Modelling a reverse flow reactor for the catalytic combustion of fugitive methane emissions

This paper describes the development and validation of a computer simulator for the modelling of a reverse flow catalytic reactor for the combustion of lean mixtures of methane in air. The simulator uses a heterogeneous two dimensional model for the reactor. The reactor uses a packed bed for catalytic sections and ceramic monoliths for inert sections, although the simulator is written in a general fashion so that any combination of packing can be used, in any desired variety. Validation is performed using a 200 mm internal diameter reactor over various flowrates and methane concentrations. The reverse flow reactor is observed to yield stable auto-thermal operation even for low methane concentrations. Higher methane concentrations are observed to give dual temperature peaks in the reactor. The transfer of energy is observed to be a significant factor in the reactor operation, which is shown by comparison of the heterogeneous model to a pseudo-homogeneous reactor model. The simulator can model the pilot reactor in real time for typical operating conditions.

[1]  C. F. Cullis,et al.  Pulse flow reactor studies of the oxidation of methane over palladium catalysts , 1971 .

[2]  Jörg Frauhammer,et al.  Modelling steady state and ignition during catalytic methane oxidation in a monolith reactor , 2000 .

[3]  J. Giddings,et al.  NEW METHOD FOR PREDICTION OF BINARY GAS-PHASE DIFFUSION COEFFICIENTS , 1966 .

[4]  Enrico Tronconi,et al.  Design of novel monolith catalyst supports for gas/solid reactions with heat exchange , 2000 .

[5]  Ming Zheng,et al.  Advanced Catalytic Converter System for Natural Gas Powered Diesel Engines , 1998 .

[6]  Christo G. Sapundzhiev,et al.  Influence of geometric and thermophysical properties of reaction layer on sulphur dioxide oxidation in transient conditions , 1990 .

[7]  Robert E. Hayes,et al.  The palladium catalysed oxidation of methane: reaction kinetics and the effect of diffusion barriers , 2001 .

[8]  Ryozo Echigo,et al.  Superadiabatic combustion in a porous medium , 1993 .

[9]  Robert E. Hayes,et al.  Finite-element model for a catalytic monolith reactor , 1992 .

[10]  H. Johnstone,et al.  Heat and mass transfer in packed beds , 1955 .

[11]  R. Aris On the dispersion of a solute in a fluid flowing through a tube , 1956, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[12]  Christo G. Sapundzhiev,et al.  Modelling of the reversed flow fixed bed reactor for catalytic decontamination of waste gases , 1997 .

[13]  Robert E. Hayes,et al.  Flow reversal reactor for the catalytic combustion of lean methane mixtures , 2003 .

[14]  Kyriacos Zygourakis,et al.  Transient operation of monolith catalytic converters: a two-dimensional reactor model and the effects of radially nonuniform flow distributions , 1989 .

[15]  D. Frank-Kamenetskii,et al.  Diffusion and heat exchange in chemical kinetics , 1955 .

[16]  M. D. Checkel,et al.  Experimental study of a reverse flow catalytic converter for a dual fuel engine , 2001 .

[17]  G. Bunimovich,et al.  Reverse-Flow Operation in Fixed Bed Catalytic Reactors , 1996 .

[18]  J. P. Leclerc,et al.  Modeling Catalytic Monoliths for Automobile Emission Control , 1992 .

[19]  S. Sloan An algorithm for profile and wavefront reduction of sparse matrices , 1986 .

[20]  Rutherford Aris,et al.  On the effects of radiative heat transfer in monoliths , 1977 .

[21]  Jamal Chaouki,et al.  CATALYTIC COMBUSTION OF NATURAL GAS IN A FIXED BED REACTOR WITH FLOW REVERSAL , 1993 .

[22]  Gilbert F. Froment,et al.  Modelling and simulation of the reversed flow operation of a fixed-bed reactor for methanol synthesis , 1993 .

[23]  Steffen Tischer,et al.  Transient three-dimensional simulations of a catalytic combustion monolith using detailed models for heterogeneous and homogeneous reactions and transport phenomena , 2001 .

[24]  Robert E. Hayes,et al.  Reversing flow catalytic converter for a natural gas/diesel dual fuel engine , 2001 .

[25]  R. E. Hayes,et al.  Introduction to Catalytic Combustion , 1998 .

[26]  Gilbert F. Froment,et al.  A two dimensional heterogeneous model for fixed bed catalytic reactors , 1971 .

[27]  André L. Boehman,et al.  Radiation heat transfer in catalytic monoliths , 1998 .

[28]  Pio Forzatti,et al.  Mathematical Models of Catalytic Combustors , 1999 .

[29]  James J. Carberry,et al.  Chemical and catalytic reaction engineering , 1976 .

[30]  Robert S. Brodkey,et al.  Turbulent motion and mixing in a pipe , 1964 .

[31]  G. Groppi,et al.  Catalytic Combustion for the Production of Energy , 1999 .

[32]  G. Taylor Dispersion of soluble matter in solvent flowing slowly through a tube , 1953, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[33]  Stephen Salomons,et al.  Modelling the Behaviour of a Reverse-Flow Catalytic Reactor for the Combustion of Lean Methane , 2003 .

[34]  A. D. Benedetto,et al.  TRANSIENT BEHAVIOUR OF PEROVSKITE-BASED MONOLITHIC REACTORS IN THE CATALYTIC COMBUSTION OF METHANE , 2001 .

[35]  Enrico Tronconi,et al.  Continuous vs. discrete models of nonadiabatic monolith catalysts , 1996 .

[36]  H. Sapoundjiev,et al.  Mathematical model and numerical simulations of catalytic flow reversal reactors for industrial applications , 2000 .

[37]  R. Aris A - * On the Dispersion of A Solute in A Fluid Flowing Through A Tube , 1999 .

[38]  Anthony G. Dixon,et al.  Theoretical prediction of effective heat transfer parameters in packed beds , 1979 .

[39]  Ulrich Nieken,et al.  Catalytic combustion with periodic flow reversal , 1988 .