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Sulfide-based solid electrolytes have attracted significant attention for their application in solid-state batteries due to their high ionic conductivity and good ductility. A number of sulfide electrolytes have been reported and carefully investigated. Structure and dynamics are important for researchers to understand the conduction mechanism. MAS NMR can provide structural information on sulfide electrolytes, such as site occupancy. The lithium/sodium ion diffusion processes in the sulfide electrolytes can be tracked, ranging from the short-range vibrations between different sites at extremely short time scales to ion transport over the grain boundaries or the electrode–electrolyte interfaces taking place at a time scale up to several seconds by different NMR techniques. Both the structure and dynamics features of various lithium/sodium sulfide electrolytes have been summarized and the future development of the application of NMR techniques in sulfide electrolyte-based solid-state batteries have been pointed out.

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