Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.088
Publication date: 11th July 2022
All-solid-state batteries are seen as next generation energy storage systems and heavily researched worldwide. Within the three major clases of solid electrolytes, oxide-ceramic Li-ion conductors attract significant attention due to their intrinsic safety. In case of the garnet type Li7La3Zr2O12 (LLZO), the possibility to directly use Li-metal anodes paves the way for high energy densities on cell and battery level. However, the widespread application of such an oxide-based all-solid-state cells depends on the development of scalable synthesis and manufacturing processes while increasing the cell capacity to competitive levels.
While oxides are the most stable solid electrolytes when compared to poylmers or sulfides, there is still some sensitivity to air and protic solvents due to the Li+/H+-exchange. However, with careful tailoring of the manufacturing process due to mechanistic understanding allowed for the development of a new, tailored tape-casting process for LLZO components. 70 µm thick, free-standing LLZO separators can now be fabricated via water based tape casting and all-ceramic free-standing LiCoO2/LLZO mixed cathodes show high active materials utilization. Microstructural engineering by introduction concentration gradients for the active material and the electrolyte allowed to boost discharge capacities to 2.8 mAh cm-2 utilizing 99% of the theoretical capacity. Additionally, the obtained free-standing cathodes have sufficient mechanical stability to allow the application of hybrid and ultra-thin separators to further increase the energy density on the full cell level to industrially relevant levels.
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