期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 133, 期 34, 页码 13527-13533出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja204191t
关键词
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资金
- Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geological and Biosciences of the U.S. DOE [DE-AC02-05CH11231]
The design and development of metal-cluster-based heterogeneous catalysts wit l high activity, selectivity, and stability under solution-phase reaction conditions will enable their applications as recyclable catalysts in large-scale fine chemicals production. To achieve these required catalytic properties, a heterogeneous catalyst must contain specific catalytically active species in high concentration, and the active species must be stabilized on a solid catalyst support under solution-phase reaction conditions. These requirements pose a great challenge for catalysis research to design metal-cluster-based catalysts for solution-phase catalytic processes. Here, we focus on a silica-supported, polymer-encapsulated Pt catalyst for an electrophilic hydroalkoxylation reaction in toluene, which exhibits superior selectivity and stability against leaching under mild reaction conditions. We unveil the key factors leading to the observed superior catalytic performance by combining X-ray absorption spectroscopy (XAS) and reaction kinetic studies. On the basis of the mechanistic understandings obtained in this work, we also provide useful guidelines for designing metal-cluster-based catalyst for a broader range of reactions in the solution phase.
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