A Covalent Triazine‐Based Framework Consisting of Donor–Acceptor Dyads for Visible‐Light‐Driven Photocatalytic CO2 Reduction

Abstract Photocatalytic conversion of CO 2 into value‐added chemical fuels is a promising approach to address the depletion of fossil energy and environment‐related concerns. Tailor‐making the electronic properties and band structures of photocatalysts is pivotal to improve their efficiency and selectivity in photocatalytic CO 2 reduction. Herein, a covalent triazine‐based framework was developed containing electron‐donor triphenylamine and electron‐acceptor triazine components (DA‐CTF). The engineered π‐conjugated electron donor–acceptor dyads in DA‐CTF not only optimized the optical bandgap but also contributed to visible‐light harvesting and migration of photoexcited charge carriers. The activity of photocatalytic CO 2 reduction under visible light was significantly improved compared with that of traditional g‐C 3 N 4 and reported covalent triazine‐based frameworks. This study provides molecular‐level insights into the mechanism of photocatalytic CO 2 reduction.