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<p>Developing safe and high-performance solid polymer electrolytes (SPEs) remains a critical challenge for all-solid-state batteries. Among various polymer materials, poly(ethylene oxide) (PEO) is most widely studied, while poly(vinylidene fluoride) (PVDF) has also attracted great interest recently. However, the intrinsic disadvantages of single polymers make them hardly meet the demands for practical applications. Physical blending of different types of SPEs is a simple and straightforward strategy to optimize their performance. Unfortunately, the direct blending of PEO and PVDF (or PVDF derivatives) usually leads to macro-phase separation and fails to couple together. Herein, we designed and synthesized PEO-based block copolymers as compatibilizers to prevent macroscopic phase separation in PVDF/PEO blends. By tuning the interfacial compatibility, continuous nanostructures with high optical transparency are constructed through the microphase segregation. The obtained SPEs combine the merits of high mechanical modulus (380 MPa), high ionic conductivity (2.0 × 10<sup>−4</sup> S cm<sup>−1</sup>, 30 °C), large transference number (0.60), and electrochemical stability (4.5 V). This simple and efficient chemical modification approach sheds light on alternative solutions for designing high-performance SPEs.</p>

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Tuning the interfacial compatibility of poly(vinylidene difluoride) and poly(ethylene oxide) blends for improved solid-state polymer electrolytes

  • 期刊论文

  • 发表日期：

    2025年11月19日

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  • Yongmei Zhu,
  • Jinyi Cui,
  • Yunduo Ma,
  • Yichen He,
  • Shuhao Liu,
  • Junye He,
  • Jinxin Xie,
  • Rongchun Zhang,
  • Shuqi Dai,
  • Mingjun Huang

摘要

Developing safe and high-performance solid polymer electrolytes (SPEs) remains a critical challenge for all-solid-state batteries. Among various polymer materials, poly(ethylene oxide) (PEO) is most widely studied, while poly(vinylidene fluoride) (PVDF) has also attracted great interest recently. However, the intrinsic disadvantages of single polymers make them hardly meet the demands for practical applications. Physical blending of different types of SPEs is a simple and straightforward strategy to optimize their performance. Unfortunately, the direct blending of PEO and PVDF (or PVDF derivatives) usually leads to macro-phase separation and fails to couple together. Herein, we designed and synthesized PEO-based block copolymers as compatibilizers to prevent macroscopic phase separation in PVDF/PEO blends. By tuning the interfacial compatibility, continuous nanostructures with high optical transparency are constructed through the microphase segregation. The obtained SPEs combine the merits of high mechanical modulus (380 MPa), high ionic conductivity (2.0 × 10−4 S cm−1, 30 °C), large transference number (0.60), and electrochemical stability (4.5 V). This simple and efficient chemical modification approach sheds light on alternative solutions for designing high-performance SPEs.