Enthalpy-Driven Molecular Engineering Enables High-Performance Quasi-Solid-State Electrolytes for Long Life Lithium Metal Batteries

© 2025 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - (2025) vom: 07. Apr., Seite e2419335
Auteur principal: Wang, Zilong (Auteur)
Autres auteurs: Shen, Longyun, Ma, Yilin, Law, Ho Mei, Xu, Shengjun, Bi, Yixin, Robson, Matthew J, Wang, Yuhao, Gröschel, André, Chen, Qing, Ciucci, Francesco
Format: Article en ligne
Langue:English
Publié: 2025
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article Li‐metal battery in situ polymerization polymerization enthalpy pouch‐type battery quasi‐solid‐state electrolyte
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520 |a The advancement of lithium metal batteries toward their theoretical energy density potential remains constrained by safety and performance issues inherent to liquid electrolytes. Quasi-solid-state electrolytes (QSSEs) based on poly-1,3-dioxolane (poly-DOL) represent a promising development, yet challenges in achieving satisfactory Coulombic efficiency and long-term stability have impeded their practical implementation. While lithium nitrate addition can enhance efficiency, its incorporation results in prohibitively slow polymerization rates spanning several months. In this work, high-polymerization-enthalpy 1,1,1-trifluoro-2,3-epoxypropane is introduced as a co-polymerization promoter, successfully integrating lithium nitrate into poly-DOL-based QSSEs. The resulting electrolyte demonstrates exceptional performance with 2.23 mS cm-1 of ionic conductivity at 25 °C, a Coulombic efficiency of 99.34% in Li|Cu cells, and stable lithium metal interfaces sustained through 1300 h of symmetric cell cycling. This co-polymerization approach also suppresses poly-DOL crystallization, enabling Li|LiFePO4 cells to maintain stability beyond 2000 cycles at 1C. Scale-up validation in a ≈1 Ah Li|NCM811 pouch cell achieves 94.4% capacity retention over 60 cycles. This strategy establishes a new pathway for developing high-performance, in situ polymerized quasi-solid-state batteries for practical energy storage applications 
650 4 |a Journal Article 
650 4 |a Li‐metal battery 
650 4 |a in situ polymerization 
650 4 |a polymerization enthalpy 
650 4 |a pouch‐type battery 
650 4 |a quasi‐solid‐state electrolyte 
700 1 |a Shen, Longyun  |e verfasserin  |4 aut 
700 1 |a Ma, Yilin  |e verfasserin  |4 aut 
700 1 |a Law, Ho Mei  |e verfasserin  |4 aut 
700 1 |a Xu, Shengjun  |e verfasserin  |4 aut 
700 1 |a Bi, Yixin  |e verfasserin  |4 aut 
700 1 |a Robson, Matthew J  |e verfasserin  |4 aut 
700 1 |a Wang, Yuhao  |e verfasserin  |4 aut 
700 1 |a Gröschel, André  |e verfasserin  |4 aut 
700 1 |a Chen, Qing  |e verfasserin  |4 aut 
700 1 |a Ciucci, Francesco  |e verfasserin  |4 aut 
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773 1 8 |g year:2025  |g day:07  |g month:04  |g pages:e2419335 
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