Plastic Crystal Fast Ion‐Conductor Electrolyte Enabled Ultra‐Low Temperature Rechargeable Organic Battery

Abstract Battery performance is much damaged by ultra‐low‐temperature (<−80 °C), due to the insufficient ionic conductivity and high desolvation energy barrier. The strong coupling between ion dissociation and ion‐desolvation much increases the difficulty in electrolyte‐design. Here, it is demonstrated that such issue can be fundamentally addressed by a salt‐led electrolyte engineering. The salt with poor interionic interaction can be easily dissociated under appropriate solvation force even at extremely low‐temperature. The new electrolyte‐design logic is validated by 1‐ethyl‐1‐methylpyrrolidinium bis(fluorosulfonyl)imide, an organic ionic plastic‐crystals (OIPCs)‐characteristic salt. With the mild solvation assistance from methyl acetate, the electrolyte supplies considerable conductivity of 0.36 mS cm⁻¹ at −110 °C and enables the smooth charging/discharging of polyimide/polytriphenylamine all‐organic cell at ultra‐low‐temperature. Even with high material loading, the cell reserves 65% of theoretical capacity under 0.2 C‐rate at −110 °C. This work represents a significant advancement in the low‐temperature batteries, and provides new knowledge of the ionic dynamics of electrolyte.