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Article Dans Une Revue Journal of Physical Chemistry C Année : 2010

Detailed kinetic modeling study of NOx oxidation and storage and their interactions over Pt/Ba/Al2O3 monolith catalysts

Résumé

The concept of nitrogen oxide storage-redn. (NSR) is a promising aftertreatment technol. for reducing NOx emissions from lean-burn engine exhaust. The present work focuses on the first two steps of the overall NSR mechanism, namely, NO to NO2 oxidn. and NOx storage. The governing storage mechanisms are mainly elucidated on the model catalysts such as Pt/Ba/Al2O3. A unique detailed NO oxidn. kinetic model over Pt/Al2O3 was conceived based on literature data and validated over a wide range of exptl. conditions. This detailed mechanism was then globalized to obtain a Langmuir-Hinshelwood rate expression, which resulted in a reduced CPU cost in reactor computations. The global oxidn. model predicts various exptl. NO and NO2 profiles well. Further, a detailed kinetic model for NOx storage over Ba/Al2O3 was developed and validated against different exptl. data. Finally, the detailed oxidn. and storage schemes were successfully coupled and species spillover between the noble metal and the storage material was accounted for. The exptl. NO and NO2 profiles obtained from the NOx storage expts. over Pt/Ba/Al2O3 could be reproduced by the detailed coupled model. Reaction pathway analyses and sensitivity studies were performed to provide a more comprehensive insight into the system behavior. [on SciFinder(R)]
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Dates et versions

hal-00604794 , version 1 (29-06-2011)

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Nikola Rankovic, Andre Nicolle, Patrick da Costa. Detailed kinetic modeling study of NOx oxidation and storage and their interactions over Pt/Ba/Al2O3 monolith catalysts. Journal of Physical Chemistry C, 2010, 114 (15), pp.7102-7111. ⟨10.1021/jp100192u⟩. ⟨hal-00604794⟩
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