Gates, Bruce - University of California, Davis - Department of Chemical Engineering

个人简介

Educational Background B.S., 1961, University of California, Berkeley Ph.D., 1966, University of Washington, Seattle

研究领域

Research Our program in catalysis research emphasizes fundamental investigations motivated by technologically important problems and close interactions with industry. The research involves catalyst preparation, characterization by physical methods, and testing in low- and high-pressure reactors. Catalysis by structurally simple supported metal clusters Organometallic precursors are used to prepare structurally simple metal-oxide-supported metals, including single-metal-atom complexes, metal carbonyl clusters, and metal clusters. Examples include rhenium subcarbonyls on MgO and Ir4, Ir6, and Pt15 clusters on Alumina and in zeolites. The work is leading to fundamental understanding of the structure of the metal-support interface, the structures of metal clusters on supports, and the dependence of catalytic properties on cluster size and structure and the structure of the metal-support interface. Solid superacid catalysts Solid superacids are being investigated that have activities for butane isomerization even at room temperature. These catalysts may provide the first practical routes to low-temperature paraffin isomerization for clean-burning gasoline. Zeolite catalysts We are using ship-in-a-bottle syntheses as well as more conventional preparations to synthesize metal carbonyl clusters and metal clusters in zeolite cages. The materials include structurally simple catalysts (e.g., Ir4 in NaY zeolite) and very small metal clusters in zeolite L. We have been able to interconvert metal carbonyls such as and metal clusters such as Ir6. Our group has also investigated acidic zeolites such as HZSM-5 as paraffin conversion catalysts. Novel supported bimetallic catalysts We are using organometallic precursors to prepare highly dispersed supported metal catalysts, including bimetallics. Examples include Pt-Mo catalysts supported on alumina, where the close proximity of the two metals may confer favorable properties on auto exhaust conversion catalysts. Catalyst preparation by sol-gel methods The sol-gel technique gives precise control of the physical properties of amorphous metal oxides, but it has still found little application in catalyst preparation. We are investigating the effects of preparation variables on catalyst support properties made with organometallic precursors and using the method to prepare novel supported metal catalysts. Experiments with powder and single-crystal samples Understanding of the properties of supported metal catalysts requires precise characterization of the structure, including the structure of the metal-support interface. Such understanding is emerging from characterizations of metals supported on single crystals of metal oxides with techniques including IR, EXAFS, NMR and other physical techniques.

近期论文

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“Upgrading of lignin-derived compounds: reactions of eugenol catalyzed by HY zeolite and Pt/γ-Al2O3,” T. Nimmanwudipong, R. C. Runnebaum, S. E. Ebeler, D. E. Block, and B. C. Gates, Catalysis Letters, 142, 151 (2012). “Atomically Dispersed Supported Metal Catalysis,” M. Flytzani-Stephanopoulos and B. C. Gates, Annual Reviews of Chemical and Biomolecular Engineering, Vol 3, pp. 545-74, (2012). “Imaging Isolated Gold Atom Catalytic Sites in Zeolite NaY,” J. Lu, C. Aydin, N. D. Browning, and B. C. Gates, Angewandte Chemie International Edition, 51, 5842 (2012). “Hydrogen Activation and Metal Hydride Formation Trigger Cluster Formation from Supported Iridium Complexes,” J. Lu, C. Aydin, N. D. Browning, and B. C. Gates, Journal of the American Chemical Society, 134, 5022 (2012). “A Smart Catalyst: Sinter-resistant Supported Iridium Clusters Visualized with Electron Microscopy,” C. Aydin, J. Lu, N. D. Browning, and B. C. Gates, Angewandte Chemie International Edition, 51, 5929 (2012). “Site-isolated Mononuclear Iridium Complex Catalyst Supported in the 1-Dimensional Channels of Zeolite HSSZ-53: Characterization by Spectroscopy and Aberration-Corrected Scanning Transmission Electron Microscopy,” J. Lu, C. Aydin, A. J. Liang, C. -Y. Chen, N. D. Browning, and B. C. Gates, ACS Catalysis, 2, 1002 (2012). “Catalytic Conversion of Furan to Gasoline-Range Aliphatic Hydrocarbons via Ring Opening and Decarbonylation Reactions Catalyzed by Pt/γ-Al2O3,” R. C. Runnebaum, T. Nimmanwudipong, J. Doan, D. E. Block, and B. C. Gates, Catalysis Letters, 142, 664 (2012). “A Highly Selective Catalyst for Partial Hydrogenation of 1,3-Butadiene: MgO-Supported Rhodium Clusters Selectivity Poisoned with CO,” D. Yardimci, P. Serna, and B. C. Gates, ChemCatChem, 4, 1547 (2012). “Atomically Resolved Site-Isolated Catalyst on MgO: Mononuclear Osmium Dicarbonyls formed from Os3(CO)12,” C. Aydin, A. Kulkarni, M. Chi, N. D. Browning, and B. C. Gates, Journal of Physical Chemistry Letters, 3, 1865 (2012). “Structures and Stability of Irn(CO)m,” M. Chen, J. E. Dyer, B. C. Gates, A. Katz and D. A. Dixon, Molecular Physics, 110, 1977 (2012). “Mononuclear Zeolite-Supported Iridium Catalyst: Kinetic, Spectroscopic, Electron Microscopic, and Size-Selective Poisoning Evidence for an Atomically Dispersed True Catalyst at 22 °C,” E. Bayram, J. Lu, C. Aydin, A. Uzun, N. D. Browning, B. C. Gates and R. G. Finke, ACS Catalysis, 2, 1947 (2012). “Selective Hydrodeoxygenation of Guaiacol Catalyzed by Platinum Supported on Magnesium Oxide,” T. Nimmanwudipong, C. Aydin, J. Lu, R. Runnebaum, K. Brodwater, N. D. Browning, D. E. Block and B. C. Gates, Catalysis Letters, 142, 1190 (2012). “Oxide- and Zeolite-Supported Isostructural Ir(C2H4)2 Complexes: Molecular-level Observations of Electronic Effects of Supports as Ligands,” J. Lu, C. Aydin, N. D. Browning and B. C. Gates, Langmuir, 28, 12806 (2012). “Tuning Catalytic Selectivity: Zeolite- and Magnesium Oxide-Supported Molecular Rhodium Catalysts for Hydrogenation of 1,3-Butadiene,” D. Yardimci, P. Serna, and B. C. Gates, ACS Catalysis, 2, 2100 (2012). “Sinter-Resistant Catalysts: Supported Iridium Nanoclusters with Intrinsically Limited Sizes,” J. Lu, C. Aydin, N. D. Browning, L. Wang, and B. C. Gates, Catalysis Letters, 142, 1445 (2012). “Defragmenting Catalysis” (editorial), B. C. Gates and T. J. Marks, Angewandte Chemie International Edition, 51, 11644 (2012). “Surface-Mediated Synthesis of Dimeric Rhodium Catalysts on MgO: Tracking Changes in the Nuclearity and Ligand Environment of the Catalytically Active Sites by X-Ray Absorption and Infrared Spectroscopies,” D. Yardimci, P. Serna, and B. C. Gates, Chemistry-A European Journal, 19, 1235 (2013). “Three-Dimensional Structural Analysis of MgO-Supported Osmium Clusters by Electron Microscopy with Single-Atom Sensitivity,” C. Aydin, A. Kulkarni, M. Chi, N. D. Browning, and B. C. Gates, Angewandte Chemie International Edition, in press (2013). “Quantitative Z-Contrast Imaging of Supported Metal Complexes and Clusters – A Gateway to Understanding Catalysis on the Atomic Scale,” N. D. Browning, C. Aydin, J. Lu, A. Kulkarni, N. L. Okamoto, V. Ortalan, B. W. Reed, A. Uzun, and B. C. Gates, ChemCatChem, in press (2013). “MgO-Supported Bimetallic Catalysts Consisting of Segregated, Essentially Molecular Rhodium and Osmium Species,” J. D. Kistler, P. Serna, and B. C. Gates, Dalton Transactions, in press (2013). “Zeolite-Supported Bimetallic Catalyst: Controlling Selectivity of Rhodium Complexes by Nearby Iridium Complexes,” J. Lu, C. Martinez-Macias, C. Aydin, N. D. Browning, and B. C. Gates, Catalysis Science & Technology (2013). “Formation of MgO-Supported Manganese Carbonyl Complexes by Chemisorption of Mn(CO)5CH3,” S. Khabuanchalad, J. Wittayakun, R. J. Lobo-Lapidus, S. Stoll, R. D. Britt, and B. C. Gates, Langmuir, in press (2013). “Catalysis by Solid Acids,” A. Katz and B. C. Gates, “Encyclopedia of Catalysis,” Wiley-Interscience, submitted (2013).