Metathetic oxidation of 2-butenes to acetaldehyde by molecular oxygen using the single-site olefin metathesis catalyst (≡SiO)2Mo(=O)2
AuthorsLe Quéméner, Frédéric
Aljuhani, Maha A.
Samantaray, Manoja K
Szeto, Kai C.
De Mallmann, Aimery
KAUST DepartmentPhysical Sciences and Engineering (PSE) Division
Chemical Science Program
KAUST Catalysis Center (KCC)
KAUST Grant Number2174 CGR3
Permanent link to this recordhttp://hdl.handle.net/10754/630669
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AbstractThe 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.
CitationLe Quéméner F, Barman S, Merle N, Aljuhani MA, Samantaray MK, et al. (2018) Metathetic Oxidation of 2-Butenes to Acetaldehyde by Molecular Oxygen Using the Single-Site Olefin Metathesis Catalyst (≡SiO)2Mo(═O)2. ACS Catalysis 8: 7549–7555. Available: http://dx.doi.org/10.1021/acscatal.8b01767.
SponsorsThe Competitive Research Grant Program, supported by the KAUST Research Fund (project # 2174 CGR3) is gratefully acknowledged for financial support. We wish to thank Olivier Mathon for his help during the recording of the XAS spectra on BM23 beamline at ESRF (experiment code IN-986). For computer time, this study employed the resources of the KAUST Supercomputing Laboratory (KSL).
PublisherAmerican Chemical Society (ACS)