Modifications and pelletization of limestone were investigated in order to improve the utilization of CaO-based materials for different catalytic reactions and environmental applications. Attempts to purify the limestone by ion-exchange with CaCl2 solution did not result in significant removal of impurities. On the other hand, acetification with 10 vol.% acetic acid enhanced pore surface area and pore volume of the sorbent by 42% and 3-fold, respectively. The acetification was found to widen small pores, and thus create a beneficial pore size distribution with more pores in the range of 25-100 nm. In order to utilize such powdered materials in fluidized beds, pelletization is the next step. Unfortunately, pelletization results suggested that natural kaolin is an unsuitable binder for preparing CaO-based pellets due to its negative impact on pellet morphology. By contrast, Al(OH)(3) binder obtained from kaolin leaching had a strong positive effect on the porous texture of the pellets, demonstrated by pore surface area and volume of 22.48 m(2) g(-1) and 0.051 cm(3) g(-1) for 1 mm pellets with CaO/binder ratio of 5.5, compared to 10.92 m(2) g(-1) and 0.039 cm(3) g(-1) for natural materials. The enhancement in pellet morphology is mainly attributed to transformation of Al(OH)(3) to the highly porous Al2O3 at high temperatures. Pellets synthesized from limestone modified with 10 vol.% acetic acid with Al(OH)(3) binder (ratio of 5.5) exhibited high pore surface area and volume, represented by 1.3-fold and 44% increase over those for natural limestone. It was concluded that the combination of acetified limestone with Al(OH)(3) binder is a promising approach for synthesis of CaO-based pellets with enhanced morphology. (C) 2012 Elsevier B.V. All rights reserved.