Characterization of Li + Transport through the Organic-Inorganic Interface by using Electrochemical Impedance Spectroscopy

  • Naboulsi A
  • Nguyen G
  • Franger S
  • et al.
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Abstract

Understanding Li + transport at polymer||inorganic interfaces is crucial for developing composite electrolytes in solid-state batteries. In our investigation, we employed impedance spectroscopy and established a multilayer methodology for assessing Li + transport at this interface. The inorganic phase chosen was Li 6.25 Al 0.25 La 3 Zr 2 O 12 ( Al− LLZO), and the organic phase comprised a Poly(ethylene oxide) (PEO) network with dangling chains. Li + incorporation in the polymer, as a free either salt or associated with anion grafting onto the PEO network, was explored. Additionally, the PEO network was either pressure-adhered to the inorganic surface (ex-situ configuration) or synthesized onto the Al −LLZO surfaces (in situ configuration) to investigate processing effects on Li + transport. Using a Transmission Line Model for impedance data analysis, our study identified two key elements governing Li + transport at the interface: R i , representing resistance along the ionic pathway, and R t and C t , describing distributed resistance and capacitance within the interface. We observed that R i is influenced by the polymerization process in the presence of Al −LLZO ceramic, while R t remains constant regardless of the synthesis method. This suggests varying Li + concentrations at the interphase in the in situ configuration, while interface/interphase heterogeneity remains consistent across configurations. The estimated activation energy indicates more energetically favorable direct Li + transport in the in−situ configuration.

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Naboulsi, A., Nguyen, G. T. M., Franger, S., Fichet, O., & Laberty-Robert, C. (2024). Characterization of Li + Transport through the Organic-Inorganic Interface by using Electrochemical Impedance Spectroscopy. Journal of The Electrochemical Society, 171(2), 020523. https://doi.org/10.1149/1945-7111/ad2595

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