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<p>The development of stable solid-electrolyte interphases (SEI) represents a fundamental challenge for Li-metal batteries. Although fluorinated reagents improve cycling performance through LiF-rich SEI formation, their associated costs and environmental impacts remain problematic. Here, we present a fluorine-free quasi-solid polymer electrolyte that generates an O/N -containing hybrid SEI with improved interfacial stability and Li<sup>+</sup> transport kinetics. This unique SEI architecture preferentially directs Li deposition along the (200) crystallographic plane while enhancing charge-transfer efficiency. When implemented in Li | |LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> full cells, the fluorine-free gel polymer electrolyte enables a capacity retention of 84.7% over 800 cycles at 3 C. The fluorine-free gel polymer electrolyte system reported here exhibits improved high-rate performance compared to conventional fluorinated polymer electrolytes, providing a sustainable materials design paradigm for next-generation solid-state batteries.</p>

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Fluorine-free gel polymer electrolyte for lithium oxide-rich solid electrolyte interphase and stable Li metal batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年10月21日

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  • Weijian Xu,
  • Lingxi Zhou,
  • Songxin Lu,
  • Jiahui He,
  • Yongbin Xu,
  • Lei Tian

摘要

The development of stable solid-electrolyte interphases (SEI) represents a fundamental challenge for Li-metal batteries. Although fluorinated reagents improve cycling performance through LiF-rich SEI formation, their associated costs and environmental impacts remain problematic. Here, we present a fluorine-free quasi-solid polymer electrolyte that generates an O/N -containing hybrid SEI with improved interfacial stability and Li+ transport kinetics. This unique SEI architecture preferentially directs Li deposition along the (200) crystallographic plane while enhancing charge-transfer efficiency. When implemented in Li | |LiNi0.8Co0.1Mn0.1O2 full cells, the fluorine-free gel polymer electrolyte enables a capacity retention of 84.7% over 800 cycles at 3 C. The fluorine-free gel polymer electrolyte system reported here exhibits improved high-rate performance compared to conventional fluorinated polymer electrolytes, providing a sustainable materials design paradigm for next-generation solid-state batteries.