Title

The Influence of Water Activity on the Hydration Rate of Tricalcium Silicate

Abstract

Tricalcium silicate does not undergo hydration at relative humidities (RH's) below 80%. But, the rate at which its hydration rate decreases as a function of the RH has not yet been elucidated. By invoking correspondence between RH and water activity (aH, unitless), both of which are related to the chemical potential of water, the reaction evolutions of triclinic tricalcium silicate (i.e., T1-Ca3 SiO5 or C3 S) are tracked in water + isopropanol (IPA) mixtures, prepared across a wide range of water activities. Emphasis is placed on quantifying the: (a) rate of hydration as a function of aH, and (b) the critical (initial, aH0c or the achieved) water activity at which hydration effectively ceases, i.e., does not progress; here identified to be ≈ 0.70. The hydration of tricalcium silicate is arrested even when the system remains near saturated with a liquid phase, such that small, if any, capillary stresses develop. This suggests that changes in chemical potential induced via a vapor-phase or liquid-phase route both induce similar suppressions of C3 S hydration. A phase boundary nucleation and growth (pBNG) model is fit to measured hydration rates from the onset of the acceleration period until well beyond the rate maximum when the water activity is altered. The simulations suggest that for a fixed hydrate nucleation density, any water activity reductions consistently suppress the growth of hydration products. Thermodynamic considerations of how water activity changes may influence reactions/hydrate evolutions are discussed. The outcomes improve our understanding of the chemical factors that influence the rate of Ca3 SiO5 hydration.

Department(s)

Materials Science and Engineering

Comments

The authors acknowledge financial support for this research provided by: The National Science Foundation (CMMI: 1066583 and CAREER Award: 1235269), U.S. Department of Transportation: Federal Highway Administration (DTFH61-13-H-00011) and the National Institute of Standards and Technology through the Exploratory Research Program (NIST-EARP, EL: 70NSNB13H005).

Keywords and Phrases

Atmospheric humidity; Calcium; Calcium silicate; Chemical potential; Nucleation; Silicates, Capillary stress; Chemical factors; Hydrate nucleation; Hydration products; Hydration rate; Influence of water; Nucleation and growth; Tricalcium silicate, Hydration

International Standard Serial Number (ISSN)

0002-7820; 1551-2916

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2016The American Ceramic Society, All rights reserved.

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