Elisa Gilardi^1,2*, Giuliana Materzanini^2,3*, Leonid Kahle^2,3, Max Doebeli⁴, Steven Lacey^2,5, Xi Cheng^1,2, Nicola Marzari^2,3, Daniele Pergolesi^1,5,2, Andreas Hintennach⁶, Thomas Lippert^1,7

1 Research with Neutrons and Muons (NUM), Paul Scherrer Institute, CH-5232 Villigen, Switzerland

2 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), 1015 Lausanne, Switzerland

3 Theory and Simulations of Materials (THEOS), École Polytechnique Fedérale de Lausanne, 1015 Lausanne, Switzerland

4 Ion Beam Physics, ETH Zürich, CH-8093 Zürich, Switzerland

5 Energy and Environment Research Division (ENE), Paul Scherrer Institute, CH-5232 Villigen, Switzerland

6 Daimler AG, 70546 Stuttgart, Germany

7 Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, 8093 Zürich, Switzerland

* Corresponding authors emails: elisa.gilardi@psi.ch, giuliana.materzanini@epfl.ch

DOI10.24435/materialscloud:3a-9v [version v1]

Publication date: Nov 06, 2020

How to cite this record

Elisa Gilardi, Giuliana Materzanini, Leonid Kahle, Max Doebeli, Steven Lacey, Xi Cheng, Nicola Marzari, Daniele Pergolesi, Andreas Hintennach, Thomas Lippert, Li₄₋ₓGe₁₋ₓPₓO₄, a potential solid-state electrolyte for all-oxide microbatteries, Materials Cloud Archive 2020.142 (2020), https://doi.org/10.24435/materialscloud:3a-9v

Description

Solid-state electrolytes for Li-ion batteries are attracting growing interest as they allow building safer batteries, also using lithium-metal anodes. Here, we studied a compound in the lithium superionic conductor (LISICON) family, i.e. Li₄₋ₓGe₁₋ₓPₓO₄ (LGPO). Thin films were deposited via pulsed laser deposition, and their electrical properties were compared to those of ceramic pellets. A detailed characterization of their microstructures shows that thin films can be deposited fully crystalline at higher temperatures but also partially amorphous at room temperature. The conductivity is not strongly influenced by the presence of grain boundaries, exposure to air, or lithium deficiencies. First-principles molecular dynamics simulations were employed to calculate the lithium-ion diffusion profile and the conductivity at various temperatures of the ideal LGPO crystal. Simulations give the upper limit of conductivity for a defect-free crystal, which is in the range of 10–2 S cm–1 at 300 °C. The ease of thin-film fabrication and room-temperature Li-ion conductivity in the range of a few μS cm–1 make LGPO a very appealing electrolyte material for thin-film all-solid-state all-oxide microbatteries.

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SIMULATIONS_DATA.tar.gz MD5md5:1664b9c6fb7a45a17c2f126482cef491	2.6 GiB	Data related to the first-principles molecular dynamics simulations
README.txt MD5md5:2fc26ffc8b90e5e5f922b68a4a744448	3.1 KiB	Brief description of "EXPERIMENTS_DATA.tar.gz" and "SIMULATIONS_DATA.tar.gz" archives content

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Keywords

solid-state electrolytes thin films microbatteries first-principles molecular dynamics LISICON LGPO ionic transport MARVEL/Inc1 Li4–xGe1–xPxO4 BIG-MAP