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Catalysis Letters

, Volume 141, Issue 2, pp 251–258 | Cite as

Role of the Ti(IV)-Superoxide Species in the Selective Oxidation of Alkanes with Hydrogen Peroxide in the Gas Phase on Titanium Silicalite-1: An In Situ EPR Investigation

  • Sebastian Heinrich
  • Martin Plettig
  • Elias Klemm
Article

Abstract

The interaction of TS-1 with gaseous hydrogen peroxide at temperatures above 373 K has been investigated by in situ EPR measurements. Treatment of TS-1 with hydrogen peroxide in the gas phase leads to a strong EPR signal, assigned to the Ti(IV)-superoxide species. In contrast to investigations with liquid hydrogen peroxide, here only one Ti(IV)-superoxide species could be detected in the EPR spectrum. The time constant of the reaction of the Ti(IV)-superoxide species detected by in situ EPR measurements was much larger than that observed for the rate of consumption of propane or propene via gas chromatographic analysis. Thus, we conclude that the superoxide species may take part in the oxidation reaction (via side reactions or the formation of unselective products), but is probably not the main responsible species in the oxidation of propane or propene.

Graphical Abstract

Keywords

Titanium silicalite-1 EPR Oxidation Hydrogen peroxide Superoxide Alkanes 

Notes

Acknowledgments

The authors are grateful to Prof. Rudolf Holze, Chemnitz University of Technology, for providing access to his EPR Spectrometer and to Prof. Angelika Brückner for fruitful discussions.

Supplementary material

10562_2010_534_MOESM1_ESM.doc (170 kb)
Supplementary material 1 (DOC 170 kb)

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Copyright information

© Springer Science+Business Media, LLC 2010

Authors and Affiliations

  • Sebastian Heinrich
    • 1
  • Martin Plettig
    • 2
  • Elias Klemm
    • 3
  1. 1.BAM Federal Institute for Materials Research and TestingChemical Safety EngineeringBerlinGermany
  2. 2.Department for Industrial Chemistry, Faculty of Natural SciencesChemnitz University of TechnologyChemnitzGermany
  3. 3.University of Stuttgart, Institute for Technical Chemistry, Faculty of ChemistryStuttgartGermany

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