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Related Experiment Video

Updated: Aug 1, 2025

Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Tailoring Electrolyte Distributions to Enable High-performance Li3 PS4 -based All-solid-state Batteries under

Chaochao Wei1,2, Dian Yu2, Xiangling Xu2

  • 1School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.

Chemistry, an Asian Journal
|April 27, 2023
PubMed
Summary

Researchers developed a new strategy using Li3InCl6 to improve the interface stability of solid electrolytes in all-solid-state lithium batteries. This enhances battery performance and energy density, especially at low temperatures.

Keywords:
ASSLBsLi3InCl6Li3PS4 electrolytebare NCM622 cathodeinterfacial instability

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • Lithium phosphorus sulfide (Li3PS4) shows promise as a solid electrolyte for all-solid-state lithium batteries (ASSLBs) due to high ionic conductivity and mechanical strength.
  • Poor interfacial stability between Li3PS4 and high-nickel cathode materials like LiNi0.6Mn0.2Co0.2O2 (NCM622) limits ASSLB energy density and performance.
  • Direct contact between sulfide electrolytes and active materials leads to detrimental side reactions.

Purpose of the Study:

  • To address the interfacial instability issue in ASSLBs utilizing Li3PS4 and NCM622 cathode materials.
  • To enhance the electrochemical performance and energy density of ASSLBs by improving solid-solid interface stability.
  • To investigate the effectiveness of a graded electrolyte strategy using Li3InCl6.

Main Methods:

  • Incorporation of Li3InCl6 as a Li-ion additive and isolation layer in the cathode mixture.
  • Utilizing X-ray Photoelectron Spectroscopy (XPS) and Transmission Electron Microscopy (TEM) to analyze interfacial reactions.
  • Employing in-situ Electrochemical Impedance Spectroscopy (EIS) and Distribution of Relaxation Times (DRT) to evaluate interfacial resistance.

Main Results:

  • Li3InCl6 effectively mitigates side reactions between NCM622 and Li3PS4, confirmed by XPS and TEM.
  • Graded electrolyte utilization significantly reduces interfacial resistance, as evidenced by in-situ EIS and DRT.
  • The modified battery demonstrates superior performance, including a higher initial discharge capacity (187.7 mAh g−1 vs. 92.5 mAh g−1) and coulombic efficiency (87.6% vs. 71.1%) at 0.1 C.
  • Excellent cyclability and reversible capacity are maintained even at low operating temperatures (0 °C and -20 °C).

Conclusions:

  • A hierarchical utilization strategy employing Li3InCl6 as a protective layer is effective for sulfide electrolyte-based ASSLBs.
  • This approach significantly enhances interfacial stability, leading to improved electrochemical performance and energy density.
  • The developed ASSLBs exhibit promising potential for high-performance energy storage, particularly under demanding conditions like low temperatures.