Reaction mechanism of methane activation using non-equilibrium pulsed discharge at room temperature

被引:123
作者
Kado, S
Urasaki, K
Sekine, Y
Fujimoto, K
Nozaki, T
Okazaki, K
机构
[1] Tokyo Inst Technol, Dept Mech & Control Engn, Meguro Ku, Tokyo 1528552, Japan
[2] Waseda Univ, Dept Appl Chem, Sch Sci & Engn, Shinjyu Ku, Tokyo 1698555, Japan
[3] Univ Kitakyushu, Fac Environm Engn, Dept Chem Proc & Environm, Wakamatsu Ku, Kitakyushu, Fukuoka 8080135, Japan
基金
日本学术振兴会;
关键词
spark discharge; methane dehydrogenation; acetylene;
D O I
10.1016/S0016-2361(03)00163-7
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
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 C-2 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 D-2, 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 C-2 formed from atomic carbon, and the repetition mechanism of decomposition and recombination among C, CH, C-2 and C2H,. (C) 2003 Elsevier Ltd. All rights reserved.
引用
收藏
页码:2291 / 2297
页数:7
相关论文
共 34 条
[1]  
BABARITSKYI A, 1995, VDI BER, V1166, P541
[2]   THERMAL COUPLING OF METHANE IN A TUBULAR FLOW REACTOR - PARAMETRIC STUDY [J].
BILLAUD, FG ;
BARONNET, F ;
GUERET, CP .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1993, 32 (08) :1549-1554
[3]   COLLISIONAL REMOVAL RATES FOR ELECTRONICALLY EXCITED CH RADICALS B2-SIGMA- AND C2-SIGMA+ [J].
COOPER, JL ;
WHITEHEAD, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1992, 88 (16) :2323-2327
[4]   Direct conversion of methane and carbon dioxide to higher hydrocarbons using catalytic dielectric-barrier discharges with zeolites [J].
Eliasson, B ;
Liu, CJ ;
Kogelschatz, U .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2000, 39 (05) :1221-1227
[5]   A diode laser and modeling study of mixed (CH4-H2-O2) AC plasmas [J].
Fan, WY ;
Knewstubb, PF ;
Käning, M ;
Mechold, L ;
Röpcke, J ;
Davies, PB .
JOURNAL OF PHYSICAL CHEMISTRY A, 1999, 103 (20) :4118-4128
[6]   ENERGY-TRANSFER PROCESSES IN CH A2-DELTA AND B2-SIGMA- IN AN ATMOSPHERIC-PRESSURE FLAME [J].
GARLAND, NL ;
CROSLEY, DR .
APPLIED OPTICS, 1985, 24 (23) :4229-4237
[7]   PYROLYSIS OF NATURAL-GAS - CHEMISTRY AND PROCESS CONCEPTS [J].
HOLMEN, A ;
OLSVIK, O ;
ROKSTAD, OA .
FUEL PROCESSING TECHNOLOGY, 1995, 42 (2-3) :249-267
[8]   HIGH-POWER PULSED RADIOFREQUENCY AND MICROWAVE CATALYTIC PROCESSES - SELECTIVE PRODUCTION OF ACETYLENE FROM THE REACTION OF METHANE OVER CARBON [J].
IOFFE, MS ;
POLLINGTON, SD ;
WAN, JKS .
JOURNAL OF CATALYSIS, 1995, 151 (02) :349-355
[9]   METHANE TO ETHYLENE WITH 85-PERCENT YIELD IN A GAS RECYCLE ELECTROCATALYTIC REACTOR-SEPARATOR [J].
JIANG, Y ;
YENTEKAKIS, IV ;
VAYENAS, CG .
SCIENCE, 1994, 264 (5165) :1563-1566
[10]   Direct synthesis of acetylene from methane by direct current pulse discharge [J].
Kado, S ;
Sekine, Y ;
Fujimoto, K .
CHEMICAL COMMUNICATIONS, 1999, (24) :2485-2486