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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

Abstract

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

Authors:
 [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:
Research Org.:
Princeton Univ., Princeton, NJ (United States). Dept. of Chemistry
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1465991
Alternate Identifier(s):
OSTI ID: 1361868
Grant/Contract Number:  
SC0007347
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 146; Journal Issue: 18; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wang, Honghong, An, Taicheng, and Selloni, Annabella. Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO2. United States: N. p., 2017. Web. doi:10.1063/1.4982933.
Wang, Honghong, An, Taicheng, & Selloni, Annabella. Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO2. United States. doi:10.1063/1.4982933.
Wang, Honghong, An, Taicheng, and Selloni, Annabella. Thu . "Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO2". United States. doi:10.1063/1.4982933. https://www.osti.gov/servlets/purl/1465991.
@article{osti_1465991,
title = {Effect of reducible oxide–metal cluster charge transfer on the structure and reactivity of adsorbed Au and Pt atoms and clusters on anatase TiO2},
author = {Wang, Honghong and An, Taicheng and Selloni, Annabella},
abstractNote = {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 TiO2. Pt clusters interact much more strongly with the TiO2 support than Au clusters, and, with the exception of single Pt adatoms, generally behave as electron acceptors on reduced TiO2, 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 O2. 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 TiO2 surface and/or in the presence of co-adsorbed O2. Pt clusters interact strongly with co-adsorbed O2 and form Pt–O2 complexes that can easily accept electrons from reduced surfaces. In contrast, Au clusters donate charge to co-adsorbed O2 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 with several experimental observations and highlight the important role of excess surface electrons in the behavior of supported metal catalysts on reducible oxides},
doi = {10.1063/1.4982933},
journal = {Journal of Chemical Physics},
number = 18,
volume = 146,
place = {United States},
year = {Thu May 11 00:00:00 EDT 2017},
month = {Thu May 11 00:00:00 EDT 2017}
}

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Cited by: 2 works
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Works referenced in this record:

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495