Carbonation of lignite fly ash at ambient T and P in a semi-dry reaction system for CO2 sequestration

Abstract

Abstract The global rise in atmospheric greenhouse gas concentrations calls for practicable solutions to capture CO2. In this study, a mineral carbonation process was applied in which CO2 reacts with alkaline lignite ash and forms stable carbonate solids. In comparison to previous studies, the assays were conducted at low temperatures and pressures and under semi-dry reaction conditions in an 8 L laboratory mixing device. In order to find optimum process conditions the pCO2 (10–20%), stirring rate (500–3000 rpm) and the liquid to solid ratio (L/S = 0.03–0.36 L kg−1) were varied. In all experiments a considerable CO2 uptake from the gas phase was observed. Concurrently the solid phase contents of Ca and Mg (hydr)oxides decreased and CaCO3 and MgCO3 fractions increased throughout the experiments, showing that CO2 was stabilized as a solid carbonate. The carbonation reaction depends on three factors: Dissolution of CO2 in the liquid phase, mobilization of Ca and Mg from the mineral surface and precipitation of the carbonate solids. Those limitations were found to depend strongly on the variation of the process parameters. Optimum reaction conditions could be found for L/S ratios between 0.12 and 0.18, medium stirring velocities and pCO2 between 10% and 20%. Maximum CO2 uptake by the solid phase was 4.8 mmol g−1 after 120 min, corresponding to a carbonation efficiency for the alkaline material of 53% of the theoretical CO2 binding capacity. In comparison to previous studies both CO2 uptake and carbonation efficiencies were in a similar range, but the reaction times in the semi-dry process were considerably shorter. The proposed method additionally allows for a more simple carbonation setup due to low T and P, and produces an easier to handle product with low water content.