Deciphering Coulombic Efficiency of Lithium Metal Anodes by Screening Electrolyte Properties

Abstract Coulombic efficiency (CE) is a quantifiable indicator for the reversibility of lithium metal anodes in high‐energy‐density batteries. However, the quantitative relationship between CE and electrolyte properties has yet to be established, impeding rational electrolyte design. Herein, an interpretable model for estimating CE based on data‐driven insights of electrolyte properties is proposed. Hydrogen‐bond acceptor basicity ( β ) and the energy level gap between the lowest unoccupied and the highest occupied molecular orbital (HOMO‐LUMO gap) of solvents are identified as the top two parameters impacting CE by machine learning. β and HOMO‐LUMO gap of solvents govern anode interphase chemistry. A regression model is further proposed to estimate the CE based on β and HOMO‐LUMO gap. Using the new solvent screened by above regression model, the lithium metal anode in the pouch cell with an energy density of 418 Wh kg −1 achieves the highest CE of 99.2%, which is much larger than previous CE ranging from 70%–98.5%. This work provides a reliable interpretable quantitative model for rational electrolyte design.