Condition-dependent NOx adsorption/desorption over Pd/BEA: A combined microreactor and in situ DRIFTS study
Junjie Chen
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Investigation (lead), Methodology (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorJungkuk Lee
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Conceptualization (equal), Data curation (equal), Formal analysis (equal), Investigation (equal), Methodology (equal)
Search for more papers by this authorPrateek Khatri
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Formal analysis (supporting), Writing - review & editing (supporting)
Search for more papers by this authorTodd J. Toops
Energy and Transportation Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, USA
Contribution: Conceptualization (supporting), Funding acquisition (lead), Investigation (supporting)
Search for more papers by this authorCorresponding Author
Eleni A. Kyriakidou
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Correspondence
Eleni A. Kyriakidou, Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
Email: [email protected]
Contribution: Funding acquisition (lead), Project administration (lead), Resources (lead), Supervision (lead), Validation (lead), Writing - review & editing (equal)
Search for more papers by this authorJunjie Chen
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Investigation (lead), Methodology (lead), Writing - original draft (lead), Writing - review & editing (lead)
Search for more papers by this authorJungkuk Lee
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Conceptualization (equal), Data curation (equal), Formal analysis (equal), Investigation (equal), Methodology (equal)
Search for more papers by this authorPrateek Khatri
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Contribution: Formal analysis (supporting), Writing - review & editing (supporting)
Search for more papers by this authorTodd J. Toops
Energy and Transportation Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, USA
Contribution: Conceptualization (supporting), Funding acquisition (lead), Investigation (supporting)
Search for more papers by this authorCorresponding Author
Eleni A. Kyriakidou
Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA
Correspondence
Eleni A. Kyriakidou, Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.
Email: [email protected]
Contribution: Funding acquisition (lead), Project administration (lead), Resources (lead), Supervision (lead), Validation (lead), Writing - review & editing (equal)
Search for more papers by this authorThis 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 and the publisher, by accepting the article for publication, acknowledge that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide 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).
Abstract
Pd/BEA is chosen as a model passive NOx adsorber (PNA) to elucidate the effect of the feed gas composition on the NOx adsorption/desorption behavior. The Brønsted acid and the partially hydrolyzed framework Al (P-HAl(OH)) sites in HBEA adsorb NO and NO2 under dry conditions. Moreover, the performance of HBEA is not affected by CO, while CO inhibits nitrate formation and promotes NO adsorption via the Pd(NO)(CO) complexes formation over Pd/BEA. H2O inhibits NO adsorption over the Brønsted acid and P-HAl(OH) sites, and ionic Pd is the only active site for NOx adsorption under wet conditions. Furthermore, NO adsorption over hydrated Pd (Pd2+(OH)(NO)(H2O)3) is weaker than NO adsorption over bare ionic Pd (Z2[Pd2+(NO)], Z[Pd2+(OH)(NO)]). Dehydration of Pd2+(OH)(NO)(H2O)3 forms more stable Z[Pd2+(OH)(NO)] during desorption. The NO adsorption capacity of Pd/BEA improves in the presence of CO under both dry and wet conditions by forming a stable carbonyl–nitrosyl complex.
Supporting Information
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| aic18400-sup-0001-Supinfo.docxWord 2007 document , 4.2 MB | Data S1. Supporting information. |
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