▎ 摘　　要

Aprotic Li-O-2 batteries with high theoretical energy density are regarded as promising next-generation energy storage devices. However, the accumulation of discharge products (Li2O2) during the discharge/charge processes would lead to high overpotential, low round-trip efficiency and poor cycling stability of the batteries. Soluble redox mediators (RMs) have been proved to be efficient in promoting the oxidation of Li2O2 particles. However, the self-discharge of the electrochemically oxidized RMs (RMsox) on the surface of Li metal would accelerate the formation of lithium dendrites. In this work, nitrogenous radicals, 1,1-Diphenyl-2-picrylhydrazyl radical 2,2-Diphenyl-1-(2,4,6-trinitrophenyl) hydrazyl (DPPH), is designed and employed as a RM to lower the over-potential of Li-O-2 batteries. Moreover, the self-discharge of the oxidized DPPH on the surface of Li metal and the formation of lithium dendrites are successfully suppressed by the formation of graphene/luteolin protective layer on Li metal. Consequently, an ultrastable cycle stability (>150 cycles) is achieved with DPPH and the stable graphene/luteolin protective layer for the Li metal anodes. These synergistic effect of RMs and stable Li protective layer may inspire the development of sustainable and durable Li-O-2 batteries.