Luo Changwei, Shuai Qilin, Zhao Guoqiang, Zhang Mengyang, Wu Bin, Fu Xiaolan, Sun Yujian, Wang Yian, Hua Qingsong
Key Laboratory of Beam Technology of Ministry of Education, College of Nuclear Science and Technology, Beijing Normal University, Beijing 100875, China.
Key Laboratory of Beam Technology of Ministry of Education, Center of Ion Beam Technology & Energy Materials, Beijing Normal University, Beijing 100875, China.
ACS Appl Mater Interfaces. 2023 Oct 18;15(41):48110-48121. doi: 10.1021/acsami.3c09236. Epub 2023 Oct 5.
The ionic conductivity, phase components, and microstructures of LATP depend on its synthesis process. However, their relative importance and their interactions with synthesis process parameters (such as source materials, calcination temperature, and sintering temperature) remain unclear. In this work, different source materials were used to prepare LATP via the solid-state reaction method under different calcination and sintering temperatures, and an analysis via orthogonal experiments and machine learning was used to systematically study the effects of the process parameters. Sintering temperatures had the greatest effect on the total ionic conductivity of LATP pellets, followed by the sources and calcination temperatures. Sources, as the foundational factors, directly determine the composition of a major secondary phase of LATP pellets, which influences the whole process. The calcination temperature had limited impact on the ion conductivity of LATP pellets if pellets were sintered under the optimal temperature. The sintering temperature is the most important factor that influences the ion conductivity by eliminating most secondary phases and altering the microstructure of LATP, including the intergranular contact, grain size, relative densities, etc. This work offers a novel perspective to comprehend the synthesis of solid-state electrolytes beyond LATP.
LATP的离子电导率、相组成和微观结构取决于其合成过程。然而,它们的相对重要性以及它们与合成过程参数(如原料、煅烧温度和烧结温度)之间的相互作用仍不明确。在这项工作中,采用不同的原料,通过固态反应法在不同的煅烧和烧结温度下制备LATP,并通过正交实验和机器学习分析系统地研究了工艺参数的影响。烧结温度对LATP颗粒的总离子电导率影响最大,其次是原料和煅烧温度。原料作为基础因素,直接决定了LATP颗粒主要次生相的组成,从而影响整个过程。如果颗粒在最佳温度下烧结,煅烧温度对LATP颗粒的离子电导率影响有限。烧结温度是影响离子电导率的最重要因素,它通过消除大多数次生相并改变LATP的微观结构,包括晶间接触、晶粒尺寸、相对密度等。这项工作为理解除LATP之外的固态电解质的合成提供了一个新的视角。