Solar Carboxylation Using CO₂: Interfacially Synthesized Flexible Covalent Organic Frameworks Film as a Photocatalyst for Highly Selective Solar Carboxylation of Arylamines with CO₂

Abstract

Carbon dioxide (CO 2 ) 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 2 is still an ongoing challenge. Here, we report an interfacially synthesized visiblelight-active Ni(II)-integrated covalent organic frameworks (TaTpBpy-Ni COFs) film as a photocatalyst for efficient CO 2 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 2 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 2 .

Meglumine Encapsulated CuI: A Green Heterogeneous Catalyst Derived from Low Value Biomass Meglumine to Access 1,2,3-Triazole Scaffolds

“…Ham et al prepared an acid-doped graphitic carbon nitride (g-C 3 N 4 )-based heterogeneous catalyst for the production of biodiesel . Baeg et al developed Ni­(II)-integrated COFs (TaTpBpy-Ni) which can be successfully used for efficient CO 2 conversion into carboxylic acid under ambient conditions . Li and co-workers prepared a Co/Ni-based dual-atom heterogeneous catalyst which efficiently reduced lignin-derived phenols to cyclohexanols via selective cleavage of the Csp 2 -OCH 3 bond .…”