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Spontaneous precipitation of calcium silicate hydrate in aqueous solutions

Calcium silicate hydrates (C‐S‐H) are very important not only for their contribution to the development of cement and concrete properties but also for use as fillers and in silicate glasses. In the present work, the thermodynamics and the kinetics of the spontaneous precipitation of C‐S‐H from aqueous solutions were investigated over the pH range 10‐12 at 25 °C. The thermodynamic driving force was calculated taking into consideration all equilibria involved in the supersaturated solutions. In the range of the solution supersaturation values examined the precipitation occurred spontaneously, with the exception of the series of experiments done at pH 12.0, where induction times preceded the appearance of the precipitate. The rates were measured at constant pH as a function of the solution supersaturation and were found to depend strongly on the solution supersaturation, pH and on the total calcium to total silicate molar ratio in solution. Fit of the kinetics results in a power law relating rates of precipitation with respect to C‐S‐H precipitated, suggested a surface diffusion controlled mechanism for the formation of C‐S‐H. The precipitated solids did not show significant morphological differences at different pH values. From the induction times preceding the spontaneous precipitation at pH 12.0, a value of 30 mJm‐2 was calculated for the surface energy of C‐S‐H. (© 2010 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)