Solvent reconstruction and interfacial fluorination strategy for high-performance polyether lithium metal batteries

IF 3 4区 材料科学 Q3 CHEMISTRY, PHYSICAL
Haofeng Peng, Zixuan Fang, Ming Zhang, Mengqiang Wu
{"title":"Solvent reconstruction and interfacial fluorination strategy for high-performance polyether lithium metal batteries","authors":"Haofeng Peng,&nbsp;Zixuan Fang,&nbsp;Ming Zhang,&nbsp;Mengqiang Wu","doi":"10.1016/j.ssi.2025.116849","DOIUrl":null,"url":null,"abstract":"<div><div>Lithium metal batteries based on in situ semi-solid-state polyether electrolytes have emerged as a focal point of contemporary research due to their straightforward fabrication process, high energy density, and reliable safety. The DOL monomers exhibit characteristics of low viscosity and polymerization initiated by lithium salts at room temperature, presenting a significant commercial potential for the preparation of PDOL semi-solid-state electrolytes via in situ ring-opening polymerization for high-performance lithium metal batteries. However, the intrinsic performance deficiencies and poor antioxidant properties of polyether electrolytes have severely impeded their practical application. The utilization of 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) as a diluent and fluoroethylene carbonate (FEC) as an additive for solvent reconstruction and interfacial fluorination of the semi-solid-state polyether electrolytes has effectively mitigated these issues. Density functional theory and molecular dynamics simulations demonstrate that the TTE diluent can optimize the solvent structure and enhance anionic coordination, thereby improving the electrochemical performance of PDOL-based electrolytes, which enables stable cycling of Li/Li symmetric batteries for over 2000 h at 0.1 mA cm <sup>−</sup> <sup>2</sup>. Furthermore, the introduction of the fluorinated additive FEC has achieved exceptional performance in Li/NCM811 high-voltage lithium metal batteries, with an initial discharge specific capacity of 206.3 mAh g<sup>−1</sup> at 0.1C and stable charge-discharge cycling at 0.3C.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"423 ","pages":"Article 116849"},"PeriodicalIF":3.0000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Solid State Ionics","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0167273825000682","RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Lithium metal batteries based on in situ semi-solid-state polyether electrolytes have emerged as a focal point of contemporary research due to their straightforward fabrication process, high energy density, and reliable safety. The DOL monomers exhibit characteristics of low viscosity and polymerization initiated by lithium salts at room temperature, presenting a significant commercial potential for the preparation of PDOL semi-solid-state electrolytes via in situ ring-opening polymerization for high-performance lithium metal batteries. However, the intrinsic performance deficiencies and poor antioxidant properties of polyether electrolytes have severely impeded their practical application. The utilization of 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (TTE) as a diluent and fluoroethylene carbonate (FEC) as an additive for solvent reconstruction and interfacial fluorination of the semi-solid-state polyether electrolytes has effectively mitigated these issues. Density functional theory and molecular dynamics simulations demonstrate that the TTE diluent can optimize the solvent structure and enhance anionic coordination, thereby improving the electrochemical performance of PDOL-based electrolytes, which enables stable cycling of Li/Li symmetric batteries for over 2000 h at 0.1 mA cm  2. Furthermore, the introduction of the fluorinated additive FEC has achieved exceptional performance in Li/NCM811 high-voltage lithium metal batteries, with an initial discharge specific capacity of 206.3 mAh g−1 at 0.1C and stable charge-discharge cycling at 0.3C.
高性能聚醚锂金属电池的溶剂重构及界面氟化策略
基于原位半固态聚醚电解质的锂金属电池因其制造工艺简单、能量密度高、安全可靠等优点,已成为当今研究的热点。该DOL单体具有低粘度和室温下锂盐引发聚合的特点,为高性能锂金属电池原位开环聚合制备PDOL半固态电解质提供了巨大的商业潜力。然而,聚醚电解质固有的性能缺陷和较差的抗氧化性能严重阻碍了其实际应用。利用1,1,2,2-四氟乙基2,2,3,3-四氟丙醚(TTE)作为稀释剂和氟乙烯碳酸酯(FEC)作为添加剂进行半固态聚醚电解质的溶剂重构和界面氟化,有效地缓解了这些问题。密度功能理论和分子动力学模拟表明,TTE稀释剂可以优化溶剂结构,增强阴离子配位,从而改善pdoll基电解质的电化学性能,使Li/Li对称电池在0.1 mA cm−2下稳定循环2000 h以上。此外,氟化添加剂FEC的引入在Li/NCM811高压锂金属电池中取得了优异的性能,在0.1C下具有206.3 mAh g−1的初始放电比容量,在0.3C下具有稳定的充放电循环。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Solid State Ionics
Solid State Ionics 物理-物理:凝聚态物理
CiteScore
6.10
自引率
3.10%
发文量
152
审稿时长
58 days
期刊介绍: This interdisciplinary journal is devoted to the physics, chemistry and materials science of diffusion, mass transport, and reactivity of solids. The major part of each issue is devoted to articles on: (i) physics and chemistry of defects in solids; (ii) reactions in and on solids, e.g. intercalation, corrosion, oxidation, sintering; (iii) ion transport measurements, mechanisms and theory; (iv) solid state electrochemistry; (v) ionically-electronically mixed conducting solids. Related technological applications are also included, provided their characteristics are interpreted in terms of the basic solid state properties. Review papers and relevant symposium proceedings are welcome.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信