Insight into the Synergetic Effect in Ternary Gold-Based Catalysts:  Ultrastability and High Activity of Au on Alumina Modified Titania

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Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China
Cite this: J. Phys. Chem. C 2007, 111, 36, 13539–13546
Publication Date (Web):August 22, 2007
https://doi.org/10.1021/jp074530u
Copyright © 2007 American Chemical Society
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Abstract

Nanogold particles dispersed on oxides can be highly active as catalyst and often lack the long-term stability due to the inherent instability of small gold particles. New thinking for the catalyst design is therefore urgently demanded to enhance the gold sticking on oxides while retaining the high activity. By systematically investigating the working mechanism of a ternary system, Au supported on alumina modified anatase titania, using first principles calculations, this work illustrates from the atomic level how a third component (alumina) can be used as the nucleation center to anchor Au particles while the component itself does not take part in the catalytic oxidation of CO. For Au supported on pure anatase, CO oxidation is already facile with the reaction barrier being only 0.22 eV, but the Au adsorption on anatase is rather weak as expected. The stepwise growth of alumina on anatase is shown to produce locally clustered alumina thin layers on anatase (Al2O3/TiO2). On these Al2O3/TiO2 sites, the binding energy of Au can be more than five times that on pure anatase. The active site of CO oxidation in the ternary system, however, remains at the boundary of Au/anatase, since it is found that O2 does not adsorb at the boundary between Au and Al2O3 thin films. Electronic structure analyses are utilized to rationalize the results. The synergetic effect revealed here implies that applying nonuniform mixed-oxide support could be a promising solution toward practical applications of Au-based catalysts.

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 Corresponding author. E-mail:  [email protected]

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