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Interplay of Dynamic Constriction and Interface Morphology between Reversible Metal Anode and Solid Electrolyte in

Janis K Eckhardt1,2, Peter J Klar2,3, Jürgen Janek2,4

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Summary

A 3D electric network model reveals how electrode/sample interface morphology impacts all-solid-state battery impedance. Geometric constriction, not just charge transfer, significantly influences interface impedance, especially with lithium metal anodes.

Keywords:
constriction effectelectric network modelgarnet-type solid electrolyteimpedance modelinginterface morphologypore formationreversible metal anodesolid-state battery

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Electrical contact and interface stability are crucial for all-solid-state battery performance.
  • Impedance spectroscopy is a key technique for non-destructively analyzing interfaces.
  • Correlating microscopic processes with macroscopic impedance signals remains a challenge.

Purpose of the Study:

  • To systematically investigate the effect of electrode/sample interface morphology on impedance spectra.
  • To understand the contributions of charge transfer and geometric constriction to interface impedance.
  • To analyze the origin and characteristics of constriction phenomena in battery interfaces.

Main Methods:

  • Utilized a 3D electric network model to simulate interface behavior.
  • Systematically varied electrode/sample interface morphologies in the model.
  • Analyzed the resulting impedance spectra to identify key contributing factors.

Main Results:

  • Interface impedance arises from both charge transfer and geometric constriction.
  • Geometric constriction, caused by non-ideal contacts like pores, affects the electrochemical active surface area dynamically.
  • Constriction effects are dominant in systems with low charge transfer resistance, such as garnet electrolytes with lithium metal anodes.

Conclusions:

  • Interface morphology significantly dictates the impedance response of all-solid-state batteries.
  • Understanding geometric constriction is vital for accurate impedance interpretation and battery design.
  • This model provides insights into microscopic processes relevant for reversible metal anodes.