Relevant influence of limestone crystallinity on CO₂ capture in the Ca-looping technology at realistic calcination...

We analyze the role of limestone crystallinity on its CO2 capture performance when subjected to carbonation/calcination cycles at conditions mimicking the Ca-looping (CaL) technology for postcombustion CO2 capture. The behavior of raw and pretreated limestones (milled and thermally annealed) is investigated by means of thermogravimetric analysis (TGA) tests under realistic sorbent regeneration conditions, which necessarily involve high CO2 partial pressure in the calciner and quick heating rates. The pretreatments applied lead to contrasting effects on the solid crystal structure and, therefore, on its resistance to solid-state diffusion. Our results show that decarbonation at high CO2 partial pressure is notably promoted by decreasing solid crystallinity. CaO regeneration is fully achieved under high CO2 partial pressure at 900 °C in short residence times for the milled limestone whereas complete regeneration for raw limestone requires a minimum calcination temperature of about 950 °C. Such a reduction of the calcination temperature and the consequent mitigation of multicyclic capture capacity decay would serve to enhance the efficiency of the CaL technology. On the other hand, the results of our study suggest that the use of highly crystalline limestones would be detrimental since excessively high calcination temperatures should be required to attain full decarbonation at realistic conditions.