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Beyond-thermal-equilibrium" conversion of methane to acetylene and hydrogen under pulsed corona discharge
作者姓名:朱爱民  张秀玲  李小松  宫为民
作者单位:ZHUAimin ZHANG Xiuling LI Xiaosong& GONG WeiminLaboratory of Plasma Physical Chemistry,Box 288,Dalian University of Technology,Dalian 116024,China;State Key Laboratory for Materials Modification by Laser,Ion and Electron Beams,Dal
基金项目:This work was supported by the National Natural Science Foundation of China (Grant No. 20106003).
摘    要:At ambient temperature and pressure, C2H2 and H2 are the dominating products from pure methane conversion under pulsed corona discharge (PCD). When the energy density of 194-1788 kJ/mol was applied, 7%-30% of C2H2 yield and 6%-35% of H2 yield per pass have been obtained. These results are higher than the maximum thermodynamic yield of C2H2 (5.1%) and H2 (3.8%) at 100 kPa and 1100 K, respectively. Thereby, pulsed corona discharge is a very effective tool for "beyond-thermal-equilibrium" conversion of methane to C2H2 and H2 at ambient temperature and pressure. In the PCD energy density range of 339-822 kJ/mol, the carbon distribution of the methane conversion products is found to be: C2H2 86%-89%, C2H6 4%-6%, C2H4 4%-6%, C3 -2%, C4 -1%. Through comparison of the product from pure methane, ethane and ethylene conversion at the same discharge conditions, it can be concluded that three pathways may be responsible for the C2H2 formation via CHx radicals produced from the collisions of CH4 molecules with energi

收稿时间:17 April 2008

“Beyond-thermal-equilibrium” conversion of methane to acetylene and hydrogen under pulsed corona discharge
Aimin Zhu, Xiuling Zhang, Xiaosong Li and Weimin Gong.Beyond-thermal-equilibrium" conversion of methane to acetylene and hydrogen under pulsed corona discharge[J].Science in China(Chemistry),2002,45(4):426-434.
Authors:Aimin Zhu  Xiuling Zhang  Xiaosong Li and Weimin Gong
Institution:1. Laboratory of Plasma Physical Chemistry, Box 288, Dalian University of Technology, Dalian 116024, China;State Key Laboratory for Materials Modification by Laser, Ion and Electron Beams, Dalian University of Technology, Dalian 116024, China
2. Laboratory of Plasma Physical Chemistry, Box 288, Dalian University of Technology, Dalian 116024, China
Abstract:At ambient temperature and pressure, C2H2 and H2 are the dominating products from pure methane conversion under pulsed corona discharge (PCD). When the energy density of 194-1788 kJ/mol was applied, 7%-30% of C2H2 yield and 6%-35% of H2 yield per pass have been obtained. These results are higher than the maximum thermodynamic yield of C2H2 (5.1%) and H2 (3.8%) at 100 kPa and 1100 K, respectively. Thereby, pulsed corona discharge is a very effective tool for "beyond-thermal-equilibrium" conversion of methane to C2H2 and H2 at ambient temperature and pressure. In the PCD energy density range of 339-822 kJ/mol, the carbon distribution of the methane conversion products is found to be: C2H2 86%-89%, C2H6 4%-6%, C2H4 4%-6%, C3 -2%, C4 -1%. Through comparison of the product from pure methane, ethane and ethylene conversion at the same discharge conditions, it can be concluded that three pathways may be responsible for the C2H2 formation via CHx radicals produced from the collisions of CH4 molecules with energized electrons in the PCD plasma: (i) C2H2 is formed directly from free radical reactions, (ii) C2H2 is formed through the dehydrogenation of C2H4, which is formed via free radical reactions primarily, and (iii) C2H6 is the primary product and then dehydrogenates to C2H4 (secondary product) and followed by C2H4 dehydrogenation to C2H2.
Keywords:methane conversion  pulsed corona discharge  plasma  acetylene  hydrogen  
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