Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes

Tetragonal garnet-type Li(7)La(3)Zr(2)O(12) is an important candidate solid electrolyte for all-solid-state lithium ion batteries because of its high ionic conductivity and large electrochemical potential window. Here we employ atomistic simulation methods to show that the most favourable disorder p...

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Autores principales: Kuganathan, Navaratnarajah, Rushton, Michael J. D., Grimes, Robin W., Kilner, John A., Gkanas, Evangelos I., Chroneos, Alexander
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Article
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7801511/
https://www.ncbi.nlm.nih.gov/pubmed/33432039
http://dx.doi.org/10.1038/s41598-020-79919-2
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author Kuganathan, Navaratnarajah
Rushton, Michael J. D.
Grimes, Robin W.
Kilner, John A.
Gkanas, Evangelos I.
Chroneos, Alexander
author_facet Kuganathan, Navaratnarajah
Rushton, Michael J. D.
Grimes, Robin W.
Kilner, John A.
Gkanas, Evangelos I.
Chroneos, Alexander
author_sort Kuganathan, Navaratnarajah
collection PubMed
description Tetragonal garnet-type Li(7)La(3)Zr(2)O(12) is an important candidate solid electrolyte for all-solid-state lithium ion batteries because of its high ionic conductivity and large electrochemical potential window. Here we employ atomistic simulation methods to show that the most favourable disorder process in Li(7)La(3)Zr(2)O(12) involves loss of Li(2)O resulting in lithium and oxygen vacancies, which promote vacancy mediated self-diffusion. The activation energy for lithium migration (0.45 eV) is much lower than that for oxygen (1.65 eV). Furthermore, the oxygen migration activation energy reveals that the oxygen diffusion in this material can be facilitated at higher temperatures once oxygen vacancies form.
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spelling pubmed-78015112021-01-12 Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes Kuganathan, Navaratnarajah Rushton, Michael J. D. Grimes, Robin W. Kilner, John A. Gkanas, Evangelos I. Chroneos, Alexander Sci Rep Article Tetragonal garnet-type Li(7)La(3)Zr(2)O(12) is an important candidate solid electrolyte for all-solid-state lithium ion batteries because of its high ionic conductivity and large electrochemical potential window. Here we employ atomistic simulation methods to show that the most favourable disorder process in Li(7)La(3)Zr(2)O(12) involves loss of Li(2)O resulting in lithium and oxygen vacancies, which promote vacancy mediated self-diffusion. The activation energy for lithium migration (0.45 eV) is much lower than that for oxygen (1.65 eV). Furthermore, the oxygen migration activation energy reveals that the oxygen diffusion in this material can be facilitated at higher temperatures once oxygen vacancies form. Nature Publishing Group UK 2021-01-11 /pmc/articles/PMC7801511/ /pubmed/33432039 http://dx.doi.org/10.1038/s41598-020-79919-2 Text en © The Author(s) 2021 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Kuganathan, Navaratnarajah
Rushton, Michael J. D.
Grimes, Robin W.
Kilner, John A.
Gkanas, Evangelos I.
Chroneos, Alexander
Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title_full Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title_fullStr Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title_full_unstemmed Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title_short Self-diffusion in garnet-type Li(7)La(3)Zr(2)O(12) solid electrolytes
title_sort self-diffusion in garnet-type li(7)la(3)zr(2)o(12) solid electrolytes
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7801511/
https://www.ncbi.nlm.nih.gov/pubmed/33432039
http://dx.doi.org/10.1038/s41598-020-79919-2
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