Evaluation of Ni,Ce,Zn and Cu modified Fe2 O3/Al2 O3 oxygen carriers for methane-fueled chemical looping hydrogen generation process
Methane-fueled chemical looping hydrogen generation is an efficient hydrogen production technology coupled with CO2 capture.On the basis of Fe2O3/Al2O3 oxygen carrier,Ni,Ce,Zn and Cu were added to form bimetallic oxygen carriers by impregnation method to improve the oxygen transfer performance,hydrogen production performance and carbon deposition resistance.Through thermodynamic calculation,material characterization and experimental study,the reaction properties of different bimetallic oxygen carriers in reduction stage and hydrogen production stage were studied,and the structure-activity relationship between crystal phase structure,reaction activity and hydrogen production performance of different bimetallic oxygen carriers was obtained.The stability of the cyclic reaction was further studied for the optimal oxygen carrier.Studies showed that Cu was the most suitable metal additive.CuFe2O4,a spinel phase with stable structure,was formed in Cu-modified Fe2O3/Al2O3 oxygen carriers,improving lattice oxygen activity,promoting the deep reduction of Fe2O3,and effectively inhibiting carbon deposition.The yield of hydrogen increased from 245mmol/100g oxygen carriers to 288mmol/100g oxygen carriers,and the purity of hydrogen increased from 88.3%to 95.7%.The migration of Fe3+and Cu2+ions improved the microstructure and cyclic reaction performance.The feasibility of bimetallic oxygen carriers in methane-fueled chemical looping hydrogen generation was verified.The results provided theoretical and experimental basis for the design and screening of iron-based oxygen carriers.
chemical looping hydrogen generationoxygen carriermetal additivesoxygen transportcarbon deposition