Modulating Local Electron Spin‐State at Co Site Through Ru─O─Co Configuration for Efficient Triplet Oxygen Conversion

ABSTRACT The electrocatalytic performance of oxygen evolution/reduction reactions (OER/ORR) is related to the spin‐state of the transition metal, which can be modulated by magnetic element doping. This work proposes an innovative strategy involving non‐magnetic element doping to engineer spin polarization channels through the formation of Co‐O‐Ru covalent bonds, which can induce a spin‐state transition in Co sites from intermediate‐spin state () in S CoOOH to high‐spin state () in S CoOOH‐Ru. The optimized S CoOOH‐Ru achieves a remarkably low potential difference of 0.67 V between the E 1/2 for ORR and the η 10 for OER, demonstrating an approximately 140 mV reduction compared with its low‐spin state S CoOOH. Density functional theory (DFT) calculation reveals that the RuO x layer on CoO‐termination transforms CoOOH from a paramagnetic to a ferromagnetic material, indicating the generation of high‐spin Co 3+ sites. This optimized Co electronic structure combined with the intrinsically active Ru sites reduces free energy barriers of key ORR/OER intermediates (*OH → *O → *OOH) and accelerates the reaction kinetics, enhancing catalytic performance. This work not only unveils the remote control capability of non‐magnetic elements on spin states but also establishes a novel paradigm for spin engineering in the design of advanced oxygen electrocatalysts.