To improve the CO2 fixation ability of dry desulfurization ash (DDA), a DDA must be modified by chemical methods. At the micron level, the changes in microstructure and chemical composition before and after DDA modification were analysed by Scanning Electron Microscope (SEM)
and Energy Dispersive Spectroscopy (EDS), and the reaction mechanism of the modification process was inferred. On the other hand, the chemical and mineral phase compositions of the modified DDA and its solid products were analysed by X ray Fluorescence (XRF) and X-ray diffraction (XRD). In
addition, the microstructure of the modified DDA before and after sequestration at nanometre resolution was studied by SEM-EDS so that the curing mechanism of the modified DDA was clearly defined. Then, the effects of the solid–liquid ratio, temperature, pressure and reaction time on
the sequestration of CO2 in the modified DDA were studied with aqueous carbonation. The results showed that the higher the temperature is, the higher the solid–liquid ratio, and the lower initial pressure is, the less the CO2 sequestered in the modified DDA and
the less the carbon sequestration capacity of the modified DDA. Under the experimental conditions, the carbonation efficiency of the modified DDA could reach 94.42%, and 1 ton of modified DDA could sequester up to 50.61 kg CO2. Compared with conventional DDA, the carbon sequestration
capacity is effectively improved. The kinetic data confirmed that the fitting correlation of the quasi-first-order kinetics equation is more significant. The smaller the solid–liquid ratio is, the lower the temperature, the higher the initial pressure, and the higher the rate constant
of the quasi-first-order kinetics equation.