Metallic 1T-MoS₂/ZnIn₂S₄ heterojunction photocatalysts for enhanced photoredox reaction via guiding charge migration

The synergistic coupling of photocatalytic hydrogen evolution and α-C–H bond activation reactions enables the comprehensive harnessing of the redox potential of semiconductor catalysts, yielding exceptionally high utilization of photocatalytic technology. Guiding and optimizing the charge migration within photocatalysts constitute a pivotal strategy for achieving remarkable overall solar energy conversion efficiency. Here, we engineer metallic 1T-MoS₂/ZnIn₂S₄ heterojunction photocatalysts by incorporating the distinctive 1T-MoS₂ structure into the intricate flower-like ZnIn₂S₄ framework. The modulation of charge migration within the 1T-MoS₂/ZnIn₂S₄ heterojunction photocatalysts is induced by an engineered interfacial electric field and an efficient hole transfer agent (benzyl alcohol). Steering charge migration results in an impressive 4.6-fold enhancement in photocatalytic performance compared with the pristine ZnIn₂S₄. Moreover, comprehensive spectroscopy and theoretical analyses prove that the interfacial electric field facilitates the rapid electron transfer along the direction from the [S–Mo] to [In−S] layers. Simultaneously, swift hole capture is achieved by dehydrogenating the α-C–H bond in benzyl alcohol.