The advancements of lithium‐ion batteries indubitably call for advanced electrolytes with superior environmental adaptability and long‐term stability. Propylene carbonate (PC) proves to be a competitive solvent with the high permittivity and wide‐liquid range, while the application is intrinsically hindered by the poor graphite compatibility and high viscosity. Here, a PC‐based electrolyte with wide‐temperature range is developed by tuning the strength and topology of the Li+‐PC interactions via non‐solvating interactions without altering the solvation structure. Thus, the problem of graphite exfoliation caused by Li+‐PC co‐intercalation can be successfully mitigated. Consequently, such electrolyte shows compatibility with both graphite and high‐nickel cathode, exhibiting an expanded liquid range from −90 to 90 °C. This work, breaking from the traditional EC‐based formula, provides a new strategy for designing PC‐enabled electrolyte featuring high performance, wide‐temperature compatibility, and sustainability

Developing advanced electrolytes proves indispensable for next-generation lithium-ion batteries (LIBs). Yet the strong solvating interaction between Li+ and various solvents often leads to sluggish desolvation and solvent co-intercalation into graphite...

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