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Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations

The Calcium Silicate Hydrate (C-S-H) nucleation is a crucial step during cement hydration and determines to a great extent the rheology, microstructure, and properties of the cement paste. Recent evidence indicates that the C-S-H nucleation involves at least two steps, yet the underlying atomic scal...

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Autores principales: Aretxabaleta, Xabier M., López-Zorrilla, Jon, Etxebarria, Iñigo, Manzano, Hegoi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10693585/
https://www.ncbi.nlm.nih.gov/pubmed/38042823
http://dx.doi.org/10.1038/s41467-023-43500-y
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author Aretxabaleta, Xabier M.
López-Zorrilla, Jon
Etxebarria, Iñigo
Manzano, Hegoi
author_facet Aretxabaleta, Xabier M.
López-Zorrilla, Jon
Etxebarria, Iñigo
Manzano, Hegoi
author_sort Aretxabaleta, Xabier M.
collection PubMed
description The Calcium Silicate Hydrate (C-S-H) nucleation is a crucial step during cement hydration and determines to a great extent the rheology, microstructure, and properties of the cement paste. Recent evidence indicates that the C-S-H nucleation involves at least two steps, yet the underlying atomic scale mechanism, the nature of the primary particles and their stability, or how they merge/aggregate to form larger structures is unknown. In this work, we use atomistic simulation methods, specifically DFT, evolutionary algorithms (EA), and Molecular Dynamics (MD), to investigate the structure and formation of C-S-H primary particles (PPs) from the ions in solution, and then discuss a possible formation pathway for the C-S-H nucleation. Our simulations indicate that even for small sizes the most stable clusters encode C-S-H structural motifs, and we identified a C(4)S(4)H(2) cluster candidate to be the C-S-H basic building block. We suggest a formation path in which small clusters formed by silicate dimers merge into large elongated aggregates. Upon dehydration, the C-S-H basic building blocks can be formed within the aggregates, and eventually crystallize.
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spelling pubmed-106935852023-12-04 Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations Aretxabaleta, Xabier M. López-Zorrilla, Jon Etxebarria, Iñigo Manzano, Hegoi Nat Commun Article The Calcium Silicate Hydrate (C-S-H) nucleation is a crucial step during cement hydration and determines to a great extent the rheology, microstructure, and properties of the cement paste. Recent evidence indicates that the C-S-H nucleation involves at least two steps, yet the underlying atomic scale mechanism, the nature of the primary particles and their stability, or how they merge/aggregate to form larger structures is unknown. In this work, we use atomistic simulation methods, specifically DFT, evolutionary algorithms (EA), and Molecular Dynamics (MD), to investigate the structure and formation of C-S-H primary particles (PPs) from the ions in solution, and then discuss a possible formation pathway for the C-S-H nucleation. Our simulations indicate that even for small sizes the most stable clusters encode C-S-H structural motifs, and we identified a C(4)S(4)H(2) cluster candidate to be the C-S-H basic building block. We suggest a formation path in which small clusters formed by silicate dimers merge into large elongated aggregates. Upon dehydration, the C-S-H basic building blocks can be formed within the aggregates, and eventually crystallize. Nature Publishing Group UK 2023-12-02 /pmc/articles/PMC10693585/ /pubmed/38042823 http://dx.doi.org/10.1038/s41467-023-43500-y Text en © The Author(s) 2023 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
Aretxabaleta, Xabier M.
López-Zorrilla, Jon
Etxebarria, Iñigo
Manzano, Hegoi
Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title_full Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title_fullStr Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title_full_unstemmed Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title_short Multi-step nucleation pathway of C-S-H during cement hydration from atomistic simulations
title_sort multi-step nucleation pathway of c-s-h during cement hydration from atomistic simulations
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10693585/
https://www.ncbi.nlm.nih.gov/pubmed/38042823
http://dx.doi.org/10.1038/s41467-023-43500-y
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