期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 135, 期 29, 页码 10673-10683出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja402063v
关键词
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资金
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences
- NKBRSF [2011CB932400]
- NSFC of China [91026003, 21101098]
- China Scholarship Council
- PNNL-ASF
- Department of Energy's Office of Biological and Environmental Research located at PNNL
- National Energy Research Scientific Computing Center (NERSC) at Lawrence Berkeley National Laboratory
To probe metal particle/reducible oxide interactions density functional theory based ab initio molecular dynamics studies were performed on a prototypical metal cluster (Au-20) supported on reducible oxides (rutile TiO2(110)) to implicitly account for finite temperature effects and the role of excess surface charge in the metal oxide. It is found that the charge state of the Au particle is negative in a reducing chemical environment whereas in the presence of oxidizing species coadsorbed to the oxide surface the duster obtained a net positive charge. In the context of the well-known CO oxidation reaction, charge transfer facilitates the plasticization of Au-20, which allows for a strong adsorbate induced surface reconstruction upon addition of CO leading to the formation of mobile Au-CO species on the surface. The charging/discharging of the cluster during the catalytic cycle of CO oxidation enhances and controls the amount of O-2 adsorbed at oxide/cluster interface and strongly influences the energetics of all redox steps in catalytic conversions. A detailed comparison of the current findings with previous studies is presented, and generalities about the role of surface-adsorbate charge transfer for metal cluster/reducible oxide interactions are discussed.
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