期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 117, 期 4, 页码 1748-1753出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp309990e
关键词
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资金
- U.S. Department of Energy, Division of Chemical Sciences, Geosciences and Biosciences Division [DE-AC02-98CH10886]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- National Scientific Foundation of China (NSFC) [20876062, 21076089]
- China Scholarship Council
- South China University of Technology for the Study Abroad Scholarship
- DOE-BES
- Division of Chemical Sciences
- NSF Partnership for International Research and Education [OISE 0730277]
- Air Products & Chemicals, Inc.
- Department of Energy's Office of Biological and Environmental Research located at PNNL
- CNM
- NCCS
- ORNL
- U.S. Department of Energy, Office of Science [DE-AC02-06CH11357, DEAC05-00OR22725, DE-AC02-05CH11231]
The kinetics of the oxygen reduction reaction (ORR) was investigated in acid solutions on Pt monolayers that were deposited on carbon-supported Ru nanoparticles using the rotating disk electrode technique. The Pt mass and specific ORR activities greatly depend on the number of Pt monolayers, and the optimum activity occurs with two Pt monolayers. Density functional theory calculations showed that Pt overlayers destabilize O* and OH* with respect to pure Pt, leading to more favorable hydrogenation kinetics. However, with only a single Pt overlayer, the destabilization is too much, and O-O bond breaking becomes rate limiting. Two to three Pt monolayers supported on the Ru core of our nanoparticles lead to increased activity. This work demonstrates that one can modulate the ORR activity of Pt monolayers supported on other metals by eliminating a part of the ligand effect by increasing the thickness of the Pt shell on top of the supporting metal surface.
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