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Three-Component Donor−π–Acceptor Covalent–Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-14 , DOI: 10.1021/jacs.2c11893 Ziping Li 1 , Tianqi Deng 2, 3 , Si Ma 1 , Zhenwei Zhang 1 , Gang Wu 2 , Jiaao Wang 4 , Qizhen Li 5 , Hong Xia 6 , Shuo-Wang Yang 2 , Xiaoming Liu 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-03-14 , DOI: 10.1021/jacs.2c11893 Ziping Li 1 , Tianqi Deng 2, 3 , Si Ma 1 , Zhenwei Zhang 1 , Gang Wu 2 , Jiaao Wang 4 , Qizhen Li 5 , Hong Xia 6 , Shuo-Wang Yang 2 , Xiaoming Liu 1
Affiliation
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Two-dimensional covalent–organic frameworks (2D COFs) have recently emerged as great prospects for their applications as new photocatalytic platforms in solar-to-hydrogen conversion; nevertheless, their inefficient solar energy capture and fast charge recombination hinder the improvement of photocatalytic hydrogen production performance. Herein, two photoactive three-component donor−π–acceptor (TCDA) materials were constructed using a multicomponent synthesis strategy by introducing electron-deficient triazine and electron-rich benzotrithiophene moieties into frameworks through sp2 carbon and imine linkages, respectively. Compared with two-component COFs, the novel TCDA-COFs are more convenient in regulating the inherent photophysical properties, thereby realizing outstanding photocatalytic activity for hydrogen evolution from water. Remarkably, the first sp2 carbon-linked TCDA-COF displays an impressive hydrogen evolution rate of 70.8 ± 1.9 mmol g–1 h–1 with excellent reusability in the presence of 1 wt % Pt under visible-light illumination (420–780 nm). Utilizing the combination of diversified spectroscopy and theoretical prediction, we show that the full π-conjugated linkage not only effectively broadens the visible-light harvesting of COFs but also enhances charge transfer and separation efficiency.
中文翻译：
用于促进光催化析氢的三组分供体-π-受体共价-有机框架
二维共价有机框架 (2D COF) 最近出现，作为太阳能-氢转化中的新型光催化平台，具有广阔的应用前景；然而，它们低效的太阳能捕获和快速电荷复合阻碍了光催化制氢性能的提高。在此，通过 sp 2将缺电子三嗪和富电子苯并三噻吩部分引入骨架，使用多组分合成策略构建了两种光活性三组分供体-π-受体 (TCDA) 材料碳和亚胺连接，分别。与双组分COFs相比，新型TCDA-COFs更易于调节固有的光物理性质，从而实现出色的水析氢光催化活性。值得注意的是，第一个 sp 2碳连接的 TCDA-COF 显示出令人印象深刻的 70.8 ± 1.9 mmol g –1 h –1的析氢速率，在可见光照射（420–780 nm）下，在 1 wt% Pt 的存在下具有出色的可重复使用性). 利用多样化的光谱学和理论预测的结合，我们表明完整的 π 共轭键不仅有效地拓宽了 COF 的可见光收集，而且还提高了电荷转移和分离效率。
更新日期：2023-03-14
中文翻译：
用于促进光催化析氢的三组分供体-π-受体共价-有机框架
二维共价有机框架 (2D COF) 最近出现，作为太阳能-氢转化中的新型光催化平台，具有广阔的应用前景；然而，它们低效的太阳能捕获和快速电荷复合阻碍了光催化制氢性能的提高。在此，通过 sp 2将缺电子三嗪和富电子苯并三噻吩部分引入骨架，使用多组分合成策略构建了两种光活性三组分供体-π-受体 (TCDA) 材料碳和亚胺连接，分别。与双组分COFs相比，新型TCDA-COFs更易于调节固有的光物理性质，从而实现出色的水析氢光催化活性。值得注意的是，第一个 sp 2碳连接的 TCDA-COF 显示出令人印象深刻的 70.8 ± 1.9 mmol g –1 h –1的析氢速率，在可见光照射（420–780 nm）下，在 1 wt% Pt 的存在下具有出色的可重复使用性). 利用多样化的光谱学和理论预测的结合，我们表明完整的 π 共轭键不仅有效地拓宽了 COF 的可见光收集，而且还提高了电荷转移和分离效率。
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