Dominant Solvent-Separated Ion Pairs in Electrolytes Enable Superhigh Conductivity for Fast-Charging and Low-Temperature Lithium Ion Batteries.

Abstract

The low ionic conductivities of aprotic electrolytes hinder the development of extreme fast charging technologies and applications at low temperatures for lithium-ion batteries (LIBs). Herein, we present an electrolyte with LiFSI in acetone (DMK). In DMK electrolytes, the solvation number is three, and solvent-separated ion pairs (SSIPs) are the dominant structure, which is largely different from other linear aprotic electrolytes where salts primarily exist as contact ion pairs (CIPs). With incompact solvation structures due to the weak solvation ability of DMK with Li+, the ionic conductivity reaches 45 mS/cm at room temperature. The percentage of SSIPs increases as temperatures decrease in DMK electrolytes, which is totally different from the carbonate-based electrolytes but greatly beneficial to low-temperature ionic conductivity. With the appropriate addition of VC and FEC, DMK-based electrolytes still exhibit a superhigh ionic conductivity. Even at -40 °C, the ionic conductivity is greater than 10 mS/cm. With DMK-based electrolytes, LIBs with thick LiFePO4 electrodes can be cycled at high rates and at low temperatures.