Lewis Acid‐Activated High‐Entropy Layered Double Hydroxide for Superior Seawater Electrolysis

ABSTRACT Seawater electrolysis has been identified as a sustainable approach for the industrialization of green hydrogen. However, this process is hindered by two significant factors: the sluggish anodic kinetics and chloride‐induced corrosion. In this study, we introduce Zn 2+ as a Lewis acid site into high‐entropy layered double hydroxide (LDH) to modulate both the interfacial microenvironment and the bulk electronic structure. The resulting catalyst requires overpotentials of 35 and 160 mV for the hydrogen/oxygen evolution reactions at 10 mA cm −2 , respectively, accompanied by small Tafel slopes. Furthermore, an anion‐exchange membrane electrolyzer demonstrates operational stability over a duration of 900 h at 1.5 A cm −2 . Theoretical and in situ analyses reveal that Zn 2+ exhibits a preference for adsorbing OH − , thereby repelling Cl − . Concurrently, this process induces oxygen vacancies and optimizes the d‑band centers of Fe/Co sites, establishing a interfacial/bulk dual regulation. This work offers a novel paradigm for the design of robust high‑entropy catalysts via Lewis acid doping for practical applications in harsh environments.