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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Rate constant measurements for the overall reaction of OH + 1-butanol → products from 900 to 1200 K
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Rate constant measurements for the overall reaction of OH + 1-butanol → products from 900 to 1200 K

机译：OH + 1-丁醇→产物从900到1200 K的总反应速率常数

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摘要

The rate constant for the overall reaction OH + 1-butanol → products was determined in the temperature range 900 to 1200 K from measurements of OH concentration time histories in reflected shock wave experiments of tert-butyl hydroperoxide (TBHP) as a fast source of OH radicals with 1-butanol in excess. Narrow-linewidth laser absorption was employed for the quantitative OH concentration measurement. A detailed kinetic mechanism was constructed that includes updated rate constants for 1-butanol and TBHP kinetics that influence the near-first-order OH concentration decay under the present experimental conditions, and this mechanism was used to facilitate the rate constant determination. The current work improves upon previous experimental studies of the title rate constant by utilizing a rigorously generated kinetic model to describe secondary reactions. Additionally, the current work extends the temperature range of experimental data in the literature for the title reaction under combustion-relevant conditions, presenting the first measurements from 900 to 1000 K. Over the entire temperature range studied, the overall rate constant can be expressed in Arrhenius form as 3.24 × 10 ~(-10) exp(-2505/T [K]) cm ~3 molecule ~(-1) s ~(-1). The influence of secondary reactions on the overall OH decay rate is discussed, and a detailed uncertainty analysis is performed yielding an overall uncertainty in the measured rate constant of ±20% at 1197 K and ±23% at 925 K. The results are compared with previous experimental and theoretical studies on the rate constant for the title reaction and reasonable agreement is found when the earlier experimental data were reinterpreted.
机译：在900到1200 K的温度范围内，通过测量作为快速OH来源的叔丁基氢过氧化氢（TBHP）的反射波实验中的OH浓度时间历史记录，确定了整个反应OH + 1-丁醇→产物的速率常数。自由基与过量的1-丁醇。窄线宽激光吸收用于定量OH浓度测量。构建了详细的动力学机制，包括在当前实验条件下影响近一阶OH浓度衰减的1-丁醇和TBHP动力学的更新速率常数，并使用该机制促进了速率常数的确定。当前的工作通过利用严格生成的动力学模型描述次级反应，改进了标题速率常数的先前实验研究。此外，当前的工作扩展了文献中有关燃烧相关条件下标题反应的实验数据的温度范围，首次测量的范围为900 K至1000K。在研究的整个温度范围内，总速率常数可以表示为阿累尼乌斯形式为3.24×10〜（-10）exp（-2505 / T [K]）cm〜3分子〜（-1）s〜（-1）。讨论了次级反应对整体OH衰减速率的影响，并进行了详细的不确定度分析，得出在1197 K下测得的速率常数为±20％，在925 K下为±23％的总体不确定度。重新解释较早的实验数据后，发现了有关标题反应速率常数和合理一致性的先前实验和理论研究。

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