Preparation and Electrochemical Performance of Polyzwitterion Containing Intramolecular Salt as Solid Electrolytes for Lithium-ion Batteries

Shu-chang Liu; Hai-ying Wu; Ling-zhi Zhang

doi:10.11777/j.issn1000-3304.2023.23211

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Preparation and Electrochemical Performance of Polyzwitterion Containing Intramolecular Salt as Solid Electrolytes for Lithium-ion Batteries

Research Article | 更新时间：2024-02-08

- Preparation and Electrochemical Performance of Polyzwitterion Containing Intramolecular Salt as Solid Electrolytes for Lithium-ion Batteries
- Acta Polymerica Sinica Vol. 55, Issue 3, Pages: 296-308(2024)
- 作者机构：
  
  1.中国科学院可再生能源重点实验室广东省新能源和可再生能源研究开发与应用重点实验室中国科学院广州能源研究所广州 510640
  2.中国科学技术大学合肥 230026
- 作者简介：
  
  Ling-zhi Zhang, E-mail: lzzhang@ms.giec.ac.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2023.23211
  CLC：
- Published：20 March 2024，
  
  Published Online：08 December 2023，
  
  Received：18 August 2023，
  
  Accepted：19 October 2023
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刘书畅, 吴海莹, 张灵志. 锂内盐两性离子聚合物电解质的制备与电化学性能研究. 高分子学报, 2024, 55(3), 296-308

Liu, S. C.; Wu, H. Y.; Zhang, L. Z. Preparation and electrochemical performance of polyzwitterion containing intramolecular salt as solid electrolytes for lithium-ion batteries. Acta Polymerica Sinica, 2024, 55(3), 296-308
刘书畅, 吴海莹, 张灵志. 锂内盐两性离子聚合物电解质的制备与电化学性能研究. 高分子学报, 2024, 55(3), 296-308 DOI： 10.11777/j.issn1000-3304.2023.23211.

Liu, S. C.; Wu, H. Y.; Zhang, L. Z. Preparation and electrochemical performance of polyzwitterion containing intramolecular salt as solid electrolytes for lithium-ion batteries. Acta Polymerica Sinica, 2024, 55(3), 296-308 DOI： 10.11777/j.issn1000-3304.2023.23211.

摘要

与有机电解液相比，聚合物电解质可以有效提高电池的安全性和能量密度，但离子电导率低、电化学窗口较窄和对锂金属不稳定等问题限制了其实际应用. 本文工作通过自由基共聚制备了一种复合锂内盐两性离子聚合物(P(AMPSLi-IL)). 通过静电纺丝技术将不同质量比的P(AMPSLi-IL)和聚乙烯醇(PVA)制备为一系列的纳米纤维膜(PVA-P(AMPSLi-IL))，其热分解温度为280 ℃，其中PVA

-P(AMPSLi-IL)

的拉伸强度最大为13.8 MPa. 将双氟磺酰亚胺锂(LiFSI)溶于碳酸乙烯酯(EC)中，配制1 mol·L

-1

的溶液作为基础电解液. 纤维膜在基础电解液中，以二缩三丙二醇二丙烯酸酯(TPGDA)作为交联剂原位凝胶化得到电解质膜. 优化后的PVA

-P(AMPSLi-IL)

基电解质室温离子电导率高达2.87×10

-3

S·cm

-1

，锂离子迁移数高达0.85. 而且该电解质的氧化电位为4.34 V (versus Li/Li

)，优于基础电解液的3.92 V (versus

Li/Li

). 在锂锂对称电池中该电解质能保持超过1800 h的稳定循环，展示了对锂金属极佳的界面稳定性. 将该电解质应用于磷酸铁锂半电池，0.5 C下其初始放电比容量为145.7 mAh·g

-1

，200圈后的容量保持率达79.0%.

Abstract

Polymer electrolytes are known to be more effective in enhancing the safety and energy density of lithium-ion batteries as compared to organic electrolytes. However

the practical application of polymer electrolytes is hindered due to their low ionic conductivity

narrow electrochemical window

and incompatibility with lithium metal anode. In this work

a polyzwitterion (P(AMPSLi-IL)) containing intramolecular lithium salt of lithium bis(trifluoromethanesulphonyl)imide (LiTFSI) was designed and synthesized through a radical copolymerization of acryloyloxyethyltrimethyl ammonium bis(trifluoromethanesulphonyl)imide (AETATFSI) and lithium 2-acrylamido-2-methylpropanesulfonic acid (AMPSLi). A series of nanofiber membranes composed of poly(vinyl alcohol) (PVA) and P(AMPSLi-IL) were prepared by electrospinning technology. The nanofiber membrane with optimized ratio of PVA to P(AMPSLi-IL) shows a high tensile strength of 13.8 MPa and thermal decomposition temperature of 280 ℃. The nanofiber membranes were

in situ

gelated in a based electrolyte (1 mol/L LiFSI in EC) with tri-(propylene glycol) diacrylate (TPGDA) as a crosslinking agent

which was used as a polymeric solid electrolyte. The optimized electrolyte of PVA

-P(AMPSLi-IL)

exhibited a high ionic conductivity of 2.87×10

-3

S·cm

-1

at room-temperature

high lithium transference number of 0.85 and oxidation potential of 4.34 V (versus Li/Li

). The symmetric Li|Li cell with the PVA

-P(AMPSLi-IL)

electrolyte shows an excellent cycle stability for over 1800 h

demonstrating a great compatibility between Li anode and the PVA

-P(AMPSLi-IL)

electrolyte. The LFP|Li half cell with the PVA

-P(AMPSLi-IL)

electrolyte delivers an initial discharge capacity of 145.7 mAh·g

-1

at 0.5 C with a capacity retention of 79.0% after 200 cycles.

关键词

锂金属电池聚合物电解质两性离子聚合物聚乙烯醇

Keywords

Lithium metal batteryPolymer electrolytePolyzwitterionPoly(vinyl alcohol)

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