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Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes

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Abstract

The transport properties of lithium-ion conducting Li3xLa2/3-xTiO3 are studied for bulk and grain-boundary effects. This paper introduces a procedure for investigating bulk and grain-boundary polarization contributions using electrochemical impedance spectroscopy (EIS) and subsequent analysis via the distribution function of relaxation times (DRT) [1]. The frequency range of impedance spectroscopy is extended up to 120 MHz to resolve all conductivity contributions occurring in a polycrystalline solid electrolyte. Intra grain (bulk) and inter grain (grain boundary) conductivity contributions are separated using (i) a systematic variation of solid electrolyte contacting, (ii) two different solid electrolyte microstructures and activation energies were determined using adequate equivalent circuit models. Finally, these results are supported by SEM analysis, revealing different grain size distributions and different contents of inhomogeneities in Li3xLa2/3-xTiO3 solid electrolytes sintered at 1400°C and at 1450°C.

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Acknowledegments

The authors gratefully acknowledge Daniel Gil-Gaviria for continuous help with the automation of the high frequency impedance measurement setup. Sincere thanks are given to Jacob Packham for proofreading the manuscript and Michael Schönleber for the valuable discussions. The authors greatly acknowledge the funding of the BMBF project 03X4634D “Meet Hi-EnD” and the follow-up BMBF project 03XP0026G “FELIZIA”.

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Authors and Affiliations

  1. Institute for Applied Materials (IAM-WET), Karlsruhe Institute of Technology (KIT), D-76131, Karlsruhe, Germany

    Philipp Braun, Christian Uhlmann, André Weber & Ellen Ivers-Tiffée

  2. Laboratory for Electron Microscopy (LEM), Karlsruhe Institute of Technology (KIT), D-76131, Karlsruhe, Germany

    Heike Störmer & Dagmar Gerthsen

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  1. Philipp Braun
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  2. Christian Uhlmann
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Correspondence to Philipp Braun.

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Braun, P., Uhlmann, C., Weber, A. et al. Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes. J Electroceram 38, 157–167 (2017). https://doi.org/10.1007/s10832-016-0061-y

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  • DOI: https://doi.org/10.1007/s10832-016-0061-y

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