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Fluorinated Poly-oxalate Electrolytes Stabilizing both Anode and Cathode Interfaces for All-Solid-State Li/NMC811

Han Sun1, Xiaoxin Xie1, Qiu Huang1

  • 1State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, China.

Angewandte Chemie (International Ed. in English)
|June 22, 2021
PubMed
Summary

New poly-oxalate (POE) solid polymer electrolytes offer higher ionic conductivity for lithium-ion batteries. Trifluoroacetate-terminated POE-F enhances stability and interfacial compatibility in all-solid-state cells.

Keywords:
all-solid-state batterieseutectic phenomenonhigh-voltage cellsinterfacespolymer electrolytes

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Solid polymer electrolytes (SPEs) face challenges with narrow electrochemical stability and low ionic conductivity.
  • Developing advanced SPEs is crucial for next-generation lithium-ion batteries.

Purpose of the Study:

  • To synthesize and characterize a series of poly-oxalate (POE) based solid polymer electrolytes.
  • To investigate the effect of molecular structure and terminal groups on ionic conductivity and electrochemical stability.
  • To evaluate the performance of optimized POE-based electrolytes in all-solid-state lithium-metal batteries.

Main Methods:

  • Synthesis of poly-oxalate structures with varying diol chain lengths.
  • Electrochemical characterization including ionic conductivity measurements and cyclic voltammetry.
  • Surface analysis and interfacial studies of the Li-metal/electrolyte interface.
  • Fabrication and testing of all-solid-state Li/NMC811 battery cells.

Main Results:

  • Poly-oxalates derived from odd-carbon diols exhibited higher ionic conductivity than those from even-carbon diols.
  • Propanediol-based C5-POE showed the highest Li+ conductivity among the synthesized POEs.
  • Trifluoroacetate termination (POE-F) improved oxidative stability by shifting HOMO electrons and forming a protective LiF-based SEI layer.
  • All-solid-state cells using C5-POE-F demonstrated enhanced stability compared to poly-ether counterparts.

Conclusions:

  • Poly-oxalate structures, particularly C5-POE-F, represent a promising class of solid polymer electrolytes.
  • Optimized POE-F electrolytes offer improved ionic conductivity, electrochemical stability, and interfacial properties for high-voltage lithium-metal batteries.
  • The findings pave the way for developing safer and more efficient all-solid-state batteries.