Chemical looping of synthetic ilmenite. Part II: Multiscale perspective on modeling CLC and CLH

Abstract

This work investigates the chemical looping combustion (CLC) and chemical looping hydrogen (CLH) production processes of synthetic ilmenite at three relevant length scales: reactor, particle and reaction. Focusing on reduction with hydrogen, part I analyzed the reaction scale for CLC using thermogravimetric analysis (TGA). Complementary fixed bed reactor experiments for reduction and oxidation using pellets (CLC, CLH) and TGA experiments using powders or pellets (CLH) were now added. All measurements were used to develop a consistent multiscale model. Particle and reactor scales were described by one-dimensional volumetric models. The required complexity of the reaction model differed from case to case. Kinetic modeling for oxidations in the reactor was trivial, since gaseous reactants were fully consumed. Reductions with hydrogen, however, were more intricate. Considering the influence of equilibrium on the reactivity was crucial for CLH. The reduction for CLC was faster and even more complex. We novelly demonstrated how kinetics, originally derived only from TGA with powders, were not directly applicable to larger scales when underlying phenomena had been neglected. In order to overcome these limitations and achieve better consistency, equilibrium effects and the gas availability above the sample during TGA had to be considered. The suitability of the synthetic ilmenite for CLC and CLH was discussed based on the findings in this work.