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  Active Sites in Olefin Metathesis over Supported Molybdena Catalysts

Amakawa, K., Kröhnert, J., Wrabetz, S., Frank, B., Hemmann, F., Jäger, C., et al. (2015). Active Sites in Olefin Metathesis over Supported Molybdena Catalysts. ChemCatChem, 7(24), 4059-4065. doi:10.1002/cctc.201500725.

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 Creators:
Amakawa, Kazuhiko1, Author              
Kröhnert, Jutta1, Author              
Wrabetz, Sabine1, Author              
Frank, Benjamin1, Author              
Hemmann, Felix2, 3, Author
Jäger, Christian2, Author
Schlögl, Robert1, Author              
Trunschke, Annette1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2BAM Federal Institute for Materials Research and Testing, Richard-Willstätter-Strasse 11, 12489 Berlin (Germany), ou_persistent22              
3Department of Chemistry Humboldt-Universität zu Berlin , Brook-Taylor-Strasse 2, 12489 Berlin (Germany), ou_persistent22              

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Free keywords: heterogeneous catalysis;molybdenum;olefin metathesis;supported catalysts
 Abstract: Metathesis of propene to ethene and 2-butenes was studied over a series of MoOx/SBA-15 catalysts (molybdenum oxide supported on mesoporous silica SBA-15; Mo loading 2.1~13.3 wt%, apparent Mo surface density 0.2~2.5 nm-2). The catalysts have been prepared by an ion exchange technique. Nitrogen adsorption, 1H-MAS-NMR, Raman, and FTIR spectroscopies were applied to characterize the catalysts. Adsorption of the reactant propene and the probe molecule NH3 was studied by in situ FTIR, microcalorimetry and temperature-programmed desorption. Irrespective of the loading, only ca. 1% of the Mo atoms in the MoOx/SiO2 catalysts transform into active carbene (Mo=CHR) sites catalyzing propene metathesis. Isolated, distorted molybdenum di-oxo species in close vicinity to two silanol groups have been shown to be the precursor of the active site. Targeted active site creation by pretreatment with methanol resulted in an increase in initial catalytic activity by a factor of 800.

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Language(s): eng - English
 Dates: 2015-06-242015-082015-09-28
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/cctc.201500725
 Degree: -

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Title: ChemCatChem
  Other : ChemCatChem
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 7 Volume / Issue: 7 (24) Sequence Number: - Start / End Page: 4059 - 4065 Identifier: ISSN: 1867-3880
CoNE: https://pure.mpg.de/cone/journals/resource/1867-3880