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Characterization of Electrode Materials for Lithium Ion and Sodium Ion Batteries Using Synchrotron Radiation Techniques
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A Pre-Oxidation Strategy to Establish Stable Oxide Cathode/Halide Solid-State Electrolyte Interfaces for High Energy

Hanzhou Liu1, Yang Lu1, Yanchen Liu1

  • 1School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|February 28, 2025
PubMed
Summary

A new pre-oxidation strategy stabilizes halide solid-state electrolytes by forming robust Y-O bonds, preventing degradation in all-solid-state lithium metal batteries (ASSLBs) with high-energy cathodes.

Keywords:
all‐solid‐state batteriescathode‐electrolyte interfacecentral metal cationhalide‐based solid‐state electrolytespre‐oxidation

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • All-solid-state lithium metal batteries (ASSLBs) offer high energy density and safety.
  • Halide solid-state electrolytes possess high ionic conductivity and a wide electrochemical window.
  • Unstable cathode-electrolyte interfaces (CEI) due to oxygen-cation interactions limit performance.

Purpose of the Study:

  • To develop a pre-oxidation strategy for Y-based halide solid-state electrolytes.
  • To enhance the stability of the CEI in ASSLBs with oxide cathodes.
  • To improve the electrochemical performance and cycle life of ASSLBs.

Main Methods:

  • Synthesized a pre-oxidized halide solid-state electrolyte, Li₂YCl₂.₅Br₁.₅O₀.₅ (2LO-0.5).
  • Investigated the formation of robust Y-O bonds within the electrolyte structure.
  • Assembled ASSLBs using 2LO-0.5 and a LiNi₀.₈₃Co₀.₁₁Mn₀.₀₆O₂ (NCM83) cathode.
  • Evaluated the electrochemical performance and cycling stability.

Main Results:

  • The pre-oxidation strategy successfully formed robust Y-O bonds in 2LO-0.5.
  • This prevented the formation of unstable YOCl and promoted a stable Y₂O₃-based CEI.
  • ASSLBs with 2LO-0.5 and NCM83 achieved an initial discharge capacity of 208 mAh g⁻¹.
  • The batteries retained 80.6% of their capacity after 1000 cycles.

Conclusions:

  • The pre-oxidation strategy effectively regulates interfacial reactions between halide solid-state electrolytes and oxide cathodes.
  • The robust Y-O bonds are key to forming a stable CEI and preventing degradation.
  • This approach enables the rational design of high-performance ASSLBs.