Formation of pyridine N-oxides using mesoporous titanium silicalite-1

Jerrik Jørgen Mielby, Jacob Oskar Abildstrøm, Susana Perez-Ferreras, Søren Birk Rasmussen, Søren Kegnæs

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Mesoporous titanium silicalite-1 (TS-1) prepared by carbon-templating is significantly more active than conventional TS-1 for the oxidation of pyridine derivatives using aqueous hydrogen peroxide as oxidant. The catalytic activity is increased by the system of mesopores that helps to overcome the configurational diffusion limitations within the microporous catalyst. The use of a carbon-template for generation of secondary porosity is more effective than desilication. The desilicated catalyst is slightly more active than conventional TS-1, probably due to a decrease of the mean diffusion path length. In contrast, carbon-templated mesopores provides an efficient transport throughout the zeolite, thus preventing deactivation due to product confinement. All catalysts were characterised by X-ray powder diffraction, scanning electron microscopy, UV-Vis spectroscopy and nitrogen physisorption. The results indicate that desilication may cause a surface densification of less catalytically active extra-framework Ti species. Carbon-templating is thus a more gentle and effective method for generating secondary porosity. Utilization of carbon-templated mesoporous TS-1 for oxidation of pyridine derivatives represents a new and environmentally friendly method to synthesise N-oxides.
Original languageEnglish
JournalJournal of Porous Materials
Volume21
Issue number5
Pages (from-to)531-537
ISSN1380-2224
DOIs
Publication statusPublished - 2014

Keywords

  • CHEMISTRY,
  • MATERIALS
  • CAPILLARY CONDENSATION
  • MOLECULAR-SIEVES
  • ZEOLITE
  • TS-1
  • OXIDATION
  • Mesoporous TS-1
  • N-oxides
  • Catalytic oxidation
  • Carbon templating
  • Desilication
  • HASH(0x3dcdc60)

Cite this

Mielby, Jerrik Jørgen ; Abildstrøm, Jacob Oskar ; Perez-Ferreras, Susana ; Rasmussen, Søren Birk ; Kegnæs, Søren. / Formation of pyridine N-oxides using mesoporous titanium silicalite-1. In: Journal of Porous Materials. 2014 ; Vol. 21, No. 5. pp. 531-537.
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abstract = "Mesoporous titanium silicalite-1 (TS-1) prepared by carbon-templating is significantly more active than conventional TS-1 for the oxidation of pyridine derivatives using aqueous hydrogen peroxide as oxidant. The catalytic activity is increased by the system of mesopores that helps to overcome the configurational diffusion limitations within the microporous catalyst. The use of a carbon-template for generation of secondary porosity is more effective than desilication. The desilicated catalyst is slightly more active than conventional TS-1, probably due to a decrease of the mean diffusion path length. In contrast, carbon-templated mesopores provides an efficient transport throughout the zeolite, thus preventing deactivation due to product confinement. All catalysts were characterised by X-ray powder diffraction, scanning electron microscopy, UV-Vis spectroscopy and nitrogen physisorption. The results indicate that desilication may cause a surface densification of less catalytically active extra-framework Ti species. Carbon-templating is thus a more gentle and effective method for generating secondary porosity. Utilization of carbon-templated mesoporous TS-1 for oxidation of pyridine derivatives represents a new and environmentally friendly method to synthesise N-oxides.",
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author = "Mielby, {Jerrik J{\o}rgen} and Abildstr{\o}m, {Jacob Oskar} and Susana Perez-Ferreras and Rasmussen, {S{\o}ren Birk} and S{\o}ren Kegn{\ae}s",
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Formation of pyridine N-oxides using mesoporous titanium silicalite-1. / Mielby, Jerrik Jørgen; Abildstrøm, Jacob Oskar; Perez-Ferreras, Susana; Rasmussen, Søren Birk; Kegnæs, Søren.

In: Journal of Porous Materials, Vol. 21, No. 5, 2014, p. 531-537.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Formation of pyridine N-oxides using mesoporous titanium silicalite-1

AU - Mielby, Jerrik Jørgen

AU - Abildstrøm, Jacob Oskar

AU - Perez-Ferreras, Susana

AU - Rasmussen, Søren Birk

AU - Kegnæs, Søren

PY - 2014

Y1 - 2014

N2 - Mesoporous titanium silicalite-1 (TS-1) prepared by carbon-templating is significantly more active than conventional TS-1 for the oxidation of pyridine derivatives using aqueous hydrogen peroxide as oxidant. The catalytic activity is increased by the system of mesopores that helps to overcome the configurational diffusion limitations within the microporous catalyst. The use of a carbon-template for generation of secondary porosity is more effective than desilication. The desilicated catalyst is slightly more active than conventional TS-1, probably due to a decrease of the mean diffusion path length. In contrast, carbon-templated mesopores provides an efficient transport throughout the zeolite, thus preventing deactivation due to product confinement. All catalysts were characterised by X-ray powder diffraction, scanning electron microscopy, UV-Vis spectroscopy and nitrogen physisorption. The results indicate that desilication may cause a surface densification of less catalytically active extra-framework Ti species. Carbon-templating is thus a more gentle and effective method for generating secondary porosity. Utilization of carbon-templated mesoporous TS-1 for oxidation of pyridine derivatives represents a new and environmentally friendly method to synthesise N-oxides.

AB - Mesoporous titanium silicalite-1 (TS-1) prepared by carbon-templating is significantly more active than conventional TS-1 for the oxidation of pyridine derivatives using aqueous hydrogen peroxide as oxidant. The catalytic activity is increased by the system of mesopores that helps to overcome the configurational diffusion limitations within the microporous catalyst. The use of a carbon-template for generation of secondary porosity is more effective than desilication. The desilicated catalyst is slightly more active than conventional TS-1, probably due to a decrease of the mean diffusion path length. In contrast, carbon-templated mesopores provides an efficient transport throughout the zeolite, thus preventing deactivation due to product confinement. All catalysts were characterised by X-ray powder diffraction, scanning electron microscopy, UV-Vis spectroscopy and nitrogen physisorption. The results indicate that desilication may cause a surface densification of less catalytically active extra-framework Ti species. Carbon-templating is thus a more gentle and effective method for generating secondary porosity. Utilization of carbon-templated mesoporous TS-1 for oxidation of pyridine derivatives represents a new and environmentally friendly method to synthesise N-oxides.

KW - CHEMISTRY,

KW - MATERIALS

KW - CAPILLARY CONDENSATION

KW - MOLECULAR-SIEVES

KW - ZEOLITE

KW - TS-1

KW - OXIDATION

KW - Mesoporous TS-1

KW - N-oxides

KW - Catalytic oxidation

KW - Carbon templating

KW - Desilication

KW - HASH(0x3dcdc60)

U2 - 10.1007/s10934-014-9800-0

DO - 10.1007/s10934-014-9800-0

M3 - Journal article

VL - 21

SP - 531

EP - 537

JO - Journal of Porous Materials

JF - Journal of Porous Materials

SN - 1380-2224

IS - 5

ER -