Mineral sequestration of CO2 by aqueous carbonation of coal combustion fly-ash

The increasing CO2 concentration in the Earth's atmosphere, mainly caused by fossil fuel combustion, has led to concerns about global warming. A technology that could possibly contribute to reducing carbon dioxide emissions is the in-situ mineral sequestration (long term geological storage) or the ex-situ mineral sequestration (controlled industrial reactors) of CO2. In the present study, we propose to use coal combustion fly-ash, an industrial waste that contains about 4.1 wt.% of lime (CaO), to sequester carbon dioxide by aqueous carbonation. The carbonation reaction was carried out in two successive chemical reactions, first, the irreversible hydration of lime. CaO + H2O → Ca(OH)2 second, the spontaneous carbonation of calcium hydroxide suspension. Ca(OH)2 + CO2 → CaCO3 + H2O A significant CaO–CaCO3 chemical transformation (approximately 82% of carbonation efficiency) was estimated by pressure-mass balance after 2 h of reaction at 30 °C. In addition, the qualitative comparison of X-ray diffraction spectra for reactants and products revealed a complete CaO–CaCO3 conversion. The carbonation efficiency of CaO was independent on the initial pressure of CO2 (10, 20, 30 and 40 bar) and it was not significantly affected by reaction temperature (room temperature “20–25”, 30 and 60 °C) and by fly-ash dose (50, 100, 150 g). The kinetic data demonstrated that the initial rate of CO2 transfer was enhanced by carbonation process for our experiments. The precipitate calcium carbonate was characterized by isolated micrometric particles and micrometric agglomerates of calcite (SEM observations). Finally, the geochemical modelling using PHREEQC software indicated that the final solutions (i.e. after reaction) are supersaturated with respect to calcium carbonate (0.7 ≤ saturation index ≤ 1.1). This experimental study demonstrates that 1 ton of fly-ash could sequester up to 26 kg of CO2, i.e. 38.18 ton of fly-ash per ton of CO2 sequestered. This confirms the possibility to use this alkaline residue for CO2 mitigation.