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Solid-State Lithium Batteries with Ultrastable Cyclability: An Internal-External Modification Strategy.

Linshan Luo1, Zhefei Sun2, Yiwei You1

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Summary
This summary is machine-generated.

Introducing a dual modification strategy, this study stabilizes lithium-ion battery interfaces by addressing defects in lithium aluminum titanium phosphate (LATP) and protecting the lithium metal anode. This enhances battery longevity and performance under demanding conditions.

Keywords:
LiCldefectinterphaselithium dendritesolid polymer electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Batteries

Background:

  • The interface between lithium aluminum titanium phosphate (LATP) solid electrolytes and lithium metal anodes presents stability challenges, limiting battery performance.
  • Existing interlayer strategies show limited effectiveness in long-term cycling and high current density due to unaddressed internal LATP defects like grain boundaries (GBs).
  • Grain boundaries in LATP exhibit higher electronic conductivity, promoting detrimental side reactions with lithium.

Purpose of the Study:

  • To investigate the role of LATP grain boundaries in interfacial instability with lithium metal.
  • To develop a dual modification strategy for stabilizing the LATP/lithium interface.
  • To enhance the cycling stability and safety of solid-state lithium metal batteries.

Main Methods:

  • Control experiments and theoretical calculations to analyze LATP grain boundary properties.
  • LiCl solution immersion method to modify grain boundary electronic states.
  • Composite solid polymer electrolyte (CSPE) interlayering at the Li/LATP interface.
  • Fabrication and electrochemical testing of modified lithium symmetrical cells.

Main Results:

  • LiCl treatment effectively modifies LATP grain boundaries, reducing their electronic conductivity and side reactions with lithium.
  • The combined LiCl treatment and CSPE interlayering provide internal and external protection to the LATP electrolyte.
  • Modified cells demonstrate ultrastable cycling performance, exceeding 3500 hours at 0.4 mA cm⁻² and 1500 hours at 0.6 mA cm⁻².
  • The dual modification strategy effectively inhibits electron leakage, prevents side reactions, and suppresses lithium dendrite penetration.

Conclusions:

  • Addressing internal defects, specifically grain boundaries, is crucial for stabilizing LATP electrolytes.
  • A dual modification approach combining LiCl treatment and CSPE interlayering offers a highly effective strategy for interfacial stabilization.
  • This method significantly improves the long-term cycling performance and reliability of solid-state lithium metal batteries.