Accelerating the Transformation of Active β‐NiOOH on NiFe Layered Double Hydroxide via Cation–anion Collaborative Coordination for Alkaline Water Oxidation at High Current Densities

作者：Fujun Shi, Liyang Xiao, Zhenglin Zhou, Xueru Zhao, Ying Liu, Jing Mao, Jiayi Qin, Yida Deng, Jing Yang · 发表于：Advanced Functional Materials · 年份：2025 · DOI：10.1002/adfm.202501070 · 被引用次数：62 · 研究领域：Electrocatalysts for Energy Conversion、Advanced battery technologies research、Catalytic Processes in Materials Science

Abstract The NiFe‐based layered double hydroxides (LDH) undergo surface reconstruction, generating metal hydroxyl oxides that act as active species during the alkaline oxygen evolution reaction (OER). However, the sluggish reconstruction process and excessive oxidation at higher anodic potentials frustrate the alkaline OER activity and stability. Herein, a cation–anion collaborative coordination strategy is harnessed to build (Ni, Fe)─S─Zn coordination structures in NiFe LDH on the nickel foam (S‐NiFeZn LDH/NF), which lowers the reconstruction energy barrier and aids in forming highly active β‐NiOOH during the alkaline OER process. Meanwhile, the coordination structures also optimize the adsorption of oxygen‐containing intermediates, enhancing OER kinetics. As a result, S‐NiFeZn LDH/NF achieves low overpotentials of 201 mV at 10 mA cm −2 and 293 mV at 500 mA cm −2 in 1.0 m KOH. Moreover, the cell assembled with S‐NiFeZn LDH/NF as the anode and commercial NiMo foam as the cathode demonstrates excellent overall water splitting activity, with voltages of 1.62 and 1.81 V at 10 and 500 mA cm −2 in 1.0 m KOH, and exhibits ultralong‐term durability over 500 h at 500 mA cm −2 , even operating stably for 200 h in an alkaline water electrolyzer under industrial conditions (30% KOH at 80 °C).