Ternary Monolithic ZnS/CdS/rGO Photomembrane with Desirable Charge Separation/Transfer Routes for Effective Photocatalytic and Photoelectrochemical Hydrogen Generation

Abstract Highly efficient and easy recyclable monolithic photocatalysts with ideal separation/transport route for photogenerated charge carriers are much desired. In this work, a ZnO seed‐induced growth approach is developed to fabricate a ternary monolithic photomembrane, that is, ZnS/CdS heterojunction nanorods in situ grow into the interspaces of multilayer reduced graphene oxide (rGO) sheets (denoted as ZnS/CdS/rGO). The monolithic ZnS/CdS/rGO photomembrane can serve as an efficient visible‐light photoactive membrane for photocatalytic (PC) or photoelectrochemical (PEC) hydrogen generation. The fast electron transport of 1D CdS nanorods, the excellent electronic conductivity of multilayer stacked rGO sheets, the intense visible‐light absorption of CdS, the unique hierarchical structure, and double heterojunctions (ZnS/CdS and CdS/rGO) efficiently boost the photogenerated electron‐hole pairs separation and transfer across the interfacial domain of the photomembrane under visible‐light irradiation. Furthermore, the superior stability and reusability of the photomembrane is achieved by the ideal process of photogenerated electron‐hole pair separation/transfer, i.e., holes transfer to ZnS and electrons transfer to rGO to inhibit CdS from photocorrosion.