Metal Oxide/Graphene/Metal Sandwich Structure for Efficient Photoelectrochemical Water Oxidation

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 we construct a transition metal oxide/SLG/transition metal sandwich structure modified n-Si-based model photoanode 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. Our work provides a new structural design to engineer the SLG interfacial properties for high-performance energy conversion devices.