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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Unlocking solid-state conversion batteries reinforced by hierarchical microsphere stacked polymer electrolyte.

Jiulin Hu1, Keyi Chen2, Zhenguo Yao2

  • 1State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China.

Science Bulletin
|January 19, 2023
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Summary

This study introduces a novel all-solid-state lithium metal battery using a polymer electrolyte with g-C3N4 and a FeF3 cathode. This design enhances safety and energy density for advanced lithium batteries.

Keywords:
All-solid-state batteriesC-N filler reinforcementConversion fluoride cathodeLi dendrite suppressionPolymer electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • All-solid-state lithium metal batteries (ASSLMBs) offer enhanced safety and energy density but face challenges with compatible solid electrolytes and reversible conversion cathodes.
  • Electrode-electrolyte interface instability, due to cathode phase transformation and anode lithium deformation, hinders ASSLMB performance.
  • Existing solid-state battery designs struggle with issues like polysulfide leakage, limiting their true all-solid-state potential.

Purpose of the Study:

  • To develop a novel all-solid-state lithium-metal battery utilizing a hierarchical microsphere stacked polymer electrolyte with a FeF3 conversion cathode.
  • To address the challenges of interface stability and product management in conversion-type lithium metal batteries.
  • To enhance both safety and energy density in next-generation lithium metal batteries.

Main Methods:

  • Fabrication of a graphene-like carbon nitride (g-C3N4) stuffed polyethylene oxide (PEO)-based polymer electrolyte.
  • Integration of the polymer electrolyte with a Li-FeF3 conversion cathode and lithium metal anode.
  • Characterization of electrochemical performance, including cycling stability, rate capability, and interface properties.

Main Results:

  • The developed polymer electrolyte exhibits improved ionic conductivity (2.5 × 10⁻⁴ S/cm at 60°C) and a high Li⁺ transference number (0.69).
  • The battery demonstrates ultra-long lithium plating/striping cycling (>10,000 h) and high rate capability (12 C for Li/LiFePO4 cells).
  • All-solid-state Li/FeF3 cells achieve a stabilized capacity of 300 mAh/g over 200 cycles and ~200 mAh/g at 5 C, with over 1200 cycles at 1 C.

Conclusions:

  • The proposed g-C3N4 stuffed PEO polymer electrolyte effectively stabilizes the electrode-electrolyte interfaces in all-solid-state lithium metal batteries.
  • This approach provides a promising solution for high-energy and safe conversion-type lithium metal batteries, overcoming limitations of previous designs.
  • The battery's performance, driven by high pseudocapacitance and diffusion coefficients, paves the way for advanced energy storage solutions beyond Li-S batteries.