Lithium solid-state electrolytes are expected to improve next-generation energy storage technology on the basis of specific energy, safety, and cost. However, there has been limited success in the mass production of solid-state separators with transport properties and comparable thickness to a traditional polypropylene separator used in state-of-the-art lithium-ion batteries. This problem is especially difficult with both sulfide- and oxide-based solid electrolytes, such as lithium argyrodites and lithium garnets, together with integrating effective thin interlayers that enable lithium metal anodes. Several vacuum-based and sol-gel-derived methods have shown promise in making thin solid-state electrolyte films with relatively high ionic conductivity (~10<sup>-6</sup> - 10<sup>-5</sup> S/cm at room temperature), yet lithium loss during post annealing can alter the phase as well as significantly affect the lithium transport properties as well as the impedance at the Li||solid-state electrolyte interface. Therefore, the exploration of scalable fabrication techniques is of special importance to develop thin and robust films of sulfide- and oxide-based solid-state electrolytes with high ionic conductivity. In this talk, techniques based on scalable solution-based chemistries will be presented for sulfide- and oxide-based solid-state electrolytes. The crystallization and the phase transformations of the solid-state electrolytes will be discussed based on the concentration of cations and the boiling point of the solvents used in the solution-based chemistries. The results presented in this talk highlight a new opportunity for manufacturing oxide- and sulfide-based solid electrolytes with tunable electrochemical properties, thicknesses, and surface areas. The insights from this work are expected to serve as fundamental guidelines for future optimization toward solution-based processing of superionic solid-state electrolyte materials for next-generation lithium metal batteries.

Processing thin and robust sulfide and oxide solid-state electrolytes for lithium metal batteries

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ACS Fall 2022

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