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Zeitschrift für Physikalische Chemie

International journal of research in physical chemistry and chemical physics

Ed. by Rademann, Klaus

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Li Ion Dynamics in Al-Doped Garnet-Type Li7La3Zr2O12 Crystallizing with Cubic Symmetry

Alexander Kuhn* / Joon-Yong Choi1 / Lars Robben2 / Frank Tietz3 / Martin Wilkening4 / Paul Heitjans5

1 Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Jülich, Deutschland

2 Leibniz Universität Hannover, Institute of Mineralogy, Hannover, Deutschland

3 Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Jülich, Deutschland

4 Leibniz University Hannover, Institute of Phys. Chemistry and Electrochemistry, Hannover, Deutschland

5 Universität Hannover, Institut f. Physikalische Chemie und Elektrochemie, Hannover, Deutschland

* Correspondence address: Leibniz University Hannover, Institute of Phys. Chemistry and Electrochemistry, Callinstraße 3-3a, 30167 Hannover, Deutschland,

Citation Information: Zeitschrift für Physikalische Chemie. Volume 226, Issue 5-6, Pages 525–537, ISSN (Online) 2196-7156, ISSN (Print) 0942-9352, DOI: https://doi.org/10.1524/zpch.2012.0250, June 2012

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Lithium-ion dynamics in the garnet-type solid electrolyte “Li7La3Zr2O12” (LLZ) crystallizing with cubic symmetry was probed by means of variable-temperature 7Li NMR spectroscopy and ac impedance measurements. Li jump rates of an Al-containing sample follow Arrhenius behaviour being characterized by a relatively high activation energy of 0.54(3) eV and a pre-exponential factor of 2.2(5) × 1013 s-1. The results resemble those which were quite recently obtained for an Al-free LLZ sample crystallizing, however, with tetragonal symmetry. Hence, most likely, the significantly higher Li conductivity previously reported for a cubic LLZ sample cannot be ascribed solely to the slight structural distortions accompanying the change of the crystal symmetry. Here, even Al impurities, acting as stabilizer for the cubic polymorph at room temperature, do not lead to the high ion conductivity reported previously.

Keywords: Solid Electrolytes; Garnets; Lithium Ion Dynamics; NMR; Spin-Lattice Relaxation

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