Electron Spin Broken‐Symmetry of Fe–Co Diatomic Pairs to Promote Kinetics of Bifunctional Oxygen Electrocatalysis for Zinc–Air Batteries

Abstract Designing bifunctional catalysts to reduce the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) reaction barriers while accelerating the reaction kinetics is perceived to be a promising strategy to improve the performance of Zinc–air batteries. Unsymmetric configuration in single‐atom catalysts has attracted attention due to its unique advantages in regulating electron orbitals. In this work, a seesaw effect in unsymmetric Fe–Co bimetallic monoatomic configurations is proposed, which can effectively improve the OER/ORR bifunctional activity of the catalyst. Compared with the symmetrical model of Fe–Co, a strong charge polarization between Co and Fe atoms in the unsymmetric model is detected, in whom the spin‐down electrons around Co atoms are much higher than those spin‐up electrons. The seesaw effect occurred between Co atoms and Fe atoms, resulting in a negative shift of the d‐band center, which means that the adsorption of oxygen intermediates is weakened and more conducive to their dissociation. The optimized reaction kinetics of the catalyst leads to excellent performance in ZABs, with a peak power density of 215 mW cm⁻² and stable cycling for >1300 h and >4000 cycles. Flexible Zinc–air batteries have also gained excellent performance to demonstrate their potential in the field of flexible wearables.