Local Structural Investigations, Defect Formation, and Ionic Conductivity of the Lithium Ionic Conductor Li4P2S6
Local Structural Investigations, Defect Formation, and Ionic Conductivity of the Lithium Ionic Conductor Li4P2S6
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DOI：
10.1021/acs.chemmater.6b04175
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发表时间：
2016-12-13
影响因子：
8.6
通讯作者：
Zeier, Wolfgang G.
中科院分区：
文献类型：
--
作者：
Dietrich, Christian;Sadowski, Marcel;Zeier, Wolfgang G.
玻璃状、玻璃陶瓷和结晶硫代磷酸锂作为全固态电池中的固体电解质引起了人们的兴趣。尽管具有相似的结构基序，包括 PS43-、P2S64- 和 P2S74- 多面体，但这些材料表现出多种可能的组成、晶体结构和离子电导率。在这里，我们提出了布拉格衍射、对分布函数分析、拉曼光谱和 P-31 魔角旋转核磁共振光谱的组合方法来研究 Li4P2S6 的基础晶体结构。在这项工作中，我们表明该材料作为玻璃陶瓷复合材料以平面结构排列结晶，解释了观察到的相对较低的离子电导率，具体取决于玻璃含量的分数。基于密度泛函理论的计算可以帮助我们了解这种 Li+ 离子导体的扩散路径和离子电导率。
Glassy, glass ceramic, and crystalline lithium thiophosphates have attracted interest in their use as solid electrolytes in all-solid-state batteries. Despite similar structural motifs, including PS43-, P2S64-, and P2S74- polyhedra, these materials exhibit a wide range of possible compositions, crystal structures, and ionic conductivities. Here, we present a combined approach of Bragg diffraction, pair distribution function analysis, Raman spectroscopy, and P-31 magic angle spinning nuclear magnetic resonance spectroscopy to study the underlying crystal structure of Li4P2S6. In this work, we show that the material crystallizes in a planar structural arrangement as a glass ceramic composite, explaining the observed relatively low ionic conductivity, depending on the fraction of glass content. Calculations based on density functional theory provide an understanding of occurring diffusion pathways and ionic conductivity of this Li+ ionic conductor.