Mo‐Modified ZnIn2S4@NiTiO3 S‐Scheme Heterojunction with Enhanced Interfacial Electric Field for Efficient Visible‐Light‐Driven Hydrogen Evolution

Abstract Designing and developing visible‐light‐responsive materials for solar to chemical energy is an efficient and promising approach to green and sustainable carbon‐neutral energy systems. Herein, a facile in situ growth hydrothermal strategy using Mo‐modified ZnIn 2 S 4 (Mo‐ZIS) nanosheets coupled with NiTiO 3 (NTO) microrods to synthesize multifunctional Mo‐modified ZIS wrapped NTO microrods (Mo‐ZIS@NTO) photocatalyst with enhanced interfacial electric field (IEF) effect and typical S‐scheme heterojunction is reported. Mo‐ZIS@NTO catalyst possesses wide‐spectrum light absorption properties, excellent visible light‐to‐thermal energy effect, electron mobility, charges transfer, and strong IEF and exhibits excellent solar‐to‐chemical energy conversion for efficient visible‐light‐driven photocatalytic hydrogen evolution. Notably, the engineered Mo 1.4 ‐ZIS@NTO catalyst exhibits superior performance with H 2 evolution rate of up to 14.06 mmol g −1 h − 1 and the apparent quantum efficiency of 44.1% at 420 nm. The scientific explorations provide an in‐depth understanding of microstructure, S‐scheme heterojunction, enhanced IEF, Mo‐dopant facilitation effect. Moreover, the theoretical simulations verify the critical role of Mo element in promoting the adsorption and activation of H 2 O molecules, modulating the H adsorption behavior on active S sites, and thus accelerating the overall catalytic efficiency. The photocatalytic hydrogen evolution mechanism via S‐scheme heterojunction with adjustable IEF regulation over Mo 1.4 ‐ZIS@NTO is also demonstrated.