Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 17, Pages 9642-9649Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016618
Keywords
covalent organic frameworks; dynamic equilibrium; electron-transfer mediator; photocatalytic hydrogen evolution; viologen
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Funding
- National Natural Science Foundation of China [51973039, 21774023, 51633001]
- STCSM [18520744800]
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The study integrates cyclic diquats into a 2D COF platform, promoting consecutive electron transfer in photochemical processes through multi-component cooperation. The resulting materials combine photosensitizing units and ETMs into one system, exhibiting enhanced hydrogen evolution rate and sustained performance.
Electron transfer is the rate-limiting step in photocatalytic water splitting. Viologen and its derivatives are able to act as electron-transfer mediators (ETMs) to facilitate the rapid electron transfer from photosensitizers to active sites. Nevertheless, the electron-transfer ability often suffers from the formation of a stable dipole structure through the coupling between cationic-radical-containing viologen-derived ETMs, by which the electron-transfer process becomes restricted. Herein, cyclic diquats, a kind of viologen-derived ETM, are integrated into a 2,2 '-bipyridine-based covalent organic framework (COF) through a post-quaternization reaction. The content and distribution of embedded diquat-ETMs are elaborately controlled, leading to the favorable site-isolated arrangement. The resulting materials integrate the photosensitizing units and ETMs into one system, exhibiting the enhanced hydrogen evolution rate (34600 mu mol h(-1) g(-1)) and sustained performances when compared to a single-module COF and a COF/ETM mixture. The integration strategy applied in a 2D COF platform promotes the consecutive electron transfer in photochemical processes through the multi-component cooperation.
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