Unique 1D Cd1−xZnxS@O‐MoS2/NiOx Nanohybrids: Highly Efficient Visible‐Light‐Driven Photocatalytic Hydrogen Evolution via Integrated Structural Regulation

Abstract Development of noble‐metal‐free photocatalysts for highly efficient sunlight‐driven water splitting is of great interest. Nevertheless, for the photocatalytic H 2 evolution reaction (HER), the integrated regulation study on morphology, electronic band structures, and surface active sites of catalyst is still minimal up to now. Herein, well‐defined 1D Cd 1− x Zn x S@O‐MoS 2 /NiO x hybrid nanostructures with enhanced activity and stability for photocatalytic HER are prepared. Interestingly, the band alignments, exposure of active sites, and interfacial charge separation of Cd 1− x Zn x S@O‐MoS 2 /NiO x are optimized by tuning the Zn‐doping content as well as the growth of defect‐rich O‐MoS 2 layer and NiO x nanoparticles, which endow the hybrids with excellent HER performances. Specifically, the visible‐light‐driven (>420 nm) HER activity of Cd 1− x Zn x S@O‐MoS 2 /NiO x with 15% Zn‐doping and 0.2 wt% O‐MoS 2 (CZ 0.15 S‐0.2M‐NiO x ) in lactic acid solution (66.08 mmol h −1 g −1 ) is about 25 times that of Pt loaded CZ 0.15 S, which is further increased to 223.17 mmol h −1 g −1 when using Na 2 S/Na 2 SO 3 as the sacrificial agent. Meanwhile, in Na 2 S/Na 2 SO 3 solution, the CZ 0.15 S‐0.2M‐NiO x sample demonstrates an apparent quantum yield of 64.1% at 420 nm and a good stability for HER under long‐time illumination. The results presented in this work can be valuable inspirations for the exploitation of advanced materials for energy‐related applications.