Xie Ke-Hui, Wang Guang-Bo, Huang Fang, Zhao Fei, Kan Jing-Lan, Chen Zi-Zheng, Cai Lei, Han Shu-Lin, Geng Yan, Dong Yu-Bin
College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Normal University, Jinan, PR China.
Shandong Province Key Laboratory of Medical Physics and Image Processing Technology, School of Physics and Electronics, Institute of Materials and Clean Energy, Shandong Normal University, Jinan, PR China.
Nat Commun. 2025 Apr 12;16(1):3493. doi: 10.1038/s41467-025-58839-7.
The exploration of stable and functional linkages by multicomponent reactions to enrich the stability and diversity of covalent organic frameworks (COFs) and to broaden their potential applications is of fundamental significance to the development of COFs. Herein, we report the facile construction of a set of benzo[f]quinoline-linked COFs (B[f]QCOFs) via one-pot three-component [4 + 2] cyclic condensation of aldehydes and aromatic amines with easy-to-handle triethylamine as the vinyl source. These B[f]QCOFs possess high crystallinity, good physico-chemical stability as well as significant light absorption ability. More importantly, the obtained B[f]QCOF-1 exhibits a superior HO production rate of 9025 μmol g h in pure water without any sacrificial agent under visible-light irradiation, surpassing most of the previously reported COF-based photocatalysts under comparable conditions. This work not only provides a general synthetic route for the preparation of fully conjugated COFs, but also helps the rational design of COF-based photocatalysts for efficient HO photosynthesis.
通过多组分反应探索稳定且具有功能性的连接方式,以增强共价有机框架(COFs)的稳定性和多样性,并拓宽其潜在应用,这对COFs的发展具有至关重要的意义。在此,我们报道了通过醛、芳香胺与易于操作的三乙胺作为乙烯基源进行一锅三组分[4 + 2]环缩合反应,简便地构建了一系列苯并[f]喹啉连接的COFs(B[f]QCOFs)。这些B[f]QCOFs具有高结晶度、良好的物理化学稳定性以及显著的光吸收能力。更重要的是,所制备的B[f]QCOF-1在可见光照射下于纯水中无需任何牺牲剂,展现出9025 μmol g⁻¹ h⁻¹的优异产氢速率,在可比条件下超过了大多数先前报道的基于COF的光催化剂。这项工作不仅为制备完全共轭的COFs提供了一条通用的合成路线,还有助于合理设计用于高效光催化产氢的基于COF的光催化剂。