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Polyelectrolyte Complex Coating for Mitigating Decomposition at Argyrodite and Conductive Carbon Interfaces in

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A new polyelectrolyte coating on vapor-grown carbon fibers (VGCFs) protects sulfide solid electrolytes in solid-state batteries. This coating enhances cycling capacity by preventing electrolyte degradation at critical interfaces.

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interface degradationpolyelectrolyte complexpolymer coatingsolid electrolytesolid‐state batteries

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Area of Science:

  • Solid-state battery technology
  • Electrochemical energy storage
  • Materials science

Background:

  • Sulfide-based solid electrolyte batteries (SEBs) offer high energy density for large-scale commercialization.
  • Carbon additives like vapor-grown carbon fibers (VGCFs) are crucial for cathode utilization but can degrade sulfide electrolytes (e.g., Li6PS5Cl).
  • Electrolyte decomposition at interfaces with cathode active materials and VGCFs limits cell capacity.

Purpose of the Study:

  • To develop a protective coating for VGCFs to mitigate degradation in SEBs.
  • To investigate the impact of a polyelectrolyte coating on VGCF interfaces within LiIn|LPSCl|LPSCl-NCM-VGCF (LiInSEBNCM) cells.
  • To optimize coating thickness for improved cycling performance.

Main Methods:

  • Application of a novel polyelectrolyte coating onto VGCFs.
  • Evaluation of electrolyte oxidation at the VGCF interface using cyclic voltammetry.
  • Assessment of cell performance through galvanostatic charge-discharge cycling.

Main Results:

  • The polyelectrolyte coating effectively suppresses argyrodite oxidation at the VGCF|LPSCl interface.
  • Coated VGCFs lead to improved cycling capacity in the LiInSEBNCM cells.
  • An optimal polymer coating thickness was identified, balancing protection and VGCF aggregation for maximum performance.

Conclusions:

  • Polyelectrolyte coatings on VGCFs are a viable strategy to enhance the stability and performance of sulfide-based solid-state batteries.
  • Interface engineering is critical for overcoming degradation issues in high-energy-density solid-state batteries.
  • Optimizing coating parameters is essential for maximizing the benefits of protective interlayers in SEBs.