High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates

The heterogeneous nature of the cement clinker, its complex coupled dissolution/re-precipitation process and the complex defect chemistry of the hydrates formed during cement hydration, make that the nucleation and growth mechanisms of cement hydrates are not fully understood. Recent studies have su...

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Autores: Besselink, R., Poulain, A., Bella, M. la, Auzende, A. L., Goberna-Ferron, S., Asta, M. P., Magnin, V., Bureau, S., Fernández-Carrasco, L., Van Driessche, Alexander E. S., Fernández-Martínez, A.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/387440
Acceso en línea:http://hdl.handle.net/10261/387440
Access Level:acceso abierto
Palabra clave:Cement
Nucleation
Proto CSH
Calcium silicate hydrate
X-ray scattering
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spelling High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydratesBesselink, R.Poulain, A.Bella, M. laAuzende, A. L.Goberna-Ferron, S.Asta, M. P.Magnin, V.Bureau, S.Fernández-Carrasco, L.Van Driessche, Alexander E. S.Fernández-Martínez, A.CementNucleationProto CSHCalcium silicate hydrateX-ray scatteringThe heterogeneous nature of the cement clinker, its complex coupled dissolution/re-precipitation process and the complex defect chemistry of the hydrates formed during cement hydration, make that the nucleation and growth mechanisms of cement hydrates are not fully understood. Recent studies have suggested the existence of a disordered precursor prior to the crystallization of C-S-H. Here, a combination of X-ray scattering and electron microscopy experiments are used to study the structure and crystallization kinetics of this amorphous intermediate. Our results suggest that proto-C-S-H is predominantly composed of 6-fold oxygen-to-calcium coordinated CaOx polyhedra, in contrast to the 7-fold coordinated polyhedra in C-S-H with a tobermorite-like structure. The addition of gluconate, a widely used additive, resulted in an increased kinetic persistence of proto-C-S-H. Overall, our study provides new insights into the formation and structure of proto-C-S-H, and suggests that it plays an important role in the crystallization mechanism of C-S-H.This research was founded by the French National Research Agency (ANR-JCJC \u201CNUANCE\u201D, grant ANR-17-CE08-0057 ). We would like to thank Leighanne Gallington, Olaf Borkiewicz, UtaRuett and Kamila, Wiaderek for their assistance with HEXS analyses at the Advanced Photon Source (APS) beamline 11 ID-B. Use of the Advanced Photon Source was supported by the U.S. Department of Energy , Office of Science , Office of Basic Energy Sciences . Moreover, we also like to thank D. Chaudanson and A. Alti\u00E9for their assistance with the high-resolution transmission electron microscopy measurements at CINaM (Marseille, France). This work was partially performed at the Geochemistry-Mineralogy platform of ISTerre.Peer reviewedElsevier BVAgence Nationale de la Recherche (France)Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252025info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/387440reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttps://doi.org/10.1016/j.cemconres.2025.107855Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3874402026-05-22T06:33:51Z
dc.title.none.fl_str_mv High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
title High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
spellingShingle High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
Besselink, R.
Cement
Nucleation
Proto CSH
Calcium silicate hydrate
X-ray scattering
title_short High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
title_full High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
title_fullStr High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
title_full_unstemmed High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
title_sort High energy X-ray scattering reveals the short-range order of proto-C-S-H: Implications for the nucleation of cement hydrates
dc.creator.none.fl_str_mv Besselink, R.
Poulain, A.
Bella, M. la
Auzende, A. L.
Goberna-Ferron, S.
Asta, M. P.
Magnin, V.
Bureau, S.
Fernández-Carrasco, L.
Van Driessche, Alexander E. S.
Fernández-Martínez, A.
author Besselink, R.
author_facet Besselink, R.
Poulain, A.
Bella, M. la
Auzende, A. L.
Goberna-Ferron, S.
Asta, M. P.
Magnin, V.
Bureau, S.
Fernández-Carrasco, L.
Van Driessche, Alexander E. S.
Fernández-Martínez, A.
author_role author
author2 Poulain, A.
Bella, M. la
Auzende, A. L.
Goberna-Ferron, S.
Asta, M. P.
Magnin, V.
Bureau, S.
Fernández-Carrasco, L.
Van Driessche, Alexander E. S.
Fernández-Martínez, A.
author2_role author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Agence Nationale de la Recherche (France)
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Cement
Nucleation
Proto CSH
Calcium silicate hydrate
X-ray scattering
topic Cement
Nucleation
Proto CSH
Calcium silicate hydrate
X-ray scattering
description The heterogeneous nature of the cement clinker, its complex coupled dissolution/re-precipitation process and the complex defect chemistry of the hydrates formed during cement hydration, make that the nucleation and growth mechanisms of cement hydrates are not fully understood. Recent studies have suggested the existence of a disordered precursor prior to the crystallization of C-S-H. Here, a combination of X-ray scattering and electron microscopy experiments are used to study the structure and crystallization kinetics of this amorphous intermediate. Our results suggest that proto-C-S-H is predominantly composed of 6-fold oxygen-to-calcium coordinated CaOx polyhedra, in contrast to the 7-fold coordinated polyhedra in C-S-H with a tobermorite-like structure. The addition of gluconate, a widely used additive, resulted in an increased kinetic persistence of proto-C-S-H. Overall, our study provides new insights into the formation and structure of proto-C-S-H, and suggests that it plays an important role in the crystallization mechanism of C-S-H.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/387440
url http://hdl.handle.net/10261/387440
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv https://doi.org/10.1016/j.cemconres.2025.107855
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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