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Reaction mechanism of methane activation using non-equilibrium pulsed discharge at room temperature
Authors:Shigeru Kado  Kohei Urasaki  Yasushi Sekine  Kaoru Fujimoto  Tomohiro Nozaki  Ken Okazaki
Affiliation:

a Department of Mechanical and Control Engineering, Tokyo Institute of Technology, Ishikawadai 6th bldg, Room 223C, 2-12-1 O-okayama, Meguro-ku, Tokyo 152-8552, Japan

b Department of Applied Chemistry, School of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjyuku, Tokyo 169-8555, Japan

c Department of Chemical Processes and Environments, Faculty of Environmental Engineering, The University of Kitakyushu, 1-1 Hibikino, Wakamatsu-ku, Kitakyushu, Fukuoka 808-0135, Japan

Abstract:The reaction mechanism of methane activation using non-equilibrium pulsed discharge was largely clarified from the emission spectroscopic study and experiments with higher hydrocarbons and some kinds of isotopes. The strong emission of atomic carbon and C2 swan band system was observed as well as H Balmer series emission. This indicates that methane was highly dissociated into C and H by electron impact, which is consistent with the result of high C2D2 composition in produced acetylene when the mixture of CH4 and D2 was fed into discharge region. High electron energy contributed to produce atomic carbon directly from methane, and high electron density promoted the dehydrogenation from CH3, CH2 and CH to produce atomic carbon consecutively. The reason for the high selectivity to C2H2 was the high concentration of CH or C2 formed from atomic carbon, and the repetition mechanism of decomposition and recombination among C, CH, C2 and C2H2.
Keywords:Spark discharge  Methane dehydrogenation  Acetylene
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