Entropy Engineering in Multimetallic Hydroxides and Oxides: A New Paradigm for Electrocatalytic Oxygen Evolution

Abstract

The oxygen evolution reaction (OER) remains a central kinetic bottleneck in electrochemical energy-conversion technologies, motivating intensive exploration of earth-abundant electrocatalysts capable of delivering high activity and long-term stability. In recent years, high-entropy oxides and hydroxides have emerged as a powerful and versatile catalyst platform, where configurational entropy stabilizes multimetallic, defect-rich structures with highly tunable electronic and geometric environments. This review provides a comprehensive overview of entropy engineering strategies applied to oxides and hydroxides for OER electrocatalysis. We discuss the fundamental thermodynamic principles underpinning high-entropy stabilization, key structure–property relationships arising from lattice distortion, sluggish diffusion, and multication “cocktail” effects, and recent advances across crystalline and amorphous high-entropy oxides, perovskites, spinels, and high-entropy hydroxides. Particular emphasis is placed on mechanistic insights into adsorbate evolution, lattice oxygen-mediated, and emerging hybrid OER pathways in disordered lattices, as well as the role of operando reconstruction and oxygen vacancy dynamics. Finally, current challenges and future perspectives are outlined, highlighting the need for entropy-aware theoretical modeling, operando characterization, machine-learning-guided catalyst discovery, and expansion toward neutral-media and multifunctional electrocatalysis. Collectively, this review establishes high-entropy materials as a transformative paradigm for next-generation, earth-abundant OER catalysts.