P. Granger et al., An attempt at modelling the activity of Pt-Rh/Al2O3 three-way catalysts inthe CO plus NO reaction, APP CATAL A, 208(1-2), 2001, pp. 369-379
This study deals with the kinetic behaviour of a Pt-Rh/Al2O3 three-way cata
lyst (TWC) in the CO + NO reaction close to the actual conditions. Practica
lly, it consists in validating a previous rate equation, established at 300
degreesC from a selected mechanism [P. Granger. J.J. Lecomte. L. Leclercq,
G. Leclercq, J. Catal. 175 (1998) 194], in a wider range of temperature pa
rticularly near 100% NO conversion. Preliminary calculations using a non li
near least square method lead to an estimation of pre-exponential factors (
for k, the rate constant of the rate limiting step and for lambda (CO) and
lambda (NO), the adsorption equilibrium constants of CO and NO). the activa
tion energy for the dissociation of adsorbed NO molecules. and the enthalpi
es of CO and NO adsorption (DeltaH(ads.CO) and DeltaH(ads.NO)) Thr temperat
ure-programmed conversion and selectivity curves obtained in differential c
onditions using a recycle fixed bed flow reactor have been modelled using t
hese adjusted parameters. Based on CO chemisorption observations it was fou
nd that a better fit is obtained by accounting for the coverage dependency
of DeltaH(ads.co) and DeltaH(ads.NO). Finally, we have attempted to quantif
y such effects. (C) 2001 Elsevier science B.V. All rights reserved.