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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Phase regulation enabling dense polymer-based composite electrolytes for solid-state lithium metal batteries.

Qian Wu1,2, Mandi Fang3, Shizhe Jiao4

  • 1State Key Laboratory of Chemical Engineering, Institute of Pharmaceutical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, Zhejiang, China.

Nature Communications
|October 9, 2023
PubMed
Summary

This study introduces a novel dense composite electrolyte using poly(vinylidene fluoride) and MoSe2 sheets for solid-state lithium metal batteries. This approach enhances ionic conductivity and interfacial stability for improved battery performance.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Science

Background:

  • Solid polymer electrolytes are crucial for safe and scalable solid-state lithium metal batteries.
  • Poly(vinylidene fluoride)-based electrolytes offer room-temperature operation but suffer from poor ionic conductivity and porous structures.
  • Achieving large-scale processability and good interfacial compatibility remains a challenge for practical applications.

Purpose of the Study:

  • To develop a dense composite electrolyte with enhanced ionic conductivity and interfacial properties for solid-state lithium metal batteries.
  • To investigate the effect of incorporating molybdenum diselenide (MoSe2) sheets into a poly(vinylidene fluoride) matrix.
  • To improve the performance and stability of lithium metal batteries through a phase regulation strategy.

Main Methods:

  • A phase regulation strategy was employed by incorporating molybdenum diselenide (MoSe2) sheets into poly(vinylidene fluoride) (PVDF) to create a dense composite electrolyte.
  • The high dielectric constant of the electrolyte was utilized to optimize solvation structures and enhance ionic conductivity.
  • In-situ reactions between MoSe2 and lithium metal were studied to form a Li2Se fast conductor layer.

Main Results:

  • The incorporation of MoSe2 sheets disrupted the symmetry of PVDF chains, leading to a dense composite electrolyte with high ionic conductivity and low activation energy.
  • The in-situ generated Li2Se layer at the solid electrolyte interphase significantly improved Coulombic efficiency and interfacial kinetics.
  • Solid-state Li||Li cells demonstrated robust cycling stability at 1 mA cm-2.

Conclusions:

  • The proposed phase regulation strategy effectively creates a dense composite electrolyte with superior ionic conductivity and interfacial properties.
  • The developed electrolyte enables high-performance solid-state lithium metal batteries, showing practical capabilities in full cells under demanding conditions.
  • This work presents a promising pathway for advancing the practical application of solid-state lithium metal batteries.