Chemical-looping combustion (CLC) is considered to be a vital method for utilizing hydrocarbon fuel with low carbon emissions. A honeycomb fixed-bed reactor is a new kind of reactor for CLC. However, the further application of the reactor is limited by the inadequacy of the kinetic equations for CLC. In this paper, the experimental studies on the kinetic of Fe-based oxygen carriers were carried out by the CLC experiments using syngas which was obtained from one typical type of coal gasification products. The experimental results show that there were two individual stages for the kinetic characteristics during the fuel reaction process. Therefore, the CLC fuel reaction process could be described by a two-stage unreacted-core shrinking model and the reaction rate equations for each of the two phases were provided. In both stages, the dominant resistances were analyzed. The activation energy and the reaction order in both stages were calculated respectively as well. Comparing the experimental results of reaction rate with the calculated results of the obtained rate equations, it could be clearly seen that the reaction kinetics model was appropriate for the CLC in the honeycomb reactor. This work is expected to provide a guideline for the future development and industrial design of the honeycomb CLC reactors from the perspective of kinetics.
This is a preview of subscription content, log in to check access.
Buy single article
Instant unlimited access to the full article PDF.
Price includes VAT for USA
Global monitoring division ESRL GMD. Website: http://www.esrl.noaa.gov/gmd/news/pdfs/7074.pdf (accessed in 2013).
Monazam E.R., Breault R.W., Siriwardane R., Richards G., Carpenter S., Kinetics of the reduction of hematite (Fe2O3) by methane (CH4) during chemical looping combustion: A global mechanism. Chemical Engineering Journal, 2013, 232: 478–487.
Ishida M., Jin H.G., A new advanced power-generation system using chemical-looping combustion. Energy, 1994, 19: 415–422.
Lyngfelt A., Leckner B., Mattisson T., A fluidized-bed combustion process with inherent CO2 separation; application of chemical-looping combustion. Chemical Engineering Science, 2001, 56: 3101–3113.
Johansson E., Lyngfelt A., Mattisson T., Johnsson F., Gas leakage measurements in a cold model of an interconnected fluidized bed for chemical-looping combustion. Powder Technology, 2003, 134: 210–217.
Son S.R., Kim S.D., Chemical-looping combustion with NiO and Fe2O3 in a thermobalance and circulating fluidized bed reactor with double loops. Industrial & Engineering Chemistry Research, 2006, 45: 2689–2696.
Shen L.H., Wu J.H., Xiao J., Song Q.L., Xiao R., Chemical-looping combustion of biomass in a 10 kW(th) reactor with iron oxide as an oxygen carrier. Energy & Fuels, 2009, 23: 2498–2505.
Nandy A., Loha C., Gu S., Sarkar P., Karmakar M.K., Chatterjee P.K., Present status and overview of chemical looping combustion technology. Renewable & Sustainable Energy Reviews, 2016, 59: 597–619.
Jin H.G., Ishida M., Reactivity study on a novel hydrogen fueled chemical-looping combustion. International Journal of Hydrogen Energy, 2001, 26: 889–894.
Noorman S., Annaland M.V.S., Kuipers H., Packed bed reactor technology for chemical-looping combustion. Industrial & Engineering Chemistry Research, 2007, 46: 4212–4220.
Noorman S., Annaland M.V.S., Kuipers H., Experimental validation of packed bed chemical-looping combustion. Chemical Engineering Science, 2010, 65: 92–97.
Gallucci F.F., Hamers H.P., Van Zanten M., Annaland M.V.S., Experimental demonstration of chemical-looping combustion of syngas in packed bed reactors with ilmenite. Chemical Engineering Journal, 2015, 274: 156–168.
Kimball E., Hamers H.P., Cobden P.D., Gallucci F.F., Annaland M.V.S., Operation of fixed-bed chemical looping combustion. Energy Procedia, 2013, 37: 575–579.
Kimball E., Lambert A., Fossdal A., Leenman R., Comte E., Den Bos W.A.P.V., Blom R., Reactor choices for chemical looping combustion (CLC) dependencies on materials characteristics. Energy Procedia, 2013, 37: 567–574.
Xiao R., Song Q., Song M., Lu Z., Zhang S., Shen L., Pressurized chemical-looping combustion of coal with an iron ore-based oxygen carrier. Combustion and Flame, 2010, 157: 1140–1153.
Zhang Z., Yao J., Boot-Handford M., Fennell P., Pressurised chemical-looping combustion of an iron-based oxygen carrier: reduction kinetic measurements and modelling. Fuel Processing Technology, 2018, 171: 205–214.
Ishida M., Jin H., A novel combustor based on chemical-looping reactions and its reaction kinetics. Journal of Chemical Engineering of Japan, 1994, 27: 296–301.
Monazam E.R., Breault R.W., Tian H., Siriwardane R., Reaction kinetics of mixed CuO–Fe2O3 with methane as oxygen carriers for chemical looping combustion. Industrial & Engineering Chemistry Research, 2015, 54: 11966–11974.
Ishida M., Wen C.Y., Comparison of kinetic and diffusional models for solid-gas reactions. Aiche Journal, 1968, 14: 311–317.
Ishida M., Jin, H. G., Okamoto T., A Fundamental study of a new kind of medium material for chemical-looping combustion. Energy & Fuel, 1996, 10: 958–963.
Ryu H.J., Bae D.H., Han K.H., Lee S.Y., Jin G.T., Choi J.H., Oxidation and reduction characteristics of oxygen carrier particles and reaction kinetics by unreacted core model. Korean Journal of Chemical Engineering, 2001, 18: 831–837.
Abad A., García-Labiano F., de Diego L.F., Gayán P., Adánez J., Reduction kinetics of Cu-, Ni-, and Fe-based oxygen carriers using syngas (CO+H2) for chemical-looping combustion. Energy & Fuels, 2007, 21: 1843–1853.
Su M., Ma J., Tian X., Zhao H., Reduction kinetics of hematite as oxygen carrier in chemical looping combustion. Fuel Processing Technology, 2017, 155: 160–167.
Garcialabiano F., De Diego L.F., Adanez J., Abad A., Gayan P., Reduction and oxidation kinetics of a copper-based oxygen carrier prepared by impregnation for chemical-looping combustion. Industrial & Engineering Chemistry Research, 2004, 43: 8168–8177.
Sahir A.H., Lighty J.S., Sohn H.Y., Kinetics of copper oxidation in the air reactor of a chemical looping combustion system using the law of additive reaction times. Industrial & Engineering Chemistry Research, 2011, 50: 13330–13339.
Hossain M.M., Sedor K.E., de Lasa H.I., Co–Ni/Al2O3 oxygen carrier for fluidized bed chemical-looping combustion: desorption kinetics and metal-support interaction. Chemical Engineering Science, 2007, 62: 5464–5472.
Jin H., Ishida M., Reactivity study on natural-gas-fueled chemical-looping combustion by a fixed-bed reactor. Industrial & Engineering Chemistry Research, 2002; 41: 4004–4007.
Zhang H., Hong H., Jiang Q., Deng Y., Jin H., Kang Q., Development of a chemical-looping combustion reactor having porous honeycomb chamber and experimental validation by using NiO/NiAl2O4. Applied Energy, 2018, 211: 259–268.
Zhang H., Liu X., Hong H., Jin H., Characteristics of a 10 kW honeycomb reactor for natural gas fueled chemical-looping combustion. Applied Energy, 2018, 213: 285–292.
Jiao S., Study on working principle, performance and system of integrated gasification gas-steam combined cycle (IGCC). China Electric Power Press, Beijing, China, 2014. (in Chinese)
Zhao Z., Chen T., Ghoniem A.F., Rotary bed reactor for chemical-looping combustion with carbon capture. Part 2: base case and sensitivity analysis. Energy & Fuels, 2012, 27: 344–359.
Levenspiel O., Chemical reaction engineering. Industrial & Engineering Chemistry Research, 1999, 38: 4140–4143.
The authors gratefully acknowledge the support of the National Key Research and Development Program of China (No. 2016YFB0901401), and the Chinese Academy of Sciences Frontier Science Key Research Project (QYZDY-SSW-JSC036).
About this article
Cite this article
Liu, X., Zhang, H. & Hong, H. Reduction Kinetics of Fe-based Oxygen Carriers Using Syngas in a Honeycomb Fixed-Bed Reactor for Chemical-Looping Combustion. J. Therm. Sci. 29, 13–24 (2020) doi:10.1007/s11630-020-1255-9
- chemical-looping combustion
- honeycomb reactor
- reaction kinetics