光催化
材料科学
共价有机骨架
共价键
光化学
可见光谱
带隙
化学工程
催化作用
接受者
光电子学
有机化学
复合材料
化学
多孔性
工程类
物理
凝聚态物理
作者
Chenxiang Lin,Xiaolin Liu,Baoqiu Yu,Chaozheng Han,Lei Gong,Chiming Wang,Ying Gao,Yongzhong Bian,Jianzhuang Jiang
标识
DOI:10.1021/acsami.1c04880
摘要
Covalent organic frameworks (COFs) are promising crystalline materials for photocatalytic solar- to hydrogen-energy conversion due to the tunable chemical structures and energy band gaps. Herein, we report a chemical modification strategy for improving the photocatalytic activity of COFs. A benzene-1,3,5-tricarbaldehyde (BT)- and benzothiadiazole derivative-based two-dimensional donor–acceptor (D-A) COF, denoted as BT-COF, were fabricated and further modified by using an alternative electron-donating unit, 2-hydroxybenzene-1,3,5-tricarbaldehyde (HBT), to the polycondensation reaction, yielding HBT-COF with an enhanced internal D-A effect and hydrophilicity. Interestingly, the photocatalytic H2 production rate of HBT-COF reaches 19.00 μmol h–1, which is 5 times higher than that of BT-COF (3.40 μmol h–1) under visible light irradiation. The increase in photocatalytic activity of HBT-COF is rationally attributed to finely tuned energy levels and improved wettability, which in turn leads to broadened visible light absorption, efficient photoinduced charge separation and transfer, and enhanced interactions between the COF catalyst and reaction substrates. The present results demonstrate that a subtle structural modification can significantly modulate the band structure and interfacial property, thus providing a feasible strategy for the optimization of COF-based photocatalytic systems.
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