Entropy‐Stabilized Interface Coupling Activates Lattice Oxygen Inside Wood‐Channel‐Confined Electrocatalysts for Water Oxidation

ABSTRACT Triggering the lattice oxygen oxidation mechanism (LOM) presents a promising route to overcome theoretical limitations of the oxygen evolution reaction (OER). However, achieving efficient LOM activation without compromising structural stability remains challenging. Herein, we propose an entropy‐stabilized interface coupling strategy to drive the LOM within a wood‐channel‐confined electrocatalyst for high‐current‐density OER. The designed material consists of NiFe layered double hydroxide nanosheets encapsulating high‐entropy alloy nanoparticles, firmly embedded inside the wood channels (NiFe LDH@HEAs‐ACW). The composite structure induces strong interface electron coupling, enabling rapid electron transfer. Density functional theory (DFT) calculations reveal that the multi‐element HEA promotes OH − adsorption and elevates the O 2p band center, thereby promoting lattice oxygen participation in NiFe LDH at low overpotentials. Entropy stabilization within confined ACW channels mitigates metal leaching and prevents structural degradation. Consequently, the electrocatalyst achieves low overpotentials of 253, 276, and 285 mV at current densities of 100, 500, and 1000 mA cm −2 , respectively, and delivers favorable stability with 200 h of continuous operation at 500 mA cm −2 . The entropy‐promoted lattice oxygen participation strategy effectively decouples the traditional activity‐stability trade‐off in LOM‐based electrocatalysts, offering a viable pathway toward energy‐efficient water oxidation under demanding conditions.