Methane steam reforming at microscales: Operation strategies for variable power output at millisecond contact times

The potential of methane steam reforming at microscale is theoretically explored. To this end, a multifunctional catalytic plate microreactor, comprising of a propane combustion channel and a methane steam reforming channel, separated by a solid wall, is simulated with a pseudo 2-D (two-dimensional) reactor model. Newly developed lumped kinetic rate expressions for both processes, obtained from a posteriori reduction of detailed microkinetic models, are used. It is shown that the steam reforming at millisecond contact times is feasible at microscale, and in agreement with a recent experimental report. Furthermore, the attainable operating regions delimited from the materials stability limit, the breakthrough limit, and the maximum power output limit are mapped out. A simple operation strategy is presented for obtaining variable power output along the breakthrough line (a nearly iso-flow rate ratio line), while ensuring good overlap of reaction zones, and provide guidelines for reactor sizing. Finally, it is shown that the choice of the wall material depends on the targeted operating regime. Low-conductivity materials increase the methane conversion and power output at the expense of higher wall temperatures and steeper temperature gradients along the wall. For operation close to the breakthrough limit, intermediate conductivity materials, such as stainless steel, offer a good compromise between methane conversion and wall temperature. Even without recuperative heat exchange, the thermal efficiency of the multifunctional device and the reformer approaches ∼65% and ∼85%, respectively. © 2008 American Institute of Chemical Engineers AIChE J, 2009

[1]  D. Vlachos,et al.  Extending the region of stable homogeneous micro-combustion through forced unsteady operation , 2007 .

[2]  Dimos Poulikakos,et al.  Effects of microreactor wall heat conduction on the reforming process of methane , 2005 .

[3]  D. Vlachos,et al.  Stability and performance of catalytic microreactors: Simulations of propane catalytic combustion on Pt , 2008 .

[4]  Asterios Gavriilidis,et al.  Catalytic combustion assisted methane steam reforming in a catalytic plate reactor , 2003 .

[5]  Guy Marin,et al.  Evaluation of high-emissivity coatings in steam cracking furnaces using a non-grey gas radiation model , 2008 .

[6]  Steve Perry,et al.  Microchannel Process Technology for Compact Methane Steam Reforming , 2004 .

[7]  D G Vlachos,et al.  Hierarchical multiscale mechanism development for methane partial oxidation and reforming and for thermal decomposition of oxygenates on Rh. , 2005, The journal of physical chemistry. B.

[8]  Thomas Rostrup-Nielsen,et al.  Manufacture of hydrogen , 2005 .

[9]  D. Vlachos,et al.  Effect of flow configuration on the operation of coupled combustor/reformer microdevices for hydrogen production , 2005 .

[10]  G. Groppi,et al.  Steady‐state and transient analysis of a CH4–catalytic partial oxidation reformer , 2006 .

[11]  Matteo Maestri,et al.  Steam and dry reforming of methane on Rh : Microkinetic analysis and hierarchy of kinetic models , 2008 .

[12]  Hui Liu,et al.  Modeling of a metal monolith catalytic reactor for methane steam reforming–combustion coupling , 2007 .

[13]  Frédéric Vogel,et al.  Reactor modeling to simulate catalytic partial oxidation and steam reforming of methane. Comparison of temperature profiles and strategies for hot spot minimization , 2007 .

[14]  Eric D. Wetzel,et al.  Single channel and heat recirculation catalytic microburners: An experimental and computational fluid dynamics study , 2009 .

[15]  Dionisios G. Vlachos,et al.  Millisecond methane steam reforming via process and catalyst intensification , 2008 .

[16]  D. Vlachos,et al.  Optimal reactor dimensions for homogeneous combustion in small channels , 2007 .

[17]  Kenneth A. Williams,et al.  Methane catalytic partial oxidation on autothermal Rh and Pt foam catalysts: Oxidation and reforming zones, transport effects, and approach to thermodynamic equilibrium , 2007 .

[18]  Dionisios G. Vlachos,et al.  CFD Simulations of Coupled, Countercurrent Combustor/Reformer Microdevices for Hydrogen Production , 2005 .

[19]  D. G. Norton,et al.  Combustion characteristics and flame stability at the microscale: a CFD study of premixed methane/air mixtures , 2003 .

[20]  D. Vlachos,et al.  Modeling Ignition in Catalytic Microreactors , 2008 .

[21]  Kenneth A. Williams,et al.  Mechanism of H2 and CO formation in the catalytic partial oxidation of CH4 on Rh probed by steady-state spatial profiles and spatially resolved transients , 2007 .

[22]  R. Hughes,et al.  The kinetics of methane steam reforming over a Ni/α-Al2O catalyst , 2001 .

[23]  Dionisios G. Vlachos,et al.  Portable power production from methanol in an integrated thermoeletric/microreactor system , 2008 .

[24]  Jens R. Rostrup-Nielsen,et al.  Steam reforming of hydrocarbons. A historical perspective , 2004 .

[25]  Aristides Morillo,et al.  Heat-integrated reactor concepts for catalytic reforming and automotive exhaust purification , 2007 .

[26]  B. Sundén,et al.  Analysis of chemical-reaction-coupled mass and heat transport phenomena in a methane reformer duct for PEMFCs , 2007 .

[27]  G. Froment,et al.  Methane steam reforming, methanation and water‐gas shift: I. Intrinsic kinetics , 1989 .

[28]  Andrei G. Fedorov,et al.  Hydrogen generation in a reverse‐flow microreactor: 1. Model formulation and scaling , 2005 .

[29]  D. Vlachos,et al.  A reduced mechanism for methane and one-step rate expressions for fuel-lean catalytic combustion of small alkanes on noble metals , 2007 .

[30]  Lanny D. Schmidt,et al.  Steam reforming of methane and water-gas shift in catalytic wall reactors , 2003 .

[31]  Yong Wang,et al.  From seconds to milliseconds to microseconds through tailored microchannel reactor design of a steam methane reformer , 2007 .

[32]  D. G. Norton,et al.  A CFD study of propane/air microflame stability , 2004 .

[33]  Gregory S. Jackson,et al.  Transient modeling of combined catalytic combustion/CH4 steam reforming , 2003 .

[34]  David L. Trimm,et al.  ONBOARD FUEL CONVERSION FOR HYDROGEN-FUEL-CELL-DRIVEN VEHICLES , 2001 .

[35]  Matteo Maestri,et al.  A C1 microkinetic model for methane conversion to syngas on Rh/Al2O3 , 2009 .

[36]  M. Ertan Taskin,et al.  3D CFD simulations of steam reforming with resolved intraparticle reaction and gradients , 2007 .

[37]  Yong Wang,et al.  Review of developments in portable hydrogen production using microreactor technology. , 2004, Chemical reviews.