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Updated: Jun 15, 2025

Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Polar groups promoting in-situ polymerization phase separation for solid electrolytes enabling solid-state lithium

Yongrui Luo1, Yinnan Qian1, Minghui Cai1

  • 1College of Chemistry and Environmental Engineering, International Joint Research Center for Molecular Science, Shenzhen University, Shenzhen, Guangdong 518060, PR China.

Journal of Colloid and Interface Science
|August 24, 2024
PubMed
Summary

Designing plastic-crystal-embedded elastomer electrolytes (PCEEs) with specific functional groups is key for stable lithium metal batteries. Fluorinated PCEEs show superior performance due to enhanced phase separation and interfacial stability.

Keywords:
Lithium metal batteriesPolymer solid electrolytesPolymer-induced phase separationSolid-state batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Plastic-crystal-embedded elastomer electrolytes (PCEEs) are advanced solid polymer electrolytes (SPEs) produced via polymerization-induced phase separation (PIPS).
  • Investigating monomer influence on PIPS and lithium metal battery (LMB) performance is crucial for optimizing SPEs.

Purpose of the Study:

  • To explore the impact of different functional groups (OH, CN, F) on PIPS in PCEEs.
  • To evaluate the performance of PCEEs with varying functional groups in lithium metal batteries.

Main Methods:

  • In situ polymerization to synthesize PCEEs with OH, CN, and F functional groups.
  • Characterization of phase separation in PCEEs using techniques like SEM and TEM (implied).
  • Electrochemical testing of PCEEs in lithium symmetric cells and LiFePO4/Li and NCM622/Li batteries.

Main Results:

  • PCEEs with CN and F monomers achieved successful phase separation, unlike the OH-functionalized PCEE due to hydrogen bonding.
  • Fluorinated PCEE (FBA-PCEE) demonstrated excellent interfacial stability with Li metal anodes and LFP cathodes.
  • FBA-PCEE exhibited high ionic conductivity (2.02 × 10⁻³ S cm⁻¹) and a Li-ion transference number of 0.75.
  • Stable cycling of Li symmetric cells (>1000 h) and LiFePO4 batteries (>500 cycles) with FBA-PCEE.
  • Good performance in NCM622/Li batteries with 78.95% capacity retention after 100 cycles.

Conclusions:

  • Monomer functionalization critically influences PIPS and the resulting PCEE properties.
  • Fluorinated monomers are promising for developing high-performance PCEEs for advanced lithium metal batteries.
  • This work provides insights into designing novel SPEs for safer and more efficient energy storage devices.