Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 7, Issue 6, Pages 2717-2722Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ta10790d
Keywords
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Funding
- National Basic Research Program of China (973 Program) [2015CB258400]
- Program for HUST Interdisciplinary Innovation Team [2015ZDTD021]
- Certificate of China Postdoctoral Science Foundation [2017M622422]
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All-solid-state batteries receive tremendous attention owing to their potential in improving battery safety and electrochemical properties. Developing a suitable solid electrolyte (SE) is a significant factor for allsolid- state batteries. Herein, we report calculation prediction and experimental evaluation of a series of Li-argyrodites, Li(7+x)M(x)P(1-x)S6 (M = Si, Ge). The density functional theory method predicts the structural stability of argyrodite-type Li7+xMxP1-xS6 (M = Si, Ge), meanwhile, the argyrodite-type Li7+xMxP1-xS6 (M = Si, Ge) are successfully synthesized by a solid state reaction method. Using structure refinements of Xray diffraction data and Raman spectroscopy, we discover that Si and Ge substitute the P in the 4b site. Si and Ge aliovalent doping in the original composition, Li7PS6, can make the desired cubic hightemperature (HT) phase of Li-argyrodites stabilized at room temperature and improve the ionic conductivities over 10(-3) S cm(-1) which is 3 orders of magnitude higher than that of original Li7PS6. Moreover, the argyrodite-type Li7+xMxP1-xS6 (M = Si, Ge) show a wide electrochemical window and stability with lithium metal. Stabilized Li-argyrodites could be suitable solid electrolytes for application in all-solid-state batteries. This work also demonstrates that stabilizing the high-temperature phase with high ionic conductivity would be a promising approach to explore new ionic conductors.
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