Wang Jia-Rui, Song Kepeng, Luan Tian-Xiang, Cheng Ke, Wang Qiurong, Wang Yue, Yu William W, Li Pei-Zhou, Zhao Yanli
School of Chemistry and Chemical Engineering, Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion, Science Center for Material Creation and Energy Conversion, Shandong University, No. 27 Shanda South Road, Ji'nan, 250100, PR China.
School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371, Singapore, Singapore.
Nat Commun. 2024 Feb 10;15(1):1267. doi: 10.1038/s41467-024-45457-y.
Developing heterogeneous photocatalysts for the applications in harsh conditions is of high importance but challenging. Herein, by converting the imine linkages into quinoline groups of triphenylamine incorporated covalent organic frameworks (COFs), two photosensitive COFs, namely TFPA-TAPT-COF-Q and TFPA-TPB-COF-Q, are successfully constructed. The obtained quinoline-linked COFs display improved stability and photocatalytic activity, making them suitable photocatalysts for photocatalytic reactions under harsh conditions, as verified by the recyclable photocatalytic reactions of organic acid involving oxidative decarboxylation and organic base involving benzylamine coupling. Under strong oxidative condition, the quinoline-linked COFs show a high efficiency up to 11831.6 μmol·g·h and a long-term recyclable usability for photocatalytic production of HO, while the pristine imine-linked COFs are less catalytically active and easily decomposed in these harsh conditions. The results demonstrate that enhancing the linkage robustness of photoactive COFs is a promising strategy to construct heterogeneous catalysts for photocatalytic reactions under harsh conditions.
开发用于恶劣条件下应用的多相光催化剂具有高度重要性,但也具有挑战性。在此,通过将三苯胺掺入的共价有机框架(COF)中的亚胺键转化为喹啉基团,成功构建了两种光敏COF,即TFPA-TAPT-COF-Q和TFPA-TPB-COF-Q。所获得的喹啉连接的COF显示出改善的稳定性和光催化活性,使其成为恶劣条件下光催化反应的合适光催化剂,这通过涉及氧化脱羧的有机酸和涉及苄胺偶联的有机碱的可循环光催化反应得到验证。在强氧化条件下,喹啉连接的COF显示出高达11831.6 μmol·g·h的高效率以及用于光催化产生HO的长期可循环使用性,而原始的亚胺连接的COF在这些恶劣条件下催化活性较低且容易分解。结果表明,增强光活性COF的连接稳健性是构建用于恶劣条件下光催化反应的多相催化剂的一种有前景的策略。