CaO-based pellets supported with aluminate cements show superior performance in carbonation/calcination cycles for high-temperature CO(2) capture. However, like other CaO-based sorbents, their CO(2) carrying activity is reduced after increasing numbers of cycles under high-temperature, high-CO(2) concentration conditions. In this work the feasibility of their reactivation by steam or water and remaking (reshaping) was investigated. The pellets, prepared from three limestones, Cadomin and Havelock (Canada) and Katowice (Poland, Upper Silesia), were tested in a thermogravimetric analyzer (TGA). The cycles were performed under realistic CO(2) capture conditions, which included calcination in 100% CO(2) at temperatures up to 950 degrees C. Typically, after 30 cycles, samples were hydrated for 5 min with saturated steam at 100 degrees C in a laboratory steam reactor (SR). Moreover, larger amounts of pellets were cycled in a tube furnace (TF), hydrated with water and reshaped, and tested to determine their CO(2) capture activity in the TGA. It was found that, after the hydration stage, pellets recovered their activity, and more interestingly, pellets that had experienced a longer series of cycles responded more favorably to reactivation. Moreover, it was found that conversion of pellets increased after about 70 cycles (23%), reaching 33% by about cycle 210, with no reactivation step. Scanning electron microscope (SEM) analyses showed that the morphology of the low-porosity shell formed at the pellet surface during cycles, which limits conversion, was eliminated after a short period (5 min) of steam hydration. The nitrogen physisorption analyses (BET, BJH) of reshaped spent pellets from cycles in the TF confirmed that sorbent surface area and pore size distribution were similar to those of the original pellets. The main alumina compound in remade pellets as determined by XRD was mayenite (Ca(12)Al(14)O(33)). These results showed that, with periodic hydration/remaking steps, pellets can be used for extended times in CO(2) looping cycles, regardless of capture/regeneration conditions. Crown Copyright (C) 2010 Published by Elsevier Ltd. All rights reserved.