Affiliation: | aInstitute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Hönggerberg, CH-8093 Zürich, Switzerland bUmicore AG & Co. KG, Rodenbacher Chaussee 4, D-63403 Hanau-Wolfgang, Germany |
Abstract: | Differences in the NOx storage-reduction (NSR) behavior of Pt/Ba/CeO2 and Pt/Ba/Al2O3 have been identified and traced to their different chemical and structural properties. The results show that Pt/Ba/CeO2 exhibits inferior NOx storage and, particularly, reduction (regeneration) activity compared to the Al2O3 supported catalyst. The incomplete reduction of the stored NOx-species in Pt/Ba/CeO2 seems to be caused by a faster and more profound reoxidation of Pt particles during the lean period as evidenced by in situ X-ray absorption spectroscopy. Interestingly, the reduction activity could be significantly improved by a pre-reduction step at mild conditions. Exposure of the Pt/Ba/CeO2 catalyst to reducing H2 atmosphere in the temperature range 300–500 °C lead to a moderate increase of Pt particle size which beneficially influenced the regeneration activity. In contrast, pre-reduction at temperatures above 500 °C was unfavorable and resulted in a severe decrease of the regeneration activity, probably due to migration of the partially reduced CeO2 onto the surface of Pt particles. |