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

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中文摘要：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.

外文标题：Precisely succinonitrile-functionalized PEO electrolytes toward room-temperature all-solid-state lithium batteries

外文摘要：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.

外文关键词：

all-solid-state lithium batteryPEO electrolytepoly-mer functionalizationroom temperature operationfast ionic conduction

作者：

李新阳、张宗楠、封婕、阴祥凯、崔晓峰、徐巍、张宏俊、曾荣、丁书江

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作者单位：

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

School of Future Technology,Xi'an Jiaotong University,Xi'an 710049,China

State Key Laboratory of Particle Detection and Electronics,University of Science and Technology of China,Hefei 230026,China

关键词：

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

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of China

项目编号：

522730815197317122371223

出版年：

2024

DOI：

10.1007/s40843-024-2857-8

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(5)