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Updated: Aug 26, 2025

Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Fabrication of Oxide-Based All-Solid-State Batteries by a Sintering Process Based on Function Sharing of Solid

Miyuki Sakakura1, Kazutaka Mitsuishi2, Toyoki Okumura3

  • 1Department of Materials Design Innovation Engineering, Graduate School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8603, Japan.

ACS Applied Materials & Interfaces
|October 3, 2022
PubMed
Summary

A novel multilayer solid electrolyte combining garnet-type Li7La3Zr2O12 (LLZ) and LISICON-type Li3.5Ge0.5V0.5O4 (LGVO) enhances all-solid-state battery performance. This approach mitigates reactivity issues during sintering, enabling stable cycling.

Keywords:
Li7La3Zr2O12aerosol depositioninterfacesinteringsolid electrolytesolid-state battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Garnet-type Li7La3Zr2O12 (LLZ) offers high ionic conductivity and Li metal stability but reacts with electrodes during sintering.
  • LISICON-type Li3.5Ge0.5V0.5O4 (LGVO) exhibits lower reactivity but has inferior ionic conductivity.

Purpose of the Study:

  • To develop a multilayer solid electrolyte combining LLZ and LGVO to leverage their complementary properties.
  • To improve the stability and performance of oxide-based all-solid-state batteries.

Main Methods:

  • Coating thin LGVO films (2 μm) onto LLZ sheets to create a multilayer structure.
  • Annealing the LLZ-LGVO multilayer with LiCoO2 and a lithium metal anode at 700 °C.
  • Evaluating the electrochemical performance and interfacial properties of the resulting all-solid-state battery.

Main Results:

  • The LLZ-LGVO multilayer demonstrated good adhesion via Ge diffusion with minimal interfacial resistance.
  • The LGVO coating effectively suppressed resistance increases from annealing by approximately 1/40.
  • The fabricated all-solid-state battery achieved over 100 charge-discharge cycles at 25 and 60 °C.

Conclusions:

  • Function sharing between LLZ and LGVO in a multilayer solid electrolyte is a promising strategy for oxide-based all-solid-state batteries.
  • This approach overcomes sintering-induced reactivity issues, paving the way for advanced solid-state battery development.
  • The developed multilayer solid electrolyte offers a viable path towards stable and high-performance all-solid-state batteries.