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High Salt-Content Plasticized Flame-Retardant Polymer Electrolytes.

Lu Bai1, Sina Ghiassinejad1, Jérémy Brassinne1

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Summary

New flame-retardant solid polymer electrolytes using poly(dimethyl(methacryloyloxy)methyl phosphonate) (PMAPC1) offer high ionic conductivity and a wide electrochemical stability window for advanced high-energy batteries.

Keywords:
LiTFSIPMAPC1lithium-ion batteriespolyetherssolid polymer electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Conventional polyether-based electrolytes have limited voltage windows, hindering next-generation high-energy battery development.
  • Solid polymer electrolytes are crucial for overcoming these limitations and improving battery safety.

Purpose of the Study:

  • To introduce a novel flame-retardant phosphorus-containing polymer, poly(dimethyl(methacryloyloxy)methyl phosphonate) (PMAPC1), as a polymer matrix for solid polymer electrolytes.
  • To investigate the ionic conductivity, electrochemical stability, and performance of PMAPC1-based electrolytes in lithium batteries.

Main Methods:

  • Fabrication of free-standing membranes by mixing PMAPC1 with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and acetonitrile (AN).
  • Characterization of ionic conductivity and electrochemical stability window.
  • Atomistic molecular modeling simulations to understand electrolyte structure and ion transport.
  • Cycling performance evaluation using LiFePO4|PMAPC1 + LiTFSI + AN|Li battery configurations.

Main Results:

  • PMAPC1-based electrolytes achieved ionic conductivities up to 1.6 × 10-3 S cm-1 at 100 °C.
  • A stable LiF solid-electrolyte interphase was formed, suppressing Li dendrites and AN degradation.
  • Electrolyte membranes exhibited a wide electrochemical stability window above 4.7 V versus Li+/Li.
  • The phosphorus-containing polymer imparted flame-retardant properties.

Conclusions:

  • PMAPC1 is a promising polymer matrix for high-performance solid polymer electrolytes.
  • The developed electrolytes demonstrate excellent electrochemical stability, ionic conductivity, and safety features.
  • Stable cycling performance was achieved in LiFePO4|PMAPC1 + LiTFSI + AN|Li batteries, highlighting their potential for next-generation energy storage.