Effect of lean/rich high temperature aging on NO oxidation and NOx storage/release of a fully formulated lean NOx trap

Nathan A. Ottinger, Todd J. Toops, Ke Nguyen, Bruce G. Bunting, Jane Howe

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

Commercial-intent lean NOx traps (LNTs) containing Pt, Pd, Rh, Ba, Ce, Zr, and other proprietary additives were thermally aged at 750, 880, 930, and 1070°C using lean/rich cycling and then investigated for effects of aging on NOx storage capacity, NO oxidation, NOx reduction, and materials properties. Additionally, DRIFTS analysis was used to determine the effects of high temperature aging on surface chemistry and NOx storage. As platinum group metal (PGM) dispersion decreases with aging, the NO turnover frequency (TOF) for NO oxidation at 200, 300, and 400°C is shown to increase. The fraction of stored NOx that is successfully reduced also increases with aging, and it is suggested that this is accounted for by a slower release of more stable NOx species resulting from thermal aging. NOx storage and NOx release experiments performed with DRIFTS at 200, 300, and 400°C indicate that a substantial amount of NOx is stored on Al2O3 as nitrates at 200 and 300°C before aging. However, almost no nitrates are seen on alumina after aging at 900 and 1000°C, resulting in a significant reduction in NOx storage capacity. This is most likely due to a 45% reduction in total surface area and a high temperature redispersion of Ba over remaining alumina sites. No evidence of BaAl2O4 was observed with XRD.

Original languageEnglish
Pages (from-to)486-494
Number of pages9
JournalApplied Catalysis B: Environmental
Volume101
Issue number3-4
DOIs
StatePublished - Jan 14 2011

Funding

This work was funded by the U.S. Department of Energy (DOE) , Office of FreedomCar and Vehicle Technologies , and the fully formulated LNTs were provided by Delphi, whose catalyst group is now part of Umicore. The catalyst samples were coated approximately 4 years ago and should not be considered representative of current formulations. The STEM measurements and analysis were sponsored by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of FreedomCar and Vehicle Technologies, as part of the High Temperature Materials Laboratory User Program, Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy under contract number DE-AC05-00OR22725.

FundersFunder number
Office of FreedomCar
Secretary for Energy Efficiency and Renewable Energy
U.S. Department of Energy
Oak Ridge National LaboratoryDE-AC05-00OR22725

    Keywords

    • DRIFTS
    • Fully formulated
    • Lean NO trap
    • NO release
    • NO storage capacity
    • PGM dispersion
    • STEM
    • Thermal aging
    • XRD

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