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A series of experiments were undertaken to examine the effects of carbonation on the chemical composition of water in a grout/water slurry. Powdered grout samples were reacted with deionized water in sealed flasks. Progressive carbonation was induced by adding known weights of COz to the slurries at various times. Solution samples were withdrawn several days after each addition of COz, filtered, and analyzed for mdor ions. A chemical equilibria model was used to simulate the reactions between water and grout during progressive carbonation. The equilibria model provides a good representation of the experimental data. Disparities between the simulated and experimental results provide important information on the inadequacies of the physicochemical model and suggest areas for further research to improve the description of chemical equilibria in cement/ water systems. [