High-temperature oxidation of CO and CH4

一氧化碳 化学 甲烷 氧气 二氧化碳 大气温度范围 分析化学(期刊) 摩尔分数 反应速率 反应速率常数 物理化学 动力学 色谱法 催化作用 有机化学 热力学 物理 量子力学
作者
Frederick L. Dryer,Irvin Glassman
出处
期刊:Symposium (International) on Combustion [Elsevier]
卷期号:14 (1): 987-1003 被引量:361
标识
DOI:10.1016/s0082-0784(73)80090-6
摘要

The oxidation of moist carbon monoxide and the post-induction-phase oxidation of methane were studied in a turbulent flow reactor. Reactants, stable intermediates, and products were determined spatially by chemical sampling and gas-chromatographic analysis. The carbon monoxide-oxygen reaction in the presence of water was studied at atmosphericpressure, and over the following ranges: temperature, 1030°–1230°K; equivalence ratio, 0.04–0.5; and water concentration, 0.1%–3.0%. The over-all rate expression found was −d[CO]/dt=1014.6±0.25 exp[(−40,000±1200)/RT][CO]1.0[H2O]0.5[O2]0.25 mole cm−3 sec−1. The data support the fact that hydroxyl radical concentration in the reaction exceeds that at thermal equilibrium by as much as 2 orders of magnitude. The post-induction-phase reaction of methane and oxygen was studied at atmospheric pressure, over the temperature range of 1100°–1400°K and equivalence ratio range of 0.05–0.5. The over-all methane disappearance-rate expression was found to be −d[CH4]/dt=1013.2±0.20 exp[(−48,400±1200)/RT][CH4]0.7[O2]0.8, mole cm−3 sec−1. The rate was shown to be independent of water concentrations added initially or produced in the reaction. The over-all appearance rate of carbon dioxide in the methane-oxygen reaction is described byd[CO2]/dt=1014.75±0.40 exp[(−43,000±2200)/RT][CO]1.0[H2O]0.5[O2]0.25 mole cm−3 sec−1. This correlation represents rates of carbon dioxide formation 3.5 times slower than those found in the independent study of the moist carbon monoxide reaction. From these and other experiments it was possible to deduce thatCH4+OH→CH3+H2O (3) is not the only mechanism contributing to the observed rate of disappearance of methane. It was concluded that the reaction CH4+O→CH3+OH (4) is of major importance in both oxygen-and fuel-rich systems at high temperatures. Furthermore, the experimental data support that these two reactions, as well as CH3+H2→CH4+H (−5) contribute to the methane results reported here.
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