Self‐Supported Gold‐Silk‐Chrysanthemum‐Like Superstructures Arrays Derived from Mn‐doped CoPS Nanowires with Superhydrophilic and Superaerophobic Surface for Enhanced Oxygen Evolution

Abstract Metal phosphosulfides (layered MPS₃ or pyrite‐type MPS) nanostructures have emerged as promising active materials for optoelectronics, magnetism, energy storage, and catalysis. Despite great progress that has been achieved, controllable synthesis of cationic‐doped CoPS nanostructures or related superstructures arrays remains challenging, and their electrocatalytic applications toward oxygen evolution reaction (OER) are not explored. Herein, the self‐supported Mn‐doped CoPS nanowire‐based gold‐silk‐chrysanthemum‐like superstructures arrays on carbon cloth (CC) with variable Mn‐content (Mn‐CoPS‐x%/CC) are fabricated by thermal conversion of MnCo‐layered‐double‐hydroxides‐x%/CC precursors under P_xS_y vapor/Ar atmosphere. Compared with pure CoPS/CC, all the Mn‐CoPS‐x%/CC show greatly enhanced electrocatalytic OER activity. Due to the suited Mn‐doping content and unique microstructure‐induced superhydrophilic and superaerophobic surface that can optimize electronic structure, offer more available active sites, and foster desorption of O₂ product, the Mn‐CoPS‐5%/CC manifests the best OER activity with a low overpotential (270 mV) to reach 20 mA cm⁻² current density and high turnover frequency (0.13 s⁻¹), outperforming its counterparts, IrO₂/CC and most of recently reported OER catalysts. Moreover, such Mn‐CoPS‐5%/CC exhibits good catalytic stability. This work offers an efficient avenue for optimizing MPS nanostructures toward OER by combining doping and structure engineering strategies, and may promote their applications in water‐splitting or other clean energy options.