Matching high-voltage cathodes with lithium metal anodes represents the most viable technological approach for developing secondary batteries with ultra-high energy density exceeding 500 Wh kg. Nevertheless, the instability of electrolyte/electrode interface film and commercial electrolytes with cut-off voltage above 4.3 V is still a major concern. Herein, we present that excellent cycling stability with an ultra-high cut-off voltage of up to 5.0 V can be obtained by using three-component additives containing fluoroethylene carbonate (FEC), hexadecyl trimethylammonium chloride (CTAC), and tri(pentafluorophenyl)borane (TPFPB). Excellent ionic conductivity, robust interfacial films on both electrodes, and long-lasting uniform Li regulation ability can be obtained in the modifying electrolyte. Consequently, using a high plating/stripping capacity of 3 mAh cm under the current density of 1 mA cm, lithium symmetric cells demonstrate stable cycling performance exceeding 800 hours. Meanwhile, the 7.3 Ah-class Li[NiCoMn]O (x=0.83, NCM83)|Li pouch cells are assembled, which show a high energy density of 522 Wh kg and present excellent stability over 178 cycles with a high initial coulombic efficiency (CE) of 98.0 %.
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