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Title: Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO 2

We carried out density functional theory calculations to study the influence of oxide–metal charge transfers on the structure, energetics, and reactivity of Au and Pt atoms, dimers, and trimers adsorbed on the (101) surface of reduced anatase TiO 2. Pt clusters interact much more strongly with the TiO 2 support than Au clusters, and, with the exception of single Pt adatoms, generally behave as electron acceptors on reduced TiO 2, whereas Au clusters can both accept and donate charge on the reduced surface. The reactivity of the supported clusters was probed by considering their interaction with CO and co-adsorbed O 2. The effect of surface reduction on the interaction with CO is particularly significant when the CO adsorption site is an interfacial metal atom directly in contact with the TiO 2 surface and/or in the presence of co-adsorbed O 2. Pt clusters interact strongly with co-adsorbed O 2 and form Pt–O 2 complexes that can easily accept electrons from reduced surfaces. In contrast, Au clusters donate charge to co-adsorbed O 2 even in the presence of excess electrons from a reduced support. In conclusion, the computed differences in the properties of the supported Pt and Au clusters are consistent withmore » several experimental observations and highlight the important role of excess surface electrons in the behavior of supported metal catalysts on reducible oxides« less
 [1] ;  [2] ;  [3]
  1. Princeton Univ., Princeton, NJ (United States); Chinese Academy of Sciences, Guangzhou (China); Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Chinese Academy of Sciences, Guangzhou (China); Guangdong Univ. of Technology, Guangzhou (China)
  3. Princeton Univ., Princeton, NJ (United States)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 18; Journal ID: ISSN 0021-9606
American Institute of Physics (AIP)
Research Org:
Princeton Univ., Princeton, NJ (United States). Dept. of Chemistry
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1361868