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<p>Solid polymer electrolytes, particularly those based on poly(ethylene oxide) (PEO), are considered promising candidates for next-generation lithium-metal batteries due to their lightweight, low cost, and favorable processability. However, their practical application is severely hindered by low ionic conductivity and unstable electrode-electrolyte interfaces. In this study, we introduce an organic small-molecule additive, 4-methylsulfonylbenzonitrile (FCN), which improves ionic conductivity and ensures high interfacial compatibility of PEO-based electrolytes. The hydrogen bonding between FCN and PEO facilitates the formation of a cross-linked network, the strong interaction between the lone pair electrons of the −CN and −EO− groups weakens the Li−O coordination, thereby creating a fast Li<sup>+</sup> conduction pathway. Moreover, the incorporation of FCN promotes the formation of a robust, inorganic-rich solid-electrolyte interphase, which can facilitate smooth lithium deposition. As a result, the PEO-FCN electrolyte achieves an approximately 4-fold increase in ionic conductivity and up to 0.5 in Li<sup>+</sup> transference number. The assembled Li symmetrical battery exhibits a cycle life exceeding 2000 h. The cells with LiFePO<sub>4</sub> and LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> cathodes demonstrate excellent long-cycle and rate performance. These findings highlight the potential of PEO-FCN electrolytes in advancing high-performance lithium-metal batteries.</p>

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Constructing fast ion transport and stable interface in PEO-based solid-state lithium metal batteries with bifunctional additives

  • 期刊论文

  • 发表日期：

    2025年4月10日

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  • Kexin Zhang,
  • Shengjun Xu,
  • Ruogu Xu,
  • Tong Yu,
  • Zhenhua Sun,
  • Feng Li

摘要

Solid polymer electrolytes, particularly those based on poly(ethylene oxide) (PEO), are considered promising candidates for next-generation lithium-metal batteries due to their lightweight, low cost, and favorable processability. However, their practical application is severely hindered by low ionic conductivity and unstable electrode-electrolyte interfaces. In this study, we introduce an organic small-molecule additive, 4-methylsulfonylbenzonitrile (FCN), which improves ionic conductivity and ensures high interfacial compatibility of PEO-based electrolytes. The hydrogen bonding between FCN and PEO facilitates the formation of a cross-linked network, the strong interaction between the lone pair electrons of the −CN and −EO− groups weakens the Li−O coordination, thereby creating a fast Li+ conduction pathway. Moreover, the incorporation of FCN promotes the formation of a robust, inorganic-rich solid-electrolyte interphase, which can facilitate smooth lithium deposition. As a result, the PEO-FCN electrolyte achieves an approximately 4-fold increase in ionic conductivity and up to 0.5 in Li+ transference number. The assembled Li symmetrical battery exhibits a cycle life exceeding 2000 h. The cells with LiFePO4 and LiNi0.8Mn0.1Co0.1O2 cathodes demonstrate excellent long-cycle and rate performance. These findings highlight the potential of PEO-FCN electrolytes in advancing high-performance lithium-metal batteries.