Modeling of Natural Gas Steam Reforming Process in a Pd/Ag Membrane Reactor for Pure Hydrogen Production

Document Type : Research Article


Faculty of Chemical and Petroleum Engineering, Shiraz University, Shiraz, I.R. IRAN


Fuel cells will be one of the most important resources of energy in the future They use pure hydrogen, and natural gas as a feed. Converting chemical energy to electrical energy in fuel cells is a direct process without any environmental pollution. Thus the study and modeling of various hydrogen production and purification processes is necessary. Up to day, natural gas steam reforming is one of the most important chemical processes for hydrogen production. It should be mentioned that hydrogen is obtained from a produced synthesis gas (product of methane steam reforming process). A lot of researches have also done work on a direct production of pure hydrogen using various membranes. Previous studies have shown that using Pd-Ag membrane is only permeable for hydrogen is the best choice for pure hydrogen production. Thus, in the present study the modeling of natural gas steam reforming in the Pd-Ag membrane reactor has been done. Effect of some variables such as pressure, temperature, steam to methane ratio in the feed, membrane thickness and flow pattern of reactants and sweep gas on the methane conversion, hydrogen production and produced hydrogen-to-carbon monoxide ratio have been investigated and optimum operating conditions have been determined qualitatively. The proposed model has been evaluated by some data that obtained from an experimental study. The results of the proposed model have a good consistency with the results of experimental study.


Main Subjects

[1] Zhu J., Zhang D., King K.D., Reforming of CH4 by Partial Oxidation: Thermodynamic and Kinetic Analyses, Fuel, 80, p. 899 (2001).
[2] Mariana, M.V.M. Souza, M. Schmal, Autothermal Reforming of Methane over Pt/ZrO2/Al2O3 Catalysts, Applied Catalysis A: General, 281, p. 19 (2005).
[3] باقری، مهدی؛ فاطمی، شهره؛ تیراندازی، بهنام؛ غنی­یاری بنیس، سعید؛ بهینه سازی کوره و راکتور لوله­ای صنعتی فرایند ریفرمینگ گاز طبیعی با بخار با استفاده از الگوریتم ژنتیک، نشریه شیمی و مهندسی شیمی ایران، دوره 28، شماره 1 (1388).
[4] Oklany J.S., Hou K., Hughes R., A Simulative Comparison of Dense and Microporous Membrane Reactors for the Steam Reforming of Methane, Applied Catalysis A: General, 170, p. 13 (1998).
[5] Prokopiev S.I., Aristov Y.I., Parmon V.N., Giordano N., Intensification of Hydrogen Production via Methane Reforming and the Optimization of H2:CO Ratio in a Catalytic Reactor with a Hydrogen-Permeable Membrane Wall, International journal of Hydrogen Energy, 17, p. 17, 275 (1992).
[6] Lin Y.M., Liu S.L., Chuang C.H., Chu Y.T., Effect of Incipient Removal of Hydrogen Through Palladium Membrane on the Conversion of Methane Steam Reforming Experimental and Modelling, Catalysis Today, 82, p. 127 (2003).
[7] Siriwardane R.V., PostonJr J.A., Fisher E.P., Lee T.H., Dorris S.E., Balachandran U., Characterization of Ceramic Hydrogen Separation Membranes with Varying Nickel Concentrations, Applied Surface Science, 167, p. 34 (2000).
[8] Tong J., Matsumuta Y., “Effect of Catalytic Activity on Methane Steam Reforming in Hydrogen-Permeable Membrane Reactor, Applied Catalysis A: General, 286, p. 226 (2005).
[9] Yu W., Ohmori T., Kataoka S., Yamamoto T., Endo A., Nakaiwa M., Itoh N., Reforming in a Porous Ceramic Membrane Reactor Using Nitrogen and Steam as Sweep Gases, International Journal of Hydrogen Energy, 33, p. 685 (2008).
[10] Fernandes A.N.F., Soares Jr A.B., Methane Steam Reforming Modeling in a Palladium Membrane Reactor, Fuel, 85, p. 569 (2006).
[11] Barbieri G., Violante V., Maio F.P.D., Criscuoli A., Drioli E., Methane Steam Reforming Analysis in a Palladium-Based Catalytic Membrane Reactor, Industrial and Engineering Chemistry Research, 36, p. 3369 (1997).
[12] Madia G.S., Barbieri G., Drioli E., Theoretical and experimental Analysis of Methane Steam Reforming in a Membrane Reactor, Canadian journal of Chemical Engineering, 77, p. 698 (1999).
[13] Kikuchi E., Uemiya S., Matsuda T., Hydrogen Production from Methane Steam Reforming Assisted by use of Membrane Reactor, Studies in Surface Science and Catalysis, 61, p. 509 (1991).
[14] Oertel M., Schmitz J., Weirich W., Jendryssek-Neumann D., Schulten R., Steam Reforming of Natural Gas with Integrated Hydrogen Separation for Hydrogen Production, Chemical Engineering and Technology. 10, p. 248 (1987).
[15] S. Uemiya, Y. Kude, K. Sugino, N. Sato, T.Matsuda, E. Kikuchi, A Palladium/Porous Glass Composite Membrane forHydrogen Separation, Chemistry Letters, 17, p. 687 (1988).
[16] Uemiya S., Sato N., Ando H., Kude Y., Matsuda T., Kikuchi E., Separation ofHydrogen Through Palladium ThinFilm Supported on a Porous Glass Tube, Journal of Membrane Science, 56, p. 303 (1991).
[17] J. Shu, B.P.A. Grandjean, S. Kaliaguine, Methane SteamReforming in Asymmetric Pd- and Pd-Ag/Porous SS Membrane Reactors, Applied Catalysis A: General, 119, p. 305 (1994).
[18] Shu J., Grandjean B.P.A., Kaliaguine S., Aymmetric Pd-Ag/ Stainless Catalytic Membranes for Methane Steam Reforming, Catalysis Today, 25, p. 327 (1995).
[19] S.W. Nam, S.P. Yoon, H.Y. Ha, S.A. Hong, A.P., Maganyuk, Methane Steam Reforming in a Pd-Ru Membrane Reactor, Korean Journal of Chemical Engineering, 17, p. 288 (2000).
[20] Tong J., Matsumura Y., Suda H., Haraya K., Experimental Study of Steam Reforming of Methane in a Thin (6 µM) Pd-Based Membrane Reactor, Industrial and Engineering Chemistry Research, 44, p. 1454 (2005).
[21] Gallucci F., Paturzo L., Fam A., Basile A., Experimental Study of the Methane Steam Reforming Reaction in a Dense Pd/Ag Membrane Reactor, Industrial and Engineering Chemistry Research, 43, p. 928 (2004).
[22] Gallucci F., Comite A., Capannelli G., A Steam Reforming of Methane in a Membrane Reactor: An Industrial Case Study, Industrial and Engineering Chemistry Research, 45, p. 2994 (2006).
[23] Gallucci F., Paturzo, L., Basile A., A Simulation Study of the Steam Reforming of Methane in a Dense Tubular Membrane Reactor, International Journal of Hydrogen Energy, 29, p. 611 (2004).
[24] Assaf E.M., Jesus C.D.F., Assaf J.M., Mathematical Modelling of Methane Steam Reforming in a Membrane Reactor: an Isothermic Model, Brazilian Journal of Chemical Engineering, 15, p. 160 (1998).
[25] Hoang D.L., Chan S.H., Ding O.L., Kinetic and Modelling Study of Methane Steam Reforming overSulfide Nickel Catalyst on a Gamma Alumina Support, Chemical Engineering Journal, 112, p. 1 (2005).
[26] Hacarlioglu P., Gu Y., Oyama S.T., Studies of the Methane Steam Reforming Reaction at HighPressure in a Ceramic Membrane Reactor, Journal of Natural Gas Chemistry, 15, p. 73 (2006).
[27] Xu J., Froment G.F., Methane Steam Reforming Methanation and Water-Gas Shift: I. Intrinsic Kinetics, AIChE Journal, 35, p. 88 (1989).
[28] A. Stephan, Birdsell, R.S. Willms, Modeling and data Analysis of a Palladium Membrane Reactor for Tritiated Impurities Cleanup, Fusion Technology Journal, 28, p. 530 (1995).
[29] Adris A.M., Elnashaie S.S.E.H., Hughes R., A Fluidized Bed Membrane Reactor for the Steam Reforming of Methane, Canadian Journal of Chemical Engineering, 69, p. 1061 (1991).