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A Study of Support Effects for CH4 and CO Oxidation over Pd Catalysts on ALD-Modified Al2O3

  • Xinyu Mao
  • Alexandre Foucher
  • Eric A. Stach
  • Raymond J. GorteEmail author
Article
  • 8 Downloads

Abstract

Interactions between a metal and its oxide support can influence CO and CH4 oxidation, but promotion by the support can be difficult to study because oxides can have different surface structures and surface areas. To focus on the chemical aspects of support promotion for CO and CH4 oxidation, this study investigated the effect of support composition on Pd catalysts by preparing uniform films of NiO, Co3O4, Fe2O3, MnO2, CeO2, and ZrO2 on γ-Al2O3 using Atomic Layer Deposition (ALD). The structure of the films was characterized by XRD and STEM, and catalysts with ~ 1-wt% Pd were examined for CO and CH4 oxidation. CeO2/γ-Al2O3 was unique among the supports in greatly stabilizing the Pd dispersion to 1173 K. Rates for CO oxidation were enhanced by the presence of CeO2, Fe2O3, and MnO2, while the other oxides had no promotional effect. For CH4 oxidation, only NiO and Co3O4 were modest promoters, while the other reducible oxides even showed a negative effect on rates. Possible reasons for the differences between CH4 and CO oxidation activities are discussed.

Graphical Abstract

Keywords

Methane oxidation CO oxidation Palladium Support effects Atomic Layer Deposition 

Notes

Acknowledgements

This work was funded by the Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, Grant No. DE-FG02-13ER16380. The STEM work was carried out in part at the Singh Center for Nanotechnology, part of the National Nanotechnology Coordinated Infrastructure Program, which is supported by the National Science Foundation Grant NNCI-1542153.

Supplementary material

10562_2019_2699_MOESM1_ESM.pdf (328 kb)
Supplementary material 1 Figure S1, DRIFTS spectra obtained for (a) 773K-Pd/CeO2/ Al2O3, (b) 1173K-Pd/CeO2/Al2O3, (c) 773K-Pd/Al2O3 and (d) 1173K-Pd/Al2O3, after exposure to 20 mL/min pure CO at room temperature. Figure S2 (a), differential steady-state rates of CH4 oxidation on ALD-prepared Co3O4/Al2O3 and Pd/ Co3O4/Al2O3; Figure S2 (b), differential steady-state rates of CH4 oxidation on ALD-prepared NiO/Al2O3 and Pd/ NiO/Al2O3 (PDF 327 KB)

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Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2019

Authors and Affiliations

  • Xinyu Mao
    • 1
  • Alexandre Foucher
    • 2
  • Eric A. Stach
    • 2
  • Raymond J. Gorte
    • 1
    • 2
    Email author
  1. 1.Department of Chemical and Biomolecular EngineeringUniversity of PennsylvaniaPhiladelphiaUSA
  2. 2.Department of Materials Science and EngineeringUniversity of PennsylvaniaPhiladelphiaUSA

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