Independent Tuning of Intermediate Energetics for Enhanced Oxygen Evolution via Synergistic Defects

Abstract Electronic structure engineering via integrating different defects is the key to achieving independent tuning of intermediate energetics for efficient electrocatalyst design. Such a combination of defects is at the forefront of current research. Herein, W is etched from Co(OH) 2 to generate Co vacancies, which are then partially filled with La to form Co(OH) 2 ‐Co V ‐La D for oxygen evolution reaction (OER). The results show that Co vacancy and La dopant induce more high‐valence Co species under OER conditions and the most active center is a surface Co site that is adjacent to a surface Co vacancy and a subsurface La dopant on different sides, where the optimized electronic structure narrows the gap between Gibbs free energies of OH* (ΔG OH* ) and OOH* (ΔG OOH* ) and modifies ΔG O* close to the midpoint, leading to high catalytic activity. The integration of synergistic defects offers an effective strategy to generate a range of defect atomic configurations and diverse electronic states, which enable the independent tuning of intermediate energetics, thereby unlocking the catalyst's full catalytic potential.