Study and Improvement of the Regeneration of Metallic Oxides Used as Oxygen Carriers for a New Combustion Process

Abstract

A new combustion process called chemical-looping combustion, has been suggested as an energetically efficient method for separation and capture of the carbon dioxide, generated by the combustion of fossil's fuels. This process consists of a reversible combustion, based on successive fuel oxidation via the reduction of metallic oxide followed by its regeneration by air oxidation. The generated products are: the reduced oxygen carrier, which is regenerated in a second reactor by air and recycled, and a flue gas, mainly composed of CO2 and H2O, which could be separated by condensation.In chemical-looping combustion process, it is important that the metallic oxide, used as an oxygen carrier, has a high reactivity with the fuel and good regeneration ability. It should have also good mechanical characteristics, in order to avoid its attrition and agglomeration during the successive cyclic reactions.In this work, the reactivity study of various oxygen carriers was carried out, during ten successive oxidation and reduction cycles, using a thermal gravimetrical analysis apparatus. From the results obtained, two types of oxygen carriers were identified: very reactive oxygen carriers, with a decreasing of their reactivity during the successive cycles of reduction and oxidation, and oxygen carriers with low and constant reactivity during the successive cycles.In order to improve the capacity of regeneration of the reactive oxygen carrier, several mixtures were prepared by adding stable and non-reactive metallic oxide, which acts as binder or doping agent by the mechanical properties of the mixed oxygen carrier improvement.The results obtained showed that, for all mixtures prepared and tested, the addition of binders to the reactive metallic oxides improve their regeneration ability. The best results, concerning the reactivity and the regeneration performances, were obtained with Fe2O3 mixed with CaO, TiO2 or MgO, followed by NiO mixed with CaO or TiO2 and finally CuO mixed with TiO2 or MgO.