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A concentrated dual-salts LiFSI-LiNO 3 /DOL electrolyte was prepared by using LiNO 3 as the inhibitor. The LiF-Li 2 O-oligomers composite SEI layers can efficiently accommodate the rapid plating/stripping of Li metal. A high average Coulombic efficiency of 99.14% was achieved under a large current density of 8.0 mA cm−2. [Display omitted] Developing a high-rate Li metal anode with superior reversibility is a prerequisite for fast-charging Li metal batteries. However, the build-up of large concentration gradients under high current density leads to inhomogeneous Li deposition and unstable passivation layers of Li metal, resulting in lower Coulombic efficiency. Here we report a concentrated dual-salts LiFSI-LiNO 3 /DOL electrolyte to improve the high-rate performance of Li metal anode. Sufficient Li salts help passivate the fresh Li deposition quickly. Further, DOL contributes to the formation of flexible organic layers that can accommodate the rapid volume change of Li metal upon cycling. Li metal in the electrolyte remains stable over 240 cycles with the average Coulombic efficiency of 99.14% under a high current density of 8.0 mA cm−2. [ABSTRACT FROM AUTHOR]

Safe rechargeable batteries of improved energy density and high power performance are urgently needed for the development of large electric devices. Herein, an Li‐based organic liquid anode is proposed, and an organic oxygen battery with a metal organic framework membrane separator is realized, which is able to conduct Li ions and separate other large species in the system. Equipped with the dual redox mediator strategy, the organic oxygen battery exhibits superior rate performance with long cycling life and low overpotential. A "solid electrolyte interface"‐like layer is observed between the organic liquid anode and the ion conducting separator. This work not only introduces a new type of anode for Li‐based batteries, but also provides fundamental insights for the better application of biphenyl‐based liquid anodes. [ABSTRACT FROM AUTHOR]