期刊
SMALL
卷 17, 期 24, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202101017
关键词
covalent organic frameworks; functional group; hydrogen production; photocatalysis; reaction mechanism
类别
资金
- National Natural Science Foundation of China [21902051, 21773031]
- Natural Science Foundation of Fujian Province [2019J05090]
- Graphene Powder and Composite Research Center of Fujian Province [2017H2001]
- Subsidized Project for Postgraduates' Innovative Fund in Scientific Research of Huaqiao University [18013081032]
Adding cyano conjugation to a typical COF improves its stable photocatalytic rate and optimizes active centers for solar energy conversion.
2D covalent organic frameworks (COFs) are drawing intense attention in heterogenous photocatalysis due to their porous, crystalline, and tailor-made structures. For highly efficient solar-to-chemical energy conversion, revealing and modulating active centers in the skeletons of COFs are of great importance but encounter severe challenges. Herein, it is demonstrated that cyano conjugation on a typical beta-ketoenamine-linked COF via aldehyde-imine Schiff-base condensation contributes to an enhanced stable photocatalytic H-2-evolution rate of 1.8 mmol h(-1) g(-1) (lambda > 420 nm) with a superior apparent quantum yield of 2.12% at 420 nm, compared to pristine COFs. Both experimental results and density functional theory calculations disclose that the cyano conjugation can efficiently improve photoinduced charge separation and effectively decrease the energy barrier for H-intermediate generation on the carbonyl oxygen sites of the functionalized COFs. These findings present a precise organic functionalization strategy to optimize active centers on COF-based photocatalysts for the practical applications.
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