Influence of the Alkali Promoter on the Activity and Stability of Transition Metal (Cu, Co, Fe) Based Structured Catalysts for the Simultaneous Removal of Soot and NOx

Structured catalysts prepared by means of coating cordierite monoliths with alumina-based suspensions containing transition metals such as Cu, Co and Fe and alkali/alkali-earth promoters such as K and Ba. Textural and structural features of these catalysts were analyzed by means of N-2 adsorption and SEM. Their activity in the simultaneous removal of soot and NOx was assayed in a lab-scale installation, using a carbon black as diesel surrogate. Catalysts exhibited significant activity in deNO(x) and soot oxidation. K and Ba enhanced both NOx adsorption and soot-catalyst contact. However Ba contributed to a greater extent to the adsorption of N-species, which moreover presented higher thermal stability than on K-catalysts, and K showed higher mobility than Ba. Thus, Ba-containing catalysts showed increased activity towards NOx reduction but shifted to higher temperatures in comparison to K-catalysts, which on the other hand resulted more active towards soot oxidation than Ba-ones. Fe-based catalyst turned out to be less active both in soot oxidation and NOx reduction than Co and Cu-based ones. Intensive calcination of the catalysts at 800 A degrees C for 5 h resulted in substantial loss of K and Ba. Loss of promoter depends, however, on the metal contained in the catalyst. In this sense Fe-containing catalysts showed higher stability. Calcination has a substantial effect on catalytic activity. Catalyst significantly lost their NOx adsorption capacity and showed similar activity than a catalyst prepared in absence of promoter, pointing to a substantial change in reaction mechanism and reaction predominantly occurring on metallic sites upon the loss of alkali/alkali-earth compound.