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高电压锂金属电池的局部高浓度电解液设计及其电化学性能

黄德权1,阳复建1,陈元华1,张曼1,殷广达1,韦韬1,莫皓越2,莫晓敏2,梁毅1   

  1. 1. 桂林航天工业学院汽车工程学院 2. 桂林市产品质量检验所
  • 收稿日期:2026-03-30 修回日期:2026-06-09 出版日期:2026-06-10 发布日期:2026-06-10
  • 通讯作者: 梁毅 E-mail:liangyi@guat.edu.cn
  • 基金资助:
    广西自然科学基金(批准号:2026GXNSFHA00640205,2026GXNSFHA00640038)、桂林航天工业学院特色优势交叉学科发展战略研究专项(批准号:TS2024141)和广西首批青苗人才科研启动基金资助

Design and electrochemical performance of locally high concentration electrolyte for high-voltage lithium metal batteries

HUANG Dequan1, YANG Fujian1, CHEN Yuanhua1*, ZHANG Man1, YIN Guangda1, WEI Tao1, MO Haoyue2*, MO Xiaomin2, LIANG Yi1*   

  1. 1. School of Automotive Engineering, Guilin University of Aerospace Technology 2. Guilin Institute of Testing on Product Quality
  • Received:2026-03-30 Revised:2026-06-09 Online:2026-06-10 Published:2026-06-10
  • Contact: Yi LIANG E-mail:liangyi@guat.edu.cn
  • Supported by:
    Supported by the Guangxi Natural Science Foundation, China(Nos. 2026GXNSFHA00640205, 2026GXNSFHA00640038), the GUAT Special Research Project on the Strategic Development of Distinctive Interdisciplinary Fields, China(No.TS2024141) and the Guangxi's First Batch of Qingmiao Talent Universal Support Program for Scientific Research Start-up Fund, China

摘要: 锂金属负极具有极高的理论比容量和极低的电化学电位,是下一代高比能电池体系的重要发展方向。然而,高电压锂金属电池(LMBs)的实际应用仍受到锂枝晶无序生长、固态电解质界面(SEI)不稳定以及传统醚基电解液在高电压下稳定性不足等问题的制约。本文通过引入氟化共溶剂1,1,2,2-四氟乙基-2,2,3,3-四氟丙基醚(TTE),构建了一种局域高浓度电解液(LHCE)体系。结合分子动力学模拟与原位光学显微镜表征结果发现,TTE中氟原子的强电负性能够有效调控阴离子配位结构,促进富无机组分SEI膜的形成,显著改善Li+传输动力学,并有效抑制锂枝晶生长。电化学测试表明,采用LHCE的Li||Cu半电池在0.5 mA cm-2下循环670次后平均库伦效率仍可达98.5%。同时,基于LHCE的全电池同样表现出优异的电化学性能:Li||LFP全电池在1.0 C下循环400次后容量保持率为97.4%,Li||NCM811全电池在1.0 C下循环500次后容量保持率为68.8%。本研究为高电压锂金属电池的电解液设计与界面调控提供了一种有效策略。

关键词: 锂金属电池, 局部高浓度电解液, TTE共溶剂, 界面调控, 电化学性能

Abstract: Lithium metal is regarded as one of the most promising anode materials for next- generation high-energy-density batteries because of its ultrahigh theoretical specific capacity and low electrochemical potential. However, the practical application of high-voltage lithium metal batteries (LMBs) is still severely hindered by uncontrolled lithium dendrite growth, unstable solid electrolyte interphase (SEI), and the poor oxidative stability of conventional ether-based electrolytes. Herein, a localized high-concentration electrolyte (LHCE) is constructed by introducing the fluorinated co-solvent 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). Combined molecular dynamics simulations and in-situ optical microscopy reveal that the strong electronegativity of fluorine atoms in TTE effectively regulates the anion coordination structure, promotes the formation of an inorganic-rich SEI, markedly improves Li+ transport kinetics, and suppresses lithium dendrite growth. Electrochemical measurements show that the Li||Cu half-cell with LHCE delivers an average Coulombic efficiency of 98.5% after 670 cycles at 0.5 mA cm-2. The full cells based on LHCE also exhibit excellent electrochemical performance: the Li||LFP cell retains 97.4% of its capacity after 400 cycles at 1.0 C, while the Li||NCM811 cell maintains 68.8% capacity retention after 500 cycles at 1.0 C. This work provides an effective strategy for electrolyte design and interfacial regulation in high-voltage LMBs.

Key words: Lithium metal battery, Localized high-concentration electrolyte, TTE cosolvent; Interphase regulation, Electrochemical performance

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