Effects of the Nitridation of Y and USY Zeolites on their Catalytic Activity for the Base Catalyzed Knoevenagel Condensation

This contribution reports on the preparation, physicochemical characterization and catalytic performances of nitrided zeolites in the Knoevenagel condensation reaction. These basic materials were prepared by subjecting one Y zeolite (Si/Al ratio of 2.6) and two ultrastable Y zeolites (Si/Al ratio of 13 and 37) to nitridation, i.e., treatment with ammonia at high temperature. Both the amount and the chemical nature of incorporated nitrogen species were controlled by the nitridation temperature. Namely, an increase of the temperature induces an increase of the nitrogen content and the appearance of nitrogenous species in the following order of increasing temperature: NH₄ ⁺, adsorbed NH₃, –NH₂, >NH and >N–. The nitridation occurred practically in the same manner whatever the Si/Al ratio of the starting material. However, from a catalytic point of view different behavior was observed. No direct correlation was found with the nitrogen content of the samples. Nitrided zeolites were found to exhibit catalytic activity as long as the zeolitic framework was maintained.