Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 19, Issue 50, Pages 16938-16945Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201302420
Keywords
catalysis; coking; dehydrogenation; molybdenum carbide; surface chemistry
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Funding
- International Max Planck Research School (IMPRS) Complex Surfaces in Materials Sciences
- Federal Ministry of Education and Research (BMBF) within the CarboKat project of the Inno [FKZ 03X0204C]
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The effect of the gas-phase chemical potential on surface chemistry and reactivity of molybdenum carbide has been investigated in catalytic reactions of propane in oxidizing and reducing reactant mixtures by adding H-2, O-2, H2O, and CO2 to a C3H8/N-2 feed. The balance between surface oxidation state, phase stability, carbon deposition, and the complex reaction network involving dehydrogenation reactions, hydrogenolysis, metathesis, water-gas shift reaction, hydrogenation, and steam reforming is discussed. Raman spectroscopy and a surface-sensitive study by means of in situ X-ray photoelectron spectroscopy evidence that the dynamic formation of surface carbon species under a reducing atmosphere strongly shifts the product spectrum to the C-3-alkene at the expense of hydrogenolysis products. A similar response of selectivity, which is accompanied by a boost of activity, is observed by tuning the oxidation state of Mo in the presence of mild oxidants, such as H2O and CO2, in the feed as well as by V doping. The results obtained allow us to draw a picture of the active catalyst surface and to propose a structure-activity correlation as a map for catalyst optimization.
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