Deciphering Coulombic Efficiency of Lithium Metal Anodes by Screening Electrolyte Properties.

Journal: Angewandte Chemie (International ed. in English)
Published Date: Jul 21, 2025

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 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.

Authors

  • Zhao Zheng
    Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P.R. China.
  • Xinyan Liu
    ICU, DongE Hospital Affiliated to Shandong First Medical University, Shandong, China.
  • Xue-Qiang Zhang
    Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P.R. China.
  • Shu-Yu Sun
    Beijing Key Laboratory of Complex Solid State Batteries & Tsinghua Center for Green Chemical Engineering Electrification, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P.R. China.
  • Jia-Lin Li
    Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P.R. China.
  • Ya-Nan Wang
    Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P.R. China.
  • Nan Yao
    The Department of Radiology, Jiangmen Central Hospital/Affiliated Jiangmen Hospital of Sun Yat-Sen University, No. 23 Haibang Street, Jiangmen, 529000, Guangdong, China.
  • Dong-Hao Zhan
    Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P.R. China.
  • Wen-Jun Feng
    The First Affiliated Hospital, Guangzhou University of Chinese Medicine, Guangzhou, China.
  • Hong-Jie Peng
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 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
    Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing, 100081, P.R. China.
  • Qiang Zhang
    Yunan Provincial Center for Disease Control and Prevention, Kunming 650022, China.

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