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

Photocatalytic conversion of CO2 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 CO2 reduction. Herein, a covalent triazine-based framework was developed containing electron-donor triphenylamine and electron-acceptor triazine components (DA-CTF). The engineered pi-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 CO2 reduction under visible light was significantly improved compared with that of traditional g-C3N4 and reported covalent triazine-based frameworks. This study provides molecular-level insights into the mechanism of photocatalytic CO2 reduction.