光谱学与光谱分析, 2012, 32 (3): 734, 网络出版: 2012-04-16
常压等离子体作用下CO2氧化CH4转化反应的光谱分析
Spectral Analysis of the Reaction of CH4 with CO2 as Oxidant under Plasma at Atmospheric Pressure
摘要
采用光谱原位诊断技术在200~900 nm范围内采集并标识了不同CO2添加量时CH4等离子体光谱。 确定了常压下不同CO2添加量时CH4等离子体的活性物种。 CO2添加量不同活性物种谱峰相对强度变化趋势不同, O活性物种谱峰相对强度随CO2添加量增加迅速增加。 C2活性物种谱峰相对强度随CO2添加量增加逐渐降低。 反应体系产生的活性O对CH4转化反应产物具有明显影响, CO2添加量不同, CH4转化反应机理不同。 当CO2添加量小于30%时, CH4转化以偶联反应为主。 CO2添加量大于30%时, CH4转化以重整反应为主。
Abstract
The optical emission spectrometry (OES) of methane ranging from 200 to 900 nm under plasma with different carbon dioxide contents were recorded and marked. Various reactive species in methane plasma such as: CHn(n=3, 2, 1), H, C2, C, C+, CO2+, O, CO+, OH and CHO were detected in situ by OES with different CO2 contents at atmospheric pressure. The relative intensity of reactive species was different with different CO2 contents. The relative intensity of O reactive specie was increased rapidly and C2 reactive specie was reduced gradually with increasing CO2 contents. Reactive O from the dissociation of CO2 had an obvious influence on the methane conversion. The mechanism of methane conversion was changed when CO2 contents increased. The coupling of methane to C2 hydrocarbons was the main reaction when CO2 contents were smaller than 30%, while the reforming of methane played a dominant role when CO2 contents higher than 30%.
翟林燕, 于淼, 周倩, 袁学德, 张秀玲. 常压等离子体作用下CO2氧化CH4转化反应的光谱分析[J]. 光谱学与光谱分析, 2012, 32(3): 734. ZHAI Lin-yan, YU Miao, ZHOU Qian, YUAN Xue-de, ZHANG Xiu-ling. Spectral Analysis of the Reaction of CH4 with CO2 as Oxidant under Plasma at Atmospheric Pressure[J]. Spectroscopy and Spectral Analysis, 2012, 32(3): 734.