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Solid Catholyte with Regulated Interphase Redox for All-Solid-State Lithium-Sulfur Batteries.

Kaier Shen1, Weize Shi1, Huimin Song1

  • 1Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials, School of Materials Science and Engineering, Peking University, Beijing, 100871, China.

Advanced Materials (Deerfield Beach, Fla.)
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Summary
This summary is machine-generated.

This study stabilizes all-solid-state lithium-sulfur batteries (ASSLSBs) by enhancing sulfide catholyte interphase stability. A novel Li6+xP1-xWxS5I electrolyte with WS2 improves cycling life and capacity retention for next-generation energy storage.

Keywords:
interphase redoxlithium‐sulfur batteriessolid catholytesulfur redox

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • All-solid-state lithium-sulfur batteries (ASSLSBs) are promising next-generation energy storage devices due to their potential for low cost, high safety, and high specific energy.
  • Sulfide electrolytes offer high conductivity and low modulus for solid catholytes in ASSLSBs, but suffer from parasitic decomposition and interphase degradation, limiting cycle life.

Purpose of the Study:

  • To stabilize ASSLSBs by regulating the interphase redox reversibility of sulfide catholytes.
  • To introduce and validate a new sulfide electrolyte, Li6+xP1-xWxS5I (LPWSI), for improved interphase stability and cycling performance.

Main Methods:

  • Formulation and characterization of a novel sulfide electrolyte, Li6+xP1-xWxS5I (LPWSI).
  • Investigation of the interphase reaction mechanisms, focusing on the role of WS2 in regulating redox reversibility.
  • Fabrication and electrochemical testing of ambient-temperature ASSLSBs using the LPWSI catholyte.

Main Results:

  • The presence of mixed ionic-electronic conducting WS2 in the LPWSI electrolyte promotes a beneficial Li4P2S7-to-Li3PS4 reaction, preventing the accumulation of impeding P2S7 4- species.
  • The LPWSI catholyte demonstrates enhanced interphase stability, leading to significantly improved cycling performance in ASSLSBs.
  • ASSLSBs with LPWSI achieved stable cycling, retaining 92.2% of their initial capacity over 400 cycles at C/5, with an initial areal capacity of 1.95 mA h cm-2.
  • The cells exhibited excellent high-rate stability, maintaining performance over 1000 cycles at 1C and 2C rates.

Conclusions:

  • The strategy of regulating interphase redox reversibility by incorporating mixed ionic-electronic conducting materials like WS2 is effective in stabilizing sulfide catholytes.
  • The developed LPWSI electrolyte offers a viable solution for enhancing the cycling life and performance of ambient-temperature ASSLSBs.
  • This work provides new insights into the functioning of solid catholytes in composite cathodes and offers guidelines for designing advanced electrolytes for high-capacity conversion-based electrodes.