Effect of framework Al pairing on NO storage properties of Pd-CHA passive NOx adsorbers

Joseph R. Theis; Justin Ura; Andrew Bean Getsoian; Vitaly Y. Prikhodko; Calvin R. Thomas; Josh A. Pihl; Trevor M. Lardinois; Rajamani Gounder; Xinyi Wei; Yaying Ji; Robert B. Pace; Mark Crocker

doi:10.1016/j.apcatb.2022.122074

Effect of framework Al pairing on NO storage properties of Pd-CHA passive NOx adsorbers

Joseph R. Theis, Justin Ura, Andrew Bean Getsoian, Vitaly Y. Prikhodko, Calvin R. Thomas, Josh A. Pihl, Trevor M. Lardinois, Rajamani Gounder, Xinyi Wei, Yaying Ji, Robert B. Pace, Mark Crocker

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19 Scopus citations

Abstract

Three Pd/H-CHA samples were prepared containing 53.0 %, 10.8 % and 6.5 % paired Al sites at near fixed Si/Al ratio and similar Pd loading. According to H₂ temperature-programmed reduction, Pd was present almost exclusively as isolated cations in the two samples containing the higher concentrations of paired Al sites, whereas in the other sample PdO was also present. Simulated lean cold start tests on the fresh samples conducted in a microflow reactor showed that the sample containing PdO stored the lowest amount of NOx. When tested with CO/H₂, the sample containing 53.0 % paired Al sites showed significantly better storage capacity than the other samples and deactivated less rapidly upon sequential tests. Experiments using lean gasoline engine exhaust revealed similar trends. This study showed that a high concentration of paired Al sites in Pd/H-CHA is beneficial for NOx storage capacity, thermal durability, and minimizing deactivation in the presence of CO/H₂.

Original language	English
Article number	122074
Journal	Applied Catalysis B: Environmental
Volume	322
DOIs	https://doi.org/10.1016/j.apcatb.2022.122074
State	Published - Mar 2023

Funding

This work was funded by the Department of Energy Office of Vehicle Technologies award number DEEE0008213 . This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States government or any agency thereof. This work was funded by the Department of Energy Office of Vehicle Technologies award number DEEE0008213. This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States government or any agency thereof.

Keywords

Chabazite
Framework Al
LTNA
Low temperature NOx adsorber
PNA
Paired Al sites
SSZ-13

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10.1016/j.apcatb.2022.122074

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@article{72763496b9a84b299b8ceff652eff947,

title = "Effect of framework Al pairing on NO storage properties of Pd-CHA passive NOx adsorbers",

abstract = "Three Pd/H-CHA samples were prepared containing 53.0 %, 10.8 % and 6.5 % paired Al sites at near fixed Si/Al ratio and similar Pd loading. According to H2 temperature-programmed reduction, Pd was present almost exclusively as isolated cations in the two samples containing the higher concentrations of paired Al sites, whereas in the other sample PdO was also present. Simulated lean cold start tests on the fresh samples conducted in a microflow reactor showed that the sample containing PdO stored the lowest amount of NOx. When tested with CO/H2, the sample containing 53.0 % paired Al sites showed significantly better storage capacity than the other samples and deactivated less rapidly upon sequential tests. Experiments using lean gasoline engine exhaust revealed similar trends. This study showed that a high concentration of paired Al sites in Pd/H-CHA is beneficial for NOx storage capacity, thermal durability, and minimizing deactivation in the presence of CO/H2.",

keywords = "Chabazite, Framework Al, LTNA, Low temperature NOx adsorber, PNA, Paired Al sites, SSZ-13",

author = "Theis, {Joseph R.} and Justin Ura and Getsoian, {Andrew Bean} and Prikhodko, {Vitaly Y.} and Thomas, {Calvin R.} and Pihl, {Josh A.} and Lardinois, {Trevor M.} and Rajamani Gounder and Xinyi Wei and Yaying Ji and Pace, {Robert B.} and Mark Crocker",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier B.V.",

year = "2023",

month = mar,

doi = "10.1016/j.apcatb.2022.122074",

language = "English",

volume = "322",

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AU - Theis, Joseph R.

AU - Ura, Justin

AU - Getsoian, Andrew Bean

AU - Prikhodko, Vitaly Y.

AU - Thomas, Calvin R.

AU - Pihl, Josh A.

AU - Lardinois, Trevor M.

AU - Gounder, Rajamani

AU - Wei, Xinyi

AU - Ji, Yaying

AU - Pace, Robert B.

AU - Crocker, Mark

PY - 2023/3

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N2 - Three Pd/H-CHA samples were prepared containing 53.0 %, 10.8 % and 6.5 % paired Al sites at near fixed Si/Al ratio and similar Pd loading. According to H2 temperature-programmed reduction, Pd was present almost exclusively as isolated cations in the two samples containing the higher concentrations of paired Al sites, whereas in the other sample PdO was also present. Simulated lean cold start tests on the fresh samples conducted in a microflow reactor showed that the sample containing PdO stored the lowest amount of NOx. When tested with CO/H2, the sample containing 53.0 % paired Al sites showed significantly better storage capacity than the other samples and deactivated less rapidly upon sequential tests. Experiments using lean gasoline engine exhaust revealed similar trends. This study showed that a high concentration of paired Al sites in Pd/H-CHA is beneficial for NOx storage capacity, thermal durability, and minimizing deactivation in the presence of CO/H2.

AB - Three Pd/H-CHA samples were prepared containing 53.0 %, 10.8 % and 6.5 % paired Al sites at near fixed Si/Al ratio and similar Pd loading. According to H2 temperature-programmed reduction, Pd was present almost exclusively as isolated cations in the two samples containing the higher concentrations of paired Al sites, whereas in the other sample PdO was also present. Simulated lean cold start tests on the fresh samples conducted in a microflow reactor showed that the sample containing PdO stored the lowest amount of NOx. When tested with CO/H2, the sample containing 53.0 % paired Al sites showed significantly better storage capacity than the other samples and deactivated less rapidly upon sequential tests. Experiments using lean gasoline engine exhaust revealed similar trends. This study showed that a high concentration of paired Al sites in Pd/H-CHA is beneficial for NOx storage capacity, thermal durability, and minimizing deactivation in the presence of CO/H2.

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KW - Framework Al

KW - LTNA

KW - Low temperature NOx adsorber

KW - PNA

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DO - 10.1016/j.apcatb.2022.122074

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JO - Applied Catalysis B: Environmental

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ER -

Effect of framework Al pairing on NO storage properties of Pd-CHA passive NOx adsorbers

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