Reducibility of supported gold (III) precursors: influence of the metal oxide support and consequences for CO oxidation activity |
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Authors: | Laurent Delannoy Norbert Weiher Nikolaos Tsapatsaris Angela M Beesley Luanga Nchari Sven L M Schroeder Catherine Louis |
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Affiliation: | (1) Laboratoire de Réactivité de Surface, UMR 7609 CNRS, Université Pierre et Marie Curie-Paris 6, 4 place Jussieu, 75252, Paris, Cedex 05, France;(2) Molecular Materials Centre, School of Chemical Engineering and Analytical Science, The University of Manchester, PO Box 88, Sackville Street, Manchester, M60 1QD, UK;(3) School of Chemistry, The University of Manchester, Oxford Road, Manchester, M13 9PL, UK |
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Abstract: | The origin of CO oxidation performance variations between three different supported Au catalysts (Au/CeO2, Au/Al2O3, Au/TiO2) was examined by in situ XAFS and DRIFTS measurements. All samples were prepared identically, by deposition-precipitation of an aqueous Au(III) complex
with urea, and contained the same gold loading (~1 wt %). The as-prepared supported Au(III) precursors exhibited different
reduction behaviour during exposure to the CO/O2/He reaction mixture at 298 K. The reducibility of the Au(III) precursor was found to decrease as a function of the support
material in the order: titania > ceria > alumina. The as-prepared samples were inactive catalysts, but Au/TiO2 and Au/CeO2 developed catalytic activity as the reduction of Au(III) to metallic Au proceeded. Au/Al2O3 remained inactive. The developed catalytic CO oxidation activity at 298 K varied as a function of the support as follows:
titania > ceria > alumina ~ 0. The EXAFS of samples pretreated in air at 773 K and in H2 at 573 K reveals the presence of only metallic particles for Au/TiO2 and Au/Al2O3. Au(III) supported on CeO2 remains unreduced after calcination, but reduces during the treatment with H2. CO oxidation experiments performed at 298 K with the activated samples show that the presence of metallic gold is necessary
to obtain active catalysts (Au/CeO2 is not active after calcination) and that the reducible supports facilitate the genesis of active catalysts, while metallic
gold particles on alumina are not active. |
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Keywords: | gold ceria titania alumina reducibility CO oxidation DRIFTS XAFS |
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