期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 31, 页码 12909-12916出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202001701
关键词
oxygen poisoning; photocatalysis; Pt catalysts; reaction order; semiconductors
资金
- National Key R&D Program of China [2016YFA0202801]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020400]
- National Natural Science Foundation of China [21776271, CSC 201804910082]
- CAS Interdisciplinary Innovation Team [BK2018001]
- China Postdoctoral Science Foundation [2017M621171]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-FG02-03ER15476]
- Laboratory Directed Research and Development Program through Brookhaven National Laboratory under U.S. Department of Energy [LDRD 20-040, DE-SC0012704]
Photo-thermo catalysis, which integrates photocatalysis on semiconductors with thermocatalysis on supported nonplasmonic metals, has emerged as an attractive approach to improve catalytic performance. However, an understanding of the mechanisms in operation is missing from both the thermo- and photocatalytic perspectives. Deep insights into photo-thermo catalysis are achieved via the catalytic oxidation of propane (C3H8) over a Pt/TiO2-WO3 catalyst that severely suffers from oxygen poisoning at high O-2/C3H8 ratios. After introducing UV/Vis light, the reaction temperature required to achieve 70 % conversion of C3H8 lowers to a record-breaking 90 degrees C from 324 degrees C and the apparent activation energy drops from 130 kJ mol(-1) to 11 kJ mol(-1). Furthermore, the reaction order of O-2 is -1.4 in dark but reverses to 0.1 under light, thereby suppressing oxygen poisoning of the Pt catalyst. An underlying mechanism is proposed based on direct evidence of the in-situ-captured reaction intermediates.
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