期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 50, 页码 18290-18294出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201912344
关键词
covalent organic frameworks; hydrogen production; photocatalysis; nanostructures; semiconductors
资金
- NSFC [21773031]
- Natural Science Foundation of Fujian Province of P. R. China [2018J01686]
- Science and Technology Project of Education Office of Fujian Province of P.R. China [JT180020]
- State Key Laboratory of Photocatalysis on Energy and Environment [SKLPEE-2017A01, SKLPEE-2017B02]
A metal-insulator-semiconductor (MIS) photosystem based on covalent organic framework (COF) semiconductors was designed for robust and efficient hydrogen evolution under visible-light irradiation. A maximal H-2 evolution rate of 8.42 mmol h(-1) g(-1) and a turnover frequency of 789.5 h(-1) were achieved by using a MIS photosystem prepared by electrostatic self-assembly of polyvinylpyrrolidone (PVP) insulator-capped Pt nanoparticles (NPs) with the hydrophilic imine-linked TP-COFs having =C=O-H-N= hydrogen-bonding groups. The hot pi-electrons in the photoexcited n-type TP-COF semiconductors can be efficiently extracted and tunneled to Pt NPs across an ultrathin PVP insulating layer to reduce protons to H-2. Compared to the Schottky-type counterparts, the COF-based MIS photosystems give a 32-fold-enhanced carrier efficiency, attributed to the combined enhancement of photoexcitation rate, charge separation, and oxidation rate of holes accumulated in the valence band of the TP-COF semiconductor.
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