Aqueous mineral carbonation of serpentinite on a pilot scale: The effect of liquid recirculation on CO2 sequestration and carbonate precipitation

• CO2 sequestration experiments were conducted using direct flue gas provided by a cement plant.
• The carbonates were precipitated under nesquehonite form (MgCO3·3H2O) at the temperature range of 32–40 °C.
• The liquid recirculation effect on the CO2 dissolution and carbonates precipitation was studied.

Following the promising results obtained on the laboratory scale, an aqueous mineral carbonation process was tested under industrial conditions as part of a pilot project conducted in a cement plant in Quebec. Experiments were conducted using a Parr 18.7 L reactor with cement plant flue gas (14–18 vol.%CO2) and serpentinite tailings as a source of magnesium. The gas was not concentrated or separated before use. The reactions occurred at a solid/liquid ratio of 150 g/L, 22 ± 3 °C and a total pressure between 2 and 10 bar. To decrease water consumption, the effect of liquid recirculation on the rates of CO2 sequestration, Mg leaching and carbonate precipitation were studied. The solid reacted with 6 successive batches of gas (15 min each), and the liquid was recovered for the carbonate precipitation after every two batches. For the recirculation assays, after carbonate filtration, the liquid was reused with subsequent batches.The results showed that the dissolution of CO2 was not affected by the liquid recirculation since 72.5% of the CO2 introduced was dissolved; in comparison to 77% when fresh liquid was used. The captured CO2 resulted in 0.215 and 0.211 g CO2/g of residue in the experiments with and without liquid recirculation, respectively. This result corresponds to approximately 45% of serpentinite's total capacity for CO2 sequestration, which is 0.47 g CO2/g of residue. The carbonate precipitation experiments were conducted in a separate system at low temperatures (32–40 °C) and included 2 h of stirring. When the liquid was recirculated, supersaturation was reached more quickly because of the accumulation of Mg2+ and HCO3−/CO2−3 ions. Therefore, the rate of precipitation and the amount of carbonate formed were significantly more important when the liquid was recirculated. However, the overall efficiency corresponding to the captured CO2 under carbonate form does not exceed 9% even with liquid recirculation.