Transparent silicon/glass microreactor for high-pressure and high-temperature reactions

Abstract To increase mass transfer in solid catalyzed gas–liquid hydrogenations, the reactions are often operated at high pressures. Silicon/glass microreactors present a possibility to safely handle high-pressure and provide optical access into the reaction channel for flow investigations. In this study we present a Si/glass microreactor with soldered microfluidic connections for high-pressure and high-temperature applications. Mechanical testing of the device by tensile and pressure tests showed no failure for continuous operation at 140 bar and 80 °C. The improved microreactor design is applied for a well-described solid catalyzed exothermic hydrogenation at operating conditions up to 51 bar and 71 °C. Additionally the two-phase gas–liquid flow is investigated in the microreactor. Results clearly indicated the improvement of the reaction rate from 0.004 mol g cat − 1 mi n − 1 at ambient conditions to 0.046 mol g cat − 1 mi n − 1 at 51 bar and 71 °C. The reaction was observed to be mass transfer limited.

[1]  D. Hönicke,et al.  Microfabricated components for heterogeneously catalysed reactions , 1996 .

[2]  Philipp Rudolf von Rohr,et al.  Two-phase flow characteristics in gas–liquid microreactors , 2006 .

[3]  Wolfgang Ehrfeld,et al.  Microreactors: New Technology for Modern Chemistry , 2000 .

[4]  Klavs F. Jensen,et al.  Measurement of residence time distribution in microfluidic systems , 2005 .

[5]  Klavs F Jensen,et al.  Microreactor-based reaction optimization in organic chemistry--glycosylation as a challenge. , 2005, Chemical communications.

[6]  R. S. Besser,et al.  Hydrocarbon hydrogenation and dehydrogenation reactions in microfabricated catalytic reactors , 2003 .

[7]  Miko Elwenspoek,et al.  Local anodic bonding of Kovar to Pyrex aimed at high-pressure, solvent-resistant microfluidic connections , 2001 .

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

[9]  A J de Mello,et al.  A high-pressure interconnect for chemical microsystem applications. , 2001, Lab on a chip.

[10]  Weileun Fang,et al.  Micromachined rubber O-ring micro-fluidic couplers , 2000, Proceedings IEEE Thirteenth Annual International Conference on Micro Electro Mechanical Systems (Cat. No.00CH36308).

[11]  Volker Hessel,et al.  Chemical micro process engineering , 2003 .

[12]  W. Weibull.  A Statistical Distribution Function of Wide Applicability , 1951 .

[13]  M. Kothare,et al.  Novel microfluidic interconnectors for high temperature and pressure applications , 2003 .

[14]  R. Besser,et al.  Experimental study of hydrocarbon hydrogenation and dehydrogenation reactions in silicon microfabricated reactors of two different geometries , 2003 .

[15]  J. Wisniak,et al.  Hydrogen solubility in organic liquids , 1983 .

[16]  J. O’Connell,et al.  Catalytic hydrogenation of cyclohexene: Part II. Liquid phase reaction on supported platinum in a gradientless slurry reactor , 1978 .

[17]  Asterios Gavriilidis,et al.  Gas-liquid and gas-liquid-solid microstructured reactors : contacting principles and applications , 2005 .

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

[19]  Albert Renken,et al.  Microstructured reactors for catalytic reactions , 2005 .

[20]  V. T. Srikar,et al.  Fluidic packaging of microengine and microrocket devices for high-pressure and high-temperature operation , 2004, Journal of Microelectromechanical Systems.

[21]  Peter Enoksson,et al.  Micromachined flow-through filter-chamber for chemical reactions on beads , 2000 .

[22]  A. van den Berg,et al.  Novel microstructures and technologies applied in chemical analysis techniques , 1997, Proceedings of International Solid State Sensors and Actuators Conference (Transducers '97).

[23]  Z Hugh Fan,et al.  Macro-to-micro interfaces for microfluidic devices. , 2004, Lab on a chip.

[24]  C. Kappe,et al.  Heterogeneous hydrogenation reactions using a continuous flow high pressure device. , 2005, Journal of combinatorial chemistry.

[25]  K. R. Williams,et al.  Novel interconnection technologies for integrated microfluidic systems , 1998 .

[26]  M. Harold,et al.  Dynamic effects of vaporization with exothermic reaction in a porous catalytic pellet , 1993 .

[27]  M. Boudart,et al.  Catalytic hydrogenation of cyclohexene: 3. Gas-phase and liquid-phase reaction on supported palladium , 1978 .

[28]  Gunther Kolb,et al.  Micro-structured reactors for gas phase reactions , 2004 .

[29]  Aniruddha Puntambekar,et al.  Self-aligning microfluidic interconnects for glass- and plastic-based microfluidic systems , 2002 .

[30]  Thomas K. Sherwood,et al.  Mass transfer limitations in a trickle‐bed reactor , 1969 .

[31]  K. Jensen,et al.  Design and fabrication of microfluidic devices for multiphase mixing and reaction , 2002 .

[32]  M. Boudart,et al.  Catalytic hydrogenation of cyclohexene: I. Vapor-phase reaction on supported platinum , 1978 .

[33]  Wolfgang Ehrfeld,et al.  Silver-catalyzed oxidation of ethylene to ethylene oxide in a microreaction system , 2002 .

[34]  Takehiko Kitamori,et al.  A Microfluidic Device for Conducting Gas-Liquid-Solid Hydrogenation Reactions , 2004, Science.

[35]  B. Subramaniam,et al.  Fixed-bed hydrogenation of organic compounds in supercritical carbon dioxide , 2001 .

[36]  Volker Hessel,et al.  Fluidic bus system for chemical process engineering in the laboratory and for small-scale production , 2005 .

[37]  Asterios Gavriilidis,et al.  Experimental studies of nitrobenzene hydrogenation in a microstructured falling film reactor , 2004 .

[38]  K. Nitta,et al.  Continuous hydrogenation reactions in a tube reactor packed with Pd/C. , 2005, Chemical communications.

[39]  Axel Günther,et al.  A microfabricated gas-liquid segmented flow reactor for high-temperature synthesis: the case of CdSe quantum dots. , 2005, Angewandte Chemie.