A Kinetic Study on the Conversion of Methane to Higher Hydrocarbons in a Radio-Frequency Discharge

Sergey Y. Savinov; Hwaung Lee; Hyung Keun Song; Byung-Ki Na

Korean Journal of Chemical Engineering, Vol.21, No.3, 601-610, May, 2004

DOI10.1007/BF02705494 Export Citation

A Kinetic Study on the Conversion of Methane to Higher Hydrocarbons in a Radio-Frequency Discharge

Sergey Y. Savinov, Hwaung Lee¹, Hyung Keun Song¹, and Byung-Ki Na^{2, †}

Low Temperature Plasma Optics Department, P.N. Lebedev Physical Institute, Leninsky prospect, 53, 117924 Moscow, Russian Federation
¹Clean Technology Research Center, KIST, P.O.Box 131, Cheongryang, Seoul 136-791, Korea
²School of Chemical Engineering, Chungbuk National University, Cheongju, Chungbuk 361-763, Korea

E-mail:

This study investigated methane conversion with direct current discharge at low pressure in a radio frequency. The main gaseous products of the reaction were ethane, ethylene, acetylene and propane. This study was concentrated on the influence of discharge conditions on the conversion of methane to higher hydrocarbons. Reaction temperature, electron density and mean residence time were calculated from experimental data and mathematical relations. The maximum conversion of the methane was about 45% with the pure methane as a reactant. Ethane was the main product when the reaction occurred in the glow discharge. Ethane selectivity decreased with the increase of the gas temperature. The kinetics of reactions was also analyzed from possible reaction equations and various rate constant data. Consequently, the dissociation constant and the density of radicals could be obtained at any experimental conditions.

Keywords:Plasma;Methane;Conversion;Radio-frequency Discharge;Kinetics

[References]

Arigorev IS, Melihov EZ, "Physical Constants," Energoatomizdat, Moscow (1991)
Baulch DL, Drysdale DD, Horne DG, Lloyd AC, "Evaluated Kinetics Data for High Temperature Reactions," Univ. of Leads, V. 1 (1972)
Bird RB, Stewart WE, Lightfoot EN, "Transport Phenomena," John Wiley & Sons, New York (1960)
Brunet H, Lavarini B, Phys. Lett. A, 30, 181 (1969)
Cho W, Baek Y, Pang H, Kim YC, Korean J. Chem. Eng., 15(5), 500 (1998)
Dean AM, J. Phys. Chem., 94, 1432 (1990)
Granovsky VL, "Electric Current in Gas," Moscow (1952)
Hwang BB, Yeo YK, Na BK, Korean J. Chem. Eng., 20(4), 631 (2003)
Jeong HK, Kim SC, Han C, Lee H, Song HK, Na BK, Korean J. Chem. Eng., under revision (2001)
Kassel LS, Am. Chem. Soc., 54, 3949 (1932)
Kim SS, Lee H, Na BK, Song HK, Korean J. Chem. Eng., 20(5), 869 (2003)
Lee H, Savinov SY, Song HK, Na BK, J. Chem. Eng. Jpn., 34(11), 1356 (2001)
Lieberman MA, Lichtenberg AJ, "Principles of Plasma Discharge and Material Processing," John Wiley & Sons, New York (1994)
Na BK, Choi JW, Lee H, Song HK, Korean J. Chem. Eng., 19(6), 917 (2002)
Ochkin VN, Savinov YS, Sovolev NN, "Electron Excited Molecules in Nonequilibrium Plasma," N.Y. Niva Publ., Proc. Lebedev Phys. Inst., V. 179, Suppl. V.2 (1989)
Raizer YP, "Gas Discharge Physics," Springer-Verlag, Berlin (1991)
Rusanov VD, Fridman AA, "Physics of Chemically Active Plasma," Nauka, Moscow (1984)
Savinov SY, Lee H, Song HK, Na BK, Ind. Eng. Chem. Res., 38(7), 2540 (1999)
Savinov SY, Lee H, Song HK, Na BK, Korean J. Chem. Eng., 19(4), 564 (2002)
Savinov SY, Lee H, Song HK, Na BK, Plasma Chem. Plasma Process., 23(1), 159 (2003)

[Referenced By]

[Related Articles]

[1] Arigorev IS, Melihov EZ, "Physical Constants," Energoatomizdat, Moscow (1991)

[2] Baulch DL, Drysdale DD, Horne DG, Lloyd AC, "Evaluated Kinetics Data for High Temperature Reactions," Univ. of Leads, V. 1 (1972)

[3] Bird RB, Stewart WE, Lightfoot EN, "Transport Phenomena," John Wiley & Sons, New York (1960)

[4] Brunet H, Lavarini B, Phys. Lett. A, 30, 181 (1969)

[5] Cho W, Baek Y, Pang H, Kim YC, Korean J. Chem. Eng., 15(5), 500 (1998)

[6] Dean AM, J. Phys. Chem., 94, 1432 (1990)

[7] Granovsky VL, "Electric Current in Gas," Moscow (1952)

[8] Hwang BB, Yeo YK, Na BK, Korean J. Chem. Eng., 20(4), 631 (2003)

[9] Jeong HK, Kim SC, Han C, Lee H, Song HK, Na BK, Korean J. Chem. Eng., under revision (2001)

[10] Kassel LS, Am. Chem. Soc., 54, 3949 (1932)

[11] Kim SS, Lee H, Na BK, Song HK, Korean J. Chem. Eng., 20(5), 869 (2003)

[12] Lee H, Savinov SY, Song HK, Na BK, J. Chem. Eng. Jpn., 34(11), 1356 (2001)

[13] Lieberman MA, Lichtenberg AJ, "Principles of Plasma Discharge and Material Processing," John Wiley & Sons, New York (1994)

[14] Na BK, Choi JW, Lee H, Song HK, Korean J. Chem. Eng., 19(6), 917 (2002)

[15] Ochkin VN, Savinov YS, Sovolev NN, "Electron Excited Molecules in Nonequilibrium Plasma," N.Y. Niva Publ., Proc. Lebedev Phys. Inst., V. 179, Suppl. V.2 (1989)

[16] Raizer YP, "Gas Discharge Physics," Springer-Verlag, Berlin (1991)

[17] Rusanov VD, Fridman AA, "Physics of Chemically Active Plasma," Nauka, Moscow (1984)

[18] Savinov SY, Lee H, Song HK, Na BK, Ind. Eng. Chem. Res., 38(7), 2540 (1999)

[19] Savinov SY, Lee H, Song HK, Na BK, Korean J. Chem. Eng., 19(4), 564 (2002)

[20] Savinov SY, Lee H, Song HK, Na BK, Plasma Chem. Plasma Process., 23(1), 159 (2003)