Characterization of Pt,Sn/Mg(Al)O Catalysts for Light Alkane Dehydrogenation by FT-IR Spectroscopy and Catalytic Measurements
The Pt function in Pt,Sn/Mg(Al)O and in Pt/Mg(Al)O catalysts has been studied by a combination of catalytic testing for ethane dehydrogenation at 450−650 °C under a C2H6/H2/CO2/N2/Ar = 10:1.6:6.8:5.9:75.7 flow and Fourier transform infrared spectroscopy (FT-IR), using CO as a probe molecule. The aci...
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Veröffentlicht in: | Journal of physical chemistry. C 2007-10, Vol.111 (40), p.14732-14742 |
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Hauptverfasser: | , , , , |
Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | The Pt function in Pt,Sn/Mg(Al)O and in Pt/Mg(Al)O catalysts has been studied by a combination of catalytic testing for ethane dehydrogenation at 450−650 °C under a C2H6/H2/CO2/N2/Ar = 10:1.6:6.8:5.9:75.7 flow and Fourier transform infrared spectroscopy (FT-IR), using CO as a probe molecule. The acid−base properties of the support were also investigated by FT-IR, using CH3CN as a probe molecule. CO adsorption experiments revealed the presence of Pt terraces, as well as Pt sites with low coordination number (steps, edges, corners, or defects) on Pt/Mg(Al)O. The same experiments on Pt,Sn/Mg(Al)O revealed that Sn covers the steps, corners, edges, and defects of the Pt particles, thus developing simultaneously a geometric and a chemical effect on the surface properties of the exposed Pt atoms. Accordingly, the ethane dehydrogenation reaction proceeds with a lower activation energy over Pt,Sn/Mg(Al)O compared to Pt/Mg(Al)O. Further, Sn addition leads to more selective and more stable ethane dehydrogenation catalysts. The higher dehydrogenation selectivity of Pt,Sn catalysts was correlated to the masking of low-coordinated Pt sites. The Pt/Mg(Al)O and Pt,Sn/Mg(Al)O catalysts were subjected to an activation procedure consisting of several test−regeneration cycles. Good correlation was found between the number of accessible Pt sites and the catalytic activity after each cycle. |
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ISSN: | 1932-7447 1932-7455 |
DOI: | 10.1021/jp074686u |