TY - JOUR
T1 - Structure of Water Adsorbed on Nanocrystalline Calcium Silicate Hydrate Determined from Neutron Scattering and Molecular Dynamics Simulations
AU - Zhakiyeva, Zhanar
AU - Cuello, Gabriel J.
AU - Fischer, Henry E.
AU - Bowron, Daniel T.
AU - Dejoie, Catherine
AU - Magnin, Valerie
AU - Campillo, Sylvain
AU - Bureau, Sarah
AU - Poulain, Agnieszka
AU - Besselink, Rogier
AU - Gaboreau, Stephane
AU - Grangeon, Sylvain
AU - Claret, Francis
AU - Bourg, Ian C.
AU - Van Driessche, Alexander E.S.
AU - Fernandez-Martinez, Alejandro
N1 - Funding Information:
Use of the Geochemistry-Mineralogy platform at ISTerre is acknowledged. A.F.-M. and A.E.S.V.-D. acknowledge funding from the ANR-JCJC “NUANCE” project (grant ANR-17-CE08-0057). We thank the IDEX mobility scholarship program of the University of Grenoble-Alpes for supporting a research stay at Princeton University. We thank the Institut Laue-Langevin, ISIS Neutron and Muon Source European Synchrotron Radiation Facility, and Advanced Proton Source for allocated beamtimes. I.C.B. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Geosciences Program under Award DE-SC0018419. Molecular dynamics simulations were performed using resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the U.S. Department of Energy, Office of Science, under Award DE-AC02-05CH11231. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Leighanne C. Gallington is thanked for her help during data acquisition at 11-ID-B (APS, ANL). Z.Z. thanks BRGM for co-funding her PhD.
Funding Information:
Use of the Geochemistry-Mineralogy platform at ISTerre is acknowledged. A.F.-M. and A.E.S.V.-D. acknowledge funding from the ANR-JCJC “NUANCE” project (grant ANR-17-CE08-0057). We thank the IDEX mobility scholarship program of the University of Grenoble-Alpes for supporting a research stay at Princeton University. We thank the Institut Laue-Langevin, ISIS Neutron and Muon Source, European Synchrotron Radiation Facility, and Advanced Proton Source for allocated beamtimes. I.C.B. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Geosciences Program under Award DE-SC0018419. Molecular dynamics simulations were performed using resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the U.S. Department of Energy, Office of Science, under Award DE-AC02-05CH11231. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Leighanne C. Gallington is thanked for her help during data acquisition at 11-ID-B (APS, ANL). Z.Z. thanks BRGM for co-funding her PhD.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/8/4
Y1 - 2022/8/4
N2 - Calcium silicate hydrate (C-S-H) is a disordered, nanocrystalline material that acts as a primary binding phase in Portland cement. Thin films of water are present on the surfaces and in nanopores of C-S-H, impacting many of its chemical and mechanical properties, such as ion transport, creep, or thermal behavior. Despite decades of research, a full understanding of the structural details of adsorbed, confined, and bulk water in C-S-H remains elusive. In this work, we applied a multitechnique study involving molecular dynamics (MD) simulations validated by neutron diffraction with isotopic substitution (NDIS) and X-ray scattering methods to investigate the structure of water in C-S-H and C-A-S-H (an Al-bearing, low-CO2C-S-H substitute). Direct comparison of NDIS data with the MD results reveals that the structure of confined and interfacial water differs significantly from the bulk water and exhibits a larger degree of mesoscale ordering for more hydrated C-S-H structures. This observation suggests an important role of water as a stabilizer of the atomistic-level structure of C-S-H.
AB - Calcium silicate hydrate (C-S-H) is a disordered, nanocrystalline material that acts as a primary binding phase in Portland cement. Thin films of water are present on the surfaces and in nanopores of C-S-H, impacting many of its chemical and mechanical properties, such as ion transport, creep, or thermal behavior. Despite decades of research, a full understanding of the structural details of adsorbed, confined, and bulk water in C-S-H remains elusive. In this work, we applied a multitechnique study involving molecular dynamics (MD) simulations validated by neutron diffraction with isotopic substitution (NDIS) and X-ray scattering methods to investigate the structure of water in C-S-H and C-A-S-H (an Al-bearing, low-CO2C-S-H substitute). Direct comparison of NDIS data with the MD results reveals that the structure of confined and interfacial water differs significantly from the bulk water and exhibits a larger degree of mesoscale ordering for more hydrated C-S-H structures. This observation suggests an important role of water as a stabilizer of the atomistic-level structure of C-S-H.
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U2 - 10.1021/acs.jpcc.2c02626
DO - 10.1021/acs.jpcc.2c02626
M3 - Article
AN - SCOPUS:85136395822
SN - 1932-7447
VL - 126
SP - 12820
EP - 12835
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 30
ER -