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Improving Li-ion interfacial transport in hybrid solid electrolytes.

Ming Liu1, Shengnan Zhang1, Ernst R H van Eck2

  • 1Section Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of Technology, Delft, The Netherlands.

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|July 21, 2022
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Summary

Researchers enhanced hybrid solid electrolytes for better solid-state batteries. Introducing specific ionic liquids improved conductivity and stability, paving the way for efficient room-temperature battery operation.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Commercial solid-state batteries face challenges due to limitations in inorganic and organic solid electrolytes.
  • Hybrid solid electrolytes offer a promising alternative but suffer from insufficient room-temperature conductivity.
  • Understanding Li-ion transport across hybrid interfaces is crucial for performance enhancement.

Purpose of the Study:

  • To investigate the interphase structure and Li-ion transport in hybrid solid electrolytes.
  • To correlate interface chemistry with ionic conductivity in polymer-inorganic electrolytes.
  • To develop strategies for enhancing the performance of hybrid solid electrolytes for battery applications.

Main Methods:

  • Utilized solid-state nuclear magnetic resonance spectroscopy to study interphase structure.
  • Introduced two ionic liquids with varying miscibility in a polyethylene oxide polymer-inorganic electrolyte.
  • Analyzed Li-ion transport mechanisms across the polymer-inorganic interface.

Main Results:

  • A poorly miscible ionic liquid effectively wetted the polymer-inorganic interface, increasing local polarizability.
  • This modification lowered the diffusional barrier, achieving a room-temperature conductivity of 2.47 × 10⁻⁴ S cm⁻¹.
  • Demonstrated improved stability with a critical current density of 0.25 mA cm⁻² against a Li-metal anode.

Conclusions:

  • Tailoring the local interface environment in hybrid solid electrolytes is a viable strategy.
  • Optimized interface chemistry can significantly enhance Li-ion transport and overall conductivity.
  • Achieved stable room-temperature cycling of a LiFePO₄-Li-metal solid-state cell with 99.9% Coulombic efficiency.