Synergistic Integration of Phosphorus-Configured Single-Atom Sites and Nanoclusters on Polymeric Carbon Nitride for Photocatalytic Overall Water Splitting via a Two-Electron Pathway

High Resolution Image Download MS PowerPoint Slide Polymeric carbon nitride (CN) suffers from inefficient charge-carrier transfer and sluggish water redox kinetics, despite its suitable band structure for photocatalytic overall water splitting (POWS). To address these limitations, atomically dispersed Ni–P 4 sites and Co 2 P nanoclusters are coanchored onto phosphorized CN (PCN) via a two-step impregnation–phosphatization method. The optimized Ni-PCN-Co 2 P photocatalyst achieves efficient overall water splitting via a two-electron pathway, producing H 2 and H 2 O 2 with an apparent quantum yield of 2.37% at 380 nm. It is revealed that the design of Ni–P 4 and Co 2 P dual sites not only lowers the energy barrier for H 2 production at the Ni–P 4 sites and facilitates H 2 O 2 formation via optimized adsorption of oxygen intermediates at the Co 2 P nanoclusters but also promotes charge separation and transfer within PCN, thereby collectively overcoming the intrinsic kinetics limitations for overall water splitting. This cooperative strategy of customizing the single-atom- and nanocluster-coanchored structure offers a feasible scheme for designing efficient photocatalysts for solar energy conversion.