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Title: Influence of water activity on hydration of tricalcium aluminate‐calcium sulfate systems
Abstract

The hydration of tricalcium silicate (C3S)—the major phase in cement—is effectively arrested when the activity of water (aH) decreases below the critical value of 0.70. While it is implicitly understood that the reduction inaHsuppresses the hydration of tricalcium aluminate (C3A: the most reactive phase in cement), the dependence of kinetics of C3A hydration onaHand the criticalaHat which hydration of C3A is arrested are not known. This study employs isothermal microcalorimetry and complementary material characterization techniques to elucidate the influence ofaHon the hydration of C3A in [C3A + calcium sulfate (C$) + water] pastes. Reductions in water activity are achieved by partially replacing the water in the pastes with isopropanol. The results show that with decreasingaH, the kinetics of all reactions associated with C3A (eg, with C$, resulting in ettringite formation; and with ettringite, resulting in monosulfoaluminate formation) are proportionately suppressed. WhenaH ≤0.45, the hydration of C3A and the precipitation of all resultant hydrates are arrested; even in liquid saturated systems. In addition to—and separate from—the experiments, a thermodynamic analysis also indicates that the hydration of C3A does not commence or advance whenaH ≤0.45. On the basis of this criticalaH, the solubility product of C3A (KC3A) was estimated as 10−20.65. The outcomes of this work articulate the dependency of C3A hydration and its kinetics on water activity, and establish—for the first time—significant thermodynamic parameters (ie, criticalaHandKC3A) that are prerequisites for numerical modeling of C3A hydration.

 
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Award ID(s):
1932690 1661609
NSF-PAR ID:
10457693
Author(s) / Creator(s):
 ;  ;  ;  ;  
Publisher / Repository:
Wiley-Blackwell
Date Published:
Journal Name:
Journal of the American Ceramic Society
Volume:
103
Issue:
6
ISSN:
0002-7820
Page Range / eLocation ID:
p. 3851-3870
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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