ACS applied materials & interfaces, volume 14, issue 12, pages 14739-14752

Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers

Publication typeJournal Article
Publication date2022-03-17
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor9.5
ISSN19448244, 19448252
General Materials Science
Abstract
Garnet-type Li7La3Zr2O12 (LLZO) is a potential electrolyte material for all-solid-state Li-ion batteries mainly because of its reported excellent chemical stability in contact with Li metal. But good wettability of LLZO and 100% surface coverage of lithium are still a challenge. This study elucidated the suitability of magnetron-sputtered indium in Li(In)/LLZO/Li(In) symmetrical model cells as one of the promising interfacial modifications reported in the literature. Importance was given to the impact of preparation parameters on the surface coverage of Li(In)/LLZO interfaces and the consequences of impedance, cycling stability, and critical current density. SEM and EDXS analyses of In layers of thickness 100 nm to 1 μm revealed complete dissolution of indium in the lithium anode after annealing; 300 nm In layers annealed at 220 °C/10 h provided a surface coverage of >80%, best reproducibility, and a supreme interface resistance Rint of 12.4 Ω·cm2. Presuming a surface coverage of 100%, an ultimate interface resistance close to 1 Ω·cm2 can be expected. The critical current density was determined as 200-500 μA/cm2 at a charge of 100-250 μAh, whereas 500 μA/cm2 and above affected cell stability. The increasing voltage plateau was assigned to the increase of the interface resistance Rint and the electrolyte resistance RG+GB. SEM, EDXS, and X-ray microtomography analyses after voltage breakdown confirmed Li-dendrite growth along grain boundaries into LLZO, often curved parallel to the interface, indicating short-circuiting of the solid electrolyte. Grain boundary characteristics are supposed to be decisive for lithium deposition in and failure of garnet-type solid electrolytes after cycling.

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Müller M. et al. Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers // ACS applied materials & interfaces. 2022. Vol. 14. No. 12. pp. 14739-14752.
GOST all authors (up to 50) Copy
Müller M., Schmieg J., Dierickx S., Joos J., Weber A., Gerthsen D., Ivers-Tiffée E. Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers // ACS applied materials & interfaces. 2022. Vol. 14. No. 12. pp. 14739-14752.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1021/acsami.1c25257
UR - https://doi.org/10.1021/acsami.1c25257
TI - Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers
T2 - ACS applied materials & interfaces
AU - Schmieg, Johannes
AU - Joos, Jochen
AU - Weber, Andre
AU - Gerthsen, Dagmar
AU - Ivers-Tiffée, Ellen
AU - Müller, Marius
AU - Dierickx, Sebastian
PY - 2022
DA - 2022/03/17 00:00:00
PB - American Chemical Society (ACS)
SP - 14739-14752
IS - 12
VL - 14
SN - 1944-8244
SN - 1944-8252
ER -
BibTex |
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BibTex Copy
@article{2022_Müller,
author = {Johannes Schmieg and Jochen Joos and Andre Weber and Dagmar Gerthsen and Ellen Ivers-Tiffée and Marius Müller and Sebastian Dierickx},
title = {Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers},
journal = {ACS applied materials & interfaces},
year = {2022},
volume = {14},
publisher = {American Chemical Society (ACS)},
month = {mar},
url = {https://doi.org/10.1021/acsami.1c25257},
number = {12},
pages = {14739--14752},
doi = {10.1021/acsami.1c25257}
}
MLA
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Müller, Marius, et al. “Reducing Impedance at a Li-Metal Anode/Garnet-Type Electrolyte Interface Implementing Chemically Resolvable In Layers.” ACS applied materials & interfaces, vol. 14, no. 12, Mar. 2022, pp. 14739-14752. https://doi.org/10.1021/acsami.1c25257.
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