Charging Voltage-Dependent Interphase Stabilization Enabling Wide-Temperature High-Voltage Li/LiCoO 2 Battery

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Designing electrolytes that endure both high voltage and wide temperature extremes remains a key barrier to lithium metal batteries (LMBs). Here, a charging voltage-driven interfacial stabilization strategy is presented to construct a robust interphase with a thin organic layer over a LiF/borate-rich matrix, which effectively passivates both the lithium metal and cathode surface. Attributed to these superiorities, Li/LiCoO 2 cells achieve 88% capacity retention over 900 cycles at high voltage (0.5 C, 4.5 V), 83% after 300 cycles at 60 °C (3 C, 3–4.6 V), and 72% after 200 cycles at room temperature (1 C, 3–4.7 V). Even under extreme cold (−40 °C), the cell retains 92% capacity over 200 cycles at 4.6 V, reflecting superior interfacial robustness. This finding inspires researchers to reconsider the specific requirements for the cathode electrolyte interphase by tuning charging voltage rather than exclusively regulating solvation structure, progressing the development for high-voltage LMBs in extreme conditions.