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Synthesis and Lithium-ion Conductivity of Sr(La1−xLi3x)ScO4 with a K2NiF4 Structure (Supporting Information)

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posted on 26.11.2021, 02:27 by Guowei ZHAO, Kota SUZUKI, Masaaki HIRAYAMA, Ryoji KANNO

K2NiF4-type oxides are expected to be potential lithium-ion conductors because they have a structure similar to that of perovskites, which provide a reasonably flexible framework for accommodating defects such as charge carriers within the lattice. However, the K2NiF4-type structure as a framework for lithium conductors is scarcely reported. This article presents the preparation of Sr(La1−xLi3x)ScO4 with a K2NiF4 structure by a solid-state reaction at a high pressure of 2 GPa, and elucidates its lithium-ion-conducting properties. Sr(La1−xLi3x)ScO4 forms solid solutions in the x range of 0.05–0.20. Its orthorhombic lattice expands with lithium doping, indicating the incorporation of lithium ions as interstitial species in the structure. The highly doped samples exhibit high ionic conductivities (e.g., 4.66 × 10−6 S cm−1 at 250 °C for x = 0.15 and 4.29 × 10−2 S cm−1 at 375 °C for x = 0.2) with an activation energy of ∼100 kJ mol−1. The samples show an abnormal increase in the ionic conductivity at ∼300 °C, possibly due to the increase in the orthorhombicity of Sr(La1−xLi3x)ScO4. As the electronic conductivities of the developed oxide materials are a few orders of magnitude lower than their total conductivities, they can be used as solid electrolytes in all-solid-state lithium batteries. The study reveals that K2NiF4-type oxides are attractive candidates for developing novel lithium-ion conductors.

Funding

Creation of superionic conductors

Japan Society for the Promotion of Science

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Advanced Low Carbon Technology Research and Development Program

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Manuscript title

Synthesis and Lithium-ion Conductivity of Sr(La1−xLi3x)ScO4 with a K2NiF4 Structure