High-temperature CO2 capture using a Ca/AI carbonate sorbent, made of Ca-Al-CO3 powder and a TiO2 binder, was studied. Calcium aluminates were synthesized by the coprecipitation of Ca2+, Al3+, and CO32- under alkaline conditions. The results showed that TiO2 nanoparticles significantly improved surface area and cyclic 'stability of sorbents in thermogravimetric analysis (TGA) and reactor. Six types of Ca / Ti pellets were prepared, using a Ca-Al-CO3/TiO2 weight ratio of 1-6:1. These granules gave a very stable CO2 uptake, to 80% of their full capacity, for 10 cycles, compared to only 35% using Ca-Al-CO3. A possible reaction scheme for stabilizing the CaO microstructure for multi-cycle experiments is described. Crown Copyright (C) 2013 Published by Elsevier B.V. All rights reserved.