Modelling Chemical-Looping assisted by Oxygen Uncoupling (CLaOU): Assessment of natural gas combustion with calcium manganite as oxygen carrier

Chemical-Looping Combustion (CLC) is a promising technology for performing CO₂ capture in combustion processes at low cost and with lower energy consumption. Fuel conversion modelling assists in optimizing and predicting the performance of the CLC process under different operating conditions. For this work, the combustion of natural gas was modelled using a CaMnO₃-type perovskite as oxygen-carrier and taking into consideration the processes of fluid dynamics and reaction kinetics involved in fuel conversion. The CLC model was validated against experimental results obtained from the 120?kW_th CLC unit at the Vienna University of Technology (TUV). Good agreement between experimental and model predictions of fuel conversion was found when the temperature, pressure drop, solids circulation rate and fuel flow were varied. Model predictions showed that oxygen transfer by means of the gas–solid reaction of the fuel with the oxygen-carrier was relevant throughout the entire fuel-reactor. However, complete combustion could be only achieved under operating conditions where the process of Chemical-Looping assisted by Oxygen Uncoupling (CLaOU) became dominant, i.e. a relevant fraction of the fuel was burnt with molecular oxygen (O₂) released by the oxygen-carrier. This phenomenon was improved by the design configuration of the 120?kW_th CLC unit at TUV, in which oxidized particles are recirculated to the upper part of the fuel-reactor. Thus, the validated model identified the conditions at which complete combustion can be achieved, demonstrating that it is a powerful tool for the simulation and optimization of the CLC process with the CaMnO₃-type material.