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

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journal contribution
posted on 10.07.2018, 00:00 by 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
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.