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Title: Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation

Abstract

Pd-impregnated Ce-based catalysts were tested for carbon monoxide (CO) and hydrocarbon (HC) oxidation under challenging low-temperature diesel combustion conditions. The results indicate that the light-off temperatures for CO over Pd/CeO 2, Pd/MnO x-CeO 2 (Pd/MC), and Pd/SnO 2-MnO x-CeO 2 (Pd/SMC) catalysts shift to higher temperatures in the presence of simulated diesel exhaust gas. The lowest T 50 for CO is observed over Pd/MC at 173 °C, whereas Pd/CeO 2 is shown to oxidize most of the HCs at temperatures below 400 °C. In all catalysts, the oxidation of HCs starts right after the onset of CO oxidation, revealing that the competitive adsorption of CO, NO, and alkenes controls the catalytic activity. Further evaluation of the catalytic activity in the presence of only CO and C 3H 6 reveals the immediate inhibiting effect of C 3H 6 at catalyst temperatures below 150 °C. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments performed over Pd/CeO 2, Pd/MC, and Pd/SMC show that C 3H 6 inhibits the formation of carbonyl species on Pd n+ sites, which limits the catalytic activity for CO. Lastly, such inhibition is observed on all supports, implying that the activity is independent of oxygen storage capacitymore » (OSC) or lattice oxygen reducibility of the supports in the presence of C 3H 6.« less

Authors:
 [1];  [2];  [2];  [1]; ORCiD logo [1]
  1. Univ. of South Carolina, Columbia, SC (United States). SmartState Center for Strategic Approaches to the Generation of Electricity (SAGE), Dept. of Chemical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines, and Emissions Research Center
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines and Emissions Research Center (FEERC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). National Transportation Research Center (NTRC)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1356945
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Emission Control Science & Technology
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2199-3629
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Low-temperature diesel oxidation; Pd; Solid solution; Hydrocarbon inhibition

Citation Formats

Wang, Chao, Binder, Andrew J., Toops, Todd J., Lauterbach, Jochen, and Sasmaz, Erdem. Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation. United States: N. p., 2016. Web. doi:10.1007/s40825-016-0056-9.
Wang, Chao, Binder, Andrew J., Toops, Todd J., Lauterbach, Jochen, & Sasmaz, Erdem. Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation. United States. doi:10.1007/s40825-016-0056-9.
Wang, Chao, Binder, Andrew J., Toops, Todd J., Lauterbach, Jochen, and Sasmaz, Erdem. Wed . "Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation". United States. doi:10.1007/s40825-016-0056-9. https://www.osti.gov/servlets/purl/1356945.
@article{osti_1356945,
title = {Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation},
author = {Wang, Chao and Binder, Andrew J. and Toops, Todd J. and Lauterbach, Jochen and Sasmaz, Erdem},
abstractNote = {Pd-impregnated Ce-based catalysts were tested for carbon monoxide (CO) and hydrocarbon (HC) oxidation under challenging low-temperature diesel combustion conditions. The results indicate that the light-off temperatures for CO over Pd/CeO2, Pd/MnOx-CeO2 (Pd/MC), and Pd/SnO2-MnOx-CeO2 (Pd/SMC) catalysts shift to higher temperatures in the presence of simulated diesel exhaust gas. The lowest T50 for CO is observed over Pd/MC at 173 °C, whereas Pd/CeO2 is shown to oxidize most of the HCs at temperatures below 400 °C. In all catalysts, the oxidation of HCs starts right after the onset of CO oxidation, revealing that the competitive adsorption of CO, NO, and alkenes controls the catalytic activity. Further evaluation of the catalytic activity in the presence of only CO and C3H6 reveals the immediate inhibiting effect of C3H6 at catalyst temperatures below 150 °C. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments performed over Pd/CeO2, Pd/MC, and Pd/SMC show that C3H6 inhibits the formation of carbonyl species on Pdn+ sites, which limits the catalytic activity for CO. Lastly, such inhibition is observed on all supports, implying that the activity is independent of oxygen storage capacity (OSC) or lattice oxygen reducibility of the supports in the presence of C3H6.},
doi = {10.1007/s40825-016-0056-9},
journal = {Emission Control Science & Technology},
number = 1,
volume = 3,
place = {United States},
year = {Wed Dec 07 00:00:00 EST 2016},
month = {Wed Dec 07 00:00:00 EST 2016}
}

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Works referenced in this record:

MnOx–CeO2 mixed oxide catalysts for complete oxidation of formaldehyde: Effect of preparation method and calcination temperature
journal, February 2006

  • Tang, Xingfu; Li, Yonggang; Huang, Xiumin
  • Applied Catalysis B: Environmental, Vol. 62, Issue 3-4, p. 265-273
  • DOI: 10.1016/j.apcatb.2005.08.004