Contributions of distinct gold species to catalytic reactivity for carbon monoxide oxidation

Small-size (<5 nm) gold nanostructures supported on reducible metal oxides have been widely investigated because of the unique catalytic properties they exhibit in diverse redox reactions. However, arguments about the nature of the gold active site have continued for two decades, due to the lack of comparable catalyst systems with specific gold species, as well as the scarcity of direct experimental evidence for the reaction mechanism under realistic working conditions. Here we report the determination of the contribution of single atoms, clusters and particles to the oxidation of carbon monoxide at room temperature, by the aid of in situ X-ray absorption fine structure analysis and in situ diffuse reflectance infrared Fourier transform spectroscopy. We find that the metallic gold component in clusters or particles plays a much more critical role as the active site than the cationic single-atom gold species for the room-temperature carbon monoxide oxidation reaction.National Science Foundation of China (NSFC) [21301107, 21373259, 21331001, 11079005, 11405256]; Fundamental research funding of Shandong University [2014JC005]; Taishan Scholar project of Shandong Province (China); Hundred Talents project of the Chinese Academy of Sciences; Beijing National Laboratory for Molecular Science; Strategic Priority Research Program of the Chinese Academy of Sciences [XDA09030102]SCI(E)ARTICLEcma@ustc.edu.cn; sirui@sinap.ac.cn; jiacj@sdu.edu.cn