(001)-supported Au Clusters: A First-principles Density Functional Theory Investigation*

Following the discovery that gold is a viable catalyst in oxidation reactions [1], much research has focused on its use in the partial oxidation of alcohols. Several studies have demonstrated the good catalytic activity of gold nanoparticles supported on partially reducible metal oxides while the mechanism involving irreducible oxide supports has not been explored to the same extent. In this study, we investigate the reaction mechanism of the partial oxidation of methanol on Au clusters supported on the γ-Al₂O₃(001) surface. We aim to understand how cluster size and charge transfer affect the reaction mechanism. After a survey of structural and electronic properties of supported Au_n (n=1,4) clusters and the energetics of adsorption of methanol (CH₃OH) on both Au and interface sites, we present a comparative analysis of the computed activation barrier of the CH₃OH → CH₃O + H reaction on this system against those characteristic of traditional catalysts. This work is supported by the Scientific and Technological Research Council of Turkey (TUBITAK) within the 1001 program, Grant No: 113F099.

[1] M. Haruta et al. Chem. Lett., 405-408 (1987)