High-Energy Rechargeable Metallic Lithium Battery at -70 °C Enabled by a Cosolvent Electrolyte

Angew Chem Int Ed Engl. 2019 Apr 16;58(17):5623-5627. doi: 10.1002/anie.201900266. Epub 2019 Mar 26.

Abstract

Lithium metal is an ideal anode for high-energy rechargeable batteries at low temperature, yet hindered by the electrochemical instability with the electrolyte. Concentrated electrolytes can improve the oxidative/reductive stability, but encounter high viscosity. Herein, a co-solvent formulation was designed to resolve the dilemma. By adding electrochemically "inert" dichloromethane (DCM) as a diluent in concentrated ethyl acetate (EA)-based electrolyte, the co-solvent electrolyte demonstrated a high ionic conductivity (0.6 mS cm-1 ), low viscosity (0.35 Pa s), and wide range of potential window (0-4.85 V) at -70 °C. Spectral characterizations and simulations show these unique properties are associated with the co-solvation structure, in which high-concentration clusters of salt in the EA solvent were surrounded by mobile DCM diluent. Overall, this novel electrolyte enabled rechargeable metallic Li battery with high energy (178 Wh kg-1 ) and power (2877 W kg-1 ) at -70 °C.

Keywords: co-solvent electrolyte; high energy density; lithium-metal batteries; low temperature.