Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
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Author(s) • • •
Ferralis, Nicola
Jagannathan, Deepak
Grossman, Jeffrey C.
Van Vliet, Krystyn J
Date Issued
August 2015
Journal
Journal of Materials Research
Publisher
Cambridge University Press
Citation
Ferralis, Nicola, Deepak Jagannathan, Jeffrey C. Grossman, and Krystyn J. Van Vliet. “Unintended Consequences: Why Carbonation Can Dominate in Microscale Hydration of Calcium Silicates.” J. Mater. Res. 30, no. 16 (August 2015): 2425-2433. © Materials Research Society 2015.
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Final published version
Abstract
The initial microscale mechanisms and materials interfacial process responsible for hydration of calcium silicates are poorly understood even in model systems. The lack of a measured microscale chemical signature has confounded understanding of growth mechanisms and kinetics for microreaction volumes. Here, we use Raman and optical spectroscopies to quantify hydration and environmental carbonation of tricalcium silicates across length and time scales. We show via spatially resolved chemical analysis that carbonate formation during the initial byproduct in microscale reaction volumes is significant, even for subambient CO2 levels. We propose that the competition between carbonation and hydration is enhanced strongly in microscale reaction volumes by increased surface-to-volume ratio relative to macroscale volumes, and by increased concentration of dissolved Ca2+ ions under poor hydration conditions that promote evaporation. This in situ analysis provides the first direct correlation between microscale interfacial hydration and carbonation environments and chemically defined reaction products in cementitious materials.
MIT Department
Massachusetts Institute of Technology. Department of Materials Science and Engineering
Massachusetts Institute of Technology. Research Laboratory of Electronics
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DOI of Published Version
https://doi.org/10.1557/jmr.2015.224