PILLARED CLAYS AS SUPERIOR CATALYSTS FOR SELECTIVE CATALYTIC REDUCTION OF NITRIC OXIDE

摘要

Removal of NO{sub x} (NO + NO{sub 2}) from exhaust gases is a challenging subject. V{sub 2}O{sub 5}-based catalysts are commercial catalysts for selective catalytic reduction (SCR) with NH{sub 3} for stationary sources. However, for diesel and lean-burn gasoline engines in vehicles, hydrocarbons would be the preferred reducing agents over NH{sub 3} because of the practical problems associated with the use of NH{sub 3} (i.e., handling and slippage through the reactor). The noble-metal three-way catalysts are not effective under these conditions. The first catalyst found to be active for selective catalytic reduction of NO by hydrocarbons in the presence of excess oxygen was copper exchanged ZSM-5 and other zeolites, reported in 1990 by Iwamoto in Japan and Held et al. in Germany. Although Cu-ZSM-5 is very active and the most intensively studied catalyst, it suffers from severe deactivation in engine tests, mainly due to H{sub 2}O and SO{sub 2}. In this project, we found that ion-exchanged pillared clays and MCM-41 catalysts showed superior SCR activities of NO with hydrocarbon. All Cu{sup 2+}-exchanged pillared clays showed higher SCR activities than Cu-ZSM-5 reported in the literature. In particular, H{sub 2}O and SO{sub 2} only slightly deactivated the SCR activity of Cu-TiO{sub 2}-PILC, whereas severe deactivation was observed for Cu-ZSM-5. Moreover, Pt/MCM-41 provided the highest specific NO reduction rates as compared with other Pt doped catalysts, i.e., Pt/Al{sub 2}O{sub 3}, Pt/SiO{sub 2} and Pt/ZSM-5. The Pt/MCM-41 catalyst also showed a good stability in the presence of H{sub 2}O and SO{sub 2}.