Local ammonia storage and ammonia inhibition in a monolithic copper-beta zeolite SCR catalyst

Xavier Auvray, William P. Partridge, Jae Soon Choi, Josh A. Pihl, Aleksey Yezerets, Krishna Kamasamudram, Neal W. Currier, Louise Olsson

Research output: Contribution to journalArticlepeer-review

34 Scopus citations

Abstract

Selective catalytic reduction of NO with NH 3 was studied on a Cu-beta zeolite catalyst, with specific focus on the distributed NH 3 capacity utilization and inhibition. In addition, several other relevant catalyst parameter distributions were quantified including the SCR zone, or catalyst region where SCR occurs, and NO and NH 3 oxidation. We show that the full NH 3 capacity (100% coverage) is used within the SCR zone for a range of temperatures. By corollary, unused NH 3 capacity exists downstream of the SCR zone. Consequently, the unused capacity relative to the total capacity is indicative of the portion of the catalyst unused for SCR. Dynamic NH 3 inhibition distributions, which create local transient conversion inflections, are measured. Dynamic inhibition is observed where the gas phase NH 3 and NO concentrations are high, driving rapid NH 3 coverage buildup and SCR. Accordingly, we observe dynamic inhibition at low temperatures and in hydrothermally aged states, but predict its existence very near the catalyst front in higher conversion conditions where we did not specifically monitor its impact. While this paper addresses some general distributed SCR performance parameters including Oxidation and SCR zone, our major new contributions are associated with the NH 3 capacity saturation within the SCR zone and dynamic inhibition distributions and the associated observations. These new insights are relevant to developing accurate models, designs and control strategies for automotive SCR catalyst applications.

Original languageEnglish
Pages (from-to)144-152
Number of pages9
JournalApplied Catalysis B: Environmental
Volume126
DOIs
StatePublished - Sep 25 2012

Funding

Notice. This submission was sponsored by a contractor of the United States Government under contract DE-AC05-00OR22725 with the United States Department of Energy. The United States Government retains, and the publisher, by accepting this submission for publication, acknowledges that the United States Government retains, a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this submission, or allow others to do so, for United States Government purposes. This work is a collaboration between Oak Ridge National Laboratory, Competence Centre for Catalysis at Chalmers University and Cummins Inc. This research was sponsored by the U.S. Department of Energy , Office of Energy Efficiency and Renewable Energy , Vehicle Technologies Program , with Ken Howden and Gurpreet Singh as the Program Managers and the Swedish Foundation for Strategic Research ( F06-0006 ).

FundersFunder number
U.S. Department of Energy
Office of Energy Efficiency and Renewable Energy
Stiftelsen för Strategisk ForskningF06-0006

    Keywords

    • Ammonia
    • Cu-beta
    • Distributed reactions
    • NH capacity
    • NH inhibition
    • NO
    • SCR
    • Zeolite

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