A unified mechanism for oxidative coupling and partial oxidation of methane

FUEL

卷:297

Article

Simon, Yves¹  Marquaire, Paul-Marie¹ 

[1] Univ Lorraine, CNRS, ENS, Lab React & Genie Proc,UMR7274, 1 Rue Grandville,BP 20451, F-54001 Nancy, France

关键词: Methane;    Kinetic mechanism;    Partial oxidation;    Oxidative coupling;    La2O3;   

DOI  :  10.1016/j.fuel.2021.120683

来源: Elsevier

【 摘 要 】

The oxidative coupling (OCM) and the partial catalytic oxidation (POM) of methane as well as the homogeneous oxidation of methane (HOM) differ only in the ratio CH4/O-2 used and of course in the use of a catalyst. It can therefore be considered that their overall reaction mechanism should be the same with elementary reactions of varying importance depending on the type of oxidation reaction studied. We have therefore tried to represent the results obtained during the experimental study of OCM and POM over La2O3 and that of the oxidation of methane in gas phase from a single mechanism. At high temperature, OCM and POM are catalytic reactions but their reaction mechanisms are very complex because the surface reactions are coupled to reactions in gas phase by the intermediary of radicals, so both homogeneous and heterogeneous mechanisms occur at the same time. In this work, the development and the validation of a hetero-homogeneous mechanism is proposed for the three reactions. This mechanism is based on elementary steps at the catalyst surface and elementary steps in gas phase for a large range of temperature (973 K-1173 K) and residence time (0.7 s-5.5 s).

【 授权许可】

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