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Multifunctional Zwitterionic Self-Healing Polymer Electrolytes for Anode-Free Lithium-Metal Batteries: a

Liang-Ting Wu1,2, Yu-Ting Zhan1,2, Yu-Cheng Chiu1,2

  • 1Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei, 106, Taiwan.

Small (Weinheim an Der Bergstrasse, Germany)
|May 27, 2025
PubMed
Summary

A novel self-healing solid polymer electrolyte enhances anode-free lithium-metal battery performance. This zwitterionic material improves cycling stability and uniform lithium plating by creating a stable solid electrolyte interphase, enabling practical battery applications.

Keywords:
AIMD simulationDFT calculationLi‐metal batteryatomic charge distributionself‐healing polymer

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • Anode-free lithium-metal batteries (AFLMBs) face limitations in practical use due to poor cycling performance and unstable solid electrolyte interphase (SEI) formation.
  • Self-healing solid polymer electrolytes (SHSPEs) present a promising solution for enhancing battery flexibility and mitigating dendrite growth.

Purpose of the Study:

  • To investigate a novel zwitterionic SHSPE, P(SBMA-co-BA):LiTFSI, for its potential to improve AFLMB cycling performance.
  • To evaluate the electrolyte's self-healing mechanism and its effect on the SEI layer during battery operation.

Main Methods:

  • Density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations were employed to study the P(SBMA-co-BA):LiTFSI electrolyte.
  • Analysis of Li+ ion transport, self-healing mechanisms via electrostatic interactions, and electrolyte degradation on current collectors and Li metal surfaces.
  • Atomic charge distribution analysis was used to identify SEI components, with comparisons to experimental X-ray photoelectron spectroscopy (XPS) data.

Main Results:

  • The sulfonate group (RSO3-) in the SHSPE facilitates Li+ ion transport, while electrostatic interactions between sulfonate and quaternary ammonium groups enable self-healing.
  • A stable, flexible, organic/inorganic hybrid SEI layer was formed on the copper current collector and lithium metal surface.
  • The SHSPE promoted rapid Li-ion conduction and uniform Li metal plating, significantly enhancing battery cycling stability.

Conclusions:

  • The multifunctional zwitterionic SHSPE, P(SBMA-co-BA):LiTFSI, demonstrates significant potential for advancing AFLMB technology.
  • This material effectively addresses key challenges in AFLMBs, paving the way for their broader practical application.