title: Contributions of distinct gold species to catalytic reactivity for carbon monoxide oxidation.
abstract: 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.
authors.affiliation: Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.
authors.forename: Li-Wen
authors.initials: LW
authors.lastname: Guo
authors.affiliation: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China.
authors.forename: Pei-Pei
authors.initials: PP
authors.lastname: Du
authors.affiliation: Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.
authors.forename: Xin-Pu
authors.initials: XP
authors.lastname: Fu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China.
authors.forename: Chao
authors.initials: C
authors.lastname: Ma
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China.
authors.forename: Jie
authors.initials: J
authors.lastname: Zeng
authors.affiliation: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China.
authors.forename: Rui
authors.initials: R
authors.lastname: Si
authors.affiliation: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China.
authors.forename: Yu-Ying
authors.initials: YY
authors.lastname: Huang
authors.affiliation: Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.
authors.forename: Chun-Jiang
authors.initials: CJ
authors.lastname: Jia
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Lab of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Lab in Rare Earth Materials and Bioinorganic Chemistry, Peking University, Beijing 100871, China.
authors.forename: Ya-Wen
authors.initials: YW
authors.lastname: Zhang
authors.affiliation: Beijing National Laboratory for Molecular Sciences, State Key Lab of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Lab in Rare Earth Materials and Bioinorganic Chemistry, Peking University, Beijing 100871, China.
authors.forename: Chun-Hua
authors.initials: CH
authors.lastname: Yan