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A shock tube study of the decomposition of cyclohexane and 1-hexene.

机译:冲击管研究环己烷和1-己烯的分解。

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The decomposition of cyclohexane (c-C6H12) was studied in 131 experiments using a shock tube and the laser-schlieren technique over 1400-2000 K and from 25 to 200 Torr using mixtures of 2, 4, 10, and 20% cyclohexane in Kr. The reaction is shown to be an initial isomerization to 1-hexene 1 c-C6H12→1-C 6H121-hexene DH298Ko=19.19 kcal/gmol followed by rapid dissociation of 1-hexene to allyl and n-propyl radicals 2 1-C6H12→C 3H5allyl+ C3H7n-propyl DH298Ko=71.82 kcal/gmol which further decompose initiating a complex chain reaction. To facilitate analysis, the decomposition of 1-hexene is also examined over 1200-1700 K for 50 Torr and 200 Torr using 2 and 3% 1-hexene in Kr.;Fall-off rate constants were obtained for (1) and (2) by simulating experimental data using cyclohexane and 1-hexene dissociation mechanisms. High-pressure limit rate constants were obtained by extrapolating the fall-off rates using RRKM theory. The extrapolated high-pressure rates are in good agreement with much of the literature data.;At low pressures and/or at high temperatures, cyclohexane may directly dissociate via a 'one-step' process to C3H5 and C3H7 radicals through chemically activated 1- hexene. 1a c-C6H12 →C3H5+3H7;This 'one-step' process is hinted at by our low pressure experiments but still cannot be clearly distinguished from the 'two-step' process (reaction (1) followed by (2)). The presence of the 'one-step' process was ultimately found to have little effect on the rate of cyclohexane dissociation.
机译:环己烷(c-C6H12)的分解在131个实验中进行了研究,使用的是激波管和schlieren激光技术,在1400-2000 K和25至200 Torr的条件下,使用2%,4%,10%和20%的环己烷在Kr中的混合物。该反应显示为初始异构化为1-己烯1 c-C6H12→1-C 6H121-己烯DH298Ko = 19.19 kcal / gmol,然后将1-己烯快速解离为烯丙基和正丙基2 1 -C6H12→ C 3H5烯丙基+ C3H7n-丙基DH298Ko = 71.82kcal / gmol,进一步分解,引发复杂的链反应。为便于分析,还使用2%和3%的Kr溶液在1200-1700 K的温度下对50 Torr和200 Torr的1-己烯进行了分解研究;获得了(1)和(2)的衰减速率常数)通过使用环己烷和1-己烯解离机理模拟实验数据。高压极限速率常数是通过使用RRKM理论外推下降速率而获得的。外推的高压速率与许多文献数据都非常吻合。在低压和/或高温下,环己烷可能会通过“一步法”直接通过化学活化的1-解离成C3H5和C3H7自由基。己烯。 1a c-C6H12→C3H5 + 3H7;我们的低压实验暗示了这一``一步''过程,但仍不能与``两步''过程清楚地区分(反应(1)之后是(2))。最终发现“一步法”工艺的存在对环己烷的解离速率几乎没有影响。

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