Mn-S chemical bond mediated Z-scheme photocatalyst boosting efficient H2 evolution with apparent quantum yield exceeding 32% under visible light

Abstract

Developing a highly effective solar-to-H2 conversion system is a promising strategy for carbon neutrality. Here, we report a chemically bonded Z-scheme photocatalyst by specifically linking the conduction band site of ZnIn2S4 with the valence band site of Mn0.3Cd0.7S1-x. Deviates from the typical van der Waals interactions between two semiconductors, the in-built robust binding force (Mn-S bond) and charge transfer channel facilitates the electron mobility, minimizes detrimental deep charge trapping, and prolongs the active charge lifetime from 983 ps to 4250 ps. The sulfur vacancies in Mn0.3Cd0.7S1-x are partially refilled by atoms of the same element in ZnIn2S4 during the in-situ formation of heterojunctions, which promotes and solidates the establishment of interfacial chemical bonds. The optimal photocatalyst achieves a high quantum efficiency of 32.71 % at 420 nm. This study offers a new insight into the development of Z-Scheme heterojunctions via a synergistic approach involving doping, vacancy filling and strong interfacial chemical bonds.