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  Functional Analysis of Catalysts for Lower Alkane Oxidation

Kube, P., Frank, B., Wrabetz, S., Kröhnert, J., Hävecker, M., Velasco Vélez, J., et al. (2017). Functional Analysis of Catalysts for Lower Alkane Oxidation. ChemCatChem, 9(4), 573-585. doi:10.1002/cctc.201601194.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002C-83D0-5 Version Permalink: http://hdl.handle.net/21.11116/0000-0000-0305-7
Genre: Journal Article

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manuscript_cctc_201601194R1.pdf (Any fulltext), 892KB
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2017
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Wiley-VCH
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 Creators:
Kube, Pierre1, Author              
Frank, Benjamin1, 2, Author              
Wrabetz, Sabine1, Author              
Kröhnert, Jutta1, Author              
Hävecker, Michael1, 3, Author              
Velasco Vélez, Juan1, Author              
Noack, Johannes1, 2, Author              
Schlögl, Robert1, 3, Author              
Trunschke, Annette1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, escidoc:24023              
2BasCat—UniCat BASF Joint Lab TU Berlin, Sekr. EW K 01, Hardenbergstr. 36, D-10623 Berlin (Germany), escidoc:persistent22              
3Max Planck Institute for Chemical Energy Conversion, Stiftstr. 34-36, D-45470 Muelheim an der Ruhr (Germany), escidoc:persistent22              

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 Abstract: The catalytic performance of 1) crystalline MoVTeNb oxide that exhibits the electronic properties of a n-type semiconductor, 2) submonolayer vanadium oxide supported on meso-structured silica (SBA-15) as an insulating support, and 3) surface-functionalized carbon nanotubes that contain neither a redox active metal nor bulk oxygen, but only surface oxygen species have been compared in the oxidative dehydrogenation of ethane and propane under equal reaction conditions. The catalytic results indicate similarities in the reaction network over all three catalysts within the range of the studied reaction conditions implying that differences in selectivity are a consequence of differences in the rate constants. Higher activity and selectivity to acrylic acid over MoVTeNb oxide as compared to the other two catalysts are attributed to the higher density of potential alkane adsorption sites on M1 and the specific electronic structure of the semiconducting bulk catalyst. Microcalorimetry has been used to determine and quantify different adsorption sites revealing a low Vsurface/C3H8 ads ratio of 4 on M1 and a much higher ratio of 150 on silica-supported vanadium oxide. On the latter catalyst less than one per cent of the vanadium atoms adsorb propane. Barriers of propane activation increase in the order P/oCNT (139 kJ mol−1)≤M1 (143 kJ mol−1)<6V/SBA-15 (162 kJ mol−1), which is in agreement with trends predicted by theory.

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 Dates: 2016-11-012016-09-222017-01-092017-02-21
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1002/cctc.201601194
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Title: ChemCatChem
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 13 Volume / Issue: 9 (4) Sequence Number: - Start / End Page: 573 - 585 Identifier: ISSN: 1867-3880
CoNE: http://pubman.mpdl.mpg.de/cone/journals/resource/1867-3880