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  4. Reaction pathways of methane abatement in Pd-Rh three-way catalyst in heavy duty applications: A combined approach based on exhaust analysis, model gas reactor and DRIFTS measurements
 
research article

Reaction pathways of methane abatement in Pd-Rh three-way catalyst in heavy duty applications: A combined approach based on exhaust analysis, model gas reactor and DRIFTS measurements

Wang, Moyu
•
Eggenschwiler, Panayotis Dimopoulos
•
Franken, Tanja
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October 15, 2021
Chemical Engineering Journal

Methane abatement pathways in Pd/Rh three-way catalysts have been investigated in three scales ranging from a vehicle application size catalyst, a model gas reactor and the catalyst in powder form. A special test rig was designed for the investigation of vehicle size catalysts, allowing sampling along the catalyst at discrete spatial locations, which are subject to different feed compositions. Dependent on the history of chemical environment of the catalyst, significant differences in methane conversion rate at identical feed have been identified. At steady state methane conversion rate was low and the reaction pathway was identified as limited to only direct oxidation by oxygen. Following a rich-to-lean transition, the catalyst exhibited more than 8 times higher methane conversion rates compared to steady state. The high methane conversion rates have been identified and attributed to the activation of methane steam reforming (SR) related to transient reduction of ceria. Methane SR efficiency decreased with time and the conversion rate finally converged to steady state levels. The findings were validated using a model gas reactor enabling analysis under well-defined feed compositions. The deactivation of SR was further analyzed with infrared spectroscopy (DRIFTS). Evidences from DRIFTS measurements showed that the deactivation was linked to the formation of carbonaceous species on the catalyst surface, most likely carbonates. The coherent results from engine exhaust analysis, model gas reactor and DRIFTS study give important insights in the activation and deactivation of methane reaction pathways. The results of this study suggest that catalyst formulation and operation strategies of methane conversion should focus on the stimulation of SR and the maintenance of catalyst activity towards SR through targeted periodic lean/rich transitions.

  • Details
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Type
research article
DOI
10.1016/j.cej.2021.129932
Web of Science ID

WOS:000671784800001

Author(s)
Wang, Moyu
Eggenschwiler, Panayotis Dimopoulos
Franken, Tanja
Ferri, Davide
Krocher, Oliver  
Date Issued

2021-10-15

Publisher

ELSEVIER SCIENCE SA

Published in
Chemical Engineering Journal
Volume

422

Article Number

129932

Subjects

Engineering, Environmental

•

Engineering, Chemical

•

Engineering

•

natural gas engine

•

three-way catalyst

•

steam reforming

•

transient operation

•

drifts

•

chemisorbed oxygen

•

complete oxidation

•

reaction-mechanism

•

shift catalysts

•

low-temperature

•

palladium

•

water

•

deactivation

•

platinum

•

stability

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
GR-KRO  
Available on Infoscience
July 31, 2021
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/180324
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