Ethylene Hydrogenation in Pellets with Different Pore Structures, Measured in a One-Sided Single-Pellet Reactor
-
Aykut Argönül
and
Frerich J. Keil
Abstract
The ethylene hydrogenation reaction was investigated in a kinetic turbo reactor and a one-sided single-pellet reactor. An empirical kinetic expression was fitted to experimental results taken from the turbo reactor, and the gas compositions at the catalyst centers were measured for three different pore structures by means of the single-pellet reactor. A bimodal pore model was developed and applied to the computation of the gas composition profiles inside the three pore structures. The calculated results were compared to the measurements. A distinct influence of the pore structures on the gas fluxes and concentration profiles inside the pores could be detected which demonstrates that the proper choice of the pellet pore structure is of importance for a high conversion.
Appendices
Data from kinetic reactor measurements.
| Inlet Compositions [%] | Exit Composition [%] | |||
|---|---|---|---|---|
| N2 | H2 | C2H4 | C2H4 | |
| T = 30 °C | 39.15 | 19.63 | 41.22 | 40.81 |
| 39.14 | 40.1 | 20.76 | 20.45 | |
| 49.23 | 8.52 | 42.25 | 41.14 | |
| 50.08 | 39.05 | 10.87 | 10.52 | |
| 58.13 | 21.12 | 20.75 | 20.07 | |
| 58.40 | 10.65 | 30.95 | 30.57 | |
| 58.54 | 30.77 | 10.69 | 10.51 | |
| 78.36 | 11.09 | 10.55 | 10.44 | |
| 72.25 | 6.39 | 21.36 | 20.36 | |
| 68.94 | 20.65 | 10.41 | 10.25 | |
| 80.49 | 8.67 | 10.83 | 10.52 | |
| T = 50 °C | 38.79 | 17.87 | 43.34 | 42.80 |
| 39.38 | 39.96 | 20.65 | 20.16 | |
| 49.59 | 8.58 | 41.83 | 41.09 | |
| 49.61 | 40.01 | 10.38 | 10.15 | |
| 58.86 | 20.55 | 20.59 | 20.42 | |
| 59.07 | 10.21 | 30.72 | 30.48 | |
| 57.93 | 31.23 | 10.84 | 10.62 | |
| 77.85 | 11.56 | 10.59 | 10.43 | |
| 68.14 | 10.66 | 21.21 | 20.68 | |
| 68.51 | 20.79 | 10.71 | 10.51 | |
| T = 100 °C | 39.57 | 18.3 | 42.13 | 41.47 |
| 40.06 | 39.09 | 20.85 | 20.66 | |
| 49.85 | 8.62 | 41.53 | 40.66 | |
| 49.13 | 40.14 | 10.72 | 10.56 | |
| 58.55 | 20.58 | 20.87 | 20.50 | |
| 59.14 | 9.91 | 30.95 | 30.76 | |
| 58.66 | 30.74 | 10.59 | 10.45 | |
| 78.05 | 11.29 | 10.66 | 10.54 | |
| 68.60 | 10.38 | 21.02 | 20.81 | |
| 68.81 | 20.71 | 10.48 | 10.35 | |
The total inlet flow rate was fixed at 200 [mL/min] for all the experiments.
References
Adler, R., F. Schroeder, and B. Platzer. 2001. Patent (Deutsches Patent- und Markenamt), DE000010104849A1_1.pdf. DE 101 04 849 A 1.Search in Google Scholar
Balder, J. R., and E. E. Petersen. 1968a. “Application of the Single Pellet Reactor for Direct Mass Transfer Studies.” Journal of Catalysis 11: 202–10.10.1016/0021-9517(68)90033-XSearch in Google Scholar
Balder, J. R., and E. E. Petersen. 1968b. “Poisoning Studies in a Single-Pellet Reactor.” Chemical Engineering Science 23: 1287–91.10.1016/0009-2509(68)89038-4Search in Google Scholar
Bartholomew, C. H., and R. J. Farrauto. 2005. Fundamentals of Industrial Catalytic Processes, 2nd ed. New York: Wiley-AIChE.10.1002/9780471730071Search in Google Scholar
Beckmann, A. 1995. “SLP-Catalysts in Stationary and Instationary Operated Fixed-bed Reactors using the Example of Hydroformylation.” PhD Thesis, Hamburg University of Technology.Search in Google Scholar
Berty, J. M. 1979. “Testing Commercial Catalysts in Recycle Reactors.” Catalysis Reviews – Science and Engineering 20: 75–96.10.1080/03602457908065106Search in Google Scholar
Berty, J. M. 1999. Experiments in Catalytic Reaction Engineering. Surface Science and Catalysis, Vol. 124. Amsterdam: Elsevier.Search in Google Scholar
Binder, A., M. Seipenbusch, and M. Mühler. 2009. “Kinetics and Particle Size Effects in Ethylene Hydrogenation over Supported Palladium Catalysts at Atmospheric Pressure.” Journal of Catalysis 268: 150–55.10.1016/j.jcat.2009.09.013Search in Google Scholar
Cremer, P. S., G. A. Somorjai, and M. Studies. 1995. “Surface Science and Catalysis of Ethylene Hydrogenation.” Journal of the Chemical Society, Faraday Transactions 91: 3671–77.10.1039/ft9959103671Search in Google Scholar
Dogu, T. 1981. “The Importance of Pore Structure and Diffusion in the Kinetics of Gas-Solid Noncatalytic Reactions: Reaction of Calcinated Limestone with SO2.” Chemical Engineering Journal 21: 213–22.10.1016/0300-9467(81)80005-6Search in Google Scholar
Dogu, T., A. Keskin, G. Dogu, and J. M. Smith. 1986. “Single-Pellet Moment Method for Analysis of Gas-Solid Reactions.” AIChE Journal 32: 743–50.10.1002/aic.690320504Search in Google Scholar
Dogu, T., N. Yasyerli, G. Dogu, B. J. McCoy, and J. M. Smith. 1996. “One-Sided Single-Pellet Technique for Adsorption and Intraparticle Diffusion.” AIChE Journal 92: 516–23.Search in Google Scholar
Gostick, J., M. Aghighi, J. Hinebaugh, T. Trauter, M. A. Hoek, H. Day, B. Spellacy, et al. 2016. “OpenPNM: A Pore Network Modeling Package.” Computing in Science & Engineering 18: 60 (July/August).10.1109/MCSE.2016.49Search in Google Scholar
Günbulut, K. A. 2005. "Analysis of Reactive Flow through a Catalyst Pellet Using Dusty-Gas Model" Project Work Report, Hamburg University of Technology (TUHH).Search in Google Scholar
Hegedus, L. L., and E. E. Petersen. 1974. “The Single-Pellet Diffusion Reactor: Theory and Applications.” Catalysis Reviews – Science and Engineering 9: 245–66.10.1080/01614947408075376Search in Google Scholar
Hirschfelder, J., C. F. Curtiss, and R. B. Bird. 1954. Molecular Theory of Gases and Liquids. New York: Wiley.Search in Google Scholar
Horiuti, I., and M. Polanyi. 1934. “Exchange Reactions of Hyddrogen on Metallic Catalysts.” Transactions of the Faraday Society 30: 1169–72.10.1039/tf9343001164Search in Google Scholar
Horiuti, J., and K. Miyahara, 1968. “Hydrogenation of Ethylene on Metallic Catalysts.” National Standard Reference Data System (NSRDS-NBS), Vol. 13.10.6028/NBS.NSRDS.13Search in Google Scholar
Jovanov, Z. 2008. „Bachelor Thesis, Untersuchung der optimalen Reaktionsbedingungen in einem kinetischen Turbo-Reaktor.“ Hamburg University of Technology (TUHH).Search in Google Scholar
Kapteijn, F., and J. A. Moulijn. 2008. “Laboratory Testing of Solid Catalysts,” in Handbook of Heterogeneous Catalysis, edited by G. Ertl, H. Knözinger, and F. Schüth, 2nd, 1361–1398. Weinheim: Wiley-VCH Chapter 9.Search in Google Scholar
Keil, F. J. 2012. “Modeling Reactions in Porous Media.” In Modeling and Simulation of Heterogeneous Catalytic Reactions: From the Molecular Process to the Technical System, edited by O. Deutschmann, 149–86. Weinheim: Wiley-VCH.10.1002/9783527639878.ch5Search in Google Scholar
Keil, F. J. 2013. “Complexities in Modeling of Heterogeneous Catalytic Reactions.” Computers & Mathematics with Applications 65: 1674–97.10.1016/j.camwa.2012.11.023Search in Google Scholar
Keil, F. J. 2018. “Molecular Modelling for Reactor Design.” Annual Review of Chemical and Biomolecular Engineering 9: 201–27.10.1146/annurev-chembioeng-060817-084141Search in Google Scholar
Keil, F. J., and C. Rieckmann. 1994. “Optimization of Three-Dimensional Catalyst Pore Structures.” Chemical Engineering Science 49: 4811–22.10.1016/S0009-2509(05)80061-2Search in Google Scholar
Kopaç, T., G. Doğu, and T. Doğu. 1996. “Single Pellet Reactors for the Dynamic Analysis of Gas-Solid Reactions-Reaction of SO2 with Activated Soda.” Chemical Engineering Science 51: 2201–09.10.1016/0009-2509(96)00077-2Search in Google Scholar
Krishna, R., and J. A. Wesselingh. 1997. “The Maxwell-Stefan Approach to Mass Transfer.” Chemical Engineering Science 52: 861–911. doi:10.1016/S0009-2509(96)00458-7.Search in Google Scholar
Neurock, M., and R. A. van Santen. 2000. “A First Principles Analysis of C-H Bond Formation in Ethylene Hydrogenation.” The Journal of Physical Chemistry B 104: 11127–45.10.1021/jp994082tSearch in Google Scholar
Park, I.-S., and D. D. Do. 1996. “Measurement of the Effective Diffusivity in Porous Media by the Diffusion Cell Method.” Catalysis Reviews – Science and Engineering 38: 189–247.10.1080/01614949608006458Search in Google Scholar
Rao, S. M., and M-O. Coppens. 2012. “Increasing Robustness against Deactivation of Nanoporous Catalysts by Introducing an Optimized Hierarchical Pore Network – Application to Hydrodemetallation.” Chemical Engineering Science 83: 66–76.10.1016/j.ces.2011.11.044Search in Google Scholar
Rieckmann, C., and F. J. Keil. 1999. “Simulation and Experiment of Multicomponent Diffusion and Reaction in Three-Dimensional Networks.” Chemical Engineering Science 54: 3485–93.10.1016/S0009-2509(98)00480-1Search in Google Scholar
Stokes, R. L., and E. B. Naumann. 1970. “Residence Time Distribution for Stirred Tanks in Series.” The Canadian Journal of Chemical Engineering 48: 723–25.10.1002/cjce.5450480612Search in Google Scholar
Van Santen, R. A. 2017. Modern Heterogeneous Catalysis. Weinheim: Wiley-VCH.10.1002/9783527810253Search in Google Scholar
Ye, G., Y. Sun, X. Zhou, K. Zhu, and M.-O. Coppens. 2017a. “Method for Generating Pore Networks in Porous Particles of Arbitrary Shape, and Its Application to Catalytic Hydrogenation Ob Benzene.” Chemical Engineering Journal 329: 56–65.10.1016/j.cej.2017.02.036Search in Google Scholar
Ye, G., X. Zhou, and M.-O. Coppens. 2017b. “Influence of Catalyst Pore Network Structure on the Hysteresis of Multiphase Reactions.” AIChE Journal 63: 78–86.10.1002/aic.15415Search in Google Scholar
Zaera, F., and G. A. Somorjai. 1984. “Hydrogenation of Ethylene over Pt(111) Single-Crystal Surfaces.” Journal of the American Chemical Society 106: 2288–93.10.1021/ja00320a013Search in Google Scholar
Notes
Article to honour Professor Gülsen Dogu and Professor Timur Dogu
© 2019 Walter de Gruyter GmbH, Berlin/Boston
Articles in the same Issue
- Editorial
- To the Distinguished Contribution of Professor Gulsen Dogu and Professor Timur Dogu to Chemical Reaction Engineering
- Special Issue Articles
- Structural Property Improvements of Bentonite with Sulfuric Acid Activation and a Test in Catalytic Wet Peroxide Oxidation of Phenol
- Effect of Surface Area and Micropore Volume of Activated Carbons from Coal by KOH, NaOH and ZnCl2 Treatments on Methane Adsorption
- Using Volatile Organic Compounds in Waste Streams as Fuel
- Catalytic Decomposition of Ammonia for Hydrogen Production over Carbon Nanofiber Supported Fe and Mo Catalysts in a Microwave Heated Reactor
- Ethylene Hydrogenation in Pellets with Different Pore Structures, Measured in a One-Sided Single-Pellet Reactor
- Catalytic Performances of Bi-Metallic Ni-Co Catalysts in Acetic Acid Steam Reforming Reaction: Effect of Mg Incorporation
- PdIn Catalysts in a Continuous Fixed Bed Reactor for the Nitrate Removal from Groundwater
- Chemical Cross-Linking of 6FDA-6FPA Polyimides for Gas Permeation Membranes
- Revisiting Electrochemical Techniques to Characterize the Solid-State Diffusion Mechanism in Lithium-Ion Batteries
- Short Communications
- Effect of Non-Ideal Mixing on Heat Transfer of non-Newtonian Liquids in a Mechanically Agitated Vessel
Articles in the same Issue
- Editorial
- To the Distinguished Contribution of Professor Gulsen Dogu and Professor Timur Dogu to Chemical Reaction Engineering
- Special Issue Articles
- Structural Property Improvements of Bentonite with Sulfuric Acid Activation and a Test in Catalytic Wet Peroxide Oxidation of Phenol
- Effect of Surface Area and Micropore Volume of Activated Carbons from Coal by KOH, NaOH and ZnCl2 Treatments on Methane Adsorption
- Using Volatile Organic Compounds in Waste Streams as Fuel
- Catalytic Decomposition of Ammonia for Hydrogen Production over Carbon Nanofiber Supported Fe and Mo Catalysts in a Microwave Heated Reactor
- Ethylene Hydrogenation in Pellets with Different Pore Structures, Measured in a One-Sided Single-Pellet Reactor
- Catalytic Performances of Bi-Metallic Ni-Co Catalysts in Acetic Acid Steam Reforming Reaction: Effect of Mg Incorporation
- PdIn Catalysts in a Continuous Fixed Bed Reactor for the Nitrate Removal from Groundwater
- Chemical Cross-Linking of 6FDA-6FPA Polyimides for Gas Permeation Membranes
- Revisiting Electrochemical Techniques to Characterize the Solid-State Diffusion Mechanism in Lithium-Ion Batteries
- Short Communications
- Effect of Non-Ideal Mixing on Heat Transfer of non-Newtonian Liquids in a Mechanically Agitated Vessel
