Aerosol Route to TiO2–SiO2 Catalysts with Tailored Pore Architecture and High Epoxidation Activity

  • Valentin Smeets
    Valentin Smeets
    Institute of Condensed Matter and Nanosciences (IMCN), UCLouvain, Place Louis Pasteur, 1, Box L4.01.09, 1348 Louvain-la-Neuve, Belgium
  • Cédric Boissière
    Cédric Boissière
    Sorbonne Université, CNRS, Collège de France, PSL Research University, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, 4 Place Jussieu, F-75005 Paris, France
  • Clément Sanchez
    Clément Sanchez
    Sorbonne Université, CNRS, Collège de France, PSL Research University, Laboratoire Chimie de la Matière Condensée de Paris, LCMCP, 4 Place Jussieu, F-75005 Paris, France
  • Eric M. Gaigneaux
    Eric M. Gaigneaux
    Institute of Condensed Matter and Nanosciences (IMCN), UCLouvain, Place Louis Pasteur, 1, Box L4.01.09, 1348 Louvain-la-Neuve, Belgium
  • Elise Peeters
    Elise Peeters
    Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
  • Bert F. Sels
    Bert F. Sels
    Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
    More by Bert F. Sels
  • Michiel Dusselier
    Michiel Dusselier
    Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
  • , and 
  • Damien P. Debecker*
    Damien P. Debecker
    Institute of Condensed Matter and Nanosciences (IMCN), UCLouvain, Place Louis Pasteur, 1, Box L4.01.09, 1348 Louvain-la-Neuve, Belgium
    *E-mail: [email protected]. Twitter: @Deuxbeck.
Cite this: Chem. Mater. 2019, 31, 5, 1610–1619
Publication Date (Web):January 24, 2019
https://doi.org/10.1021/acs.chemmater.8b04843
Copyright © 2019 American Chemical Society
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Abstract

Herein, we present the aerosol-assisted sol–gel preparation of hierarchically porous TiO2–SiO2 catalysts having a spherelike shell morphology and a high Ti dispersion. In order to control the porosity at the micro-, meso-, and macrolevels, we use the evaporation-induced self-assembly (EISA) of a surfactant, possibly combined with polymer beads as hard templates. These catalysts are tested for the epoxidation of cyclohexene with cumene hydroperoxide as the oxidant, and their performance is compared to the reference TS-1 zeolite. The high catalytic performance observed with the catalysts prepared by aerosol stems from their high specific surface area, but also from the short diffusion path length generated by the meso-/macropore architecture which provides entryways for bulky reactants and products. Besides, these materials can incorporate a higher Ti loading than TS-1 zeolite, while ensuring a good control over the Ti speciation. Thus, the unique features of the aerosol process—which is also known to be scalable—allow us to prepare catalytic materials with high epoxidation activity, also for bulky olefins.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.8b04843.

  • Detailed procedure for the preparation of the reference TS-1 catalyst, XPS Ti 2p spectra, PXRD patterns, t-plots, PSD on desorption of Aer_PMMA, catalytic tests in the presence of hydrogen peroxide and recyclability study, hot filtration test of Aer_20, N2 adsorption–desorption isotherm, PSD, and t-plot of Aer_15_2%, estimation of the band gap energy values of Aer_15_2% and Aer_15, and example of calculation of the initial TOF value for Aer_15 (PDF)

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