A comparative study of silver- and palladium-exchanged zeolites in propylene and nitrogen oxide adsorption and desorption for cold-start applications

Eleni A. Kyriakidou; Jungkuk Lee; Jae Soon Choi; Michael Lance; Todd J. Toops

doi:10.1016/j.cattod.2020.05.019

A comparative study of silver- and palladium-exchanged zeolites in propylene and nitrogen oxide adsorption and desorption for cold-start applications

Eleni A. Kyriakidou, Jungkuk Lee, Jae Soon Choi, Michael Lance, Todd J. Toops

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

37 Scopus citations

Abstract

Silver and palladium ion-exchanged BEA zeolites (Si/Al = 12.5) and silver ion-exchanged ZSM-5 zeolites (Si/Al = 15) were studied for their ability to adsorb and desorb propylene and NO under simulated diesel exhaust conditions. The adsorption experiment results demonstrated the excellent ability of bare BEA zeolites to adsorb propylene, but only a small amount of NO. The presence of H₂O inhibited the adsorption of both C₃H₆ and NO. Ion-exchanging BEA zeolites with Ag (1.2 and 5.1 wt.% Ag/BEA) attenuated the inhibiting effect of H₂O on C₃H₆ adsorption, while NO storage remained inhibited. Adsorption experiments indicated that C₃H₆ and NO competed with each other for Pd sites with C₃H₆ showing stronger adsorption compared to NO, whereas Ag sites preferentially adsorbed C₃H₆. DRIFTS data indicated the formation of nitrate, formate and acetate species on Ag and Pd, while C₃H₆ and NO adsorption was also observed on the zeolite hydroxyl groups in the absence of H₂O. However, the C₃H₆ and NO adsorption on the zeolite hydroxyl groups was significantly inhibited in the presence of H₂O. Additionally, nitrosyl, acrolein and carbonate species were formed over 1.0 wt.% Pd/BEA. The effluent analysis during the temperature-programmed desorption in the DRIFTS reactor revealed that adsorbed C₃H₆ and NO reacted during the release to form oxidation reaction byproducts. The 1.0 wt.% Pd/BEA zeolite showed the greatest oxidation ability during desorption with the majority of stored C₃H₆ converted to CO₂.

Original language	English
Pages (from-to)	220-233
Number of pages	14
Journal	Catalysis Today
Volume	360
DOIs	https://doi.org/10.1016/j.cattod.2020.05.019
State	Published - Jan 15 2021

Funding

This research was sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office (Program Managers: Gurpreet Singh and Ken Howden). The access to the FEI Talos F200X STEM was provided by the Department of Energy, Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science Facilities. We thank Dr. Michael J. Lance at ORNL for the microscopic analysis. Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 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 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). This research was sponsored by the U.S. Department of Energy , Office of Energy Efficiency and Renewable Energy , Vehicle Technologies Office (Program Managers: Gurpreet Singh and Ken Howden). The access to the FEI Talos F200X STEM was provided by the Department of Energy, Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science Facilities. We thank Dr. Michael J. Lance at ORNL for the microscopic analysis. Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 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 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 ).

Keywords

BEA
DRIFTS
Hydrocarbon trap
Ion-exchange
Passive NO adsorber
ZSM-5
Zeolites

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10.1016/j.cattod.2020.05.019

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title = "A comparative study of silver- and palladium-exchanged zeolites in propylene and nitrogen oxide adsorption and desorption for cold-start applications",

abstract = "Silver and palladium ion-exchanged BEA zeolites (Si/Al = 12.5) and silver ion-exchanged ZSM-5 zeolites (Si/Al = 15) were studied for their ability to adsorb and desorb propylene and NO under simulated diesel exhaust conditions. The adsorption experiment results demonstrated the excellent ability of bare BEA zeolites to adsorb propylene, but only a small amount of NO. The presence of H2O inhibited the adsorption of both C3H6 and NO. Ion-exchanging BEA zeolites with Ag (1.2 and 5.1 wt.% Ag/BEA) attenuated the inhibiting effect of H2O on C3H6 adsorption, while NO storage remained inhibited. Adsorption experiments indicated that C3H6 and NO competed with each other for Pd sites with C3H6 showing stronger adsorption compared to NO, whereas Ag sites preferentially adsorbed C3H6. DRIFTS data indicated the formation of nitrate, formate and acetate species on Ag and Pd, while C3H6 and NO adsorption was also observed on the zeolite hydroxyl groups in the absence of H2O. However, the C3H6 and NO adsorption on the zeolite hydroxyl groups was significantly inhibited in the presence of H2O. Additionally, nitrosyl, acrolein and carbonate species were formed over 1.0 wt.% Pd/BEA. The effluent analysis during the temperature-programmed desorption in the DRIFTS reactor revealed that adsorbed C3H6 and NO reacted during the release to form oxidation reaction byproducts. The 1.0 wt.% Pd/BEA zeolite showed the greatest oxidation ability during desorption with the majority of stored C3H6 converted to CO2.",

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author = "Kyriakidou, {Eleni A.} and Jungkuk Lee and Choi, {Jae Soon} and Michael Lance and Toops, {Todd J.}",

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AU - Kyriakidou, Eleni A.

AU - Lee, Jungkuk

AU - Choi, Jae Soon

AU - Lance, Michael

AU - Toops, Todd J.

PY - 2021/1/15

Y1 - 2021/1/15

N2 - Silver and palladium ion-exchanged BEA zeolites (Si/Al = 12.5) and silver ion-exchanged ZSM-5 zeolites (Si/Al = 15) were studied for their ability to adsorb and desorb propylene and NO under simulated diesel exhaust conditions. The adsorption experiment results demonstrated the excellent ability of bare BEA zeolites to adsorb propylene, but only a small amount of NO. The presence of H2O inhibited the adsorption of both C3H6 and NO. Ion-exchanging BEA zeolites with Ag (1.2 and 5.1 wt.% Ag/BEA) attenuated the inhibiting effect of H2O on C3H6 adsorption, while NO storage remained inhibited. Adsorption experiments indicated that C3H6 and NO competed with each other for Pd sites with C3H6 showing stronger adsorption compared to NO, whereas Ag sites preferentially adsorbed C3H6. DRIFTS data indicated the formation of nitrate, formate and acetate species on Ag and Pd, while C3H6 and NO adsorption was also observed on the zeolite hydroxyl groups in the absence of H2O. However, the C3H6 and NO adsorption on the zeolite hydroxyl groups was significantly inhibited in the presence of H2O. Additionally, nitrosyl, acrolein and carbonate species were formed over 1.0 wt.% Pd/BEA. The effluent analysis during the temperature-programmed desorption in the DRIFTS reactor revealed that adsorbed C3H6 and NO reacted during the release to form oxidation reaction byproducts. The 1.0 wt.% Pd/BEA zeolite showed the greatest oxidation ability during desorption with the majority of stored C3H6 converted to CO2.

AB - Silver and palladium ion-exchanged BEA zeolites (Si/Al = 12.5) and silver ion-exchanged ZSM-5 zeolites (Si/Al = 15) were studied for their ability to adsorb and desorb propylene and NO under simulated diesel exhaust conditions. The adsorption experiment results demonstrated the excellent ability of bare BEA zeolites to adsorb propylene, but only a small amount of NO. The presence of H2O inhibited the adsorption of both C3H6 and NO. Ion-exchanging BEA zeolites with Ag (1.2 and 5.1 wt.% Ag/BEA) attenuated the inhibiting effect of H2O on C3H6 adsorption, while NO storage remained inhibited. Adsorption experiments indicated that C3H6 and NO competed with each other for Pd sites with C3H6 showing stronger adsorption compared to NO, whereas Ag sites preferentially adsorbed C3H6. DRIFTS data indicated the formation of nitrate, formate and acetate species on Ag and Pd, while C3H6 and NO adsorption was also observed on the zeolite hydroxyl groups in the absence of H2O. However, the C3H6 and NO adsorption on the zeolite hydroxyl groups was significantly inhibited in the presence of H2O. Additionally, nitrosyl, acrolein and carbonate species were formed over 1.0 wt.% Pd/BEA. The effluent analysis during the temperature-programmed desorption in the DRIFTS reactor revealed that adsorbed C3H6 and NO reacted during the release to form oxidation reaction byproducts. The 1.0 wt.% Pd/BEA zeolite showed the greatest oxidation ability during desorption with the majority of stored C3H6 converted to CO2.

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KW - DRIFTS

KW - Hydrocarbon trap

KW - Ion-exchange

KW - Passive NO adsorber

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AN - SCOPUS:85085623231

SN - 0920-5861

VL - 360

SP - 220

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JO - Catalysis Today

JF - Catalysis Today

ER -

A comparative study of silver- and palladium-exchanged zeolites in propylene and nitrogen oxide adsorption and desorption for cold-start applications

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