Gallium-Doped Li7La3Zr2O12 Garnet-Type Electrolytes with High Lithium-Ion Conductivity
Owing to their high conductivity, crystalline Li 7–3 x Ga x La 3 Zr 2 O 12 garnets are promising electrolytes for all-solid-state lithium-ion batteries. Herein, the influence of Ga doping on the phase, lithium-ion distribution, and conductivity of Li 7–3 x Ga x La 3 Zr 2 O 12 garnets is investigated, with the determined concentration and mobility of lithium ions shedding light on the origin of the high conductivity of Li 7–3 x Ga x La 3 Zr 2 O 12 . When the Ga concentration exceeds 0.20 Ga per formula unit, the garnet-type material is found to assume a cubic structure, but lower Ga concentrations result in the coexistence of cubic and tetragonal phases. Most lithium within Li 7–3 x Ga x La 3 Zr 2 O 12 is found to reside at the octahedral 96 h site, away from the central octahedral 48 g site, while the remaining lithium resides at the tetrahedral 24 d site. Such kind of lithium distribution leads to high lithium-ion mobility, which is the origin of the high conductivity; the highest lithium-ion conductivity of 1.46 mS/cm at 25 °C is found to be achieved for Li 7–3 x Ga x La 3 Zr 2 O 12 at x = 0.25. Additionally, there are two lithium-ion migration pathways in the Li 7–3 x Ga x La 3 Zr 2 O 12 garnets: 96 h -96 h and 24 d -96 h -24 d , but the lithium ions transporting through the 96 h -96 h pathway determine the overall conductivity. Graphic Abstract
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