Abstract

Water in calcium silicate hydrate (C-S-H) is one of the key parameters driving the macroscopic behavior of cement materials, for which water vapor partial pressure has a impact on the Young's modulus and the volumic properties. Several samples of C-S-H with bulk Ca/Si ratio ranging between 0.6 and 1.6 were characterized to study their dehydration/hydration behavior under water-controlled conditions, using 29Si NMR, water adsorption volumetry, X-ray diffraction, and Fourier-transform near-infrared diffuse reflectance, under various water pressures. Coherent with several previous studies, it was observed that an increase in the Ca/Si ratio is due to the progressive omission of Si bridging tetrahedra, with the resulting charge being compensated for by interlayer Ca and that water conditioning influences the layer-to-layer distance and the achieved NMR spectral resolution. Water desorption experiments exhibit one step toward low relative pressure, accompanied by a decrease in the layer-to-layer distance. When sufficient energy is provided to the system (T ≥ 40 °C under vacuum) to remove the interlayer water, the shrinkage/swelling is partially reversible in our experimental conditions. A change in layer-to-layer distance of less than 3 Å is measured in the C-S-H between the wet and dried states. When the bridging SiO2 tetrahedra are omitted, interlayer Ca interacts with layer O and water interacts with the cations and potentially with the surfaces. This structural organization is interpreted as a mid-plane monolayer of water in the interlayer space, this latter accounting for about 30 % of the volume of C-S-H particles.

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