Top-Level Design Strategy to Construct an Advanced High-Entropy Co–Cu–Fe–Mo (Oxy)Hydroxide Electrocatalyst for the Oxygen Evolution Reaction

High-entropy materials are new-generation electrocatalysts for water splitting due to their excellent reactivity and highly tailorable electrochemical properties. Herein, a powerful top-level design strategy is reported to guide and design advanced high-entropy electrocatalysts by establishing reaction models (e.g., reaction energy barrier, conductivity, adsorption geometries for intermediates, and rate-determining step) to predict performance with the help of density functional theory (DFT) calculations. Accordingly, novel high-entropy Co–Cu–Fe–Mo (oxy)hydroxide electrocatalysts are fabricated by a new low-temperature electrochemical reconstruction method and their oxygen evolution reaction (OER) properties are thoroughly characterized. These as-prepared quaternary metallic (oxy)hydroxides present much better OER performance than ternary Co–Cu–Mo (oxy)hydroxide, Co–Fe–Mo (oxy)hydroxide, and other counterparts, and are demonstrated with a low overpotential of 199 mV at a current density of 10 mA cm⁻² and a 48.8 mV dec⁻¹ Tafel slope in 1 m KOH and excellent stability without decay over 72 h. The performance enhancement mechanism is also unraveled by synchrotron radiation. The work verifies the usefulness of high-entropy design and the great synergistic effect on OER performance by the incorporation of four elements, and also provides a new method for the construction of advanced high-entropy materials for energy conversion and storage.