期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 127, 期 37, 页码 12924-12932出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja052543k
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The Sri silicate zeolite, Sn-beta, has been shown to be an efficient, selective heterogeneous catalyst for Baeyer-Villiger oxidations. Using primarily a multishell fit to extended X-ray absorption fine structure (EXAFS) data, we show that the Sri does not randomly insert into the beta-zeolite structure but rather occupies identical, specific, crystallographic sites. These sites are the T5/T6 sites in the six-membered rings. Moreover, the Sri is substituted in pairs on opposite sides of these six-membered rings. We believe that it is the specific, uniform crystallographic location of the Sri in the beta crystal structure that leads to sites with uniform catalytic activity, and consequently to the high chemical selectivity demonstrated for this catalyst. This manifests itself in the almost enzyme-like selectivity of this catalyst in Baeyer-Villiger oxidations. This uniform site distribution of the Sn suggests that there is likely a symbiotic relationship between the structure directing agent in the zeolite synthesis and the Sri heteroatoms during the framework formation.
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