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The chemical properties of the CaO-Al2O3-SiO2-H2O system are important for understanding and predicting the behaviour of Portland cements in cementitious wasteforms and radioactive waste repositories. Solids of known average composition in this system have been synthesised by the co-hydrolysis of mixed alkoxides. The solids have been equilibrated with water at 25°C and the composition of the aqueous phase characterised. A thermodynamic model for the system has been developed by extending an earlier model of solid solutions in amorphous gels to include aluminium compounds. The model accounts for most of the experimental data and predicts that the main influence of aluminium is to form a hydrogarnet solid solution of general composition C3AH6−2xSx The model can be used to predict the chemistry of hydrated cements and the interaction of cements with groundwaters.

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