Tailoring defects in In2S3/Zn0.3Cd0.7S heterojunctions for efficient photocatalytic CO2 conversion

Defect engineering is a highly effective approach to regulate the electronic structure of the catalyst surface, widely employed in the field of photocatalytic energy conversion. In this study, we have successfully synthesized a novel dual-defective In2S3/Zn0.3Cd0.7S (IS/ZCS) heterojunction structure via a self-assembly method, composed of Zn-vacancy-rich Zn0.3Cd0.7S and S-vacancy-rich In2S3. Under visible light illumination, 3% IS/ZCS sample exhibits remarkable photocatalytic performance in the synergistic reaction of CO2 reduction and 4-chlorobenzyl alcohol (Cl-PhCH2OH) oxidation with the CO yield significantly improved by a factor of 3.5 and 51 compared to that of ZCS and IS, respectively. The combined experimental data and theoretical calculations demonstrate that the dual-defective structure and Z-scheme transfer mode are the key factors behind the enhanced photocatalytic activity, providing more active sites and effectively improving the utilization of photogenerated charge carriers (PCCs). Moreover, the reaction pathway and catalytic mechanism of photocatalytic CO2 reduction were elucidated by the in-situ FTIR technique combined with DFT calculations, monitoring the intermediate and final products during the reaction period. Our results provide a powerful example of designing novel heterojunction photocatalysts with high activity and accelerating the separation of PCCs, with broad implications for the development of efficient photocatalytic systems.