Experimental and Modeling Study of the Selective Homogeneous Gas Phase Oxidation of Methane to Methanol

Experimental and Modeling Study of the Selective Homogeneous Gas Phase Oxidation of Methane to Methanol
复制标题

甲烷选择性均相气相氧化制甲醇的实验与模拟研究

DOI:
10.1021/ie00043a006
复制
发表时间:
1995
影响因子:
4.2
通讯作者:
O. Onsager
O. Onsager
中科院分区:
工程技术3区
文献类型:
--
作者:
R. Lødeng;O. A. Lindvaag;P. Soraker;P. Roterud;O. Onsager

文献摘要

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The partial oxidation of CH{sub 4} to CH{sub 3}OH with air has been. investigated experimentally and theoretically. Experimentally, the homogeneous gas phase reaction was studied at pressures in the range 40 {times} 10{sup 5}--60 {times} 10{sup 5} Pa, temperatures in the range 723--823 K, and O{sub 2} concentrations in the range 2.6--4.4% relative to CH{sub 4}. CH{sub 3}OH selectivities between 35 and 55% were obtained at low conversions, 1.2--2.6%. A kinetic model, based on 61 elementary reactions, was able to reproduce experimental observations, indicating that only moderate selectivities to CH{sub 3}OH (50--65%) are obtainable at low CH{sub 4} conversion (<4%). The model is used to investigate an extended span of temperatures, pressures, and O{sub 2} concentrations in search of favorable conditions for CH{sub 3}OH formation. The model predicts CH{sub 3}OH formation to be favored by high pressure, moderate temperature 673--723 K, and low O{sub 2} concentrations 2--4%. The predicted effects are discussed and illustrated in a mechanistic perspective.
The partial oxidation of CH{sub 4} to CH{sub 3}OH with air has been. investigated experimentally and theoretically. Experimentally, the homogeneous gas phase reaction was studied at pressures in the range 40 {times} 10{sup 5}--60 {times} 10{sup 5} Pa, temperatures in the range 723--823 K, and O{sub 2} concentrations in the range 2.6--4.4% relative to CH{sub 4}. CH{sub 3}OH selectivities between 35 and 55% were obtained at low conversions, 1.2--2.6%. A kinetic model, based on 61 elementary reactions, was able to reproduce experimental observations, indicating that only moderate selectivities to CH{sub 3}OH (50--65%) are obtainable at low CH{sub 4} conversion (<4%). The model is used to investigate an extended span of temperatures, pressures, and O{sub 2} concentrations in search of favorable conditions for CH{sub 3}OH formation. The model predicts CH{sub 3}OH formation to be favored by high pressure, moderate temperature 673--723 K, and low O{sub 2} concentrations 2--4%. The predicted effects are discussed and illustrated in a mechanistic perspective.