preparing system. In the two heavy oils ( LGAR,Du-84) and two coals(Shenhua bitumite or Neimeng brown coal) co-processing system at 420 X., 1 h, 8.0 Mpa H2(cold) and the mass ratio of coal to oil 1 =3, the catalysts

  20. Modeling the melting temperature of nanoscaled bimetallic alloys.

    Science.gov (United States)

    Li, Ming; Zhu, Tian-Shu

    2016-06-22

    The effect of size, composition and dimension on the melting temperature of nanoscaled bimetallic alloys was investigated by considering the interatomic interaction. The established thermodynamics model without any arbitrarily adjustable parameters can be used to predict the melting temperature of nanoscaled bimetallic alloys. It is found that, the melting temperature and interatomic interaction of nanoscaled bimetallic alloys decrease with the decrease in size and the increasing composition of the lower surface energy metal. Moreover, for the nanoscaled bimetallic alloys with the same size and composition, the dependence of the melting temperature on the dimension can be sequenced as follows: nanoparticles > nanowires > thin films. The accuracy of the developed model is verified by the recent experimental and computer simulation results.

  1. Oxidation catalyst

    Science.gov (United States)

    Ceyer, Sylvia T.; Lahr, David L.

    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.

  2. Reaction pathways of model compounds of biomass-derived oxygenates on Fe/Ni bimetallic surfaces

    Science.gov (United States)

    Yu, Weiting; Chen, Jingguang G.

    2015-10-01

    Controlling the activity and selectivity of converting biomass-derivatives to fuels and valuable chemicals is critical for the utilization of biomass feedstocks. There are primarily three classes of non-food competing biomass, cellulose, hemicellulose and lignin. In the current work, glycolaldehyde, furfural and acetaldehyde are studied as model compounds of the three classes of biomass-derivatives. Monometallic Ni(111) and monolayer (ML) Fe/Ni(111) bimetallic surfaces are studied for the reaction pathways of the three biomass surrogates. The ML Fe/Ni(111) surface is identified as an efficient surface for the conversion of biomass-derivatives from the combined results of density functional theory (DFT) calculations and temperature programmed desorption (TPD) experiments. A correlation is also established between the optimized adsorption geometry and experimental reaction pathways. These results should provide helpful insights in catalyst design for the upgrading and conversion of biomass.

  3. Simultaneous Detection of Electronic Structure Changes from Two Elements of a Bifunctional Catalyst Using Wavelength-Dispersive X-ray Emission Spectroscopy and in situ Electrochemistry

    OpenAIRE

    Gul, Sheraz; Desmond Ng, Jia Wei; Alonso-Mori, Roberto; Kern, Jan; Sokaras, Dimosthenis; Anzenberg, Eitan; Lassalle-Kaiser, Benedikt; Gorlin, Yelena; Weng, Tsu-Chien; Zwart, Petrus H.; Zhang, Jin Z.; Bergmann, Uwe; Yachandra, Vittal K.; Jaramillo, Thomas F.; Yano, Junko

    2015-01-01

    Multielectron catalytic reactions, such as water oxidation, nitrogen reduction, or hydrogen production in enzymes and inorganic catalysts often involve multimetallic clusters. In these systems, the reaction takes place between metals or metals and ligands to facilitate charge transfer, bond formation/breaking, substrate binding, and release of products. In this study, we present a method to detect X-ray emission signals from multiple elements simultaneously, which allows for the study of char...

  4. Synchrotron radiation applied to the study of heterogeneous model catalyst surfaces

    International Nuclear Information System (INIS)

    The application of synchrotron radiation-based experimental techniques for the characterization of model catalyst surfaces is reviewed. The planar model systems considered are distinguished by their heterogeneous surface character. Prototypical examples are discussed to illustrate various aspects of model catalyst surfaces and they include oxide thin films on metal single crystal substrates, metal nanoparticles deposited on ordered oxide films, thin layers of oxides on oxide substrates, heterogeneous bimetallic surfaces and metal single crystal surfaces decorated by oxide nanoparticles. (author)

  5. Theoretical and experimental aspects of the bimetallic reinforcement bars steel - steel resistant to corrosion rolling process

    Directory of Open Access Journals (Sweden)

    S. Sawicki

    2010-11-01

    Full Text Available Purpose: Bimetallic bars which possess higher corrosion resistance and mechanical properties, it is the new kind of bimetallic bars, which are better than standard bars. The bimetallic bars are more often applied in concrete construction.Design/methodology/approach: The simulations of the bar rolling were carried out using the Forge2007® commercial program.Findings: The use of non-corrosive steel on plating layer assures receipt on a high durability and esthetics bimetallic bars.Practical implications: Bimetallic bars are chiefly used in the building industry at production of concrete constructions, and as working elements in bridge building in aggressive environment.Originality/value: Production of bimetallic bars is very difficult. One from many problems during production bimetallic bars is assurance good strength of bimetallic layer bond.

  6. Shaped Ir-Ni bimetallic nanoparticles for minimizing Ir utilization in oxygen evolution reaction.

    Science.gov (United States)

    Lim, Jinkyu; Yang, Sungeun; Kim, Chanyeon; Roh, Chi-Woo; Kwon, Yongwoo; Kim, Yong-Tae; Lee, Hyunjoo

    2016-04-25

    Shaped Ir-Ni bimetallic nanoparticles were synthesized and used for electrocatalytic oxygen evolution reaction (OER). The obtained bimetallic nanoparticles showed significantly enhanced Ir mass activity and durability compared with Ir nanoparticles. PMID:27034092

  7. Silver doped catalysts for treatment of exhaust

    Energy Technology Data Exchange (ETDEWEB)

    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.

  8. Dispersion state and catalytic properties of vanadia species on the surface of V2O5/TiO2 catalysts

    Institute of Scientific and Technical Information of China (English)

    许波连; 陈懿; 范以宁; 刘浏; 林明

    2002-01-01

    The dispersion state and catalytic properties of anatase-supported vanadia species are studied by means of X-ray diffraction (XRD), laser Raman spectroscopy (LRS), H2 temperature-programmed reduction (TPR) and the selective oxidation of o-xylene to phthalic anhydride. The almost identical values of the experimental dispersion capacity of V2O5 on anatase and the surface vacant sites available on the preferentially exposed (001) plane of anatase suggest that the highly dispersed vanadium cations are bonded to the vacant sites on the surface of anatase as derived by the incorporation model. When the loading amount of V2O5 is far below its dispersion capacity, the dispersed vanadia species might mainly consist of isolated VOx species bridging to the surface through V-O-Ti bonds. With the increase of V2O5 loading the isolated vanadia species interact with their nearest neighbors (either isolated or polymerized vanadia) through bridging V-O-V at the expenses of V-O-Ti bonds, resulting in the increase of the ra

  9. Preparation and Catalytic Activity for Aerobic Glucose Oxidation of Crown Jewel Structured Pt/Au Bimetallic Nanoclusters

    Science.gov (United States)

    Zhang, Haijun; Wang, Liqiong; Lu, Lilin; Toshima, Naoki

    2016-08-01

    Understanding of the “structure-activity” relations for catalysts at an atomic level has been regarded as one of the most important objectives in catalysis studies. Bimetallic nanoclusters (NCs) in its many types, such as core/shell, random alloy, cluster-in-cluster, bi-hemisphere, and crown jewel (one kind of atom locating at the top position of another kind of NC), attract significant attention owing to their excellent optical, electronic, and catalytic properties. PVP-protected crown jewel-structured Pt/Au (CJ-Pt/Au) bimetallic nanoclusters (BNCs) with Au atoms located at active top sites were synthesized via a replacement reaction using 1.4-nm Pt NCs as mother clusters even considering the fact that the replacement reaction between Pt and Au3+ ions is difficult to be occurred. The prepared CJ-Pt/Au colloidal catalysts characterized by UV-Vis, TEM, HR-TEM and HAADF-STEM-EELS showed a high catalytic activity for aerobic glucose oxidation, and the top Au atoms decorating the Pt NCs were about 15 times more active than the Au atoms of Au NCs with similar particle size.

  10. A New Class of Highly Dispersed VOx Catalysts on Mesoporous Silica: Synthesis, Characterization, and Catalytic Activity in the Partial Oxidation of Ethanol

    Energy Technology Data Exchange (ETDEWEB)

    Kwak, Ja Hun; Herrera, Jose E.; Hu, Jian Zhi; Wang, Yong; Peden, Charles HF

    2006-01-26

    The morphology of vanadium oxide supported on a titania-modified mesoporous silica (MCM-41), obtained by means of a careful grafting process through atomic layer deposition, was studied using a variety of characterization techniques. The XRD together with TEM, 51V-NMR, Raman, FTIR and DRS-UV-Vis results showed that the vanadia species are extremely well dispersed onto the surface of the mesoporous support; the dispersion being stable upon thermal treatments up to 400 °C. Studies of the catalytic activity of these materials were performed using the partial oxidation of ethanol as a probe reaction. The results indicate an intrinsic relationship between dispersion, the presence of a TiO2-VOx phase, and catalytic activity for oxidation and dehydration.

  11. Ammonia Decomposition over Bimetallic Nitrides Supported on γ-Al2O3

    Institute of Scientific and Technical Information of China (English)

    Chun Shan LU; Xiao Nian LI; Yi Feng ZHU; Hua Zhang LIU; Chun Hui ZHOU

    2004-01-01

    A series of monometallic nitrides and bimetallic nitrides were prepared by temperature-programmed reaction with NH3. The effects of Co, Ni and Fe additives and the synergic action between Fe, Co, Ni and Mo on the ammonia decomposition activity were investigated. TPR-MS, XRD were also carried out to obtain better insight into the structure of the bimetallic nitride. The results of ammonia decomposition activity show that bimetallic nitrides are more active than monometallic nitrides or bimetallic oxides.

  12. New synthesis ways of supported metallic catalysts and structure-reactivity relations in catalysis by metals; Nouvelles voies de syntheses de catalyseurs metalliques supportes et relations structure-reactivite en catalyse par les metaux

    Energy Technology Data Exchange (ETDEWEB)

    Uzio, D.

    2006-01-15

    This work deals with some research studies in the field of supported metallic catalysts. In all these works have been studied the characteristics bound to the active sites and the relations between these characteristics and the catalytic performances. The genesis of colloidal suspensions of transition metallic oxide has been used for the preparation of selective hydrogenation catalysts. At first studied in the case of palladium, this new synthesis way has been used for other metals such as Pt, Ni or Co. These studies have then been developed for preparing bimetallic catalysts (PdSn) with as supplementary aim the control of the homogeneity of the bimetallic character at the scale of nano-metric particles. These works have particularly allowed to specify the chemistry of the solutions of some metallic complexes and to rationalize the chemical processes carried out in the usual fabrication processes. Studies on size effects and the study of the reactivity of the nano and sub nano-metric particle have then been developed. Indeed, the clusters containing some atoms can see their intrinsic properties varied very strongly under the influence of several parameters as the number of atoms, the nature of the support, the reactional atmosphere. Using the knowledge acquired during the preceding works (chemistry of palladium aqueous solutions), the study of new methods of preparation of particles containing very few atoms has brought new data on the properties of hyper dispersed particles as well as on the principle of sensitivity to structure. The contribution of the support to the catalytic process for the hydrogenation of different substrates has been studied too. (O.M.)

  13. Investigating the Dispersion Behavior in Solvents, Biocompatibility, and Use as Support for Highly Efficient Metal Catalysts of Exfoliated Graphitic Carbon Nitride.

    Science.gov (United States)

    Ayán-Varela, M; Villar-Rodil, S; Paredes, J I; Munuera, J M; Pagán, A; Lozano-Pérez, A A; Cenis, J L; Martínez-Alonso, A; Tascón, J M D

    2015-11-01

    The liquid-phase exfoliation of graphitic carbon nitride (g-C3N4) to afford colloidal dispersions of two-dimensional flakes constitutes an attractive route to facilitate the processing and implementation of this novel material toward different technological applications, but quantitative knowledge about its dispersibility in solvents is lacking. Here, we investigate the dispersion behavior of exfoliated g-C3N4 in a wide range of solvents and evaluate the obtained results on the basis of solvent surface energy and Hildebrand/Hansen solubility parameters. Estimates of the three Hansen parameters for exfoliated g-C3N4 from the experimentally derived data yielded δD ≈ 17.8 MPa(1/2), δP ≈ 10.8 MPa(1/2), and δH ≈ 15.4 MPa(1/2). The relatively high δH value suggested that, contrary to the case of other two-dimensional materials (e.g., graphene or transition metal dichalcogenides), hydrogen-bonding plays a substantial role in the efficient interaction, and thus dispersibility, of exfoliated g-C3N4 with solvents. Such an outcome was attributed to a high density of primary and/or secondary amines in the material, the presence of which was associated with incomplete condensation of the structure. Furthermore, cell proliferation tests carried out on thin films of exfoliated g-C3N4 using murine fibroblasts suggested that this material is highly biocompatible and noncytotoxic. Finally, the exfoliated g-C3N4 flakes were used as supports in the synthesis of Pd nanoparticles, and the resulting hybrids exhibited an exceptional catalytic activity in the reduction of nitroarenes.

  14. Bimetallic layered castings alloy steel – carbon cast steel

    Directory of Open Access Journals (Sweden)

    T. Wróbel

    2011-01-01

    Full Text Available In paper is presented technology of bimetallic layered castings based on founding method of layer coating directly in cast processso-called method of mould cavity preparation. Prepared castings consist two fundamental parts i.e. bearing part and working part (layer. The bearing part of bimetallic layered casting is typical foundry material i.e. ferritic-pearlitic carbon cast steel, whereas working part (layer is plate of austenitic alloy steel sort X10CrNi 18-8. The ratio of thickness between bearing and working part is 8:1. The quality of the bimetallic layered castings was evaluated on the basis of ultrasonic NDT (non-destructive testing, structure and macro- and microhardness researches.

  15. Examples of material solutions in bimetallic layered castings

    Directory of Open Access Journals (Sweden)

    S. Tenerowicz

    2011-07-01

    Full Text Available In paper is presented technology of bimetallic layered castings based on founding method of layer coating directly in cast process so-called method of mould cavity preparation. Prepared castings consist two fundamental parts i.e. bearing part and working part (layer. The bearing part of bimetallic layered casting is typical foundry material i.e. pearlitic grey cast iron, whereas working part (layer is depending on accepted variant plates of alloy steels sort X6Cr13, X12Cr13, X10CrNi18-8 and X2CrNiMoN22-5-3. The ratio of thickness between bearing and working part is 8:1. The verification of the bimetallic layered castings was evaluated on the basis of ultrasonic NDT (non-destructive testing, structure and macro- and microhardness researches.

  16. Spin waves in antiferromagnetically coupled bimetallic oxalates.

    Science.gov (United States)

    Reis, Peter L; Fishman, Randy S

    2009-01-01

    Bimetallic oxalates are molecule-based magnets with transition-metal ions M(II) and M(')(III) arranged on an open honeycomb lattice. Performing a Holstein-Primakoff expansion, we obtain the spin-wave spectrum of antiferromagnetically coupled bimetallic oxalates as a function of the crystal-field angular momentum L(2) and L(3) on the M(II) and M(')(III) sites. Our results are applied to the Fe(II)Mn(III), Ni(II)Mn(III) and V(II)V(III) bimetallic oxalates, where the spin-wave gap varies from 0 meV for quenched angular momentum to as high as 15 meV. The presence or absence of magnetic compensation appears to have no effect on the spin-wave gap. PMID:21817242

  17. Structural, spectral and mechanical studies of bimetallic crystal: cadmium manganese thiocyanate single crystals

    Science.gov (United States)

    Manikandan, M.; Vijaya Prasath, G.; Bhagavannarayan, G.; Vijayan, N.; Mahalingam, T.; Ravi, G.

    2012-09-01

    A nonlinear optical bimetallic thiocyanate complex crystal, cadmium manganese thiocyanate (CMTC) has been successfully synthesized. The growth of single crystals of cadmium manganese thiocyanate has been accomplished from aqueous solution using slow evaporation method. The presence of manganese and cadmium in the synthesized material was confirmed through energy dispersive spectrum (EDS) analysis. Structural analysis was carried out using powder X-ray diffractometer (PXRD) and crystalline perfection of the grown crystals was ascertained by high-resolution X-ray diffraction (HRXRD) analysis. Fourier transform infrared (FTIR) spectrum was taken to confirm the functional groups. The transmittance spectrum of the crystal in the UV-visible region has been recorded and the cutoff wavelength has been determined. The dielectric measurements for the crystals were performed for various frequencies and temperatures. The mechanical properties were evaluated by Vickers microhardness testing, which reveals hardness and stiffness constant of the crystals.

  18. Structural, spectral and mechanical studies of bimetallic crystal: cadmium manganese thiocyanate single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Manikandan, M.; Vijaya Prasath, G.; Mahalingam, T.; Ravi, G. [Alagappa University, Department of Physics, Karaikudi (India); Bhagavannarayan, G.; Vijayan, N. [National Physical Laboratory, Materials Characterization Division, New Delhi (India)

    2012-09-15

    A nonlinear optical bimetallic thiocyanate complex crystal, cadmium manganese thiocyanate (CMTC) has been successfully synthesized. The growth of single crystals of cadmium manganese thiocyanate has been accomplished from aqueous solution using slow evaporation method. The presence of manganese and cadmium in the synthesized material was confirmed through energy dispersive spectrum (EDS) analysis. Structural analysis was carried out using powder X-ray diffractometer (PXRD) and crystalline perfection of the grown crystals was ascertained by high-resolution X-ray diffraction (HRXRD) analysis. Fourier transform infrared (FTIR) spectrum was taken to confirm the functional groups. The transmittance spectrum of the crystal in the UV-visible region has been recorded and the cutoff wavelength has been determined. The dielectric measurements for the crystals were performed for various frequencies and temperatures. The mechanical properties were evaluated by Vickers microhardness testing, which reveals hardness and stiffness constant of the crystals. (orig.)

  19. Effect of surface structure on the catalytic behavior of Ni:Cu/Al and Ni:Cu:K/Al catalysts for methane decomposition

    Institute of Scientific and Technical Information of China (English)

    S.Tajammul Hussain; Sheraz Gul; Muhammed Mazhar; Dalaver H.Anjum; Faical Larachi

    2008-01-01

    Methane decomposition using nickel, copper, and aluminum (Ni:Cu/Al) and nickel, copper, potassium, and alu-minum (Ni:Cu:K/Al) modified nano catalysts has been investigated for carbon fibers, hydrogen and hydrocarbon production. X-ray photoelectron spectroscopy (XPS), static secondary ion mass spectrometry (SSIMS), thermal gravimetric analysis (TGA),Fourier transform infrared (FT-IR), secondary electron microscopy/X-ray energy dispersive (SEM-EDX), and temperature pro-grammed desorption (TPD) were used to depict the chemistry of the catalytic results. These techniques revealed the changes in surface morphology and structure of Ni, Cu, Al, and K, and formation of bimetallic and trimetallic surface cationic sites with sifferent cationic species, which resulted in the production of graphitic form of pure carbon on Ni:Cu/Al catalyst. The addition of K has a marked effect on the product selectivity and reactivity of the catalyst system. K addition restricts the formation of carbon on the surface and increases the production of hydrogen and C2, C3 hydrocarbons during the catalytic reaction whereas no hydrocarbons are produced on the sample without K. This study completely maps the modified surface structure and its re-lationship with the catalytic behavior of both systems. The process provides a flexible route for the production of carbon fibers and hydrogen on Ni:Cu/Al catalyst and hydrogen along with hydrocarbons on Ni:Cu:K/Al catalyst. The produced carbon fibers are imaged using a transmission electron microscope (TEM) for diameter size and wall structure determination. Hydrogen produced is COx free, which can be used directly in the fuel cell system. The effect of the addition of Cu and its transformation and interaction with Ni and K is responsible for the production of CO/CO2 free hydrogen, thus producing an environmental friendly clean energy.

  20. Fe/Al bimetallic particles for the fast and highly efficient removal of Cr(VI) over a wide pH range: Performance and mechanism

    International Nuclear Information System (INIS)

    Highlights: • Bimetallic particles with different Fe/Al mass ratios were prepared. • High removal rate of Cr(VI) was achieved in acidic, neutral, and alkaline pH. • No total iron ions at pH 3.0–11.0 and nearly no Al3+ at pH 3.0–7.0 were released. • Galvanic cell effect and high specific surface area contributed to Cr(VI) removal. - Abstract: The iron/aluminum (Fe/Al) bimetallic particles with high efficiency for the removal of Cr(VI) were prepared. Fe/Al bimetallic particles were characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), SEM mapping, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). SEM mapping showed that the core of bimetal was Al, and the planting Fe was deposited on the surface of Al. In acidic and neutral conditions, Fe/Al bimetal can completely remove Cr(VI) from wastewater in 20 min. Even at pH 11.0, the Cr(VI) removal efficiency achieved was 93.5%. Galvanic cell effect and high specific surface area are the main reasons for the enhanced removal of Cr(VI) by bimetallic particles. There were no iron ions released in solutions at pH values ranging from 3.0 to 11.0. The released Al3+ ions concentrations in acidic and neutral conditions were all less than 0.2 mg/L. The bimetal can be used 4 times without losing activity at initial pH 3.0. XPS indicated that the removed Cr(VI) was immobilized via the formation of Cr(III) hydroxide and Cr(III)–Fe(III) hydroxide/oxyhydroxide on the surface of Fe/Al bimetal. The Fe/Al bimetallic particles are promising for further testing for the rapid and effective removal of contaminants from water

  1. Characterization measurements of Ti-SS bimetallic transition joint samples

    International Nuclear Information System (INIS)

    A small set of bimetallic tubes has been investigated for the purpose to determine characteristics of samples at different conditions of tests for more statistics. Nine bimetallic samples have been manufactured at the Russian Federal Nuclear Center - VNIIEF (Sarov, Russia) using explosion technology for welding titanium and stainless steel tubes. During the tests eight samples have shown an excellent behaviour. This result is very good and we believe that these samples can be used for the construction of the cavity vessels. A preliminary measurement on the residual magnetic moment around junction line between the two materials has been carried out

  2. Low-temperature steam-reforming of ethanol over ZnO-supported Ni and Cu catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Homs, Narcis; Llorca, Jordi; De la Piscina, Pilar Ramirez [Departament de Quimica Inorganica, Universitat de Barcelona, C/Marti i Franques 1-11, 08028 Barcelona (Spain)

    2006-08-15

    ZnO-supported Ni and Cu as well as bimetallic Co-Ni and Co-Cu catalysts containing ca. 0.7wt% sodium promoter and prepared by the co-precipitation method were tested in the ethanol steam-reforming reaction at low temperature (523-723K), using a bioethanol-like mixture diluted in Ar. Monometallic ZnO-supported Cu or Ni samples do not exhibit good catalytic performance in the steam-reforming of ethanol for hydrogen production. Copper catalyst mainly dehydrogenates ethanol to acetaldehyde, whereas nickel catalyst favours ethanol decomposition. However, the addition of Ni to ZnO-supported cobalt has a positive effect both on the production of hydrogen at low temperature (<573K), and on catalyst stability. Evidence for alloy formation as well as mixed oxides at the microstructural level was found in the bimetallic systems after running the ethanol steam-reforming reaction by HRTEM-EELS. (author)

  3. Magnetic bimetallic nanoparticles supported reduced graphene oxide nanocomposite: Fabrication, characterization and catalytic capability

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Lei; Wu, Tao; Xu, Xiaoyang; Xia, Fengling; Na, Heya [School of Science, Tianjin University, Tianjin 300072 (China); Liu, Yu, E-mail: liuyuls@163.com [School of Science, Tianjin University, Tianjin 300072 (China); Qiu, Haixia [School of Science, Tianjin University, Tianjin 300072 (China); Wang, Wei [School of Chemical Engineering, Tianjin University, Tianjin 300072 (China); Gao, Jianping, E-mail: jianpinggao2012@126.com [School of Science, Tianjin University, Tianjin 300072 (China)

    2015-04-15

    Highlights: • Ni and Ag nanoparticles loaded on RGO (Ni–Ag@RGO) were fabricated in a one-pot reaction. • The Ni–Ag@RGO were excellent catalysts for the reduction of 4-nitrophenol. • The Ni–Ag@RGO showed superior catalytic activity for photodegradation of methyl orange. • The Ni–Ag@RGO exhibit good reusability in a magnetic field. - Abstract: A facile method for preparing Ni–Ag bimetallic nanoparticles supported on reduced graphene oxide (Ni–Ag@RGO hybrid) has been established. Hydrazine hydrate was used as the reducing agent to reduce the graphene oxide, Ni{sup 2+} and Ag{sup +} to form Ni–Ag@RGO hybrid. The prepared hybrid was further characterized by X-ray diffraction, thermogravimetric analysis, X-ray photoelectron spectroscopy, and transmission electron microscopy. Interestingly, the prepared material shown good magnetic properties, which were determined by vibrating sample magnetometer. In addition, the Ni–Ag@RGO hybrid exhibited excellent catalytic activity for the reduction of 4-nitrophenol and the photodegradation of methyl orange. The catalytic process was monitored by determining the change in the concentration of the reactants with time using ultraviolet–visible absorption spectroscopy. After completion of the reaction, the catalyst can be separated from the reaction system simply under a magnet field and shows good recyclability.

  4. Synthesis of Pt-Pd bimetallic nanoparticles anchored on graphene for highly active methanol electro-oxidation

    Science.gov (United States)

    Zhang, Yuting; Chang, Gang; Shu, Honghui; Oyama, Munetaka; Liu, Xiong; He, Yunbin

    2014-09-01

    A simple, one-step reduction route was employed to synthesize bimetallic Pt-Pd nanoparticles (Pt-PdNPs) supported on graphene (G) sheets, in which the reduction of graphite oxide and metal precursor was carried out simultaneously using ascorbic acid as a soft reductant. The morphology and structure of Pt-PdNPs/G composites were characterized using X-ray diffraction, Transmission Electron Microscopy, Field Emission Scanning Electron Microscopy and X-ray Photoelectron Spectroscopy analysis. The results show that Pt-Pd bimetallic nanoparticles were successfully synthesized and evenly anchored on the graphene sheets. Electrochemical experiments, including cyclic voltammetry and chronoamperometric measurements, were performed to investigate the electrochemical and electrocatalytic properties of the Pt-PdNPs/G composites. It was found that Pt-PdNPs/G composites show better electrocatalytic activity and stability towards the electro-oxidation of methanol than its counterparts such as composites composed of graphene-supported monometallic nanoparticles (PtNPs/G, PdNPs/G) and free-standing (Pt-PdNPs) and Vulcan-supported bimetallic Pt-Pd nanoparticles (Pt-PdNPs/V). The results could be attributed to the synergetic effects of the Pt-Pd nanoparticles and the enhanced electron transfer of graphene. The electrocatalytic activity of Pt-PdNPs/G changed with the Pd content in the Pt-Pd alloy, and the best performance was achieved with a Pt-Pd ratio of 1/3 in an alkaline environment. Our study indicates the potential use of Pt-PdNPs/G as new anode catalyst materials for direct methanol fuel cells.

  5. Advanced liquefaction using coal swelling and catalyst dispersion techniques. Volume 2, appendices. Final technical report, October 1, 1991--September 30, 1994

    Energy Technology Data Exchange (ETDEWEB)

    Curtis, C.W. [Auburn Univ., AL (United States); Chander, S. [Pennsylvania State Univ., College Park, PA (United States); Gutterman, C.

    1995-04-01

    Liquefaction experiments were undertaken using subbituminous Black Thunder mine coal to observe the effects of aqueous SO{sub 2} coal beneficiation and the introduction of various coal swelling solvents and catalyst precursors. Aqueous SO{sub 2} beneficiation of Black Thunder coal removed alkali metals and alkaline earth metals, increased the sulfur content and increased the catalytic liquefaction conversion to THF solubles compared to untreated Black Thunder coal. The liquefaction solvent had varying effects on coal conversion, depending upon the type of solvent added. The hydrogen donor solvent, dihydroanthracene, was most effective, while a coal-derived Wilsonville solvent promoted more coal conversion than did relatively inert 1-methylnaphthalene. Swelling of coal with hydrogen bonding solvents tetrahydrofuran (THF), isopropanol, and methanol, prior to reaction resulted in increased noncatalytic conversion of both untreated and SO{sub 2} treated Black Thunder coals, while dimethylsulfoxide (DMSO), which was absorbed more into the coal than any other swelling solvent, was detrimental to coal conversion. Swelling of SO{sub 2} treated coal before liquefaction resulted in the highest coal conversions; however, the untreated coal showed the most improvements in catalytic reactions when swelled in either THF, isopropanol, or methanol prior to liquefaction. The aprotic solvent DMSO was detrimental to coal conversion.

  6. Growth Mechanism of Single-Walled Carbon Nanotubes on Iron–Copper Catalyst and Chirality Studies by Electron Diffraction

    DEFF Research Database (Denmark)

    He, Maoshuai; Liu, Bilu; Chernov, Alexander I.;

    2012-01-01

    Chiralities of single-walled carbon nanotubes grown on an atomic layer deposition prepared bimetallic FeCu/MgO catalyst were evaluated quantitatively using nanobeam electron diffraction. The results reveal that the growth yields nearly 90% semiconducting tubes, 45% of which are of the (6,5) type...... by impregnation, showing similar catalytic performance as the atomic layer deposition-prepared catalyst, yielding single-walled carbon nanotubes with a similar narrow chirality distribution....

  7. Methanol Oxidation on Model Elemental and Bimetallic Transition Metal Surfaces

    DEFF Research Database (Denmark)

    Tritsaris, G. A.; Rossmeisl, J.

    2012-01-01

    Direct methanol fuel cells are a key enabling technology for clean energy conversion. Using density functional theory calculations, we study the methanol oxidation reaction on model electrodes. We discuss trends in reactivity for a set of monometallic and bimetallic transition metal surfaces, flat...

  8. New bimetallic EMF cell shows promise in direct energy conversion

    Science.gov (United States)

    Hesson, J. C.; Shimotake, H.

    1968-01-01

    Concentration cell, based upon a thermally regenerative cell principle, produces electrical energy from any large heat source. This experimental bimetallic EMF cell uses a sodium-bismuth alloy cathode and a pure liquid sodium anode. The cell exhibits reliability, corrosion resistance, and high current density performance.

  9. Bimetallic alloy electrocatalysts with multilayered platinum-skin surfaces

    Science.gov (United States)

    Stamenkovic, Vojislav R.; Wang, Chao; Markovic, Nenad M.

    2016-01-26

    Compositions and methods of preparing a bimetallic alloy having enhanced electrocatalytic properties are provided. The composition comprises a PtNi substrate having a surface layer, a near-surface layer, and an inner layer, where the surface layer comprises a nickel-depleted composition, such that the surface layer comprises a platinum skin having at least one atomic layer of platinum.

  10. Electrochemical oxidation of ammonia on carbon-supported bi-metallic PtM (M = Ir, Pd, SnO{sub x}) nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Lomocso, Thegy L. [Department of Chemical and Biological Engineering, University of Ottawa, 161 Louis-Pasteur, Ottawa, ON K1N 6N5 (Canada); Baranova, Elena A., E-mail: elena.baranova@uottawa.ca [Department of Chemical and Biological Engineering, University of Ottawa, 161 Louis-Pasteur, Ottawa, ON K1N 6N5 (Canada)

    2011-10-01

    Highlights: > Oxidation of NH{sub 3} is investigated on carbon-supported Pt and PtM (M = Pd, Ir, SnO{sub x}) nanoparticles. > Carbon supported PtPd and PtIr nanoparticles show higher catalytic activity if compared to Pt nanocatalyst. > Pt{sub 7}Ir{sub 3} nanoparticles combine good catalytic activity and enhanced stability for NH{sub 3} oxidation. > Electronic effect between two metals in PtIr is responsible for increase in the catalytic activity. - Abstract: Ammonia electro-oxidation was studied in alkaline solution on carbon-supported Pt and bimetallic Pt{sub y}M{sub 1-y} (M = Pd, Ir, SnO{sub x} and y = 70, 50 at.%) nanoparticles. Catalysts were synthesized using the modified polyol method and deposited on carbon, resulting in 20 wt.% of metal loading. Particle size, structure and surface composition of the particles were investigated using TEM, XRD and XPS. Mean size of PtM bi-metallic nanoparticles varied between 2.0 and 4.7 nm, depending on the second metal (M). XRD revealed the structure of all bi-metallic particles to be face-centered cubic and confirmed alloy formation for Pt{sub y}Pd{sub 1-y} (y = 70, 50 at.%) and Pt{sub 7}Ir{sub 3}nanoparticles, as well as partial alloying between Pt and SnO{sub x}. Electrochemical behaviour of ammonia on Pt and PtM nanoparticles is comparable to that expected for bulk Pt and PtM alloys. Addition of Pd to Pt at the nanoscale decreased the onset potential of ammonia oxidation if compared to pure platinum nanoparticles; however stability of the catalyst was poor. For Pt{sub 7}(SnO{sub x}){sub 3}, current densities were similar to Pt, whereas catalyst stability against deactivation was improved. It is found that carbon supported Pt{sub 7}Ir{sub 3} nanoparticles combine good catalytic activity with enhanced stability for ammonia electro-oxidation. Electronic effect generated between two metals in the bimetallic nanoparticles might be responsible for increase in the catalytic activity of Pd- and Ir-containing catalysts, causing

  11. Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts.

    Science.gov (United States)

    Yin, Peiqun; Yao, Tao; Wu, Yuen; Zheng, Lirong; Lin, Yue; Liu, Wei; Ju, Huanxin; Zhu, Junfa; Hong, Xun; Deng, Zhaoxiang; Zhou, Gang; Wei, Shiqiang; Li, Yadong

    2016-08-26

    A new strategy for achieving stable Co single atoms (SAs) on nitrogen-doped porous carbon with high metal loading over 4 wt % is reported. The strategy is based on a pyrolysis process of predesigned bimetallic Zn/Co metal-organic frameworks, during which Co can be reduced by carbonization of the organic linker and Zn is selectively evaporated away at high temperatures above 800 °C. The spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements both confirm the atomic dispersion of Co atoms stabilized by as-generated N-doped porous carbon. Surprisingly, the obtained Co-Nx single sites exhibit superior ORR performance with a half-wave potential (0.881 V) that is more positive than commercial Pt/C (0.811 V) and most reported non-precious metal catalysts. Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C. Our findings open up a new routine for general and practical synthesis of a variety of materials bearing single atoms, which could facilitate new discoveries at the atomic scale in condensed materials. PMID:27491018

  12. Physicochemical and isomerization property of Pt/SAPO-11 catalysts promoted by rare earths

    Institute of Scientific and Technical Information of China (English)

    刘维桥; 尚通明; 周全发; 任杰; 孙予罕

    2009-01-01

    Monometallic catalyst Pt/SAPO-11 was prepared by impregnation method.Bimetallic catalysts LaPt/SAPO-11 or CePt/SAPO-11 was prepared by sequential impregnation method.The catalysts were characterized by X-ray diffraction(XRD),nitrogen adsorption,temperature-programmed desorption of ammonia(NH3-TPD),and Fourier transform infrared spectroscopy(FT-IR) techniques.The results showed that with the addition of rare earths the BET surface areas,pore volume,the amount of Bronsted acid and the total acidity of catalys...

  13. Three-Dimensional Graphene Supported Bimetallic Nanocomposites with DNA Regulated-Flexibly Switchable Peroxidase-Like Activity.

    Science.gov (United States)

    Yuan, Fang; Zhao, Huimin; Zang, Hongmei; Ye, Fei; Quan, Xie

    2016-04-20

    A synergistic bimetallic enzyme mimetic catalyst, three-dimensional (3D) graphene/Fe3O4-AuNPs, was successfully fabricated which exhibited flexibly switchable peroxidase-like activity. Compared to the traditional 2D graphene-based monometallic composite, the introduced 3D structure, which was induced by the addition of glutamic acid, and bimetallic anchoring approach dramatically improved the catalytic activity, as well as the catalysis velocity and its affinity for substrate. Herein, Fe3O4NPs acted as supporters for AuNPs, which contributed to enhance the efficiency of electron transfer. On the basis of the measurement of Mott-Schottky plots of graphene and metal anchored hybrids, the catalysis mechanism was elucidated by the decrease of Fermi level resulted from the chemical doping behavior. Notably, the catalytic activity was able to be regulated by the adsorption and desorption of single-stranded DNA molecules, which laid a basis for its utilization in the construction of single-stranded DNA-based colorimetric biosensors. This strategy not only simplified the operation process including labeling, modification, and imprinting, but also protected the intrinsic affinity between the target and biological probe. Accordingly, based on the peroxidase-like activity and its controllability, our prepared nanohybrids was successfully adopted in the visualized and label-free sensing detections of glucose, sequence-specific DNA, mismatched nucleotides, and oxytetracycline. PMID:27018504

  14. Fabrication of electrically conductive nickel-silver bimetallic particles via polydopamine coating.

    Science.gov (United States)

    Kim, Sung Yeop; Kim, Jieun; Choe, Jaehoon; Byun, Young Chang; Seo, Jung Hyun; Kim, Do Hyun

    2013-11-01

    Inspired by adhesive proteins excreted by marine mussels, dopamine can act as a versatile surface modification agent for various organic and inorganic materials. By using adhesive polydopamine (PDA) as an intermediate layer, a simple and novel method for fabricating nickel-PDA-silver (Ni-PDA-Ag) bimetallic composite particles was developed. Ni-PDA-Ag bimetallic particles were fabricated by dispersing Ni particles in an aqueous dopamine solution followed by electroless Ag plating on the prepared Ni-PDA particles. A PDA layer with nano-meter thickness was deposited spontaneously on the surface of the Ni particles by oxidative self-polymerization of dopamine under alkaline conditions. Electroless Ag plating on the prepared Ni-PDA particles was carried out in the presence of a glucose solution as a reducing agent. Ni-PDA particles and Ni-PDA-Ag composite particles with a PDA intermediate layer were characterized by X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared (FT-IR) spectroscopy, field-emission scanning electron microscopy (FE-SEM), field-emission transmission electron microscopy (FE-TEM), and X-ray diffraction (XRD). In addition, the electrical conductivity of as-prepared composite particles was evaluated by a 4-point probe. The PDA layer deposited on the surface of Ni was confirmed by XPS spectra, FT-IR spectroscopy, and FE-TEM. FE-SEM images demonstrated that Ag nanoparticles were successfully plated on the PDA layer-coated Ni particles after the electroless Ag plating process. XRD patterns also confirmed the presence of Ag in a metallic state. In addition, the sheet resistance of as-prepared composite particles showed a tendency to decrease with increasing AgNO3 concentration. PMID:24245300

  15. Monodispersed bimetallic PdAg nanoparticles with twinned structures: Formation and enhancement for the methanol oxidation

    OpenAIRE

    Zhen Yin; Yining Zhang; Kai Chen; Jing Li; Wenjing Li; Pei Tang; Huabo Zhao; Qingjun Zhu; Xinhe Bao; Ding Ma

    2014-01-01

    Monodispersed bimetallic PdAg nanoparticles can be fabricated through the emulsion-assisted ethylene glycol (EG) ternary system. Different compositions of bimetallic PdAg nanoparticles, Pd80Ag20, Pd65Ag35 and Pd46Ag54 can be obtained via adjusting the reaction parameters. For the formation process of the bimetallic PdAg nanoparticles, there have two-stage growth processes: firstly, nucleation and growth of the primary nanoclusters; secondly, formation of the secondary nanoparticles with the s...

  16. Facile growth of Ag@Pt bimetallic nanorods on electrochemically reduced graphene oxide for an enhanced electrooxidation of hydrazine

    Indian Academy of Sciences (India)

    Jeena S E; Selvaraju T

    2016-03-01

    An efficient transducer was constructed by the direct growth of bimetallic Ag@Pt nanorods (NRDs) on L−tryptophan functionalized electrochemically reduced graphene oxide (L−ERGO) modified electrode using galvanic displacement method for the electrooxidation of hydrazine.Initially, one dimensionalbimetallic Ag@Cu core−shell NRDs were grown on L−ERGO modified electrode by simple seed mediated growth method. Then, the Cu shells at bimetallic NRDs were exchanged by Pt through galvanic displacement method. Accordingly, the synergetic effect produced by the combination of Ag and Pt as NRDs at L−ERGO surface enabled an enhancement in the electrocatalytic efficiency for hydrazine oxidation. L−ERGO supported bimetallic Ag@Pt NRDs were characterised by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX) and cyclic voltammetric techniques. Finally, the modified electrode was successfully used for the electrooxidation of hydrazine in PB (pH 7.4)with a detection limit of 6*10−7M(SdivN=3). Importantly, the presence of Pt on Ag surface plays a vital role in the electrooxidation of [N2H4] at−0.2 V with an onset potential at−0.5 V where its overpotential has decreased. On the other hand, L−ERGO nanosheets tend to facilitate an effective immobilization of low density Ag seeds (Agseeds) on its surface. Chronoamperometric studies were used to study the linear correlation of [N2H4] between 1 mM and 10 mM. The modified electrode shows a high sensitivity and selectivity for a trace amount of N2H4 in the presence of different interfering cations and anions

  17. Characterization and Dehydrogenation Activity of SBA-15 and HMS Supported Chromia Catalysts

    Institute of Scientific and Technical Information of China (English)

    YUE,Hong-Yong(乐洪咏); ZHENG,Bo(郑波); YUE,Ying-Hong(乐英红); ZHANG,Xue-Zheng(张雪峥); HUA,Wei-Ming(华伟明); GAO,Zi(高滋)

    2002-01-01

    SBA-15 and HMS supported chromia catalysts were prepared and characterized. Chromia is highly dispersed on the mesoporous supports when its loading is ≤7 wt%. The supported catalysts display high activity, selectivity and stability for dehydrogenation of ethyibenzene and propane. ESR measurement of the catalysts before and after reaction shows that the active species for dehydrogenation reaction might be Cr3 + species on the catalyst surface, and the activity of the catalyst is probably correlated with the dispersion of Cr3+ species.

  18. Dehalogenation of Aryl Halides Catalyzed by MontK10 Immobilized PVP-Pd-Sn Catalyst in Aqueous System

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    A series of PVP-Pd-Sn/MontK10 catalysts were prepared by immobilization of PVP[poly(N-vinyl-2-pyrrolidone)] supported bimetallic catalyst using MontK10 as carrier. This catalyst has good catalytic activity for hydrogen transfer dehalogenation of aryl halides. The catalytic reaction was carried out in aqueous system in the presence of phase transfer catalyst and sodium formate as hydrogen source. The catalyst with loading Pd 0.19wt% and molar ratio of Pd/Sn 8:1 gives the highest activity and good stability. This catalyst is more reducible with NaBH4. It is also found that the catalyst is easily separated from the reaction system.

  19. In/Co-ferrierite. A highly active catalyst for the CH4-SCR NO process under presence of steam

    International Nuclear Information System (INIS)

    A series of monometallic (In, Co) and bimetallic (In/Co and Co/In) catalysts supported on ferrierite type zeolite were tested in the selective catalytic reduction of nitric oxide, in the presence of methane and excess of oxygen. All the catalysts were prepared by contact-induced ion exchange. A strong synergistic effect was observed for the catalysts containing both indium and cobalt, in comparison with the monometallic samples. For these bimetallic catalysts, a very high selectivity to nitrogen and rather efficient fuel economy were observed under the standard reaction conditions (NO=1000ppm, CH4=2000ppm, O2=4%, H2O=2500ppm). Moreover, the In/Co-ferrierite catalyst displays significant stability under a prolonged test (≅200h) in the presence of 2.5% of steam: the activity dropped rather moderately but was completely restored if steam supply was cut off, while the selectivity of the reaction was not affected in the whole temperature range scanned (300-500oC). The study suggests that a redox-type promotional effect of Co species on NO oxidation may be responsible of the strong synergistic effect detected in bimetallic In-Co formulations. (author)

  20. Homogeneous catalysts

    CERN Document Server

    Chadwick, John C; Freixa, Zoraida; van Leeuwen, Piet W N M

    2011-01-01

    This first book to illuminate this important aspect of chemical synthesis improves the lifetime of catalysts, thus reducing material and saving energy, costs and waste.The international panel of expert authors describes the studies that have been conducted concerning the way homogeneous catalysts decompose, and the differences between homogeneous and heterogeneous catalysts. The result is a ready reference for organic, catalytic, polymer and complex chemists, as well as those working in industry and with/on organometallics.

  1. Compositional changes of Pd-Au bimetallic nanoclusters upon hydrogenation

    OpenAIRE

    Di Vece, M; Bals, S.; Verbeeck, J.; Lievens, P.; van Tendeloo, G.

    2009-01-01

    Changes in the size distribution and composition of bimetallic Pd-Au nanoclusters have been observed after hydrogen exposure. This effect is caused by hydrogen-induced Ostwald ripening whereby the hydrogen reduces the binding energy of the cluster atoms leading to their detachment from the cluster. The composition changes due to a difference in mobility of the detached palladium and gold atoms on the surface. Fast palladium atoms contribute to the formation of larger nanoclusters, while the s...

  2. Thermoelastic stability of bimetallic shallow shells of revolution

    OpenAIRE

    Batista, Milan; Kosel, Franc

    2015-01-01

    This article considers the thermoelastic stability of bimetallic shallow shells of revolution. Basic equations are derived from Reissner's non-linear theory of shells by assuming that deformations and rotations are small and that materials are linear elastic. The equations are further specialized for the case of a closed spherical cup. For this case the perturbated initial state is considered and it is shown that only in the cases when the cup edge is free or simply supported buckling under h...

  3. In situ XAFS characterization of bimetallic nanoparticle catalysts PtCo/C structure changes in the working conditions%原位XAFS表征双金属纳米催化剂PtCo/C在工作状态下的结构变化

    Institute of Scientific and Technical Information of China (English)

    尚明丰; 赵天天; 鲍洪亮; 段佩权; 林瑞; 黄宇营; 王建强

    2016-01-01

    用两步还原法制备的PtCo/C (10 wt% Pt)纳米催化剂具有与商业催化剂Pt/C (20 wt% Pt)接近的催化反应活性,使贵金属Pt的用量减少了50%。利用上海光源BL14W1线站的质子交换膜燃料电池(Proton exchange membrane fuel cell, PEMFC)原位X射线吸收精细结构谱(X-ray absorption fine structure, XAFS)实验装置,在以该PtCo/C作为燃料电池的阴极催化剂,以Pd/C作为阳极催化剂的条件下,原位表征PtCo/C在工作状态下的结构变化,PtCo/C 的非原位 XAFS 数据没有观察到 Pt−Co 合金成分,发现存在显著的 Co−O 键和 Co−O−Co键贡献,且与Pt/C相比,Pt的氧化程度更高且具有更短的Pt−Pt金属键长,说明PtCo/C中的Co主要以氧化物种形式存在,且Co的存在影响着活性成分Pt的结构。原位XAFS数据表明随着电压的逐渐降低,PtCo/C中Pt和Co的氧化程度降低,揭示了在催化反应过程中Pt的d电子向过渡金属Co的转移过程。%AbstractBackground:The proton exchange membrane fuel cell (PEMFC) is considered as one of the most promising clean energy sources in the future, because of its high energy density and simple construction. However, the large scale commercial application of fuel cell is limited by the factors such as cost, durability and reliability. Purpose: For the purpose of reducing the cost and improving the performance of the PEMFC, transition metal elements alloy Pt nanoparticles (PtFe/C, PtCo/C, PtNi/C) catalysts have been studied in recent years.Methods:In situ X-ray absorption fine structure (XAFS) experimental testing device for PEMFC on beamline (BL14W1) of XAFS spectroscopy at the Shanghai Synchrotron Radiation Facility (SSRF) is conducted to explore the nanostructure changes of PtCo/C during the fuel cell operation. Results:In situ XAFS spectra indicts that Pt, and Co are gradually being reduced as the voltage of fuel cell decreases.Ex-situ XAFS spectra show Pt and Co did not form Pt

  4. Mg-AI Mixed Oxides Supported Bimetallic Au-Pd Nanoparticles with Superior Catalytic Properties in Aerobic Oxidation of Benzyl Alcohol and Glycerol

    Institute of Scientific and Technical Information of China (English)

    王亮; 张伟; 曾尚景; 苏党生; 孟祥举; 肖丰收

    2012-01-01

    Nano-sized Au and Pd catalysts are favorable for oxidations with molecular oxygen, and the preparation of this kind of nanoparticles with high catalytic activities is strongly desirable. We report a successful synthesis of bimetal- lic Au-Pd nanoparticles with rich edge and comer sites on unique support of Mg-AI mixed oxides (Au-Pd/MAO), which are favorable for producing metal nanoparticles with high degree of coordinative unsaturation of metal atoms The systematic microscopic characterizations confirm the bimetallic Au-Pd nanoparticles are present as Au-Pd alloy The irregular shape of the bimetallic nanoparticles are directly observed in HRTEM images. As we expected, Au-Pd/MAO gives very excellent catalytic performances in the aerobic oxidation of benzyl alcohol and glycerol. For example, Au-Pd/MAO shows very high TOF of 91000 h i at 433 K with molecular oxygen at air pressure in solvent-free oxidation of benzyl alcohol; this catalyst also shows relatively high selectivity for tartronic acid (TA- RAC, 36.6%) at high conversion (98.5%) in aerobic oxidation of glycerol. The superior catalytic properties of Au-Pd/MAO would be potentially important tbr production of fine chemicals.

  5. Synthesis by Microwaves of Bimetallic Nano-Rhodium-Palladium

    Directory of Open Access Journals (Sweden)

    M. Ugalde

    2013-01-01

    Full Text Available An improved acrylamide sol-gel technique using a microwave oven in order to synthesize bimetallic Rh-Pd particles is reported and discussed. The synthesis of Pd and Rh nanoparticles was carried out separately. The polymerization to form the gel of both Rh and Pd was carried out at 80°C under constant agitations. The method chosen to prepare the Rh and Pd xerogels involved the decomposition of both gels. The process begins by steadily increasing the temperature of the gel inside a microwave oven (from 80°C to 170°C. In order to eliminate the by-products generated during the sol-gel reaction, a heat treatment at a temperature of 1000°C for 2 h in inert atmosphere was carried out. After the heat treatment, the particle size increased from 50 nm to 200 nm, producing the bimetallic Rh-Pd clusters. It can be concluded that the reported microwave-assisted, sol-gel method was able to obtain nano-bimetallic Rh-Pd particles with an average size of 75 nm.

  6. Moessbauer study of function of magnesium in iron oxide catalysts

    Institute of Scientific and Technical Information of China (English)

    YangJie-Xin; MaoLian-Sheng; 等

    1997-01-01

    Moessbauer spectroscopy has been utilized for studying the action of Mg element in iron oxide catalysts used for the dehydrogenation of ethylbenzene to sytrene.The experimental results show that the presence of opportune amount of Mg can enhance the stability and dispersion of catalysts,i.e.Mg is an sueful structure promoter in this kind of catalysts.

  7. Sulfide Catalysts Supported on Porous Aromatic Frameworks for Naphthalene Hydroprocessing

    Directory of Open Access Journals (Sweden)

    Eduard Karakhanov

    2016-08-01

    Full Text Available This paper describes the first example of using porous aromatic frameworks as supports for sulfide catalysts for the hydrogenation of aromatic hydrocarbons. The synthesis of bimetallic Ni-W and Ni-Mo sulfides was performed by in situ decomposition of [(n-Bu4N]2[Ni(MeS42] (Me = W, Mo complexes, supported on mesoporous aromatic framework with a diamond-like structure. It is shown that the highest naphthalene conversions were achieved in the case of additional sulfidation with sulfur. After the reaction, catalysts were characterized by X-ray photoelectron spectroscopy and high-resolution transmission electron microscopy. The activity of synthesized catalysts has been studied using naphthalene as a model substrate. The materials used in this study were substantially active in hydrogenation and slightly in hydrocracking of naphthalene.

  8. Multiphase catalysts for selective reduction of NOx with hydrocarbons

    International Nuclear Information System (INIS)

    Among the existing proposed solutions to reduce emission of NOx there is a promising alternative, the so-called (HC-SCR) selective catalytic reduction of NOx using hydrocarbons as reductant. This thesis is part of a worldwide effort devoted to gain knowledge on the selective catalytic reduction of NOx with hydrocarbons with the final goal to contribute to the development of suitable catalysts for the above mentioned process. Chapter 2 describes the details of the experimental set-up and of the analytical methods employed. Among the catalyst for HC-SCR, Co-based catalyst are known to be active and selective, thus, a study on a series of Co-based catalysts, supported on zeolites, was undertaken and the results are presented in Chapter 3. Correlation between catalytic characteristics and kinetic results are employed to understand the working catalyst and this is used as a basis for catalyst optimization. With the intention to prepare a multi-functional catalyst that will preserve the desired characteristics of the individual components, minimizing their negative aspects, catalysts based on Co-Pt, supported on ZSM-5, were investigated. In Chapter 4 the results of this study are discussed. A bimetallic Co-Pt/ZSM-5 catalysts with low Pt contents (0.1 wt %) showed a synergistic effect by combining high stability and activity of Pt catalysts with the high N2 selectivity of Co catalysts. Furthermore, it was found to be sulfur- and water-tolerant. Its positive qualities brought us to study the mechanism that takes place over this catalyst during HC-SCR. The results of an in-situ i.r mechanistic study over this catalyst is reported in Chapter 5. From the results presented in Chapter 5 a mechanism operating over the Co-Pt/ZSM-5 catalyst is proposed. The modification of Co catalyst with Pt improved the catalysts. However, further improvement was found to be hindered by high selectivity to N2O. Since Rh catalysts are generally less selective to N2O, the modification of Co

  9. Characterization of the impregnated iron based catalyst for direct coal liquefaction by EXAFS

    Institute of Scientific and Technical Information of China (English)

    JianliYang; JishengZhun; 等

    2001-01-01

    Catalyst plays an important role in direct cola liquefaction(DCL)[1],Due to relatively high activity,low cost and environmentally benign for disposal,iron catalysts are regarded as the most attractive catalysts for DCL.To maximize catalytic effect and minimize catalyst usage,ultra-fine size catalysts are preferred.The most effective catalysts are found to be those impregnated onto coal because of their high dispersion on coal surface and intimate contact with coal particles.

  10. Titania Supported Pt and Pt/Pd Nano-particle Catalysts for the Oxidation of Sulfur Dioxide

    DEFF Research Database (Denmark)

    Koutsopoulos, Sotiris; Johannessen, Tue; Eriksen, Kim Michael;

    2006-01-01

    Several types of titania (anatase) were used as supports for pure platinum and Pt–Pd bimetallic alloy catalysts. The preparation methods, normal wet impregnation technique and flame aerosol synthesis, obtained metal loadings of 2% by weight. The prepared catalysts were tested for SO2 oxidation...... activity at atmospheric pressure in the temperature range 250–600 °C. The SO2 to SO3 conversion efficiency of the Pt–Pd alloy was significantly higher than that of the individual metals. The effects of the preparation method and the titania type used on the properties and activity of the resulting catalyst...

  11. PREPARATION OF NOVEL METALLIC AND BIMETALLIC CROSS-LINKED POLY (VINYL ALCOHOL) NANOCOMPOSITES UNDER MICROWAVE IRRADIATION

    Science.gov (United States)

    A facile method utilizing microwave irradiation is described that accomplishes the cross-linking reaction of PVA with metallic and bimetallic systems. Nanocomposites of PVA-cross-linked metallic systems such as Pt, Cu, and In and bimetallic systems such as Pt-In, Ag-Pt, Pt-Fe, Cu...

  12. NOVEL METALLIC AND BIMETALLIC CROSS-LINKED POLY (VINYL ALCOHOL) NANOCOMPOSITES PREPARED UNDER MICROWAVE IRRADIATION

    Science.gov (United States)

    A facile microwave irradiation approach that results in a cross-linking reaction of poly (vinyl alcohol) (PVA) with metallic and bimetallic systems is described. Nanocomposites of PVA cross-linked metallic systems such as Pt, Cu, and In and bimetallic systems such as Pt-In, Ag-P...

  13. Copper Based Bi-metallic Core Pin Using DMD: Industrial Evaluation

    Directory of Open Access Journals (Sweden)

    M. Khalid Imran

    2012-01-01

    Full Text Available Bi-metallic core pins were prepared and the performance was evaluated in a specially designed die that had the provision to investigate core pins under semi-industrial HPDC conditions. A comparison between bi-metallic core pin with that of tool steel revealed that bi-metallic core pin performed better in terms of soldering under HPDC environment. Due to slow cooling, die holding time needed to be increased in tool steel core pin to allow sufficient solidification of the casting part. The bi-metallic core pins also operated without any catastrophic failure in the clad which particularly substantiated the applicability of DMD deposited tool steel clad on copper alloy substrate to manufacture bi-metallic tooling.

  14. Formation of bimetallic nanoalloys by Au coating of size-selected Cu clusters

    International Nuclear Information System (INIS)

    Bimetallic clusters display new characteristics that could not be obtained by varying either the size of pure metallic systems or the composition of bulk bimetals alone. Coating of pre-deposited clusters by vapour deposition is a typical synthesis process of bimetallic clusters. Here, we have demonstrated that hierarchical, gold cluster-decorated copper clusters as well as both heterogeneous and homogeneous Cu–Au bimetallic clusters (4.6 to 10.7 nm) can be prepared by coating pre-deposited, size-selected Cu5000 (4.6 ± 0.2 nm) with Au evaporation at various temperatures. These bimetallic clusters were analyzed by aberration-corrected scanning transmission electron microscopy and associated electron energy loss spectroscopy. The results indicate that the growth of bimetallic clusters is controlled by a competition between nucleation and diffusion of the coating Au atoms.

  15. Cleave and capture chemistry illustrated through bimetallic-induced fragmentation of tetrahydrofuran

    Science.gov (United States)

    Mulvey, Robert E.; Blair, Victoria L.; Clegg, William; Kennedy, Alan R.; Klett, Jan; Russo, Luca

    2010-07-01

    The cleavage of ethers is commonly encountered in organometallic chemistry, although rarely studied in the context of new, emerging bimetallic reagents. Recently, it was reported that a bimetallic sodium-zinc base can deprotonate cyclic tetrahydrofuran under mild conditions without opening its heterocyclic (OC4) ring. In marked contrast to this synergic sedation, herein we show that switching to the more reactive sodium-magnesium or sodium-manganese bases promotes cleavage of at least six bonds in tetrahydrofuran, but uniquely the ring fragments are captured in separate crystalline complexes. Oxide fragments occupy guest positions in bimetallic, inverse crown ethers and C4 fragments ultimately appear in bimetallated butadiene molecules. These results demonstrate the special synergic reactivity that can be executed by bimetallic reagents, which include the ability to capture and control, and thereby study, reactive fragments from sensitive substrates.

  16. Preparation and Reactivity of Niobium-Containing Hydrotreating Catalysts

    OpenAIRE

    Schwartz, Viviane

    2000-01-01

    A series of niobium-containing nitride and carbides were prepared by a temperature-programmed synthesis method. The catalysts synthesized comprised a monometallic niobium oxynitride and a new bimetallic oxycarbide supported system, Nb-Mo-O-C/Al2O3 (Mo/Nb = 1.2; 1.6; 2.0).In the case of the niobium oxynitride, the progress of formation was analyzed by interrupting the synthesis at various stages. The effect of the heating rate on product properties was also investigated. The solid intermedi...

  17. Photocatalytic Degradation of DIPA Using Bimetallic Cu-Ni/TiO2 Photocatalyst under Visible Light Irradiation

    Directory of Open Access Journals (Sweden)

    Nadia Riaz

    2014-01-01

    Full Text Available Bimetallic Cu-Ni/TiO2 photocatalysts were synthesized using wet impregnation (WI method with TiO2 (Degussa-P25 as support and calcined at different temperatures (180, 200, and 300°C for the photodegradation of DIPA under visible light. The photocatalysts were characterized using TGA, FESEM, UV-Vis diffuse reflectance spectroscopy, fourier transform infrared spectroscopy (FTIR and temperature programmed reduction (TPR. The results from the photodegradation experiments revealed that the Cu-Ni/TiO2 photocatalysts exhibited much higher photocatalytic activities compared to bare TiO2. It was found that photocatalyst calcined at 200°C had the highest photocatalyst activities with highest chemical oxygen demand (COD removal (86.82%. According to the structural and surface analysis, the enhanced photocatalytic activity could be attributed to its strong absorption into the visible region and high metal dispersion.

  18. Synthesis and Characterization of Monometallic (Ag, Cu and Bimetallic Ag-Cu Particles for Antibacterial and Antifungal Applications

    Directory of Open Access Journals (Sweden)

    Marta Paszkiewicz

    2016-01-01

    Full Text Available In this paper, the experimental studies are concerned with the effect of the synthesis parameters on the formation of monometallic Ag and Cu nanoparticles (NPs. We consider the synthesis strategies verification for the bimetallic core-shell and alloy particles preparation. It was successfully obtained by chemical reduction method. The obtained colloidal solution is characterized by the transmission electron microscopy (TEM with energy-dispersive X-ray spectroscopy (EDX data, UV-Vis spectra, particle size distribution, and zeta potential. This work presents a comprehensive overview of experimental studies of the most stable colloidal solutions to impregnate fabrics that will exhibit a bactericidal and fungicidal activity against Candida albicans, Escherichia coli, and Staphylococcus aureus.

  19. Fabrication a new modified electrochemical sensor based on Au-Pd bimetallic nanoparticle decorated graphene for citalopram determination.

    Science.gov (United States)

    Daneshvar, Leili; Rounaghi, Gholam Hossein; Es'haghi, Zarrin; Chamsaz, Mahmoud; Tarahomi, Somayeh

    2016-12-01

    This paper proposes a simple approach for sensing of citalopram (CTL) using gold-palladium bimetallic nanoparticles (Au-PdNPs) decorated graphene modified gold electrode. Au-PdNPs were deposited at the surface of a graphene modified gold electrode with simple electrodeposition method. The morphology and the electrochemical properties of the modified electrode were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscopy (AFM), energy dispersion spectroscopy (EDS), electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and square wave voltammetry (SWV). The novel sensor exhibited an excellent catalytic activity towards the oxidation of CTL. The oxidation peak current of CTL, was linear in the range of 0.5-50μM with a detection limit 0.049μM with respect to concentration of citalopram. The proposed sensor was successfully applied for determination of CTL tablet and human plasma samples with satisfactory results. PMID:27612758

  20. Fabrication a new modified electrochemical sensor based on Au-Pd bimetallic nanoparticle decorated graphene for citalopram determination.

    Science.gov (United States)

    Daneshvar, Leili; Rounaghi, Gholam Hossein; Es'haghi, Zarrin; Chamsaz, Mahmoud; Tarahomi, Somayeh

    2016-12-01

    This paper proposes a simple approach for sensing of citalopram (CTL) using gold-palladium bimetallic nanoparticles (Au-PdNPs) decorated graphene modified gold electrode. Au-PdNPs were deposited at the surface of a graphene modified gold electrode with simple electrodeposition method. The morphology and the electrochemical properties of the modified electrode were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscopy (AFM), energy dispersion spectroscopy (EDS), electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and square wave voltammetry (SWV). The novel sensor exhibited an excellent catalytic activity towards the oxidation of CTL. The oxidation peak current of CTL, was linear in the range of 0.5-50μM with a detection limit 0.049μM with respect to concentration of citalopram. The proposed sensor was successfully applied for determination of CTL tablet and human plasma samples with satisfactory results.

  1. Alumina supported model Pd Ag catalysts: A combined STM, XPS, TPD and IRAS study

    Science.gov (United States)

    Khan, N. A.; Uhl, A.; Shaikhutdinov, S.; Freund, H.-J.

    2006-05-01

    The bimetallic Pd-Ag model catalysts were prepared by physical vapor deposition on thin alumina films. The morphology and structure of the Pd-Ag particles were studied by STM, XPS, and by TPD and IRAS of CO. The results showed the formation of true alloy particles with Ag segregated at the surface. The addition of Ag first suppresses the most strongly bonded CO on threefold hollow sites of Pd. With further increasing Ag coverage, only isolated Pd atoms surrounded by Ag atoms are likely present on the surface. The results on CO adsorption suggest that the model Pd-Ag system mimics the structure of the real Pd-Ag catalysts.

  2. Pt5Gd as a Highly Active and Stable Catalyst for Oxygen Electroreduction

    DEFF Research Database (Denmark)

    Escribano, Maria Escudero; Verdaguer-Casadevall, Arnau; Verdaguer Casadevall, Arnau;

    2012-01-01

    -fold increase in ORR activity, relative to pure Pt at 0.9 V, approaching the most active in the literature for catalysts prepared in this way. AR-XPS profiles after electrochemical measurements in 0.1 M HClO4 show the formation of a thick Pt overlayer on the bulk Pt5Gd, and the enhanced ORR activity...... can be explained by means of compressive strain effects. Furthermore, these novel bimetallic electrocatalysts are highly stable, which, in combination with their enhanced activity, makes them very promising for the development of new cathode catalysts for fuel cells....

  3. Photo-oxidation catalysts

    Science.gov (United States)

    Pitts, J. Roland; Liu, Ping; Smith, R. Davis

    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.

  4. Atomic Structure of Au−Pd Bimetallic Alloyed Nanoparticles

    KAUST Repository

    Ding, Yong

    2010-09-08

    Using a two-step seed-mediated growth method, we synthesized bimetallic nanoparticles (NPs) having a gold octahedron core and a palladium epitaxial shell with controlled Pd-shell thickness. The mismatch-release mechanism between the Au core and Pd shell of the NPs was systematically investigated by high-resolution transmission electron microscopy. In the NPs coated with a single atomic layer of Pd, the strain between the surface Pd layer and the Au core is released by Shockley partial dislocations (SPDs) accompanied by the formation of stacking faults. For NPs coated with more Pd (>2 nm), the stacking faults still exist, but no SPDs are found. This may be due to the diffusion of Au atoms into the Pd shell layers to eliminate the SPDs. At the same time, a long-range ordered L11 AuPd alloy phase has been identified in the interface area, supporting the assumption of the diffusion of Au into Pd to release the interface mismatch. With increasing numbers of Pd shell layers, the shape of the Au-Pd NP changes, step by step, from truncated-octahedral to cubic. After the bimetallic NPs were annealed at 523 K for 10 min, the SPDs at the surface of the NPs coated with a single atomic layer of Pd disappeared due to diffusion of the Au atoms into the surface layer, while the stacking faults and the L11 Au-Pd alloyed structure remained. When the annealing temperature was increased to 800 K, electron diffraction patterns and diffraction contrast images revealed that the NPs became a uniform Au-Pd alloy, and most of the stacking faults disappeared as a result of the annealing. Even so, some clues still support the existence of the L11 phase, which suggests that the L11 phase is a stable, long-range ordered structure in Au-Pd bimetallic NPs. © 2010 American Chemical Society.

  5. CATALYTIC BEHAVIOR OF SILICA-SUPPORTED POLY-γ-AMINOPROPYL-SILOXANE-Co-Ru BIMETALLIC COMPLEX FOR THE HYDROFORMYLATION OF CYCLOHEXENE

    Institute of Scientific and Technical Information of China (English)

    GUAN Shiyou; HUANG Meiyu; JIANG Yingyan

    1993-01-01

    The cobalt and ruthenium bimetallic complex of poly-γ-amino-propylsiloxane(abbr.as Si-CH2-Co-Ru) was prepared,and it was found that it can catalyze the hydroformylation of cyclohexene effectively with the conversion amounting to over 90%.Cyclohexanecarboxaldehyde was first formed in the hydrofor mylation,and then further hydrogenated to form cylcohexanemethanol.The coversion was affected obviously by the Co/Ru ratio.When Co/Ru molar ratio was 100-150,i.e.in the very low content of noble metal Ru,the catalytic activity of Si-NH2-Co-Ru was also very high.The product composition was affected by CO/H2 ratio in the reaction gas.Aldehyde can be got high selectively by controlling CO/H2 ratio.Compared with other catalyst system,the Si-NH2-Co-Ru catalyst has higher catalytic activity and efficiency with very low Ru/Co ratio.The total turnover number was more than 28,800(based on the amount of ruthenium used).

  6. Enhanced plasmonic behavior of bimetallic (Ag-Au multilayered spheres

    Directory of Open Access Journals (Sweden)

    Pal Umapada

    2011-01-01

    Full Text Available Abstract In this article we study the plasmonic behavior of some stable, highly biocompatible bimetallic metal-dielectric-metal (MDM and double concentric nanoshell (DCN structures. By simply switching the material of the inner structure from Au to Ag, the intensity of their surface plasmon resonance could be increased in the optical transparency region of the human tissues up to 20 and 60 percent for the MDM and DCN, respectively, while the biocompatibility is retained. The obtained results indicate that these novel structures could be highly suitable for surface enhanced Raman scattering and photothermal cancer therapy.

  7. 1D antiferromagnetism in spin‐alternating bimetallic chains

    OpenAIRE

    Coronado Miralles, Eugenio; Sapiña Navarro, Fernando; Drillon, M.; De Jongh, L.J.

    1990-01-01

    The magnetic and thermal properties of the ordered bimetallic chain CoNi(EDTA)⋅6H2O in the very low‐temperature range are reported. The magnetic behavior does not exhibit the characteristic features of 1D ferrimagnets, but a continuous decrease of χmT towards zero at absolute zero. This 1D antiferromagnetic behavior results from an accidental compensation between the moments located at the two sublattices. This behavior, as well as the specific‐heat results, are modeled on the basis of an Isi...

  8. Bimetallic Ag-Pd nanoparticles-decorated graphene oxide: a fascinating three-dimensional nanohybrid as an efficient electrochemical sensing platform for vanillin determination

    International Nuclear Information System (INIS)

    Highlights: • A 3D Ag-Pd/GO nanohybrid was fabricated via a green and in situ chemical route. • Ag-Pd/GO shows excellent electro-catalytic properties for the oxidation of vanillin. • The 3D hybrid-based sensor shows excellent performances for the vanillin detection. • This proposed method was successfully used to detect vanillin in children’s snacks. - Abstract: In this work, a fascinating hybrid based on Ag-Pd bimetallic nanoparticles-decorated graphene oxide (Ag-Pd/GO) has been successfully synthesized by a green and in situ chemical reduction strategy. The resultant hybrid was particularly characterized by scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, ultraviolet-visible spectroscopy and electrochemical techniques. The morphological results illustrate that Ag-Pd nanoparticles in microspheric appearances are highly dispersed and embedded on the GO layers, resulting in a rough surface and three-dimensional (3D) microstructure with a high Ag-Pd content in the matrix. The as-synthesized 3D Ag-Pd/GO hybrid displays distinctly enhanced electrocatalytic activity for the vanillin oxidation in comparison with that of the monometal-decorated GO, revealing a synergistic effect of the matrix GO and the doped bimetallic Ag-Pd. Therefore, the Ag-Pd/GO composite can be used as an enhanced electrochemical sensing platform for the sensitive determination of vanillin, and the fabricated sensor displays a wide detection range of 0.02–45 μmol dm−3, low detection limit of 5 nmol dm−3 and satisfactory recoveries between 98.8 % and 103.5 %. All the results demonstrate that the 3D hybrids integrated graphene with bimetallic nanoparticles are promising candidates for the development of high-performance electrochemical sensors

  9. Fe/Al bimetallic particles for the fast and highly efficient removal of Cr(VI) over a wide pH range: Performance and mechanism

    Energy Technology Data Exchange (ETDEWEB)

    Fu, Fenglian, E-mail: fufenglian2006@163.com [School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006 (China); Environmental Engineering and Science Program, Department of Biomedical, Chemical and Environmental Engineering (DBCEE), University of Cincinnati, OH 45221-0012 (United States); Cheng, Zihang [School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006 (China); Dionysiou, Dionysios D., E-mail: dionysios.d.dionysiou@uc.edu [Environmental Engineering and Science Program, Department of Biomedical, Chemical and Environmental Engineering (DBCEE), University of Cincinnati, OH 45221-0012 (United States); Tang, Bing [School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006 (China)

    2015-11-15

    Highlights: • Bimetallic particles with different Fe/Al mass ratios were prepared. • High removal rate of Cr(VI) was achieved in acidic, neutral, and alkaline pH. • No total iron ions at pH 3.0–11.0 and nearly no Al{sup 3+} at pH 3.0–7.0 were released. • Galvanic cell effect and high specific surface area contributed to Cr(VI) removal. - Abstract: The iron/aluminum (Fe/Al) bimetallic particles with high efficiency for the removal of Cr(VI) were prepared. Fe/Al bimetallic particles were characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), SEM mapping, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). SEM mapping showed that the core of bimetal was Al, and the planting Fe was deposited on the surface of Al. In acidic and neutral conditions, Fe/Al bimetal can completely remove Cr(VI) from wastewater in 20 min. Even at pH 11.0, the Cr(VI) removal efficiency achieved was 93.5%. Galvanic cell effect and high specific surface area are the main reasons for the enhanced removal of Cr(VI) by bimetallic particles. There were no iron ions released in solutions at pH values ranging from 3.0 to 11.0. The released Al{sup 3+} ions concentrations in acidic and neutral conditions were all less than 0.2 mg/L. The bimetal can be used 4 times without losing activity at initial pH 3.0. XPS indicated that the removed Cr(VI) was immobilized via the formation of Cr(III) hydroxide and Cr(III)–Fe(III) hydroxide/oxyhydroxide on the surface of Fe/Al bimetal. The Fe/Al bimetallic particles are promising for further testing for the rapid and effective removal of contaminants from water.

  10. Development of Novel Resid Hydrometallization Catalyst RDM-3

    Institute of Scientific and Technical Information of China (English)

    Hu Dawei; Niu Chuanfeng; Yang Qinghe; Liu Tao

    2007-01-01

    Based on the reaction mechanism of resid hydrodemetallization,a new catalyst carrier was designed and prepared.As compared with the similar type of catalyst carder,the said new carrier featured a higher pore volume,a larger pore diameter and a weaker surface acidity,which could improve the diffusion performance and stable reaction performance of the catalyst.The active metal components were loaded on the said carrier by a new technique for better metal dispersion,thus the impurity removal rate of the new catalyst,RDM-3,was improved significantly.The commercial test of the RDM-3 catalyst showed that the process of catalyst preparation was stable,the catalyst performance was slightly better than the catalyst prepared in the lab,therefore,the catalyst could be manufactured in commercial scale.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  12. Preparation of Dispersive Cobalt Naphthenate Catalyst and Its Application in Suspended-Bed Hydrocracking of Heavy Oil%分散型环烷酸钴催化剂的制备及其在重油悬浮床加氢裂化中的应用

    Institute of Scientific and Technical Information of China (English)

    李传; 尚猛; 邓文安; 阙国和

    2011-01-01

    采用皂化反应和复分解反应合成了适用于重油悬浮床加氧裂化反应的分散型环烷酸钴催化剂,并优化了合成条件;通过光学显微镜、激光粒度仪、XRD和SEM方法对硫化后的催化剂进行了表征;通过釜式反应评价了该催化剂在委内瑞拉380号燃料油悬浮床加氢裂化反应中的性能.实验结果表明,合成分散型环烷酸钴催化剂的优化条件为:在皂化反应中,NaOH质量分数15%,环烷酸与NaOH摩尔比1:0.995,皂化温度95℃,皂化时间3h;在复分解反应中,CoSO4溶液质量分数15%,以滴加方式加入CoSO4溶液,复分解反应温度90℃,复分解反应时间2h.该催化剂硫化后颗粒分散度较大,团聚不明显,表面粗糙,有较大的比表而积,主要以立方晶系Co9S8晶型存在,并对重油悬浮床加氢裂化反应有较好的抑焦效果.%A dispersive cobalt naphthenate catalyst which was used in suspended-bed hydrocracking of heavy oil was prepared through saponification and double-decomposition, and the catalyst after sulfurization was characterized by means of optical microscopy, laser scattering particle analyzer, XRD and SEM. The effect of the catalyst on the suspended-bed hydrocracking of Venezuela 380* fuel oil was studied in a autoclave. The results showed that the optimal preparation conditions for the dispersive cobalt naphthenate catalyst were mass content of NaOH 15% , mole ratio of naphthenic acid to NaOH1: 0.995, saponification temperature 95 t, saponification time 3 h, mass content of CoSO4 solution (distributive droplets) 15% , double-decomposition temperature 90 t and double-decomposition time2 h. The dispersive cobalt naphthenate catalyst after sulfurization had the advantages of high particle dispersion, slight particle aggregation, coarse surface and big specific surface area, and the catalyst particles mainly existed in the form of Co9S8 cubic crystal. And the catalyst showed a good ability of inhibiting coke formation.

  13. Physical and Numerical Analysis of Extrusion Process for Production of Bimetallic Tubes

    Energy Technology Data Exchange (ETDEWEB)

    Misiolek, W.Z.; Sikka, V.K.

    2006-08-10

    Bimetallic tubes are used for very specific applications where one of the two metals provides strength and the other provides specific properties such as aqueous corrosion and carburization, coking resistance, and special electrical and thermal properties. Bimetallic tubes have application in pulp and paper industry for heat-recovery boilers, in the chemical industry for ethylene production, and in the petrochemical industry for deep oil well explorations. Although bimetallic tubes have major applications in energy-intensive industry, they often are not used because of their cost and manufacturing sources in the United States. This project was intended to address both of these issues.

  14. 二苯并噻吩在分散型钼催化剂和原位产生的氢存在下的加氢脱硫Ⅲ.催化剂前身物、硫化氢、一氧化碳和水对反应的影响%HDS OF DBT USING in situ GENERATED HYDROGEN IN THE PRESENCE OF DISPERSED Mo CATALYSTS Ⅲ. Effects of Catalyst Precursors, H2S, CO and H2O

    Institute of Scientific and Technical Information of China (English)

    刘晨光; Flora T.T.Ng

    1999-01-01

    研究了水水/甲苯乳化液中二苯并噻吩(硫芴)在分散型钼酸、磷钼酸和四硫钼酸铵催化剂存在下的加氢脱硫反应.反应在高压釜中于340℃及三种不同的气氛即H2,H2/H2O和CO/H2O(CO和H2O经水煤气转换反应(WGSR)产生原位氢)的存在下进行.用GC和GC-MS鉴定、分析了气体和液体产物的组成.结果表明:对硫芴的加氢脱硫反应,在分散型四硫钼酸铵催化剂存在下,原位产生的氢的效果仅比加入的氢气稍好,而在分散型钼酸和磷钼酸催化剂存在下,原位产生的氢远比加入的氢气有效.实验结果还表明:硫化氢能显著提高分散型钼酸和磷钼酸催化剂的加氢脱硫活性,但在分散型四硫钼酸铵催化剂存在下,硫化氢能促进加氢反应而抑制氢解反应.一氧化碳和水均选择性地抑制氢解反应.%The hydrodesulfurization (HDS) of dibenzothiophene (DBT) was investigated using dispersed catalyst precursors molybdic acid (MA), phosphomolybdic acid (PMA), and ammonium tetrathiomolybdate (ATTM). The results indicated that with ATTM catalyst, in situ hydrogen was slightly more active than the externally supplied molecular H2 for HDS of DBT, but is not so active as with MA and PMA catalysts. The experimental results also indicated that H2S has a significant promotional effect on the catalytic activity of MA or PMA catalyst. While the H2 S promoted the hydrogenation pathway, inhibited the hydrogenolysis pathway with ATTM catalyst.Both CO and H2O selectively inhibited the hydrogenolysis route.

  15. Microwave-assisted synthesis and characterization of bimetallic PtRu alloy nanoparticles supported on carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Rahsepar, Mansour, E-mail: rahsepar@shirazu.ac.ir [Department of Materials Science and Engineering, School of Engineering, Shiraz University, Zand Boulevard, Shiraz, 7134851154 (Iran, Islamic Republic of); Kim, Hasuck, E-mail: hasuckim@snu.ac.kr [Department of Chemistry, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul, 151-747 (Korea, Republic of); Department of Energy Systems Engineering, Daegu Gyeongbuk Institute of Science & Technology, Daegu, 711-873 (Korea, Republic of)

    2015-11-15

    Multiwalled carbon nanotube (MWCNT) supported PtRu nanoparticles were synthesized by using a microwave-assisted improved impregnation technique. X-ray diffraction, transmission electron microscopy and X-ray photo electron spectroscopy were used to characterize the prepared PtRu/MWCNT nanoparticles. The PtRu nanoparticles with a satisfactory dispersion were formed on the external surface of MWCNTs. The CO stripping experiment was performed to evaluate the poisoning resistance of the prepared PtRu/MWCNT nanoparticles. Results of electrochemical measurements indicate that the prepared PtRu/MWCNTs shows an enhanced performance toward CO poisoning. The results of characterization revealed that microwave-assisted improved impregnation technique have a high yield of alloy phase formation and could be effectively used as a simple, quick and efficient technique for preparation of bimetallic PtRu/MWCNT nanoparticles. - Highlights: • Highly dispersed PtRu/MWCNTs were formed without use of any stabilizing agent. • Microwave irradiation enhances the uniform dispersion of the PtRu nanoparticles. • Microwave-assisted improved impregnation have a high yield of alloy phase formation. • The prepared PtRu/MWCNTs shows an enhanced performance toward CO poisoning.

  16. Catalyst composition

    Energy Technology Data Exchange (ETDEWEB)

    Onodera, T.; Sakai, T.; Sumitani, K.; Yamasaki, Y.

    1984-11-27

    A catalyst composition comprising a crystalline aluminosilicate selected from the group consisting of zeolite ZSM-5, zeolite ZSM-11, zeolite ZSM-12, zeolite ZSM-35 and zeolite ZSM-38 and having a silica/alumina mole ratio of 20 to 1,000; and at least two metals which are platinum and at least one other metal selected from the group consisting of titanium, chromium, zinc, gallium, germanium, strontium, yttrium, zirconium, molybdenum, palladium, tin, barium, cerium, tungsten, osmium, lead, cadmium, mercury, indium, lanthanum and beryllium. This catalyst composition is useful particularly for the isomerization of aromatic hydrocarbons and reforming of naphtha.

  17. Core-shell Au-Pd nanoparticles as cathode catalysts for microbial fuel cell applications

    Science.gov (United States)

    Yang, Gaixiu; Chen, Dong; Lv, Pengmei; Kong, Xiaoying; Sun, Yongming; Wang, Zhongming; Yuan, Zhenhong; Liu, Hui; Yang, Jun

    2016-01-01

    Bimetallic nanoparticles with core-shell structures usually display enhanced catalytic properties due to the lattice strain created between the core and shell regions. In this study, we demonstrate the application of bimetallic Au-Pd nanoparticles with an Au core and a thin Pd shell as cathode catalysts in microbial fuel cells, which represent a promising technology for wastewater treatment, while directly generating electrical energy. In specific, in comparison with the hollow structured Pt nanoparticles, a benchmark for the electrocatalysis, the bimetallic core-shell Au-Pd nanoparticles are found to have superior activity and stability for oxygen reduction reaction in a neutral condition due to the strong electronic interaction and lattice strain effect between the Au core and the Pd shell domains. The maximum power density generated in a membraneless single-chamber microbial fuel cell running on wastewater with core-shell Au-Pd as cathode catalysts is ca. 16.0 W m−3 and remains stable over 150 days, clearly illustrating the potential of core-shell nanostructures in the applications of microbial fuel cells. PMID:27734945

  18. Core-shell Au-Pd nanoparticles as cathode catalysts for microbial fuel cell applications

    Science.gov (United States)

    Yang, Gaixiu; Chen, Dong; Lv, Pengmei; Kong, Xiaoying; Sun, Yongming; Wang, Zhongming; Yuan, Zhenhong; Liu, Hui; Yang, Jun

    2016-10-01

    Bimetallic nanoparticles with core-shell structures usually display enhanced catalytic properties due to the lattice strain created between the core and shell regions. In this study, we demonstrate the application of bimetallic Au-Pd nanoparticles with an Au core and a thin Pd shell as cathode catalysts in microbial fuel cells, which represent a promising technology for wastewater treatment, while directly generating electrical energy. In specific, in comparison with the hollow structured Pt nanoparticles, a benchmark for the electrocatalysis, the bimetallic core-shell Au-Pd nanoparticles are found to have superior activity and stability for oxygen reduction reaction in a neutral condition due to the strong electronic interaction and lattice strain effect between the Au core and the Pd shell domains. The maximum power density generated in a membraneless single-chamber microbial fuel cell running on wastewater with core-shell Au-Pd as cathode catalysts is ca. 16.0 W m‑3 and remains stable over 150 days, clearly illustrating the potential of core-shell nanostructures in the applications of microbial fuel cells.

  19. Copper Modified Magnetic Bimetallic Nano-catalysts Ligand Regulated Catalytic Activity

    Science.gov (United States)

    Postsynthetic modification of magnetic nano ferrites (Fe3O4) has been accomplished by anchoring glutathione and dopamine on the surface. The Cu nano particles immobilized over these surfaces were investigated for the coupling and cyclo addition reactions. The Fe3O4-DOPA-Cu (na...

  20. Balance of Nanostructure and Bimetallic Interactions in Pt Model Fuel Cell Catalysts

    DEFF Research Database (Denmark)

    Friebel, Daniel; Viswanathan, Venkatasubramanian; Miller, Daniel J.;

    2012-01-01

    We have studied the effect of nanostructuring in Pt monolayer model electrocatalysts on a Rh(111) single-crystal substrate on the adsorption strength of chemisorbed species. In situ high energy resolution fluorescence detection X-ray absorption spectroscopy at the Pt L3 edge reveals characteristi...

  1. How to Determine the Core-Shell Nature in Bimetallic Catalyst Particles?

    NARCIS (Netherlands)

    Westsson, E.E.; Koper, G.J.M.

    2014-01-01

    Nanometer-sized materials have significantly different chemical and physical properties compared to bulk material. However, these properties do not only depend on the elemental composition but also on the structure, shape, size and arrangement. Hence, it is not only of great importance to develop sy

  2. Characterization of platinum–iron catalysts supported on MCM-41 synthesized with rice husk silica and their performance for phenol hydroxylation

    OpenAIRE

    Jitlada Chumee, Nurak Grisdanurak, Arthit Neramittagapong and Jatuporn Wittayakun

    2009-01-01

    Mesoporous material RH-MCM-41 was synthesized with rice husk silica by a hydrothermal method. It was used as a support for bimetallic platinum−iron catalysts Pt–Fe/RH-MCM-41 for phenol hydroxylation. The catalysts were prepared by co-impregnation with Pt and Fe at amounts of 0.5 and 5.0 wt.%, respectively. The RH-MCM-41 structure in the catalysts was studied with x-ray diffraction, and their surface areas were determined by nitrogen adsorption. The oxidation number of Fe supported on RH-MCM-4...

  3. Surface organometallic chemistry on metals. III. Formation of a bimetallic Ni-Sn phase generated by reaction of a Sn(n-C sub 4 H sub 9 ) sub 4 and silica-supported nickel oxide

    Energy Technology Data Exchange (ETDEWEB)

    Agnelli, M.; Candy, J.P.; Basset, J.M. (l' Universite Claude Bernard, Villeurbanne (France)); Bournonville, J.P.; Ferretti, O.A. (Institut Francais du Petrole, Rueil-Malmaison (France))

    1990-02-01

    Reaction of Sn(n-C{sub 4}H{sub 9}){sub 4} with NiO/SiO{sub 2} occurs above 423 K according to the apparent following stoichiometry: NiO + xSn(n-C{sub 4}H{sub 9}){sub 4} {yields} NiSn{sub x} + (2x + 1)C{sub 4}H{sub 8} + (2x {minus} 1)C{sub 4}H{sub 10} + H{sub 2}O. Various compositions of the bimetallic phase can be achieved by changing the initial Sn/Ni ratio. The obtained catalysts were very active and selective in the hydrogenation of ethyl acetate to ethanol. Characterization of the bimetallic phase has shown that the particles are bimetallic (STEM). As a result of chemisorption IR, and magnetic measurements, it appears that the presence of tin has four effects: (i) it decreases significantly the amount of CO and H{sub 2} adsorbed; (ii) it isolates nickel atoms from their neighbors; (iii) it increases electron density on nickel; and (IV) it suppresses the magnetic properties of nickel. Redox behavior of Ni-Sn/SiO{sub 2} toward surface OH indicates that surface hydroxyls can oxidize Sn{sup (0)}, probably to Sn{sup (II)} with evolution of H{sub 2}, the process being reversible with H{sub 2}. It is suggested that during this oxidation process, tin migrates to the periphery of the bimetallic particle with formation of (chemical bond Si-O){sub 2}Sn{sup (II)} surface species.

  4. Clean Catalysts for Water Recovery Systems in Long-Duration Missions Project

    Data.gov (United States)

    National Aeronautics and Space Administration — Oxidation catalysts based on innovative, physically-robust activated carbon materials containing dispersed noble metals are essential in process optimization for...

  5. Analysis of Al-Cu Bimetallic Bars Properties After Explosive Welding and Rolling in Modified Passes

    Directory of Open Access Journals (Sweden)

    Mróz S.

    2015-04-01

    Full Text Available The paper presents the results of the experimental tests of Al-Cu bimetallic bars rolling process in multi-radial modified passes. The bimetallic bars consist of aluminium core, grade 1050A and copper outer layer, grade M1E. The stocks were round bars with diameter 22 mm with a copper layer share of 15 and 30%. As a result of rolling in four passes, bars of a diameter of about 16.0 mm were obtained. A bimetallic stock was manufactured using an explosive welding method. The use of the designed arrangement of multi-radial modified stretching passes resulted in obtaining Al-Cu bimetallic bars with the required lateral dimensions, an uniform distribution of the cladding layer over the bar perimeter and high quality of shear strength between individual layers.

  6. Microbially supported synthesis of catalytically active bimetallic Pd-Au nanoparticles

    DEFF Research Database (Denmark)

    Hosseinkhani, Baharak; Søbjerg, Lina Sveidal; Rotaru, Amelia-Elena;

    2012-01-01

    Bimetallic nanoparticles are considered the next generation of nanocatalysts with increased stability and catalytic activity. Bio-supported synthesis of monometallic nanoparticles has been proposed as an environmentally friendly alternative to the conventional chemical and physical protocols. In ...

  7. Nonchromophoric halide ligand variation in polyazine-bridged Ru(II),Rh(III) bimetallic supramolecules offering new insight into photocatalytic hydrogen production from water.

    Science.gov (United States)

    Rogers, Hannah Mallalieu; White, Travis A; Stone, Brittany N; Arachchige, Shamindri M; Brewer, Karen J

    2015-04-01

    The new bimetallic complex [(Ph2phen)2Ru(dpp)RhBr2(Ph2phen)](PF6)3 (1) (Ph2phen = 4,7-diphenyl-1,10-phenanthroline; dpp = 2,3-bis(2-pyridyl)pyrazine) was synthesized and characterized to compare with the Cl(-) analogue [(Ph2phen)2Ru(dpp)RhCl2(Ph2phen)](PF6)3 (2) in an effort to better understand the role of halide coordination at the Rh metal center in solar H2 production schemes. Electrochemical properties of complex 1 display a reversible Ru(II/III) oxidation, and cathodic scans indicate multiple electrochemical mechanisms exist to reduce Rh(III) by two electrons to Rh(I) followed by a quasi-reversible dpp(0/-) ligand reduction. The weaker σ-donating ability of Br(-) vs Cl(-) impacts the cathodic electrochemistry and provides insight into photocatalytic function by these bimetallic supramolecules. Complexes 1 and 2 exhibit identical light-absorbing properties with UV absorption dominated by intraligand (IL) π → π* transitions and visible absorption by metal-to-ligand charge transfer (MLCT) transitions to include a lowest energy Ru(dπ) → dpp(π*) (1)MLCT transition (λ(abs) = 514 nm; ε = 16 000 M(-1) cm(-1)). The relatively short-lived, weakly emissive Ru(dπ) → dpp(π*) (3)MLCT excited state (τ = 46 ns) for both bimetallic complexes is attributed to intramolecular electron transfer from the (3)MLCT excited state to populate a low-energy Ru(dπ) → Rh(dσ*) triplet metal-to-metal charge transfer ((3)MMCT) excited state that allows photoinitiated electron collection. Complex 1 outperforms the related Cl(-) bimetallic analogue 2 as a H2 photocatalyst despite identical light-absorbing and excited-state properties. Additional H2 experiments with added halide suggest ion pairing plays a role in catalyst deactivation and provides new insight into observed differences in H2 production upon halide variation in Ru(II),Rh(III) supramolecular architectures. PMID:25782053

  8. Levelling the playing field: screening for synergistic effects in coalesced bimetallic nanoparticles

    Science.gov (United States)

    Tan, Rachel Lee Siew; Song, Xiaohui; Chen, Bo; Chong, Wen Han; Fang, Yin; Zhang, Hua; Wei, Jun; Chen, Hongyu

    2016-02-01

    Depending on the synthetic methods, bimetallic nanoparticles can have either core-shell, phase segregated, alloy, or partially coalesced structures, presenting different degrees of atomic mixing on their surface. Along with the variations of size and morphology, the structural differences make it difficult to compare the catalytic activity of bimetallic nanoparticles. In this article, we developed a facile screening method that can focus on the synergistic effects rather than structural differences. Prefabricated nanoparticles are mixed together to form linear aggregates and coalesced to form bimetallic junctions. Their hollow silica shells allow materials transport but prevent further aggregation. With a level playing field, this screening platform can identify the best bimetallic combination for a catalytic reaction, before optimizing the synthesis. This approach is more advantageous than the conventional approaches where structural difference may have dominant effects on the catalytic performance.Depending on the synthetic methods, bimetallic nanoparticles can have either core-shell, phase segregated, alloy, or partially coalesced structures, presenting different degrees of atomic mixing on their surface. Along with the variations of size and morphology, the structural differences make it difficult to compare the catalytic activity of bimetallic nanoparticles. In this article, we developed a facile screening method that can focus on the synergistic effects rather than structural differences. Prefabricated nanoparticles are mixed together to form linear aggregates and coalesced to form bimetallic junctions. Their hollow silica shells allow materials transport but prevent further aggregation. With a level playing field, this screening platform can identify the best bimetallic combination for a catalytic reaction, before optimizing the synthesis. This approach is more advantageous than the conventional approaches where structural difference may have dominant

  9. Studies of Heterogeneous Catalyst Selectivity and Stability for Biorefining Applications

    Science.gov (United States)

    O'Neill, Brandon J.

    The conversion of raw resources into value-added end products has long underlain the importance of catalysts in economic and scientific development. In particular, the development of selective and stable heterogeneous catalysts is a challenge that continues to grow in importance as environmental, sociological, and economic concerns have motivated an interest in sustainability and the use of renewable raw materials. Within this context, biomass has been identified as the only realistic source of renewable carbon for the foreseeable future. The development of processes to utilize biomass feedstocks will require breakthroughs in fundamental understanding and practical solutions to the challenges related to selectivity and stability of the catalysts employed. Selectivity is addressed on multiple fronts. First, the selectivity for C-O bond scission reactions of a bifunctional, bimetallic RhRe/C catalyst is investigated. Using multiple techniques, the origin of Bronsted acidity in the catalyst and the role of pretreatment on the activity, selectivity, and stability are explored. In addition, reaction kinetics experiments and kinetic modeling are utilized to understand the role of chemical functional group (i.e. carboxylic acid versus formate ester) in determining the decarbonylation versus decarboxylation selectivity over a Pd/C catalyst. Finally, kinetic studies over Pd/C and Cu/gamma-Al2O3 were performed so that that may be paired with density functional theory calculations and microkinetic modeling to elucidate the elementary reaction mechanism, identify the active site, and provide a basis for future rational catalyst design. Next, the issue of catalyst stability, important in the high-temperature, liquid-phase conditions of biomass processing, is examined, and a method for stabilizing the base-metal nanoparticles of a Cu/gamma-Al2O 3 catalyst using atomic layer deposition (ALD) is developed. This advancement may facilitate the development of biorefining by enabling

  10. Gas-Phase Growth of Heterostructures of Carbon Nanotubes and Bimetallic Nanowires

    Directory of Open Access Journals (Sweden)

    Whi Dong Kim

    2011-01-01

    Full Text Available A simple, inexpensive, and viable method for growing multiple heterostructured carbon nanotubes (CNTs over the entire surface of Ni-Al bimetallic nanowires (NWs in the gas phase was developed. Polymer-templated bimetallic nitrate NWs were produced by electrospinning in the first step, and subsequent calcination resulted in the formation of bimetallic oxide NWs by thermal decomposition. In the second step, free-floating bimetallic NWs were produced by spray pyrolysis in an environment containing hydrogen gas as a reducing gas. These NWs were continuously introduced into a thermal CVD reactor in order to grow CNTs in the gas phase. Scanning electron microscopy (SEM, transmission electron microscopy (TEM, and Raman spectrometry analyses revealed that the catalytic Ni sites exposed in the non-catalytic Al matrix over the entire surface of the bimetallic NWs were seeded to radially grow highly graphitized CNTs, which resembled “foxtail” structures. The grown CNTs were found to have a relatively uniform diameter of approximately 10±2 nm and 10 to 15 walls with a hollow core. The average length of the gas-phase-grown CNTs can be controlled between 100 and 1000 nm by adjusting the residence time of the free-floating bimetallic NWs in the thermal CVD reactor.

  11. Session 4: Low-temperature CO oxidation on Ni-Pt/SiO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Arenas-Alatorre, J.; Gomez-Cortes, A.; Diaz, G. [Instituto de Fisica UNAM, Mexico, D.F. (Mexico); Avalos Borja, M [Centro de Cciencias de la Materia Condensada, Ensenada, B.C. (Mexico)

    2004-07-01

    In the present study a set of Ni-Pt catalysts supported on silica have been examined as catalysts for the CO oxidation in the presence of hydrogen. The obtained results show that bimetallic Ni{sub 25}Pt{sub 75} catalyst is very active; total conversion of CO is achieved at 70 C and no significant diminution is observed at higher temperatures. Hydrogen concentration in the gas phase did not changed significantly indicating a very good selectivity towards CO oxidation. Bimetallic Ni{sub 50}Pt{sub 50} and Ni{sub 75}Pt{sub 25} catalysts showed also a good activity but the selectivity for CO oxidation decreases in favor of hydrogen oxidation at higher temperatures. It is interesting to note the performance of mono-metallic Ni/SiO{sub 2} since nickel is known to be not very active for oxidation reactions; at 120 C more than 80% of the CO is converted. On the other hand, Pt/SiO{sub 2} performance is not so good in comparison. (authors)

  12. Selective catalytic reduction of nitric oxide by ethylene over metal-modified ZSM-5- and {gamma}-Al{sub 2}O{sub 3}-catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Eraenen, K.; Kumar, N.; Lindfors, L.E. [Aabo Akademi, Turku (Finland). Lab. of Industrial Chemistry

    1996-12-31

    Metal-modified ZSM-5 and {gamma}-Al{sub 2}O{sub 3} catalysts were tested in reduction of nitric oxide by ethylene. Different metals were introduced into the ZSM-5 catalyst by ion-exchange and by introduction of metals during the zeolite synthesis. To prepare bimetallic catalysts a combination of these methods was used. The {gamma}-Al{sub 2}O{sub 3} was impregnated with different metals by the incipient wetness technique and by adsorption. Activity measurements showed that the ZSM-5 based catalysts were more active than the {gamma}-Al{sub 2}O{sub 3} based catalysts. The highest conversion was obtained over a ZSM-5 catalyst prepared by introduction of Pd during synthesis of the zeolite and subsequently ion-exchanged with copper. (author)

  13. Towards the Rational Design of Nanoparticle Catalysts

    Science.gov (United States)

    Dash, Priyabrat

    This research is focused on development of routes towards the rational design of nanoparticle catalysts. Primarily, it is focused on two main projects; (1) the use of imidazolium-based ionic liquids (ILs) as greener media for the design of quasi-homogeneous nanoparticle catalysts and (2) the rational design of heterogeneous-supported nanoparticle catalysts from structured nanoparticle precursors. Each project has different studies associated with the main objective of the design of nanoparticle catalysts. In the first project, imidazolium-based ionic liquids have been used for the synthesis of nanoparticle catalysts. In particular, studies on recyclability, reuse, mode-of-stability, and long-term stability of these ionic-liquid supported nanoparticle catalysts have been done; all of which are important factors in determining the overall "greenness" of such synthetic routes. Three papers have been published/submitted for this project. In the first publication, highly stable polymer-stabilized Au, Pd and bimetallic Au-Pd nanoparticle catalysts have been synthesized in imidazolium-based 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM]PF6) ionic liquid (Journal of Molecular Catalysis A: Chemical, 2008, 286, 114). The resulting nanoparticles were found to be effective and selective quasi-homogeneous catalysts towards a wide-range of hydrogenation reactions and the catalyst solution was reused for further catalytic reactions with minimal loss in activity. The synthesis of very pure and clean ILs has allowed a platform to study the effects of impurities in the imidazolium ILs on nanoparticle stability. In a later study, a new mode of stabilization was postulated where the presence of low amounts of 1-methylimidazole has substantial effects on the resulting stability of Au and Pd-Au nanoparticles in these ILs (Chemical Communications, 2009, 812). In further continuation of this study, a comparative study involving four stabilization protocols for nanoparticle

  14. EXAFS Determination of the Change in the Structure of Rhodium in Highly Dispersed Rhodium/gamma-Aluminum Oxide Catalysts after Carbon Monoxide and/or Hydrogen Adsorption at Different Temperatures

    NARCIS (Netherlands)

    Koningsberger, D.C.; Blik, H.F.J. van 't; Zon, J.B.A.D. van; Prins, R.

    1984-01-01

    Extended X-ray absorption spectroscopy (EXAFS) has been applied to study the Rh K-edge of two ultradisperse Rh/Al{2}O{3} catalysts containing 0.47 and 1.04 wt.% rhodium respectively. The structural properties of the Rh crystallites were determined after reduction with H{2}, evacuation at elevated te

  15. New catalysts for coal processing: Metal carbides and nitrides

    Energy Technology Data Exchange (ETDEWEB)

    S. Ted Oyama; David F. Cox

    1999-12-03

    The subject of this research project was to investigate the catalytic properties of a new class of materials, transition metal carbides and nitrides, for treatment of coal liquid and petroleum feedstocks. The main objectives were: (1) preparation of catalysts in unsupported and supported form; (2) characterization of the materials; (3) evaluation of their catalytic properties in HDS and HDN; (4) measurement of the surface properties; and (5) observation of adsorbed species. All of the objectives were substantially carried out and the results will be described in detail below. The catalysts were transition metal carbides and nitrides spanning Groups 4--6 in the Periodic Table. They were chosen for study because initial work had shown they were promising materials for hydrotreating. The basic strategy was first to prepare the materials in unsupported form to identify the most promising catalyst, and then to synthesize a supported form of the material. Already work had been carried out on the synthesis of the Group VI compounds Mo{sub 2}C, Mo{sub 2}N, and WC, and new methods were developed for the Group V compounds VC and NbC. All the catalysts were then evaluated in a hydrotreating test at realistic conditions. It was found that the most active catalyst was Mo{sub 2}C, and further investigations of the material were carried out in supported form. A new technique was employed for the study of the bulk and surface properties of the catalysts, near edge x-ray absorption spectroscopy (NEXAFS), that fingerprinted the electronic structure of the materials. Finally, two new research direction were explored. Bimetallic alloys formed between two transition metals were prepared, resulting in catalysts having even higher activity than Mo{sub 2}C. The performance of the catalysts in hydrodechloration was also investigated.

  16. Reduced graphene oxide nanosheets decorated with Au-Pd bimetallic alloy nanoparticles towards efficient photocatalytic degradation of phenolic compounds in water

    Science.gov (United States)

    Darabdhara, Gitashree; Boruah, Purna K.; Borthakur, Priyakshree; Hussain, Najrul; Das, Manash R.; Ahamad, Tansir; Alshehri, Saad M.; Malgras, Victor; Wu, Kevin C.-W.; Yamauchi, Yusuke

    2016-04-01

    Reduced graphene oxide nanosheets decorated with Au-Pd bimetallic alloy nanoparticles are successfully prepared via a chemical approach consisting of reducing the metal precursors using ascorbic acid as reductant at an elevated temperature. The prepared nanocomposite is employed as a photocatalyst for the degradation of organic contaminants such as phenol, 2-chlorophenol (2-CP), and 2-nitrophenol (2-NP). The complete degradation of phenol is achieved after 300 min under natural sunlight irradiation whereas the degradation of 2-CP and 2-NP is completed after 180 min. The activity of the photocatalyst is evaluated considering several parameters such as the initial phenol concentration, the photocatalyst loading, and the pH of the solution. The degradation kinetics of all the compounds is carefully studied and found to follow a linear Langmuir-Hinshelwood model. Furthermore, the reusability of the photocatalyst is successfully achieved up to five cycles and the catalyst exhibits an excellent stability.Reduced graphene oxide nanosheets decorated with Au-Pd bimetallic alloy nanoparticles are successfully prepared via a chemical approach consisting of reducing the metal precursors using ascorbic acid as reductant at an elevated temperature. The prepared nanocomposite is employed as a photocatalyst for the degradation of organic contaminants such as phenol, 2-chlorophenol (2-CP), and 2-nitrophenol (2-NP). The complete degradation of phenol is achieved after 300 min under natural sunlight irradiation whereas the degradation of 2-CP and 2-NP is completed after 180 min. The activity of the photocatalyst is evaluated considering several parameters such as the initial phenol concentration, the photocatalyst loading, and the pH of the solution. The degradation kinetics of all the compounds is carefully studied and found to follow a linear Langmuir-Hinshelwood model. Furthermore, the reusability of the photocatalyst is successfully achieved up to five cycles and the catalyst

  17. The role of Pt and Pd in enhancing the conversion of sorbitol to hydrogen over supported Ni-Pt and Ni-Pd catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Tanksale, A.; Lu, G.Q. [Queensland Univ., Brisbane (Australia); Beltramini, J.N. [Queensland Univ., Brisbane (Australia). ARC Centre of Excellence for Functional Nanomaterials

    2009-07-01

    This study investigated the enhanced activity of bimetallic nickel-platinum (Ni-Pt) and nickel-palladium (Ni-Pd) catalysts for the production of hydrogen from reformed biomass-based products. The catalysts were prepared on an aluminum oxide (Al203) nanofibre. Mesoporous zirconia and composite silica-zirconia-ceria were used to determine the role of noble metals and supports. Desorption, oxidation, and temperature programmed reduction studies were conducted to investigate metal-metal and metal-support interactions. The study showed that Pt and Pd additions increased the reducibility of Ni catalysts. The bimetallic catalysts exhibited rates of hydrogen production 6 times higher than rates observed in pure metal catalysts. Sorbitol conversion increased from 35 per cent for the Ni catalyst to 62 per cent for the Ni-Pt catalyst. It was concluded that the alloying effect of the Ni-Pt and Ni-Pd systems lowered the carbon monoxide (CO) adsorption heat, and facilitated removal of the adsorbed CO by the water gas shift reaction.

  18. Catalyst Architecture

    DEFF Research Database (Denmark)

    Kiib, Hans; Marling, Gitte; Hansen, Peter Mandal

    2014-01-01

    How can architecture promote the enriching experiences of the tolerant, the democratic, and the learning city - a city worth living in, worth supporting and worth investing in? Catalyst Architecture comprises architectural projects, which, by virtue of their location, context and their combinatio...... meaningful for everyone. The exhibited works are designed by SANAA, Diller Scofidio + Renfro, James Corner Field Operation, JBMC Arquitetura e Urbanismo, Atelier Bow-Wow, Ateliers Jean Nouvel, COBE, Transform, BIG, Topotek1, Superflex, and by visual artist Jane Maria Petersen....

  19. EFFECT OF CONCENTRATION METAL PRECURSOR Co AND Mo ON CHARACTER OF CoMo / USY CATALYST

    Directory of Open Access Journals (Sweden)

    Khoirina Dwi Nugrahaningtyas

    2016-08-01

    Full Text Available The preparation and characterization of bimetallic catalysts using impregnation method with a variation of concentration of precursor sequence Co and Mo metal obtained catalyst K 1 [Co (0.018 M - Mo (0.037 M/USY]. K 2 [Co (0.026 M - Mo (0.055 M/USY], K 3 [Co (0.035 M - Mo (0.074 M/USY], K 4 [Co (0.05 M - Mo (0.11 M /USY] and K 5 [Co (0.107 M - Mo (0.22 M/USY]. Character of the catalyst in terms of crystallinity was analyzed by XRD. The result shows that there is no cristalinity damage of USY after impregnation but the amorphous cristalin structure was obtained. Amount of metal content was analyzed by XRF and the catalyst morphology by SEM-EDS. The result shows that the higher the concentration of Co and Mo so that find the higher content of metal in catalyst of the prepared catalyst increase. K 4 shows the best characteristic of catalysts prepared in this research. Analysis of K 4 is proving that Co and Mo are presented in catalyst.

  20. DNA-templated synthesis of PtAu bimetallic nanoparticle/graphene nanocomposites and their application in glucose biosensor

    Science.gov (United States)

    Leng, Jing; Wang, Wen-Min; Lu, Li-Min; Bai, Ling; Qiu, Xin-Lan

    2014-02-01

    In this paper, single-stranded DNA (ss-DNA) is demonstrated to functionalize graphene (GR) and to further guide the growth of PtAu bimetallic nanoparticles (PtAuNPs) on GR with high densities and dispersion. The obtained nanocomposites (PtAuNPs/ss-DNA/GR) were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectrometer (EDS), and electrochemical techniques. Then, an enzyme nanoassembly was prepared by self-assembling glucose oxidase (GOD) on PtAuNP/ss-DNA/GR nanocomposites (GOD/PtAuNPs/ss-DNA/GR). The nanocomposites provided a suitable microenvironment for GOD to retain its biological activity. The direct and reversible electron transfer process between the active site of GOD and the modified electrode was realized without any extra electron mediator. Thus, the prepared GOD/PtAuNP/ss-DNA/GR electrode was proposed as a biosensor for the quantification of glucose. The effects of pH, applied potential, and temperature on the performance of the biosensor were discussed in detail and were optimized. Under optimal conditions, the biosensor showed a linearity with glucose concentration in the range of 1.0 to 1,800 μM with a detection limit of 0.3 μM (S/N = 3). The results demonstrate that the developed approach provides a promising strategy to improve the sensitivity and enzyme activity of electrochemical biosensors.

  1. Nickel/ruthenium catalyst and method for aqueous phase reactions

    Science.gov (United States)

    Elliott, Douglas C.; Sealock, John L.

    1998-01-01

    A method of hydrogenation using 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 ruthenium metal deposited onto the support in a second dispersed phase. The additional ruthenium metal is effective in retarding or reducing agglomeration or sintering of the nickel metal catalytic phase thereby increasing the life time of the catalyst during hydrogenation reactions.

  2. Characterization of bimetallic Fe/Pd nanoparticles by grape leaf aqueous extract and identification of active biomolecules involved in the synthesis.

    Science.gov (United States)

    Luo, Fang; Yang, Die; Chen, Zuliang; Megharaj, Mallavarapu; Naidu, Ravi

    2016-08-15

    This paper reports the detailed composition and morphology of one-step green synthesized bimetallic Fe/Pd nanoparticles (NPs) using grape leaf aqueous extract and identification of active biomolecules involved in the synthesis employing various techniques. Transmission Electron Microscopy (TEM) and Scanning Electron Microscopy (SEM) revealed that Fe/Pd NPs were polydispersed and quasi-spherical with a diameter ranging from 2 to 20nm. X-ray Photoelectron Spectroscopy (XPS) and Energy Dispersive X-ray Spectroscopy (EDS) provided evidence for the composition of Fe and Pd and for their species existing on the surface of Fe/Pd NPs. In addition, biomolecules in the grape leaf aqueous extract were identified but their functions are still unclear. Biomolecules in the aqueous extract such as methoxy-phenyl-oxime, N-benzoyl-2-cyano-histamine, 2-ethyl-phenol, 1,2-benzenediol, β-hydroxyquebracamine, hydroquinone, 2-methoxy-4-vinylphenol, 5-methyl-2-furancarboxaldehyde, 4-(3-hydroxybutyl)-3,5,5-trimethyl-2-cyclohexen and some polyphenolic compounds were identified as reducing and capping agents, which were studied by Chromatography-Mass Spectroscopy (GC-MS), XPS and Fourier Transform Infrared Spectroscopy (FTIR). Our finding suggests a new insight into cost-effective, simple, and environmentally benign production of bimetallic Fe/Pd NPs. PMID:27110966

  3. Green-chemistry Compatible Approach to TiO2-supported PdAu Bimetallic Nanoparticles for Solvent-free 1-Phenylethanol Oxidation under Mild Conditions

    Institute of Scientific and Technical Information of China (English)

    Jian-Bing Chang; Chang-Hai Liu; Jie Liu; Yu-Yan Zhou; Xu Gao; Sui-Dong Wang

    2015-01-01

    TiO2-supported PdAu bimetallic nanoparticles (NPs) with small size and good dispersity were prepared by the room-temperature ionic liquid-assisted bimetal sputtering, which is simple, environmentally friendly, and free of additives and byproducts. Pd/Au atomic ratio can be tuned by controlling the sputtering conditions simply. High catalytic activity was found in PdAu–NPs–TiO2 hybrids for solvent-free selective oxidation of 1-phenylethanol using O2 as the oxidant at the low temperature of 50 °C and low pressure of 1 atm. It was found that Pd/Au ratio strongly affected the catalytical activity, and the highest conversion of about 35%and turnover frequency of about 421 h-1 were achieved at 1:1 of Pd/Au atomic ratio. The synergistic effect in PdAu NPs was also discussed based on the comprehensive characterization results. The present approach may offer an alternative platform for future development of green-chemistry compatible bimetallic nanocatalysts.

  4. Preparation methods of mixed metal sulfide catalysts for deep hydrogenation of crude oils%原油深度加氢复合多金属硫化物催化剂的制备方法

    Institute of Scientific and Technical Information of China (English)

    蒋丽娟; 李来平; 张文钲

    2014-01-01

    复合多金属硫化物( MMS)催化剂主要用于原油的深度加氢,用于生产高十六烷值、低硫和低芳族化合物柴油。MMS催化剂包含NiMoS、NiWS、NiMoO、NiWO、NiMoWS和ZnMoWS催化剂等。综述MMS催化剂中二元复合金属硫化物催化剂和三元复合金属硫化物催化剂的制备方法,采用二步法即添加有机物作孔成形剂先制得催化剂前驱体,再由前驱体制得的MMS催化剂结构更松散,具有较大的比表面积(90 m2·g-1)和大孔容(大于0.3 cm3·g-1),因而具有更好的催化活性。对比不同MMS催化剂对重质柴油、焦油等的加氢裂解、加氢脱硫和加氢脱氮性能,认为NiMoW三元复合金属硫化物催化剂(50%Ni25%Mo25%W)的活性最优。%Mixed metal sulfide catalyst( MMS)catalysts are mainly used for deep hydroprocessing of refractory crudes to produce diesel oil with higher cetane number,lower sulfur and lower aromatic compounds. MMS catalysts include NiMoS,NiWS,NiMoO,NiWO,NiMoWS and ZnMoWS,etc. The preparation methods of MMS catalysts,including bi-metallic sulfide catalysts and tri-metallic sulfide catalysts,were summarized in this paper. The catalyst precursors were prepared by adding organic compounds as pore forming agents,and then the catalysts were prepared. The catalysts prepared by the two-steps method possessed dispersive structure. The attained catalyst with BET specific surface area of 90 m2·g-1 and pore volume of 0. 3 cm3 ·g-1 exhibited better catalytic activity. Compared with other several MMS catalysts,the hydrocracking,hydrodesulfurization and hydrodenitrification activities of NiMoW(50mol%Ni,25mol%Mo,25mol%W)tri-metallic sulfide catalysts for processing heavy diesel oil and tar were the best.

  5. Synthesis and Characterization of Platinum-Ruthenium-Tin Catalysts

    Science.gov (United States)

    Uffalussy, Karen

    Magnesia-supported trimetallic Pt-Ru-Sn catalysts prepared through a cluster and a conventional synthetic route have been investigated in terms of their structural properties and their catalytic activity for the hydrogenation of citral and crotonaldehyde. FTIR results indicate that the majority of the stabilizing ligands remain attached to the PtRu5(μ-SnPh 2)(C)(CO)15 cluster used following impregnation onto the MgO support. Under H2 reduction conditions, partial and full ligand removal are both observed at 473 and 573 K, respectively. HRSTEM analysis shows that cluster-derived samples exhibit significantly smaller average metal particle sizes, as well as narrower particle size distributions than the corresponding conventionally prepared ones. EDX measurements show that in the cluster-derived catalysts, the majority of the metal particles present are trimetallic in nature, with metal compositions similar to those of the original cluster. In contrast, the conventionally prepared materials contain mostly bimetallic and monometallic particles with variable compositions. XPS was used to determine how the variation in method of Sn addition to bimetallic Pt-Ru affects the electronic state for the trimetallic Pt-Ru-Sn/MgO system prepared by impregnation using multimetallic clusters, metal-salts, and the combination of both precursor types. Results show that the PtRu5Sn/MgO material has a significantly higher percentage of Sn0 in comparison to Pt-Ru-Sn/MgO and PtRu5-Sn/MgO, and a corresponding shift in both Pt and Ru peaks can be correlated to this relative change in Sn oxidation state. The formation of smaller metal particles and electronic modification of Pt and Ru by Sn in the cluster-derived catalysts and the presence of the three metals in these particles in close proximity result in higher activity and selectivity to the unsaturated alcohols for the hydrogenation of both citral and crotonaldehyde.

  6. Sol-gel based oxidation catalyst and coating system using same

    Science.gov (United States)

    Watkins, Anthony N. (Inventor); Leighty, Bradley D. (Inventor); Oglesby, Donald M. (Inventor); Patry, JoAnne L. (Inventor); Schryer, Jacqueline L. (Inventor)

    2010-01-01

    An oxidation catalyst system is formed by particles of an oxidation catalyst dispersed in a porous sol-gel binder. The oxidation catalyst system can be applied by brush or spray painting while the sol-gel binder is in its sol state.

  7. Hydrothermally Stable Fe–W–Ti SCR Catalysts Prepared by Deposition–Precipitation

    DEFF Research Database (Denmark)

    Putluru, Siva Sankar Reddy; Schill, Leonhard; Mossin, Susanne;

    2014-01-01

    Fe/TiO2 based catalysts were prepared by incipient wetness impregnation and deposition–precipitation (DP). The catalysts were characterized by activity measurements, N2 physisorption, X-ray powder diffraction, electron paramagnetic resonance spectroscopy, energy dispersive X-ray spectroscopy, H2-.......Relative SCR activity of catalysts at 450 °C....

  8. Quantitative study of catalytic activity and catalytic deactivation of Fe–Co/Al2O3 catalysts for multi-walled carbon nanotube synthesis by the CCVD process

    OpenAIRE

    Pirard, Sophie; Heyen, Georges; Pirard, Jean-Paul

    2010-01-01

    The catalytic deactivation during multi-walled carbon nanotube (MWNT) synthesis by the CCVD process and the influence of hydrogen on it were quantified. Initial specific reaction rate, relative specific productivity and catalytic deactivation were studied. Carbon source was ethylene, and a bimetallic iron–cobalt catalyst supported on alumina was used. The catalytic deactivation was modeled by a decreasing hyperbolic law, reflecting the progressive accumulation of amorphous carbon on active si...

  9. Promotion Effects of Nickel Catalysts of Dry Reforming with Methane

    Institute of Scientific and Technical Information of China (English)

    YAN,Zi-Feng(阎子峰); DING,Rong-Gang(丁荣刚); LIU,Xin-Mei(刘欣梅); SONG,Lin-Hua(宋林花)

    2001-01-01

    The promotion effects of nickel catalyst of dry reforming with methane were extensively investigated by means of XRD,SEM, EDX, N2-adsorption and H2-adsorption. XRD characterization indicated that good dispersion of nickel oxide and MgO promoter is achieved over γ-Al2O3 support. Addition of MgO promoter effectively retards the formation of NiS12O4 phase. SEM and EDX analysis exhibited that the addition ofrare-earth metal oxide CeO2 effectively promotes the Ni metal dispersion on the surface of the catalysts despite of undesirable self-dispersion of CeO2 promoter. Furthermore, the nickel component is gradually dispersed on the surface of the support following the exposure to reaction gas mixture for a period of time. The addition of MgO inhibited the self-dispersion and promotion effect of CeO2 on Ni dispersion on the catalysts. H2 chemisorption revealed that the addition of the alkaline oxide MgO promoter significantly prohibits the metal dispersion on the catalyst. Inappropriate promoter addition can result in sharp decrease of the metal dispersion. N2-adsorption indicated that oxide promoter was mostly concentrated on the outer layer of the alumina support while the nickel metal was generally dispersed in the support pores. Addition of promoters contributed to more reduction in mesopore volume.

  10. Characterization of Bimetallic Fe-Ru Oxide Nanoparticles Prepared by Liquid-Phase Plasma Method.

    Science.gov (United States)

    Lee, Sung-Jin; Lee, Heon; Jeon, Ki-Joon; Park, Hyunwoong; Park, Young-Kwon; Jung, Sang-Chul

    2016-12-01

    The bimetallic Fe-Ru oxide nanoparticles were synthesized in the liquid-phase plasma (LPP) method which employed iron chloride and ruthenium chloride as precursors. The active species (OH·, Hα, Hβ, and O(I)) and the iron and ruthenium ions were observed in the plasma field created by the LPP process. The spherical-shaped bimetallic Fe-Ru oxide nanoparticles were synthesized by the LPP reaction, and the size of the particles was growing along with the progression of the LPP reaction. The synthesized bimetallic Fe-Ru oxide nanoparticles were comprised of Fe2O3, Fe3O4, RuO, and RuO2. Ruthenium had a higher reduction potential than iron and resulted in higher ruthenium composition in the synthesized bimetallic nanoparticles. The control of the molar ratio of the precursors in the reactant solution was found to be employed as a means to control the composition of the elements in bimetallic nanoparticles. PMID:27456502

  11. Cr(VI) reduction in wastewater using a bimetallic galvanic reactor

    International Nuclear Information System (INIS)

    The electrochemical reduction of Cr(VI)-Cr(III) in wastewater by iron and copper-iron bimetallic plates was evaluated and optimized. Iron has been used as a reducing agent, but in this work a copper-iron galvanic system in the form of bimetallic plates is applied to reducing hexavalent chromium. The optimal pH (2) and ratio of copper to iron surface areas (3.5:1) were determined in batch studies, achieving a 100% reduction in about 25 min. The Cr(VI) reduction kinetics for the bimetallic system fit a first order mechanism with a correlation of 0.9935. Thermodynamic analysis shows that the Cr(VI) reduction is possible at any pH value. However, at pH values above 3.0 for iron and 5.5 for chromium insoluble species appear, indicating that the reaction will be hindered. Continuous column studies indicate that the bimetallic copper-iron galvanic system has a reduction capacity of 9.5890 mg Cr(VI) cm-2 iron, whereas iron alone only has a capacity of 0.1269 mg Cr(VI) cm-2. The bimetallic copper-iron galvanic system is much more effective in reducing hexavalent chromium than iron alone. The exhausted plates were analyzed by SEM, EDS, and XRD to determine the mechanism and the surface effects, especially surface fouling.

  12. Thermal diffusivity of nanofluids containing Au/Pd bimetallic nanoparticles of different compositions.

    Science.gov (United States)

    Sánchez-Ramírez, J F; Jiménez Pérez, J L; Cruz Orea, A; Gutierrez Fuentes, R; Bautista-Hernández, A; Pal, U

    2006-03-01

    Colloidal suspensions of bimetallic Au/Pd nanoparticles were prepared by simultaneous reduction of the metal ions from their corresponding chloride salts with polymer (PVP) stabilizer. Thermal properties of water containing bimetallic nanoparticles with different nominal compositions (Au/Pd = 12/1, 5/1, 1/1, 1/5) were measured using the mode mismatched dual-beam thermal lens technique to determine the effect of particle composition on the thermal diffusivity of the nanofluids. The characteristic time constant of the transient thermal lens was estimated by fitting the experimental data to the theoretical expression for transient thermal lens. The thermal diffusivity of the nanofluids (water, containing Au/Pd bimetallic nanoparticles) is seen to be strongly dependent on the composition of the particles. The maximum diffusivity was achieved for the nanoparticles with highest Au/Pd molar ratio. A possible mechanism for such high thermal diffusivity of the nanofluids with bimetallic particles is given. UV-Vis spectroscopy, TEM and high-resolution electron microscopy (HREM) techniques were used to characterize the Au/Pd bimetallic nanoparticles. PMID:16573121

  13. Monte Carlo simulation of the PEMFC catalyst layer

    Institute of Scientific and Technical Information of China (English)

    WANG Hongxing; CAO Pengzhen; WANG Yuxin

    2007-01-01

    The performance of the polymer electrolyte membrane fuel cell (PEMFC) is greatly controlled by the structure of the catalyst layer.Low catalyst utilization is still a significant obstacle to the commercialization of the PEMFC.In order to get a fundamental understanding of the electrode structure and to find the limiting factor in the low catalyst utilization,it is necessary to develop the mechanical model on the effect of catalyst layer structure on the catalyst utilization and the performance of the PEMFC.In this work,the structure of the catalyst layer is studied based on the lattice model with the Monte Carlo simulation.The model can predict the effects of some catalyst layer components,such as Pt/C catalyst,electrolyte and gas pores,on the utilization of the catalyst and the cell performance.The simulation result shows that the aggregation of conduction grains can greatly affect the degree of catalyst utilization.The better the dispersion of the conduction grains,the larger the total effective area of the catalyst is.To achieve higher utilization,catalyst layer components must be distributed by means of engineered design,which can prevent aggregation.

  14. Polymer nanocomposite membranes with hierarchically structured catalysts for high throughput dehalogenation

    Science.gov (United States)

    Crock, Christopher A.

    Halogenated organics are categorized as primary pollutants by the Environmental Protection Agency. Trichloroethylene (TCE), which had broad industrial use in the past, shows persistence in the environment because of its chemical stability. The large scale use and poor control of TCE resulted in its prolonged release into the environment before the carcinogenic risk associated with TCE was fully understood. TCE pollution stemmed from industrial effluents and improper disposal of solvent waste. Membrane reactors are promising technology for treating TCE polluted groundwater because of the high throughput, relatively low cost of membrane fabrication and facile retrofitting of existing membrane based water treatment facilities with catalytic membrane reactors. Compared to catalytic fluidized or fixed bed reactors, catalytic membrane reactors feature minimal diffusional limitation. Additionally, embedding catalyst within the membrane avoids the need for catalyst recovery and can prevent aggregation of catalytic nanoparticles. In this work, Pd/xGnP, Pd-Au/xGnP, and commercial Pd/Al2O3 nanoparticles were employed in batch and flow-through membrane reactors to catalyze the dehalogenation of TCE in the presence of dissolved H2. Bimetallic Pd-Au/xGnP catalysts were shown to be more active than monometallic Pd/xGnP or commercial Pd/Al 2O3 catalysts. In addition to synthesizing nanocomposite membranes for high-throughput TCE dehalogenation, the membrane based dehalogenation process was designed to minimize the detrimental impact of common catalyst poisons (S2-, HS-, and H2S -) by concurrent oxidation of sulfide species to gypsum in the presence of Ca2+ and removal of gypsum through membrane filtration. The engineered membrane dehalogenation process demonstrated that bimetallic Pd-Au/xGnP catalysts resisted deactivation by residual sulfide species after oxidation, and showed complete removal of gypsum during membrane filtration.

  15. The kinetics of CO poisoning in simulated reformate and effect of Ru island morphology on PtRu fuel cell catalysts as determined by operando XANES

    Energy Technology Data Exchange (ETDEWEB)

    Scott, F.; Roth, C; Ramaker, D

    2007-01-01

    In situ X-ray absorption spectroscopy (XAS) measurements, including both X-ray absorption near edge spectroscopy (XANES) and extended X-ray absorption fine structure (EXAFS), were carried out on commercially produced Pt and PtRu bimetallic electrocatalysts as well as on a mechanically mixed PtRu bimetallic electrocatalyst in an operating fuel cell in H{sub 2} doped with 150 ppm CO. By use of the novel {Delta}XANES technique, the coverages of CO and ontop and n-fold H (overpotential deposited and underpotential deposited hydrogen) are obtained and compared for the three catalysts, and the results are correlated with PtRu cluster morphology. The mechanical mixing process used to create the bimetallic PtRu catalyst is found to maximize CO tolerance, although the PtRu commercial electrocatalyst exhibits an increased electronic effect, most probably due to the presence of Ru(O){sub x} islands at the catalyst surface. The mobility of the CO on both Ru and Pt is found to be sharply dependent on the CO coverage, decreasing dramatically beyond 0.4 fractional coverage.

  16. Bifunctional Catalysts for Upgrading of Biomass-Derived Oxygenates: A Review

    Energy Technology Data Exchange (ETDEWEB)

    Robinson, Allison M.; Hensley, Jesse E.; Medlin, J. Will

    2016-08-05

    Deoxygenation is an important reaction in the conversion of biomass-derived oxygenates to fuels and chemicals. A key route for biomass refining involves the production of pyrolysis oil through rapid heating of the raw biomass feedstock. Pyrolysis oil as produced is highly oxygenated, so the feasibility of this approach depends in large part on the ability to selectively deoxygenate pyrolysis oil components to create a stream of high-value finished products. Identification of catalytic materials that are active and selective for deoxygenation of pyrolysis oil components has therefore represented a major research area. One catalyst is rarely capable of performing the different types of elementary reaction steps required to deoxygenate biomass-derived compounds. For this reason, considerable attention has been placed on bifunctional catalysts, where two different active materials are used to provide catalytic sites for diverse reaction steps. Here, we review recent trends in the development of catalysts, with a focus on catalysts for which a bifunctional effect has been proposed. We summarize recent studies of hydrodeoxygenation (HDO) of pyrolysis oil and model compounds for a range of materials, including supported metal and bimetallic catalysts as well as transition-metal oxides, sulfides, carbides, nitrides, and phosphides. Particular emphasis is placed on how catalyst structure can be related to performance via molecular-level mechanisms. These studies demonstrate the importance of catalyst bifunctionality, with each class of materials requiring hydrogenation and C-O scission sites to perform HDO at reasonable rates.

  17. Salt flux synthesis of single and bimetallic carbide nanowires

    Science.gov (United States)

    Leonard, Brian M.; Waetzig, Gregory R.; Clouser, Dale A.; Schmuecker, Samantha M.; Harris, Daniel P.; Stacy, John M.; Duffee, Kyle D.; Wan, Cheng

    2016-07-01

    Metal carbide compounds have a broad range of interesting properties and are some of the hardest and highest melting point compounds known. However, their high melting points force very high reaction temperatures and thus limit the formation of high surface area nanomaterials. To avoid the extreme synthesis temperatures commonly associated with these materials, a new salt flux technique has been employed to reduce reaction temperatures and form these materials in the nanometer regime. Additionally, the use of multiwall carbon nanotubes as a reactant further reduces the diffusion distance and provides a template for the final carbide materials. The metal carbide compounds produced through this low temperature salt flux technique maintain the nanowire morphology of the carbon nanotubes but increase in size to ˜15-20 nm diameter due to the incorporation of metal in the carbon lattice. These nano-carbides not only have nanowire like shape but also have much higher surface areas than traditionally prepared metal carbides. Finally, bimetallic carbides with composition control can be produced with this method by simply using two metal precursors in the reaction. This method provides the ability to produce nano sized metal carbide materials with size, morphology, and composition control and will allow for these compounds to be synthesized and studied in a whole new size and temperature regime.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  19. Synthesis and characterization of Ni-Mo bimetallic nitride from the mixture of nitrogen and hydrogen

    International Nuclear Information System (INIS)

    A new method for the synthesis of Ni-Mo bimetallic nitrides was reported in the present paper. The bimetallic nitrides were successfully prepared by a temperature-programmed reaction between bimetallic oxide precursors and the mixed gases of N2 and H2 instead of NH3. By adjusting pH values of the solution in the process of co-precipitation, pure NiMoO4 or NiMoO4 with excess MoO3 was obtained, and then pure Ni3Mo3N or Ni3Mo3N with γ-Mo2N was synthesized by nitriding the precursors. The structural properties of the precursors and their corresponding nitrides were investigated by means of X-ray diffraction (XRD), ultraviolet laser Raman spectroscopy, thermogravimetric (TG) analysis and chemical analysis of total nitrogen content

  20. Bimetallic Metal-Organic Frameworks for Controlled Catalytic Graphitization of Nanoporous Carbons

    Science.gov (United States)

    Tang, Jing; Salunkhe, Rahul R.; Zhang, Huabin; Malgras, Victor; Ahamad, Tansir; Alshehri, Saad M.; Kobayashi, Naoya; Tominaka, Satoshi; Ide, Yusuke; Kim, Jung Ho; Yamauchi, Yusuke

    2016-07-01

    Single metal-organic frameworks (MOFs), constructed from the coordination between one-fold metal ions and organic linkers, show limited functionalities when used as precursors for nanoporous carbon materials. Herein, we propose to merge the advantages of zinc and cobalt metals ions into one single MOF crystal (i.e., bimetallic MOFs). The organic linkers that coordinate with cobalt ions tend to yield graphitic carbons after carbonization, unlike those bridging with zinc ions, due to the controlled catalytic graphitization by the cobalt nanoparticles. In this work, we demonstrate a feasible method to achieve nanoporous carbon materials with tailored properties, including specific surface area, pore size distribution, degree of graphitization, and content of heteroatoms. The bimetallic-MOF-derived nanoporous carbon are systematically characterized, highlighting the importance of precisely controlling the properties of the carbon materials. This can be done by finely tuning the components in the bimetallic MOF precursors, and thus designing optimal carbon materials for specific applications.

  1. Design and performance benchmark of various architectures of a piezoelectric bimetallic strip heat engine

    Science.gov (United States)

    Boughaleb, J.; Arnaud, A.; Monfray, S.; Cottinet, P. J.; Quenard, S.; Boeuf, F.; Guyomar, D.; Skotnicki, T.

    2016-06-01

    This paper deals with an investigation of a thermal energy harvester based on the coupling of a piezoelectric membrane and a bimetallic strip heat engine. The general working principle of the device consists of a double conversion mechanism: the thermal energy is first converted into mechanical energy by means of a bimetallic strip, then the mechanical energy is converted into electricity with a piezoelectric membrane. This paper deals with the study and optimization of the harvester's design. First, the piezoelectric membrane configuration is studied to find the most efficient way to convert mechanical energy into electricity. A benchmark of various piezoelectric materials is then presented to point out the most efficient materials. Finally, our study focuses on the bimetallic strip's properties: the effect of its dimensions of its thermal hysteresis on the harvester's performances are studied and compared. Thanks to these different steps, we were able to point out the best configuration to convert efficiently thermal heat flux into electricity.

  2. Plasmonic emission enhancement of colloidal quantum dots in the presence of bimetallic nanoparticles

    International Nuclear Information System (INIS)

    We studied plasmonic features of bimetallic nanostructures consisting of gold nanoisland cores semi-coated with a chromium layer and explored how they influence emission of CdSe/ZnS quantum dots. We showed that, compared with chromium-covered glass substrates without the gold cores, the bimetallic nanostructures could significantly enhance the emission of the quantum dots. We studied the impact of the excitation intensity and thickness of the chromium layer on this process and utilized numerical means to identify the mechanisms behind it. Our results suggest that when the chromium layer is thin, the enhancement process is the result of the bimetallic plasmonic features of the nanostructures. As the chromium layer becomes thick, the impact of the gold cores is screened and the enhancement mostly happens mostly via the field enhancement of chromium nanoparticles in the absence of significant energy transfer from the quantum dots to these nanoparticles

  3. Melting Behaviour of Core-Shell Structured Ag-Rh Bimetallic Clusters

    Institute of Scientific and Technical Information of China (English)

    PAN Yang; CHENG Dao-Jian; HUANG Shi-Ping; WANG Wen-Chuan

    2007-01-01

    The me/ting behaviour of four typical core-shell structured 309-atom Ag-Rh bimetallic clusters, with decahedral and icosahedral geometric configurations, is investigated by using molecular dynamics simulation, based on the Sutton-Chen potential. The initial atomic configurations are obtained from semi-grand canonical ensemble Monte Carlo simulations. It is found that the melting point temperature Tm increases with the mole fraction of Rh in the bimetallic clusters, and Tm of Ag-Rh icosahedral clusters is higher than those of Ag-Rh decahedral clusters with the same Rh mole fraction. It is also found that the Ag atoms lie on the surface of Ag-Rh bimetallic clusters even after melting.

  4. Description of the performances of a thermo-mechanical energy harvester using bimetallic beams

    Science.gov (United States)

    Arnaud, A.; Boughaleb, J.; Monfray, S.; Boeuf, F.; Cugat, O.; Skotnicki, T.

    2016-06-01

    Many recent researches have been focused on the development of thermal energy harvesters using thermo-mechanical or thermo-electrical coupling phenomena associated to a first-order thermodynamic transition. In the case of the bimetallic strip heat engine, the exploitation of the thermo-mechanical instability of bimetallic membranes placed in a thermal gradient enables to convert heat into kinetic energy. This paper is a contribution to the modeling and the comprehension of these heat engines. By restraining the study to the simply-supported bimetallic beams and using a Ritz approximation of the beam shape, this paper aims to give an analytical solution to the first mode of the composite beams and then to evaluate the efficiency of the harvesters exploiting these kinds of instability.

  5. The quality of the joint between alloy steel and unalloyed cast steel in bimetallic layered castings

    Directory of Open Access Journals (Sweden)

    T. Wróbel

    2012-01-01

    Full Text Available In paper is presented technology of bimetallic layered castings based on founding method of layer coating directly in cast process so-called method of mould cavity preparation. Prepared castings consist two fundamental parts i.e. bearing part and working part (layer. The bearing part of bimetallic layered casting is typical foundry material i.e. ferritic-pearlitic unalloyed cast steel, whereas working part (layer is plate of austenitic alloy steel sort X2CrNi 18-9. The ratio of thickness between bearing and working part is 8:1. The aim of paper was assessed the quality of the joint between bearing and working part in dependence of pouring temperature and carbon concentration in cast steel. The quality of the joint in bimetallic layered castings was evaluated on the basis of ultrasonic non-destructive testing, structure and microhardness researches.

  6. Ni-based heterogeneous catalyst from a designed molecular precursor for the efficient electrochemical water oxidation.

    Science.gov (United States)

    Kuznetsov, Denis A; Konev, Dmitry V; Komarova, Natal'ya S; Ionov, Andrey M; Mozhchil, Rais N; Fedyanin, Ivan V

    2016-07-28

    Bimetallic Ni-Mo alkoxide was synthesized and exploited as the single-source precursor for the solution-processed deposition of the mixed-oxide layers on different conducting surfaces. Upon potential cycling in 1 M NaOH, these composites convert, in situ, into highly porous NiOx/NiOOH catalysts characterized by the high electrocatalytic activity for water oxidation under both basic (pH 13.6) and near neutral (pH 9.2) conditions. PMID:27354324

  7. Formulation of cracking catalyst based on zeolite and natural clays

    Energy Technology Data Exchange (ETDEWEB)

    Aliev, R.R.; Lupina, M.I.

    1995-11-01

    Domestically manufactured cracking catalysts are based on a synthetic amorphous aluminosilicate matrix and Y zeolite. A multistage {open_quotes}gel{close_quotes} technology is used in manufacturing the catalysts. The process includes mixing solutions of sodium silicate and acidic aluminum sulfate, forming, syneresis, and activation of the beaded gel. In the manufacture of bead catalysts, the next steps in the process are washing, drying, and calcining; in the manufacture of microbead catalysts, the next steps are dispersion and formation of a hydrogel slurry, spray-drying, and calcining. The Y zeolite is either introduced into the alumina-silica sol in the stage of forming the beads, or introduced in the dispersion stage. With the aim of developing an active and selective cracking catalyst based on Y zeolite and natural clays, with improved physicomechanical properties, the authors carried out a series of studies, obtaining results that are set forth in the present article.

  8. Research advances in the catalysts for the selective oxidation of ethane to aldehydes

    Institute of Scientific and Technical Information of China (English)

    ZHANG Zhe; ZHAO Zhen; XU Chunming

    2005-01-01

    Selective oxidation of ethane to aldehydes is one of the most difficult processes in the catalysis researches of low alkanes. The development of selective oxidation of ethane to aldehydes (formaldehyde, acetaldehyde and acrolein) is discussed. The latest progress of the catalysts, including bulk or supported metal oxide catalysts, highly dispersed and isolated active sites catalysts, and the photo-catalytic ethane oxidation catalysts, partial oxidation of ethane in the gas phase, and the proposed reaction pathways from ethane to aldehydes are involved.

  9. Chemical dispersants

    NARCIS (Netherlands)

    Rahsepar, Shokouhalsadat; Smit, Martijn P.J.; Murk, Albertinka J.; Rijnaarts, Huub H.M.; Langenhoff, Alette A.M.

    2016-01-01

    Chemical dispersants were used in response to the Deepwater Horizon oil spill in the Gulf of Mexico, both at the sea surface and the wellhead. Their effect on oil biodegradation is unclear, as studies showed both inhibition and enhancement. This study addresses the effect of Corexit on oil biodeg

  10. Structure analysis of bimetallic Co-Au nanoparticles formed by sequential ion implantation

    Science.gov (United States)

    Chen, Hua-jian; Wang, Yu-hua; Zhang, Xiao-jian; Song, Shu-peng; chen, Hong; Zhang, Ke; Xiong, Zu-zhao; Ji, Ling-ling; Dai, Hou-mei; Wang, Deng-jing; Lu, Jian-duo; Wang, Ru-wu; Zheng, Li-rong

    2016-08-01

    Co-Au alloy Metallic nanoparticles (MNPs) are formed by sequential ion implantation of Co and Au into silica glass at room temperature. The ion ranges of Au ions implantation process have been displayed to show the ion distribution. We have used the atomic force microscopy (AFM) and transmission electron microscopy (TEM) to investigate the formation of bimetallic nanoparticles. The extended X-ray absorption fine structure (EXAFS) has been used to study the local structural information of bimetallic nanoparticles. With the increase of Au ion implantation, the local environments of Co ions are changed enormously. Hence, three oscillations, respectively, Co-O, Co-Co and Co-Au coordination are determined.

  11. Resonance parameters based analysis for metallic thickness optimization of a bimetallic plasmonic structure

    Science.gov (United States)

    Bera, Mahua; Banerjee, Jayeta; Ray, Mina

    2014-02-01

    Metallic film thickness optimization in mono- and bimetallic plasmonic structures has been carried out in order to determine the correct device parameters. Different resonance parameters, such as reflectivity, phase, field enhancement, and the complex amplitude reflectance Argand diagram (CARAD), have been investigated for the proposed optimization procedure. Comparison of mono- and bimetallic plasmonic structures has been carried out in the context of these resonance parameters with simultaneous angular and spectral interrogation. Differential phase analysis has also been performed and its application to sensing has been discussed along with a proposed interferometric set-up.

  12. Polyfunctional two- (2D) and three- (3D) dimensional oxalate bridged bimetallic magnets

    CERN Document Server

    Clément, R; Gruselle, M; Train, C

    2003-01-01

    We report major results concerning polyfunctional two- (2D) and three- (3D) dimensional oxalate bridged bimetallic magnets. As a consequence of their specific organization they are composed of an anionic sub-lattice and a cationic counter-part. These bimetallic polymers can accommodate various counter-cations possessing specific physical properties in addition to the magnetic ones resulting from the interactions between the metallic ions in the anionic sub-lattice. Thus, molecular magnets possessing paramagnetic, conductive and optical properties are presented in this review. Refs. 60 (author)

  13. Electrochemical catalyst recovery method

    Science.gov (United States)

    Silva, Laura J.; Bray, Lane A.

    1995-01-01

    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.

  14. Chemical and electrochemical promotion of supported rhodium catalyst

    OpenAIRE

    Baranova, Olena; Comninellis, Christos

    2007-01-01

    The chemical and electrochemical promotion of highly dispersed nanofilm Rh catalysts (dispersion: about 10 %, film thickness: 40 nm) has been investigated for the first time. To this end Rh metal was sputter-deposited, either on a purely ionic conductor (8 % Y2O3-stabilized ZrO2) or on a mixed ionic-electronic conductor (TiO2), the latter being a highly dispersed layer of TiO2 (4 µm) deposited on YSZ. These catalysts are designated as Rh/YSZ and Rh/TiO2/YSZ, respectively. It was established a...

  15. Design strategies for the molecular level synthesis of supported catalysts.

    Science.gov (United States)

    Wegener, Staci L; Marks, Tobin J; Stair, Peter C

    2012-02-21

    Supported catalysts, metal or oxide catalytic centers constructed on an underlying solid phase, are making an increasingly important contribution to heterogeneous catalysis. For example, in industry, supported catalysts are employed in selective oxidation, selective reduction, and polymerization reactions. Supported structures increase the thermal stability, dispersion, and surface area of the catalyst relative to the neat catalytic material. However, structural and mechanistic characterization of these catalysts presents a formidable challenge because traditional preparations typically afford complex mixtures of structures whose individual components cannot be isolated. As a result, the characterization of supported catalysts requires a combination of advanced spectroscopies for their characterization, unlike homogeneous catalysts, which have relatively uniform structures and can often be characterized using standard methods. Moreover, these advanced spectroscopic techniques only provide ensemble averages and therefore do not isolate the catalytic function of individual components within the mixture. New synthetic approaches are required to more controllably tailor supported catalyst structures. In this Account, we review advances in supported catalyst synthesis and characterization developed in our laboratories at Northwestern University. We first present an overview of traditional synthetic methods with a focus on supported vanadium oxide catalysts. We next describe approaches for the design and synthesis of supported polymerization and hydrogenation catalysts, using anchoring techniques which provide molecular catalyst structures with exceptional activity and high percentages of catalytically significant sites. We then highlight similar approaches for preparing supported metal oxide catalysts using atomic layer deposition and organometallic grafting. Throughout this Account, we describe the use of incisive spectroscopic techniques, including high

  16. Chemisorption Techniques for the Determination of Metal Dispersion

    International Nuclear Information System (INIS)

    Chemisorption is an effective and un expensive analytical technique for characterizing and titrating active centers of the catalyst surface and for evaluating its activity with good approximation. The paper describes experimental procedures and the nature of information that can be obtained about active metal dispersion and area, diameter of active particles and isosteric heat of dispersion

  17. Atomic level study of water-gas shift catalysts via transmission electron microscopy and x-ray spectroscopy

    Science.gov (United States)

    Akatay, Mehmed Cem

    Water-gas shift (WGS), CO + H2O ⇆ CO2 + H2 (DeltaH° = -41 kJ mol -1), is an industrially important reaction for the production of high purity hydrogen. Commercial Cu/ZnO/Al2O3 catalysts are employed to accelerate this reaction, yet these catalysts suffer from certain drawbacks, including costly regeneration processes and sulfur poisoning. Extensive research is focused on developing new catalysts to replace the current technology. Supported noble metals stand out as promising candidates, yet comprise intricate nanostructures complicating the understanding of their working mechanism. In this study, the structure of the supported Pt catalysts is explored by transmission electron microscopy and X-ray spectroscopy. The effect of the supporting phase and the use of secondary metals on the reaction kinetics is investigated. Structural heterogeneities are quantified and correlated with the kinetic descriptors of the catalysts to develop a fundamental understanding of the catalytic mechanism. The effect of the reaction environment on catalyst structure is examined by in-situ techniques. This study benefitted greatly from the use of model catalysts that provide a convenient medium for the atomic level characterization of nanostructures. Based on these studies, Pt supported on iron oxide nano islands deposited on inert spherical alumina exhibited 48 times higher WGS turnover rate (normalized by the total Pt surface area) than Pt supported on bulk iron oxide. The rate of aqueous phase glycerol reforming reaction of Pt supported on multiwall carbon nanotubes (MWCNT) is promoted by co-impregnating with cobalt. The synthesis resulted in a variety of nanostructures among which Pt-Co bimetallic nanoparticles are found to be responsible for the observed promotion. The unprecedented WGS rate of Pt supported on Mo2C is explored by forming Mo 2C patches on top of MWCNTs and the rate promotion is found to be caused by the Pt-Mo bimetallic entities.

  18. Development of structural characterisation tools for catalysts; Developpement d'outils de caracterisation structurale de catalyseurs

    Energy Technology Data Exchange (ETDEWEB)

    Lynch, J.

    1999-10-01

    Because of the diversity of their compositions and structures, and the treatments needed to render them active, heterogeneous catalysts present a major challenge in structural characterisation. Electron microscopy provides textural and structural information at the scale of the individual particle. We have been able to analyse epitaxial relationships between nanometer size particles and their support and to determine which crystal faces are most exposed. Chemical analysis can be carried out on individual particles in a bimetallic catalyst. Limitations of this technique are shown for characterisation of catalysts at the atomic scale or in reactive conditions. Here, global analysis methods based on X-ray absorption and diffraction provide more information. W-ray absorption fine structure analysis has been applied to sub-nanometer size particles in platinum based catalysts to explore interactions between the metal and reactive gases such as hydrocarbons and H{sub 2}S. Differences observed between mono-metallic and bimetallic solids lead to structural models to explain differences in catalyst reactivity. X-ray diffraction, combined with electron microscopy, shows the presence of different forms of extra-framework aluminium is steamed zeolites. Quantification of some these forms has been possible and a study of their reactivity towards different de-aluminating agents has been achieved. Work in progress shows the advantages of a combination of X-ray diffraction and absorption to study decomposition of hydrotalcites to form mixed oxides as well as possibilities in infra-red spectroscopy of adsorbed CO to determine surface sites in Fischer Tropsch catalysts. Use of in-situ analysis cells enables a detailed description of catalyst structure in reactive atmospheres and opens the possibility of correlating structure with catalytic activity. (author)

  19. Fabrication of Cu/Pd bimetallic nanostructures with high gas sorption ability towards development of LPG sensor

    International Nuclear Information System (INIS)

    A one-step synthesis of bimetallic Cu/Pd nanorods with rod's diameter ∼3 nm and their length in the range 10–15 nm is presented. The average size, size distribution, surface morphology and structure of the bimetallic Cu/Pd have been determined by transmission electron microscope (TEM), acoustic particle sizer (APS), scanning electron microscope (SEM) and X-ray diffraction (XRD), respectively. Further, thin films of bimetallic Cu/Pd nanostructures have been fabricated via spin-coating method. Fabricated films are, then, investigated for humidity and liquefied petroleum gas (LPG) sensors for the first time. The sensitivity and sensor response of the films towards the LPG are found better in comparison to the humidity. The investigated sensing parameters demonstrate that the fabricated LPG sensor using Cu/Pd bimetallic nanostructures is challenging for the detection of LPG at room temperature. - Highlights: • Fabrication of Cu/Pd meso-porous bimetallic thin film. • Cu/Pd nanostructures were characterized by SEM, TEM, APS and XRD. • Bimetallic nanostructures with smaller sizes and narrower size distributions. • First report on Cu/Pd bimetallic nanostructures as sensors. • Sensitivity of the sensor was simply enhanced by Cu-incorporation

  20. Electronic characterization and reactivity of bimetallic clusters of the Ti(Mg){sub n} type for hydrogen storage applications

    Energy Technology Data Exchange (ETDEWEB)

    Silva, Wilber [Institute of Chemistry, University of Antioquia, A.A. 1226, Medellin (Colombia); Truong, Thanh N. [Henry Eyring, Center for Theoretical Chemistry, Department of Chemistry, University of Utah, 315 South 1400 East, Rm 2020, Salt Lake City, UT 84112 (United States); Mondragon, Fanor, E-mail: fmondra@udea.edu.co [Institute of Chemistry, University of Antioquia, A.A. 1226, Medellin (Colombia)

    2011-08-25

    Highlights: > Magnesium-titanium clusters were modeled employing DFT and MP2. > Bimetallic systems have larger stability than monometallic magnesium clusters. > Reactivity of the bimetallic cluster is centered in the transition metal. > Bimetallic clusters are more reactive towards hydrogen to produce more stable hydrides. > Magnesium titanium systems are better for hydrogen storage than pure magnesium systems. - Abstract: This paper describes the variations in the properties, characteristics and hydrogenation energy barriers of magnesium clusters induced by titanium. DFT approach was used to determine the most stable structures at this theory level and then MP2 was used to refine the energy calculations with the basis set 6-311g(d) for magnesium and hydrogen, and pseudopotential lanl2dz for titanium. Bimetallic clusters showed higher stability and reactivity than the corresponding magnesium ones. Titanium induces a change in the magnesium atoms in their electronic configuration reflected in an increase of the population of their orbitals. At the same time titanium electronic populations is modified. These changes cause variations in some reactivity parameters such as the Fukui indexes which modify the hydrogenation of the magnesium clusters and bimetallic clusters. For example, there is a reduction in the energy barrier for dissociation of the H{sub 2} molecule in the bimetallic clusters. In the hydrogenated cluster the hydrogen atoms form bridges between all of the magnesium or magnesium-titanium atoms. These results indicate that, energetically, bimetallic systems can be more promising systems for hydrogen storage.

  1. Exploring the decomposition pathways of iron asymmetric transfer hydrogenation catalysts.

    Science.gov (United States)

    Lagaditis, Paraskevi O; Sues, Peter E; Lough, Alan J; Morris, Robert H

    2015-07-21

    Our group has developed a series of iron-based asymmetric transfer hydrogenation (ATH) catalysts for the reduction of polar double bonds. The activation of the precatalysts as well as the catalytic mechanism have been thoroughly investigated, but the decomposition pathways of these systems are poorly understood. Herein, we report a study of the deactivation pathways for an iron ATH catalyst under catalytically relevant conditions. The decomposition pathways were examined using experimental techniques and density functional theory (DFT) calculations. The major decomposition products that formed, Fe(CO)((Et)2PCH2CH2CHCHNCH2CH2P(Et)2) (3a) and Fe(CO)((Et)2PCH2CH2C(Ph)C(Ph)NCH2CH2P(Et)2) (3b), had two amido donors as well as a C=C bond on the diamine backbone of the tetradentate ligand. These species were identified by NMR studies and one was isolated as a bimetallic complex with Ru(II)Cp*. Two minor iron hydride species also formed concurrently with 3a, as determined by NMR studies, one of which was isolated and contained a fully saturated ligand as well as a hydride ligand. None of the compounds that were isolated were found to be active ATH catalysts. PMID:25373607

  2. Synthesis of bimetallic gold-silver alloy nanoclusters by simple mortar grinding.

    Science.gov (United States)

    Murugadoss, Arumugam; Kai, Noriko; Sakurai, Hidehiro

    2012-02-21

    A macroscale quantity of bimetallic Au-Ag alloy nanoclusters was achieved through sequential reduction by simple mortar grinding. The chitosan biopolymer was used as both a stabilizing and reducing agent. These nanoclusters exhibit excellent catalytic activity toward the reduction of 4-nitrophenol.

  3. Density and Shape Effects in the Acoustic Propulsion of Bimetallic Nanorod Motors.

    Science.gov (United States)

    Ahmed, Suzanne; Wang, Wei; Bai, Lanjun; Gentekos, Dillon T; Hoyos, Mauricio; Mallouk, Thomas E

    2016-04-26

    Bimetallic nanorods are propelled without chemical fuels in megahertz (MHz) acoustic fields, and exhibit similar behaviors to single-metal rods, including autonomous axial propulsion and organization into spinning chains. Shape asymmetry determines the direction of axial movement of bimetallic rods when there is a small difference in density between the two metals. Movement toward the concave end of these rods is inconsistent with a scattering mechanism that we proposed earlier for acoustic propulsion, but is consistent with an acoustic streaming model developed more recently by Nadal and Lauga ( Phys. Fluids 2014 , 26 , 082001 ). Longer rods were slower at constant power, and their speed was proportional to the square of the power density, in agreement with the acoustic streaming model. The streaming model was further supported by a correlation between the disassembly of spinning chains of rods and a sharp decrease in the axial speed of autonomously moving motors within the levitation plane of the cylindrical acoustic cell. However, with bimetallic rods containing metals of different densities, a consistent polarity of motion was observed with the lighter metal end leading. Speed comparisons between single-metal rods of different densities showed that those of lower density are propelled faster. So far, these density effects are not explained in the streaming model. The directionality of bimetallic rods in acoustic fields is intriguing and offers some new possibilities for designing motors in which shape, material, and chemical asymmetry might be combined for enhanced functionality. PMID:26991933

  4. Foundation Flash Catalyst

    CERN Document Server

    Goralski, Greg

    2010-01-01

    This book offers an introduction to Flash Catalyst for designers with intermediate to advanced skills. It discusses where Catalyst sits within the production process and how it communicates with other programs. It covers all of the features of the Flash Catalyst workspace, teaching you how to create designs from scratch, how to build application designs and add functionality, and how to master the Catalyst/Flex workflow. * Introduces Flash Catalyst * Focuses on production process * Covers the interrelation between Flash Catalyst and Photoshop/Illustrator/Flex/Flash What you'll learn Starting f

  5. Characterization of hydrophobic catalysts for hydrogen isotope exchange

    International Nuclear Information System (INIS)

    Domestic hydrophobic catalysts, KC-1 and KC-2, which were developed for the liquid phase catalytic exchange process separating hydrogen isotopes, were tested against Japanese catalyst, Kogel, which is being used in the Fugen's heavy water upgrader in Japan. KC-1 and KC-2 have different characteristics due to the differences of the solvent and solvent composition used. The test results of domestic hydrophobic catalysts characteristics such as pore distribution, specific surface area, platinum loading, and platinum dispersion from AECL agreed well with the results obtained by KEPRI/KAERI. The shape of KC-1 and KC-2 were 4x4 mm cylindrial pellet and that of Kogel catalyst was 4∼5.5mm sphere. The platinum loading of all catalysts were 0.8 wt%. The BET surface areas were 442, 247, 514m2 ·g-1 for KC-1, KC-2, and Kogel respectively, among which the BET surface area of KC-2 was the smallest. The platinum dispersion area was 2.47, 2.07, 1.90 m2g-1 and the platinum dispersion was 100, 100, 92% for KC-1, KC-2, and Kogel respectively, which showed domestic catalysts had higher values than Kogel catalyst. The average pore size was the largest in KC-2

  6. Cobalt-Lead-Manganese oxides combined cathode catalyst for air electrode in Zinc –air battery

    International Nuclear Information System (INIS)

    Highlights: • Bi and trimetallic oxides based on Mn, Pb and Co were prepared and characterized. • Introduction of Pb and Co in MnOx catalyst promote four electron ORR. • Zinc air battery with Mn2Pb2CoOx catalyst displays much smaller charge transfer resistance in contrast to the pure MnOx. • Mn2Pb2CoOx catalyst has lower loss of performance after 500C-D cycles than the rest of the catalysts. • Zinc air battery containing Mn2Pb2CoOx has promising current and power density and also discharge capacity. - Abstract: Bi and tri metalic oxides based on Mn, Pb and Co composite catalysts were prepared by oxidation of metal acetates with KMnO4. The structure of the catalysts was characterized by X-ray diffraction (XRD). It is found that the Mn2Pb2CoOx catalyst has amorphous structure and contains various oxides of Mn, Pb and Co. Electrocatalytic activity of catalysts in 6 M KOH was studied using Cyclic Voltammetry (CV) and polarization. Cyclic Voltammetry plot of Mn2Pb2CoOx catalyst showed higher electrocatalytic activity towards the Oxygen Reduction Reaction (ORR) compared to other tri and bimetallic composite catalysts. The kinetics of ORR on the catalysts was investigated using the rotating disk electrode technique in 6 M KOH solution. From the slope of Koutecky–Levich plots, it is evident that the ORR on Mn2Pb2CoOx is a 4-electron transfer process. With these inherent features, the zinc–air battery was fabricated using various catalysts and their performance was examined for practical applications

  7. Noble metal catalysts in the production of biofuels

    Energy Technology Data Exchange (ETDEWEB)

    Gutierrez, A.

    2013-11-01

    The energy demand is increasing in the world together with the need to ensure energy security and the desire to decrease greenhouse gas emissions. While several renewable alternatives are available for the production of electricity, e.g. solar energy, wind power, and hydrogen, biomass is the only renewable source that can meet the demand for carbon-based liquid fuels and chemicals. The technology applied in the conversion of biomass depends on the type and complexity of the biomass, and the desired fuel. Hydrogen and hydrogen-rich mixtures (synthesis gas) are promising energy sources as they are more efficient and cleaner than existing fuels, especially when they are used in fuel cells. Hydrotreatment is a catalytic process that can be used in the conversion of biomass or biomass-derived liquids into fuels. In autothermal reforming (ATR), catalysts are used in the production of hydrogen-rich mixtures from conventional fuels or bio-fuels. The different nature of biomass and biomass-derived liquids and mineral oil makes the use of catalysts developed for the petroleum industry challenging. This requires the improvement of available catalysts and the development of new ones. To overcome the limitations of conventional hydrotreatment and ATR catalysts, zirconia-supported mono- and bimetallic rhodium, palladium, and platinum catalysts were developed and tested in the upgrading of model compounds for wood-based pyrolysis oil and in the production of hydrogen, using model compounds for gasoline and diesel. Catalysts were also tested in the ATR of ethanol. For comparative purposes commercial catalysts were tested and the results obtained with model compounds were compared with those obtained with real feedstocks (hydrotreatmet tests with wood-based pyrolysis oil and ATR tests with NExBTL renewable diesel). Noble metal catalysts were active and selective in the hydrotreatment of guaiacol used as the model compound for the lignin fraction of wood-based pyrolysis oil and wood

  8. Ni Catalysts Supported on Modified Alumina for Diesel Steam Reforming

    Directory of Open Access Journals (Sweden)

    Antonios Tribalis

    2016-01-01

    Full Text Available Nickel catalysts are the most popular for steam reforming, however, they have a number of drawbacks, such as high propensity toward coke formation and intolerance to sulfur. In an effort to improve their behavior, a series of Ni-catalysts supported on pure and La-, Ba-, (La+Ba- and Ce-doped γ-alumina has been prepared. The doped supports and the catalysts have been extensively characterized. The catalysts performance was evaluated for steam reforming of n-hexadecane pure or doped with dibenzothiophene as surrogate for sulphur-free or commercial diesel, respectively. The undoped catalyst lost its activity after 1.5 h on stream. Doping of the support with La improved the initial catalyst activity. However, this catalyst was completely deactivated after 2 h on stream. Doping with Ba or La+Ba improved the stability of the catalysts. This improvement is attributed to the increase of the dispersion of the nickel phase, the decrease of the support acidity and the increase of Ni-phase reducibility. The best catalyst of the series doped with La+Ba proved to be sulphur tolerant and stable for more than 160 h on stream. Doping of the support with Ce also improved the catalytic performance of the corresponding catalyst, but more work is needed to explain this behavior.

  9. 镁铝复合氧化物负载铜催化剂上甘油选择性氢解合成丙二醇%Selective Hydrogenolysis of Glycerol to Propylene Glycol on MgO-Al2O3 Dispersed Cu Catalysts

    Institute of Scientific and Technical Information of China (English)

    王帅; 李洋; 刘海超

    2012-01-01

    我们通过乙醇溶液浸渍法合成出了具有高分散度金属Cu的Cu/MgO-Al2O3(Mg/Al原子比=1/1,3/1,4/1)、Cu/MgO和Cu/Al2O3等催化剂.在200℃,6.0 MPa H2和二氧六环溶剂中,这些催化剂高选择性地将甘油氢解为1,2-丙二醇(选择性〉90%),而单位表面Cu原子的甘油转化速率则随催化剂表面碱中心与Cu原子比例的提高而增大.N2O化学吸附-H2程序升温还原实验表明Cu粒子的本征氢解能力不随其负载量以及载体中的Mg/Al原子比发生明显改变,加之碱性MgO-Al2O3载体本身不催化甘油的转化,我们推测在甘油氢解反应中金属Cu粒子与载体界面处的碱中心辅助Cu粒子活化甘油分子的α位C—H键,从而加速甘油脱氢为甘油醛步骤以及甘油氢解反应的进行.CO2程序升温脱附实验以及对甘油氢解反应中Cu/MgO-Al2O3催化剂稳定性的考察结果暗示在甘油氢解反应中起主要作用的碱中心是载体表面上与Mg2+键连的羟基基团(即B碱OH-).这些对甘油氢解反应中金属中心与碱性中心协同作用的认识对进一步理性设计高效的甘油或其它多元醇分子氢解催化剂具有重要指导意义.%Cu/MgO-Al2O3(Mg/Al atomic ratio=1/1,3/1,4/1),Cu/MgO and Cu/Al2O3 catalysts with high Cu dispersions were prepared by an impregnation method using ethanol as solvent instead of water.Compared to water,ethanol as solvent was favorable not only for obtaining the high dispersions of the Cu clusters on the basic oxide supports,but also for retaining the basicity and structures of the supports during the catalyst preparation.The density of the basic sites for the dispersed Cu catalysts increased with increasing the MgO contents in the basic supports.These catalysts catalyzed glycerol hydrogenolysis to propylene glycol with a high selectivity(〉90%),and showed slight deactivation in dioxane at 200 ℃ and 6.0 MPa H2.Their reaction rates normalized by per exposed Cu atom increased

  10. Structure sensitive adsorption of hydrogen on ruthenium and ruthenium-silver catalysts supported on silica

    Energy Technology Data Exchange (ETDEWEB)

    Kumar, N.

    1999-02-12

    Supported metal catalysts typically consist of particles with sizes less than 10 nm, and because of the small crystallite size, low coordination number sites (edges and corners) represent a significant fraction of all surface sites. Furthermore, it has been demonstrated that adsorption rates can be much greater at these low coordination sites than on basal plane sites. What has not been generally appreciated, however, is that preferential adsorption at edge and corner sites may explain the mechanism by which a promoter, or the addition of a second metal to form a bimetallic, can alter the selectivity and rate of reaction. For example, the measurements of hydrogen adsorption onto supported Ru-Ag catalysts show marked decreases in the amount of hydrogen adsorbed relative to the amount adsorbed on Ru catalysts. Although it is known that Ag does not dissociatively adsorb hydrogen, this decrease cannot be explained by a simple one-to-one site blocking mechanism unless Ag preferentially populates edges and corners, thereby reducing the number of Ru edge sites. Indeed, Monte Carlo simulations of Ru-Group IB metal catalysts predict that Group IB metal atoms preferentially populate corner and edge sites of ruthenium crystals. This evidence, taken together, suggests that adsorption occurs preferentially at Ru corner and edge sites, which act as portals onto basal planes. A model based on this portal theory for hydrogen adsorption onto supported ruthenium bimetallic catalysts has been developed using a rate equation approach. Specifically, the model accounts for the following features: (1) preferential adsorption through portals, (2) basal plane site-energy multiplicity, and (3) hydrogen spillover onto the support. A comparison of model predictions with experiment is presented for different concentration of Ag in Ru-Ag catalysts. The portal model of hydrogen adsorption can explain the observed decreased in the amount of hydrogen adsorbed on Ru-Ag catalysts. The model can be

  11. PROGRESS IN PHASE INVERSION EMULSIFICATION FOR EPOXY RESIN WATERBORNE DISPERSIONS

    Institute of Scientific and Technical Information of China (English)

    Zhen-zhong Yang

    2007-01-01

    In this review,our recent work in phase inversion emulsification (PIE)for polymer(especially epoxy resin) waterborne dispersions is summarized.Based on experimental results about PIE process,the physical model is proposed which Can guide the synthesis of the waterborne dispersions such as polymer/nanoparticle composite dispersion.In the presence of a latent curing catalyst,PIE can give a crosslinkable epoxy resin waterborne dispersion.The dispersions can form cured transparent coatings with some unique properties such as UV shielding.They are promising in functional coatings,waterborne resin matrices for composites,and sizing for high performance fibers.

  12. Supported Molten Metal Catalysis. A New Class of Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ravindra Datta; Ajeet Singh; Manuela Serban; Istvan Halasz

    2006-06-02

    We describe a new class of heterogeneous catalysts called supported molten metal catalysis (SMMC), in which molten metal catalysts are dispersed as nanodroplets on the surface of porous supports, allowing much larger active surface area than is possible in conventional contacting techniques for catalytic metals that are molten under reaction conditions, thus greatly enhancing their activity and potential utility. Specific examples of different types of reactions are provided to demonstrate the broad applicability of the technique in designing active, selective, and stable new catalysts. It is shown that dispersing the molten metal on a support in the suggested manner can enhance the rate of a reaction by three to four orders of magnitude as a result of the concomitant increase in the active surface area. New reaction examples include {gamma}-Al{sub 2}O{sub 3} supported molten Te (melting point 450 C) and Ga (MP 30 C) catalysts for bifunctional methylcyclohexane dehydrogenation. These catalysts provide activity similar to conventional Pt-based catalysts for this with better resistance to coking. In addition, results are described for a controlled pore glass supported molten In (MP 157 C) catalyst for the selective catalytic reduction of NO with ethanol in the presence of water, demonstrating activities superior to conventional catalysts for this reaction. A discussion is also provided on the characterization of the active surface area and dispersion of these novel supported catalysts. It is clear based on the results described that the development of new active and selective supported molten metal catalysts for practical applications is entirely plausible.

  13. Carbon supported Cu-Pd nanoparticles as anode catalyst for direct borohydride-hydrogen peroxide fuel cells

    International Nuclear Information System (INIS)

    Carbon supported Cu-Pd bimetallic nanoparticles were prepared by a successive reduction method in aqueous solution and used as anode electrocatalyst for direct borohydride-hydrogen peroxide fuel cell (DBHFC). The physical and electrochemical properties of the as-prepared electrocatalysts are investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD), cyclic voltammetry (CV), chronopotentiometry (CP), linear sweep voltammetry (LSV) and fuel cell test. The results show that the size of the crystallite is around 12.5 nm, the Cu1Pd1/C catalyst presents the highest catalytic activity among all the resultant catalysts, and the DBHFC using Cu1Pd1/C as anode catalyst and Pt mesh (1 cm × 1 cm) as cathode electrode obtains the maximum power density as high as 39.8 mW cm-2 at a discharge current density of 80.1 mA cm-2 at 20 °C

  14. Phytogenic silver, gold, and bimetallic nanoparticles as novel antitubercular agents

    Science.gov (United States)

    Singh, Richa; Nawale, Laxman; Arkile, Manisha; Wadhwani, Sweety; Shedbalkar, Utkarsha; Chopade, Snehal; Sarkar, Dhiman; Chopade, Balu Ananda

    2016-01-01

    Purpose Multi- and extensively drug-resistant tuberculosis (TB) is a global threat to human health. It requires immediate action to seek new antitubercular compounds and devise alternate strategies. Nanomaterials, in the present scenario, have opened new avenues in medicine, diagnosis, and therapeutics. In view of this, the current study aims to determine the efficacy of phytogenic metal nanoparticles to inhibit mycobacteria. Methods Silver (AgNPs), gold (AuNPs), and gold–silver bimetallic (Au–AgNPs) nanoparticles synthesized from medicinal plants, such as Barleria prionitis, Plumbago zeylanica, and Syzygium cumini, were tested against Mycobacterium tuberculosis and M. bovis BCG. In vitro and ex vivo macrophage infection model assays were designed to determine minimum inhibitory concentration (MIC) and half maximal inhibitory concentration of nanoparticles. Microscopic analyses were carried out to demonstrate intracellular uptake of nanoparticles in macrophages. Besides this, biocompatibility, specificity, and selectivity of nanoparticles were also established with respect to human cell lines. Results Au–AgNPs exhibited highest antitubercular activity, with MIC of <2.56 μg/mL, followed by AgNPs. AuNPs did not show such activity at concentrations of up to 100 μg/mL. In vitro and ex vivo macrophage infection model assays revealed the inhibition of both active and dormant stage mycobacteria on exposure to Au–AgNPs. These nanoparticles were capable of entering macrophage cells and exhibited up to 45% cytotoxicity at 30 μg/mL (ten times MIC concentration) after 48 hours. Among these, Au–AgNPs synthesized from S. cumini were found to be more specific toward mycobacteria, with their selectivity index in the range of 94–108. Conclusion This is the first study to report the antimycobacterial activity of AuNPs, AgNPs, and Au–AgNPs synthesized from medicinal plants. Among these, Au–AgNPs from S. cumini showed profound efficiency, specificity, and

  15. Phytogenic silver, gold, and bimetallic nanoparticles as novel antitubercular agents

    Directory of Open Access Journals (Sweden)

    Singh R

    2016-05-01

    Full Text Available Richa Singh,1 Laxman Nawale,2 Manisha Arkile,2 Sweety Wadhwani,1 Utkarsha Shedbalkar,1 Snehal Chopade,1 Dhiman Sarkar,2 Balu Ananda Chopade1,3 1Department of Microbiology, Savitribai Phule Pune University, 2Combichem-Bioresource Center, Organic Chemistry Division, National Chemical Laboratory, Pune, 3Dr Babasaheb Ambedkar Marathwada University, Aurangabad, Maharashtra, India Purpose: Multi- and extensively drug-resistant tuberculosis (TB is a global threat to human health. It requires immediate action to seek new antitubercular compounds and devise alternate strategies. Nanomaterials, in the present scenario, have opened new avenues in medicine, diagnosis, and therapeutics. In view of this, the current study aims to determine the efficacy of phytogenic metal nanoparticles to inhibit mycobacteria. Methods: Silver (AgNPs, gold (AuNPs, and gold–silver bimetallic (Au–AgNPs nanoparticles synthesized from medicinal plants, such as Barleria prionitis, Plumbago zeylanica, and Syzygium cumini, were tested against Mycobacterium tuberculosis and M. bovis BCG. In vitro and ex vivo macrophage infection model assays were designed to determine minimum inhibitory concentration (MIC and half maximal inhibitory concentration of nanoparticles. Microscopic analyses were carried out to demonstrate intracellular uptake of nanoparticles in macrophages. Besides this, biocompatibility, specificity, and selectivity of nanoparticles were also established with respect to human cell lines. Results: Au–AgNPs exhibited highest antitubercular activity, with MIC of <2.56 µg/mL, followed by AgNPs. AuNPs did not show such activity at concentrations of up to 100 µg/mL. In vitro and ex vivo macrophage infection model assays revealed the inhibition of both active and dormant stage mycobacteria on exposure to Au–AgNPs. These nanoparticles were capable of entering macrophage cells and exhibited up to 45% cytotoxicity at 30 µg/mL (ten times MIC concentration after 48 hours

  16. A Highly Efficient Bifunctional Catalyst for Alkaline Air-Electrodes Based on a Ag and Co3O4 Hybrid: RRDE and Online DEMS Insights

    International Nuclear Information System (INIS)

    Enhanced catalytic activity towards oxygen reduction (ORR) and evolution (OER) reactions has been achieved by combination of spinel Co3O4 nanoparticles with Ag particles. Quasi-stationary polarization curves showed that the mixed catalyst, Ag + Co3O4 (10 wt%), outperformed its components. Rotating ring-disc electrode (RRDE) measurements revealed a negligible peroxide species formation and a 4-electron pathway for ORR. A tafel slope of ca. 75 mV dec−1 has been observed. The overpotential for ORR at 10% Co3O4 catalyst is ca. 70 mV lower than that of Ag and only ca. 80 mV higher than that of the commercial Pt catalyst. DEMS technique provided a direct evidence for oxygen evolution at these bimetallic catalysts. This hybrid is therefore one of the (or even the) most active, carbon-free, durable, non-precious ORR and OER electrocatalysts reported to date

  17. Structure, Mobility, and Composition of Transition Metal Catalyst Surfaces. High-Pressure Scanning Tunneling Microscopy and Ambient-Pressure X-ray Photoelectron Spectroscopy Studies

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, Zhongwei [Univ. of California, Berkeley, CA (United States)

    2013-12-06

    Surface structure, mobility, and composition of transition metal catalysts were studied by high-pressure scanning tunneling microscopy (HP-STM) and ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) at high gas pressures. HP-STM makes it possible to determine the atomic or molecular rearrangement at catalyst surfaces, particularly at the low-coordinated active surface sites. AP-XPS monitors changes in elemental composition and chemical states of catalysts in response to variations in gas environments. Stepped Pt and Cu single crystals, the hexagonally reconstructed Pt(100) single crystal, and Pt-based bimetallic nanoparticles with controlled size, shape and composition, were employed as the model catalysts for experiments in this thesis.

  18. Organophilic worm-like ruthenium nanoparticles catalysts by the modification of CTAB on montmorillonite supports.

    Science.gov (United States)

    Zhou, Limei; Qi, Xiaolong; Jiang, Xiaohui; Zhou, Yafen; Fu, Haiyan; Chen, Hua

    2013-02-15

    A supported Ru catalyst was prepared by using cetyltrimethylammonium bromide (CTAB) intercalated montmorillonite as the supporting matrix. The as-prepared Ru catalyst was subsequently characterized by XRD, XPS, N(2) sorption, TEM, and dispersibility measurement. The results showed that the Ru nanoparticles were in the modified montmorillonite interlayers, and the morphology of Ru nanoparticle was worm-like. Moreover, this supported Ru catalyst could be well dispersed in organic solvents such as toluene. The catalyst exhibited high activity and selectivity in the hydrogenation of quinoline even without stirring. PMID:23141762

  19. X-Ray Absorption Spectroscopy of Mo and Ni K-edge of Supported Hydrotreating Catalysts

    Institute of Scientific and Technical Information of China (English)

    DuanAijun; XuChunming; ZhaoZhen; DongPeng

    2005-01-01

    X-ray absorption fine structure (XAFS) and other techniques have been used to characterize Ni-Mo/Al2O3 supported catalysts. The analysis of Mo K-edge spetrum shows that the active species over sulfide catalysts are MoS2-alike and the dispersion of Mo is high at the level of nanometer particles. There may exist some distortion of the local environment of MoS2, which has an influence on the hydrotreating activities of catalysts. Ni K-edge analysis shows that the coordination effects of Ni-Mo favor the dispersion state of active phase and imply a close relationship with catalyst activities.

  20. Studies on Macro—kinetics of Gas Phase Polymerization of Butadiene with Rare—earch Catalyst

    Institute of Scientific and Technical Information of China (English)

    FANGDonyu; SUNJianzhong; 等

    2002-01-01

    The study of the kinetics of gas phase polymerization of butadiene with heterogeneous catalyst based on neodymium(Nd) was carried out.The effects of reaction temperature,reaction pressure,dispersing medium, and types of catalyst on kinetics of polymerization were investigated .A kinetic model with two kinds of active sites was proposed.The results show that the effects of the reaction temperature and the types of dispersing medium and catalyst on the kinetic performance of polymerization are significant,and that the combined model of first and second order decay of active site of catalyst can be used to describe the phenomena.

  1. Renovation and Reuse of Reactive Dyeing Effluent by a Novel Heterogeneous Fenton System Based on Metal Modified PTFE Fibrous Catalyst/H2O2

    Directory of Open Access Journals (Sweden)

    Bing Li

    2013-01-01

    Full Text Available Cu-Fe bimetallic grafted polytetrafluoroethylene (PTFE fiber complexes were prepared and optimized as the novel heterogeneous Fenton catalysts for the degradation of reactive dyes under UV irradiation. Cotton fabrics were dyed with three reactive dyes, namely, Reactive Red 195, Reactive Yellow 145, and Reactive Blue 222, in tap fresh water using exhaustion process. The spent dyeing effluents were then collected and degraded with the optimized Cu-Fe bimetallic grafted PTFE fiber complex/H2O2 system. The treated dyeing effluents were characterized and reused for the dyeing of cotton fabrics through the same process. The effect of reuse process number on quality of the dyed cotton fabrics was examined. The results indicated that the Cu-Fe bimetallic modified PTFE fiber complex with a Cu/Fe molar ratio of 2.87 was found to be the most effective fibrous catalyst, which enhanced complete decolorization of the treated dyeing effluents with H2O2 in 4 h. However, the TOC removal for the treated dyeing effluents was below 80%. The dyeing quality was not affected for three successive cycles. The increase in residual TOC value influences fourth dyeing cycle. Further TOC reduction of the treated effluents is needed for its repeated reuse in more than three dyeing cycles.

  2. Productions of palm oil bio diesel whit heterogeneous basic catalysts compared to conventional homogeneous catalysts

    International Nuclear Information System (INIS)

    The conventional process to produce biodiesel involves the presence of homogeneous basic catalysts. However, these catalysts have disadvantages associated to the need of purification steps, which increase the cost of the final product and generate pollution problems caused by the effluents. This paper compares different homogeneous and heterogeneous catalysts for the biodiesel production from palm oil. For this, heterogeneous catalysts supported on alumina were prepared and characterized by nitrogen adsorption, scanning electron microscopy, energy dispersive X ray spectroscopy and X ray diffraction. Transesterification of palm oil with methanol was accomplished at 60 celsius degrade and one hour, varying methanol/oil ratio, the type of catalyst and its concentration. Yields of the reaction and purity of the so obtained biodiesel were evaluated. Comparing the catalysts performance, based on the amount, was found that sodium methoxide (CH3 ONa) and potassium carbonate supported on alumina (K2 CO3 /Al2O3) were the catalysts that give the higher purity of biodiesel (96.8 and 95.85% respectively). When was determined the active site quality, by dividing the performance by each mole of active sites, it was found that calcined Na2SO4 /Al2O3 has the most active sites.

  3. Thermo-mechanical efficiency of the bimetallic strip heat engine at the macro-scale and micro-scale

    International Nuclear Information System (INIS)

    Bimetallic strip heat engines are energy harvesters that exploit the thermo-mechanical properties of bistable bimetallic membranes to convert heat into mechanical energy. They thus represent a solution to transform low-grade heat into electrical energy if the bimetallic membrane is coupled with an electro-mechanical transducer. The simplicity of these devices allows us to consider their miniaturization using MEMS fabrication techniques. In order to design and optimize these devices at the macro-scale and micro-scale, this article proposes an explanation of the origin of the thermal snap-through by giving the expressions of the constitutive equations of composite beams. This allows us to evaluate the capability of bimetallic strips to convert heat into mechanical energy whatever their size is, and to give the theoretical thermo-mechanical efficiencies which can be obtained with these harvesters. (paper)

  4. Tuning the surface electronic structure of a Pt3Ti(111) electro catalyst.

    Science.gov (United States)

    Paßens, M; Caciuc, V; Atodiresei, N; Moors, M; Blügel, S; Waser, R; Karthäuser, S

    2016-07-21

    Increasing the efficiency and stability of bimetallic electro catalysts is particularly important for future clean energy technologies. However, the relationship between the surface termination of these alloys and their catalytic activity is poorly understood. Therefore, we report on fundamental UHV-SPM, LEED, and DFT calculations of the Pt3Ti(111) single crystal surface. Using voltage dependent imaging the surface termination of Pt3Ti(111) was studied with atomic resolution. Combining these images with simulated STM maps based on ab initio DFT calculations allowed us to identify the three upper layers of the Pt3Ti(111) single crystal and their influence upon the surface electronic structure. Our results show that small changes in the composition of the second and third atomic layer are of significant influence upon the surface electronic structure of the Pt3Ti electro catalyst. Furthermore, we provide relevant insights into the dependence of the surface termination on the preparation conditions. PMID:26865393

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. Self-assembly of noble metal monolayers on transition metal carbide nanoparticle catalysts.

    Science.gov (United States)

    Hunt, Sean T; Milina, Maria; Alba-Rubio, Ana C; Hendon, Christopher H; Dumesic, James A; Román-Leshkov, Yuriy

    2016-05-20

    We demonstrated the self-assembly of transition metal carbide nanoparticles coated with atomically thin noble metal monolayers by carburizing mixtures of noble metal salts and transition metal oxides encapsulated in removable silica templates. This approach allows for control of the final core-shell architecture, including particle size, monolayer coverage, and heterometallic composition. Carbon-supported Ti(0.1)W(0.9)C nanoparticles coated with Pt or bimetallic PtRu monolayers exhibited enhanced resistance to sintering and CO poisoning, achieving an order of magnitude increase in specific activity over commercial catalysts for methanol electrooxidation after 10,000 cycles. These core-shell materials provide a new direction to reduce the loading, enhance the activity, and increase the stability of noble metal catalysts.

  7. Pd Close Coupled Catalyst

    Institute of Scientific and Technical Information of China (English)

    Zhong Hua SHI; Mao Chu GONG; Yao Qiang CHEN

    2006-01-01

    A catalyst comprised novel high surface area alumina support was prepared to control emission of automobiles. The results showed that prepared catalyst could satisfy the requirements of a high performance close coupled catalyst for its good catalytic activity at low temperature and good stability at high temperature.

  8. Coating powdered copper catalyst with yttria sol

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Kuan-Ying [Department of Chemical and Engineering and Materials Science, Yuan Ze University, Chung-Li, Taiwan (China); Fuel Cell Center, Yuan Ze University, Chung-Li, Taiwan (China); Shen, Chia-Chieh, E-mail: ccshen@saturn.yzu.edu.tw [Fuel Cell Center, Yuan Ze University, Chung-Li, Taiwan (China); Department of Mechanical Engineering, Yuan Ze University, Chung-Li, Taiwan (China); Graduate School of Renewable Energy Engineering, Yuan Ze University, Chung-Li, Taiwan (China); Lee, Chi-Yuan; Lee, Shuo-Jen [Fuel Cell Center, Yuan Ze University, Chung-Li, Taiwan (China); Department of Mechanical Engineering, Yuan Ze University, Chung-Li, Taiwan (China); Graduate School of Renewable Energy Engineering, Yuan Ze University, Chung-Li, Taiwan (China); Leu, Chih-Hsing [Energy and Environment Research Laboratories, Industrial Technology Research Institute, Hsinchu, Taiwan (China); Wang, Jung-Hui [Fuel Cell Center, Yuan Ze University, Chung-Li, Taiwan (China); Yeh, Chuin-Tih [Department of Chemical and Engineering and Materials Science, Yuan Ze University, Chung-Li, Taiwan (China); Fuel Cell Center, Yuan Ze University, Chung-Li, Taiwan (China)

    2011-07-15

    Research highlights: {yields} The neutral Y{sub 2}O{sub 3} sol is an effective binder for coating powders of CuZnAl catalyst. {yields} A particle size ratio of 15 for catalyst to binder is suggested for stable coating. {yields} Sufficient stirring is an important step in the catalyst slurry preparation. - Abstract: A commercial Y{sub 2}O{sub 3} sol was tested as a binder for coating CuZnAl catalyst powder onto microchannels of a stainless steel plate (SSP). Coated plates were used to fabricate microchannel reactors that generate hydrogen via the steam reforming of methanol (SRM). Washcoating slurries were prepared by suspending catalyst powders into the sol. Slurry parameters, such as solid content, binder content, pH value, and stir time, were optimized to achieve a stable catalyst coating and good SRM performance. The expected stable coating could be obtained from neutral (pH 7) Y{sub 2}O{sub 3} slurry that is required for a negligible dissolution of the copper component of the catalyst. The experimental coating stability generally improved with the slurry stir time. Observed improvements were attributed to a dispersion of catalyst powders in the slurry through a two-step mechanism: the mechanical disassembly of agglomerated CuZnAl powders into primary particles, and the repelling of dissembled particles through adsorption of positively charged Y{sub 2}O{sub 3} binders. A reasonable reaction temperature of 280 deg. C was found for 95% conversion of methanol in SRM from the resulted microchannel reactors. A low CO fraction of 0.3% was also found in the hydrogen-rich gas reformed.

  9. Synthesis, characterization and hydrotreating performance of supported tungsten phosphide catalysts

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    Supported tungsten phosphide catalysts were prepared by temperature-programmed reduction of their precursors (supported phospho-tungstate catalysts) in H2 and characterized by X-ray diffraction (XRD),BET,temperature-programmed desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS).The reduction-phosphiding processes of the precursors were investigated by thermogravimetry and differential thermal analysis (TG-DTA) and the suitable phosphiding temperatures were defined.The hydrodesulfurization (HDS) and hydrodenitrogenation (HDN) activities of the catalysts were tested by using thiophene,pyridine,dibenzothiophene,carbazole and diesel oil as the feed-stock.The TiO2,γ-Al2O3 supports and the Ni,Co promoters could remarkably increase and stabilize active W species on the catalyst surface.A suitable amount of Ni (3%-5%),Co (5%-7%) and V (1%-3%) could increase dispersivity of the W species and the BET surface area of the WP/γ-Al2O3 catalyst.The WP/γ-Al2O3 catalyst possesses much higher thiophene HDS and carbazole HDN activities and the WP/TiO2 catalyst has much higher dibenzothiophene (DBT) HDS and pyridine HDN activities.The Ni,Co and V can obviously promote the HDS activity and inhibit the HDN activity of the WP/γ-Al2O3 catalyst.The G-Ni5 catalyst possesses a much higher diesel oil HDS activity than the sulphided industrial NiW/γ-Al2O3 catalyst.In general,a support or promoter in the WP/γ-Al2O3 catalyst which can increase the amount and dispersivity of the active W species can promote its HDS and HDN activities.

  10. Tuning the surface electronic structure of a Pt3Ti(111) electro catalyst

    Science.gov (United States)

    Paßens, M.; Caciuc, V.; Atodiresei, N.; Moors, M.; Blügel, S.; Waser, R.; Karthäuser, S.

    2016-07-01

    Increasing the efficiency and stability of bimetallic electro catalysts is particularly important for future clean energy technologies. However, the relationship between the surface termination of these alloys and their catalytic activity is poorly understood. Therefore, we report on fundamental UHV-SPM, LEED, and DFT calculations of the Pt3Ti(111) single crystal surface. Using voltage dependent imaging the surface termination of Pt3Ti(111) was studied with atomic resolution. Combining these images with simulated STM maps based on ab initio DFT calculations allowed us to identify the three upper layers of the Pt3Ti(111) single crystal and their influence upon the surface electronic structure. Our results show that small changes in the composition of the second and third atomic layer are of significant influence upon the surface electronic structure of the Pt3Ti electro catalyst. Furthermore, we provide relevant insights into the dependence of the surface termination on the preparation conditions.Increasing the efficiency and stability of bimetallic electro catalysts is particularly important for future clean energy technologies. However, the relationship between the surface termination of these alloys and their catalytic activity is poorly understood. Therefore, we report on fundamental UHV-SPM, LEED, and DFT calculations of the Pt3Ti(111) single crystal surface. Using voltage dependent imaging the surface termination of Pt3Ti(111) was studied with atomic resolution. Combining these images with simulated STM maps based on ab initio DFT calculations allowed us to identify the three upper layers of the Pt3Ti(111) single crystal and their influence upon the surface electronic structure. Our results show that small changes in the composition of the second and third atomic layer are of significant influence upon the surface electronic structure of the Pt3Ti electro catalyst. Furthermore, we provide relevant insights into the dependence of the surface termination on the

  11. Dechlorination of disinfection by-product monochloroacetic acid in drinking water by nanoscale palladized iron bimetallic particle

    Institute of Scientific and Technical Information of China (English)

    CHEN Chao; WANG Xiangyu; CHANG Ying; LIU Huiling

    2008-01-01

    Nanoscale palladized iron (Pd/Fe) bimetallic particles were prepared by reductive deposition method. The particles were characterized by X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscope (SEM), transmission electron microscope (TEM), and Brunauer-Emmett-Teller-nitrogen (BET-N2) method. Data obtained from those methods indicated that nanoscale Pd/Fe bimetallic particles contained α-Fe0. Detected Pd to Fe ratio by weight (PFRW) was close to theoretical PFRW. Spherical granules with diameter of 47±11.5 nm connected with one another to form chains and the chains composed nanoscale Pd/Fe bimetallic particles. Specific surface area of particles was 51 m2/g. Factors, such as species of reductants, PFRW, dose of nanoscale Pd/Fe bimetallic particles added into solutions, solution initial pH, and a variety of solvents were studied. Dechlorination effect of monochloroacetic acid (MCAA) by different reductants followed the trend: nanoscale Pd/Fe bimetallic particles of 0.182% PFRW > nanoscale Fe > reductive Fe. When PFRW was lower than 0.083%, increasing PFRW would increase dechlorination efficiency (DE) of MCAA. But when the PFRW was higher than 0.083%, increasing PFRW caused decrease in DE. Adding more nanoscale Pd/Fe bimetallic particles to solution would enhance DE. The DE of MCAA decreased as initial pH of solution increased.

  12. Surface plasmon resonance sensing of a biomarker of Alzheimer disease in an intensity measurement mode with a bimetallic chip

    Science.gov (United States)

    Kim, Hyung Jin; Sohn, Young-Soo; Kim, Chang-duk; Jang, Dae-ho

    2016-09-01

    A surface plasmon resonance (SPR) sensor system with a bimetallic chip has been utilized to sense the very low concentration of amyloid-beta (A β)(1-42) by measurement of the reflectance variation. The bimetallic chip was comprised of Au (10 nm) and Ag (40 nm) on Cr (2 nm)-coated BK-7 glass substrate. Protein A was used to efficiently immobilize the antibody of A β(1-42) on the surface of the bimetallic chip. The reflectance curve of the bimetallic chip represented a narrower linewidth compared to that of the conventional gold (Au) chip. The SPR sensor using the bimetallic chip in the intensity interrogation mode acquired the response of A β(1-42) at concentrations of 250, 500, 750 and 1,000 pg/ml. The calibration plot showed a linear relationship between the mean reflectance variation and the A β(1-42) concentration. The results proved that the SPR sensor system with the bimetallic chip in the intensity interrogation mode can successfully detect various concentrations of A β(1-42), including critical concentration, to help diagnose Alzheimer's disease.

  13. Pt-Re-Sn/Al{sub 2}O{sub 3} trimetallic catalysts for naphtha reforming processes without presulfiding step

    Energy Technology Data Exchange (ETDEWEB)

    Mazzieri, V.A.; Grau, J.M.; Vera, C.R.; Yori, J.C.; Parera, J.M.; Pieck, C.L. [Instituto de Investigaciones en Catalisis y Petroquimica, INCAPE, FIQ-UNL, CONICET, Santiago del Estero 2654, 3000 Santa Fe (Argentina)

    2005-12-12

    The n-heptane reforming and the cyclopentane hydrogenolysis reactions over noble metal monometallic catalysts (0.3% Pt), bimetallic catalysts (0.3% Pt, x% Re, x=0.1, 0.3, 0.9 and 2.0, sulfided) and trimetallic catalysts (0.3% Pt, 0.3% Re, y% Sn, y=0.1, 0.3, 0.6 and 0.9, unsulfided) were studied. The metal function was supported over a chlorided {gamma}-alumina that provided the acid function. The reforming of n-heptane was performed at 450{sup o}C, molar ratio H{sub 2}/n-C{sub 7}=4 and WHSV=7.3 while the hydrogenolysis of cyclopentane was performed at 350{sup o}C, H{sub 2}/CP=20 and WHSV=2.4. The sulfided 0.3Pt-0.3Re catalyst (with 0.06% S) was found to be the best performing bimetallic one. It had a great stability, typical of this kind of catalysts, and also produced a reformate with a high iso-heptanes/toluene ratio. This is advantageous for fulfilling the current environmental regulations that limit the amount of aromatic hydrocarbons in reformulated gasolines. The best trimetallic catalyst was 0.3Pt-0.3Re-0.6Sn which had a similar activity and selectivity as sulfided 0.3Pt-0.3Re, though it displayed a higher stability and a lower hydrogenolysis activity, without the need of presulfidation. Tin affected the metal and acid functions of the catalyst simultaneously and inhibited them to such different degrees that a very convenient metal/acid activity ratio was obtained, resulting in an improvement of the activity, selectivity and stability of the catalysts. It can be concluded that it is possible to prepare trimetallic naphtha reforming catalysts of the Pt-Re-Sn kind with a better performance than conventional sulfided Pt-Re catalysts and with the additional advantage that they do not need complicated sulfiding pretreatments. This simplifies the commercial operation of the reformer unit and enables the application of this catalyst to continuously operated processes.

  14. Final Technical Report - High-Performance, Oxide-Dispersion-Strengthened Tubes for Production of Ethylene adn Other Industrial Chemicals

    Energy Technology Data Exchange (ETDEWEB)

    McKimpson, Marvin G.

    2006-04-06

    This project was undertaken by Michigan Technological University and Special Metals Corporation to develop creep-resistant, coking-resistant oxide-dispersion-strengthened (ODS) tubes for use in industrial-scale ethylene pyrolysis and steam methane reforming operations. Ethylene pyrolysis tubes are exposed to some of the most severe service conditions for metallic materials found anywhere in the chemical process industries, including elevated temperatures, oxidizing atmospheres and high carbon potentials. During service, hard deposits of carbon (coke) build up on the inner wall of the tube, reducing heat transfer and restricting the flow of the hydrocarbon feedstocks. About every 20 to 60 days, the reactor must be taken off-line and decoked by burning out the accumulated carbon. This decoking costs on the order of $9 million per year per ethylene plant, accelerates tube degradation, and requires that tubes be replaced about every 5 years. The technology developed under this program seeks to reduce the energy and economic cost of coking by creating novel bimetallic tubes offering a combination of improved coking resistance, creep resistance and fabricability not available in current single-alloy tubes. The inner core of this tube consists of Incoloy(R) MA956, a commercial ferritic Fe-Cr-Al alloy offering a 50% reduction in coke buildup combined with improved carburization resistance. The outer sheath consists of a new material - oxide dispersion strengthened (ODS) Alloy 803(R) developed under the program. This new alloy retains the good fireside environmental resistance of Alloy 803, a commercial wrought alloy currently used for ethylene production, and provides an austenitic casing to alleviate the inherently-limited fabricability of the ferritic Incoloy(R) MA956 core. To provide mechanical compatibility between the two alloys and maximize creep resistance of the bimetallic tube, both the inner Incoloy(R) MA956 and the outer ODS Alloy 803 are oxide dispersion

  15. A hydrophobic catalyst for recombining H2/D2 and O2 in nuclear reactors

    International Nuclear Information System (INIS)

    A catalyst is developed for efficient recombination of hydrogen and oxygen in presence of water vapor and without requirement of an external heat source. The catalyst, comprising of finely dispersed platinum on a large area polymeric sheet, is hydrophobic in nature and is therefore resistant to water poisoning. The recombination reaction is exothermic which results in the rise of catalyst temperature and hence in its high and automatically sustained catalytic activity. In order to prevent catalyst overheating, the catalyst sheet is sandwiched between the two perforated metallic plates, which help in maintaining the catalyst panel at an isothermal temperature below its melting point. The performance of this catalyst, evaluated on both bench and pilot plant scale, is found to be long lasting. Due to the flexible nature of this catalyst material, different convenient recombiner designs may be envisaged for use in nuclear reactors, either for reaction of radiolytically generated hydrogen and oxygen or for mitigation of hydrogen under severe accident conditions

  16. Study of Carbon Nanotube Supported Co-Mo Selective Hydrodesulphurization Catalysts for Fluid Catalytic Cracking Gasoline

    Institute of Scientific and Technical Information of China (English)

    Wenkui Yin; Mei Li; Hongyan Shang; Chenguang Liu; Fei Wei

    2005-01-01

    In this paper,carbon nanotube supported Co-Mo catalysts for selective hydrodesulphurization (HDS) of fluid catalytic cracking (FCC) gasoline were studied,using di-isobutylene,cyclohexene,1-octene and thiophene as model compounds to simulate FCC gasoline. The results show that the Co-Mo/CNT has very high HDS activity and HDS/hydrogenation selectivity comparing with the Co-Mo/γ-Al2O3 and Co-Mo/AC catalyst systems. The saturation ratio of cyclohexene was lower than 50%,and the saturation ratio of 1,3-di-isobutylene lower than 60% for the Co-Mo/CNT catalysts. Co/Mo atomic ratio was found to be one of the most important key factors in influencing the hydrogenation selectivity and HDS activity,and the most suitable Co/Mo atomic ratio was 0.4. Co/CNT and Mo/CNT mono-metallic catalysts showed lower HDS activity and selectivity than the Co-Mo/CNT bi-metallic catalysts.

  17. Surface coatings and catalyst production by electrodeposition

    Science.gov (United States)

    May, Chester B.; Riley, Clyde; Coble, H. Dwain; Loo, Boon H.

    1987-01-01

    Electrodeposition and electrocodeposition in low gravity are discussed. The goal is to provide a better understanding of the role of convection and buoyancy in the mechanisms of formation of some electrodeposited surfaces, fluid flow in the vicinity of electrodepositing surfaces, the influence of a moving medium upon codeposition, the effect of gravity upon the dispersion (coagulation) of neutral particles that are desired for codeposition and preparation of improved surface coatings and metal catalysts.

  18. Autothermal reforming of propane over Ni-based hydrotalcite catalysts.

    Science.gov (United States)

    Park, Sun-Young; Kim, Jong-Ho; Moon, Dong-Ju; Park, Nam-Cook; Kim, Young-Chul

    2010-05-01

    Ni-based hydrotalcite catalysts were investigated for ATR of propane in a fixed-bed flow reactor. The reactions were carried out with a H2O/C/O2 stream ratio of 3/1/0.73 at temperatures ranging from 300 to 700 degrees C. The solvents used in the manufacture of Ni-based catalysts noble metal/Ni/MgAl catalysts or substituted active material were changed in order to decrease the level of catalyst deactivation. The use of a mixture of ethanol and water during the formation of the Pd-Ni/MgAl catalyst produced a higher hydrogen yield than that using water only. In addition, the use of acetone in the synthesis of Ru-Ni/MgAl catalyst produced a higher hydrogen yield than using water only. This shows that the solvents used for the noble metals affect the degree of dispersion and particle size of the nickel and prevented carbon deposition resulting in the enhanced hydrogen selectivity and catalyst activity. Active metals were substituted during the preparation of hydrotalcite catalysts. Among the catalysts prepared with various ratio (Ni:Fe) tested at high temperature, the ratio, Ni:Fe = 75:25, showed best performance. There was less sintering of Ni particles due to substitution of the active metal at the optimal ratio. PMID:20358916

  19. A Phenomenological Study on the Synergistic Role of Precious Metals in the Steam Reforming of Logistic Fuels on Bimetal-Supported Catalysts

    Directory of Open Access Journals (Sweden)

    Abdul-Majeed Azad

    2011-01-01

    Full Text Available Fuel processors are required to convert sulfur-laden logistic fuels into hydrogen-rich reformate and deliver to the fuel cell stack with little or no sulfur. Since sulfur poisons and deactivates the reforming catalyst, robust sulfur-tolerant catalysts ought to be developed. In this paper, the development, characterization and evaluation of a series of reforming catalysts containing two noble metals (with total metal loading not exceeding 1 weight percent supported on nanoscale ceria for the steam-reforming of kerosene is reported. Due to inherent synergy, a bimetallic catalyst is superior to its monometallic analog, for the same level of loading. The choice of noble metal combination in the bimetallic formulations plays a vital and meaningful role in their performance. Presence of ruthenium and/or rhodium in formulations containing palladium showed improved sulfur tolerance and significant enhancement in their catalytic activity and stability. Rhodium was responsible for higher hydrogen yields in the logistic fuel reformate. Duration of steady hydrogen production was higher in the case of RhPd (75 h than for RuPd (68 h; hydrogen generation was stable over the longest period (88 h with RuRh containing no Pd. A mechanistic correlation between the characteristic role of precious metals in the presence of each other is discussed.

  20. Role of clay as catalyst in Friedel–Craft alkylation

    Indian Academy of Sciences (India)

    Tanushree Choudhury; Nirendra M Misra

    2011-10-01

    Solid acids have become increasingly important for many liquid-phase industrial reactions these days. Montmorillonite clays (2:1 clay mineral) have been used as efficient solid acid catalysts for a number of organic and liquid phase reactions and offer several advantages over classic acids. Tailor made catalysts can be prepared from clays by suitably adjusting their acidity and surface area by acid activation. In the present work, preparation, characterization and performance of Pt (II) clays, Cu (II) clays, acid clay, and sol–gel hybrids of Cu (II) clays as solid catalysts in a test Friedel–Craft alkylation reaction of benzyl chloride with toluene using differential scanning calorimeter (DSC) are reported. Product formation has been analysed by FTIR spectroscopy. The main objective of this work is to show how clay as a solid catalyst affects reaction rates and activation energies. Acidity and dispersion of solid catalysts are twomain factors which govern a catalysis reaction. Kinetic parameter analysis and XRD studies confirm that acid Pt (II) clay and Pt (II) clay dispersed by natural dispersants aremore effective catalysts. In contrast to the reactions using AlCl3, the experimental conditions are non-polluting and the final work up does not require any aqueous treatment.

  1. Dispersed Indeterminacy

    CERN Document Server

    Fayngold, Moses

    2013-01-01

    A state of a single particle can be represented by a quantum blob in the corresponding phase space, or a patch (granule) in its 2-D subspace. Its area is frequently stated to be no less than, implying that such a granule is an indivisible quantum of the 2-D phase space. But this is generally not true, as is evident, for instance, from representation of some states in the basis of innately discrete observables like angular momentum. Here we consider some dispersed states involving the evanescent waves different from that in the total internal reflection. Such states are represented by a set of separated granules with individual areas, but with the total indeterminacy . An idealized model has a discrete Wigner function and is described by a superposition of eigenstates with eigenvalues and forming an infinite periodic array of dots on the phase plane. The question about the total indeterminacy in such state is discussed. We argue that the eigenstates corresponding to the considered EW cannot be singled out by a...

  2. Ethylbenzene dehydrogenation over Mg3Fe0.5−xCoxAl0.5 catalysts derived from hydrotalcites: Comparison with Mg3Fe0.5−yNiyAl0.5 catalysts

    KAUST Repository

    Atanda, Luqman A.

    2011-04-01

    A series of Mg3Fe0.5-xCoxAl0.5 (x = 0-0.5) catalysts were prepared from hydrotalcite precursors and their activities in the dehydrogenation of ethylbenzene were compared with those of a series of Mg3Fe0.5-yNiyAl0.5 (y = 0-0.5) catalysts also derived from hydrotalcite. The hydrotalcites prepared by co-precipitation were calcined at 550 °C to the mixed oxides with a high surface area of 150-240m2gcat-1; they were composed of Mg(Fe,Me,Al)O periclase and Mg(Me)(Fe,Al)2O4 spinel (Me = Co or Ni). Bimetallic Fe3+-Co2+ system showed a synergy, i.e., an increase in the activity, whereas Fe3+-Ni2+ bimetallic system showed no synergy. The high styrene yield was obtained on Mg 3Fe0.1Co0.4Al0.5; however, a large substitution of Fe3+ with Co2+ caused a decrease in styrene selectivity along with coking on the catalysts, due to an isolation of CoOx on the catalyst surface. The highest yield as well as the highest selectivity for styrene production was obtained at x = 0.25 at time on stream of 30 min. The coprecipitation at pH = 10.0 and the composition of Mg3Fe0.25Co0.25Al0.5 were the best for preparing the active catalyst. This is partly due to the formation of a good hydrotalcite structure. On this catalyst, the active Fe3+ species was reduced at a low temperature by the Fe3+-Co2+ bimetal formation, leading to a high activity. Simultaneously, the amount of reducible Fe3+ was the smallest, resulting in a high stability of the active Fe3+ species. It is likely that the dehydrogenation was catalyzed by the reduction-oxidation between Fe3+ and Fe2+ and that Co2+ assisted the reduction-oxidation by forming Fe 3+-Co2+ (1/1) bimetallic active species. © 2011 Elsevier B.V. All rights reserved.

  3. Uncovering the Stabilization Mechanism in Bimetallic Ruthenium-Iridium Anodes for Proton Exchange Membrane Electrolyzers.

    Science.gov (United States)

    Saveleva, Viktoriia A; Wang, Li; Luo, Wen; Zafeiratos, Spyridon; Ulhaq-Bouillet, Corinne; Gago, Aldo S; Friedrich, K Andreas; Savinova, Elena R

    2016-08-18

    Proton exchange membrane (PEM) electrolyzers are attracting an increasing attention as a promising technology for the renewable electricity storage. In this work, near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) is applied for in situ monitoring of the surface state of membrane electrode assemblies with RuO2 and bimetallic Ir0.7Ru0.3O2 anodes during water splitting. We demonstrate that Ir protects Ru from the formation of an unstable hydrous Ru(IV) oxide thereby rendering bimetallic Ru-Ir oxide electrodes with higher corrosion resistance. We further show that the water splitting occurs through a surface Ru(VIII) intermediate, and, contrary to common opinion, the presence of Ir does not hinder its formation. PMID:27477824

  4. Kinetic Study on the Formation of Bimetallic Core-Shell Nanoparticles via Microemulsions

    Directory of Open Access Journals (Sweden)

    Concha Tojo

    2014-11-01

    Full Text Available Computer calculations were carried out to determine the reaction rates and the mean structure of bimetallic nanoparticles prepared via a microemulsion route. The rates of reaction of each metal were calculated for a particular microemulsion composition (fixed intermicellar exchange rate and varying reduction rate ratios between both metal and metal salt concentration inside the micelles. Model predictions show that, even in the case of a very small difference in reduction potential of both metals, the formation of an external shell in a bimetallic nanoparticle is possible if a large reactant concentration is used. The modification of metal arrangement with concentration was analyzed from a mechanistic point of view, and proved to be due to the different impact of confinement on each metal: the reaction rate of the faster metal is only controlled by the intermicellar exchange rate but the slower metal is also affected by a cage-like effect.

  5. Synthesis and Characterization of Optically Active Fractal Seed Mediated Silver Nickel Bimetallic Nanoparticles

    Directory of Open Access Journals (Sweden)

    Joseph Adeyemi Adekoya

    2014-01-01

    Full Text Available The synthesis of new seed mediated AgNi allied bimetallic nanocomposites was successfully carried out by the successive reduction of the metal ions in diethylene glycol, ethylene glycol, glycerol, and pentaerythritol solutions, with concomitant precipitation of Ag/Ni bimetal sols. The optical measurement revealed the existence of distinct band edge with surface plasmon resonance (SPR in the region of 400–425 nm and excitonic emission with maximum peak at 382 nm which were reminiscent of cluster-in-cluster surface enriched bimetallic silver-nickel sols. The morphological characterization by transmission electron microscopy, high resolution transmission electron microscopy, and X-ray diffraction analyses complimented by surface scan using X-ray photoelectron spectroscopy strongly supported the formation of intimately alloyed face-centered silver/nickel nanoclusters.

  6. Stability of the Shallow Axisymmetric Parabolic-Conic Bimetallic Shell by Nonlinear Theory

    OpenAIRE

    M. Jakomin; F. Kosel

    2011-01-01

    In this contribution, we discuss the stress, deformation, and snap-through conditions of thin, axi-symmetric, shallow bimetallic shells of so-called parabolic-conic and plate-parabolic type shells loaded by thermal loading. According to the theory of the third order that takes into account the balance of forces on a deformed body, we present a model with a mathematical description of the system geometry, displacements, stress, and thermoelastic deformations. The equations are based on the lar...

  7. Ultrasonic double-wall shadow control of laminations in bimetallic tubes

    International Nuclear Information System (INIS)

    Nondestructive method of control of laminations in 10, 12KhN3A and 0Kh18N10T steel tube plated with copper, bronze or nickel has been developed. The method is based on the excitation and reception of longitudinal ultrasonic oscillations passing through two walls of the bimetallic tube filled with water. The method sensitivity depends on the damping in the tube wall, difference in wall thickness, ovality and surface roughness

  8. Tuning the porosity of bimetallic nanostructures by a soft templating approach

    OpenAIRE

    Lehoux, Anaïs; Ramos, Laurence; Beaunier, Patricia; Uribe, Daniel Bahena; Dieudonné, Philippe; Audonnet, Fabrice; Etcheberry, Arnaud; José-Yacaman, Miguel; Remita, Hynd

    2012-01-01

    We use hexagonal mesophases made of oil-swollen surfactant-stabilized tubes arranged on a triangular lattice in water and doped with metallic salts as templates for the radiolytic synthesis of nanostructures. The nanostructures formed in this type of soft matrix are bimetallic palladium-platinum porous nanoballs composed of 3D-connected nanowires, of typical thickness 2.5 nm, forming hexagonal cells. We demonstrate using electron microscopy and small-angle X-ray scattering that the pore size ...

  9. Electrochemical synthesis of fractal bimetallic Cu/Ag nanodendrites for efficient surface enhanced Raman spectroscopy.

    Science.gov (United States)

    Li, Da; Liu, Jingquan; Wang, Hongbin; Barrow, Colin J; Yang, Wenrong

    2016-09-21

    Here, we for the first time synthesized bimetallic Cu/Ag dendrites on graphene paper (Cu/Ag@G) using a facile electrodeposition method to achieve efficient SERS enhancement. Cu/Ag@G combined the electromagnetic enhancement of Cu/Ag dendrites and the chemical enhancement of graphene. SERS was ascribed to the rough metal surface, the synergistic effect of copper and silver nanostructures and the charge transfer between graphene and the molecules. PMID:27522964

  10. Development of hydrophobic catalysts for deuterium exchange between hydrogen and water (Preprint No. CI-4)

    International Nuclear Information System (INIS)

    This paper deals with the salient features of catalyst development work carried out in Chemistry Division for isotopic exchange between hydrogen and water. The catalysts with noble metals dispersed over PTFE coated supports (such as activated charcoal, zeolites etc) or over polymer supports (such as polyester, nylon) are prepared. Catalysts with Pt dispersed over PTFE coated charcoal are found to be highly active and resistant to water poisoning. These catalysts maintained their physical form and catalytic property at temperatures upto 200degC and performed better than the catalysts prepared by reported method, viz, supporting Pt on charcoal blended with teflon powder. A laboratory scale plant is set up to evaluate catalyst activity under continuous countercurrent flow of hydrogen and water under experimental conditions of elevated temperatures (∼150degC) and pressures (10 atm). (author). 5 refs., 3 figs

  11. NANOPARTICLES OF TUNGSTEN AS LOW-COST MONOMETALLIC CATALYST FOR SELECTIVE HYDROGENATION OF 3-HEXYNE

    Directory of Open Access Journals (Sweden)

    María Juliana Maccarrone

    2016-01-01

    (5 wt% Pd. The alumina supported tungsten catalysts are low-cost potential replacements for the Lindlar industrial catalyst. These catalysts could also be used for preparing bimetallic W-Pd catalysts for selective hydrogenation of terminal and non-terminal alkynes.

  12. Developments of modeling tools for the ultrasonic propagation in bimetallic welds

    International Nuclear Information System (INIS)

    This study fits into the field of ultrasonic non-destructive evaluation. It consists in the development of a dynamic ray tracing model to simulate the ultrasonic propagation in bimetallic welds. The approach has been organised in three steps. First of all, an image processing technique has been developed and applied on the macro-graphs of the weld in order to obtain a smooth cartography of the crystallographic orientation. These images are used as input data for a dynamic ray tracing model adapted to the study of anisotropic and inhomogeneous media such as bimetallic welds. Based on a kinematic and a dynamic ray tracing model, usually used in geophysics, it allows the evaluation of ray trajectories between a source point and an observation point, and the computation of the ultrasonic amplitude through the geometrical spreading of an elementary ray tube. This model has been validated in 2D by comparison of the results with a hybrid semi-analytical/finite elements code, then in 3D thanks to experimental results made on the mock-ups of the studied bimetallic welds. (author)

  13. Synthesis, Study, and Discrete Dipole Approximation Simulation of Ag-Au Bimetallic Nanostructures.

    Science.gov (United States)

    Hu, Yang; Zhang, An-Qi; Li, Hui-Jun; Qian, Dong-Jin; Chen, Meng

    2016-12-01

    Water-soluble Ag-Au bimetallic nanostructures were prepared via co-reduction and seed-mediated growth routes employing poly-(4-styrenesulfonic acid-co-maleic acid) (PSSMA) as both a reductant and a stabilizer. Ag-Au alloy nanoparticles were obtained by the co-reduction of AgNO3 and HAuCl4, while Ag-Au core-shell nanostructures were prepared through seed-mediated growth using PSSMA-Au nanoparticle seeds in a heated AgNO3 solution. The optical properties of the Ag-Au alloy and core-shell nanostructures were studied, and the growth mechanism of the bimetallic nanoparticles was investigated. Plasmon resonance bands in the range 422 to 517 nm were observed for Ag-Au alloy nanoparticles, while two plasmon resonances were found in the Ag-Au core-shell nanostructures. Furthermore, discrete dipole approximation theoretical simulation was used to assess the optical property differences between the Ag-Au alloy and core-shell nanostructures. Composition and morphology studies confirmed that the synthesized materials were Ag-Au bimetallic nanostructures. PMID:27094823

  14. Microstructure and mechanical properties of carbon steel A210-superalloy Sanicro 28 bimetallic tubes

    Energy Technology Data Exchange (ETDEWEB)

    Gomez, X.; Echeberria, J

    2003-05-15

    The viability by hot co-extrusion of a new bimetallic tube: carbon steel A-210-G deg. A1/iron based superalloy Sanicro 28 (UNS N08028) both by hot torsion tests and by diffusion bonding experiments using hipping has been verified. An excellent metallurgical bond was obtained after the industrial hot co-extrusion process. Both the interdiffusion of the elements across the interface, and the microstructure have been analysed by optical microscopy, SEM, TEM and EBSD (electron backscattered diffraction). On the Sanicro 28 side a profuse precipitation of Cr/Mo carbides was found in the region close to the interface. In the hipped specimens and in the heat-treated bimetallic tubes, as result of the nickel and chromium diffusion from the superalloy to the carbon steel, austenite and martensite sub-bands were observed parallel to the interface on the steel side. The optimum heat treatment performed on the bimetallic tubes consisted of an austenitising-solution treatment at 1100 deg. C, and a stabilisation annealing at 900 deg. C, followed by air cooling.

  15. Ferrocenyl-cymantrenyl hetero-bimetallic chalcones: Synthesis, structure and biological properties

    Science.gov (United States)

    Mishra, Sasmita; Tirkey, Vijaylakshmi; Ghosh, Avishek; Dash, Hirak R.; Das, Surajit; Shukla, Madhulata; Saha, Satyen; Mobin, Sheikh M.; Chatterjee, Saurav

    2015-04-01

    Two new ferrocenyl-cymantrenyl bimetallic chalcones, [(CO)3Mn(η5-C5H4)C(O)CHdbnd CH(η5-C5H4)Fe(η5-C5H5)] (1) and [{(CO)3Mn(η5-C5H4)C(O)CHdbnd CH(η5-C5H4)}2Fe] (2) have been synthesized. Their reactivity study with triphenylphosphine and bis-(diphenylphosphino)ferrocene led to the isolation of phosphine substituted bimetallic chalcones (3-6). Single crystal X-ray structural characterization for 1 and its phosphine analogue (3) reveals their different conformational identity with anti-conformation for 1, while syn-conformation for 3. Investigation of antimalarial and antibacterial activities was carried out for compounds 1 and 2 against two strains of Plasmodium falciparum (3D7, K1) and four bacterial strains. TD-DFT calculation was performed for compound 1 and electrochemical properties were studied for bimetallic chalcone compounds by cyclic voltammetric technique.

  16. Preparation of onion-like Pt-terminated Pt-Cu bimetallic nano-sized electrocatalysts for oxygen reduction reaction in fuel cells

    Science.gov (United States)

    Lim, Taeho; Kim, Ok-Hee; Sung, Yung-Eun; Kim, Hyun-Jong; Lee, Ho-Nyun; Cho, Yong-Hun; Kwon, Oh Joong

    2016-06-01

    Onion-like Pt-terminated Pt-Cu bimetallic nano-sized electrocatalysts (Pt/Cu/Pt/C) were synthesized by using an electroless deposition method. The synthesized Pt/Cu/Pt/C consisted of a Pt-enriched shell, a sandwiched Pt-Cu alloy layer, and a Pt core. The Pt/Cu/Pt/C showed higher electrocatalytic activity toward oxygen reduction reaction in half-cell test than that of commercial Pt/C due to an electronic structure change in the Pt-enriched shell, resulting from the sandwiched Pt-Cu alloy layer underneath. The stability of the Pt/Cu/Pt/C was examined by using both half-cell and single-cell degradation tests. In both tests, the Pt/Cu/Pt/C exhibited stronger resistance to catalyst degradation than that of the commercial Pt/C. It is notable that cell performance with the Pt/Cu/Pt/C was fully recovered by N2 purging after single-cell degradation testing, indicating there was no permanent damage to the electrocatalyst during the test. It is suggested that thermodynamically-stable structure of the Pt/Cu/Pt/C contributed to the improved stability.

  17. Catalytic activity of nanostructured Au: Scale effects versus bimetallic/bifunctional effects in low-temperature CO oxidation on nanoporous Au

    Directory of Open Access Journals (Sweden)

    Lu-Cun Wang

    2013-02-01

    Full Text Available The catalytic properties of nanostructured Au and their physical origin were investigated by using the low-temperature CO oxidation as a test reaction. In order to distinguish between structural effects (structure–activity correlations and bimetallic/bifunctional effects, unsupported nanoporous gold (NPG samples prepared from different Au alloys (AuAg, AuCu by selective leaching of a less noble metal (Ag, Cu were employed, whose structure (surface area, ligament size as well as their residual amount of the second metal were systematically varied by applying different potentials for dealloying. The structural and chemical properties before and after 1000 min reaction were characterized by scanning electron microscopy (SEM, X-ray diffraction (XRD and X-ray photoelectron spectroscopy (XPS. The catalytic behavior was evaluated by kinetic measurements in a conventional microreactor and by dynamic measurements in a temporal analysis of products (TAP reactor. The data reveal a clear influence of the surface contents of residual Ag and Cu species on both O2 activation and catalytic activity, while correlations between activity and structural parameters such as surface area or ligament/crystallite size are less evident. Consequences for the mechanistic understanding and the role of the nanostructure in these NPG catalysts are discussed.

  18. Synthesis and Photocatalytic Activity of TiO2/V2O5 Composite Catalyst Doped with Rare Earth Ions

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    TiO2/V2O5 catalyst doped with rare earth ions was prepared by sol-gel method. Titanium tetrapropoxide and vanadium pentoxide were used as precursor of the composite catalyst and rare earth ions were used as dopant. The crystal phases, crystalline sizes, microstructure, absorption spectra of doped composite catalyst were studied by XRD, EDS, FT-IR and UV-Vis. Photoactivity of the prepared catalyst under ultraviolet irradiation were evaluated by degradation of methyl orange (MO) in aqueous solution. It is shown that the prepared catalyst is composed of anatase and rutile. The rare earth ions are highly dispersed in composite catalyst. All the doped catalysts appear higher photocatalytic activity than TiO2/V2O5 catalyst and catalyst doped with Ce4+ present the best activity to MO.

  19. Preparation of Mesoporous Silica-Supported Palladium Catalysts for Biofuel Upgrade

    OpenAIRE

    Ling Fei; Harvind Kumar Reddy; Joshua Hill; Qianglu Lin; Bin Yuan; Yun Xu; Peter Dailey; Shuguang Deng; Hongmei Luo

    2012-01-01

    We report the preparation of two hydrocracking catalysts Pd/CoMoO4/silica and Pd/CNTs/CoMoO4/silica (CNTs, carbon nanotubes). The structure, morphologies, composition, and thermal stability of catalysts were studied by X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy, transmission electron microscopy (TEM), energy-dispersive X-ray (EDX), and thermogravimetric analysis (TGA). The catalyst activity was measured in a Parr reactor with camelina fatty acid methyl est...

  20. H2 production by catalytic methane decomposition on Cu based catalyst

    International Nuclear Information System (INIS)

    The thermo-catalytic decomposition (TCD) of methane has been investigated in a laboratory scale fixed bed reactor using a copper dispersed on γ-alumina as a catalyst. The usefulness of a fluidized bed operation instead of a fixed bed one has been assessed in terms of methane to hydrogen conversion, amount of carbon accumulated on the catalyst, possibility of the catalyst regeneration. The results highlight some promising features in using fluidized bed reactors in the TCD process. (authors)

  1. Alloy catalyst material

    DEFF Research Database (Denmark)

    2014-01-01

    The present invention relates to a novel alloy catalyst material for use in the synthesis of hydrogen peroxide from oxygen and hydrogen, or from oxygen and water. The present invention also relates to a cathode and an electrochemical cell comprising the novel catalyst material, and the process use...... of the novel catalyst material for synthesising hydrogen peroxide from oxygen and hydrogen, or from oxygen and water....

  2. Resin Catalyst Hybrids

    Institute of Scientific and Technical Information of China (English)

    S. Asaoka

    2005-01-01

    @@ 1Introduction: What are resin catalyst hybrids? There are typically two types of resin catalyst. One is acidic resin which representative is polystyrene sulfonic acid. The other is basic resin which is availed as metal complex support. The objective items of this study on resin catalyst are consisting of pellet hybrid, equilibrium hybrid and function hybrid of acid and base,as shown in Fig. 1[1-5].

  3. Catalytic decomposition of methane to COx-free hydrogen and carbon nanotubes over Co–W/MgO catalysts

    Directory of Open Access Journals (Sweden)

    Ahmed E. Awadallah

    2015-09-01

    Full Text Available Bimetallic catalysts containing a series of Co/W at 40/10, 30/20, 20/30 and 10/40 wt% supported on MgO with a total metal content of 50 wt% were prepared and used for the catalytic decomposition of methane to COx-free hydrogen and multi-walled carbon nanotubes (MWCNTs. The solid fresh and exhausted catalysts were characterized structurally and chemically through XRD, TPR, BET, TGA, TEM and Raman spectroscopy. The 40%Co–10%W/MgO catalyst exhibited the highest activity for the production of both hydrogen and MWCNTs. The formation of a large amount of non-interacted Co3O4 species is considered as the main reason for the catalyst superiority in its activity. On the contrary, catalysts formulations of 20%Co–30%W and 10%Co–40%W demonstrated the formation of a large amount of hardly reducible CoWO4 and MgWO4 particles causing lower activity of these catalysts toward methane decomposition as evidenced through the XRD and TPR results.

  4. Exposure of metallic copper surface on Cu-Al2O3-carbon catalysts

    NARCIS (Netherlands)

    Menon, P.G.; Prasad, J.

    1970-01-01

    The bifunctional nature of Cu---Al2O3-on-carbon catalysts, used in the direct catalytic conversion of ethanol to ethyl acetate, prompted an examination of the dispersion of Cu on the composite catalyst. For this, the N2O-method of Osinga et al. for estimation of bare metallic copper surface on compo

  5. Atomistic Processes of Catalyst Degradation

    Energy Technology Data Exchange (ETDEWEB)

    None

    2004-11-27

    The purpose of this cooperative research and development agreement (CRADA) between Sasol North America, Inc., and the oak Ridge National Laboratory (ORNL) was to improve the stability of alumina-based industrial catalysts through the combination of aberration-corrected scanning transmission electron microscopy (STEM) at ORNL and innovative sample preparation techniques at Sasol. Outstanding progress has been made in task 1, 'Atomistic processes of La stabilization'. STEM investigations provided structural information with single-atom precision, showing the lattice location of La dopant atoms, thus enabling first-principles calculations of binding energies, which were performed in collaboration with Vanderbilt University. The stabilization mechanism turns out to be entirely due to a particularly strong binding energy of the La tom to the {gamma}-alumina surface. The large size of the La atom precludes incorporation of La into the bulk alumina and also strains the surface, thus preventing any clustering of La atoms. Thus highly disperse distribution is achieved and confirmed by STEM images. la also affects relative stability of the exposed surfaces of {gamma}-alumina, making the 100 surface more stable for the doped case, unlike the 110 surface for pure {gamma}-alumina. From the first-principles calculations, they can estimate the increase in transition temperature for the 3% loading of La used commercially, and it is in excellent agreement with experiment. This task was further pursued aiming to generate useable recommendations for the optimization of the preparation techniques for La-doped aluminas. The effort was primarily concentrated on the connection between the boehmitre-{gamma}-Al{sub 2}O{sub 3} phase transition (i.e. catalyst preparation) and the resulting dispersion of La on the {gamma}-Al{sub 2}O{sub 3} surface. It was determined that the La distribution on boehmite was non-uniform and different from that on the {gamma}-Al{sub 2}O{sub 3} and thus

  6. States of Carbon Nanotube Supported Mo-Based HDS Catalysts

    Institute of Scientific and Technical Information of China (English)

    Hongyan Shang; Chenguang Liu; Yongqiang Xu; Jieshan Qiu; Fei Wei

    2006-01-01

    The dispersion of the active phase and loading capacity of the Mo species on carbon nanotube (CNT) was studied by the XRD technique. The reducibility properties of Co-Mo catalysts in the oxide state over CNTs were investigated by TPR, while the sulfided Co-Mo/CNT catalysts were characterized by means of the XRD and LRS techniques. The activity and selectivity with respect to the hydrodesulfurization (HDS) performances on carbon nanotube supported Co-Mo catalysts were evaluated. It was found that the main active molybdenum species in the oxide state MoO3/CNT catalysts were MoO2, but not MoO3, as generally expected. The maximum loading before the formation of the bulk phase was lower than 6% (percent by mass, based on MoO3). TPR studies revealed that the active species in the oxide state Co-Mo/CNT catalysts were reduced more easily at relatively lower temperatures in comparison to those of the Co-Mo/γ-Al2O3 catalysts, indicating that the CNT support promoted or favored the reduction of the active species. The active species of a Co-Mo-0.7/CNT catalyst were more easily reduced than those of the Co-Mo/CNT catalysts with Co/Mo atomic ratios of 0.2, 0.35, and 0.5, respectively, suggesting that the Co/Mo atomic ratio has a great effect on the reducibility of the active species. It was found that the incorporation of cobalt improved the dispersion of the molybdenum species on the support, and a phenomenon of mobilization and re-dispersion had occurred during the sulfurization process, resulting in low valence state Mo3S4 and Co-MoS2.17 active phases. HDS measurements showed that the Co-Mo/CNT catalysts were more active than the Co-Mo/γ-Al2O3 ones for the desulfurization of DBT, and the hydrogenolysis/hydrogenation selectivity of the Co-Mo/CNT catalysts was also much higher than those of the Co-Mo/γ-Al2O3. The Co-Mo/CNT catalyst with a Co/Mo atomic ratio of 0.7 showed the highest activity, whereas the catalyst with a Co/Mo atomic ratio of 0.35 had the highest selectivity.

  7. Gas-Phase Synthesis of Bimetallic Oxide Nanoparticles with Designed Elemental Compositions for Controlling the Explosive Reactivity of Nanoenergetic Materials

    Directory of Open Access Journals (Sweden)

    Ji Young Ahn

    2011-01-01

    Full Text Available We demonstrate a simple and viable method for controlling the energy release rate and pressurization rate of nanoenergetic materials by controlling the relative elemental compositions of oxidizers. First, bimetallic oxide nanoparticles (NPs with a homogeneous distribution of two different oxidizer components (CuO and Fe2O3 were generated by a conventional spray pyrolysis method. Next, the Al NPs employed as a fuel were mixed with CuO-Fe2O3 bimetallic oxide NPs by an ultrasonication process in ethanol solution. Finally, after the removal of ethanol by a drying process, the NPs were converted into energetic materials (EMs. The effects of the mass fraction of CuO in the CuO-Fe2O3 bimetallic oxide NPs on the explosive reactivity of the resulting EMs were examined by using a differential scanning calorimeter and pressure cell tester (PCT systems. The results clearly indicate that the energy release rate and pressurization rate of EMs increased linearly as the mass fraction of CuO in the CuO-Fe2O3 bimetallic oxide NPs increased. This suggests that the precise control of the stoichiometric proportions of the strong oxidizer (CuO and mild oxidizer (Fe2O3 components in the bimetallic oxide NPs is a key factor in tuning the explosive reactivity of EMs.

  8. Ultrahighly Dispersed Titanium Oxide on Silica : Effect of Precursors on the Structure and Photocatalysis

    OpenAIRE

    Yoshida, S.; Takenaka, S.; Tanaka, T.; Funabiki, T.

    1997-01-01

    The effect of precursor on the dispersion and catalytic performance of titanium oxide supported on silica has ben investigated. The catalysts were prepared by a simple impregnation method with three kinds of titanium complexes of different ligands (bis(isopropyato)-bis(pivaroylmethanato) : DPM, acetylacetonato : ACAC, tetrakis(isopropylato) : IPRO) with the aim of preparing ultrahighly dispersed titanium oxide on silica. The XAFS study revealed that titanium species in the catalyst prepared f...

  9. Effect of heat treatment on the physical properties of bimetallic doped catalyst, Cu-Ni/TiO2

    International Nuclear Information System (INIS)

    Post heat treatment is critical for the doped semiconductor oxide in order to improve its photocatalytic performance. Thus work had been carried out to understand the effect of different calcination temperature (400, 450 and 500°C) on the physical properties of nanosized Cu-Ni/TiO2Cu-Ni doped TiO2 nanoparticles prepared using a combined method of sol-gel and hydrothermal. The treated samples were characterized using Raman spectroscopy, Brunauer–Emmett–teller (BET) measurement, high resolution transmission electron microscopy (HRTEM), field-emission scanning electron microscopy (FESEM), and diffuse reflectance UV-Vis spectroscopy (DR-UV-Vis). Raman analysis showed that all samples displayed anatase (101) phase of TiO2, which is in good agreement with the TEM results. BET data showed that all prepared Cu-Ni/TiO2 with different calcination temperature are mesoporous. SEM images displayed spherical particles with typical size of about 15 to 20 nm. UV-Vis spectra illustrated that the absorbance edge of all prepared Cu-Ni/TiO2 have extended to the visible region with bandgap energies (2-2.1 eV) less than the pure anatase TiO2 (3.2 eV). Calcination temperature of 450°C is considered to be the optimum as it converts the synthesized Cu-Ni/TiO2 sample to have smaller average particle size with higher surface area that lead to more absorbance in the visible region and lower bandgap energy

  10. Effect of heat treatment on the physical properties of bimetallic doped catalyst, Cu-Ni/TiO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Bashiri, Robabeh, E-mail: noranimuti-mohamed@petronas.com.my; Sufian, Suriati [Chemical Engineering Dept. Universiti Teknologi PETRONAS, 31750 Tronoh, Perak (Malaysia); Mohamed, Norani Muti, E-mail: noranimuti-mohamed@petronas.com.my; Kait, Chong Fai, E-mail: chongfaikait@petronas.com.my [Fundamental and Applied Sciences Dept., Universiti Teknologi PETRONAS, 31750 Tronoh, Perak (Malaysia)

    2015-07-22

    Post heat treatment is critical for the doped semiconductor oxide in order to improve its photocatalytic performance. Thus work had been carried out to understand the effect of different calcination temperature (400, 450 and 500°C) on the physical properties of nanosized Cu-Ni/TiO{sub 2}Cu-Ni doped TiO{sub 2} nanoparticles prepared using a combined method of sol-gel and hydrothermal. The treated samples were characterized using Raman spectroscopy, Brunauer–Emmett–teller (BET) measurement, high resolution transmission electron microscopy (HRTEM), field-emission scanning electron microscopy (FESEM), and diffuse reflectance UV-Vis spectroscopy (DR-UV-Vis). Raman analysis showed that all samples displayed anatase (101) phase of TiO{sub 2}, which is in good agreement with the TEM results. BET data showed that all prepared Cu-Ni/TiO{sub 2} with different calcination temperature are mesoporous. SEM images displayed spherical particles with typical size of about 15 to 20 nm. UV-Vis spectra illustrated that the absorbance edge of all prepared Cu-Ni/TiO{sub 2} have extended to the visible region with bandgap energies (2-2.1 eV) less than the pure anatase TiO{sub 2} (3.2 eV). Calcination temperature of 450°C is considered to be the optimum as it converts the synthesized Cu-Ni/TiO{sub 2} sample to have smaller average particle size with higher surface area that lead to more absorbance in the visible region and lower bandgap energy.

  11. Hydrotreatment of wood-based pyrolysis oil using zirconia-supported mono- and bimetallic (Pt, Pd, Rh) catalysts

    NARCIS (Netherlands)

    Ardiyanti, A. R.; Gutierrez, A.; Honkela, M. L.; Krause, A. O. I.; Heeres, H. J.

    2011-01-01

    Fast pyrolysis oil (PO), the liquid product of fast pyrolysis of lignocellulosic biomass, requires upgrading to extent its application range and for instance to allow for co-feeding in an existing oil-refinery. Catalytic hydrotreatment reactions (350 degrees C, 20 MPa total pressure, and 4h reaction

  12. Autothermal reforming of simulated and commercial fuels on zirconia-supported mono- and bimetallic noble metal catalysts

    OpenAIRE

    Kaila, Reetta

    2008-01-01

    New energy sources are needed if energy supply and demand are to remain in balance. At the same time, the level of emissions needs to be reduced to minimise their contribution to the greenhouse effect. Renewable energy sources, and hydrogen (H2), have been attracting much attention, and more efficient technologies for energy recovery have been developed. Among these are fuel cells. H2 is not a source of energy but an energy carrier, which needs to be produced from a primary fuel (hydroca...

  13. Balance of Nanostructure and Bimetallic Interactions in Pt Model Fuel Cell Catalysts: An in Situ XAS and DFT Study

    Energy Technology Data Exchange (ETDEWEB)

    Friebel, Daniel; Viswanathan, Venkatasubramanian; Miller, Daniel James; Anniyev, Toyli; Ogasawara, Hirohito; Larsen, Ask Hjorth; O' Grady, Christopher P.; Norskov, Jens K.; Nilsson, Anders

    2012-05-31

    We have studied the effect of nanostructuring in Pt monolayer model electrocatalysts on a Rh(111) single-crystal substrate on the adsorption strength of chemisorbed species. In situ high energy resolution fluorescence detection X-ray absorption spectroscopy at the Pt L(3) edge reveals characteristic changes of the shape and intensity of the 'white-line' due to chemisorption of atomic hydrogen (H(ad)) at low potentials and oxygen-containing species (O/OH(ad)) at high potentials. On a uniform, two-dimensional Pt monolayer grown by Pt evaporation in ultrahigh vacuum, we observe a significant destabilization of both H(ad) and O/OH(ad) due to strain and ligand effects induced by the underlying Rh(111) substrate. When Pt is deposited via a wet-chemical route, by contrast, three-dimensional Pt islands are formed. In this case, strain and Rh ligand effects are balanced with higher local thickness of the Pt islands as well as higher defect density, shifting H and OH adsorption energies back toward pure Pt. Using density functional theory, we calculate O adsorption energies and corresponding local ORR activities for fcc 3-fold hollow sites with various local geometries that are present in the three-dimensional Pt islands.

  14. Magnetic catalyst bodies

    NARCIS (Netherlands)

    Teunissen, Wendy; Bol, A.A.; Geus, John W.

    2001-01-01

    After a discussion about the importance of the size of the catalyst bodies with reactions in the liquid-phase with a suspended catalyst, the possibilities of magnetic separation are dealt with. Deficiencies of the usual ferromagnetic particles are the reactivity and the clustering of the particles.

  15. Novel 2D RuPt core-edge nanocluster catalyst for CO electro-oxidation

    Science.gov (United States)

    Grabow, Lars C.; Yuan, Qiuyi; Doan, Hieu A.; Brankovic, Stanko R.

    2015-10-01

    A single layer, bi-metallic RuPt catalyst on Au(111) is synthesized using surface limited red-ox replacement of underpotentially deposited Cu and Pb monolayers though a two-step process. The resulting 2D RuPt monolayer nanoclusters have a unique core-edge structure with a Ru core and Pt at the edge along the perimeter. The activity of this catalyst is evaluated using CO monolayer oxidation as the probe reaction. Cyclic voltammetry demonstrates that the 2D RuPt core-edge catalyst morphology is significantly more active than either Pt or Ru monolayer catalysts. Density functional theory calculations in combination with infra-red spectroscopy data point towards oscillating variations (ripples) in the adsorption energy landscape along the radial direction of the Ru core as the origin of the observed behavior. Both, CO and OH experience a thermodynamic driving force for surface migration towards the Ru-Pt interface, where they adsorb most strongly and react rapidly. We propose that the complex interplay between epitaxial strain, ligand and finite size effects is responsible for the formation of the rippled RuPt monolayer cluster, which provides optimal conditions for a quasi-ideal bi-functional mechanism for CO oxidation, in which CO is adsorbed mainly on Pt, and Ru provides OH to the active Pt-Ru interface.

  16. Heterogeneous hydrogenation catalysts

    International Nuclear Information System (INIS)

    The main types of heterogeneous catalysts used for hydrogenation, the methods for their preparation, and the structure and chemistry of their surfaces are considered, as well as the catalytic activity and the mechanism of action in the hydrogenation of unsaturated and aromatic compounds, of CO, and of carbonyl compounds and in the hydrorefining of fuels. Chief attention is paid to supported Ni catalysts, to the methods for their preparation and physicochemical studies, and to the development of novel catalytic systems through modification. A novel type of catalyst for hydrogenation, viz. metal carbides, is described. Some aspects of the mechanochemical treatment of hydrogenation catalysts, including in situ methods, are discussed. Sulfide catalysts for hydrotreating are also discussed in detail. The bibliography includes 340 references.

  17. Design of heterogeneous catalysts

    DEFF Research Database (Denmark)

    Frey, Anne Mette

    . Previously it has been shown that calcination of cobalt catalyst in a NO/He mixture resulted in improved catalytic activity compared to standard air calcined samples, since more homogenous cobalt particles with a narrow particle size distribution were formed. Unfortunately the C5+ selectivity decreased....... Since Mn is known to improve C5+ selectivity the addition of this promoter, combined with NO calcination, was studied. The influence of parameters such as Co:Mn ratio, drying conditions, and reduction temperatures on the catalytic performance were investigated. The promotion strategy turned out to work...... well, and the best catalyst prepared had a C5+ yield almost a factor of two higher than a standard air calcined Co catalyst. In the NH3-SCR reaction it is desirable to develop an active and stable catalyst for NOx removal in automotive applications, since the traditionally used vanadium-based catalyst...

  18. Cluster-derived Ir-Sn/SiO2 catalysts for the catalytic dehydrogenation of propane: A spectroscopic study

    KAUST Repository

    Gallo, Alessandro

    2013-01-01

    Ir-Sn bimetallic silica-based materials have been prepared via deposition of the molecular organometallic clusters (NEt4)2[Ir 4(CO)10(SnCl3)2] and NEt 4[Ir6(CO)15(SnCl3)] or via deposition of Sn organometallic precursor Sn(n-C4H9) 4 onto pre-formed Ir metal particles. These solids possess promising properties, in terms of selectivity, as catalysts for propane dehydrogenation to propene. Detailed CO-adsorption DRIFTS, XANES and EXAFS characterization studies have been performed on these systems in order to compare the structural and electronic evolution of systems in relation to the nature of the Ir-Sn bonds present in the precursor compounds and to propose a structural model of the Ir-Sn species present at the silica surface of the final catalyst. © 2013 The Royal Society of Chemistry.

  19. Ethylene Polymerization Using Improved Polyethylene Catalyst%改进的催化剂的乙烯聚合动力学研究

    Institute of Scientific and Technical Information of China (English)

    朱孝恒; 郭子芳; 岑为; 毛炳权

    2011-01-01

    The study concerns the use of MgCl2-supported high-activity Ziegler-Natta catalysts for the polymerization of ethylene. In particular, two types of catalysts were investigated, which were N-catalyst (BRICI) and improved polyethylene catalyst. The effects of catalyst structure on kinetic behavior were examined. The distribution of active centers in these catalysts was investigated by energy dispersive analysis by X-rays (EDAX), and morphologies of catalyst particles and polymer products were examined by scanning electron microscope (SEM). Hydrogen response and copolymerization performance were investigated and compared with the two catalysts. The results were correlated with the kinetic behavior of the two catalysts and appropriate models for polymer particle growth were presented. The improved polyethylene catalyst showed higher activity, better hydrogen response and copolymerization performance.

  20. 1: Redox chemistry of bimetallic fulvalene complexes; 2: Oligocyclopentadienyl complexes

    Energy Technology Data Exchange (ETDEWEB)

    Brown, D. S. [Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley Lab., CA (United States). Chemical Sciences Div.

    1993-11-01

    The electrochemistry of the heterobimetallic complexes (fulvalene)WFe(CO){sub 5} (30) and (fulvalene)WRu(CO){sub 5} (31) has been investigated. Compound 30 is reduced in two one-electron processes, and this behavior was exploited synthetically to prepare a tetranuclear dimer by selective metal reduction. Complex 31 displayed a distinction between the metals upon reoxidation of the dianion, allowing the formation of a dimer by selective metal anion oxidation. The redox behavior of 30 led to an investigation of the use of electrocatalysis to effect metal-specific ligand substitution. It was found that reduction of 30 with a catalytic amount of CpFe(C{sub 6}Me{sub 6}) (97) in the presence of excess P(OMe){sub 3} or PMe{sub 3} led to the formation of the zwitterions (fulvalene)[W(CO){sub 3}{sup {minus}}][Fe(CO)PR{sub 3}{sup +}] (107, R = P(OMe){sub 3}; 108, R = PMe{sub 3}). Compound 31 also displayed unique behavior with different reducing agents, as the monosubstituted zwitterion (fulvalene)[W(CO){sub 3}{sup {minus}}][Ru(CO){sub 2}(PMe{sub 3}){sup +}] was obtained when 97 was used while the disubstituted complex (fulvalene) [W(CO){sub 3}{sup {minus}}] [Ru(CO)(PMe{sub 3}){sub 2}{sup +}] was produced when Cp*Fe(C{sub 6}Me{sub 6}) was the catalyst. Potential synthetic routes to quatercyclopentadienyl complexes were also explored. Various attempts to couple heterobimetallic fulvalene compounds proved to be unsuccessful. 138 refs.