Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 18, Issue 3, Pages 887-898Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201101223
Keywords
cobalt; epoxidation; heterogeneous catalysis; metal-organic frameworks; stilbene oxides
Categories
Funding
- Technical University of Denmark
- Graduate School MP2T
- Haldor Topsoe A/S
- European Community [RII3-CT-2004-506008]
- Engineering and Physical Sciences Research Council [EP/F008384/1] Funding Source: researchfish
- EPSRC [EP/F008384/1] Funding Source: UKRI
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A Co-based metalorganic framework (MOF) was investigated as a catalytic material in the aerobic epoxidation of olefins in DMF and exhibited, based on catalyst mass, a remarkably high catalytic activity compared with the Co-doped zeolite catalysts that are typically used in this reaction. The structure of STA-12(Co) is similar to that of STA-12(Ni), as shown by XRD Rietveld refinement and is stable up to 270 degrees C. For the epoxidation reaction, significantly different selectivities were obtained depending on the substrate. Although styrene was epoxidized with low selectivity due to oligomerization, (E)-stilbene was converted with high selectivities between 80 and 90%. Leaching of Co was low and the reaction was found to proceed mainly heterogeneously. The catalyst was reusable with only a small loss of activity. The catalytic epoxidation of stilbene with the MOF featured an induction period, which was, interestingly, considerably reduced by styrene/stilbene co-epoxidation. This could be traced back to the formation of benzaldehyde promoting the reaction. Detailed parameter and catalytic studies, including in situ EPR and EXAFS spectroscopy, were performed to obtain an initial insight into the reaction mechanism.
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