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Time-Space-Resolved Chemical Deconvolution of Cementitious Colloidal Systems Using Raman Spectroscopy

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    Time-Space-Resolved Chemical Deconvolution of Cementitious Colloidal Systems Using Raman Spectroscopy
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    Langmuir

    Cite this: Langmuir 2021, 37, 23, 7019–7031
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    https://doi.org/10.1021/acs.langmuir.1c00609
    Published June 7, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Concrete is one of the most used materials in the world, second only to water. One of the key advantages of this versatile material is its workability in the early stages before setting. Here, we use in situ underwater Raman microspectroscopy to investigate and visualize the early hydration kinetics of ordinary Portland cement (OPC) with submicron spatial and high temporal resolution. First, the spectral features of the C–S–H gel were analyzed in the hydroxyl stretching region to confirm the coexistence of Ca–OH and Si–OH bonds in a highly disordered C–S–H gel. Second, the disordered calcium hydroxide (Ca(OH)2) is experimentally identified for the first time in the mixture before setting, suggesting that Ca(OH)2 crystallization and growth are essential in the setting of cement paste. Finally, the phase transformations of clinker, C–S–H, and Ca(OH)2 are spatially and temporally resolved, and the hydration kinetics are studied by analyzing the spatial relationships of these phases using two-point correlation functions. The results quantitatively validate that the setting occurs as a percolation process, wherein the hydration products intersect and form an interconnected network. This time-space-resolved characterization method can map and quantitatively analyze the heterogeneous reaction of the cementitious colloidal system and thus provide potential application value in the field of cement chemistry and materials design more broadly.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.langmuir.1c00609.

    • Chemical composition of the materials; C–S–H Raman band deconvolution resul; depth scan of a cement paste sample; average Raman spectra during the early stage cement hydration; color-gradient representation of the chemical phases; OH peak position and width of DCH and CH; Raman heatmaps of the sulfate phases; auto- and cross-correlation graph calculation procedures; auto- and cross-correlation graphs of the phases; long-term observation of cement hydration; color gradient assignment (PDF)

    • Scatter-histogram graphs (0–24 h) (MP4)

    • Clinker phase hydration mapping (0–24 h) (MP4)

    • Sulfate phase hydration mapping (0–24 h) (MP4)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

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    This article is cited by 10 publications.

    1. Krishna C. Polavaram, Nishant Garg. Elucidating the Size and Shape of Individual Clinker Phases via Raman Imaging: Impact on Cement Hydration. The Journal of Physical Chemistry C 2023, 127 (34) , 17157-17170. https://doi.org/10.1021/acs.jpcc.3c03453
    2. Teresa Liberto, Andreas Nenning, Maurizio Bellotto, Maria Chiara Dalconi, Dominik Dworschak, Lukas Kalchgruber, Agathe Robisson, Markus Valtiner, Joanna Dziadkowiec. Detecting Early-Stage Cohesion Due to Calcium Silicate Hydration with Rheology and Surface Force Apparatus. Langmuir 2022, 38 (48) , 14988-15000. https://doi.org/10.1021/acs.langmuir.2c02783
    3. Mohamed-Nadjib Brahim, Jean-Michel Mechling, Sarah Janvier-Badosa, Mario Marchetti. Early stage ettringite and monosulfoaluminate carbonation investigated by in situ Raman spectroscopy coupled with principal component analysis. Materials Today Communications 2023, 35 , 105539. https://doi.org/10.1016/j.mtcomm.2023.105539
    4. Sonali Srivastava, Nishant Garg. Tracking spatiotemporal evolution of cementitious carbonation via Raman imaging. Journal of Raman Spectroscopy 2023, 54 (4) , 414-425. https://doi.org/10.1002/jrs.6483
    5. Jiseul Park, Myungjun Jung, Yang-woo Lee, Hee-Young Hwang, Sung-gul Hong, Juhyuk Moon. Quantified analysis of 2D dispersion of carbon nanotubes in hardened cement composite using confocal Raman microspectroscopy. Cement and Concrete Research 2023, 166 , 107102. https://doi.org/10.1016/j.cemconres.2023.107102
    6. Damian Stefaniuk, Marcin Hajduczek, James C Weaver, Franz J Ulm, Admir Masic, . Cementing CO2 into C-S-H: A step toward concrete carbon neutrality. PNAS Nexus 2023, 2 (3) https://doi.org/10.1093/pnasnexus/pgad052
    7. K. Zhang, M. H. N. Yio, H. S. Wong, N. R. Buenfeld. Optimising confocal Raman microscopy for spectral mapping of cement-based materials. Materials and Structures 2022, 55 (4) https://doi.org/10.1617/s11527-022-01979-9
    8. Omar Abdelrahman, Nishant Garg. Impact of Na/Al Ratio on the Extent of Alkali-Activation Reaction: Non-linearity and Diminishing Returns. Frontiers in Chemistry 2022, 9 https://doi.org/10.3389/fchem.2021.806532
    9. Rachel Camerini, Giovanna Poggi, Francesca Ridi, Piero Baglioni. The kinetic of calcium silicate hydrate formation from silica and calcium hydroxide nanoparticles. Journal of Colloid and Interface Science 2022, 605 , 33-43. https://doi.org/10.1016/j.jcis.2021.06.168
    10. Krishna C. Polavaram, Nishant Garg. Enabling phase quantification of anhydrous cements via Raman imaging. Cement and Concrete Research 2021, 150 , 106592. https://doi.org/10.1016/j.cemconres.2021.106592
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    Langmuir

    Cite this: Langmuir 2021, 37, 23, 7019–7031
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.langmuir.1c00609
    Published June 7, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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