PNNL

Abstract

By means of density functional theory calculations, the properties of Al2O3/Au(111), the interface between Al2O3 and Au(111), the adsorption of O2, and CO oxidation over Al2O3/Au(111) have been investigated. This study shows that the binding of small Al2O3 clusters on Au(111) is strong because of the charge transfer between them. The study of O2 adsorption on different sites indicates that the interfacial site is the most stable one via the bonding of oxygen with Au and Al atoms. The full catalytic cycles for the oxidation of CO by O2 in either association or dissociation pathway are calculated. The oxidation in the association pathway is significantly easier than that in the dissociation one. This study reveals not only the origin of inverse catalysts for CO oxidation but also the role of the interface in CO oxidation on Au catalysts. This work was supported by National Basic Research Program of China (973 Program) (2013CB733501), the National Natural Science Foundation of China (NSFC-21176221, 21136001, 21101137, 21306169, and 91334013). D. Mei acknowledges the support from the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. Computing time was granted by the grand challenge of computational catalysis of the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL).