Zhi Lin, Binglan Wu, Yucheng Huang, Kaini Zhang, Yiqing Wang, Ruizhe Wang, Fei Zhang, Jie Chen, Shaohua Shen
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.