Multiscale Grain Structure Regulation of Ionic Conductivity in Poly(ethylene oxide)-based Solid-state Electrolytes

LI Jia-hao; SONG Qi; WAN Lu; LI Zhao-lei

doi:10.14028/j.cnki.1003-3726.2025.25.245

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Multiscale Grain Structure Regulation of Ionic Conductivity in Poly(ethylene oxide)-based Solid-state Electrolytes

更新时间：2025-12-05

- Multiscale Grain Structure Regulation of Ionic Conductivity in Poly(ethylene oxide)-based Solid-state Electrolytes
  增强出版
- Polymer Bulletin Vol. 38, Issue 12, Pages: 1856-1865(2025)
- 作者机构：
  
  江苏科技大学材料科学与工程学院，镇江 212100
- 作者简介：
- 基金信息：
- DOI：10.14028/j.cnki.1003-3726.2025.25.245
  CLC：
- Received：28 August 2025，
  
  Accepted：30 September 2025，
  
  Published Online：14 November 2025，
  
  Published：20 December 2025
- 稿件说明：
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李佳豪, 宋琪, 万露, 李照磊. 聚环氧乙烷基固态电解质离子电导率的多尺度晶粒结构调控机制. 高分子通报, 2025, 38(12), 1856–1865.

Li, J. H.; Song, Q.; Wan, L.; Li, Z. L. Multiscale grain structure regulation of ionic conductivity in poly(ethylene oxide)-based solid-state electrolytes. Polym. Bull. (in Chinese), 2025, 38(12), 1856–1865.
李佳豪, 宋琪, 万露, 李照磊. 聚环氧乙烷基固态电解质离子电导率的多尺度晶粒结构调控机制. 高分子通报, 2025, 38(12), 1856–1865. DOI： 10.14028/j.cnki.1003-3726.2025.25.245.

Li, J. H.; Song, Q.; Wan, L.; Li, Z. L. Multiscale grain structure regulation of ionic conductivity in poly(ethylene oxide)-based solid-state electrolytes. Polym. Bull. (in Chinese), 2025, 38(12), 1856–1865. DOI： 10.14028/j.cnki.1003-3726.2025.25.245.

摘要

聚环氧乙烷(PEO)基固态电解质在室温下的高结晶度严重限制了其离子电导率，而传统降低结晶度的方法往往会牺牲其机械性能。本研究旨在探索除结晶度大小外，影响离子电导率的关键因素。通过退火工艺，系统调控了PEO/LiTFSI固态电解质的聚集态结构，并结合多尺度表征，分析了其结晶行为与离子电导率的关系。研究发现，离子电导率的变化与结晶度并非简单线性关系，晶粒尺寸是更为关键的调控离子电导率大小的参数。通过退火工艺将PEO平均晶粒尺寸从29.2 nm细化至6 nm，室温离子电导率从4.26×10

−7

S·cm

−1

提高至3.18×10

−6

S·cm

−1

，提升7.5倍。此外，研究进一步揭示了晶粒尺寸、表面形貌与片层结构等多尺度因素的协同机制。研究结果表明，精确调控晶粒尺寸而非简单降低结晶度，是显著提升PEO基固态电解质离子电导率的有效策略，为设计高性能聚合物电解质提供了新的思路。

Abstract

The high crystallinity of poly(ethylene oxide) (PEO)-b

ased solid electrolytes at room temperature severely limits their ionic conductivity

while traditional strategies of reducing crystallinity often compromise mechanical properties. This study aimed to explore key factors influencing ionic conductivity beyond the degree of crystallinity. By employing annealing processes

we systematically regulated the aggregation structure of PEO/LiTFSI solid electrolytes and correlated their crystallization behavior with ionic conductivity through multi-scale characterization. The results revealed that the variation in ionic conductivity did not follow a simple linear relationship with crystallinity; instead

grain size was identified as a more critical parameter. Refining the average grain size of PEO from 29.2 nm to 6.0 nm

via

annealing increased the room-temperature ionic conductivity from 4.26×10

-7

S·cm

-1

to 3.18×10

-6

S·cm

-1

representing a 7.5-fold enhancement. Furthermore

the synergistic effects of multi-scale factors—including grain size

surface morphology

and lamellar structure—were elucidated. This work demonstrates that precise control of grain size

rather than simply reducing crystallinity

is an effective strategy for significantly improving the ionic conductivity of PEO-based solid electrolytes

offering new insights for the design of high-performance polymer electrolytes.

关键词

Keywords

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