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Li-In-S composite foil with built-in electric fields to stabilize Li/Li<sub>6</sub>PS<sub>5</sub>Cl interface for long-life all-solid-state batteries.

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Electronic Localization Enables Long-Cycling Sulfides-Based All-Solid-State Lithium Batteries.

Dewen Wang1, Chong Liu1, Ruoyu Wang1

  • 1Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.

Angewandte Chemie (International Ed. in English)
|February 25, 2025
PubMed
Summary

Researchers developed a new strategy for stable solid-state lithium batteries by modifying sulfide electrolytes. This electron localization approach enhances air-stability and prevents dendrite growth, enabling long-lasting battery performance.

Keywords:
All‐solid‐state lithium batteryElectronic localizationInterfacial stabilityOrbital hybridizationSulfide solid electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • Argyrodite-based sulfide electrolytes offer high ionic conductivity for solid-state lithium metal batteries.
  • Interfacial reactions and dendrite growth between sulfide electrolytes and lithium anodes limit practical applications.

Purpose of the Study:

  • To enhance the stability of Li6PS5Cl sulfide electrolytes by modulating orbital hybridization.
  • To suppress interfacial reactions and dendrite formation in all-solid-state lithium metal batteries.

Main Methods:

  • Incorporation of yttrium (Y) and oxygen (O) into the Li6PS5Cl structure to modulate d-p orbital hybridization.
  • Investigating the effects of Y and O on electronic structure and interfacial properties.
  • Fabricating and testing symmetric Li cells and all-solid-state batteries.

Main Results:

  • Yttrium incorporation strengthens Madelung energy and induces electron localization on sulfur atoms, reducing lithium-sulfur interaction.
  • Oxygen introduction enhances air-stability and promotes in situ formation of a Li2O protective interphase.
  • The modified electrolyte enabled stable Li plating/stripping for over 4800 hours in Li symmetric cells.
  • All-solid-state batteries demonstrated 100% capacity retention after 1300 cycles at 0.5 C.

Conclusions:

  • Electron localization via orbital hybridization is an effective strategy for stabilizing sulfide-based solid-state lithium batteries.
  • The Y- and O-modified Li6PS5Cl electrolyte offers a promising pathway for ultrastable interfaces in next-generation batteries.