Microfabricated Differential Reactor for Heterogeneous Gas Phase Catalyst Testing

Abstract A differential packed-bed reactor microfabricated in silicon is presented for heterogeneous gas phase catalyst testing. A novel cross-flow design achieves uniform flow distribution over a wide (25.5 mm) but shallow (400 μm long × 500 μm deep) catalyst bed to realize differential conversions with sufficient reaction to allow monitoring with conventional analysis techniques. The use of catalyst particles (diameters 53–71 μm) implies that conventional synthesis procedures can be used and experimental results translated to catalysts in macroscopic reactors. A set of shallow microfabricated channels maintains a spatially uniform pressure drop irrespective of variations in catalyst packing. Experiments and finite element simulations confirm the bed is isobaric with even distribution of flow. Quantitative analysis of transport effects indicates the microreactor also suppresses thermal and mass gradients in the catalyst bed. These characteristics make the cross-flow microreactor a useful tool for experiments to obtain kinetics and optimize reaction conditions. Experiments with CO oxidation confirm the ability of the microreactor to obtain kinetic and mechanistic information that compare well with parameters previously determined in macroscale systems. Reactor modeling also indicates that the catalyst bed operates differentially even at total conversions that would be considered large in traditional plug flow reactors, adding to the utility of the cross-flow microreactor as a laboratory tool.

[1]  Klavs F. Jensen,et al.  Microfabricated packed‐bed reactor for phosgene synthesis , 2001 .

[2]  P. Claus,et al.  Miniaturization of screening devices for the combinatorial development of heterogeneous catalysts , 2001 .

[3]  Klavs F. Jensen,et al.  Microfabricated multiphase packed-bed reactors : Characterization of mass transfer and reactions , 2001 .

[4]  Selim Senkan,et al.  Combinatorial Heterogeneous Catalysis-A New Path in an Old Field. , 2001, Angewandte Chemie.

[5]  J. Michael Ramsey,et al.  Micro Total Analysis Systems 2001 , 2001 .

[6]  K. Jensen Microreaction engineering * is small better? , 2001 .

[7]  S. Senturia Microsystem Design , 2000 .

[8]  Freek Kapteijn,et al.  The six-flow reactor technology: A review on fast catalyst screening and kinetic studies , 2000 .

[9]  Orschel,et al.  Detection of Reaction Selectivity on Catalyst Libraries by Spatially Resolved Mass Spectrometry. , 1999, Angewandte Chemie.

[10]  Zengin,et al.  High-Throughput Testing of Heterogeneous Catalyst Libraries Using Array Microreactors and Mass Spectrometry. , 1999, Angewandte Chemie.

[11]  Jandeleit,et al.  Combinatorial Materials Science and Catalysis. , 1999, Angewandte Chemie.

[12]  W. H. Weinberg,et al.  High-Throughput Synthesis and Screening of Combinatorial Heterogeneous Catalyst Libraries. , 1999, Angewandte Chemie.

[13]  M. Schmidt,et al.  Characterization of a Time Multiplexed Inductively Coupled Plasma Etcher , 1999 .

[14]  W. Prins,et al.  Platinum catalyzed oxidation of carbon monoxide as a model reaction in mass transfer measurements , 1998 .

[15]  M. Schmidt Wafer-to-wafer bonding for microstructure formation , 1998, Proc. IEEE.

[16]  D. Goodman,et al.  CO + O2 and CO + NO Reactions over Pd/Al2O3 Catalysts , 1997 .

[17]  Mass transfer in packed beds at low Peclet numbers, wrong experiments or wrong interpretations? , 1997 .

[18]  Dan Luss,et al.  Infrared Thermographic Screening of Combinatorial Libraries of Heterogeneous Catalysts , 1996 .

[19]  X. Verykios,et al.  CO Oxidation over Rh Dispersed on SiO2, Al2O3 and TiO2: Kinetic Study and Oscillatory Behavior , 1995 .

[20]  R. Gorte,et al.  CO Oxidation on Pt/α-Al2O3(0001): Evidence for Structure Sensitivity , 1993 .

[21]  S. Oh,et al.  Influence of metal particle size and support on the catalytic properties of supported rhodium: CO$z.sbnd;O2 and CO$z.sbnd;NO reactions , 1991 .

[22]  M. Maple,et al.  Oscillatory oxidation of CO over Pt at pressures from 10 to 760 torr , 1991 .

[23]  D. W. Goodman,et al.  Comparative kinetic studies of CO$z.sbnd;O2 and CO$z.sbnd;NO reactions over single crystal and supported rhodium catalysts , 1986 .

[24]  O. Levenspiel Chemical Reaction Engineering , 1972 .

[25]  K. Daizo,et al.  Particle-to-fluid heat and mass transfer in packed beds of fine particles , 1967 .