Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 9, Issue 25, Pages 3298-3303Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/b703179c
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We present a detailed study on the exact location and dynamics of Li ions in the garnet-type material Li5La3Nb2O12 employing advanced solid state NMR strategies. Applying temperature-dependent Li-7-NMR, Li-6-MAS-NMR, Li-6-{Li-7}-CPMAS-NMR, Li-6-{Li-7}-CPMAS-REDOR-NMR as well as 2D-Li-6-{Li-7}-CPMAS-Exchange-NMR spectroscopy, we were able to quantify the distribution of the Li cations among the various possible sites within the garnet-type structure and to identify intrinsic details of Li migration. The results indicate a sensitive dependence of the distribution of Li cations among the tetrahedral and octahedral sites on the temperature of the final annealing process. This distribution profoundly affects the mobility of the Li cations within the garnet-type framework structure. Extended Li mobility at ambient temperature is only possible if the majority of the Li cations is accommodated in the octahedral sites, as observed for the sample annealed at 900 degrees C. Octahedrally-coordinated Li cations could be identified as the mobile Li species, whereas the tetrahedral sites seem to act as a trap for the Li cations, rendering the tetrahedrally-coordinated Li cations immobile on the time scale of the NMR experiments.
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