Precisely Engineering of Ångström‐Scale Dual Single Atom Drive [Co‐O] Spin‐Orbit Coupling to Boost Lithium–Oxygen Batteries Electrocatalysis

Abstract Dual‐atom catalysts (DACs) have emerged as a novel area of investigation in lithium–oxygen (Li‐O₂) batteries due to their distinctive synergistic mechanisms. However, achieving precise control of the active site structure and unraveling the synergistic effects of bimetallic species remains a significant challenge. Here, the study reports a pre‐encapsulated pyrolysis strategy using a Co‐based Robson‐type binuclear complex as a precursor to mediate the synthesis of dual single‐atom Co (Co‐DAC) with precise angstrom‐scale inter‐site distance configuration, serving as an efficient catalyst for Li‐O₂ batteries. The tailored structure induces significant charge redistribution, reducing crystal field splitting energy (Δ_O). The high‐spin Co species generate a strong electronic driving force, forming flexible σ and δ‐like bonds with the crucial oxygen intermediate (^*O). Simultaneously, enhanced Co‐O spin‐orbit coupling facilitates electron transport along the bridging O‐channel, forming highly active Co‐O‐O‐Co electron chains that synergistically adsorb ^*O, establishing a favorable reaction pathway. Significant optimization of Li‐O₂ batteries redox kinetics is achieved based on the well‐defined local structure of dual single‐atom Co sites. This work enhances the understanding of the dependence between rational design of custom structures and corresponding electron transfer dynamics, while providing new strategies and theoretical guidance for DACs to help develop high‐performance Li‐O₂ batteries.