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Functional Analysis of Catalysts for Lower Alkane Oxidation

MPS-Authors
/persons/resource/persons21768

Kube,  Pierre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21519

Frank,  Benjamin
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
BasCat—UniCat BASF Joint Lab TU Berlin, Sekr. EW K 01;

/persons/resource/persons22257

Wrabetz,  Sabine
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21766

Kröhnert,  Jutta
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21590

Hävecker,  Michael
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Max Planck Institute for Chemical Energy Conversion;

/persons/resource/persons104341

Velasco Vélez,  Juan
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons71845

Noack,  Johannes
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
BasCat—UniCat BASF Joint Lab TU Berlin, Sekr. EW K 01;

/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Max Planck Institute for Chemical Energy Conversion;

/persons/resource/persons22181

Trunschke,  Annette
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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manuscript_cctc_201601194R1.pdf
(Any fulltext), 892KB

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Citation

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.


Cite as: http://hdl.handle.net/11858/00-001M-0000-002C-83D0-5
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.