Investigation of Aging Mechanisms in Lean NOx Traps
Lean NO{sub x} traps (LNTs) represent a promising technology for the abatement of NO{sub x} under lean conditions. Although LNTs are starting to find commercial application, the issue of catalyst durability remains problematic. LNT susceptibility to sulfur poisoning is the single most important factor determining effective catalyst lifetime. The NO{sub x} storage element of the catalyst has a greater affinity for SO{sub 3} than it does for NO{sub 2}, and the resulting sulfate is more stable than the stored nitrate. Although this sulfate can be removed from the catalyst by means of high temperature treatment under rich conditions, the required conditions give rise to deactivation mechanisms such as precious metal sintering, total surface area loss, and solid state reactions between the various oxides present. The principle objective of this project was to improve understanding of the mechanisms of lean NO{sub x} trap aging, and to understand the effect of washcoat composition on catalyst aging characteristics. The approach utilized involved detailed characterization of model catalysts prior to and after aging, in tandem with measurement of catalyst performance in NO{sub x} storage and reduction. In this manner, NO{sub x} storage and reduction characteristics were correlated with the evolution of catalyst physico-chemical properties upon aging. Rather than using poorly characterized proprietary catalysts, or simple model catalysts of the Pt/BaO/Al{sub 2}O{sub 3} type (representing the first generation of LNTs), Pt/Rh/BaO/Al{sub 2}O{sub 3} catalysts were employed which also incorporated CeO{sub 2} or CeO{sub 2}-ZrO{sub 2}, representing a model system which more accurately reflects current LNT formulations. Catalysts were prepared in which the concentration of each of the main components was systematically varied: Pt (50, 75 or 100 g/ft{sup 3}), Rh (10 or 20 g/ft{sup 3}), BaO (15, 30 or 45 g/L), and either CeO{sub 2} (0, 50 or 100 g/L) or CeO{sub 2}-ZrO{sub 2} (0, 50 or 100 g/L). A high surface area La-stabilized alumina was used to support the BaO phase. Catalysts were obtained by washcoating onto standard cordierite substrates, the total washcoat loading being set at 260 g/L. La-stabilized alumina was used as the balance. Subsequent to de-greening, the NO{sub x} storage and reduction characteristics of the catalysts were evaluated on a bench reactor, after which the catalysts were aged on a bench reactor to the equivalent of ca. 75,000 miles of road aging using a published accelerated aging protocol. The aged catalysts were then subjected to the same evaluation proecdure used for the de-greened catalysts. In addition to the use of standard physico-chemical analytical techniques for studying the fresh and aged model catalysts, use was made of advanced analytical tools for characterizing their NO{sub x} storage/reduction and sulfation/desulfation characteristics, such as Spatially resolved capillary-inlet Mass Spectrometry (SpaciMS) and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS).
- Research Organization:
- Univ. of Kentucky, Lexington, KY (United States)
- Sponsoring Organization:
- USDOE
- DOE Contract Number:
- FC26-05NT42631
- OSTI ID:
- 989105
- Country of Publication:
- United States
- Language:
- English
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