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Title: Methane Chemisorption on Oxide‐Supported Pt Single Atom

Journal Article · · ChemPhysChem
 [1];  [2];  [3]; ORCiD logo [1]
  1. Department of Chemistry University of California Riverside, California 92521 United States
  2. Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge, Tennessee 37831 United States
  3. Department of Chemical and Petroleum Engineering University of Kansas Lawrence KS 66045
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Abstract Methane chemisorption has been recently demonstrated on the rutile IrO 2 (110) surface. However, it remains unclear how the general requirements are for methane chemisorption or complexation with a single atom on an oxide surface. By exploring methane adsorption on Pt 1 substitutionally doped on many rutile‐type oxides using hybrid density functional theory, we show that the occupancy of the Pt d z 2 orbital is the key to methane chemisorption. Pt single atom on the semiconducting or wide‐gap oxides such as TiO 2 and GeO 2 strongly chemisorbs methane, because the empty Pt d z 2 orbital is located in the gap and can effectively accept σ‐electron donation from the methane C−H bond. In contrast, Pt single atom on metallic oxides such as IrO 2 and RuO 2 does not chemisorb methane, because the Pt d z 2 orbital strongly mixes with the support‐oxide electronic states and become more occupied, losing its ability to chemisorb methane. This study sheds further light on the impact of the interaction between a Pt single atom and the oxide support on methane adsorption.

Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-05CH11231; SC0014561
OSTI ID:
1545401
Journal Information:
ChemPhysChem, Journal Name: ChemPhysChem Journal Issue: 17 Vol. 20; ISSN 1439-4235
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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