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An overview: Comparative kinetic behaviour of Pt, Rh and Pd in the NO + CO and NO + H2 reactions

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This paper reports a comparative kinetic investigation of the overall reduction of NO in the presence of CO or H2 over supported Pt-, Rh- and Pd-based catalysts. Different activity sequences have been established for the NO+H2 reaction Pt/Al2O3>Pd/Al2O3>Rh/Al2O3 and for the NO+CO reaction Rh/Al2O3>Pd/Al2O3> Pt/Al2O3. It was found that both reactions differ from the rate determining step usually ascribed to the dissociation of chemisorbed NO molecules. The rate enhancement observed for the NO+H2 reaction has been mainly related to the involvement of a dissociation step of chemisorbed NO molecules assisted by adjacent chemisorbed H atoms. The calculation of the kinetic and thermodynamic constants from steady-state rate measurements and subsequent comparisons show that Pd and Rh are predominantly covered by chemisorbed NO molecules in our operating conditions which could explain either changes in activity or in selectivity with the lack of ammonia formation on Rh/Al2O3 during the NO+H2 reaction. Interestingly, Pd and Rh exhibit similar selectivity behaviour towards the production of nitrous oxide (N2O) irrespective of the nature of the reducing agent (CO or H2). A weak partial pressure dependency of the selectivity is observed which can be related to the predominant formation of N2 via a reaction between chemisorbed NO molecules and N atoms, while over Pt-based catalysts the associative desorption of two adjacent N atoms would occur simultaneously. Such tendencies are still observed under lean conditions in the presence of an excess of oxygen. However, a detrimental effect is observed on the selectivity with an enhancement of the competitive H2+O2 reaction, and on the activity behaviour with a strong oxygen inhibiting effect on the rate of NO conversion, particularly on Rh.

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Authors and Affiliations

  1. Université des Sciences et Technologies de Lille, Laboratoire de Catalyse de Lille, UMR CNRS 8010, bâtiment C3, 59655, Villeneuve d’Ascq, France

    P. Granger, F. Dhainaut, P. Malfoy, A. S. Mamede, L. Leclercq & G. Leclercq

  2. Ecole Centrale de Lille, Laboratoire de Catalyse de Lille, UMR CNRS 8010, bâtiment C3, 59655, Villeneuve d’Ascq, France

    S. Pietrzik

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  1. P. Granger
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Granger, P., Dhainaut, F., Pietrzik, S. et al. An overview: Comparative kinetic behaviour of Pt, Rh and Pd in the NO + CO and NO + H2 reactions. Top Catal 39, 65–76 (2006). https://doi.org/10.1007/s11244-006-0039-0

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