NO2 Reaction Pathways With NH3 on an Fe-Zeolite SCR Catalyst

Abstract

One approach for nitrogen oxides (NOx) emission control of medium duty diesel engines is through the use of a combination Lean NOx Trap and Selective Catalytic Reduction (LNT-SCR) catalyst system. In this system, part of the NOx conversion occurs via an NH3 SCR catalyst that is dependent on the NO2 to NOx ratio of the feed gas with NO2 being a more advantageous oxidizer. One benefit of using this system is the conversion of NO to NO2 over the LNT which increases the NO2:NOx ratio of the feed gas to the SCR catalyst. An experimental study has been performed to investigate the NO2-NH3 reaction for an Fe-based zeolite SCR catalyst using a bench top flow reactor. The increase in NO2 concentration at the inlet of the SCR results in the formation of large quantities of N2O from 200°C to 400°C. Further experiments determined that N2O and NH3 react above 350°C. This has led to a hypothesis that one primary SCR reaction (Slow SCR) can be replaced with two reaction steps featuring NH3, NO2, and N2O. As a result, this paper proposes five NOx reduction reactions as part of a global mechanism, which would account for the observed experimental behavior.