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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]

Li metal can potentially deliver much higher specific capacity than commercially used anodes. Nevertheless, because of its poor reversibility, abundant excess Li (usually more than three times) is required in Li metal batteries, leading to higher costs and decreased energy density. Here, a concentrated lithium bis(trifluoromethane sulfonyl) imide (LiTFSI)–lithium nitrate (LiNO3)–lithium bis(fluorosulfonyl)imide (LiFSI) ternary‐salts electrolyte is introduced to realize a high stable Li metal full‐cell with only a slight excess of Li. LiNO3 and LiFSI contribute to the formation of stable Li2O–LiF‐rich solid electrolyte interface layers, and LiTFSI helps to stabilize the electrolyte under high concentration. Li metal in the electrolyte remains stable over 450 cycles and the average Coulombic efficiency reaches 99.1%. Moreover, with 0.5 × excess Li metal, the Coulombic efficiency of Li metal in the LiTFSI–LiNO3–LiFSI reaches 99.4%. The electrolyte also presents high stability to the LiFePO4 cathode, the capacity retention after 500 cycles is 92.0% and the Coulombic efficiency is 99.8%. A Li metal full‐cell with only 0.44 × excess Li is also assembled, it remains stable over 70 cycles and 83% of the initial capacity is maintained after 100 cycles. A concentrated ternary‐salts electrolyte is developed for Li metal batteries. The LiNO3 and LiFSI in the electrolyte promote the formation of Li2O–LiF‐rich solid electrolyte interface layers, contributing to the high Coulombic efficiency of the Li anode. With the ternary‐salts electrolyte, the Li metal full‐cell with only 0.44 × excess Li remains stable over 70 cycles without evident capacity fading. [ABSTRACT FROM AUTHOR]