In Situ Alloying Enabled by Active Liquid Metal Filler for Self‐Healing Composite Polymer Electrolytes

Wu, Kai; Ju, Zhengyu; Zhang, Bowen; Marschilok, Amy C.; Takeuchi, Esther S.; Takeuchi, Kenneth J.; Yu, Guihua

doi:10.1002/anie.202410463

Title: In Situ Alloying Enabled by Active Liquid Metal Filler for Self‐Healing Composite Polymer Electrolytes

Journal Article · 15 October 2024 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202410463 · OSTI ID:2476719

Wu, Kai ^[1]; Ju, Zhengyu ^[1]; Zhang, Bowen ^[1]; Marschilok, Amy C. ^[2]; Takeuchi, Esther S. ^[2]; Takeuchi, Kenneth J. ^[2];

^[1]

Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin 78712 Austin TX USA
Institute of Energy Sustainability, Environment, and Equity Stony Brook University 11794 Stony Brook NY USA, Department of Chemistry Stony Brook University 11794 Stony Brook NY USA, Interdisciplinary Science Department Brookhaven National Laboratory 11973 Upton NY USA, Department of Materials Science and Chemical Engineering Stony Brook University 11794 Stony Brook NY USA

Abstract Solid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces Ga _62.5 In _21.5 Sn ₁₆ (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self‐healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li‐ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li‐LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid‐state Li/LiFePO ₄ battery achieves promising full‐cell functionality with notable rate performance and stable cycle life. This active filler‐mediated self‐healing approach could bring new insights into the battery design in versatile solid‐state systems.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0012673

OSTI ID:: 2476719

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 47 Vol. 63; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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