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Recyclable Li-Metal Battery Electrolytes via In Situ Cyclic Carbonate Polymerization.

Hui Gao1,2,3, Victor Riesgo-Gonzalez1,3, James R Runge1,3

  • 1Chemistry Research Laboratory, University of Oxford, Oxford, OX1 3TA, UK.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
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Summary

This study introduces a novel semi-solid polymer electrolyte for lithium batteries, formed via in situ polymerization of trimethylene carbonate (TMC). The electrolyte offers excellent performance and enables efficient chemical recycling of the polymer, advancing battery sustainability.

Keywords:
batteriesin situ polymerizationslithium metalpolymer electrolytesrecycling

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Next-generation rechargeable batteries require improved electrolyte performance and recyclability.
  • Current battery electrolytes face challenges in balancing efficiency, stability, and environmental impact.

Purpose of the Study:

  • To develop a novel semi-solid polymer electrolyte for lithium batteries using in situ polymerization.
  • To evaluate the electrochemical performance and recyclability of the developed electrolyte.
  • To demonstrate a strategy for enhancing battery sustainability and circular economy principles.

Main Methods:

  • Equilibrium ring-opening polymerization of trimethylene carbonate (TMC) in the presence of lithium difluoro(oxalato)borate salt.
  • In situ electrolyte formation during coin cell fabrication.
  • Electrochemical performance testing (cycling, rate capability) with lithium iron phosphate cathodes.
  • Solid-state chemical recycling of the polymer electrolyte.

Main Results:

  • A semi-solid poly(trimethylene carbonate) electrolyte was successfully synthesized in situ.
  • The electrolyte exhibited high ionic conductivity (0.52 mS cm⁻¹), thermal stability (160 °C), and oxidative stability (4.7 V).
  • Cells demonstrated excellent cycling stability (97% retention after 350 cycles at 2C) and rate capability.
  • A solid-state chemical recycling process effectively recovered the TMC monomer, enabling identical repolymerization and cell performance.

Conclusions:

  • Exploiting polymerization-depolymerization equilibria is a viable strategy for advanced battery electrolytes.
  • The developed electrolyte enhances battery performance and facilitates efficient material recycling.
  • This approach contributes to sustainable battery technologies and a circular economy.