Publication date: 10th April 2024
To develop efficient all-solid-state batteries, solid-state electrolyte separator need to meet several criteria, such as high electronic resistance and low ionic one, (electro)chemical, mechanical and thermal stability, and scalable processing.[1] As a thin-film, only the compounds from the oxide family meet these requirements. The most popular one, used in solid-state μ-batteries, is the lithium phosphate oxynitride (LiPON), thanks to its stability against lithium metal and its low electronic conductivity.[2, 3] However, its low ionic conductivity in the range of 10-6 S/cm, and its low deposition rate during reactive RF magnetron sputtering restrict its scale-up for industrial applications.
In this work, we use a carbon-doped Li3PO4 sputtering target to enable faster deposition rates. The high electronic conductivity of the target allows us to use a power density up to ~15 W/cm2, thus increasing the deposition rate threefold in RF mode and tenfold in DC mode, as compared to the standard RF mode of LiPON, while maintaining comparable electrochemical properties. Secondly, we investigate a Si- variant of LiPON, known as LiSiPON[5], by co-sputtering Li3PO4 and Li4SiO4 in reactive nitrogen gas to further improve the ionic conductivity. Finally, hybrid cells are fabricated to demonstrate the potential application of these separators in bulk solid-state batteries, consisting of composite cathodes, sputtered thin-film separators, and evaporated lithium metal anode.
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