Improved Thermal Stability of Oxysulfide Glassy Solid-State Electrolytes

Gonzalez Malabet, Hernando J.; Zhang, Yubin; Salvador, James R.; Schmidt, Robert D.; Yersak, Thomas A. (ORCID:0000000182757960)

doi:10.1149/1945-7111/ad07ff

DOE OSTI · 2205243

Improved Thermal Stability of Oxysulfide Glassy Solid-State Electrolytes

Gonzalez Malabet, Hernando J.·Zhang, Yubin·Salvador, James R.·Schmidt, Robert D.·Yersak, Thomas A. (ORCID:0000000182757960)

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Abstract

In this study, the crystallization kinetics of (oxy)sulfide 70Li 2 S·(30-x)P 2 S 5 ·xP 2 O 5 (x = 0, 2, 5) solid-state electrolytes are reported. It was found that 5 mol% P 2 O 5 glass co-former slowed the crystallization rate of the Li 7 P 3 S 11−x/4 O x/4 ceramic phase by a factor of 10. After 10 min at 230 °C, a 70Li 2 S·30P 2 S 5 sulfide glass was 92% devitrified whereas a 70Li 2 S·25P 2 S 5 ·5P 2 O 5 oxysulfide glass was only 8% devitrified. The improved thermal stability of oxysulfide glasses was then utilized to demonstrate the fabrication of a standalone, reinforced SSE separator by hot pressing. More importantly, it was recognized that the microstructure of 70Li 2 S·25P 2 S 5 ·5P 2 O 5 oxysulfide SSE separators could be modified by hot pressing without changing ionic conductivity. This result was achieved because the precipitation of a superionically conductive Li 7 P 3 S 11−x/4 O x/4 ceramic phase was limited. A study was then conducted to determine what effect microstructure has on the susceptibility of SSE separators to shorting by lithium metal penetration. Hot-pressed separators were found to be more susceptible to shorting than cold-pressed separators. X-ray Computer Tomography (XCT) of post-mortem samples showed that hot-pressed samples failed by transverse microcrack pathways, which underscores the importance of low defect density in dense SSE separators.

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Gonzalez Malabet, Hernando J., Zhang, Yubin, Salvador, James R., Schmidt, Robert D., Yersak, Thomas A. (ORCID:0000000182757960). 2023-11-08. Improved Thermal Stability of Oxysulfide Glassy Solid-State Electrolytes. https://doi.org/10.1149/1945-7111%2Fad07ff

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