Abstract
The effects of the partial pressures of oxygen and methane as well as temperature on the rates of C 2 hydrocarbon formation, carbon oxide formation, and total methane conversion in the oxidative coupling of methane over a NaOH/CaO catalyst were studied at differential operating conditions in a microcatalytic fixed-bed reactor. Temperature and partial pressures of the reactants were varied within the following ranges: 933 K ≤ T ≤ 1033 K, 5 kPa ≤ P CH 4 ° ≤ 80 kPa, 0.3 kPa ≤ P O 2 ° ≤ kPa. The rate of CO x formation was of 0.5 order in methane as well as in oxygen; the rate of C 2 hydrocarbon formation was first order in methane while it passed through a maximum with respect to oxygen partial pressure. The rate of methane conversion was well described by a power-law rate equation. Mechanistic assumptions derived from these kinetic results and corroborated by kinetic isotope effects are presented. In addition, kinetic equations for C 2 hydrocarbon formation, carbon oxide formation, and methane conversion as reported in the literature were scrutinized for their applicability to describing the experimental data obtained in this work.
Published Version
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