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50至296K温度范围内O(D)原子与乙烷和乙炔反应的速率常数及氢原子产物产率

Rate Constants and H-Atom Product Yields for the Reactions of O(D) Atoms with Ethane and Acetylene from 50 to 296 K.

作者信息

Nuñez-Reyes Dianailys, Hickson Kevin M

机构信息

Université de Bordeaux , Institut des Sciences Moléculaires , F-33400 Talence , France.

CNRS , Institut des Sciences Moléculaires , F-33400 Talence , France.

出版信息

J Phys Chem A. 2018 May 24;122(20):4696-4703. doi: 10.1021/acs.jpca.8b02267. Epub 2018 May 11.

DOI:10.1021/acs.jpca.8b02267
PMID:29715024
Abstract

The gas phase reactions of atomic oxygen in its first excited state with ethane and acetylene have been investigated in a continuous supersonic flow reactor over the temperature range from 50 to 296 K. O(D) atoms were produced by the pulsed laser photolysis of ozone at 266 nm. Two different types of experiments, kinetics measurements and H-atom product yield determinations, were performed by detecting O(D) atoms and H(S) atoms, respectively, by vacuum ultraviolet laser-induced fluorescence. The measured rate constants are in agreement with previous work at room temperature, and little or no temperature dependence was observed as the temperature was decreased to 50 K. H-atom yields were found to be independent of temperature for the reaction of O(D) with ethane. These product yields are discussed in the context of earlier dynamics measurements at higher temperature. Due to the influence of secondary reactions, no H-atom yields could be obtained for the reaction of O(D) with acetylene.

摘要

在50至296K的温度范围内,利用连续超声速流动反应器研究了处于第一激发态的原子氧与乙烷和乙炔的气相反应。通过266nm脉冲激光光解臭氧产生O(D)原子。分别通过真空紫外激光诱导荧光检测O(D)原子和H(S)原子,进行了两种不同类型的实验,即动力学测量和H原子产物产率测定。测得的速率常数与之前在室温下的工作一致,当温度降至50K时,几乎未观察到温度依赖性。发现O(D)与乙烷反应的H原子产率与温度无关。这些产物产率将结合早期在较高温度下的动力学测量结果进行讨论。由于二级反应的影响,无法获得O(D)与乙炔反应的H原子产率。

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