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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Understanding buried solid-solid interfaces is critical for advancing solid-state electrochemical devices.
  • Interfacial void evolution presents a major challenge in solid-state battery performance and longevity.

Purpose of the Study:

  • To uncover the principles governing interfacial void evolution in solid-state batteries.
  • To develop a model for void nucleation and growth, drawing parallels with bubble formation in liquid phases.
  • To investigate void formation mechanisms in solid-state lithium metal batteries during lithium stripping.

Main Methods:

  • Development of a solid-state void nucleation and growth model.
  • Utilizing rational electrochemistry calculations to quantify void-induced contact loss.
  • Employing in situ visualization techniques to observe morphological evolutions and void defect features.

Main Results:

  • Quantified void-induced contact loss processes in a phase diagram across current densities (1.0–10.0 mA/cm²).
  • Revealed microscopic features of void defects under various lithium stripping conditions.
  • Established an electrochemical-morphological relationship elucidating void nucleation and growth mechanisms.

Conclusions:

  • Void formation during lithium stripping is a primary driver of morphological instabilities and failure in solid-state lithium metal batteries.
  • Void nucleation and growth are dependent on current density and areal capacity.
  • The findings provide critical insights for designing robust solid-solid interfaces in advanced solid-state batteries.