Interlayer Photoelectron Transfer Boosted by Bridged Ru^IV Atoms in GaS Nanosheets for Efficient Water Splitting

Photocatalytic water splitting over layered nanosheet (NS) catalysts has caught a lot of attention for renewable hydrogen fuel production. However, the weak van der Waals interlayer interactions make it a great challenge to realize an effective dissociation of photogenerated excitons and efficient charge transfer across the interior of layered catalysts during the photocatalysis process. Here, we propose an intercalation strategy of high-valence Ru^IV atoms to render two-dimensional GaS NS photocatalysts with rapid electron-hole dissociation and long photocarrier lifetime in visible-light-driven water splitting. Experimental and theoretical results unravel that the intercalated single-site Ru, confined in interlayer of GaS NSs, with a hexagonal structural configuration of "Ru₁-S₆", can serve as an electron-trapped high-speed channel toward simultaneously accelerating electron-hole pairs dissociation and promoting photoelectron transportation through the van der Waals interlayer. Consequently, the as-developed Ru-intercalated GaS NSs can give a notable H₂ production rate of 340 μmol g^-1 h^-1 under visible-light irradiation and an apparent yield of 7% at 420 nm, 38 times that of pure GaS NSs. This study opens up a feasible way for a new design of highly active layered photocatalysts toward high-efficiency solar energy conversion.