Aspects of kinetic modeling of fixed bed reactors

This paper briefly reviews the most important aspects of catalyst testing in packed-bed catalytic laboratory reactors to properly assess the intrinsic chemical kinetics. Next it discusses approaches to assess the kinetics of fast reactions or those accompanied with strong heat effects that cannot be performed in a packed-bed reactor configuration free from transport limitations. As an example the partial oxidation of methane is presented in a steady-state fixed bed reactor as well as in a TAP (temporal analysis of products) reactor. The continuing increase in computational power leads to more sophisticated reaction and reactor models due to the increasing use of computational chemistry and computational fluid dynamics in reaction engineering.

[1]  Anthony G. Dixon,et al.  Packed Tubular Reactor Modeling and Catalyst Design using Computational Fluid Dynamics , 2006 .

[2]  S. Churchill,et al.  A Correlating Equation for Forced Convection From Gases and Liquids to a Circular Cylinder in Crossflow , 1977 .

[3]  Gerhard Emig,et al.  Kinetic Modeling of the Heterogeneously Catalyzed Oxidation of Propene to Acrolein in a Catalytic Wall Reactor , 2003 .

[4]  Dale F. Rudd,et al.  The Microkinetics of heterogeneous catalysis , 1993 .

[5]  G. Germani,et al.  Platinum/ceria/alumina catalysts on microstructures for carbon monoxide conversion , 2005 .

[6]  Y. Schuurman,et al.  Unraveling mechanistic features for the methane reforming by carbon dioxide over different metals and supports by TAP experiments , 1998 .

[7]  G. Froment,et al.  Chemical Reactor Analysis and Design , 1979 .

[8]  Jacob Bear,et al.  Fundamentals of transport phenomena in porous media , 1984 .

[9]  Yves Schuurman,et al.  TAP-2: An interrogative kinetics approach , 1997 .

[10]  G. Groppi,et al.  Development of a molecular kinetic scheme for methane partial oxidation over a Rh/α-Al2O3 catalyst , 2006 .

[11]  G. Groppi,et al.  Comparison among structured and packed-bed reactors for the catalytic partial oxidation of CH4 at short contact times , 2005 .

[12]  Manfred Baerns,et al.  Primary reaction steps and active surface sites in the rhodium-catalyzed partial oxidation of methane to CO and H2 , 1996 .

[13]  Daniel A. Hickman,et al.  Synthesis gas formation by direct oxidation of methane over Pt monoliths , 1992 .

[14]  G. Marin,et al.  Kinetics for the partial oxidation of methane on a Pt gauze at low conversions , 2000 .

[15]  G. Groppi,et al.  Structured reactors for kinetic measurements in catalytic combustion , 2001 .

[16]  G. Germani,et al.  Water-gas shift reaction kinetics over μ-structured Pt/CeO2/Al2O3 catalysts , 2006 .

[17]  G. Marin,et al.  An experimental reactor to study the intrinsic kinetics of catalytic partial oxidation of methane in the presence of heat-transport limitations , 1999 .

[18]  F. Kapteijn,et al.  Mathematical treatment of transient kinetic data: Combination of parameter estimation with solving the related partial differential equations , 1997 .

[19]  Charles T. Campbell,et al.  Future Directions and Industrial Perspectives Micro- and macro-kinetics: Their relationship in heterogeneous catalysis , 1994 .

[20]  Linda J. Broadbelt,et al.  A multiscale scheme for modeling catalytic flow reactors , 2006 .

[21]  N. Dupont,et al.  Specificities of micro-structured reactors for hydrogen production and purification , 2007 .

[22]  Jan J. Lerou,et al.  Chemical reaction engineering : A multiscale approach to a multiobjective task , 1996 .

[23]  X. Rozanska,et al.  Theory of zeolite catalysis , 1991 .

[24]  Lynn F. Gladden,et al.  Magnetic Resonance Imaging of Catalysts and Catalytic Processes , 2006 .

[25]  P. Galtier.  Kinetic Methods in Petroleum Process Engineering , 2007 .

[26]  Donghai Mei,et al.  From First Principles to Catalytic Performance: Tracking Molecular Transformations , 2004 .

[27]  Y. Schuurman,et al.  Silicon nitride supported platinum catalysts for the partial oxidation of methane at high temperatures , 2001 .

[28]  G. Ertl,et al.  Handbook of Heterogeneous Catalysis , 1997 .

[29]  Per Stoltze.  Microkinetic simulation of catalytic reactions , 2000 .

[30]  Daniel A. Hickman,et al.  Steps in CH4 oxidation on Pt and Rh surfaces: High‐temperature reactor simulations , 1993 .

[31]  J. Corriou,et al.  Microchannel reactors for kinetic measurement: Influence of diffusion and dispersion on experimental accuracy , 2001 .

[32]  Yves Schuurman,et al.  HCN synthesis from methane and ammonia over platinum , 2007 .

[33]  Gbmm Guy Marin,et al.  The Reaction Mechanism of the Partial Oxidation of Methane to Synthesis Gas: A Transient Kinetic Study over Rhodium and a Comparison with Platinum , 1997 .

[34]  R. S. Besser,et al.  Preferential oxidation (PrOx) in a thin-film catalytic microreactor: Advantages and limitations , 2005 .

[35]  Frank Behrendt,et al.  Modelling and simulation of heterogeneous oxidation of methane on a platinum foil , 1994 .

[36]  Manfred Baerns,et al.  Selectivity-directing factors of ammonia oxidation over PGM gauzes in the Temporal Analysis of Products reactor: Primary interactions of NH3 and O2 , 2004 .

[37]  Simulation of selective tungsten chemical vapour deposition , 1998 .

[38]  G. Froment,et al.  Single Event Kinetic Modeling of Complex Catalytic Processes , 2005 .

[39]  L. Kiwi-Minsker,et al.  Structured combustion catalysts based on sintered metal fibre filters , 2003 .

[40]  K. Wintermantel.  PROCESS AND PRODUCT ENGINEERING ACHIEVEMENTS, PRESENT AND FUTURE CHALLENGES , 1999 .

[41]  Guy Marin,et al.  Eurokin. Chemical Reaction Kinetics in Practice , 2001 .

[42]  Y. Schuurman,et al.  Reactive Oxygen Species on Platinum Gauzes during Partial Oxidation of Methane into Synthesis Gas , 2000 .

[43]  D. Mears,et al.  Tests for Transport Limitations in Experimental Catalytic Reactors , 1971 .

[44]  Olaf Deutschmann,et al.  Modeling the partial oxidation of methane in a short‐contact‐time reactor , 1998 .

[45]  M. D. Croon,et al.  The preparation of highly ordered single layer ZSM-5 coating on prefabricated stainless steel microchannels , 2001 .

[46]  Manfred Baerns,et al.  Determination of kinetic parameters for complex heterogeneous catalytic reactions by numerical evaluation of TAP experiments , 2000 .

[47]  Y. Schuurman.  Assessment of kinetic modeling procedures of TAP experiments , 2007 .

[48]  J. Chaouki,et al.  Noninvasive Tomographic and Velocimetric Monitoring of Multiphase Flows , 1997 .

[49]  L. Broadbelt,et al.  Applications of molecular modeling in heterogeneous catalysis research , 2000 .

[50]  Charles N. Satterfield,et al.  Mass transfer in heterogeneous catalysis , 1969 .

[51]  Gbmm Guy Marin,et al.  An investigation on the reaction mechanism for the partial oxidation of methane to synthesis gas over platinum , 1995 .

[52]  Albert Renken,et al.  Supported glass fibers catalysts for novel multi-phase reactor design , 1999 .