期刊
CHEMISTRY-AN ASIAN JOURNAL
卷 5, 期 1, 页码 78-86出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.200900399
关键词
gold; mechanism; oxidation; selectivity; styrene
资金
- U.S. Department of Energy [FG02-84-ER13289]
- National Science Foundation, Chemistry Division [CHE-0545335]
We demonstrate that intermolecular interactions, controlled by both oxygen and styrene coverage, alter reaction selectivity for styrene oxidation on oxygen-covered Au(111). Several partial oxidation products are formed-styrene oxide, acetophenone, benzoic acid, benzeneacetic acid, and phenylketene-in competition with combustion. The maximum ratio of the yields of styrene oxide to the total CO2 produced is obtained for the maximum styrene coverage for the first two layers (0.28 ML) adsorbed on Au(111) precovered with 0.2 ML of O. Furthermore, our reactivity and infrared studies support a mechanism whereby styrene oxidation proceeds via two oxa-metallacycle intermediates which, under oxygen-lean conditions, lead to the formation of styrene oxide, acetophenone, and phenylketene. Benzoate, identified on the basis of infrared reflection absorption spectroscopy, is converted into benzoic acid during temperature-programmed reaction. These results demonstrate the ability to tune the epoxidation selectivity using reactant coverages and provide important mechanistic insight into styrene oxidation reactions.
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