Rational Modification of Two-Dimensional Donor–Acceptor Covalent Organic Frameworks for Enhanced Visible Light Photocatalytic Activity,ACS Applied Materials & Interfaces

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Rational Modification of Two-Dimensional Donor–Acceptor Covalent Organic Frameworks for Enhanced Visible Light Photocatalytic Activity
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-07 , DOI: 10.1021/acsami.1c04880
Chenxiang Lin ₁ , Xiaolin Liu ₁ , Baoqiu Yu ₁ , Chaozheng Han ₁ , Lei Gong ₁ , Chiming Wang ₁ , Ying Gao ₁ , Yongzhong Bian _{1,

2} , Jianzhuang Jiang _{1,

3}

Affiliation

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.

中文翻译：

二维供体-受体共价有机骨架的合理修饰以增强可见光光催化活性

由于可调节的化学结构和能带隙，共价有机框架 (COF) 是用于光催化太阳能到氢能转换的有前途的晶体材料。在此，我们报告了一种用于提高 COF 光催化活性的化学修饰策略。一种基于苯-1,3,5-三甲醛 (BT)-和苯并噻二唑衍生物的二维供体-受体 (DA) COF，表示为 BT-COF，通过使用替代电子供体单元进一步修饰， 2-羟基苯-1,3,5-三甲醛 (HBT) 进行缩聚反应，产生具有增强的内部 DA 效应和亲水性的 HBT-COF。有趣的是，HBT-COF的光催化 H ₂产率达到 19.00 μmol h ^–1，在可见光照射下比 BT-COF (3.40 μmol h ^–1 )高 5 倍。HBT-COF 光催化活性的增加合理地归因于精细调整的能级和改善的润湿性，这反过来导致可见光吸收变宽、有效的光诱导电荷分离和转移以及 COF 催化剂与反应底物之间的相互作用增强。目前的结果表明，细微的结构修饰可以显着调节能带结构和界面性质，从而为优化基于 COF 的光催化体系提供可行的策略。

更新日期：2021-06-16

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