Furthermore it is demonstrated that the number of calcination carbonation cycles changes the sulphation patterns of the CaO from heterogeneous to homogeneous in all the limestones tested. For 50 carbonation calcination cycles and for particle sizes below 200 µm, the sulphation pattern is in all cases homogeneous. The sulphation rates were found to be first order with respect to SO 2 , and zero with respect to CO 2 . Steam was observed to have a positive effect only in the diffusion through the product layer controlled regime, as it leads to an improvement in the sulfation rates and effectiveness of the sorbent. Most of the experimental results of sulfation of highly cycled sorbents under all conditions can be fitted by means of the Random Pore Model (RPM) assuming that the kinetics and diffusion through the product layer of the CaSO 4 are the controlling regimes.