D‐Band Center Regulation for Durable Catalysts and Constructing a Robust Hybrid Layer on Li Anode Enable Long‐Life Li‐O2 Batteries

Abstract Rechargeable Li‐O 2 batteries (LOBs) are regarded as promising candidates for the next generation of energy storage devices. One of the major impediments is the poor cycle stability resulting from unreliable cathode catalysts and serious corrosion of Li anode, hindering the commercial application of LOBs. Herein, a synergetic strategy is proposed, including the design of a stable Co 3 Ru cathode catalyst via d‐band center modulation and the construction of a robust LiF/Sn/Li 5 Sn 2 ‐PFDTMS hybrid protective layer on Li anode. Theoretical calculations reveal that the negative shift of the d‐band center provides a dominant descriptor for improving the catalysis activity and stability of Ru‐based catalysts. In situ construction of the PFDTMS‐enhanced LiF/Sn/Li 5 Sn 2 hybrid layer possesses excellent mechanical stability and toughness, which can effectively shield the Li anode from corrosive reaction and ensure good Li + transport. Consequently, the LOBs exhibit a long cycle life of 990 cycles (≈1980 h). This work confers the concept for high‐performance LOBs via rationally constructing stable catalysts and Li anodes.