This content is not included in your SAE MOBILUS subscription, or you are not logged in.
Conversion Performance Prediction of Thermal-Deteriorated Three-Way Catalysts: Surface Reaction Model Development Considering Platinum Group Metals and Co-Catalyst
ISSN: 0148-7191, e-ISSN: 2688-3627
Published September 05, 2021 by SAE International in United States
This content contains downloadable datasetsAnnotation ability available
Three-way catalyst (TWC) converters can purify harmful substances, such as carbon monoxide, nitrogen oxides, and hydrocarbons, from the exhaust gases of gasoline engines. However, large amounts of these substances may be emitted before the TWC reaches its light-off temperature during cold starts, and its performance may be impaired by thermal deterioration during high-load driving. In this work, a simulation model was developed using axisuite commercial software by Exothermia S.A to predict the light-off conversion performance of Pd/CeO2-ZrO2-Al2O3 catalysts with different degrees of thermal deterioration. The model considered detailed surface reactions and the main factor of the deterioration mechanism. In the detailed reaction mechanism, adsorption, desorption, and surface reactions of each gas species at active sites of the platinum group metal (PGM) particles were considered based on the Langmuir-Hinshelwood mechanism. Model gas experiments were performed to identify each reaction rate parameter. The PGM particles supported on the co-catalyst CeO2-ZrO2 had two types of active sites with different properties, i.e., sites in the particles' surface region and in a three-phase boundary (TPB) region PGM, CeO2−ZrO2 of the co-catalyst, and gas meet. The TPB active sites were more active than the PGM surface active sites. As the main factor of the catalyst deterioration mechanism, quantitative changes at the two active sites related to PGM sintering were included in the model. After sintering, the occupancy of the TPB active sites on the PGM decreased. The final TWC model was able to accurately predict the light-off conversion performance of a thermal-deteriorated Pd/CeO2-ZrO2-Al2O3 catalyst.
Data Sets - Support Documents
|Unnamed Dataset 1|
|Unnamed Dataset 2|
|Unnamed Dataset 3|
|Unnamed Dataset 4|
|Unnamed Dataset 5|
|Unnamed Dataset 6|
|Unnamed Dataset 7|
|Unnamed Dataset 8|
|Unnamed Dataset 9|
- Machida , M. , Fujiwara , A. , Yoshida , H. , and Ohyama , J. Deactivation Mechanism of Pd/CeO 2 -ZrO 2 Three-Way Catalysts Analyzed by Chassis-Dynamometer Tests and In Situ Diffuse Reflectance Spectroscopy ACS Catalyst 1 2019 6415 6424 10.1021/acscatal.9b01669
- Ramanathan , K. and Shekhar , C. Kinetic Parameters Estimation for Three Way Catalyst Modeling Industrial & Engineering Chemistry Research 50 2011 9960 9979 10.1021/ie200726j
- Chatterjee , D. , Deutschman , O. , and Warnatz , J. Detailed Surface Reaction Mechanism in a Three-Way Catalyst Faraday Discussions 119 2001 371 384 10.1039/B101968F
- 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. Product Res. Dev. 12 1973 294 301
- Kwon , H.J. , Baik , J.H. , Kwon , Y.T. , Nama , I.-S. et al. Detailed Reaction Kinetics Over Commercial Three-Way Catalysts Chemical Engineering Science 62 2007 5042 5047 10.1016/j.ces.2007.01.082
- 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 Chemical Engineering Science 241 2014 273 287 10.1016/j.cej.2013.12.039
- Mukadi , L.S. and Hayes , R.E. Modelling the Three-Way Catalytic Converter with Mechanistic Kinetics Using the Newton-Krylov Method on a Parallel Computer Computers and Chemical Engineering 26 2002 439 455 10.1016/S0098-1354(01)00763-3
- Stewart , J. , Douglas , R. , Goguet , A. , and Stere , C. Detailed Validation of an Automotive Catalysis Model Using Spatially Resolved Measurements within the Catalyst Substrate The Canadian Journal of Chemical Engineering 92 2014 1535 1541 10.1002/cjce.21993.
- Rankovic , N. , Nicolle , A. , Berthout , D. , and Da Costa , P. Kinetic Modeling Study of the Oxidation of Carbon Monoxide/Hydrogen Mixtures Over Pt/Al 2 O 3 and Rh/Al 2 O 3 Catalysts Journal of Physical. Chemistry C 115 41 2011 20225 20236 10.1021/jp205476y
- Lang , W. , Laing , P. , Cheng , Y. , Hubbard , C. et al. Co-oxidation of CO and Propylene on Pd/CeO 2 -ZrO 2 and Pd/Al 2 O 3 Monolith Catalysts: A Light-Off, Kinetics, and Mechanistic Study Applied Catalyst B: Environmental 218 2017 430 442 10.1016/j.apcatb.2017.06.064
- Set Naing , I. , Kristyawan , P.A. , Murakami , H. , Hinokuma , S. et al. Development of Detailed Surface Reaction Mechanism of C 2 H 4 /C 3 H 6 Oxidation on Pt/Al 2 O 3 Monolith Catalyst Based on Gas Phase and Surface Species Analyses Combustion Science and Technology 2020 10.1080/00102202.2020.1817905
- Vorotnikov , V. , Wang , S. , and Vlachos , D.G. Group Additivity for Estimating Thermochemical Properties of Furanic Compounds on Pd(111) Industrial & Engineering Chemistry Research 53 30 2014 11929 11938 10.1021/ie502049a
- Gong , J. , Wang , D. , Li , J. , Currier , N. et al. Dynamic Oxygen Storage Modeling in a Three-Way Catalyst for Natural Gas Engines: A Dual-Site and Shrinking-Core Diffusion Approach Applied Catalysis B: Environmental 203 2017 936 945 10.1016/j.apcatb.2016.11.005.
- Gong , J. , Wang , D. , Li , J. , Kamasamudram , K. et al. An Experimental and Kinetic Modeling Study of Aging Impact on Surface and Subsurface Oxygen Storage in Three-Way Catalysts Catalysis Today 320 2019 51 60 10.1016/j.cattod.2017.11.038.