On the thermal stabilization of carbon-supported SiO2 catalysts by phosphorus: evaluation in the oxidative dehydrogenation of ethylbenzene to styrene and a comparison with relevant catalysts

Valeriya Zarubina, Hesamoddin Talebi, Harrie Jansma, Kinga Góra-Marek, Christian Nederlof, Freek Kapteijn, Michiel Makkee, Ignacio Melián-Cabrera*

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

A strategy to enhance the thermal stability of C/SiO2 hybrids for the O2-based oxidative dehydrogenation of ethylbenzene to styrene (ST) by P addition is proposed. The preparation consists of the polymerization of furfuryl alcohol (FA) on a mesoporous precipitated SiO2. The polymerization is catalyzed by oxalic acid (OA) at 160 °C (FA:OA = 250). Phosphorous was added as H3PO4 after the polymerization and before the pyrolysis that was carried out at 700 °C and will extend the overall activation procedure. Estimation of the apparent activation energies reveals that P enhances the thermal stability under air oxidation, which is a good indication for the ODH tests. Catalytic tests show that the P/C/SiO2 hybrids are readily active, selective and indeed stable in the applied reactions conditions for 60 h time on stream. Coke build-up during the reaction attributed to the P-based acidity is substantial, leading to a reduction of the surface area and pore volume. The comparison with a conventional MWCNT evidences that the P/C/SiO2 hybrids are more active and selective at high temperatures (450–475 °C) while the difference becomes negligible at lower temperature. However, the comparison with reference P/SiO2 counterparts shows a very similar yield than the hybrids but more selective to ST. The benefit of the P/C/SiO2 hybrid is the lack of stabilization period, which is observed for the P/SiO2 to create an active coke overlayer. For long term operation, P/SiO2 appears to be a better choice in terms of selectivity, which is crucial for commercialization.
Original languageEnglish
Pages (from-to)173-181
Number of pages9
JournalApplied Catalysis A: General
Volume514
Early online date21 Jan 2016
DOIs
Publication statusPublished - 25 Mar 2016

Bibliographical note

© 2015, Elsevier. Licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/

Keywords

  • ethylbenzene
  • styrene
  • oxidative dehydrogenation
  • carbon-based catalysts
  • phosphorus
  • thermal stability

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