New operation strategy for driving the selectivity of NOx reduction to N2, NH3 or N2O during lean/rich cycling of a lean NOx trap catalyst

David Mráček, Petr Kočí, Jae Soon Choi, William P. Partridge

Research output: Contribution to journalArticlepeer-review

39 Scopus citations

Abstract

Periodical regeneration of NOx storage catalyst (also known as lean NOx trap) by short rich pulses of CO, H2 and hydrocarbons is necessary for the reduction of nitrogen oxides adsorbed on the catalyst surface. Ideally, the stored NOx is converted into N2, but N2O and NH3 by-products can be formed as well, particularly at low-intermediate temperatures. The N2 and N2O products are formed concurrently in two peaks. The primary peaks appear immediately after the rich-phase inception, and tail off with the breakthrough of the reductant front accompanied by NH3 product. The secondary N2 and N2O peaks then appear at the rich-to-lean transition as a result of reactions between surface-deposited reductants/intermediates (CO, HC, NH3, NCO) and residual stored NOx under increasingly lean conditions.Based on these mechanistic insights, we propose and demonstrate a novel strategy for driving the selectivity of the secondary peaks towards desired products. It is based on a transition phase of neutral or slightly lean (nearly stoichiometric) character inserted between the rich and the fully lean phase. This strategy allows more complete regeneration of the catalyst with higher N2 yield and without the undesired formation of a secondary N2O peak. Furthermore, NH3 can be formed during this slightly lean transition phase without any CO or hydrocarbons breakthrough. Such ammonia formation is desirable in the exhaust gas aftertreatment systems combining LNT with passive SCR technology.

Original languageEnglish
Pages (from-to)109-114
Number of pages6
JournalApplied Catalysis B: Environmental
Volume182
DOIs
StatePublished - Mar 1 2016

Funding

This work has been financially supported by the Czech Ministry of Education (Project LH 12086 ), the Specific University Research (MSMT No. 20/2015 ) and the U.S. Department of Energy (DOE) Vehicle Technologies Office (program managers: Gurpreet Singh, Ken Howden and Leo Breton). Notice: This manuscript has been co-authored by UT-Battelle, LLC , under Contract No. DE-AC0500OR22725 with the U.S. Department of Energy . The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for the United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

FundersFunder number
U.S. Department of Energy
UT-BattelleDE-AC0500OR22725
Ministerstvo Školství, Mládeže a TělovýchovyLH 12086, 20/2015

    Keywords

    • Automotive catalysts
    • Exhaust gas aftertreatment
    • Lean NO trap
    • NO formation
    • NO reduction
    • NO storage catalyst

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