Spatiotemporal distribution of NOx storage and impact on NH3 and N2O selectivities during lean/rich cycling of a Ba-based lean NOx trap catalyst
- ORNL
- Institute of Chemical Technology, Prague, Czech Republic
We summarize results from an investigation of the spatiotemporal distribution of NO{sub x} storage and intermediate gas species in determining the performance of a fully formulated, Ba-based, lean NO{sub x} trap catalyst under lean/rich cycling conditions. By experimentally resolving spatiotemporal profiles of gas composition, we found that stored NO{sub x} was significantly redistributed along the monolith axis during the rich phase of the cycle by release and subsequent downstream re-adsorption. Sulfur poisoning of upstream NO{sub x} storage sites caused the active NO{sub x}-storage zone to be displaced downstream. This axial displacement in turn influenced rich-phase NO{sub x} release and re-adsorption. As sulfur poisoning increased, NH3 slip at the catalyst exit also increased due to its formation closer to the catalyst outlet and decreased exposure to downstream oxidation by surface oxygen. N{sub 2}O formation was found to be associated with nitrate reduction rather than oxidation of NH3 by stored oxygen. We propose that the observed evolution of N{sub 2}O selectivity with sulfation can be explained by changes in the spatiotemporal distribution of NO{sub x} storage resulting in either increased or decreased number of precious-metal sites surrounded by nitrates.
- Research Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines and Emissions Research Center (FEERC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). National Transportation Research Center (NTRC)
- Sponsoring Organization:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- DOE Contract Number:
- DE-AC05-00OR22725
- OSTI ID:
- 1038795
- Journal Information:
- Catalysis Today, Vol. 184, Issue 1; ISSN 0920-5861
- Country of Publication:
- United States
- Language:
- English
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