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作 者:沈长圣[1] 孙永志[1] 孙德坤[2] 杨鸿生[1]
机构地区:[1]东南大学电子科学与工程学院,毫米波国家重点实验室,南京210096 [2]南京大学化学化工学院,南京210093
出 处:《中国科学(B辑)》2009年第12期1620-1626,共7页Science in China(Series B)
摘 要:通过优化设计矩形波导谐振腔微波化学反应器,可以大幅提高微波等离子体下甲烷转化率(最高为93.7%)、C2烃收率(最高为91.0%)和乙炔收率(最高为88.6%).且优化后,在实验的压强范围内,甲烷转化率和C2烃收率较为稳定,C2烃主要是乙炔,其选择性都在90%以上.生成乙炔的能量产率和时空产率也都比较高.利用发射光谱法对微波等离子体下甲烷偶联制乙炔的反应进行了诊断研究,在300nm~750nm波长范围内激发态物种有:CH,C2,H2,Hα.根据反应产物和激发态物种从化学反应热力学和动力学上对反应机理进行了初步探索.By optimizing the microwave chemistry reactor made of the rectangular waveguide resonator, the methane conversion (the maximum of 93.7%), the C2 hydrocarbon yield (the maximum of 91.0%) and the acetylene yield (the maximum of 88.6%) all were greatly increased under microwave plasma. Furthermore, for the optimal reactor, the change of the methane conversion and the C2 hydrocarbon yield is little with the change of the pressure in the range of experiments. For the C2 hydrocarbon, acetylene is most, and the selectivity for acetylene is above 90%. Energy yield and space time yield of acetylene are also high. Optical emission spectroscopy (OES) was adopted for the diagnosis of methane coupling to acetylene under microwave plasma. The excited species (CH, C2, H2, Hα) were detected in the spectra range of 300-750 nm. Based on the products and the excited species, the reaction mechanism of methane coupling under microwave plasma was investigated, using the thermodynamics and kinetics of the chemical reaction.
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