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

  • Special Issue: 2016 CLEERS April 6-8, Ann Arbor, MI, USA
  • Published:
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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/CeO2, Pd/MnO x -CeO2 (Pd/MC), and Pd/SnO2-MnO x -CeO2 (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/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. 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.

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Acknowledgments

This work was supported by the South Carolina SmartState Center for Strategic Approaches to the Generation of Electricity (SAGE), a SPARC graduate research grant from the University of South Carolina, the University of South Carolina XPS facility, and the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Program. The authors wish to express their gratitude to program managers Ken Howden, Leo Breton, and Gurpreet Singh for their support. This manuscript has been co-authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the US Department of Energy. This research was performed, in part, using instrumentation (FEI Talos F200X STEM) provided by the Department of Energy, Office of Nuclear Energy, Fuel Cycle R&D Program, and the Nuclear Science User Facilities. The authors thank Dr. Michael J. Lance for the elemental mapping and imaging of particles.

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Authors and Affiliations

  1. SmartState Center for Strategic Approaches to the Generation of Electricity (SAGE), Department of Chemical Engineering, University of South Carolina, Columbia, SC, 29208, USA

    Chao Wang, Jochen Lauterbach & Erdem Sasmaz

  2. Fuels, Engines, and Emissions Research Center, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    Andrew J. Binder & Todd J. Toops

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  1. Chao Wang
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Correspondence to Erdem Sasmaz.

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This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the US Department of Energy. The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US 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 US 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).

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Wang, C., Binder, A.J., Toops, T.J. et al. Evaluation of Mn and Sn-Modified Pd-Ce-Based Catalysts for Low-Temperature Diesel Exhaust Oxidation. Emiss. Control Sci. Technol. 3, 37–46 (2017). https://doi.org/10.1007/s40825-016-0056-9

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