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New solid electrolytes with iodine enhance all-solid-state lithium-sulfur batteries (ASSLSBs). These materials boost sulfur conversion kinetics and ionic conductivity, enabling high-rate capability and record areal capacities for advanced energy storage.

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catholyteredox mediationredox‐active electrolytesolid‐state lithium‐sulfur battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • All-solid-state lithium-sulfur batteries (ASSLSBs) offer high theoretical capacity but face challenges like slow kinetics and poor ionic conductivity.
  • Volume changes during cycling and limited ionic percolation in composite cathodes hinder ASSLSB practical application.

Purpose of the Study:

  • To develop novel solid electrolytes for ASSLSBs with improved ionic conductivity and electrochemical activity.
  • To investigate the effect of iodine incorporation on the properties and performance of Li-Si-P-S solid electrolytes.

Main Methods:

  • Synthesis of Li10.5-xSi1.5P1.5S12-xIx solid electrolytes with varying iodine content (x = 0, 0.2, 0.4).
  • Characterization of ionic conductivity, phase composition, and electrochemical behavior of the synthesized electrolytes.
  • Fabrication and testing of ASSLSBs utilizing the novel electrolytes as catholytes.

Main Results:

  • Solid electrolytes with high ionic conductivities (≥ 7 mS cm-1) were achieved.
  • Increased iodine content led to altered phase composition and reversible redox activity, enhancing sulfur conversion kinetics.
  • ASSLSBs demonstrated high sulfur utilization (86% at C/2), excellent rate capability (1175 mAh gsulfur-1 at 5C), and record areal capacities (14 mAh cm-2).

Conclusions:

  • The developed redox-active catholytes significantly improve ASSLSB performance by enhancing ionic percolation and sulfur conversion kinetics.
  • Iodine plays a crucial role in mediating redox activity and enabling high-performance ASSLSBs.
  • These findings offer new strategies for designing advanced solid electrolytes for next-generation energy storage devices.