This content is not included in
your SAE MOBILUS subscription, or you are not logged in.
Experimental and Kinetic Modeling of Degreened and Aged Three-way Catalysts: Aging Impact on Oxygen Storage Capacity and Catalyst Performance
Technical Paper
2018-01-0950
ISSN: 0148-7191, e-ISSN: 2688-3627
This content contains downloadable datasets
Annotation ability available
Sector:
Language:
English
Abstract
The aging impact on oxygen storage capacity (OSC) and catalyst performance was investigated on one degreened and one aged (hydrothermally aged at 955 °C for 50 h) commercial three-way catalyst (TWC) by experiments and modeling. The difference of OSC between the degreened and aged TWCs was dependent on catalyst temperature. The largest difference was found at 600 °C, at which the amount of OSC decreased by 45.5%. Catalyst performance was evaluated through lightoff tests at two simulated engine exhaust conditions (lean and rich) on a micro-reactor. The aging impact on the catalyst performance was different under lean and rich environments and investigated separately. At the lean condition, oxidation of CO and C3H6 was significantly suppressed while oxidation of C3H8 was relatively less degraded. At the rich condition, the inhibition effect was more pronounced on the aged TWC and inhibiting hydrocarbon species from C3H6 partial oxidation can survive at temperatures up to 450 °C. However, NO reduction activity declined less compared to CO and C3H6 oxidation. More NH3 formed at low temperature and N2O formation was suppressed on the aged TWC.
A generic TWC model including a dual-site oxygen storage sub-model and PGM kinetics was developed to predict the aging impact on dynamic OSC and catalyst performance. The PGM kinetics include oxidation of H2, CO, and hydrocarbons as well as water-gas shift (WGS) and hydrocarbon steam reforming. NO reduction kinetics including N2O and NH3 formation and decomposition were also considered. The TWC models were calibrated on the degreened and aged TWCs separately based on experimental data. With the dual-site OSC model and calibrated kinetics, the dynamic OSC and lightoff performance on the fresh and aged TWCs were successfully predicted. The resulting changes of the OSC as well as lightoff performance due to aging were quantified and discussed with the help of the TWC models.
Recommended Content
Authors
Citation
Gong, J., Wang, D., Li, J., Kamasamudram, K. et al., "Experimental and Kinetic Modeling of Degreened and Aged Three-way Catalysts: Aging Impact on Oxygen Storage Capacity and Catalyst Performance," SAE Technical Paper 2018-01-0950, 2018, https://doi.org/10.4271/2018-01-0950.Data Sets - Support Documents
Title | Description | Download |
---|---|---|
Unnamed Dataset 1 | ||
Unnamed Dataset 2 | ||
Unnamed Dataset 3 | ||
Unnamed Dataset 4 |
Also In
References
- Gandhi , H.S. , Graham , G.W. , and McCabe , R.W. Automotive Exhaust Catalysis J. Catal. 216 1-2 433 442 2003 10.1016/S0021-9517(02)00067-2
- Gong , J. and Rutland , C. A Quasi-Dimensional NO x Emission Model for Spark Ignition Direct Injection (SIDI) Gasoline Engines SAE Technical Paper 2013-01-1311 2013 10.4271/2013-01-1311
- Hori , C.E. , Permana , H. , Ng , K.Y.S. , Brenner , A. et al. Thermal Stability of Oxygen Storage Properties in a Mixed CeO2-ZrO2 System Appl. Catal. B Environ. 16 105 117 1998 10.1016/S0926-3373(97)00060-X
- Baik , J.H. , Kwon , H.J. , Kwon , Y.T. , Nam , I.-S. , and Oh , S.H. Effects of Catalyst Aging on the Activity and Selectivity of Commercial Three-way Catalysts Top. Catal. 42-43 1-4 337 340 2007 10.1007/s11244-007-0201-3
- Heo , I. , Choung , J.W. , Kim , P.S. , Nam , I.-S. et al. The Alteration of the Performance of Field-Aged Pd-Based TWCs towards CO and C3H6 Oxidation Appl. Catal. B Environ 92 1-2 114 125 2009 10.1016/j.apcatb.2009.07.016
- Zhao , M. , Shen , M. , and Wang , J. Effect of Surface Area and Bulk Structure on Oxygen Storage Capacity of Ce0.67Zr0.33O2 J. Catal. 248 2 258 267 2007 10.1016/j.jcat.2007.03.005
- Christou , S.Y. , Bradshaw , H. , Butler , C. , Darab , J. , and Efstathiou , A.M. Effect of Thermal Aging on the Transient Kinetics of Oxygen Storage and Release of Commercial CexZr1−xO2-based Solids Top. Catal. 52 13-20 2013 2018 2009 10.1007/s11244-009-9402-2
- Schmieg , S.J. and Belton , D.N. Effect of Hydrothermal Aging on Oxygen Storage/Release and Activity in a Commercial Automotive Catalyst Appl. Catal. B, Environ. 6 2 127 144 1995 10.1016/0926-3373(95)00011-9
- Bunluesin , T. , Gottea , R.J. , and Grahamb , G.W. CO oxidation for the Characterization of Reducibility in Oxygen Storage Components of Three-Way Automotive Catalysts Appl. Catal. B, Environ. 14 105 115 1997
- Gong , J. , Wang , D. , Li , J. , Currier , N. , and Yezerets , A. Dynamic Oxygen Storage Modeling in a Three-Way Catalyst for Natural Gas Engines: A Dual-Site and Shrinking-Core Diffusion Approach Appl. Catal. B Environ. 203 936 945 2017 10.1016/j.apcatb.2016.11.005
- Lambrou , P.S. , Costa , C.N. , Christou , S.Y. , and Efstathiou , A.M. Dynamics of Oxygen Storage and Release on Commercial Aged Pd-Rh Three-way Catalysts and their Characterization by Transient Experiments Appl. Catal. B Environ. 54 4 237 250 2004 10.1016/j.apcatb.2004.06.018
- Sabatini , S. , Kil , I. , Hamilton , T. , Wuttke , J. et al. Characterization of Aging Effect on Three-Way Catalyst Oxygen Storage Dynamics SAE Technical Paper 2016-01-0971 2016 10.4271/2016-01-0971
- Gong , J. , Wang , D. , Brahma , A. , Li , J. et al. Lean Breakthrough Phenomena Analysis for TWC OBD on a Natural Gas Engine using a Dual-Site Dynamic Oxygen Storage Capacity Model SAE Technical Paper 2017-01- 0962 2017 10.4271/2017-01-0962
- Koltsakis , G.C. , Konstantinidis , P.A. , and Stamatelos , A.M. Development and Application Range of Mathematical Models for 3-way Catalytic Converters Appl. Catal. B Environ. 12 2-3 161 191 1997 10.1016/S0926-3373(96)00073-2
- Tsinoglou , D.N. , Koltsakis , G.C. , and Peyton Jones , J.C. Oxygen Storage Modeling in Three-Way Catalytic Converters Ind. Eng. Chem. Res. 41 5 1152 1165 2002 10.1021/ie010576c
- Gong , J. and Rutland , C. Three Way Catalyst Modeling with Ammonia and Nitrous Oxide Kinetics for a Lean Burn Spark Ignition Direct Injection (SIDI) Gasoline Engine SAE Technical Paper 2013-01-1572 2013 10.4271/2013-01-1572
- Koč , P. , Kubíč , M. , and Marek , M. Modeling of Three-Way-Catalyst Monolith Converters with Microkinetics and Diffusion in the Washcoat Ind. Eng. Chem. Res. 43 16 4503 4510 2004 10.1021/ie034137k
- Gong , J. , Wang , D. , Li , J. , Kamasamudram , K. et al. Catal. Today 2017 10.1016/j.cattod.2017.11.038
- Depcik , C. and Assanis , D. One-Dimensional Automotive Catalyst Modeling Prog. Energy Combust. Sci. 31 4 308 369 2005 10.1016/j.pecs.2005.08.001
- Gong , J. , Narayanaswamy , K. , and Rutland , C.J. Heterogeneous Ammonia Storage Model for NH3 -SCR Modeling Ind. Eng. Chem. Res. 55 20 5874 5884 2016 10.1021/acs.iecr.6b01097
- AVL BOOST Aftertreatment Manual, AVL 2016 http://www.avl.com
- Yao , H.C. and Yao , Y.F.Y. Ceria in Automotive Exhaust Catalysts J. Catal. 265 254 265 1984 10.1016/0021-9517(84)90371-3
- Schimming , S.M. , Foo , G.S. , LaMont , O.D. , Rogers , A.K. et al. Kinetics of Hydrogen Activation on Ceria-Zirconia J. Catal. 329 335 347 2015 10.1016/j.jcat.2015.05.027
- Zhao , M. , Shen , M. , and Wang , J. Effect of Surface Area and Bulk Structure on Oxygen Storage Capacity of Ce0.67Zr0.33O2 J. Catal. 248 2 258 267 2007 10.1016/j.jcat.2007.03.005
- Trovarelli , A. Catalytic Properties of Ceria and CeO2-Containing Materials Catal. Rev. 38 4 439 520 1996 10.1080/01614949608006464
- Kaspar , J. , Fornasiero , P. , and Graziani , M. Use of CeO2 -Based Oxides in the Three-Way Catalysis Catal. Today 50 285 298 1999
- Olsson , L. , Blint , R.J. , and Fridell , E. Global Kinetic Model for Lean NO × Traps Ind. Eng. Chem. Res. 44 3021 3032 2005
- Voltz , S.E. , Morgan , C.R. , Liederman , D. , and Jacob , S.M. Kinetic Study of Carbon Monoxide and Propylene Oxidation on Platinum Catalysts Ind. Eng. Chem. Prod. Res. Dev. 12 4 294 301 1973 10.1021/i360048a006
- Brinkmeier , C. , Eigenberger , G. , Büchner , S. , and Donnerstag , A. Transient Emissions of a SULEV Catalytic Converter System Dynamic Simulation vs. Dynamometer Measurements SAE Technical Paper 2003-01-1001 2003 724 2003 10.4271/2003-01-1001
- Montreuil , C.N. , Williams , S.C. , and Adamczyk , A.A. Converters: Laboratory Experiments and SAE Technical Paper 1992
- Koci , P. 2015 CLEERS Workshop 2015
- Ramanathan , K. and Sharma , C.S. Kinetic Parameters Estimation for Three Way Catalyst Modeling Ind. Eng. Chem. Res. 50 17 9960 9979 2011 10.1021/ie200726j
- Burch , R. , Crittle , D.J. , and Hayes , M.J. C-H Bond Activation in Hydrocarbon Oxidation on Heterogeneous Catalysts Catal. Today 47 1-4 229 234 1999 10.1016/S0920-5861(98)00303-4
- Michael , B.C. , Donazzi , A. , and Schmidt , L.D. Effects of H2O and CO2 Addition in Catalytic Partial Oxidation of Methane on Rh J. Catal. 265 1 117 129 2009 10.1016/j.jcat.2009.04.015
- Hecker , W.C. and Bell , A.T. Reduction of NO by CO over Silica-Supported Rhodium: Infrared and Kinetic Studies J. Catal. 84 200 215 1983
- Granger , P. and Parvulescu , V.I. Catalytic NOx Abatement Systems for Mobile Sources : From Three-Way to Lean Burn after-Treatment Technologies Chem. Rev. 111 3155 3207 2011
- Papapolymerou , G.A. and Schmidt , L.D. Unimolecular Reactions of NO, N20, NO2, and NH3 on Rh and Ptt Langmuir 1 488 495 1985
- Kang , S.B. , Han , S.J. , Nam , I.S. , Cho , B.K. et al. Detailed Reaction Kinetics for Double-Layered Pd/Rh Bimetallic TWC Monolith Catalyst Chem. Eng. J. 241 273 287 2014 10.1016/j.cej.2013.12.039
- Bedrane , S. , Descorme , C. , and Duprez , D. Towards the Comprehension of Oxygen Storage Processes on Model Three-Way Catalysts Catal. Today 73 233 238 2002 10.1016/S0920-5861(02)00005-6
- Holder , R. , Bollig , M. , Anderson , D.R. , and Hochmuth , J.K. A Discussion on Transport Phenomena and Three-Way Kinetics of Monolithic Converters Chem. Eng. Sci. 61 24 8010 8027 2006 10.1016/j.ces.2006.09.030
- Hahn , C. , Endisch , M. , Schott , F.J.P. , and Kureti , S. Kinetic Modelling of the NOx Reduction by H2 on Pt/WO3/ZrO2 Catalyst in Excess of O2 Appl. Catal. B Environ. 168-169 x 429 440 2015 10.1016/j.apcatb.2014.12.033
- Oh , S.H. and Triplett , T. Reaction Pathways and Mechanism for Ammonia Formation and Removal Over Palladium-Based Three-Way Catalysts: Multiple Roles of CO Catal. Today 231 22 32 2014 10.1016/j.cattod.2013.11.048
- Hazlett , M.J. , Moses-Debusk , M. , Parks , J.E. , Allard , L. , and Epling , W.S. Kinetic and Mechanistic Study of Bimetallic Pt-Pd/Al2O3 Catalysts for CO and C3H6 Oxidation Appl. Catal. B Environ. 202 404 417 2017
- Herrmann , M. , Hayes , R.E. , and Votsmeier , M. Propene Induced Reversible Deactivation Effects in Diesel Oxidation Catalysts Appl. Catal. B Environ. 220 446 461 2018 10.1016/j.apcatb.2017.08.026