Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations

Zhanar Zhakiyeva; Valérie Magnin; Agnieszka Poulain; Sylvain Campillo; María P. Asta; Rogier Besselink; Stéphane Gaboreau; Francis Claret; Sylvain Grangeon; Svemir Rudic; Stéphane Rols; Mónica Jiménez-Ruiz; Ian C. Bourg; Alexander E.S. Van Driessche; Gabriel J. Cuello; Alejandro Fernández-Martínez

doi:10.1016/j.cemconres.2024.107616

Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations

Zhanar Zhakiyeva, Valérie Magnin, Agnieszka Poulain, Sylvain Campillo, María P. Asta, Rogier Besselink, Stéphane Gaboreau, Francis Claret, Sylvain Grangeon, Svemir Rudic, Stéphane Rols, Mónica Jiménez-Ruiz, Ian C. Bourg, Alexander E.S. Van Driessche, Gabriel J. Cuello, Alejandro Fernández-Martínez

Research output: Contribution to journal › Article › peer-review

Abstract

Calcium-silicate-hydrate (C-S-H) is a disordered, nanocrystalline material, acting as a primary binding phase in Portland cement. C-S-H and C-A-S-H (an Al-bearing substitute present in low-CO₂ cement) contain thin films of water on solid surfaces and inside nanopores. Water controls multiple chemical and mechanical properties of C-S-H, including drying shrinkage, ion transport, creep, and thermal behavior. Therefore, obtaining a fundamental understanding of its properties is essential. We applied a combination of inelastic incoherent neutron scattering and molecular dynamics simulations to unravel water dynamics in synthetic C-(A)-S-H conditioned at five hydration states (from drier to more hydrated) and with three Ca/Si ratios (0.9, 1, and 1.3). Our results converge towards a picture where the evolution from thin layers of interfacial water to bulk-like capillary water is dampened by the structure of C-(A)-S-H. In particular, the hydrophilic Ca²⁺ sites organize the distribution of interfacial C-(A)-S-H water.

Original language	English (US)
Article number	107616
Journal	Cement and Concrete Research
Volume	184
DOIs	https://doi.org/10.1016/j.cemconres.2024.107616
State	Published - Oct 2024
Externally published	Yes

All Science Journal Classification (ASJC) codes

Building and Construction
General Materials Science

Keywords

C-(A)-S-H
Inelastic neutron scattering
Interfacial water
Low CO cements
Molecular dynamics simulations
Nanoporous vs bulk-like water
Water dynamics

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10.1016/j.cemconres.2024.107616

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Zhakiyeva, Z., Magnin, V., Poulain, A., Campillo, S., Asta, M. P., Besselink, R., Gaboreau, S., Claret, F., Grangeon, S., Rudic, S., Rols, S., Jiménez-Ruiz, M., Bourg, I. C., Van Driessche, A. E. S., Cuello, G. J., & Fernández-Martínez, A. (2024). Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations. Cement and Concrete Research, 184, Article 107616. https://doi.org/10.1016/j.cemconres.2024.107616

@article{593c47960e5943e6a01a42230887aaa7,

title = "Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations",

abstract = "Calcium-silicate-hydrate (C-S-H) is a disordered, nanocrystalline material, acting as a primary binding phase in Portland cement. C-S-H and C-A-S-H (an Al-bearing substitute present in low-CO2 cement) contain thin films of water on solid surfaces and inside nanopores. Water controls multiple chemical and mechanical properties of C-S-H, including drying shrinkage, ion transport, creep, and thermal behavior. Therefore, obtaining a fundamental understanding of its properties is essential. We applied a combination of inelastic incoherent neutron scattering and molecular dynamics simulations to unravel water dynamics in synthetic C-(A)-S-H conditioned at five hydration states (from drier to more hydrated) and with three Ca/Si ratios (0.9, 1, and 1.3). Our results converge towards a picture where the evolution from thin layers of interfacial water to bulk-like capillary water is dampened by the structure of C-(A)-S-H. In particular, the hydrophilic Ca2+ sites organize the distribution of interfacial C-(A)-S-H water.",

keywords = "C-(A)-S-H, Inelastic neutron scattering, Interfacial water, Low CO cements, Molecular dynamics simulations, Nanoporous vs bulk-like water, Water dynamics",

author = "Zhanar Zhakiyeva and Val{\'e}rie Magnin and Agnieszka Poulain and Sylvain Campillo and Asta, {Mar{\'i}a P.} and Rogier Besselink and St{\'e}phane Gaboreau and Francis Claret and Sylvain Grangeon and Svemir Rudic and St{\'e}phane Rols and M{\'o}nica Jim{\'e}nez-Ruiz and Bourg, {Ian C.} and {Van Driessche}, {Alexander E.S.} and Cuello, {Gabriel J.} and Alejandro Fern{\'a}ndez-Mart{\'i}nez",

note = "Publisher Copyright: {\textcopyright} 2024",

year = "2024",

month = oct,

doi = "10.1016/j.cemconres.2024.107616",

language = "English (US)",

volume = "184",

journal = "Cement and Concrete Research",

issn = "0008-8846",

publisher = "Elsevier Ltd",

}

Zhakiyeva, Z, Magnin, V, Poulain, A, Campillo, S, Asta, MP, Besselink, R, Gaboreau, S, Claret, F, Grangeon, S, Rudic, S, Rols, S, Jiménez-Ruiz, M, Bourg, IC, Van Driessche, AES, Cuello, GJ & Fernández-Martínez, A 2024, 'Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations', Cement and Concrete Research, vol. 184, 107616. https://doi.org/10.1016/j.cemconres.2024.107616

TY - JOUR

T1 - Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations

AU - Zhakiyeva, Zhanar

AU - Magnin, Valérie

AU - Poulain, Agnieszka

AU - Campillo, Sylvain

AU - Asta, María P.

AU - Besselink, Rogier

AU - Gaboreau, Stéphane

AU - Claret, Francis

AU - Grangeon, Sylvain

AU - Rudic, Svemir

AU - Rols, Stéphane

AU - Jiménez-Ruiz, Mónica

AU - Bourg, Ian C.

AU - Van Driessche, Alexander E.S.

AU - Cuello, Gabriel J.

AU - Fernández-Martínez, Alejandro

PY - 2024/10

Y1 - 2024/10

N2 - Calcium-silicate-hydrate (C-S-H) is a disordered, nanocrystalline material, acting as a primary binding phase in Portland cement. C-S-H and C-A-S-H (an Al-bearing substitute present in low-CO2 cement) contain thin films of water on solid surfaces and inside nanopores. Water controls multiple chemical and mechanical properties of C-S-H, including drying shrinkage, ion transport, creep, and thermal behavior. Therefore, obtaining a fundamental understanding of its properties is essential. We applied a combination of inelastic incoherent neutron scattering and molecular dynamics simulations to unravel water dynamics in synthetic C-(A)-S-H conditioned at five hydration states (from drier to more hydrated) and with three Ca/Si ratios (0.9, 1, and 1.3). Our results converge towards a picture where the evolution from thin layers of interfacial water to bulk-like capillary water is dampened by the structure of C-(A)-S-H. In particular, the hydrophilic Ca2+ sites organize the distribution of interfacial C-(A)-S-H water.

AB - Calcium-silicate-hydrate (C-S-H) is a disordered, nanocrystalline material, acting as a primary binding phase in Portland cement. C-S-H and C-A-S-H (an Al-bearing substitute present in low-CO2 cement) contain thin films of water on solid surfaces and inside nanopores. Water controls multiple chemical and mechanical properties of C-S-H, including drying shrinkage, ion transport, creep, and thermal behavior. Therefore, obtaining a fundamental understanding of its properties is essential. We applied a combination of inelastic incoherent neutron scattering and molecular dynamics simulations to unravel water dynamics in synthetic C-(A)-S-H conditioned at five hydration states (from drier to more hydrated) and with three Ca/Si ratios (0.9, 1, and 1.3). Our results converge towards a picture where the evolution from thin layers of interfacial water to bulk-like capillary water is dampened by the structure of C-(A)-S-H. In particular, the hydrophilic Ca2+ sites organize the distribution of interfacial C-(A)-S-H water.

KW - C-(A)-S-H

KW - Inelastic neutron scattering

KW - Interfacial water

KW - Low CO cements

KW - Molecular dynamics simulations

KW - Nanoporous vs bulk-like water

KW - Water dynamics

UR - http://www.scopus.com/inward/record.url?scp=85199910499&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85199910499&partnerID=8YFLogxK

U2 - 10.1016/j.cemconres.2024.107616

DO - 10.1016/j.cemconres.2024.107616

M3 - Article

AN - SCOPUS:85199910499

SN - 0008-8846

VL - 184

JO - Cement and Concrete Research

JF - Cement and Concrete Research

M1 - 107616

ER -

Water dynamics in calcium silicate hydrates probed by inelastic neutron scattering and molecular dynamics simulations

Abstract

All Science Journal Classification (ASJC) codes

Keywords

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