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On the interfacial charge transfer between solid and liquid Li+ electrolytes.

Marco Schleutker1, Jochen Bahner, Chih-Long Tsai

  • 1Institute of Energy and Climate Research, Electrochemical Process Engineering (IEK-3), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany. c.korte@fz-juelich.de.

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Summary
This summary is machine-generated.

This study investigates lithium-ion (Li+) transfer at solid-liquid interfaces using DC polarization. A constant resistance from a degraded surface layer and a concentration-dependent ion transfer process were identified, crucial for solid-state battery development.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Solid-State Ionics

Background:

  • Investigating Li+ ion transfer is critical for developing advanced energy storage devices, particularly solid-state batteries.
  • Understanding interfacial phenomena between solid electrolytes and liquid electrolytes is key to improving battery performance and stability.

Purpose of the Study:

  • To characterize the Li+ ion transfer kinetics at the interface between a Ta-substituted lithium lanthanum zirconate solid electrolyte and a liquid electrolyte.
  • To determine the contributions of interfacial resistance and charge transfer processes to the overall Li+ transport.

Main Methods:

  • Utilized DC polarization techniques to measure current density as a function of electrochemical potential drop.
  • Employed a liquid electrolyte of LiPF6 in ethylene carbonate/dimethyl carbonate (1:1) with varying Li+ concentrations.
  • Analyzed the current-potential data to model the interfacial behavior.

Main Results:

  • Identified a serial connection of a constant areal resistance (R_slei ≈ 300 Ω cm² at room temp) and a current-dependent, thermally activated ion transfer process.
  • The R_slei is attributed to a low-conductivity surface layer formed by degradation reactions, which increases with water content.
  • The ion transfer process follows Butler-Volmer kinetics, with an exchange current density (i0) dependent on Li+ concentration (i0 ≈ 53.1 μA cm⁻² at 1 mol L⁻¹) and a charge transfer coefficient (α ≈ 0.44).

Conclusions:

  • The solid-liquid electrolyte interphase (SLI) introduces a significant ohmic resistance, independent of bulk liquid electrolyte concentration.
  • The interfacial charge transfer is a thermally activated process, sensitive to Li+ concentration and exhibiting Butler-Volmer characteristics.
  • These findings, consistent with AC impedance spectroscopy studies, provide a comprehensive understanding of interfacial impedance in solid-liquid electrolyte systems for battery applications.