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The increasing use of energy resources recovered from subsurface environments and the resulting carbon imbalance in the environment has motivated the need to develop thermodynamically downhill pathways to convert and store CO2 as water-insoluble calcium or magnesium carbonates. While previous studies extensively explored aqueous routes to produce calcium and magnesium carbonates from CO2, there is limited scientific understanding of the phase evolution and textural changes during the direct gas–solid conversion routes to produce calcium carbonate from calcium hydroxide, which is one of the abundant constituents of alkaline industrial residues. With increasing interest in developing integrated pathways for capturing, converting, and storing CO2 from dilute flue gases, understanding the composition of product phases as they evolve is essential for evaluating the efficacy of a given processing route. Therefore, in this study, we investigate the phase evolution and the corresponding textural changes as calcium hydroxide is converted to calcium carbonate under the continuous flow of CO2 at an ambient pressure of 1 atm with continuous heating from 30 °C to 500 °C using in-operando wide angle X-ray scattering (WAXS), small angle X-ray scattering (SAXS), and ultrasmall angle X-ray scattering (USAXS) measurements.

Phase Evolution and Textural Changes during the Direct Conversion and Storage of CO2 to Produce Calcium Carbonate from Calcium Hydroxide