Carbonation of cementitious wasteforms under supercritical and high pressure subcritical conditions

Abstract

A comparison of cement wasteform carbonation under subcritical and supercritical CO2 conditions has been conducted, as well as leach tests on the carbonated products. Cement samples were prepared with water containing As, Cs, Sr, Ni and Cl, and dried under vacuum prior to exposure to CO2 gas at sub and supercritical conditions. Carbonation under supercritical conditions (50°C, 1200 psi) showed similar CO2 mass uptake as subcritical carbonation (25°C, 800 psi). The apparent depth of carbonation from microscopic examination, however, appeared greater with the supercritical treatment. Microscopic examination also revealed a dark intermediate zone, likely a chemical transition area, between the uncarbonated and carbonated material. Results from experiments where the initial water to cement ratio (w/c) and curing time were varied indicate that high w/c ratios and short curing times promote greater carbonation. In addition, the pore network in specimens with low w/c ratios (0.45) completely filled with water during carbonation. This caused pore water containing soluble contaminants to exude from the specimens. This does not occur at a w/c of 0.60 because the larger pore network after the drying step easily accommodates all the water produced during the reaction. No measurable arsenic or nickel were released in leach tests conducted on both carbonated and uncarbonated specimens. Calcium, cesium and strontium leachability were reduced by carbonation while the teachability of chloride and nitrate were increased with carbonation. Samples carbonated under supercritical pressure conditions showed similar leaching characteristics as samples carbonated under subcritical conditions.