介质阻挡甲烷等离子体偶联合成C2烃的放大研究.docVIP

甲烷介质阻挡研究（天津大学化工学院绿色合成与转化教育部重点实验室, 天津 300072DBD反应器对甲烷转化进行了研究。考察了介质阻挡放电甲烷非平衡等离子体转化合成碳二烃（C2）的反应。结果表明：乙烷是主要的C2烃产物。不同反应器参数、高压位置、内电极形式和冷却方式等对甲烷转化有重要影响。优化条件后甲烷转化率可达44.43%, C2烃选择性最高为71%，其余为碳三烃。对比不同反应器中甲烷偶联的情况，结果显示反应器参数对甲烷转化以及产物分布有明显的影响。 关键词：甲烷；介质阻挡放电；C2烃；反应器 中图分类号：TQ203.7 文献标识码：A Studies on Conversion of Methane Through Dielectric-barrier Discharges WANG Bao-wei, YANG Kuan-hui, YAN Yi-gang, LIU Yong-wei, XU Gen-hui (Key Laboratory for Green Chemical Technology, School of Chemical Engineering Technology, Tianjin University, Tianjin 300072,China) Abstract: It is all known that reactor plays a key role in methane conversion. Four DBD reactors used for methane conversion were investigated in this work at room temperature and atmospheric pressure. In this paper the reaction of methane coupling to produce C2 hydrocarbons through dielectric-barrier discharge (DBD) of non-equilibrium plasma reaction was studied. It was found that ethane was the main C2 hydrocarbons product in the reaction. The optimization of reaction condition was investigated. The results showed that different parameters of reactors, high voltage position, types of inner electrode and cooling method had obvious effects on methane reaction. It was concluded that with the increase of volume energy density, the amount of C2 hydrocarbons increased. The optimal conversion of methane was 44.43%, and the highest selectivity of C2 hydrocarbons was 71%, while the other was C3 hydrocarbons. It was found that the sizes of reactor had obvious effects on methane conversion and products contribution, for methane conversion was compared with each other in different reactors. Keywords: methane; dielectric-barrier discharge; C2 hydrocarbons; reactor 引言 甲烷偶联合成C2烃的研究已引起广泛的关注[1-7]，介质阻挡放电等离子体甲烷转化技术以其温和洁净的反应条件为甲烷转化提出了新的工艺。特别是在石油资源日益减少的情况下,利用等离子体技术转化甲烷制C2烃是最有吸引力的研究课题之一[1]。 目前研究集中在改变放电条件和参数以期实现甲烷的高转化率和产物的高选择性 [2,3]。Chang等[3]设计并建立了放大实验系统，考察了气体温度、放电电压以及停留时间对CH4转化的影响。发现添加气O2与H2O可以提高CH4转化率及C2烃收率。加入氧化剂CO2，对CH4的解离影响显著，优化进料比后能显著