2006 AIChE Annual Meeting
(233e) Product Speciation during Regeneration of Lean NoX Traps
Authors
Daw, C. S. - Presenter, Oak Ridge National Laboratory
Larson, R. S., Sandia National Laboratory
Pihl, J. A., Oak Ridge National Laboratory
Chakravarthy, .. V. K., Oak Ridge National Laboratory
Formation of products other than N2 during regeneration of a fully formulated lean NOx trap (LNT) catalyst was investigated using a bench-scale flow reactor. Both NH3 and N2O were observed during the regeneration phase of fast lean/rich cycles that simulated engine operation. Formation of both byproducts increased with higher reductant concentrations and lower temperatures. Steady flow experiments were used to decouple the regeneration reactions from the NOx storage and release processes. This approach enabled a detailed investigation into the reactions that cause both formation and destruction of byproducts. Pseudo-steady state experiments with simultaneous flow of NOx and reductant indicated that high concentrations of CO or H2 drive the reduction reactions toward NH3 formation, while mixtures that are stoichiometric for N2 formation favor N2. These experiments also showed that NH3 is readily oxidized by both NO and O2 over the LNT catalyst. The steady state experiments were used to develop a detailed microkinetic mechanism for the regeneration process. Simulations performed with a model incorporating the regeneration mechanism showed good agreement with the steady flow experimental results.