Local structure of the zeolitic catalytically active site during reaction

被引:40
作者
van Bokhoven, JA [1 ]
van der Eerden, AMJ
Prins, R
机构
[1] ETH, Swiss Fed Inst Technol, CH-8093 Zurich, Switzerland
[2] Univ Utrecht, Debye Inst, NL-3584 CH Utrecht, Netherlands
关键词
D O I
10.1021/ja031755j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The structural changes of the catalytic active site that occur during catalytic reaction in an acidic zeolite are detected. The local structure of the zeolitic Brønsted active site is a distorted tetrahedrally coordinated aluminum that has three short and one long aluminum?oxygen bond. Using in situ Al K edge X-ray absorption spectroscopy, the adsorption of a reactive intermediate in the oligomerization of ethene changed the local structure of the catalytic active site; the long aluminum oxygen bond is partially relaxed. At increasingly higher temperature, extensive coking of the catalyst frees the Brønsted acid site from the reactive intermediate, restoring the asymmetric coordination. These measurements show that application of in situ Al K edge spectroscopy provides fundamental insight into the structure of zeolitic catalytically active sites during catalytic action. Copyright © 2004 American Chemical Society.
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收藏
页码:4506 / 4507
页数:2
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