Singh Chandani, Kim Jae Young, Park No-Joong, Kim Chul Ung, Yadav Rajesh Kumar, Baeg Jin-Ook
CO2 Energy Research Center, Korea Research Institute of Chemical Technology (KRICT), 100 Jang-dong, Yuseong, Daejeon 34114, Republic of Korea.
Department of Chemistry and Environmental Science, Madan Mohan Malaviya University of Technology, Gorakhpur, Uttar Pradesh 273016, India.
ACS Appl Mater Interfaces. 2024 Jun 19;16(24):31085-31097. doi: 10.1021/acsami.4c03688. Epub 2024 Jun 5.
Carbon dioxide (CO) conversion into value-added chemicals/fuels by utilizing solar energy is a sustainable way to mitigate our dependence on fossil fuels and stimulate a carbon-neutral economy. However, the efficient and affordable conversion of CO is still an ongoing challenge. Here, we report an interfacially synthesized visible-light-active Ni(II)-integrated covalent organic frameworks (TaTpBpy-Ni COFs) film as a photocatalyst for efficient CO conversion into carboxylic acid under ambient conditions. Notably, the TaTpBpy-Ni COFs film showed excellent photocatalytic activity for the carboxylation of various arylamines with CO to the corresponding arylcarboxylic acid via C-N bond activation under solar-light irradiation. Moreover, this carboxylation protocol exhibits mild reaction conditions and good functional group tolerance without the necessity of using stoichiometric metallic reductants. This work shows a benchmark example of not only the interfacially synthesized COFs film used as a photocatalyst for solar-light energy utilization but also the selective solar chemical production system of arylcarboxylic acid directly from CO.
利用太阳能将二氧化碳（CO）转化为高附加值化学品/燃料是减轻我们对化石燃料依赖并推动碳中性经济发展的可持续途径。然而，CO的高效且经济可行的转化仍然是一个持续存在的挑战。在此，我们报道了一种界面合成的可见光活性镍（II）集成共价有机框架（TaTpBpy-Ni COFs）薄膜，作为在环境条件下将CO高效转化为羧酸的光催化剂。值得注意的是，TaTpBpy-Ni COFs薄膜在太阳光照射下，通过C-N键活化，对各种芳胺与CO羧基化生成相应芳基羧酸表现出优异的光催化活性。此外，该羧基化反应方案反应条件温和，对官能团耐受性良好，无需使用化学计量的金属还原剂。这项工作不仅展示了界面合成的COFs薄膜用作太阳光能利用光催化剂的一个基准示例，还展示了直接由CO制备芳基羧酸的选择性太阳能化学生产系统。
