Optimizing Li+ transport in Li7La3Zr2O12 solid electrolytes

Kade Parascos, Joshua L. Watts, Jose A. Alarco, Yan Chen, Peter C. Talbot

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5 Scopus citations

Abstract

The Li + conductivity of Li7La3Zr2O12 (LLZO) solid electrolytes was optimized by controlling the addition of the dopant (Al) into the crystal structure. A solution-based synthesis method was used to minimize Al segregation and ensure a homogeneous substitution into the garnet framework. Neutron and x-ray diffraction were used to monitor the structural transition from tetragonal to cubic LLZO. It was found that the critical dopant concentration (xc) required to stabilize the cubic phase was 0.18 mol pfu. The maximum ionic conductivity of 5.54 × 10−4 S/cm was obtained at the critical composition. The enhanced conductivity was achieved by accurately controlling the vacancy density at the active Li octahedral sites. Neutron structure refinements were used to validate the changes in Li vacancy distribution at different dopant concentrations. Impedance measurements reveal a strong dependence of Li+ transport properties on Al concentration, specifically around the critical dopant concentration xc = 0.18 mol pfu. These findings demonstrate the importance of fine-tuning composition and provide guidance for engineering improvements in ionic conductivity.

Original languageEnglish
Pages (from-to)23082-23090
Number of pages9
JournalCeramics International
Volume49
Issue number14
DOIs
StatePublished - Jul 15 2023

Funding

This research was financially supported by the Future Battery Industries Cooperative Research Centre (FBICRC) . Additional funding for this work was also provided by the Australasian Institute of Mining and Metallurgy (AusIMM) . The authors thank the assistance of staff from the Banyo Pilot Plant Precinct (PPP) and Central Analytical Research Facility (CARF) at Queensland University of Technology (QUT). The authors also appreciate the technical assistance from Tony Wang (CARF, QUT) for his valuable support in diffraction data analysis and refinement. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors thank Dr. Dunji Yu and Mrs. Bekki Mills for technical assistance with neutron diffraction experiments. This research was financially supported by the Future Battery Industries Cooperative Research Centre (FBICRC). Additional funding for this work was also provided by the Australasian Institute of Mining and Metallurgy (AusIMM). The authors thank the assistance of staff from the Banyo Pilot Plant Precinct (PPP) and Central Analytical Research Facility (CARF) at Queensland University of Technology (QUT). The authors also appreciate the technical assistance from Tony Wang (CARF, QUT) for his valuable support in diffraction data analysis and refinement. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors thank Dr. Dunji Yu and Mrs. Bekki Mills for technical assistance with neutron diffraction experiments.

Keywords

  • Batteries (E)
  • Impedance (C)
  • Ionic conductivity (C)
  • Sol-gel processes (A)

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