The solid-state Li-ion conductor Li7TaO6: A combined computational and experimental study

Authors: Leonid Kahle1*, Xi Cheng2, Tobias Binninger3, Steven D. Lacey4, Aris Marcolongo3, Federico Zipoli3, Elisa Gilardi2, Claire Villevieille4, Mario El Kazzi4, Nicola Marzari1, Daniele Pergolesi2

  1. Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland
  2. Laboratory for Multiscale Materials Experiments, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland
  3. IBM Research–Zurich, CH-8803 Rüschlikon, Switzerland
  4. Electrochemistry Laboratory, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland
  • Corresponding author email: leonid.kahle@epfl.ch

DOI10.24435/materialscloud:2019.0068/v1 (version v1, submitted on 25 October 2019)

How to cite this entry

Leonid Kahle, Xi Cheng, Tobias Binninger, Steven D. Lacey, Aris Marcolongo, Federico Zipoli, Elisa Gilardi, Claire Villevieille, Mario El Kazzi, Nicola Marzari, Daniele Pergolesi, The solid-state Li-ion conductor Li7TaO6: A combined computational and experimental study, Materials Cloud Archive (2019), doi: 10.24435/materialscloud:2019.0068/v1.

Description

We study the oxo-hexametallate Li7TaO6 with first-principles and classical molecular dynamics simulations, obtaining a low activation barrier for diffusion of ∼0.29 eV and a high ionic conductivity of 5.7×10−4 S cm−1 at room temperature (300 K). We find evidence for a wide electrochemical stability window from both calculations and experiments, suggesting its viable use as a solid-state electrolyte in next-generation solid-state Li-ion batteries. To assess its applicability in an electrochemical energy storage system, we performed electrochemical impedance spectroscopy measurements on multicrystalline pellets, finding substantial ionic conductivity, if below the values predicted from simulation. We further elucidate the relationship between synthesis conditions and the observed ionic conductivity using X-ray diffraction, inductively coupled plasma optical emission spectrometry, and X-ray photoelectron spectroscopy, and study the effects of Zr and Mo doping.

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Files

File name Size Description
tantalate.aiida
MD5MD5: 68ee160ede7788c651879b46eee57adb
1.1 GiB This AiiDA export file contains the first-principles molecular dynamics trajectories, all produced and stored with AiiDA.
README.txt
MD5MD5: a58ddff142a8766fd397a33fe0022d40
1.3 KiB The README contains information on the main content. It describes the AiiDA export file that contains the first-principles molecular dynamics trajectories and the folder structure where the classical trajectories are saved.
trajectories.zip
MD5MD5: f403d4f195fb2fc132afdfe31a9082ae
6.9 GiB This zip file contains the classical trajectories of Li7TaO6. How the folders are structured is described in the README.

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.

Keywords

molecular dynamics MARVEL/Inc1 electrochemical stability polarizable force-fields density-functional theory solid-state electrolyte Li-ion batteries

Version history

25 October 2019 [This version]