期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 10, 页码 2594-2598出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201609317
关键词
interfaces; kinetics; oxidation; phase transitions; surface chemistry
资金
- Cluster of Excellence Engineering of Advanced Materials (EAM) at the Friedrich-Alexander-University Erlangen Nurnberg
- DFG (Deutsche Forschungsgemeinschaft)
- European Research Council through the ERC-StartingGrant THEOFUN [259608]
- Alexander von Humboldt Foundation
- National Science Foundation [CBET-1032979, CHE-1505607]
- DFG [INST40/467-1 FUGG]
Detailed knowledge of the structure and degree of oxidation of platinum surfaces under operando conditions is essential for understanding catalytic performance. However, experimental investigations of platinum surface oxides have been hampered by technical limitations, preventing in situ investigations at relevant pressures. As a result, the time-dependent evolution of oxide formation has only received superficial treatment. In addition, the amorphous structures of many surface oxides have hindered realistic theoretical studies. Using near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) we show that a time scale of hours (t >= 4 h) is required for the formation of platinum surface oxides. These experimental observations are consistent with ReaxFF grand canonical Monte Carlo (ReaxFF-GCMC) calculations, predicting the structures and coverages of stable, amorphous surface oxides at temperatures between 430-680K and an O-2 partial pressure of 1 mbar.
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