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Field assisted sintering of fine-grained Li7−3xLa3Zr2AlxO12 solid electrolyte and the influence of the microstructure on the electrochemical performance

Botros, Miriam and Djenadic, Ruzica and Clemens, Oliver and Möller, Matthias and Hahn, Horst (2016):
Field assisted sintering of fine-grained Li7−3xLa3Zr2AlxO12 solid electrolyte and the influence of the microstructure on the electrochemical performance.
In: Journal of Power Sources, 309, pp. 108-115. Elsevier Science Publishing, ISSN 03787753,
DOI: 10.1016/j.jpowsour.2016.01.086,
[Article]

Abstract

The synthesis and processing of fine-grained Li7−3xLa3Zr2AlxO12 (x = 0.15, 0.17, 0.20) solid electrolyte (LLZO) is performed for the first time using a combination of nebulized spray pyrolysis (NSP) and field assisted sintering technique (FAST). Using FAST, the grain growth is suppressed and highly dense ceramics with 93% of the theoretical density are obtained. A tetragonal lattice distortion is observed after the sintering process. Although this structural modification has been reported to have lower Li-ion mobility compared to the cubic modification, the total conductivity of the sample at room temperature is found to be 0.33 mS cm−1, i.e. comparable to phase-pure cubic LLZO. The activation energy of 0.38 eV is also comparable to the literature values. Galvanostatic cycling of a symmetrical cell Li|LLZO|Li shows a good cycling stability over 100 h. The interfacial resistance in contact with Li-metal is determined using alternating current impedance spectroscopy to be 76 Ω cm2 and 69 Ω cm2 before and after cycling at different current densities, respectively.

Item Type: Article
Erschienen: 2016
Creators: Botros, Miriam and Djenadic, Ruzica and Clemens, Oliver and Möller, Matthias and Hahn, Horst
Title: Field assisted sintering of fine-grained Li7−3xLa3Zr2AlxO12 solid electrolyte and the influence of the microstructure on the electrochemical performance
Language: English
Abstract:

The synthesis and processing of fine-grained Li7−3xLa3Zr2AlxO12 (x = 0.15, 0.17, 0.20) solid electrolyte (LLZO) is performed for the first time using a combination of nebulized spray pyrolysis (NSP) and field assisted sintering technique (FAST). Using FAST, the grain growth is suppressed and highly dense ceramics with 93% of the theoretical density are obtained. A tetragonal lattice distortion is observed after the sintering process. Although this structural modification has been reported to have lower Li-ion mobility compared to the cubic modification, the total conductivity of the sample at room temperature is found to be 0.33 mS cm−1, i.e. comparable to phase-pure cubic LLZO. The activation energy of 0.38 eV is also comparable to the literature values. Galvanostatic cycling of a symmetrical cell Li|LLZO|Li shows a good cycling stability over 100 h. The interfacial resistance in contact with Li-metal is determined using alternating current impedance spectroscopy to be 76 Ω cm2 and 69 Ω cm2 before and after cycling at different current densities, respectively.

Journal or Publication Title: Journal of Power Sources
Journal volume: 309
Publisher: Elsevier Science Publishing
Uncontrolled Keywords: All-solid-state Li-ion battery, Garnet, Solid electrolyte, Microstructure, Spark plasma sintering, Interfacial resistance
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Fachgebiet Materialdesign durch Synthese
11 Department of Materials and Earth Sciences > Material Science > Joint Research Laboratory Nanomaterials
Date Deposited: 12 Apr 2017 12:15
DOI: 10.1016/j.jpowsour.2016.01.086
Official URL: https://doi.org/10.1016/j.jpowsour.2016.01.086
Funders: The authors would like to thank Helmholtz Association (Germany) for financial support through the Helmholtz Portfolio Project “Electrochemical Storage in Systems - Reliability and Integration”.
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