期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 39, 页码 16902-16909出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202006925
关键词
charge transfer; covalent organic frameworks; halogenation; photocatalytic water splitting; solar energy conversion
资金
- National Key Research and Development Program of China [2017YFA0207500]
- National Natural Science Foundation of China [51973153, 21875235]
- Natural Science Foundation of Tianjin City [17JCJQJC44600]
- Postdoctoral Science Foundation of China [BX20200317]
Two-dimensional covalent organic frameworks (2D COFs), an emerging class of crystalline porous polymers, have been recognized as a new platform for efficient solar-to-hydrogen energy conversion owing to their pre-designable structures and tailor-made functions. Herein, we demonstrate that slight modulation of the chemical structure of a typical photoactive 2D COF (Py-HTP-BT-COF) via chlorination (Py-ClTP-BT-COF) and fluorination (Py-FTP-BT-COF) can lead to dramatically enhanced photocatalytic H(2)evolution rates (HER=177.50 mu mol h(-1)with a high apparent quantum efficiency (AQE) of 8.45 % for Py-ClTP-BT-COF). Halogen modulation at the photoactive benzothiadiazole moiety can efficiently suppress charge recombination and significantly reduce the energy barrier associated with the formation of H intermediate species (H*) on polymer surface. Our findings provide new prospects toward design and synthesis of highly active organic photocatalysts toward solar-to-chemical energy conversion.
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