This content is not included in your SAE MOBILUS subscription, or you are not logged in.
Microkinetic Modelling for Propane Oxidation in Channel Flows of a Silver-Based Automotive Catalytic Converter
ISSN: 0148-7191, e-ISSN: 2688-3627
Published August 30, 2011 by SAE International in United States
Annotation ability available
Computational Fluid Dynamics (CFD) is used to simulate chemical reactions and transport phenomena occurring in a single channel of a honeycomb-type automotive catalytic converter under lean burn combustion. Microkinetic analysis is adopted to develop a detailed elementary reaction mechanism for propane oxidation on a silver catalyst. Activation energies are calculated based on the theory of the Unity Bond Index-Quadratic Exponential Potential (UBI-QEP) method. The order-of-magnitude of the pre-exponential factors is obtained from Transition State Theory (TST). Sensitivity analysis is applied to identify the important elementary steps and refine the pre-exponential factors of these reactions. These pre-exponential factors depend on inlet temperatures and propane concentration; therefore optimised pre-exponential factors are written in polynomial forms. The results of numerical simulations are validated by comparison with experimental data.
CitationSawatmongkhon, B., Tsolakis, A., York, A., and Theinnoi, K., "Microkinetic Modelling for Propane Oxidation in Channel Flows of a Silver-Based Automotive Catalytic Converter," SAE Technical Paper 2011-01-2094, 2011, https://doi.org/10.4271/2011-01-2094.
- Ansell, G. P., Bennett, P. S., Cox, J. P., Frost, J. C., Gray, P. G., Jones, A. M., Rajaram, R. R., Walker, A. P., Litorell, M., and Smedler, G., 1996, “The development of a model capable of predicting diesel lean NOx catalyst performance under transient conditions,” Applied Catalysis B: Environmental, 10(1-3), pp. 183-201.
- Wanker, R., Raupenstrauch, H., and Staudinger, G., 2000, “A fully distributed model for the simulation of a catalytic combustor,” Chemical Engineering Science, 55(20), pp. 4709-4718.
- Westerberg, B., Künkel, C., and Odenbrand, C. U. I., 2003, “Transient modelling of a HC-SCR catalyst for diesel exhaust aftertreatment,” Chemical Engineering Journal, 92(1-3), pp. 27-39.
- Wurzenberger, J. C., and Wanker, R., 2005, “Multi-scale SCR modeling, 1D kinetic analysis and 3D system simulation,” SAE, Paper No. 2005-01-0948.
- Liu, B., Hayes, R. E., Yi, Y., Mmbaga, J., Checkel, M. D., and Zheng, M., 2007, “Three dimensional modelling of methane ignition in a reverse flow catalytic converter,” Computers & Chemical Engineering, 31(4), pp. 292-306.
- Voltz, S. E., Morgan, C. R., Liederman, D., and Jacob, S. M., 1973, “Kinetic study of carbon monoxide and propylene oxidation on platinum catalysts,” Industrial Engineering Chemistry Production Research and Development, 12, pp. 294-301.
- Santos, H., and Costa, M., 2009, “Modelling transport phenomena and chemical reactions in automotive three-way catalytic converters,” Chemical Engineering Journal, 148(1), pp. 173-183.
- Dumesic, J. A., Rudd, D. F., Aparicio, L. M., Rekoske, J. E., and Treviño, A. A., 1993, The Microkinetics of Heterogeneous Catalysis, American Chemical Society, Washington DC.
- Park, Y. K., Aghalayam, P., and Vlachos, D. G., 1999, “A generalized approach for predicting coverage-dependent reaction parameters of complex surface reactions: Application to H2 oxidation over platinum,” The Journal of Physical Chemistry A (ACS Publications), 103, pp. 8101-8107.
- Aghalayam, P., Park, Y. K., and Vlachos, D. G., 2000, “Construction and optimization of complex surface-reaction mechanism,” AIChE Journal, 46(10), pp. 2017-2029.
- Mhadeshwar, A. B., Aghalayam, P., Papavassiliou, V., and Vlachos, D. G., 2002, “Surface reaction mechanism development for platinum-catalyzed oxidation of methane,” Proceedings of the Combustion Institute, 29(1), pp. 997-1004.
- Aghalayam, P., Park, Y. K., Fernandes, N., Papavassiliou, V., Mhadeshwar, A. B., and Vlachos, D. G., 2003, “A C1 mechanism for methane oxidation on platinum,” Journal of Catalysis, 213(1), pp. 23-38.
- Mhadeshwar, A. B., and Vlachos, D. G., 2005, “Hierarchical multiscale mechanism development for methane partial oxidation and reforming and for thermal decomposition of oxygenates on Rh,” The Journal of Physical Chemistry B (ACS Publications), 109, pp. 16819-16835.
- Mhadeshwar, A. B., and Vlachos, D. G., 2005, “A thermodynamically consistent surface reaction mechanism for CO oxidation on Pt,” Combustion and Flame, 142(3), pp. 289-298.
- Mhadeshwar, A. B., and Vlachos, D. G., 2005, “Hierarchical, multiscale surface reaction mechanism development: CO and H2 oxidation, water-gas shift, and preferential oxidation of CO on Rh,” Journal of Catalysis, 234(1), pp. 48-63.
- Mhadeshwar, A. B., Winkler, B. H., Eiteneer, B., and Hancu, D., 2009, “Microkinetic modeling for hydrocarbon (HC)-based selective catalytic reduction (SCR) of NOx on a silver-based catalyst,” Applied Catalysis B: Environmental, 89(1-2), pp. 229-238.
- Deutschmann, O., Maier, L. I., Riedel, U., Stroemman, A. H., and Dibble, R. W., 2000, “Hydrogen assisted catalytic combustion of methane on platinum,” Catalysis Today, 59(1-2), pp. 141-150.
- Chatterjee, D., Deutschmann, O., and Warnatz, J., 2001, “Detailed surface reaction mechanism in a three-way catalyst,” Faraday Discussions, 119, pp. 371-384.
- Quiceno, R., Pérez-Ramírez, J., Warnatz, J., and Deutschmann, O., 2006, “Modeling the high-temperature catalytic partial oxidation of methane over platinum gauze: Detailed gas-phase and surface chemistries coupled with 3D flow field simulations,” Applied Catalysis A: General, 303(2), pp. 166-176.
- Sch??del, B. T., Duisberg, M., and Deutschmann, O., 2009, “Steam reforming of methane, ethane, propane, butane, and natural gas over a rhodium-based catalyst,” Catalysis Today, 142(1-2), pp. 42-51.
- Storsæter, S., Chen, D., and Holmen, A., 2006, “Microkinetic modelling of the formation of C1 and C2 products in the Fischer-Tropsch synthesis over cobalt catalysts,” Surface Science, 600(10), pp. 2051-2063.
- Braun, J., Hauber, T., Többen, H., Zacke, P., Chatterjee, D., Deutschmann, O., and Warnatz, J., 2000, “Influence of physical and chemical parameters on the conversion rate of a catalytic converter: A numerical simulation study,” SAE, Paper No. 2000-01-0211.
- Chafik, T., Kameoka, S., Ukisu, Y., and Miyadera, T., 1998, “In situ diffuse reflectance infrared Fourier transform spectroscopy study of surface species involved in NOx reduction by ethanol over alumina-supported silver catalyst,” Journal of Molecular Catalysis A: Chemical, 136(2), pp. 203-211.
- Yu, Y., He, H., and Feng, Q., 2003, “Novel enolic surface species formed during partial oxidation of CH3CHO, C2H5OH, and C3H6 on Ag/Al2O3: An in situ DRIFTS study,” The Journal of Physical Chemistry B, 107(47), pp. 13090-13092.
- Yeom, Y. H., Wen, B., Sachtler, W. M. H., and Weitz, E., 2004, “NOx Reduction from Diesel Emissions over a Nontransition Metal Zeolite Catalyst: A Mechanistic Study Using FTIR Spectroscopy,” The Journal of Physical Chemistry B, 108(17), pp. 5386-5404.
- Yu, Y., He, H., Feng, Q., Gao, H., and Yang, X., 2004, “Mechanism of the selective catalytic reduction of NOx by C2H5OH over Ag/Al2O3,” Applied Catalysis B: Environmental, 49(3), pp. 159-171.
- Yeom, Y. H., Li, M., Sachtler, W. M. H., and Weitz, E., 2006, “A study of the mechanism for NOx reduction with ethanol on γ-alumina supported silver,” Journal of Catalysis, 238(1), pp. 100-110.
- Yeom, Y. H., Li, M., Sachtler, W. M. H., and Weitz, E., 2007, “Low-temperature NOx reduction with ethanol over Ag/Y: A comparison with Ag/y-Al2O3 and BaNa/Y,” Journal of Catalysis, 246(2), pp. 413-427.
- Yeom, Y., Li, M., Savara, A., Sachtler, W., and Weitz, E., 2008, “An overview of the mechanisms of NOx reduction with oxygenates over zeolite and Y-Al2O3 catalysts,” Catalysis Today, 136(1-2), pp. 55-63.
- Zhang, X., Yu, Y., and He, H., 2007, “Effect of hydrogen on reaction intermediates in the selective catalytic reduction of NOx by C3H6,” Applied Catalysis B: Environmental, 76(3-4), pp. 241-247.
- Shimizu, K.-i., Kawabata, H., Satsuma, A., and Hattori, T., 1999, “Role of Acetate and Nitrates in the Selective Catalytic Reduction of NO by Propene over Alumina Catalyst as Investigated by FTIR,” The Journal of Physical Chemistry B, 103(25), pp. 5240-5245.
- Shimizu, K.-i., Shibata, J., Yoshida, H., Satsuma, A., and Hattori, T., 2001, “Silver-alumina catalysts for selective reduction of NO by higher hydrocarbons: structure of active sites and reaction mechanism,” Applied Catalysis B: Environmental, 30(1-2), pp. 151-162.
- Burch, R., Breen, J. P., and Meunier, F. C., 2002, “A review of the selective reduction of NOx with hydrocarbons under lean-burn conditions with nonzeolitic oxide and platinum group metal catalysts,” Applied Catalysis B: Environmental, 39(4), pp. 283-303.
- Shimizu, K.-i., and Satsuma, A., 2006, “Selective catalytic reduction of NO over supported silver catalysts-practical and mechanistic aspects,” Physical Chemistry Chemical Physics, 8(23), pp. 2677-2695.
- Yu, Y., Zhang, X., and He, H., 2007, “Evidence for the formation, isomerization and decomposition of organo-nitrite and -nitro species during the NOx reduction by C3H6 on Ag/Al2O3,” Applied Catalysis B: Environmental, 75(3-4), pp. 298-302.
- Shibata, J., Shimizu, K.-i., Satokawa, S., Satsuma, A., and Hattori, T., 2003, “Promotion effect of hydrogen on surface steps in SCR of NO by propane over alumina-based silver catalyst as examined by transient FT-IR,” Physical Chemistry Chemical Physics, 5, pp. 2154-2160.
- Bettahar, M. M., Costentin, G., Savary, L., and Lavalley, J. C., 1996, “On the partial oxidation of propane and propylene on mixed metal oxide catalysts,” Applied Catalysis A: General, 145(1-2), pp. 1-48.
- Luo, Y.-R., 2007, Comprehensive Handbook of Chemical Bond Energies, CRC Press.
- Shustorovich, E., and Sellers, H., 1998, “The UBI-QEP method: A practical theoretical approach to understanding chemistry on transition metal surfaces,” Surface Science Reports, 31(1-3), pp. 1-119.
- Sellers, H., and Shustorovich, E., 2002, “Intrinsic activation barriers and coadsorption effects for reactions on metal surfaces: unified formalism within the UBI-QEP approach,” Surface Science, 504, pp. 167-182.
- Shustorovich, E., and Zeigarnik, A. V., 2003, “The UBI-QEP treatment of polyatomic molecules without bond-energy partitioning,” Surface Science, 527(1-3), pp. 137-148.
- Frenklach, M., Wang, H., and Rabinowitz, M. J., 1992, “Optimization and analysis of large chemical kinetic mechanisms using the solution mapping method--combustion of methane,” Progress in Energy and Combustion Science, 18(1), pp. 47-73.
- Eränen, K., Lindfors, L.-E., Klingstedt, F., and Murzin, D. Y., 2003, “Continuous reduction of NO with octane over a silver/alumina catalyst in oxygen-rich exhaust gases: combined heterogeneous and surface-mediated homogeneous reactions,” Journal of Catalysis, 219(1), pp. 25-40.