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Dynamics of self-reorganization explains passivation of silicate glasses

Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer––called...

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Autores principales: Gin, Stéphane, Collin, Marie, Jollivet, Patrick, Fournier, Maxime, Minet, Yves, Dupuy, Laurent, Mahadevan, Thiruvilla, Kerisit, Sebastien, Du, Jincheng
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5986767/
https://www.ncbi.nlm.nih.gov/pubmed/29867088
http://dx.doi.org/10.1038/s41467-018-04511-2
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author Gin, Stéphane
Collin, Marie
Jollivet, Patrick
Fournier, Maxime
Minet, Yves
Dupuy, Laurent
Mahadevan, Thiruvilla
Kerisit, Sebastien
Du, Jincheng
author_facet Gin, Stéphane
Collin, Marie
Jollivet, Patrick
Fournier, Maxime
Minet, Yves
Dupuy, Laurent
Mahadevan, Thiruvilla
Kerisit, Sebastien
Du, Jincheng
author_sort Gin, Stéphane
collection PubMed
description Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer––called gel––that can in some circumstances control the reactivity of the buried interface. Here, we report experimental and simulation results deciphering the mechanisms by which the gel becomes passivating. The study conducted on a six-oxide borosilicate glass shows that gel reorganization involving high exchange rate of oxygen and low exchange rate of silicon is the key mechanism accounting for extremely low apparent water diffusivity (∼10(−21) m(2) s(−1)), which could be rate-limiting for the overall reaction. These findings could be used to improve kinetic models, and inspire the development of new molecular sieve materials with tailored properties as well as highly durable glass for application in extreme environments.
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spelling pubmed-59867672018-06-06 Dynamics of self-reorganization explains passivation of silicate glasses Gin, Stéphane Collin, Marie Jollivet, Patrick Fournier, Maxime Minet, Yves Dupuy, Laurent Mahadevan, Thiruvilla Kerisit, Sebastien Du, Jincheng Nat Commun Article Understanding the dissolution of silicate glasses and minerals from atomic to macroscopic levels is a challenge with major implications in geoscience and industry. One of the main uncertainties limiting the development of predictive models lies in the formation of an amorphous surface layer––called gel––that can in some circumstances control the reactivity of the buried interface. Here, we report experimental and simulation results deciphering the mechanisms by which the gel becomes passivating. The study conducted on a six-oxide borosilicate glass shows that gel reorganization involving high exchange rate of oxygen and low exchange rate of silicon is the key mechanism accounting for extremely low apparent water diffusivity (∼10(−21) m(2) s(−1)), which could be rate-limiting for the overall reaction. These findings could be used to improve kinetic models, and inspire the development of new molecular sieve materials with tailored properties as well as highly durable glass for application in extreme environments. Nature Publishing Group UK 2018-06-04 /pmc/articles/PMC5986767/ /pubmed/29867088 http://dx.doi.org/10.1038/s41467-018-04511-2 Text en © The Author(s) 2018 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/.
spellingShingle Article
Gin, Stéphane
Collin, Marie
Jollivet, Patrick
Fournier, Maxime
Minet, Yves
Dupuy, Laurent
Mahadevan, Thiruvilla
Kerisit, Sebastien
Du, Jincheng
Dynamics of self-reorganization explains passivation of silicate glasses
title Dynamics of self-reorganization explains passivation of silicate glasses
title_full Dynamics of self-reorganization explains passivation of silicate glasses
title_fullStr Dynamics of self-reorganization explains passivation of silicate glasses
title_full_unstemmed Dynamics of self-reorganization explains passivation of silicate glasses
title_short Dynamics of self-reorganization explains passivation of silicate glasses
title_sort dynamics of self-reorganization explains passivation of silicate glasses
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5986767/
https://www.ncbi.nlm.nih.gov/pubmed/29867088
http://dx.doi.org/10.1038/s41467-018-04511-2
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