Two-Dimensional All-in-One Sulfide Monolayers Driving Photocatalytic Overall Water Splitting

For realizing scalable solar hydrogen synthesis, the development of visible-light-absorbing photocatalysts capable of overall water splitting is essential. Metal sulfides can capture visible light efficiently; however, their utilization in water splitting has long been plagued by the poor resilience against hole oxidation. Herein, we report that the ZnIn₂S₄ monolayers with dual defects (Ag dopants and nanoholes) accessed via cation exchange display stoichiometric H₂ and O₂ evolution in pure water under visible light irradiation. In-depth characterization and modeling disclose that the dual-defect structure endows the ZnIn₂S₄ monolayers with optimized light absorption and carrier dynamics. More significantly, the dual defects cooperatively function as active sites for water oxidation (Ag dopants) and reduction (nanoholes), thus leading to steady performance in photocatalytic overall water splitting without the assistance of cocatalysts. This work demonstrates a feasible way for fulfilling "all-in-one" photocatalyst design and manifests its great potential in addressing the stability issues associated with sulfide-based photocatalysts.