Chemical Engineering Journal, Vol.323, 347-360, 2017
Experimental and modeling study of CO and hydrocarbons light-off on various Pt-Pd/gamma-Al2O3 diesel oxidation catalysts
A global kinetic model is developed for the oxidation of mixtures of CO, C2H4 (ethylene), C7H8 (toluene), C6H14 (hexane), and C2H6 (ethane) over Pt-Pd/gamma-Al2O3 diesel oxidation catalysts with different Pt/Pd molar ratios (100:0, 75:25, 50:50, 25:75, 0:100). The kinetic model is based on bench flow reactor data obtained by temperature-programmed oxidation, ramping up the feed gas temperature at a fixed rate of 8 degrees C/min. The kinetic model is developed in stages starting with pure CO oxidation, followed by oxidation of the individual hydrocarbons (HCs) and then mixtures over all Pt/Pd ratios. Examination of the inhibition terms containing the effect of CO, HCs, and NO shows that CO has the most dominant inhibition effect on light-off over the range of conditions investigated. The kinetic model is validated with experimental data at different feed concentrations and is found to simulate the light-off behavior for all catalyst compositions with acceptable accuracy. Comparison of the light-off temperatures and trend investigation for kinetic parameters of CO, C2H4, and C7H8 in the mixture over all Pt/Pd ratios is also presented. Considering trade-offs between having a low light-off temperature, low deactivation impact on the catalyst, and higher conversion of HCs within the temperature domain of interest, the Pt/Pd (1:1) molar ratio is found to be the optimal catalyst under the conditions examined. (C) 2017 Elsevier B.V. All rights reserved.