Arylboron functional covalent organic frameworks for synergistic photocatalytic hydrogen evolution,Journal of Materials Chemistry A

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Arylboron functional covalent organic frameworks for synergistic photocatalytic hydrogen evolution
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-08-08 , DOI: 10.1039/d2ta04748a
Xuan Wu ₁ , Mingcai Zhang ₁ , Yusong Xia ₁ , Chenglong Ru ₁ , Peiyan Chen ₁ , Hao Zhao _{1,

2} , Lian Zhou ₃ , Chenliang Gong ₁ , Jincai Wu ₁ , Xiaobo Pan _{1,

3}

Affiliation

Covalent organic frameworks (COFs) are attractive organic polymers that can serve as promising photocatalysts for water reduction. Herein, two novel arylboron functional COFs, TAB-TFB-COF and TAB-TFP-COF, were synthesized and their photocatalytic hydrogen evolution ability was evaluated. Under visible light irradiation (λ > 420 nm), the hydrogen evolution rate of TAB-TFP-COF is 666.4 μmol g⁻¹ h⁻¹ at the stationary point (0.5 g L⁻¹), reaching 1140 μmol g⁻¹ h⁻¹ after long cycle stabilization, which is 76 and 1.4 times higher than that of TAB-TFB-COF (8.8 μmol g⁻¹ h⁻¹) and TAB-TFP-CMP (489.6 μmol g⁻¹ h⁻¹), respectively. It is demonstrated that the construction of β-ketoenamine improves the separation and transfer ability of light-induced charge carriers. Specifically, F⁻-loading experiments and density functional theory (DFT) calculations suggested that the introduction of arylboron units promoted intramolecular charge transfer which was conducive to photocatalytic reactions. Overall, the good photocatalytic performance of TAB-TFP-COF is due to the synergistic catalytic effect of arylboron and β-ketoenamine dual acceptors. The arylboron functionalization may open up new avenues for the development of COFs in photocatalytic materials, making them promising for a variety of applications as advanced solar energy conversion platforms.

中文翻译：

用于协同光催化析氢的芳基硼功能共价有机框架

共价有机骨架（COFs）是有吸引力的有机聚合物，可以作为有前途的减水光催化剂。在此，合成了两种新型芳基硼功能 COF，TAB-TFB-COF和TAB-TFP-COF，并评估了它们的光催化析氢能力。在可见光照射（λ > 420 nm）下， TAB-TFP-COF在静止点（0.5 g L ^-1 ）的析氢速率为666.4 μmol g ^-1 h ^-1，达到1140 μmol g ^-1 h ^{- 1}长循环稳定后，分别是TAB-TFB-COF (8.8 μmol g ^-1 ) 的 76 和 1.4 倍h ^-1 ) 和TAB-TFP-CMP (489.6 μmol g ^-1 h ^-1 )，分别。结果表明，β-酮烯胺的构建提高了光诱导载流子的分离和转移能力。具体而言，F ^-负载实验和密度泛函理论 (DFT) 计算表明，芳基硼单元的引入促进了分子内电荷转移，有利于光催化反应。总体而言，TAB-TFP-COF具有良好的光催化性能是由于芳基硼和β-酮烯胺双受体的协同催化作用。芳基硼功能化可能为光催化材料中 COF 的开发开辟新途径，使其有望作为先进的太阳能转换平台应用于各种应用。

更新日期：2022-08-08

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