中国科学:材料科学(英文)2024,Vol.67Issue(5) :1412-1421.DOI:10.1007/s40843-024-2857-8

用于室温全固态锂金属电池的精准丁二腈官能团化聚氧化乙烯固态电解质

Precisely succinonitrile-functionalized PEO electrolytes toward room-temperature all-solid-state lithium batteries

李新阳 张宗楠 封婕 阴祥凯 崔晓峰 徐巍 张宏俊 曾荣 丁书江
中国科学:材料科学(英文)2024,Vol.67Issue(5) :1412-1421.DOI:10.1007/s40843-024-2857-8

用于室温全固态锂金属电池的精准丁二腈官能团化聚氧化乙烯固态电解质

Precisely succinonitrile-functionalized PEO electrolytes toward room-temperature all-solid-state lithium batteries

李新阳 1张宗楠 1封婕 1阴祥凯 1崔晓峰 2徐巍 3张宏俊 3曾荣 1丁书江1
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作者信息

  • 1. School of Chemistry,Engineering Research Center of Energy Storage Materials and Devices,Ministry of Education,State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Xi'an 710049,China
  • 2. School of Future Technology,Xi'an Jiaotong University,Xi'an 710049,China
  • 3. State Key Laboratory of Particle Detection and Electronics,University of Science and Technology of China,Hefei 230026,China
  • 折叠

摘要

聚环氧乙烷(PEO)聚合物电解质有望应用于全固态锂金属电池.然而,目前还没有提出有效的方法制备全固态PEO电解质,以克服其在室温下无法使用的局限性.在本研究中,我们基于聚合物C-H键功能化策略,通过在聚合物链上直接共价连接具有锂配位活性的丁二腈官能团,设计出了一种高离子导电性PEO电解质.该官能团有效增强了PEO链的无序性和流动性,同时也作为链间快速离子传导的活性位点,从而实现了离子周围自由体积和迁移行为的双重优化.得益于官能团对离子输运的精准调节,新型电解质表现出更强的离子传导性(离子电导率提升100倍)、更高的转移数(tLi+=0.51)和更宽的电化学窗口(>0.47 V).特别是功能化的PEO300k电解质具有超高室温离子电导率(25℃时为1.01×10-4 S cm-1)并且能够在室温下稳定工作,该研究为开发具有实际应用价值的聚合物电解质提供了新的途径.

Abstract

Poly(ethylene oxide)(PEO)polymer electrolytes have the potential for the use in all-solid-state lithium-metal batteries(ASSLMBs).However,no effective rules have been proposed to prepare all-solid-state PEO electrolytes that overcome the limitation being unusable at room temperature.In this study,based on the polymer C-H functionalization strategy,we design a highly ion-conductive PEO electrolyte by directly covalently linking succinonitrile functional-groups with lithium coordination activity on the polymer chains.The functional-groups enhance the disorder and mobility of the PEO chains while acting as effective sites for the fast ionic-conduction in the interchain,thus achieving a dual optimi-zation of the free volume around ions and the migration be-havior.Due to the precise tuning by functional-groups,the functionalized electrolyte exhibits enhanced ionic con-ductivity(>102 times),high transference number(~0.51)and wide electrochemical window(~0.47 V).In particular,the functionalized PEO30ok electrolyte with a high ionic con-ductivity(1.01x10-4 S cm-1 at 25℃)enables the stable opera-tion at room temperature,providing a path for the development of polymer-based electrolytes with practical ap-plications.

关键词

all-solid-state lithium battery/PEO electrolyte/poly-mer functionalization/room temperature operation/fast ionic conduction

Key words

all-solid-state lithium battery/PEO electrolyte/poly-mer functionalization/room temperature operation/fast ionic conduction

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基金项目

National Natural Science Foundation of China(52273081)

National Natural Science Foundation of China(51973171)

National Natural Science Foundation of China(22371223)

出版年

2024
中国科学:材料科学(英文)

中国科学:材料科学(英文)

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