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Engineering a High-Voltage Durable Cathode/Electrolyte Interface for All-Solid-State Lithium Metal Batteries via In

Qi Li1, Xiaoyu Zhang1, Jian Peng1

  • 1State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, People's Republic of China.

ACS Applied Materials & Interfaces
|April 28, 2022
PubMed
Summary

Researchers developed a new interface layer for poly(ethylene oxide) (PEO)-based solid polymer electrolytes. This innovation enhances stability for high-voltage lithium-ion batteries, improving energy density and paving the way for next-generation solid-state batteries.

Keywords:
all-solid-state lithium batterycathode electrolyte interphasehigh voltageinterface engineeringpoly(trifluoroethyl methacrylate)

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Poly(ethylene oxide) (PEO)-based polymer electrolytes offer flexibility and good interface contact for lithium metal anodes.
  • The poor oxidation resistance of PEO limits its use with high-voltage cathodes, restricting energy density in solid-state batteries.

Purpose of the Study:

  • To develop a high-voltage stable solid-state interface layer for PEO-based polymer electrolytes.
  • To overcome the oxidation limitations of PEO for compatibility with high-voltage cathodes.
  • To enable higher energy density in solid-state lithium batteries.

Main Methods:

  • In situ solvent-free bulk electropolymerization was used to construct a polyfluoroalkyl acrylate interface layer.
  • The interface layer was formed between a LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode and a PEO-based solid polymer electrolyte.
  • Electrochemical characterization was performed to assess the oxidation window and ionic conductivity.

Main Results:

  • The electrochemical oxidation window of the electrolyte was expanded from 4.3 V to 5.1 V.
  • Ionic conductivity was improved to 1.02 × 10^-4 S cm^-1 at ambient temperature and 4.72 × 10^-4 S cm^-1 at 60 °C.
  • Enhanced Li+ migration contributed to the improved ionic conductivity.

Conclusions:

  • The in situ electrochemical fabrication of an interface buffer layer is an innovative and universal strategy for engineering solid-state batteries.
  • This approach enables high-performance, high-energy-density solid-state lithium batteries with improved voltage stability.
  • The developed method paves the way for the large-scale production of next-generation solid-state lithium batteries.