Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates

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 volume...

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Main Authors: Ferralis, Nicola, Jagannathan, Deepak, Grossman, Jeffrey C., Van Vliet, Krystyn J
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Language:en_US
Published: Cambridge University Press 2016
Online Access:http://hdl.handle.net/1721.1/105387
https://orcid.org/0000-0003-4148-2424
https://orcid.org/0000-0003-1281-2359
https://orcid.org/0000-0001-5735-0560
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author Ferralis, Nicola
Jagannathan, Deepak
Grossman, Jeffrey C.
Van Vliet, Krystyn J
author2 Massachusetts Institute of Technology. Department of Materials Science and Engineering
author_facet Massachusetts Institute of Technology. Department of Materials Science and Engineering
Ferralis, Nicola
Jagannathan, Deepak
Grossman, Jeffrey C.
Van Vliet, Krystyn J
author_sort Ferralis, Nicola
collection MIT
description 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.
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spelling mit-1721.1/1053872022-09-29T11:30:49Z Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates Ferralis, Nicola Jagannathan, Deepak Grossman, Jeffrey C. Van Vliet, Krystyn J Massachusetts Institute of Technology. Department of Materials Science and Engineering Massachusetts Institute of Technology. Research Laboratory of Electronics Ferralis, Nicola Jagannathan, Deepak Grossman, Jeffrey C. Van Vliet, Krystyn J 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. United States. Department of Homeland Security. Science and Technology Directorate MIT Concrete Sustainability Hub Portland Cement Association Ready Mixed Concrete (RMC) Research & Education Foundation 2016-11-21T20:04:12Z 2016-11-21T20:04:12Z 2015-08 2015-04 Article http://purl.org/eprint/type/JournalArticle 0884-2914 2044-5326 http://hdl.handle.net/1721.1/105387 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. https://orcid.org/0000-0003-4148-2424 https://orcid.org/0000-0003-1281-2359 https://orcid.org/0000-0001-5735-0560 en_US http://dx.doi.org/10.1557/jmr.2015.224 Journal of Materials Research Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Cambridge University Press Prof. Grossman via Angie Locknar
spellingShingle Ferralis, Nicola
Jagannathan, Deepak
Grossman, Jeffrey C.
Van Vliet, Krystyn J
Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title_full Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title_fullStr Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title_full_unstemmed Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title_short Unintended consequences: Why carbonation can dominate in microscale hydration of calcium silicates
title_sort unintended consequences why carbonation can dominate in microscale hydration of calcium silicates
url http://hdl.handle.net/1721.1/105387
https://orcid.org/0000-0003-4148-2424
https://orcid.org/0000-0003-1281-2359
https://orcid.org/0000-0001-5735-0560
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