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Topics in Catalysis
Published in: Topics in Catalysis 1-2/2017

19-09-2016 | Original Paper

Methane Oxidation over Palladium: On the Mechanism in Fuel-Rich Mixtures at High Temperatures

Authors: H. Stotz, L. Maier, O. Deutschmann

Published in: Topics in Catalysis | Issue 1-2/2017

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Abstract

A kinetic modeling study on methane oxidation over reduced Pd for various fuel-rich conditions around the stoichiometric point of the partial oxidation at high temperatures (900–1100 K) is presented. A thermodynamically consistent detailed surface reaction mechanism is developed within the mean field approximation. The proposed kinetic model consists of 54 elementary-step based reactions including seven gas-phase species and 15 surface intermediates. Three different methane activation paths are implemented, comprising pyrolytic C–H bond dissociation steps, oxygen-assisted and dual-oxygen-assisted CH4 activation. In situ experimental measurements in a quasi-autothermally operated flow reactor, using the capillary sampling technique, are performed for model evaluation. The provided experimental data includes spatially resolved temperature and concentration profiles within a single catalytic channel of a Pd/Al2O3-coated monolith. Supplementary numerical simulations based on literature data for fuel-lean and fuel-rich conditions at high temperatures extend the model’s capability to predict a wide range of different experimental conditions.
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Metadata
Title
Methane Oxidation over Palladium: On the Mechanism in Fuel-Rich Mixtures at High Temperatures
Authors
H. Stotz
L. Maier
O. Deutschmann
Publication date
19-09-2016
Publisher
Springer US
Published in
Topics in Catalysis / Issue 1-2/2017
Print ISSN: 1022-5528
Electronic ISSN: 1572-9028
DOI
https://doi.org/10.1007/s11244-016-0717-5

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