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Passivation-Induced Species Dynamics and Microstructural Evolution in Solid-State Lithium-Sulfur Cathodes.

Arpan K Sharma1, Bairav S Vishnugopi1, Elif Pınar Alsaç2

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Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
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Summary
This summary is machine-generated.

Solid-state lithium-sulfur batteries face challenges with sulfur utilization and rechargeability due to lithium sulfide (Li2S) passivation. This study reveals how Li2S formation limits performance by blocking transport and hindering reactions in the cathode microstructure.

Keywords:
electrode microstructurelithium–sulfur cathodereaction kineticssolid‐state batteriestransport limitations

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Solid-state lithium-sulfur (SSLS) batteries promise high energy density but suffer from poor sulfur utilization and limited rechargeability.
  • The passivation effect of lithium sulfide (Li2S) hinders ionic/electronic transport and electrochemical reaction reversibility.

Purpose of the Study:

  • To elucidate the mechanistic origins of performance limitations in SSLS batteries.
  • To resolve the spatial evolution of charge/discharge species within the cathode microstructure.
  • To provide design guidance for enhancing sulfur utilization in SSLS cathodes.

Main Methods:

  • In-situ analysis of species distribution at the particle scale.
  • Coupling Raman spectroscopy and X-ray diffraction.
  • Investigating varied current densities and electrode compositions.

Main Results:

  • Li2S formation causes localized surface passivation, progressively limiting electrochemical accessibility.
  • Sulfur utilization is governed by sulfur loading, porosity, and interfacial architecture.
  • High sulfur content leads to isolated domains; low content causes solid electrolyte (SE) degradation.

Conclusions:

  • Understanding species evolution and Li2S passivation is crucial for SSLS battery design.
  • Sulfur-porosity maps define reversible and transport-limited regimes.
  • Optimized interfacial architecture and controlled sulfur loading are key for improved SSLS cathode performance.