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Issue 6, 2019
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Design and synthesis of room temperature stable Li-argyrodite superionic conductors via cation doping

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Abstract

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 all-solid-state batteries. Herein, we report calculation prediction and experimental evaluation of a series of Li-argyrodites, Li7+xMxP1−xS6 (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 X-ray 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 high-temperature (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.

Graphical abstract: Design and synthesis of room temperature stable Li-argyrodite superionic conductors via cation doping

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Supplementary files

Article information


Submitted
08 Nov 2018
Accepted
03 Jan 2019
First published
04 Jan 2019

J. Mater. Chem. A, 2019,7, 2717-2722
Article type
Paper

Design and synthesis of room temperature stable Li-argyrodite superionic conductors via cation doping

Z. Zhang, Y. Sun, X. Duan, L. Peng, H. Jia, Y. Zhang, B. Shan and J. Xie, J. Mater. Chem. A, 2019, 7, 2717
DOI: 10.1039/C8TA10790D

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