Electrochemical Stability Windows of Sulfone-Based Electrolyte System for Lithium Metal Batteries: Insight from MD-Assisted DFT Calculation

Lithium metal batteries using lithium metal as the anode are attractive for a next-generation energy storage device due to their high theoretical energy density. Nevertheless, electrolytes with wider electrochemical stability windows are also necessary for realizing a high voltage. Despite its advantageous characteristics, including excellent oxidation stability and low flammability, there is a general lack of understanding of the handling of a sulfone-based electrolyte, and thus, there exists a demand for a framework that can accurately estimate the stability of the electrolyte system. Here, we examine the solvation structures and electrochemical stability of electrolyte systems with dimethyl sulfone and lithium-bis(fluoromethanesulfonyl)imide as the solvent and salt, respectively. Based on this case, strategies are provided, including the level of theory and generation of configuration…