Development of lithium batteries capable of operating over ultrawide temperature ranges, from subzero to temperatures ≥ 100 °C, is urgently needed yet remains highly challenging. This is primarily due to the inherent trade-off between sluggish kinetics at low temperatures and poor structural stability at high temperatures and high voltages. Herein, by systemically investigating the temperature responsiveness of various anions, a temperature-adaptive weakly solvating electrolyte (TAE) is elaborately designed in which the solvation structures are sensitive to temperature. As a result, TAE not only exhibits a higher Li+ transference number and ionic conductivity comparable to commercial electrolytes at ambient and subzero temperatures, but also leads to anion-derived gradient inorganic-rich interphases at high temperatures/cutoff voltages. Consequently, LiCoO2 || Li cells using TAE achieve capacity retentions of 89.6% after 500 cycles at ambient temperature and a cutoff voltage of 4.5 V, and 90.8% after 450 cycles at 80 °C. Moreover, 6.5 Ah pouch lithium-ion cells using TAE, with enhanced safety and ultrawide temperature ranges from -30 to 130 °C, deliver a capacity retention of 86.1% after 100 cycles at 100 °C. Notably, even at 120 °C, the cells retain 71.1% of their initial capacity over 60 cycles without significant swelling. This strategy empowers lithium batteries to autonomously adapt to external temperature, enabling reliable operation across diverse extreme environments.
Teng et al. (Fri,) studied this question.