1 Solubility and Structure of Calcium Silicate Hydrate Jeffrey J. Chena†, Jeffrey J. Thomasb, Hal F. W. Taylorc‡, and Hamlin M. Jenningsab* aNorthwestern University, Department of Materials Science and Engineering, Evanston, IL 60208; bNorthwestern University, Department of Civil and Environmental Engineering, Evanston, IL 60208; cMaudry Bank, Lake Road, Coniston, Cumbria, LA21 8EW, UK *Corresponding author: Tel: +1–847–491–4858, Fax: +1–847–491–4011 Email addresses:
[email protected] (J.J. Chen),
[email protected] (H.M. Jennings) † Present address: Lafarge Laboratoire Central de Recherche, 38291 Saint Quentin Fallavier Cedex, France ‡ Deceased as of 25 November 2002 Keywords: Calcium silicate hydrate (C–S–H), Solubility, Spectroscopy Abstract C–S–H, the poorly crystalline calcium silicate hydrate formed in cement paste and aqueous suspension, is characterized by extensive disorder and structural variations at the nanometer scale. An analysis of new and published solubility data for C–S–H formed by different preparation methods and with a broad range of compositions illustrates a previously unrecognized family of solubility curves in the CaO–SiO2–H2O system at room temperature. As demonstrated by 29Si magic-angle spinning (MAS) NMR data and by charge balance calculations, the observed differences in solubility arise from systematic variations in Ca/Si ratio, silicate structure, and Ca–OH content. Based on this evidence, the family of solubility curves are interpreted to represent a spectrum of metastable C–S–H phases whose structures range from purely tobermorite-like to largely jennite-like. These findings give an improved understanding of the structure of these phases and reconcile some of the discrepancies in the literature regarding the structure of C–S–H at high Ca/Si ratios.