Research ArticleChemistry

Subsurface catalysis-mediated selectivity of dehydrogenation reaction

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Science Advances  10 Aug 2018:
Vol. 4, no. 8, eaar5418
DOI: 10.1126/sciadv.aar5418
  • Fig. 1 Structural characterization of the Pt and PtFe nanoparticle catalysts.

    TEM images of leached (A) PtFe@Pt/SiO2 and (B) PtFe@Pt/SBA-15 via same reduction treatment. The insets in (A) and (B) show the size distribution of PtFe@Pt/SiO2 and PtFe@Pt/SBA-15, respectively. (C) Concentration of Fe and Pt in acid solution as a function of leaching time. The values from the unreduced sample are included as a reference. (D) EDS line profiles of leached PtFe@Pt/SBA-15 (inset of the nanoparticle). a.u., arbitrary units. (E) XPS Fe2p peaks from unleached PtFe/SBA-15 and leached PtFe@Pt/SBA-15 catalysts after air exposure at room temperature. (F) XANES Fe K-edge structures from PtFe/SBA-15 and PtFe@Pt/SBA-15 catalysts after air exposure at room temperature. Standard Fe foil and Fe2O3 samples are included as references. NP, nanoparticle.

  • Fig. 2 Catalytic performance in PDH.

    (A) C3H6 selectivity and C3H8 conversion over different unleached Pt-3dTM/SBA-15 catalysts. (B) C3H8 conversion and (C) C3H6 selectivity over leached PtFe@Pt/SBA-15 and Pt/SBA-15 catalysts. (D) Summed selectivity of CH4, C2H6, and C2H4 by-products as a function of reaction time. (E) TPO profiles of spent Pt/SBA-15 and PtFe@Pt/SBA-15 catalysts.

  • Fig. 3 Relationship between C3H6 selectivity and d-band center shifting.

    Relationship between experimental C3H6 selectivity and calculated d-band center positions over different catalysts.

  • Fig. 4 Calculated energy barriers for PDH.

    Energy barriers for dehydrogenation steps of propane on Pt and Pt-3dTM@Pt. The dotted lines indicate the desorption barrier of C3H6* to gaseous C3H6.

  • Schema 1 Model structures.

    Reasonable design of efficient Pt-3dTM@Pt catalysts for PDH reaction.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/8/eaar5418/DC1

    Fig. S1. XRD and TEM characterization of the Pt and PtFe nanoparticles.

    Fig. S2. The EDS line profiles of unleached PtFe/SBA-15 catalyst.

    Fig. S3. XPS Pt4f peaks from PtFe and PtFe@Pt catalysts.

    Fig. S4. TPO profiles from spent catalysts.

    Fig. S5. C3H6-TPD of Pt and PtFe catalysts.

    Fig. S6. Relative PDH reactivity of Pt and different Pt-3dTM catalysts.

    Table S1. Calculated d-band center and adsorption energies of C3H6.

  • Supplementary Materials

    This PDF file includes:

    • Fig. S1. XRD and TEM characterization of the Pt and PtFe nanoparticles.
    • Fig. S2. The EDS line profiles of unleached PtFe/SBA-15 catalyst.
    • Fig. S3. XPS Pt4f peaks from PtFe and PtFe@Pt catalysts.
    • Fig. S4. TPO profiles from spent catalysts.
    • Fig. S5. C3H6-TPD of Pt and PtFe catalysts.
    • Fig. S6. Relative PDH reactivity of Pt and different Pt-3dTM catalysts.
    • Table S1. Calculated d-band center and adsorption energies of C3H6.

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