Parascos Kade, Watts Joshua L, Alarco Jose A, Chen Yan, Talbot Peter C
National Battery Testing Centre, Queensland University of Technology Brisbane QLD 4001 Australia
Centre for Clean Energy Technologies and Practices, Centre for Materials Science, Queensland University of Technology Brisbane 4001 Australia.
RSC Adv. 2022 Aug 17;12(36):23466-23480. doi: 10.1039/d2ra03303h. eCollection 2022 Aug 16.
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 LiLaZrO (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.
石榴石基固态电解质（SSEs）是一类很有前景的材料，可用于下一代安全性和性能更高的电池。然而，对著名的LiLaZrO（LLZO）石榴石材料的成分和晶体结构缺乏控制，导致其重现性较差，文献中报道的离子电导率范围很广。在本研究中，探索了前驱体均匀性在控制铝掺杂LLZO的成分和结构演变中的作用。与传统的固态制备方法相比，采用了一种新颖的基于溶液的合成方法来证明起始材料在原子尺度上的混合得到了增强。通过该技术表明，高导电立方相的稳定性和形成温度直接受到前驱体混合物中掺杂元素和反应物物种空间分布的影响。前驱体均匀性也是减轻不需要的二次杂质形成的一个重要因素。这些发现可用于指导具有可重现材料特性和增强电解性能的固态电解质的合成。
