Combined Oxides of Iron, Manganese and Silica as Oxygen Carriers for Chemical-Looping Combustion

Spray-dried particles with the chemical compositions of Fe0.66Mn1.33SiO3 and FeMnSiO3 have been examined as oxygen carrier materials for chemical-looping combustion. The performance of the materials was examined in oxygen release experiments and during fuel operation with natural gas and syngas. The experiments were carried out in a fluidized-bed chemical-looping reactor system designed for a thermal power of 300 W. The reactor system includes an air reactor and a fuel reactor, as well as loop seals and means for circulation of the oxygen carrier particles. Both materials were able to release gas phase oxygen in inert atmosphere at temperatures between 800-950°C, and with approximately equal oxygen concentrations. Fe0.66Mn1.33SiO3 provided higher conversion of natural gas as compared to FeMnSiO3 and the fuel conversion increased with temperature for both materials. During natural gas operation with Fe0.66Mn1.33SiO3 the conversion reached 100% at around 950°C with a fuel reactor inventory of 235 kg/MW. The fuel conversion was improved when the solids inventory was increased; this improvement could especially be observed for FeMnSiO3 as the fuel conversion was lower for this material. Fe0.66Mn1.33SiO3 provided higher fuel conversion than FeMnSiO3 also when syngas was used as fuel. The fuel conversion increased with temperature for both materials and full conversion was reached above 800°C with a fuel reactor inventory of 225 kg/MW for Fe0.66Mn1.33SiO3, while FeMnSiO3 was incapable of providing full conversion. A rather large elutriation of fines and a significant change in particle size distribution could be observed during operation for both materials. Both materials could work as oxygen carrier for chemical-looping with oxygen uncoupling. Fe0.66Mn1.33SiO3 would be preferred as it has higher conversion of both syngas and natural gas, but the attrition behavior of the material would need to be further investigated.