Structural and Computational Assessment of the Influence of Wet-Chemical Post-Processing of the Al-Substituted Cubic Li7La3Zr2O12 Article Swipe
Róbert Kun
,
Frederieke Langer
,
Massimo Delle Piane
,
Saneyuki Ohno
,
Wolfgang G. Zeier
,
Michael Gockeln
,
Lucio Colombi Ciacchi
,
Matthias Busse
,
István Fekete
·
YOU?
·
· 2018
· Open Access
·
· DOI: https://doi.org/10.1021/acsami.8b09789
YOU?
·
· 2018
· Open Access
·
· DOI: https://doi.org/10.1021/acsami.8b09789
Li7La3Zr2O12 (LLZO) and related compounds are considered as promising candidates for future all-solid-state Li-ion battery applications. Still, the processing of those materials into thin membranes with the right stoichiometry and crystal structure is difficult and laborious. The sensitivity of the Li-ion conductive garnets against moisture and the associated Li+/H+ cation exchange makes their processing even more difficult. Formulation of suitable polymer/ceramic hybrid solid state electrolytes could be a prosperous way to reach the future large scale production of solid state Li-ion batteries. In fact, solvent mediated and/or slurry based wet-processing of the LLZO, e.g., tape-casting, could result in irreversible Li-ion loss of the pristine material due to Li+/H+ cation exchange. The concomitant structural changes and loss in functionality in terms of Li-ion conductivity are the results of the above process. Therefore, in the present work a systematic study on the chemical stability and structural retention of Al-substituted LLZO in different solvents is reported. It was found that Li+/H+ exchange in LLZO occurs upon solvent immersion, and its magnitude is dependent on the availability of -OH functional groups of the solvent molecules. As a result, a larger degree of Li+/H+ exchange causes higher increase of the lattice parameter of the LLZO, determined by synchrotron diffraction analyses. The expansion of the cubic unit cell was ascertained, when Li+ was replaced by H+ in the host lattice, by ab initio computational studies. The application of the most common solvent as dispersion medium, i.e., high purity water, causes the most significant Li+/H+ exchange and, therefore, structural change, while acetonitrile was proven to be the best suitable solvent for wet postprocessing of LLZO. Finally, computational calculations suggested that the Li+/H+ exchange could result in diminished ionic, i.e., mixed Li+-H+, conductivity due to the insertion of protons with lower mobility than that of Li-ions.
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- Type
- article
- Language
- en
- Landing Page
- https://doi.org/10.1021/acsami.8b09789
- OA Status
- green
- Cited By
- 40
- References
- 52
- Related Works
- 10
- OpenAlex ID
- https://openalex.org/W2895259980
All OpenAlex metadata
Raw OpenAlex JSON
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https://openalex.org/W2895259980Canonical identifier for this work in OpenAlex
- DOI
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https://doi.org/10.1021/acsami.8b09789Digital Object Identifier
- Title
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Structural and Computational Assessment of the Influence of Wet-Chemical Post-Processing of the Al-Substituted Cubic Li7La3Zr2O12Work title
- Type
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articleOpenAlex work type
- Language
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enPrimary language
- Publication year
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2018Year of publication
- Publication date
-
2018-10-08Full publication date if available
- Authors
-
Róbert Kun, Frederieke Langer, Massimo Delle Piane, Saneyuki Ohno, Wolfgang G. Zeier, Michael Gockeln, Lucio Colombi Ciacchi, Matthias Busse, István FeketeList of authors in order
- Landing page
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https://doi.org/10.1021/acsami.8b09789Publisher landing page
- Open access
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YesWhether a free full text is available
- OA status
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greenOpen access status per OpenAlex
- OA URL
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https://www.osti.gov/biblio/1483095Direct OA link when available
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Materials science, Crystallography, Physical chemistry, Mineralogy, Chemical engineering, Engineering, ChemistryTop concepts (fields/topics) attached by OpenAlex
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40Total citation count in OpenAlex
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2025: 5, 2024: 6, 2023: 6, 2022: 5, 2021: 8Per-year citation counts (last 5 years)
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10Other works algorithmically related by OpenAlex
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