▎ 摘　　要

Single-layer graphene (SLG) has drawn considerable interest in photoelectrochemical (PEC) cells due to its atomically flat pinhole-free structure and remarkable in-plane carrier mobility. It is challenging, however, to obtain efficient SLG-modified photoelectrodes for PEC water splitting mainly due to the inefficient charge transfer interface. Here, a transition metal oxide/SLG/transition metal sandwich structure modified n-Si-based model photoanode is constructed to regulate the interfacial charge transfer behavior for enhanced PEC water oxidation performance. In this sandwich configuration, SLG tailors the morphology, structure, and work function properties of surface metal electrocatalysts to obtain both higher thermodynamic photovoltage and faster kinetical charge transfer at the semiconductor/electrolyte interface. In addition, SLG promotes the surface catalytic reaction as an effective charge trap and storage layer. This study provides a new structural design to engineer the SLG interfacial properties for high-performance energy conversion devices.