Propane dissociation in a non-thermal high-pressure nitrogen plasma

被引:37
作者
Moreau, N. [1 ]
Pasquiers, S. [1 ]
Blin-Simiand, N. [1 ]
Magne, L. [1 ]
Jorand, F. [1 ]
Postel, C. [1 ]
Vacher, J-R [1 ]
机构
[1] Univ Paris Sud, CNRS, Phys Gaz & Plasmas Lab, UMR8578, F-91405 Orsay, France
关键词
PHOTO-TRIGGERED DISCHARGE; ENERGY-TRANSFER REACTIONS; NO REMOVAL; ATMOSPHERIC-PRESSURE; CHEMICAL-KINETICS; METHANE; HYDROCARBONS; REACTIVITY; CHEMISTRY; IGNITION;
D O I
10.1088/0022-3727/43/28/285201
中图分类号
O59 [应用物理学];
学科分类号
摘要
The removal and the conversion processes of propane in N-2/C3H8 mixtures (concentration of hydrocarbon molecules up to 5500 ppm) energized by a photo-triggered discharge (homogeneous plasma) are studied at 460 mbar total pressure, both experimentally and theoretically. A self-consistent 0D discharge and kinetic model is used to interpret chromatographic measurements of propane and some by-products' concentrations (hydrogen and hydrocarbons with two or three carbon atoms). It is suggested, from the comparison between measurements and model predictions, that quenching processes of nitrogen metastable states by C3H8 lead to the dissociation of the hydrocarbon molecule, and are the most important processes for the removal of propane. Such a result is obtained using the quenching coefficient value previously determined by Callear and Wood (1971 Trans. Faraday Soc. 67 272) for the A (3)Sigma(+)(u) state, whereas the coefficient for collisions of the singlet states with C3H8 is estimated to be 3.0 x 10(-10) cm(3) s(-1) in order to explain the measured propane disappearance in the N-2/C3H8 mixture excited by the photo-triggered discharge. The hydrogen molecule is the measured most populated by-product and, also from the comparison between experimental results and model predictions, the most probable dissociation products of propane appear to be H-2 and C3H6. The propene molecule is also efficiently dissociated by the quenching processes of N-2 states, and probably leads to the production of hydrogen atoms and methyl radicals with equivalent probabilities. The kinetic model predicts that the carbon atom is distributed amongst numerous molecules, including HCN, CH4, C2H2, C2H4, C2H6 and C3H6.
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页数:14
相关论文
共 51 条
[1]   Plasma assisted ignition and high-speed flow control: non-thermal and thermal effects [J].
Adamovich, I. V. ;
Choi, I. ;
Jiang, N. ;
Kim, J-H ;
Keshav, S. ;
Lempert, W. R. ;
Mintusov, E. ;
Nishihara, M. ;
Samimy, M. ;
Uddi, M. .
PLASMA SOURCES SCIENCE & TECHNOLOGY, 2009, 18 (03)
[2]   EVALUATED BIMOLECULAR ION-MOLECULE GAS-PHASE KINETICS OF POSITIVE-IONS FOR USE IN MODELING PLANETARY-ATMOSPHERES, COMETARY COMAE, AND INTERSTELLAR CLOUDS [J].
ANICICH, VG .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1993, 22 (06) :1469-1569
[3]  
[Anonymous], 1998, NIST CHEM KINETICS D
[4]   Improvement of the Diluted Propane Efficiency Treatment Using a Non-thermal Plasma [J].
Aubry, Olivier ;
Cormier, Jean-Marie .
PLASMA CHEMISTRY AND PLASMA PROCESSING, 2009, 29 (01) :13-25
[5]   Plasma reactivity and plasma-surface interactions during treatment of toluene by a dielectric barrier discharge [J].
Blin-Simiand, N. ;
Jorand, F. ;
Magne, L. ;
Pasquiers, S. ;
Postel, C. ;
Vacher, J. -R. .
PLASMA CHEMISTRY AND PLASMA PROCESSING, 2008, 28 (04) :429-466
[6]   Removal of formaldehyde in nitrogen and in dry air by a DBD: importance of temperature and role of nitrogen metastable states [J].
Blin-Simiand, N. ;
Pasquiers, S. ;
Jorand, F. ;
Postel, C. ;
Vacher, J-R .
JOURNAL OF PHYSICS D-APPLIED PHYSICS, 2009, 42 (12)
[7]  
BLINSIMIAND N, 2009, 19 INT S PLASM CHEM
[8]  
BLINSIMIAND N, 2008 11 INT S HIGH P
[9]  
BOHMER E, 1991, Z PHYS CHEM, V170, P15
[10]   RATES OF ENERGY TRANSFER FROM N2A3SIGMA+U TO VARIOUS MOLECULES - INITIAL AND FINAL QUANTUM STATES IN TRANSFER TO NOX2PI AND HG(61S0), AND VIBRATIONAL RELAXATION OF N2A3SIGMA+U(V=1) IN HELIUM [J].
CALLEAR, AB ;
WOOD, PM .
TRANSACTIONS OF THE FARADAY SOCIETY, 1971, 67 (578) :272-&