In-situ investigation of gas phase radical chemistry in the catalytic partial oxidation of methane on Pt

The catalytic partial oxidation of methane on platinum was studied in situ under atmospheric pressure and temperatures between 1000 and 1300 °C. By combining radical measurements using a molecular beam mass spectrometer and threshold ionization with GC, GC–MS and temperature profile measurements it...

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Veröffentlicht in:Catalysis today 2009-04, Vol.142 (1), p.61-69
Hauptverfasser: Geske, M., Pelzer, K., Horn, R., Jentoft, F.C., Schlögl, R.
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container_end_page 69
container_issue 1
container_start_page 61
container_title Catalysis today
container_volume 142
creator Geske, M.
Pelzer, K.
Horn, R.
Jentoft, F.C.
Schlögl, R.
description The catalytic partial oxidation of methane on platinum was studied in situ under atmospheric pressure and temperatures between 1000 and 1300 °C. By combining radical measurements using a molecular beam mass spectrometer and threshold ionization with GC, GC–MS and temperature profile measurements it was demonstrated that a homogeneous reaction pathway is opened at temperatures above 1100 °C, in parallel to heterogeneous reactions which start already at 600 °C. Before ignition of gas phase chemistry, only CO, H 2, CO 2 and H 2O are formed at the catalyst surface. Upon ignition of gas chemistry, CH 3 radicals, C2 coupling products and traces of C3 and C4 hydrocarbons are observed. Because the formation of CH 3 radicals correlates with the formation of C2 products it can be concluded that C2 products are formed by coupling of methyl radicals in the gas phase followed by dehydrogenation reactions. This formation pathway was predicted by numerical simulations and this work presents an experimental confirmation under high temperature atmospheric pressure conditions.
doi_str_mv 10.1016/j.cattod.2009.01.005
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subjects Catalysis
Catalytic partial oxidation
Chemical Sciences
Chemistry
Exact sciences and technology
Gas phase chemistry
General and physical chemistry
Methane
Methyl radical
Molecular beam mass spectrometry
Platinum
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
title In-situ investigation of gas phase radical chemistry in the catalytic partial oxidation of methane on Pt
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