Solid State Ionics, volume 337, pages 154-160
Germanium as a donor dopant in garnet electrolytes
Publication type: Journal Article
Publication date: 2019-09-01
General Chemistry
Condensed Matter Physics
General Materials Science
Abstract
Cubic Li7La3Zr2O12 (LLZO) garnet electrolytes continue to be viewed as an enabler of all-solid-state lithium battery technologies, or as protective membranes for next-generation lithium battery systems. Supervalent dopants at the lithium sublattice are commonly used to stabilise the conductive cubic phase, through the creation of lithium vacancies. The use of germanium (Ge4+) as a higher valent dopant substituting for Li+ was studied here and shown to stabilise the cubic LLZO phase through substitution of x = 0.10 mol of Ge (at the tetrahedral 24d Li sites of the space group Ia-3d, based on the neutron powder diffraction result). This substitution preference follows that of Al3+ (having a similar ionic radius and reported to reside at 24d sites), but with a lower critical concentration for cubic phase stabilisation, in agreement with charge neutrality arguments to obtain the required Li content (ca. 6.4–6.6 per formula unit) for optimum conductivity. The x = 0.10 composition gave the highest bulk Li ion conductivity of 2.8 × 10−4 S cm−1 at 25 °C, on the order of reported values for Al-doped LLZO. Surface chemical analysis using time of flight secondary ion mass spectrometry showed Ge homogeneously distributed within the grains as well as some Li-, O- and Ge- enrichment along the grain boundaries. Cyclic voltammetry of the cells containing Ge-doped LLZO showed a redox stability up to +5 V.
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Brugge R. H. et al. Germanium as a donor dopant in garnet electrolytes // Solid State Ionics. 2019. Vol. 337. pp. 154-160.
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Brugge R. H., Kilner J. A., Kilner J., AGUADERO A., Aguadero A. Germanium as a donor dopant in garnet electrolytes // Solid State Ionics. 2019. Vol. 337. pp. 154-160.
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TY - JOUR
DO - 10.1016/j.ssi.2019.04.021
UR - https://doi.org/10.1016/j.ssi.2019.04.021
TI - Germanium as a donor dopant in garnet electrolytes
T2 - Solid State Ionics
AU - Brugge, Rowena Helen
AU - Kilner, J. A.
AU - AGUADERO, A.
AU - Kilner, John
AU - Aguadero, Ainara
PY - 2019
DA - 2019/09/01 00:00:00
PB - Elsevier
SP - 154-160
VL - 337
SN - 0167-2738
ER -
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@article{2019_Brugge,
author = {Rowena Helen Brugge and J. A. Kilner and A. AGUADERO and John Kilner and Ainara Aguadero},
title = {Germanium as a donor dopant in garnet electrolytes},
journal = {Solid State Ionics},
year = {2019},
volume = {337},
publisher = {Elsevier},
month = {sep},
url = {https://doi.org/10.1016/j.ssi.2019.04.021},
pages = {154--160},
doi = {10.1016/j.ssi.2019.04.021}
}