Carbonation and calcination looping cycles were carried out on four limestones in a thermogravimetric analyzer (TGA). The CO2 carrying capacity of a limestone particle decays very quickly in the first 10 cycles, reducing to about 20% of its original uptake capacity after 10 cycles for the four limestones studied in this work, and it decreases further to 6-12% after 50 cycles. A new steam reactivation method was applied on the spent sorbent to recover the loss of reactivity. The steam reactivation of multi-cycled samples was conducted at atmospheric pressure. Steam reactivation for 5 min at 130 °C of particles that had undergone 10 cycles resulted in an immediate increase (by 45-60% points) in carrying capacity. The morphological changes of limestone particles during the cycling and steam reactivation were studied using both an optical microscope and scanning electron microscopy (SEM). The diameters of limestone particles shrank by about 2-7% after 10 carbonation/calcination cycles, and the particle diameters swelled significantly (12-22% increase) after steam reactivation. These size changes are important for studies of attrition and mathematical modeling of carbonation. © 2010 American Chemical Society.