Confined Growth High‐Entropy Layered Hydroxides with Organic Molecular Intercalated Structure for High‐Performance Oxygen Evolution Catalysis

Abstract High‐entropy layered (oxy)hydroxides (HE‐LDHs), with efficient intrinsic activity and ideal “cocktail effect,” are considered promising candidates for achieving stable and active oxygen evolution reaction (OER). However, due to the dissolution of high‐valence intermediates and unpredictable phase transition during the OER process, it remains challenging to solve the trade‐off problems occurring between the stability and activity of HE‐LDHs. Herein, HE‐LDHs with an intercalation structure constructed on a metal–organic framework with heterointerface confinement are reported, realizing the alleviation of metal dissolution and optimized valence of catalytic sites during the OER process, for highly active and durable water electrooxidation. The prepared HE‐LDH@Mn‐MIL‐100 shows ultralow overpotential of 211 mV at 10 mA cm ⁻² and wonderful stability operated in 1.0 m KOH for 100 h. Besides, the constructed anion exchange membrane water electrolyzer (AEMWE) delivers 1.0 A cm ⁻² at only 2.33 V for cell voltage in 1.0 m KOH, indicating promising prospects for practical applications. This work provides an innovative strategy in improving high‐entropy materials systems by confined ligand release for intercalation and offers new insights for tailoring highly active and stable catalysts for alkaline water electrooxidation.