Deciphering Coulombic Efficiency of Lithium Metal Anodes by Screening Electrolyte Properties
Abstract
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.
Article Details
Authors (13)
Zhao Zheng
Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering
Xinyan Liu
Institute of Fundamental and Frontier Science
Xue‐Qiang Zhang
School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China
Shu‐Yu Sun
Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China
Jia‐Lin Li
School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China
Ya‐Nan Wang
School of Materials Science and Engineering Beijing Institute of Technology Beijing 100081 P.R. China
Nan Yao
Dong‐Hao Zhan
Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing 100081 P.R. China
Wen‐Jun Feng
Beijing Key Laboratory of Complex Solid State Batteries Department of Chemical Engineering Tsinghua University Beijing 100084 P.R. China
Hong‐Jie Peng
Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu Sichuan 611731 P.R. China
Jiang‐Kui Hu
Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing 100081 P.R. China
Jia‐Qi Huang
School of Interdisciplinary Science Beijing Institute of Technology Beijing P. R. China
Qiang Zhang