Loison Jean-Christophe, Bergeat Astrid
Université de Bordeaux, UMR 5255, ISM, Groupe Astrochimie, 351 cours de la Libération, F-33405 Talence Cedex, France.
Phys Chem Chem Phys. 2009 Jan 28;11(4):655-64. doi: 10.1039/b812810c.
The reactions of the CH radical with several unsaturated hydrocarbons C2H2 (acetylene), C2H4 (ethylene), C3H4 (methyl-acetylene and allene), C3H6 (propene) and C4H8 (trans-butene) were studied at room temperature, in a low-pressure fast-flow reactor. CH(X2pi, v = 0) radicals were obtained from the reaction of CHBr3 with potassium atoms. The overall rate constants at 300 K are CH + C2H2: (3.6 +/- 0.6) x 10(-10), CH + C2H4: (3.1 +/- 0.6) x 10(-10), CH + C3H4 (methyl-acetylene): (3.4 +/- 0.6) x 10(-10), CH + C3H4 (allene): (3.6 +/- 0.6) x 10(-10), CH + C3H6 (propene): (4.2 +/- 0.8) x 10(-10) and CH + C4H8 (trans-butene): (4.0 +/- 0.80) x 10(-10) cm3 molecule(-1) s(-1) (errors are cited at the level of +/- 1 sigma). Absolute atomic hydrogen production was determined by vacuum ultra-violet (VUV) resonance fluorescence, H production from the CH + CH4 reaction being used as a reference. Observed H branching ratios for these CH reactions were: C2H2: 0.90 +/- 0.08, C2H4: 0.94 +/- 0.08, C3H4 (methyl-acetylene): 0.98 +/- 0.08, C3H4 (allene): 0.97 +/- 0.08, C3H6 (propene): 0.78 +/- 0.10, C4H8 (trans-butene): 0.69 +/- 0.12 (errors are cited at the level of +/- 1 sigma). A compilation of the available kinetic data on these reactions has been made in order to propose rate coefficients for each possible channel of the different reactions for astrochemical models.
在室温下,于低压快速流动反应器中研究了CH自由基与几种不饱和烃C2H2(乙炔)、C2H4(乙烯)、C3H4(甲基乙炔和丙二烯)、C3H6(丙烯)和C4H8(反-丁烯)的反应。CH(X2π, v = 0)自由基由CHBr3与钾原子的反应获得。300K时的总速率常数为:CH + C2H2:(3.6 ± 0.6)×10^(-10),CH + C2H4:(3.1 ± 0.6)×10^(-10),CH + C3H4(甲基乙炔):(3.4 ± 0.6)×10^(-10),CH + C3H4(丙二烯):(3.6 ± 0.6)×10^(-10),CH + C3H6(丙烯):(4.2 ± 0.8)×10^(-10),CH + C4H8(反-丁烯):(4.0 ± 0.80)×10^(-10) cm³·分子⁻¹·s⁻¹(误差为±1σ水平)。通过真空紫外(VUV)共振荧光测定绝对氢原子生成量,以CH + CH4反应产生的H作为参考。这些CH反应中观察到的H分支比为:C2H2:0.90 ± 0.08,C2H4:0.94 ± 0.08,C3H4(甲基乙炔):0.98 ± 0.08,C3H4(丙二烯):0.97 ± 0.08,C3H6(丙烯):0.78 ± 0.10,C4H8(反-丁烯):0.69 ± 0.12(误差为±1σ水平)。已对这些反应的现有动力学数据进行汇编,以便为天体化学模型中不同反应的每个可能通道提出速率系数。