Palladium-exchanged MFI-type zeolites in the catalytic reduction of nitrogen monoxide by methane. Influence of the Si/Al ratio on the activity and the hydrothermal stability

摘要

Pd-exchanged MFI-type zeolites containing 3.7 and 0.7 framework aluminium atoms per unit cell (corresponding to Si/Al ratios of 25 and 131) were found active in the selective reduction of nitrogen monoxide in the presence of excess oxygen. Upon steaming at 800°C, both catalysts exhibited the total loss of their catalytic activity in the reduction of NO. Such a behaviour was ascribed to the complete aggregation of Pd ions into large metal particles on the external surface of the zeolite crystals. Both supports, although maintaining their crystallinity, are shown to experience extended dealumination upon steaming. Although the loss of Pd exchange capacity could partially explain the Pd migration and sintering, a mechanism involving the formation of mobile Pd hydroxyl entities condensing into PdO particles outside the zeolite crystallites is preferred.