Abstract
Garnet-based solid-state electrolytes (SSEs) represent a promising class of materials for next-generation batteries with improved safety and performance. However, lack of control over the composition and crystal structure of the well-known Li7La3Zr2O12 (LLZO) garnet material has led to poor reproducibility with a wide range of ionic conductivities reported in the literature. In this study, the role of precursor homogeneity in controlling the compositional and structural evolution of Al-doped LLZO is explored. A novel solution-based synthesis approach is employed to demonstrate enhanced atomic-scale mixing of the starting materials in comparison to conventional solid-state preparation methods. Through this technique, it is shown that the stability and formation temperature of the highly conductive cubic phase is directly impacted by the spatial distribution of the doping element and reactant species in the precursor mixture. Precursor homogeneity was also an important factor in mitigating the formation of unwanted secondary impurities. These findings can be used to guide the synthesis of SSEs with reproducible material characteristics and enhanced electrolytic performance.
| Original language | English |
|---|---|
| Pages (from-to) | 23466-23480 |
| Number of pages | 15 |
| Journal | RSC Advances |
| Volume | 12 |
| Issue number | 36 |
| DOIs | |
| State | Published - Aug 17 2022 |
Funding
This work was financially supported by the Future Battery Industries Cooperative Research Centre (FBICRC). The corresponding author also thanks the Australian Institute of Mining and Metallurgy (AusIMM) for providing additional funding in support of this work. The authors thank the support of staff and provisions from the Banyo Pilot Plant Precinct (PPP) and Central Analytical Research Facility (CARF) at Queensland University of Technology (QUT) for assisting with the synthesis and characterisation of materials. The authors gratefully appreciate the scientific and technical assistance from Jamie Riches and Tony Wang (CARF, QUT) for their support in laboratory microscopy and powder diffraction. 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 at SNS for the technical support.