Electron Localization in Single Atomic Ga ₁ /PdNi Metallene Boosts Ethylene Glycol Assisted Rechargeable Zn‐Air Battery via Accelerating *OH Adsorption

ABSTRACT Alcohol‐assisted rechargeable Zn‐air batteries (ZAABs) are considered as one of the most promising energy storage devices due to their ultrahigh theoretical energy density and lower overpotential, yet they face the critical issues of the unavoidable CO _ads poisoning and incomplete oxidation behavior. Herein, the concept of holding single atomic alloy catalysts is proposed to strengthen the catalytic ability of Pd‐based metallene through implanting the oxyphilic Ga species. The prepared Ga ₁ /PdNiene with unconventional p‐d orbital hybridization shows the enhanced ethylene glycol oxdaition reaction (EGOR) performance with achieving excellent mass activity of 1.70 A/mg, 4.86 times higher than commercial Pd/C. Advanced characterizations and theoretical calculations reveal that the oxyphilic Ga site favors the formation of active *OH, accelerating the adsorption of EG molecules via electron localization, consequently promoting the C─C bond‐cleavage and oxidation/removal of poisonous CO _ads intermediates. In addition, the ethylene glycol assisted ZAABs based on Ga ₁ /PdNiene exhibits extraordinary power density of 160.3 mW/cm ² , 2.59 times higher than that of Pd/C catalyst. More importantly, Ga ₁ /PdNiene demonstrates an ultralong lifespan of 500 h (20 days) at 10 mA/cm ² with negligible performance loss in ZAABs.