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A novel coating effectively protects sulfide solid electrolytes from oxidation, significantly improving the performance and stability of high-voltage solid-state batteries with nickel-rich cathodes.

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DFTargyrodite electrolytecathode coating by designcathode-electrolyte interfacesolid-state battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • Sulfide solid electrolytes offer high ionic conductivity for solid-state batteries.
  • Their low oxidation potential (~2.5 V) limits compatibility with high-voltage nickel-rich cathodes (e.g., LiNiₓCoᵧMn₁₋ₓ₋ᵧO₂, x≥0.8).
  • Oxidative decomposition of electrolytes leads to poor battery performance and cycle life.

Purpose of the Study:

  • To develop an effective, conformal, and thin coating for nickel-rich cathodes.
  • To suppress the oxidative decomposition of sulfide solid electrolytes.
  • To enhance the electrochemical performance and stability of solid-state batteries.

Main Methods:

  • Density Functional Theory (DFT) calculations guided material design.
  • Fabrication of a nanometric coating on nickel-rich NMC85 cathode active material.
  • Electrochemical testing of solid-state batteries using Li₆PS₅Cl solid electrolyte and coated/uncoated cathodes.

Main Results:

  • The nanometric coating on NMC85 improved capacity retention to 82% after 200 cycles (2.8–4.3 V vs Li⁺/Li), compared to 56% for uncoated cathodes.
  • Coated cells exhibited superior rate performance and higher capacity.
  • A stable amorphous cathode-electrolyte interphase formed from LiPO₂F₂ decomposition products, protecting the sulfide electrolyte from oxidation.

Conclusions:

  • A cost-effective, conformal coating effectively enables the use of sulfide electrolytes with high-voltage nickel-rich cathodes.
  • The coating strategy, guided by DFT and based on decomposition products, significantly enhances battery performance and stability.
  • This approach offers a promising pathway for developing advanced sulfide electrolyte-based all-solid-state batteries.