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On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering

The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li(2)S) via soluble polysulfides (PSs) formation impedes the development of high-performance lithium-sulfur (Li-S) batteries with non-aqueous electrolyte solutions. Here, we use operando...

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Autores principales: Prehal, Christian, von Mentlen, Jean-Marc, Drvarič Talian, Sara, Vizintin, Alen, Dominko, Robert, Amenitsch, Heinz, Porcar, Lionel, Freunberger, Stefan A., Wood, Vanessa
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9592616/
https://www.ncbi.nlm.nih.gov/pubmed/36280671
http://dx.doi.org/10.1038/s41467-022-33931-4
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author Prehal, Christian
von Mentlen, Jean-Marc
Drvarič Talian, Sara
Vizintin, Alen
Dominko, Robert
Amenitsch, Heinz
Porcar, Lionel
Freunberger, Stefan A.
Wood, Vanessa
author_facet Prehal, Christian
von Mentlen, Jean-Marc
Drvarič Talian, Sara
Vizintin, Alen
Dominko, Robert
Amenitsch, Heinz
Porcar, Lionel
Freunberger, Stefan A.
Wood, Vanessa
author_sort Prehal, Christian
collection PubMed
description The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li(2)S) via soluble polysulfides (PSs) formation impedes the development of high-performance lithium-sulfur (Li-S) batteries with non-aqueous electrolyte solutions. Here, we use operando small and wide angle X-ray scattering and operando small angle neutron scattering (SANS) measurements to track the nucleation, growth and dissolution of solid deposits from atomic to sub-micron scales during real-time Li-S cell operation. In particular, stochastic modelling based on the SANS data allows quantifying the nanoscale phase evolution during battery cycling. We show that next to nano-crystalline Li(2)S the deposit comprises solid short-chain PSs particles. The analysis of the experimental data suggests that initially, Li(2)S(2) precipitates from the solution and then is partially converted via solid-state electroreduction to Li(2)S. We further demonstrate that mass transport, rather than electron transport through a thin passivating film, limits the discharge capacity and rate performance in Li-S cells.
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spelling pubmed-95926162022-10-26 On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering Prehal, Christian von Mentlen, Jean-Marc Drvarič Talian, Sara Vizintin, Alen Dominko, Robert Amenitsch, Heinz Porcar, Lionel Freunberger, Stefan A. Wood, Vanessa Nat Commun Article The inadequate understanding of the mechanisms that reversibly convert molecular sulfur (S) into lithium sulfide (Li(2)S) via soluble polysulfides (PSs) formation impedes the development of high-performance lithium-sulfur (Li-S) batteries with non-aqueous electrolyte solutions. Here, we use operando small and wide angle X-ray scattering and operando small angle neutron scattering (SANS) measurements to track the nucleation, growth and dissolution of solid deposits from atomic to sub-micron scales during real-time Li-S cell operation. In particular, stochastic modelling based on the SANS data allows quantifying the nanoscale phase evolution during battery cycling. We show that next to nano-crystalline Li(2)S the deposit comprises solid short-chain PSs particles. The analysis of the experimental data suggests that initially, Li(2)S(2) precipitates from the solution and then is partially converted via solid-state electroreduction to Li(2)S. We further demonstrate that mass transport, rather than electron transport through a thin passivating film, limits the discharge capacity and rate performance in Li-S cells. Nature Publishing Group UK 2022-10-24 /pmc/articles/PMC9592616/ /pubmed/36280671 http://dx.doi.org/10.1038/s41467-022-33931-4 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/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 license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license 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 license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Prehal, Christian
von Mentlen, Jean-Marc
Drvarič Talian, Sara
Vizintin, Alen
Dominko, Robert
Amenitsch, Heinz
Porcar, Lionel
Freunberger, Stefan A.
Wood, Vanessa
On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title_full On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title_fullStr On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title_full_unstemmed On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title_short On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
title_sort on the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9592616/
https://www.ncbi.nlm.nih.gov/pubmed/36280671
http://dx.doi.org/10.1038/s41467-022-33931-4
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