Solvent Molecule Cooperation Enhancing Lithium Metal Battery Performance at Both Electrodes

Abstract

Developing electrolytes compatible with efficient and reversible cycling of electrodes is critical to the success of rechargeable Li metal batteries (LMBs). The Coulombic efficiencies and cycle lives of LMBs with ethylene carbonate (EC), dimethyl carbonate, ethylene sulfite (ES), and their combinations as electrolyte solvents show that in a binary‐solvent electrolyte the extent of electrolyte decomposition on the electrode surface is dependent on the solvent component that dominates the solvation sheath of Li+. This knowledge led to the development of an EC‐ES electrolyte exhibiting high performance for Li||LiFePO4 batteries. Carbonate molecules occupy the solvation sheath and improve the Coulombic efficiencies of both the anode and cathode. Sulfite molecules lead to desirable morphology and composition of the solid electrolyte interphase and extend the cycle life of the Li metal anode. The cooperation between these components provides a new example of electrolyte optimization for improved LMBs.