Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes

Solid electrolyte is the key component in all-solid-state batteries (ASBs). It is required in electrodes to enhance Li-conductivity and can be directly used as a separator. With its high Li-conductivity and chemical stability towards metallic lithium, lithium-stuffed garnet material Li<sub>7&l...

Descripción completa

Guardado en:
Detalles Bibliográficos
Autores principales: Markus Mann, Michael Küpers, Grit Häuschen, Martin Finsterbusch, Dina Fattakhova-Rohlfing, Olivier Guillon
Formato: article
Lenguaje:EN
Publicado: MDPI AG 2021
Materias:
T
Acceso en línea:https://doaj.org/article/a747b39944454088a91116b1c1fd9a72
Etiquetas: Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
id oai:doaj.org-article:a747b39944454088a91116b1c1fd9a72
record_format dspace
spelling oai:doaj.org-article:a747b39944454088a91116b1c1fd9a722021-11-25T18:13:45ZEvaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes10.3390/ma142268091996-1944https://doaj.org/article/a747b39944454088a91116b1c1fd9a722021-11-01T00:00:00Zhttps://www.mdpi.com/1996-1944/14/22/6809https://doaj.org/toc/1996-1944Solid electrolyte is the key component in all-solid-state batteries (ASBs). It is required in electrodes to enhance Li-conductivity and can be directly used as a separator. With its high Li-conductivity and chemical stability towards metallic lithium, lithium-stuffed garnet material Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is considered one of the most promising solid electrolyte materials for high-energy ceramic ASBs. However, in order to obtain high conductivities, rare-earth elements such as tantalum or niobium are used to stabilize the highly conductive cubic phase. This stabilization can also be obtained via high levels of aluminum, reducing the cost of LLZO but also reducing processability and the Li-conductivity. To find the sweet spot for a potential market introduction of garnet-based solid-state batteries, scalable and industrially usable syntheses of LLZO with high processability and good conductivity are indispensable. In this study, four different synthesis methods (solid-state reaction (SSR), solution-assisted solid-state reaction (SASSR), co-precipitation (CP), and spray-drying (SD)) were used and compared for the synthesis of aluminum-substituted LLZO (Al:LLZO, Li<sub>6.4</sub>Al<sub>0.2</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>), focusing on electrochemical performance on the one hand and scalability and environmental footprint on the other hand. The synthesis was successful via all four methods, resulting in a Li-ion conductivity of 2.0–3.3 × 10<sup>−4</sup> S/cm. By using wet-chemical synthesis methods, the calcination time could be reduced from two calcination steps for 20 h at 850 °C and 1000 °C to only 1 h at 1000 °C for the spray-drying method. We were able to scale the synthesis up to a kg-scale and show the potential of the different synthesis methods for mass production.Markus MannMichael KüpersGrit HäuschenMartin FinsterbuschDina Fattakhova-RohlfingOlivier GuillonMDPI AGarticleall-solid-state batteryceramic solid electrolyteLLZOscale-upTechnologyTElectrical engineering. Electronics. Nuclear engineeringTK1-9971Engineering (General). Civil engineering (General)TA1-2040MicroscopyQH201-278.5Descriptive and experimental mechanicsQC120-168.85ENMaterials, Vol 14, Iss 6809, p 6809 (2021)
institution DOAJ
collection DOAJ
language EN
topic all-solid-state battery
ceramic solid electrolyte
LLZO
scale-up
Technology
T
Electrical engineering. Electronics. Nuclear engineering
TK1-9971
Engineering (General). Civil engineering (General)
TA1-2040
Microscopy
QH201-278.5
Descriptive and experimental mechanics
QC120-168.85
spellingShingle all-solid-state battery
ceramic solid electrolyte
LLZO
scale-up
Technology
T
Electrical engineering. Electronics. Nuclear engineering
TK1-9971
Engineering (General). Civil engineering (General)
TA1-2040
Microscopy
QH201-278.5
Descriptive and experimental mechanics
QC120-168.85
Markus Mann
Michael Küpers
Grit Häuschen
Martin Finsterbusch
Dina Fattakhova-Rohlfing
Olivier Guillon
Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
description Solid electrolyte is the key component in all-solid-state batteries (ASBs). It is required in electrodes to enhance Li-conductivity and can be directly used as a separator. With its high Li-conductivity and chemical stability towards metallic lithium, lithium-stuffed garnet material Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) is considered one of the most promising solid electrolyte materials for high-energy ceramic ASBs. However, in order to obtain high conductivities, rare-earth elements such as tantalum or niobium are used to stabilize the highly conductive cubic phase. This stabilization can also be obtained via high levels of aluminum, reducing the cost of LLZO but also reducing processability and the Li-conductivity. To find the sweet spot for a potential market introduction of garnet-based solid-state batteries, scalable and industrially usable syntheses of LLZO with high processability and good conductivity are indispensable. In this study, four different synthesis methods (solid-state reaction (SSR), solution-assisted solid-state reaction (SASSR), co-precipitation (CP), and spray-drying (SD)) were used and compared for the synthesis of aluminum-substituted LLZO (Al:LLZO, Li<sub>6.4</sub>Al<sub>0.2</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>), focusing on electrochemical performance on the one hand and scalability and environmental footprint on the other hand. The synthesis was successful via all four methods, resulting in a Li-ion conductivity of 2.0–3.3 × 10<sup>−4</sup> S/cm. By using wet-chemical synthesis methods, the calcination time could be reduced from two calcination steps for 20 h at 850 °C and 1000 °C to only 1 h at 1000 °C for the spray-drying method. We were able to scale the synthesis up to a kg-scale and show the potential of the different synthesis methods for mass production.
format article
author Markus Mann
Michael Küpers
Grit Häuschen
Martin Finsterbusch
Dina Fattakhova-Rohlfing
Olivier Guillon
author_facet Markus Mann
Michael Küpers
Grit Häuschen
Martin Finsterbusch
Dina Fattakhova-Rohlfing
Olivier Guillon
author_sort Markus Mann
title Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
title_short Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
title_full Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
title_fullStr Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
title_full_unstemmed Evaluation of Scalable Synthesis Methods for Aluminum-Substituted Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Solid Electrolytes
title_sort evaluation of scalable synthesis methods for aluminum-substituted li<sub>7</sub>la<sub>3</sub>zr<sub>2</sub>o<sub>12</sub> solid electrolytes
publisher MDPI AG
publishDate 2021
url https://doaj.org/article/a747b39944454088a91116b1c1fd9a72
work_keys_str_mv AT markusmann evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
AT michaelkupers evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
AT grithauschen evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
AT martinfinsterbusch evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
AT dinafattakhovarohlfing evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
AT olivierguillon evaluationofscalablesynthesismethodsforaluminumsubstitutedlisub7sublasub3subzrsub2subosub12subsolidelectrolytes
_version_ 1718411456905478144