Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries

Abstract Gel polymer electrolyte (GPE) has garnered widespread attention in the field of lithium batteries because of its low interfacial impedance, high thermal stability, and flexibility. However, the high‐voltage compatibility and Li+ transport kinetics of GPE have yet to meet the requirements of...

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Main Authors: Qingjie Zhou, Mengxue He, Shuyang Gao, Wangshu Hou, Yulin Ma, Hua Huo, Chunyu Du, Geping Yin, Pengjian Zuo
Format: Article
Language:English
Published: Wiley 2025-05-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202417169
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author Qingjie Zhou
Mengxue He
Shuyang Gao
Wangshu Hou
Yulin Ma
Hua Huo
Chunyu Du
Geping Yin
Pengjian Zuo
author_facet Qingjie Zhou
Mengxue He
Shuyang Gao
Wangshu Hou
Yulin Ma
Hua Huo
Chunyu Du
Geping Yin
Pengjian Zuo
author_sort Qingjie Zhou
collection DOAJ
description Abstract Gel polymer electrolyte (GPE) has garnered widespread attention in the field of lithium batteries because of its low interfacial impedance, high thermal stability, and flexibility. However, the high‐voltage compatibility and Li+ transport kinetics of GPE have yet to meet the requirements of future high‐energy secondary battery systems. In this regard, a comprehensive and insightful review of high‐voltage lithium batteries with GPE has attracted significant attention, focusing on molecular design and intermolecular interactions. Molecular regulation involves customizing the polymer matrix, solvent, additive, and Li salt, while intermolecular interactions encompass hydrogen bond interactions, Lewis acid‐base interactions, electrostatic interactions, and π–π stacking interactions. Besides, strategies to enhance the stability of the cathode electrolyte interphase and Li+ transport kinetics are summarized. It is hoped that this review will provide a deeper understanding of the direct regulation of GPE at the molecular level, further accelerating the commercialization of GPE in high‐energy secondary lithium batteries.
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series Advanced Science
spelling doaj-art-e67bbf939f404ff3a3e9579351e5fc1e2025-08-20T03:11:14ZengWileyAdvanced Science2198-38442025-05-011218n/an/a10.1002/advs.202417169Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium BatteriesQingjie Zhou0Mengxue He1Shuyang Gao2Wangshu Hou3Yulin Ma4Hua Huo5Chunyu Du6Geping Yin7Pengjian Zuo8State Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaState Key Laboratory of Space Power‐Sources School of Chemistry and Chemical Engineering Harbin Institute of Technology No.92 West‐Da Zhi Street Harbin 150001 ChinaAbstract Gel polymer electrolyte (GPE) has garnered widespread attention in the field of lithium batteries because of its low interfacial impedance, high thermal stability, and flexibility. However, the high‐voltage compatibility and Li+ transport kinetics of GPE have yet to meet the requirements of future high‐energy secondary battery systems. In this regard, a comprehensive and insightful review of high‐voltage lithium batteries with GPE has attracted significant attention, focusing on molecular design and intermolecular interactions. Molecular regulation involves customizing the polymer matrix, solvent, additive, and Li salt, while intermolecular interactions encompass hydrogen bond interactions, Lewis acid‐base interactions, electrostatic interactions, and π–π stacking interactions. Besides, strategies to enhance the stability of the cathode electrolyte interphase and Li+ transport kinetics are summarized. It is hoped that this review will provide a deeper understanding of the direct regulation of GPE at the molecular level, further accelerating the commercialization of GPE in high‐energy secondary lithium batteries.https://doi.org/10.1002/advs.202417169gel polymer electrolytehigh‐voltage compatibilityintermolecular interactionsLi⁺ transport kineticsmolecular regulation
spellingShingle Qingjie Zhou
Mengxue He
Shuyang Gao
Wangshu Hou
Yulin Ma
Hua Huo
Chunyu Du
Geping Yin
Pengjian Zuo
Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
Advanced Science
gel polymer electrolyte
high‐voltage compatibility
intermolecular interactions
Li⁺ transport kinetics
molecular regulation
title Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
title_full Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
title_fullStr Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
title_full_unstemmed Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
title_short Molecular Regulation and Intermolecular Chemistry in Gel Polymer Electrolytes for High‐Voltage Lithium Batteries
title_sort molecular regulation and intermolecular chemistry in gel polymer electrolytes for high voltage lithium batteries
topic gel polymer electrolyte
high‐voltage compatibility
intermolecular interactions
Li⁺ transport kinetics
molecular regulation
url https://doi.org/10.1002/advs.202417169
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