Metathetic Oxidation of 2-Butenes to Acetaldehyde by Molecular Oxygen Using the Single-Site Olefin Metathesis Catalyst (≡SiO)2Mo(=O)2

Frédéric Le Quéméner, Samir Barman, Nicolas Merle, Maha A. Aljuhani, Manoja K. Samantaray, Youssef Saih, Kai C. Szeto, Aimery De Mallmann, Yury Minenkov, Kuo Wei Huang*, Luigi Cavallo, Mostafa Taoufik, Jean Marie Basset

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

20 Scopus citations

Abstract

The catalytic oxidation of cis-2-butene and propylene with molecular oxygen in the presence of a well-defined surface coordination compound, (≡SiO)2Mo(=O)2, affords acetaldehyde. Using a cis-2-butene/O2 feed at 350-400 °C, the reaction yields a conversion of approximately 10% and an acetaldehyde selectivity of approximately 70%. This performance is maintained up to an experimental time of 20 h in a continuous flow reactor. The Mo(bis-oxo) surface compound was fully characterized by multiple spectroscopic techniques as well as surface microanalysis. The results from quantum mechanics calculations indicate that the reaction proceeds via [2 + 2] cycloaddition/cycloelimination steps with the formation of metalla-oxacyclobutane intermediates, analogous to the Chauvin mechanism in olefin metathesis.

Original languageEnglish (US)
Pages (from-to)7549-7555
Number of pages7
JournalACS Catalysis
Volume8
Issue number8
DOIs
StatePublished - Aug 3 2018

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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