The practical development of Li-O batteries is often hindered by poor cycling stability, which arises from volatile liquid electrolytes, an unstable anode/electrolyte interface, and sluggish reaction kinetics related to LiO. In this study, we design a long-life quasi-solid-state Li-O battery by integrating a gel polymer electrolyte (GPE) with a tetramethylpiperidinyloxy (TEMPO) redox mediator anchored in a poly(2,2,6,6-tetramethylpiperidinyloxy-4-methacrylate) (PTMA) cathode. During cycling, the GPE stabilizes the lithium/electrolyte interface and retains the electrolyte, while the TEMPO moieties anchored in the PTMA cathode effectively enhance the catalytic selectivity for LiO formation and decomposition. This innovative design significantly improves electrochemical performance, achieving an impressive lifespan of 800 h. The advancements in rechargeability and efficiency presented in this work are expected to pave the way for the development of long-lived solid-state Li-O batteries.
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