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In Situ Time-Resolved Characterization of Au-CeO2 Catalysts During Water Gas Shift Reactions: presence of Au and O Vacancies in the Active Phase

Journal Article · · J. Chem. Phys.
DOI:https://doi.org/10.1063/1.2136876· OSTI ID:913728

Synchrotron-based in situ time-resolved x-ray diffraction and x-ray absorption spectroscopies were used to study the behavior of nanostructured {l_brace}Au+AuO{sub x}{r_brace}-CeO{sub 2} catalysts under the water-gas shift (WGS) reaction. At temperatures above 250 C, a complete AuO{sub x}{yields}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{sub 2}(111) single crystal corroborate that cationic Au{sup {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.

Research Organization:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Organization:
Doe - Office Of Science
DOE Contract Number:
AC02-98CH10886
OSTI ID:
913728
Report Number(s):
BNL--78296-2007-JA
Journal Information:
J. Chem. Phys., Journal Name: J. Chem. Phys. Vol. 123; ISSN JCPSA6; ISSN 0021-9606
Country of Publication:
United States
Language:
English