Citation: Xiaofei Wang, Shuonan Wang, Zhangkuo Han, Jiahan Zheng, Yu Chen, Libing Liao, Hao Liu. Shear-engineered flower-like spherulites enable record ionic conductivity of PEO-based electrolytes for solid-state lithium batteries[J]. Chinese Chemical Letters, ;2026, 37(2): 111434. doi: 10.1016/j.cclet.2025.111434 shu

Shear-engineered flower-like spherulites enable record ionic conductivity of PEO-based electrolytes for solid-state lithium batteries

Xiaofei Wang ^{a, b} ,
Shuonan Wang ^a ,
Zhangkuo Han ^c ,
Jiahan Zheng ^c ,
Yu Chen ^d ,
Libing Liao ^{a, *,} ,
Hao Liu ^{c, *,}

a.
Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources, Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China
b.
Shandong Haihua Group Co., Ltd., Weifang 261000, China
c.
School of Science, China University of Geosciences, Beijing 100083, China
d.
Beijing Synchrotron Radiation Facility Institute of High Energy Physics, Chinese Academy of Science, Beijing 100049, China

clayl@cugb.edu.cn

liuhao1398@cugb.edu.cn

Received Date: 11 May 2025
Revised Date: 7 June 2025
Accepted Date: 10 June 2025
Available Online: 10 June 2025

Figures(6)

Polyethylene oxide (PEO)-based solid polymer electrolytes (SPEs) have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes. Here, we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions, which self-assemble into flower-like spherulites with radially aligned lamellar crystals. This unique structure creates continuous Li⁺ transport highways through densely packed crystalline domains, achieving a record-high ionic conductivity of 1.70 × 10^–4 S/cm at 25 ℃ for pristine PEO-based systems. Strategic incorporation of lithium montmorillonite (MMTli, 10 wt%) further optimizes the composite electrolyte, balancing high ionic conductivity (1.47 × 10^–4 S/cm) with enhanced electrochemical stability (4.99 V vs. Li⁺/Li), elevated Li⁺ transference number (0.62), and mechanical robustness. The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO₄||Li solid-state batteries with 82% capacity retention after 200 cycles at 0.2 C under ambient conditions. This work pioneers a scalable processing paradigm for crystalline polymer electrolytes, offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.
- Solid polymer electrolytes,
- Polyethylene oxide,
- Flower-like spherulite,
- Montmorillonite,
- Solid-state lithium batteries
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