In situ time-resolved characterization of Au-CeO2 and AuOx-CeO2 catalysts during the water-gas shift reaction: presence of Au and O vacancies in the active phase |
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Authors: | Wang X Rodriguez J A Hanson J C Pérez M Evans J |
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Institution: | Department of Chemistry, Brookhaven National Laboratory, Upton, NY 11973, USA. rodrigez@bnl.gov |
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Abstract: | Synchrotron-based in situ time-resolved x-ray diffraction and x-ray absorption spectroscopies were used to study the behavior of nanostructured {Au+AuO(x)}-CeO(2) catalysts under the water-gas shift (WGS) reaction. At temperatures above 250 degrees C, a complete AuO(x)-->Au transformation was observed with high catalytic activity. Photoemission results for the oxidation and reduction of Au nanoparticles supported on rough ceria films or a CeO(2)(111) single crystal corroborate that cationic Au(delta+) species cannot be the key sites responsible for the WGS activity at high temperatures. The rate determining steps for the WGS seem to occur at the gold-ceria interface, with the active sites involving small gold clusters (<2 nm) and O vacancies. |
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