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The nanomechanical properties of non-crosslinked calcium aluminosilicate hydrate: The influences of tetrahedral Al and curing age

Li, Jiaqi and Zhang, Wenxin and Sanz-Camacho, Paula and Duttine, Mathieu and Gardner, David and Carraro, Carlo and Maboudian, Roya and Huthwelker, Thomas (2022) The nanomechanical properties of non-crosslinked calcium aluminosilicate hydrate: The influences of tetrahedral Al and curing age. Cement and Concrete Research, 159 . Art. No. 106900. ISSN 0008-8846. doi:10.1016/j.cemconres.2022.106900.

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Calcium aluminosilicate hydrate (C-A-S-H) is the binding phase of both blended cement-based and alkali-activated materials. The intrinsic mechanical properties of non-cross-linked C-A-S-H are important while experimentally unvalidated. Here, the properties are for the first time measured using high-pressure X-ray diffraction. The incompressibility and bulk modulus K₀ of C-A-S-Hs are correlated to their nanostructure and stability using nuclear magnetic resonance and X-ray absorption spectroscopies. Al coordination in stable C-A-S-H (Al/Si = 0.1) cured for 546 days is purely tetrahedral (Alᴵⱽ), while in metastable C-A-S-H (Al/Si = 0.05) cured for only 182 days is both Alᴵⱽ and pentahedral (Alⱽ). The stable C-A-S-H is stiffer along the a,b,c-axis with higher K₀ relative to C-S-H. Short-curing-induced metastable C-A-S-H (Al/Si = 0.05) shows expanded interlayer and softer c-axis, thus lower K₀ than C-S-H and the stable C-A-S-H. Our results highlight the stiffening effect of Alᴵⱽ incorporation and the negative influences of insufficient curing on the nanomechanical properties of non-cross-linked C-A-S-H at Ca/Si = 1.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Li, Jiaqi0000-0003-2021-2310
Sanz-Camacho, Paula0000-0003-4898-8225
Duttine, Mathieu0000-0002-6120-8716
Maboudian, Roya0000-0002-5121-6560
Huthwelker, Thomas0000-0003-4174-8958
Additional Information:© 2022 Elsevier. Received 19 September 2020, Revised 24 June 2022, Accepted 1 July 2022, Available online 9 July 2022, Version of Record 9 July 2022. This work was partially performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. This study is funded by the US National Science Foundation under the Division of Materials Research Ceramics Program, DMR-CER, grant # 1935604. This work is further supported by the Republic of Singapore National Research Foundation through a grant to the Berkeley Education Alliance for Research in Singapore (BEARS) for the Singapore-Berkeley Building Efficiency and Sustainability in the Tropics (SinBerBEST) Program. We thank Dr. Lothenbach for providing the samples synthesized by Dr. L'Hôpital at the Laboratory for Concrete & Construction Chemistry (EMPA). We thank Dr. Paulo Monteiro at UC Berkeley for sharing the beamtime. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Beamline 12.2.2 is partially supported by COMPRES, the Consortium for Materials Properties Research in Earth Sciences under NSF Cooperative Agreement EAR 1606856. We thank the support from Dr. Andrew Doran, Dr. Jinyuan Yan, and Dr. Martin Kunz at the Advanced Light Source. We acknowledge the Paul Scherrer Institut, Villigen, Switzerland for provision of synchrotron radiation beamtime at beamline PHOENIX of the SLS. LLNL IM release number: LLNL-JRNL-836263. CRediT authorship contribution statement. Jiaqi Li: Conceptualization, Methodology, Investigation, Validation, Visualization, Writing – original draft, Funding acquisition. Wenxin Zhang: Investigation, Visualization, Writing – review & editing. Paula Sanz-Camacho: Investigation, Visualization, Writing – review & editing. Mathieu Duttine: Investigation, Visualization, Writing – review & editing. David Gardner: Investigation, Visualization, Writing – review & editing. Carlo Carraro: Visualization, Writing – review & editing. Roya Maboudian: Validation, Writing – review & editing, Funding acquisition. Thomas Huthwelker: Validation, Writing – review & editing. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC52-07NA27344
National Research Foundation (Singapore)UNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
Subject Keywords:C-A-S-H; C-S-H; High-pressure X-ray diffraction; Bulk modulus; Blended cement
Record Number:CaltechAUTHORS:20220711-653016000
Persistent URL:
Official Citation:Jiaqi Li, Wenxin Zhang, Paula Sanz-Camacho, Mathieu Duttine, David Gardner, Carlo Carraro, Roya Maboudian, Thomas Huthwelker, The nanomechanical properties of non-crosslinked calcium aluminosilicate hydrate: The influences of tetrahedral Al and curing age, Cement and Concrete Research, Volume 159, 2022, 106900, ISSN 0008-8846,
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:115466
Deposited By: George Porter
Deposited On:12 Jul 2022 15:16
Last Modified:11 Nov 2022 22:25

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