Silica-Based Catalyst Supports Are Inert, Are They Not?

Striking Differences in Ethanol Decomposition Reaction Originated from Meso- and Surface-Fine-Structure Evidenced by Small-Angle X-ray Scattering

András Sápi, Dorina G. Dobó, Dániel Sebok, Gyula Halasi, Koppány L. Juhász, Ákos Szamosvölgyi, Péter Pusztai, Erika Varga, Ildikó Kálomista, G. Galbács, Á. Kukovecz, Z. Kónya

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

6.6 nm Pt nanoparticles with narrow size distribution were anchored on mostly identical, amorphous silica supports (SBA-15, MCF-17, silica foam) and were tested in ethanol decomposition reactions at <300°C. The reaction on the Pt/SBA-15 was ∼2 times faster (0.073 molecules·site-1·s-1) compared with Pt/MCF-17 (0.042 molecules·site-1·s-1) and Pt/SF (0.040 molecules·site-1·s-1) at 300°C. In the case of Pt/SF, selectivity toward acetaldehyde was ∼2 times higher compared with the Pt/MCF-17 and Pt/SBA-15 catalysts. In the case of Pt/MCF-17 and Pt/SBA-15, the methane to acetaldehyde ratio was ∼4 times higher compared with the Pt/SF catalyst. The ethene selectivity was ∼1.5 times higher in the case of Pt/SBA-15 compared with Pt/MCF-17 and Pt/SF. Small-angle X-ray scattering (SAXS) studies showed striking differences in the nature of the surface of the different silica supports, which may be responsible for the activation and selectivity deviation in ethanol decomposition reactions. The SBA-15 has the most disordered mesostructure, and SF has a fine surface structure with a diffuse phase boundary, which may result in the high activity and varying selectivity, respectively. (Graph Presented).

Original languageEnglish
Pages (from-to)5130-5136
Number of pages7
JournalJournal of Physical Chemistry C
Volume121
Issue number9
DOIs
Publication statusPublished - Mar 9 2017

Fingerprint

X ray scattering
Catalyst supports
Silicon Dioxide
Ethanol
ethyl alcohol
Acetaldehyde
selectivity
fine structure
Silica
silicon dioxide
Decomposition
decomposition
catalysts
acetaldehyde
scattering
Catalysts
x rays
Catalyst selectivity
Phase boundaries
Surface structure

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

Silica-Based Catalyst Supports Are Inert, Are They Not? Striking Differences in Ethanol Decomposition Reaction Originated from Meso- and Surface-Fine-Structure Evidenced by Small-Angle X-ray Scattering. / Sápi, András; Dobó, Dorina G.; Sebok, Dániel; Halasi, Gyula; Juhász, Koppány L.; Szamosvölgyi, Ákos; Pusztai, Péter; Varga, Erika; Kálomista, Ildikó; Galbács, G.; Kukovecz, Á.; Kónya, Z.

In: Journal of Physical Chemistry C, Vol. 121, No. 9, 09.03.2017, p. 5130-5136.

Research output: Contribution to journalArticle

Sápi, András ; Dobó, Dorina G. ; Sebok, Dániel ; Halasi, Gyula ; Juhász, Koppány L. ; Szamosvölgyi, Ákos ; Pusztai, Péter ; Varga, Erika ; Kálomista, Ildikó ; Galbács, G. ; Kukovecz, Á. ; Kónya, Z. / Silica-Based Catalyst Supports Are Inert, Are They Not? Striking Differences in Ethanol Decomposition Reaction Originated from Meso- and Surface-Fine-Structure Evidenced by Small-Angle X-ray Scattering. In: Journal of Physical Chemistry C. 2017 ; Vol. 121, No. 9. pp. 5130-5136.
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abstract = "6.6 nm Pt nanoparticles with narrow size distribution were anchored on mostly identical, amorphous silica supports (SBA-15, MCF-17, silica foam) and were tested in ethanol decomposition reactions at <300°C. The reaction on the Pt/SBA-15 was ∼2 times faster (0.073 molecules·site-1·s-1) compared with Pt/MCF-17 (0.042 molecules·site-1·s-1) and Pt/SF (0.040 molecules·site-1·s-1) at 300°C. In the case of Pt/SF, selectivity toward acetaldehyde was ∼2 times higher compared with the Pt/MCF-17 and Pt/SBA-15 catalysts. In the case of Pt/MCF-17 and Pt/SBA-15, the methane to acetaldehyde ratio was ∼4 times higher compared with the Pt/SF catalyst. The ethene selectivity was ∼1.5 times higher in the case of Pt/SBA-15 compared with Pt/MCF-17 and Pt/SF. Small-angle X-ray scattering (SAXS) studies showed striking differences in the nature of the surface of the different silica supports, which may be responsible for the activation and selectivity deviation in ethanol decomposition reactions. The SBA-15 has the most disordered mesostructure, and SF has a fine surface structure with a diffuse phase boundary, which may result in the high activity and varying selectivity, respectively. (Graph Presented).",
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AU - Sápi, András

AU - Dobó, Dorina G.

AU - Sebok, Dániel

AU - Halasi, Gyula

AU - Juhász, Koppány L.

AU - Szamosvölgyi, Ákos

AU - Pusztai, Péter

AU - Varga, Erika

AU - Kálomista, Ildikó

AU - Galbács, G.

AU - Kukovecz, Á.

AU - Kónya, Z.

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AB - 6.6 nm Pt nanoparticles with narrow size distribution were anchored on mostly identical, amorphous silica supports (SBA-15, MCF-17, silica foam) and were tested in ethanol decomposition reactions at <300°C. The reaction on the Pt/SBA-15 was ∼2 times faster (0.073 molecules·site-1·s-1) compared with Pt/MCF-17 (0.042 molecules·site-1·s-1) and Pt/SF (0.040 molecules·site-1·s-1) at 300°C. In the case of Pt/SF, selectivity toward acetaldehyde was ∼2 times higher compared with the Pt/MCF-17 and Pt/SBA-15 catalysts. In the case of Pt/MCF-17 and Pt/SBA-15, the methane to acetaldehyde ratio was ∼4 times higher compared with the Pt/SF catalyst. The ethene selectivity was ∼1.5 times higher in the case of Pt/SBA-15 compared with Pt/MCF-17 and Pt/SF. Small-angle X-ray scattering (SAXS) studies showed striking differences in the nature of the surface of the different silica supports, which may be responsible for the activation and selectivity deviation in ethanol decomposition reactions. The SBA-15 has the most disordered mesostructure, and SF has a fine surface structure with a diffuse phase boundary, which may result in the high activity and varying selectivity, respectively. (Graph Presented).

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