Layered Heterostructures of Ultrathin Polymeric Carbon Nitride and ZnIn2S4 Nanosheets for Photocatalytic CO2 Reduction

Abstract The rational construction of heterostructures by using layered semiconductors with two‐dimensional (2D) nanosheet configurations is promising to improve the efficiency of CO 2 photoreduction. Herein, the fabrication of layered heterojunction photocatalysts (PCN/ZnIn 2 S 4 ) by in situ growth of 2D ZnIn 2 S 4 nanosheets on the surfaces of ultrathin polymeric carbon nitride (PCN) layers is presented for greatly enhanced CO 2 conversion with visible light. The solution‐processed self‐assembly strategy renders the building of uniform and intimate junctions between PCN layers and ZnIn 2 S 4 subunits, which remarkably accelerates the separation and transfer of photogenerated charge carriers. In addition, the layered composites can also promote CO 2 adsorption and strengthen the visible‐light absorption. Consequently, the optimized PCN/ZnIn 2 S 4 sheet‐shaped composite shows reinforced photoactivity for deoxygenative CO 2 conversion, affording a high CO‐production rate of 44.6 μmol h −1 , which is 223 times higher than that of the pristine PCN nanosheets. Moreover, the heterojunction photocatalyst also exhibits high stability during repeated runs for five cycles.