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Li oxide garnets are among the most promising candidates for solid-state electrolytes in novel Li ion and Li metal based battery concepts. Cubic Li 7 La 3 Zr 2 O 12 stabilized by a partial substitution of Zr 4+ by Bi 5+ has not been the focus of research yet, despite the fact that Bi 5+ would be a cost-effective alternative to other stabilizing cations such as Nb 5+ and Ta 5+ . In this study, Li 7-x La 3 Zr 2-x Bi x O 12 (x = 0.10, 0.20, ..., 1.00) was prepared by a low-temperature solid-state synthesis route. The samples have been characterized by a rich portfolio of techniques, including scanning electron microscopy, X-ray powder diffraction, neutron powder diffraction, Raman spectroscopy, and 7 Li NMR spectroscopy. Pure-phase cubic garnet samples were obtained for x ≥ 0.20. The introduction of Bi 5+ leads to an increase in the unit-cell parameters. Samples are sensitive to air, which causes the formation of LiOH and Li 2 CO 3 and the protonation of the garnet phase, leading to a further increase in the unit-cell parameters. The incorporation of Bi 5+ on the octahedral 16a site was confirmed by Raman spectroscopy. 7 Li NMR spectroscopy shows that fast Li ion dynamics are only observed for samples with high Bi 5+ contents.

Synthesis, Crystal Structure, and Stability of Cubic Li7–xLa3Zr2–xBixO12

Synthesis, Crystal Structure, and Stability of Cubic Li_7–xLa₃Zr_2–xBi_xO₁₂