期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 13, 页码 5326-5331出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201915537
关键词
active-site distance; dehydrogenation; metal-organic frameworks; photocatalysis; porphyrins
资金
- National Natural Science Foundation of China [91545205, 91622103, 21971199]
- National Key research and Development Project [2018YFA0704000]
- Innovation Team of Wuhan University [2042017kf0232]
Discoveries of the accurate spatial arrangement of active sites in biological systems and cooperation between them for high catalytic efficiency are two major events in biology. However, precise tuning of these aspects is largely missing in the design of artificial catalysts. Here, a series of metal-organic frameworks (MOFs) were used, not only to overcome the limit of distance between active sites in bio-systems, but also to unveil the critical role of this distance for efficient catalysis. A linear correlation was established between photocatalytic activity and the reciprocal of inter active-site distance; a smaller distance led to higher activity. Vacancies created at selected crystallographic positions of MOFs promoted their photocatalytic efficiency. MOF-525-J33 with 15.6 angstrom inter active-site distance and 33 % vacancies exhibited unprecedented high turnover frequency of 29.5 h(-1) in visible-light-driven acceptorless dehydrogenation of tetrahydroquinoline at room temperature.
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