High‐Entropy Oxides Facilitated Heterojunction Engineering With Superlattice Cd _0.6 Mn _0.4 S for Enhanced Photocatalytic Hydrogen Evolution

This study successfully constructed a highly efficient and stable photocatalytic system based on a triple synergistic catalytic mechanism involving multimetal component synergy, interfacial charge rearrangement, and Schottky barrier modulation. One‐dimensional axially oriented superlattice Cd _0.6 Mn _0.4 S nanorods were prepared via a solvothermal method. The unique periodic arrangement of CdS and MnS units creates axial separation channels for electrons and holes, significantly reducing the bulk charge recombination rate. Subsequently, CuCoNiZnAlO high‐entropy oxide was successfully loaded onto the surface of Cd _0.6 Mn _0.4 S using a wet chemical precipitation method. Hydrogen evolution experiments demonstrate that the CC‐15 composite catalyst exhibits 3.73 times the activity of pristine Cd _0.6 Mn _0.4 S. Experimental characterizations collectively confirm a substantial enhancement in photogenerated carrier separation efficiency within the CC‐15 composite. Subsequently, in situ XPS and charge density difference analyses provide direct dynamic evidence, indicating the directional transfer of electrons from Cd _0.6 Mn _0.4 S to HEO under light illumination. This work offers a new perspective for replacing noble‐metal cocatalysts with transition‐metal‐based alternatives.