Deposition of carbonaceous species over Ag/alumina catalysts for the HC-SCR of NOx under lean conditions: a qualitative and quantitative study

Abstract

The deposition of carbonaceous species on fresh and aged Ag/Al₂O₃ catalysts used for the selective catalytic reduction of NO_x (HC-SCR) was investigated by a combination of analytical techniques including SEM-EDXA, nitrogen physisorption, GC-MS and TGA. Time-on-stream (TOS) experiments were carried out to determine the level of deactivation over the catalysts. Short-term deactivation was monitored with a MicroGC with a short retention time. In addition, long-term deactivation was also investigated. Hexadecane, a paraffinic component that can be produced by decarboxylation and/or decarbonylation of natural oils and fats, and a standard Finnish commercial diesel fuel were used as the reducing agents. Finally, the influence of hydrogen on the carbonaceous deposition over the catalyst was also investigated. The NO-to-N₂ activity improved in the temperature range 200–500 °C as hexadecane and H₂ were used as reducing agents. In the case of commercial diesel fuel, a similar positive effect of H₂ on the activity was also observed, however, at somewhat higher temperature, e.g., 350–500 °C. The results from the qualitative and quantitative analyses of the carbon deposits on the catalysts are presented and discussed. Indications of decreased activity over the catalyst were found, especially at low temperatures (<350 °C). Nevertheless, only small amounts of carbon were found on the catalytic surface. It is suggested that the deactivation phenomenon could not only be attributed to the deposition of carbonaceous species on the catalysts surface but the dependence of the adsorption kinetics of the reacting species as a function of temperature and partial pressure should also be carefully taken into account.