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From Dead Lithium to Functional Fillers: An in Situ Conversion Strategy for High-Performance All-Solid-State Lithium

Guoping Liu1, Xinyu Zhang1, Maochun Wu1

  • 1Department of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon, Hong Kong SAR 999077, China.

ACS Applied Materials & Interfaces
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PubMed
Summary

This study presents a novel ultrathin solid electrolyte for lithium metal batteries. It transforms "dead lithium" into functional fillers, enhancing battery performance and lifespan for safer, high-energy-density applications.

Keywords:
PEO solid electrolyteall-solid-state lithium metal batteriesdead lithium fillerultrathin thickness

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Poly(ethylene oxide) (PEO) solid electrolytes are promising for safe, high-energy-density all-solid-state lithium metal batteries.
  • Challenges include fabricating ultrathin electrolytes for practical current densities and long lifespans.

Purpose of the Study:

  • To develop an ultrathin (19 μm) PEO-based solid electrolyte with enhanced mechanical strength and dendrite suppression.
  • To utilize "dead lithium" as functional fillers within the electrolyte to improve performance.

Main Methods:

  • Fabrication of a 19 μm-thick PEO-based solid electrolyte supported by porous polyethylene.
  • Repeated lithium plating/stripping at high current density to form "dead lithium" fillers.
  • Characterization of in situ formed surface layers (LiOH, Li2CO3, Li2O, LiF) on dead lithium.

Main Results:

  • In situ formed fillers on "dead lithium" block electronic transport, acting as effective functional components.
  • These fillers enhance lithium-ion transport and suppress dendrite growth, promoting uniform lithium deposition.
  • Li||Li symmetric cells achieved a critical current density of 1 mA cm-2 and stable operation for 400 h.
  • A Li||LiFePO4 full cell retained 90.9% capacity after 600 cycles.

Conclusions:

  • The developed ultrathin PEO solid electrolyte with functionalized "dead lithium" fillers significantly improves lithium metal battery performance and safety.
  • This strategy offers a viable pathway for next-generation high-energy-density and long-lifespan all-solid-state batteries.