Enabling Stable Operation of Lithium‐Ion Batteries under Fast‐Operating Conditions by Tuning the Electrolyte Chemistry

Inferior fast-charging and low-temperature performances remain a hurdle for lithium-ion batteries. Overcoming this hurdle is extremely challenging primarily due to the low conductivity of commercial ethylene carbonate (EC)-based electrolytes and the formation of undesirable solid electrolyte interphases with poor Li⁺-ion diffusion kinetics. Here, a series of EC-free fast-charging electrolytes (FCEs) by incorporating a fluorinated ester, methyl trifluoroacetate (MTFA), as a special cosolvent into a practically viable LiPF₆-dimethyl carbonate-fluoroethylene carbonate system, is reported. With a solvent-dominated solvation structure, MTFA facilitates the formation of thin, yet robust, interphases on both the cathode and anode. Commercial 1 Ah graphite|LiNi_0.8Mn_0.1Co_0.1O₂ pouch cells filled with the FCE exhibit ≈80% capacity retention over 3000 cycles at 3 C and 4 C (15 min) charging rates in the full range of 0-100% state-of-charge. Moreover, even at a low operating temperature of -20 °C, the 1 Ah cell retains a high capacity of 0.65 Ah at a 2 C discharge rate and displays virtually no capacity fade on cycling at a C/5 rate. The work highlights the power of electrolyte design in achieving extra-fast-charging and low-temperature performances.