Published November 6, 2020 | Version v1
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Li₄₋ₓGe₁₋ₓPₓO₄, a potential solid-state electrolyte for all-oxide microbatteries

  • 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

* Contact person

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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References

Journal reference (Original scientific publication (paper))
E. Gilardi, G. Materzanini, L. Kahle, M. Döbeli, S. Lacey, X. Cheng, N. Marzari, D. Pergolesi, A. Hintennach, T. Lippert, ACS Applied Energy Materials, 3, 10, 9910–9917 (2020), doi: 10.1021/acsaem.0c01601

Preprint
E. Gilardi, G. Materzanini, L. Kahle, M. Döbeli, S. Lacey, X. Cheng, N. Marzari, D. Pergolesi, A. Hintennach, T. Lippert, arXiv:2010.02608