Metathetic oxidation of 2-butenes to acetaldehyde by molecular oxygen using the single-site olefin metathesis catalyst (≡SiO)2Mo(=O)2

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

Research output: Contribution to journalArticlepeer-review

7 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 - Jul 10 2018

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