Decomposition of benzene in the RF plasma environment - Part II. Formation of polycyclic aromatic hydrocarbons

被引:18
作者
Shih, SI [1 ]
Lin, TC [1 ]
Shih, ML [1 ]
机构
[1] Natl Cheng Kung Univ, Dept Environm Engn, Tainan 70101, Taipei, Taiwan
关键词
polycyclic aromatic hydrocarbons (PAHs); radio-frequency (RF); plasma; benzene (C6H6); decomposition;
D O I
10.1016/j.jhazmat.2004.09.030
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study investigated the characteristics of polycyclic aromatic hydrocarbons (PAHs) formed during the decomposition of benzene (C6H6) in radio-frequency (RF) plasma environments. The identification and quantification were accomplished by using a GC/MS for PAHS and an on-line Fourier transform infrared (FT-IR) spectrometer for the reactants and gaseous products. The analytical results show that PAHs were formed in both C6H6/Ar and C6H6/Ar,/Ar systems. In terms of individual PAHs, naphthalene (C10HS) was the predominant species was found among the 21 PAHs under all operational conditions, phenanthrene and chrysene are the next. High-ring RAHs did not form easily in the C6H6/Ar and C6H6/Ar,/Ar system, especially at high input power and high C-6 feed concentration (C-C6H6) for the former system. Yields of PAHs with different ring numbers decreased with increasing ring number. At low input power, increasing C-C6H6 would promote yields of PAHs, while adding hydrogen as the auxiliary gas suppressed PAHs formation. Higher input power or addition of oxygen not only effectively suppresses PAHs formation but also completely destroys C6H6. Owing to the absence of the principal intermediate species. phenol (C6H6OH). from the gas products of C6H6/O-2/Ar system, H-abstraction-C2H2-addition (HACA) pathway is proposed as the primary mechanism for PAHs formation in the present study. Gas phase distribution of total-PAHs accounts for 20-95.3 % at -2 % of CC6H6 among C6H6/Ar, C6H6/H-2/Ar and C6H6/O-2/Ar systems. This study suggests that gas-phase PAHs should not be ignored, particularly in C6H6/Ar systems under high input power and high C-C6H6, or in C6H6/O-2/Ar systems. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:149 / 159
页数:11
相关论文
共 37 条
[1]   ABSORPTION SPECTRA OF POLYATOMIC MOLECULES AT HIGH TEMPERATURES .2. BENZENE AND PERFLUOROBENZENE. KINETICS OF PYROLYSIS OF BENZENE [J].
BAUER, SH ;
ATEN, CF .
JOURNAL OF CHEMICAL PHYSICS, 1963, 39 (05) :1253-&
[2]   Mechanisms for polycyclic aromatic hydrocarbon (PAH) growth [J].
Bauschlicher, CW ;
Ricca, A .
CHEMICAL PHYSICS LETTERS, 2000, 326 (3-4) :283-287
[3]   LASER IONIZATION TIME-OF-FLIGHT MASS-SPECTROMETRY COMBINED WITH RESIDUAL-GAS ANALYSIS FOR THE INVESTIGATION OF MODERATE TEMPERATURE BENZENE OXIDATION [J].
BERMUDEZ, G ;
PFEFFERLE, L .
COMBUSTION AND FLAME, 1995, 100 (1-2) :41-51
[4]   Destruction of benzene with non-thermal plasma in dielectric barrier discharge reactors [J].
Cal, MP ;
Schluep, M .
ENVIRONMENTAL PROGRESS, 2001, 20 (03) :151-156
[5]   Ultrasound-induced cracking and pyrolysis of some aromatic and naphthenic hydrocarbons [J].
Cataldo, F .
ULTRASONICS SONOCHEMISTRY, 2000, 7 (01) :35-43
[6]   An experimental study of benzene oxidation at fuel-lean and stoichiometric equivalence ratio conditions [J].
Chai, Y ;
Pfefferle, LD .
FUEL, 1998, 77 (04) :313-320
[7]   Baseline contamination assessment for a new resource facility in Germany .6. Levels and profiles of polycyclic aromatic hydrocarbons (PAH) in ambient air [J].
Dorr, G ;
Hippelein, M ;
Kaupp, H ;
Hutzinger, O .
CHEMOSPHERE, 1996, 33 (08) :1569-1578
[8]   Methane pyrolysis: Thermodynamics [J].
Gueret, C ;
Daroux, M ;
Billaud, F .
CHEMICAL ENGINEERING SCIENCE, 1997, 52 (05) :815-827
[9]   KINETICS OF THERMAL DECOMPOSITION OF BENZENE IN A FLOW SYSTEM [J].
HOU, KC ;
PALMER, HB .
JOURNAL OF PHYSICAL CHEMISTRY, 1965, 69 (03) :863-&
[10]   Converting methane by using an RF plasma reactor [J].
Hsieh, LT ;
Lee, WJ ;
Chen, CY ;
Chang, MB ;
Chang, HC .
PLASMA CHEMISTRY AND PLASMA PROCESSING, 1998, 18 (02) :215-239