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Licensed Unlicensed Requires Authentication Published by De Gruyter December 6, 2018

Development of Fast Solving Monolith Reactor Simulators: Computational Fluid Dynamics Studies of Methane Oxidation

Mopeli Khama, Randhir Rawatlal and Glenn Jones


The optimisation of complex geometries such as that of monolith reactors can be supported by computation and simulation. However, complex boundaries such as those found in multi-channel monoliths where mass and heat transfer of characteristic of the reaction diffusion equation render such simulations of extremely high computational expense. In the first step toward developing a fast-solving hybrid simulation, a detailed CFD simulation was used to obtain the unsteady state, spatial temperature and concentration (and hence reaction rate) profiles for a range of input conditions. The results of the CFD simulation were then accepted as the benchmark to which faster-solving models were measured against to be considered as viable descriptions. The model evaluated here is a modified plug flow with effectiveness factor correction for wall mass-transfer. A close agreement between both temperature and species mole fraction profiles predicted from the modified plug flow model and a detailed CFD model was found with R2 values of 0.994 for temperature. The time needed to find a converged solution for plug flow model on an Intel(R) Core(TM) i5-5300U CPU @ 2.30 GHz workstation was found to be 53 seconds in comparison to 1.3 hours taken by a CFD model.


The authors are grateful to thank Johnson Matthey for financial support.



Surface area


Specific heat


diffusion coefficient


acceleration due to gravity


Mass specific enthalpy


Identity tensor


heat released by the heterogeneous reaction


Reaction rate




Surface Temperature


velocity vector


Mass fraction






Greek letters


Site fraction




Site density


Dynamic viscosity


Thermal conductivity


maximum temperature difference


Arrhenius number


[1] Chisti Y. Biodiesel from microalgae. Biotechnol Adv. 2007;25:294–306.10.1016/j.biotechadv.2007.02.001Search in Google Scholar PubMed

[2] Corbo P, Migliardini F. Hydrogen production by catalytic partial oxidation of methane and propane on Ni and Pt catalysts. Int J Hydrogen Energy. 2007;32:55–66.10.1016/j.ijhydene.2006.06.032Search in Google Scholar

[3] Verlato E, Cimino S, Lisi L, Mancino G, Musiani M, Va L Catalytic partial oxidation of CH4 – H2 mixtures over Ni foams modified with Rh and Pt. 2012:7.10.1016/j.ijhydene.2012.08.022Search in Google Scholar

[4] Pino L, Recupero V, Beninati S, Kumar A, Subraya M, Bera P. Catalytic partial-oxidation of methane on a ceria-supported platinum catalyst for application in fuel cell electric vehicles. Applied Catalysis A: General. 2002;225:63–7510.1016/S0926-860X(01)00734-7Search in Google Scholar

[5] Larentis AL, De Resende NS, Salim VM, Pinto JC. Modeling and optimization of the combined carbon dioxide reforming and partial oxidation of natural gas. Appl Catal A Gen. 2001;215:211–24.10.1016/S0926-860X(01)00533-6Search in Google Scholar

[6] Rafiq MH, Jakobsen HA, Hustad JE. Modeling and simulation of catalytic partial oxidation of methane to synthesis gas by using a plasma-assisted gliding arc reactor. Fuel Process Technol. 2012;101:44–57.10.1016/j.fuproc.2011.12.044Search in Google Scholar

[7] Arutyunov VS, Krylov OV. Oxidative conversion of methane. Russ Chem Rev. 2007;74:1111–37.10.1070/RC2005v074n12ABEH001199Search in Google Scholar

[8] Deutschmann O, Schmidt LD. Modeling the partial oxidation of methane in a short‐contact‐time reactor. AIChE J. [Internet]. 1998;44:2465–77. Available at: in Google Scholar

[9] Bizzi M, Basini L, Saracco G, Specchia V. Short contact time catalytic partial oxidation of methane : analysis of transport phenomena effects. Chemical Engineering Journal. 2002;90:97–10610.1016/S1385-8947(02)00071-2Search in Google Scholar

[10] Bizzi M, Saracco G. Modeling the partial oxidation of methane in a fixed bed with detailed chemistry. AIChE Journal. 2004;50:1289–9910.1002/aic.10118Search in Google Scholar

[11] Quiceno R, Pérez-Ramírez J, Warnatz J, Deutschmann O Modeling the high-temperature catalytic partial oxidation of methane over platinum gauze: detailed gas-phase and surface chemistries coupled with 3D flow field simulations. Appl Catal A Gen. 2006;303:166–76.10.1016/j.apcata.2006.01.041Search in Google Scholar

[12] Zamaniyan A, Behroozsarand A, Mehdizadeh H, Ghadirian HA. Modeling of microreactor for syngas production by catalytic partial oxidation of methane. J Nat Gas Chem. [Internet]. CAS/DICP; 2010;19:660–8. Available at: in Google Scholar

[13] IndiaMART. Ceramic honeycomb, usage: industrial use [Internet]. 2009 Available at: Accessed: 2 Aug 2018.Search in Google Scholar

[14] Deutschmann O, Schwiedemoch R, Maier LI, Chatterjee D. Natural gas conversion in monolithic catalysts: interaction of chemical reactions and transport phenomena. 2001:251–8. Available at: in Google Scholar

[15] Mladenov N, Koop J, Tischer S, Deutschmann O. Modeling of transport and chemistry in channel flows of automotive catalytic converters. Chem Eng Sci. 2010;65:812–26.10.1016/j.ces.2009.09.034Search in Google Scholar

[16] Rebughini S, Cuoci A, Dixon AG, Maestri M. Cell agglomeration algorithm for coupling microkinetic modeling and steady-state CFD simulations of catalytic reactors. Comput Chem Eng. [Internet]. Elsevier Ltd; 2017;97:175–82. Available at: in Google Scholar

[17] Chaniotis AK, Poulikakos D. Modeling and optimization of catalytic partial oxidation methane reforming for fuel cells. J Power Sources. 2005;142:184–93.10.1016/j.jpowsour.2004.10.018Search in Google Scholar

[18] Stutz MJ, Poulikakos D. Optimum washcoat thickness of a monolith reactor for syngas production by partial oxidation of methane. Chemical Engineering Science. 2008;63:1761–7010.1016/j.ces.2007.11.032Search in Google Scholar

[19] Huang H, Zhou X, Liu H. A CFD model for partial oxidation of methane over self-sustained electrochemical promotion catalyst. Int J Hydrogen Energy. 2016;41:208–18.10.1016/j.ijhydene.2015.11.091Search in Google Scholar

[20] Korup O, Goldsmith CF, Weinberg G, Geske M, Kandemir T, Schlögl R, et al. Catalytic partial oxidation of methane on platinum investigated by spatial reactor profiles, spatially resolved spectroscopy, and microkinetic modeling. J Catal. [Internet]. Elsevier Inc.; 2013;297:1–16. Available at: in Google Scholar

[21] Schwiedernoch R, Tischer S, Correa C, Deutschmann O. Experimental and numerical study on the transient behavior of partial oxidation of methane in a catalytic monolith. Chem Eng Sci. 2003;58:633–42.10.1016/S0009-2509(02)00589-4Search in Google Scholar

[22] Maffei T, Rebughini S, Gentile G, Lipp S, Cuoci A, Maestri M. CFD analysis of the channel shape effect in monolith catalysts for the CH 4 partial oxidation on Rh. Chemie-Ingenieur-Technik. 2014;86:1099–106.10.1002/cite.201400013Search in Google Scholar

[23] Pawlowski S, Nayak N, Meireles M, Velizarov S, Crespo JG. CFD modelling of fl ow patterns, tortuosity and residence time distribution in monolithic porous columns reconstructed from X-ray tomography data. Chem Eng J. [Internet]. Elsevier; 2018;350:757–66. Available at: in Google Scholar

[24] Iwaniszyn M, Piątek M, Gancarczyk A, Jodłowski PJ, Łojewska J, Kołodziej A Flow resistance and heat transfer in short channels of metallic monoliths: experiments versus CFD. Int J Heat Mass Transf. 2017;109:778–85.10.1016/j.ijheatmasstransfer.2017.02.019Search in Google Scholar

[25] Inbamrung P, Sornchamni T, Prapainainar C, Tungkamani S, Narataruksa P, Jovanovic GN. Modeling of a square channel monolith reactor for methane steam reforming. Energy. [Internet]. Elsevier Ltd; 2018;152:383–400. Available at: in Google Scholar

[26] Cui X, Kær SK. Two-dimensional thermal analysis of radial heat transfer of monoliths in small-scale steam methane reforming. Int J Hydrogen Energy. 2018;43:11952–68.10.1016/j.ijhydene.2018.04.142Search in Google Scholar

[27] Sadeghi F, Tirandazi B, Khalili-Garakani A, Nasseri S, Nabizadeh Nodehi R, Mostoufi N. Investigating the effect of channel geometry on selective catalytic reduction of NOxin monolith reactors. Chem Eng Res Des. [Internet]. Institution of Chemical Engineers; 2017;118:21–30. Available at: in Google Scholar

[28] Liu H, Zhao J, Li C, Ji S. Conceptual design and CFD simulation of a novel metal-based monolith reactor with enhanced mass transfer. Catal Today. 2005;105:401–6.10.1016/j.cattod.2005.06.060Search in Google Scholar

[29] Irani M, Alizadehdakhel A, Pour AN, Hoseini N, Adinehnia M. CFD modeling of hydrogen production using steam reforming of methane in monolith reactors: surface or volume-base reaction model? Int J Hydrogen Energy. [Internet]. Elsevier Ltd; 2011;36:15602–10. Available at: in Google Scholar

[30] Nogare DD, Degenstein NJ, Horn R, Canu P, Schmidt LD. Modeling spatially resolved data of methane catalytic partial oxidation on Rh foam catalyst at different inlet compositions and flowrates. J Catal. [Internet]. Elsevier Inc.; 2011;277:134–48. Available at: in Google Scholar

[31] Zhao LJ, Sun Q. Calculations of effectiveness factors and the criteria of mass transfer effect for hightemperature methanation (HTM) catalyst. Int J Low-Carbon Technol. 2013;10:288–93.10.1093/ijlct/ctu005Search in Google Scholar

[32] Fogler HS. Elements of chemical reaction engineering, 4th ed. Massachusetts: Pearson Education, Inc, 2006:1–1088.Search in Google Scholar

[33] Nugroho G, Ali AM, Abdul Karim ZA. On a special class of analytical solutions to the three-dimensional incompressible Navier-Stokes equations. Appl Math Lett. 2009;22:11.10.1016/j.aml.2009.05.010Search in Google Scholar

[34] Maestri M, Cuoci A. Coupling CFD with detailed microkinetic modeling in heterogeneous catalysis. Chem Eng Sci. [Internet]. Elsevier; 2013;96:106–17. Available at: in Google Scholar

[35] Ren Z, Pope SB. Second-order splitting schemes for a class of reactive systems. Journal of Computational Physics. 2008;227:8165–7610.1016/ in Google Scholar

[36] Takahashi M. Generalization of mean-field approximations by the Feynman inequality and application to long-range ising chain. J Phys Soc Jpn. 1981;50:1854–60.10.1143/JPSJ.50.1854Search in Google Scholar

[37] Onuchc N, Socc ND, Design F, Kortemme T, Pro LB. Atomic and macroscopic reaction rates of a surface-catalyzed reaction. Science. 1997;278:1931–410.1126/science.278.5345.1931Search in Google Scholar PubMed

[38] Janardhanan VM, Deutschmann O. Computational fluid dynamics of catalytic reactors. [Internet]. WILEY-VCH Verlag GmbH & Co. KGaA; Weinheim; 2011 Available at: Accessed: 15 May 2018.10.1002/9783527639878.ch8Search in Google Scholar

[39] Shaughnessy BO, Vavylonis D. Interfacial reaction kinetics. Phys J E. 2000;177:159–77.Search in Google Scholar

[40] Kunz L, Maier L, Tischer S, Deutschmann O. Modeling the rate of heterogeneous reactions. Model Simul Heterog Catal React. 2011;113–48.10.1002/9783527639878.ch4Search in Google Scholar

[41] Ferraris GB, Manca D. BzzOde: a new C++ class for the solution of stiff and non-stiff ordinary differential equation systems. Comput Chem Eng. 1998;22:1595–621.10.1016/S0098-1354(98)00233-6Search in Google Scholar

[42] Dudukovic MP, Felder RM. Mixing effects in chemical reactors - III-dispersion model. Reactor stability, sensitivity and mixing effects (module E4.7). AIChE Modular Instruction. 1983;4:39–49.Search in Google Scholar

[43] Herz RK. Notes on reaction-diffusion cases with effectiveness factors greater than one!. Chem Ser. [Internet]. 1975;143:116–32. Available at: Accessed: 16 May 2018.Search in Google Scholar

[44] Donazzi A, Beretta A, Groppi G, Forzatti P. Catalytic partial oxidation of methane over a 4 % Rh/??-Al2O3 catalyst. part I: kinetic study in annular reactor. J Catal. 2008;255:241–58.10.1016/j.jcat.2008.02.009Search in Google Scholar

Received: 2018-08-04
Revised: 2018-11-01
Accepted: 2018-11-03
Published Online: 2018-12-06

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