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Stable Thiophosphate-Based All-Solid-State Lithium Batteries through Conformally Interfacial Nanocoating.

Daxian Cao1, Yubin Zhang2, Adelaide M Nolan3

  • 1Department of Mechanical and Industrial Engineering, Northeastern University, Boston, Massachusetts 02115, United States.

Nano Letters
|September 24, 2019
PubMed
Summary
This summary is machine-generated.

All-solid-state lithium batteries (ASLBs) achieve improved stability and high energy density by coating Li6PS5Cl electrolytes with amorphous Li0.35La0.5Sr0.05TiO3 (LLSTO). This enhances compatibility with high-voltage cathodes, enabling long-lasting performance.

Keywords:
Thiophosphateall solid-state batterieshigh-voltage cathodeinterface engineeringnanocoatingstability

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • All-solid-state lithium batteries (ASLBs) offer enhanced safety for next-generation energy storage.
  • Thiophosphate-based electrolytes, like Li6PS5Cl, exhibit high ionic conductivity but suffer from limited voltage windows and poor cathode compatibility.
  • Developing high-energy ASLBs requires overcoming interfacial instability with high-voltage cathode materials.

Purpose of the Study:

  • To investigate the failure mechanisms of Li6PS5Cl at high voltages.
  • To enhance the electrochemical stability of Li6PS5Cl with high-voltage LiNi1/3Mn1/3Co1/3O2 (NMC) cathodes.
  • To optimize interfacial coatings for improved ASLB performance.

Main Methods:

  • In situ Raman spectroscopy to study Li6PS5Cl degradation.
  • Wet chemical coating of amorphous Li0.35La0.5Sr0.05TiO3 (LLSTO) on NMC cathodes.
  • First-principles thermodynamic calculations to assess electrochemical stability.

Main Results:

  • A 15-20 nm LLSTO coating significantly improves interfacial stability between NMC and Li6PS5Cl.
  • Optimized LLSTO coating and NMC dimensions lead to ASLBs with 107 mAh g-1 capacity at room temperature.
  • The developed ASLBs demonstrate remarkable cycling stability, retaining 91.5% capacity over 850 cycles at C/3 within a 2.5-4.0 V window.

Conclusions:

  • The LLSTO interfacial layer effectively suppresses degradation of Li6PS5Cl at high voltages.
  • The combination of LLSTO and Li6PS5Cl provides excellent electrochemical stability and ionic conductivity.
  • This work presents a viable strategy for developing high-energy, safe, and long-lasting all-solid-state lithium batteries.