Metal Hydroxide Organic Frameworks: Design Principles and Applications in Electrocatalytic Oxidation

Electrocatalysts play a central role in electrochemical energy storage and conversion technologies; however, their practical applications are often hindered by structural degradation and active site deactivation under operating conditions. Therefore, achieving high catalytic activity while maintaining long‐term structural stability remains a persistent challenge in catalyst design. Metal hydroxide organic frameworks (MHOFs), an emerging class of hybrid materials that integrate metal hydroxide layers with tunable organic linkers, have attracted increasing attention owing to their structural robustness, compositional versatility, and highly adjustable electronic environments. In electrocatalytic oxidation reactions, MHOFs provide opportunities to overcome the limitations of conventional catalysts through the synergistic regulation of hydroxide layers and organic ligands, thereby optimizing intermediate adsorption, interfacial configurations, and charge transfer pathways. Over the past several years, these features have enabled substantial improvements in electrocatalytic activity and durability. This review systematically summarizes recent advances in MHOF electrocatalysts, with a particular focus on structural classification, synthetic strategies, and structure performance relationships that govern electrocatalytic behavior. Particular attention is devoted to elucidating the mechanistic roles of hydroxide layer engineering and ligand modulation in regulating catalytic processes. Finally, current challenges, unresolved mechanistic questions, and future opportunities are discussed to provide design principles for next‐generation MHOF electrocatalysts and facilitate their practical implementation.