Effect of Pelletization and Addition of Steam on the Cyclic Performance of Carbon-Templated, CaO-Based CO2 Sorbents

In this work, we report the development of a synthetic CO2 sorbent that possesses a high cyclic CO2 uptake capacity and, in addition, sufficient mechanical strength to allow it to be used in fluidized-bed reactors. To overcome the problem of elutriation of the original powdered material, the synthetic CO2 sorbent was pelletized. An important aspect of this work was to assess the effect of steam on the cyclic CO2 capture capacity of the original, powdered CO2 sorbent and the pelletized material. After 30 cycles of repeated calcination and carbonation reactions conducted in a fluidized bed, the CO2 uptake of the pellets was 0.29 g of CO2/g of sorbent, a value that is 45% higher than that measured for the reference limestone. For the case that carbonation/calcination cycles were conducted in a thermogravimetric analyzer under steam-free carbonation conditions, the CO2 uptake of the best sorbent was 0.33 g of CO2/g of sorbent (after 10 cycles). Importantly, it should be noted that, after 10 cycles using wet carbonation conditions, the CO2 uptake of this material increased by 55% when compared to dry conditions. This observation was attributed to enhanced solid-state diffusion in the CaCO3 product layer under wet conditions. However, independent of the reaction conditions, the pelletized material showed a lower cyclic CO2 uptake when compared to the original powder. A detailed morphological characterization of the pellets indicated that the destruction of the primary, hollow micrometer-sized spheres during pelletization was responsible for the lower cyclic CO2 uptake of the pellets.