Charge Polarization at a Au–TiC Interface and the Generation of Highly Active and Selective Catalysts for the Low-Temperature Water–Gas Shift Reaction†
Corresponding Author
Dr. José A. Rodriguez
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)Search for more papers by this authorDr. Pedro J. Ramírez
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020A (Venezuela)
Search for more papers by this authorGian Giacomo Asara
Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, C/Marcel⋅lí Domingo s/n, 43007 Tarragona (Spain)
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorDr. Francesc Viñes
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorProf. Jaime Evans
Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020A (Venezuela)
Search for more papers by this authorDr. Ping Liu
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Search for more papers by this authorProf. Josep M. Ricart
Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, C/Marcel⋅lí Domingo s/n, 43007 Tarragona (Spain)
Search for more papers by this authorProf. Francesc Illas
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorCorresponding Author
Dr. José A. Rodriguez
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)Search for more papers by this authorDr. Pedro J. Ramírez
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020A (Venezuela)
Search for more papers by this authorGian Giacomo Asara
Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, C/Marcel⋅lí Domingo s/n, 43007 Tarragona (Spain)
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorDr. Francesc Viñes
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorProf. Jaime Evans
Facultad de Ciencias, Universidad Central de Venezuela, Caracas 1020A (Venezuela)
Search for more papers by this authorDr. Ping Liu
Chemistry Department, Brookhaven National Laboratory, Upton, NY 11973 (USA)
Search for more papers by this authorProf. Josep M. Ricart
Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, C/Marcel⋅lí Domingo s/n, 43007 Tarragona (Spain)
Search for more papers by this authorProf. Francesc Illas
Departament de Química Física and IQTCUB, Universitat de Barcelona, C/Martí i Franquès 1, 08028 Barcelona (Spain)
Search for more papers by this authorThe research at BNL (Chemistry Department, National Synchrotron Light Source, Center for Functional Nanomaterials) was financed by the US Department of Energy (DOE), Office of Basic Energy Science (DE-AC02-98CH10086). This research has been supported by the Spanish MINECO (grants CTQ2011-29054-CO2-01/BQU and CTQ2012-30751) and, in part, by Generalitat de Catalunya grants 2014SGR97, 2014SGR199, and XRQTC. INTEVEP and IDB financed the research carried out at UCV. G.-G.A. thanks the Universitat Rovira i Virgili for supporting his predoctoral research. F.V. thanks the MINECO for a postdoctoral Ramón y Cajal grant (RYC-2012-10129). F.I. acknowledges additional support through an ICREA Academic Award for excellence in research. Computational time at the MareNostrum supercomputer was generously provided by the Barcelona Supercomputing Center through a grant from Red Española de Supercomputación.
Abstract
Au atoms in contact with TiC(001) undergo significant charge polarization. Strong metal–support interactions make Au/TiC(001) an excellent catalyst for the low-temperature water–gas shift (WGS), with turnover frequencies orders of magnitude larger than those observed for conventional metal/oxide catalysts. DFT calculations indicate that the WGS reaction follows an associative mechanism with HOCO as a key intermediate.
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