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<p>Quasi-solid-state composite electrolytes (QSCEs) show promise for high-performance solid-state batteries, while they still struggle with interfacial stability and cycling performance. Herein, a F-grafted QSCE (F-QSCE) was developed via copolymerizing the F monomers and ionic liquid monomers. The F-QSCE demonstrates better overall performance, such as high ionic conductivity of 1.21&#xa0;mS&#xa0;cm<sup>–1</sup> at 25&#xa0;°C, wide electrochemical windows of 5.20&#xa0;V, and stable cycling stability for Li//Li symmetric cells over 4000&#xa0;h. This is attributed to the significant electronegativity difference between C and F in the fluorinated chain (‒CF<sub>2</sub>‒CF‒CF<sub>3</sub>), which causes the electron cloud to shift toward the F atom, surrounding it with a negative charge and producing the inductive effect. Furthermore, the interactions between Li<sup>+</sup> and F, TFSI<sup>‒</sup>, and C are enhanced, reducing ion pair aggregation (Li<sup>+</sup>‒TFSI<sup>‒</sup>‒Li<sup>+</sup>) and promoting Li<sup>+</sup> transport. Besides, ‒CF<sub>2</sub>‒CF‒CF<sub>3</sub> decomposes to form LiF preferentially over TFSI<sup>–</sup>, resulting in better interfacial stability for F-QSCE. This work provides a pathway to enable the development of high-performance Li metal batteries.</p>

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Induction Effect of Fluorine-Grafted Polymer-Based Electrolytes for High-Performance Lithium Metal Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月13日

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  • Haiman Hu,
  • Jiajia Li,
  • Fei Lin,
  • Jiaqi Huang,
  • Huaiyang Zheng,
  • Haitao Zhang,
  • Xiaoyan Ji

摘要

Quasi-solid-state composite electrolytes (QSCEs) show promise for high-performance solid-state batteries, while they still struggle with interfacial stability and cycling performance. Herein, a F-grafted QSCE (F-QSCE) was developed via copolymerizing the F monomers and ionic liquid monomers. The F-QSCE demonstrates better overall performance, such as high ionic conductivity of 1.21 mS cm–1 at 25 °C, wide electrochemical windows of 5.20 V, and stable cycling stability for Li//Li symmetric cells over 4000 h. This is attributed to the significant electronegativity difference between C and F in the fluorinated chain (‒CF2‒CF‒CF3), which causes the electron cloud to shift toward the F atom, surrounding it with a negative charge and producing the inductive effect. Furthermore, the interactions between Li+ and F, TFSI‒, and C are enhanced, reducing ion pair aggregation (Li+‒TFSI‒‒Li+) and promoting Li+ transport. Besides, ‒CF2‒CF‒CF3 decomposes to form LiF preferentially over TFSI–, resulting in better interfacial stability for F-QSCE. This work provides a pathway to enable the development of high-performance Li metal batteries.