Condition-dependent NOx adsorption/desorption over Pd/BEA: A combined microreactor and in situ DRIFTS study

Junjie Chen; Jungkuk Lee; Prateek Khatri; Todd J. Toops; Eleni A. Kyriakidou

doi:10.1002/aic.18400

Condition-dependent NO_x adsorption/desorption over Pd/BEA: A combined microreactor and in situ DRIFTS study

Junjie Chen, Jungkuk Lee, Prateek Khatri, Todd J. Toops, Eleni A. Kyriakidou

Applied Catalysis&Emissions Res. Group

Research output: Contribution to journal › Article › peer-review

Abstract

Pd/BEA is chosen as a model passive NO_x adsorber (PNA) to elucidate the effect of the feed gas composition on the NO_x 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 NO_x 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.

Original language	English
Article number	e18400
Journal	AIChE Journal
Volume	70
Issue number	6
DOIs	https://doi.org/10.1002/aic.18400
State	Published - Jun 2024

Funding

The UB authors were supported by start‐up funding from the Department of Chemical and Biological Engineering, University at Buffalo, SUNY. This work was partially sponsored by the U.S. Department of Energy (DOE) Vehicle Technologies Office (VTO). The authors gratefully acknowledge the support and direction of Siddiq Khan, Kevin Stork, and Gurpreet Singh. 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 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 ).

Funders	Funder number
Department of Chemical and Biological Engineering, University at Buffalo
U.S. Department of Energy
State University of New York
UT-Battelle

Keywords

Pd/BEA
adsorption sites
adsorption/desorption mechanism
passive NO adsorber

Access to Document

10.1002/aic.18400

Cite this

@article{3cefdbb84e5c45eb89fce6134d947cf6,

title = "Condition-dependent NOx adsorption/desorption over Pd/BEA: A combined microreactor and in situ DRIFTS study",

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 Br{\o}nsted 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 Br{\o}nsted 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.",

keywords = "Pd/BEA, adsorption sites, adsorption/desorption mechanism, passive NO adsorber",

author = "Junjie Chen and Jungkuk Lee and Prateek Khatri and Toops, {Todd J.} and Kyriakidou, {Eleni A.}",

note = "Publisher Copyright: {\textcopyright} 2024 American Institute of Chemical Engineers.",

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AU - Lee, Jungkuk

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AU - Toops, Todd J.

AU - Kyriakidou, Eleni A.

PY - 2024/6

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N2 - 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.

AB - 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.

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