Experimental study of mass transfer limitations in Fe- and Cu-zeolite-based NH 3-SCR monolithic catalysts

Abstract

An experimental study of steady-state selective catalytic reduction (SCR) of NO x with NH 3 on both Fe-ZSM-5 and Cu-ZSM-5 monolithic catalysts was carried out to investigate the extent of mass transfer limitations in various SCR reactions. Catalysts with different washcoat loadings, washcoat thicknesses and lengths were synthesized for this purpose. SCR system reactions examined included NO oxidation, NH 3 oxidation, standard SCR, fast SCR and NO 2 SCR. Comparisons of conversions obtained on catalysts with the same washcoat volumes but different washcoat thicknesses indicated the presence of washcoat diffusion limitations. NH 3 oxidation, an important side reaction in SCR system, showed the presence of washcoat diffusion limitations starting at 350 °C on Fe-zeolite and 300 °C on Cu-zeolite catalysts. Washcoat diffusion limitations were observed for the standard SCR reaction (NH 3+NO+O 2) on both Fe-zeolite (≥350 °C) and Cu-zeolite (≥250 °C). For the fast (NH 3+NO+NO 2) and NO 2 SCR (NH 3+NO 2) reactions, diffusion limitations were observed throughout the temperature range explored (200–550 °C). The experimental findings are corroborated by theoretical analyses. Even though the experimentally observed differences in conversions clearly indicate the presence of washcoat diffusion limitations, the contribution of external mass transfer was also found to be important under certain conditions. The transition temperatures for shifts in controlling regimes from kinetic to washcoat diffusion to external mass transfer are determined using simplified kinetics. The findings indicate the necessity of inclusion of mass transfer limitations in SCR modeling, catalyst design and optimization.