Regulating redox sites for photocatalytic phenylcarbinol conversion and H2 production on lattice-matched Schottky junction

The photocatalytic coupling of selective phenylcarbinol oxidation with hydrogen evolution has attracted considerable attention as a promising dual-functional reaction system. Herein, a lattice-matched 2D/3D NiS/CdIn 2 S 4 (NiS/CIS) Schottky heterojunction is rationally designed for efficient dual-functional photocatalysis under visible light. Structural analyses confirm the uniform deposition of NiS nanosheets on octahedral CIS with a lattice mismatch below 5%, ensuring coherent interfacial contact. The optimal 3% NiS/CIS composite exhibits exceptional hydrogen and benzaldehyde production rates of 2636.4 and 2717.6 μmol g −1 h −1 , respectively—representing enhancements of 39.7 and 38.0 times over pristine CIS. The catalyst also demonstrates remarkable stability, retaining over >99.0% activity after six cycles. Mechanistic studies reveal that the Schottky junction facilitates spatial separation of photogenerated carriers: electrons migrate to NiS, prolonging charge carrier lifetimes and lowering the hydrogen evolution overpotential, while holes accumulate on CIS that facilitated phenylcarbinol adsorption to drive selective phenylcarbinol oxidation via a carbon-radical pathway. This work provides a viable approach for designing efficient bifunctional photocatalysts through lattice-matched interface engineering. Lattice-matched 2D/3D NiS/CdIn 2 S 4 Schottky junction was designed and prepared for efficiently separation and guided transfer of photogenerated electrons and holes into targeted redox sites, leading to efficiently and sustainably dual-functional photocatalysis. • Phenylcarbinol adsorption and H 2 evolution sites were regulated and spatial separated. • Photogenerated electrons and holes were efficiently separated and directly transferred into redox sites for targeted reactions. • Photocatalytic hydrogen production was enhanced by 38.7 times under visible light. • Lattice-matched Schottky junction showed a great potential for dual-functional photocatalysis.