{"title":"双氟化分子设计为具有腐蚀性化学物质的5.0 V锂金属电池提供聚醚固体电解质","authors":"Guo Ye, Yue Ma, Lujun Zhu, Chengxi Zheng, Mengxue He, Kaier Shen, Zhitong Xiao, Yongfeng Jia, Xufeng Hong, Mohammadhosein Safari, Quanquan Pang","doi":"10.1002/adfm.202509547","DOIUrl":null,"url":null,"abstract":"Polyether‐based solid electrolytes (PESEs) are uniquely advantageous for solid‐state batteries owed to their segmental flexibility and compatibility with lithium metal anodes (LMAs). However, PESEs face challenges with poor ionic conductivity, low Li<jats:sup>+</jats:sup> transference number, and low oxidation stability. Here it is reported a dual fluorination strategy by incorporating two types of fluorine, bound and exchangeable states, which enables PESEs with excellent physiochemical properties and stability with aggressive high‐voltage cathodes and LMAs at 25 °C. While a stiff pentafluorobenzene unit − as the <jats:italic>bound</jats:italic> fluorine − is integrated into the flexible polyether backbone to enhance oxidation stability, mechanical properties, and the Li<jats:sup>+</jats:sup> transference number (via anion‐π interactions), a solid‐state organic molecule 2,2,2‐trifluoro‐N‐methylacetamide – as the <jats:italic>exchangeable</jats:italic> fluorine – serves to construct a fluorine‐rich solid‐electrolyte interphase. As a result, the PESE enables high‐stability 5.0‐V class Li|LiNi<jats:sub>0.5</jats:sub>Mn<jats:sub>1.5</jats:sub>O<jats:sub>4</jats:sub> cells maintaining 85.6% capacity over 600 cycles. The described dual fluorination strategy, applicable to PESEs herein and possibly beyond, is expected to pave the way toward practical, long‐life, and high‐energy solid‐state lithium‐metal batteries.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"152 1","pages":""},"PeriodicalIF":18.5000,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Dual Fluorination Molecular Design Enabling Polyether Solid Electrolytes for 5.0 V Lithium‐Metal Batteries With Aggressive Chemistries\",\"authors\":\"Guo Ye, Yue Ma, Lujun Zhu, Chengxi Zheng, Mengxue He, Kaier Shen, Zhitong Xiao, Yongfeng Jia, Xufeng Hong, Mohammadhosein Safari, Quanquan Pang\",\"doi\":\"10.1002/adfm.202509547\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Polyether‐based solid electrolytes (PESEs) are uniquely advantageous for solid‐state batteries owed to their segmental flexibility and compatibility with lithium metal anodes (LMAs). However, PESEs face challenges with poor ionic conductivity, low Li<jats:sup>+</jats:sup> transference number, and low oxidation stability. Here it is reported a dual fluorination strategy by incorporating two types of fluorine, bound and exchangeable states, which enables PESEs with excellent physiochemical properties and stability with aggressive high‐voltage cathodes and LMAs at 25 °C. While a stiff pentafluorobenzene unit − as the <jats:italic>bound</jats:italic> fluorine − is integrated into the flexible polyether backbone to enhance oxidation stability, mechanical properties, and the Li<jats:sup>+</jats:sup> transference number (via anion‐π interactions), a solid‐state organic molecule 2,2,2‐trifluoro‐N‐methylacetamide – as the <jats:italic>exchangeable</jats:italic> fluorine – serves to construct a fluorine‐rich solid‐electrolyte interphase. As a result, the PESE enables high‐stability 5.0‐V class Li|LiNi<jats:sub>0.5</jats:sub>Mn<jats:sub>1.5</jats:sub>O<jats:sub>4</jats:sub> cells maintaining 85.6% capacity over 600 cycles. The described dual fluorination strategy, applicable to PESEs herein and possibly beyond, is expected to pave the way toward practical, long‐life, and high‐energy solid‐state lithium‐metal batteries.\",\"PeriodicalId\":112,\"journal\":{\"name\":\"Advanced Functional Materials\",\"volume\":\"152 1\",\"pages\":\"\"},\"PeriodicalIF\":18.5000,\"publicationDate\":\"2025-06-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Functional Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/adfm.202509547\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202509547","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
聚醚基固体电解质(PESEs)由于其节段灵活性和与锂金属阳极(lma)的兼容性,在固态电池中具有独特的优势。然而,PESEs面临着离子电导率差、Li+转移数低、氧化稳定性低等挑战。本文报道了一种双氟化策略,通过结合两种类型的氟,结合态和交换态,使PESEs具有优异的物理化学性能和稳定性,具有侵略性高压阴极和25°C的lma。刚性的五氟苯单元(作为结合氟)被整合到柔性聚醚骨架中,以增强氧化稳定性、机械性能和Li+转移数(通过阴离子- π相互作用),而固态有机分子2,2,2 -三氟- N -甲基乙酰胺(作为可交换氟)用于构建富氟固体-电解质界面。因此,PESE能够实现高稳定性的5.0 V级Li|LiNi0.5Mn1.5O4电池,在600次循环中保持85.6%的容量。所描述的双氟化策略,适用于PESEs,并可能超越,有望为实用,长寿命,高能固态锂金属电池铺平道路。
Dual Fluorination Molecular Design Enabling Polyether Solid Electrolytes for 5.0 V Lithium‐Metal Batteries With Aggressive Chemistries
Polyether‐based solid electrolytes (PESEs) are uniquely advantageous for solid‐state batteries owed to their segmental flexibility and compatibility with lithium metal anodes (LMAs). However, PESEs face challenges with poor ionic conductivity, low Li+ transference number, and low oxidation stability. Here it is reported a dual fluorination strategy by incorporating two types of fluorine, bound and exchangeable states, which enables PESEs with excellent physiochemical properties and stability with aggressive high‐voltage cathodes and LMAs at 25 °C. While a stiff pentafluorobenzene unit − as the bound fluorine − is integrated into the flexible polyether backbone to enhance oxidation stability, mechanical properties, and the Li+ transference number (via anion‐π interactions), a solid‐state organic molecule 2,2,2‐trifluoro‐N‐methylacetamide – as the exchangeable fluorine – serves to construct a fluorine‐rich solid‐electrolyte interphase. As a result, the PESE enables high‐stability 5.0‐V class Li|LiNi0.5Mn1.5O4 cells maintaining 85.6% capacity over 600 cycles. The described dual fluorination strategy, applicable to PESEs herein and possibly beyond, is expected to pave the way toward practical, long‐life, and high‐energy solid‐state lithium‐metal batteries.
期刊介绍:
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