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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetics of the O(~3P) + N_2O Reaction. 1. Direct Measurements at Intermediate Temperatures
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Kinetics of the O(~3P) + N_2O Reaction. 1. Direct Measurements at Intermediate Temperatures

机译：O（〜3P）+ N_2O反应的动力学。 1.中间温度下的直接测量

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Rate coefficients for the consumption of O atoms by their reaction with N_2O have been measured, at pressures from 130 to 500 mbar, using the high-temperature photochemistry technique. These represent the first direct measurements of k values of the reaction. The ground-state oxygen atoms were produced by laser photolysis of SO_2, or by flash photolysis of either SO_2 or O_2, and monitored by time-resolved resonance fluorescence. The results yield k(1075-1140 K) = 3.2 * 10~(-11) exp(-9686K/T) cm~3 molecule~(-1) s~(-1) with 2σ precision limits of ±12% and corresponding 2σ accuracy limits of ±25%. Results from several sources in the literature indicate a high sensitivity of the O + N_2O reaction system to traces of H_2O, which increases the rates if present as a contaminant. For this reason, possible effects of traces of H_2O on the results were modeled. Simulated decay curves with a hypothetical H_2O contaminant were used as a test of the experimental data reduction procedures. Although the concentration of H_2O needed to significantly affect the results is small, the amount that could have been present is even less and is shown to have had negligible effects. The results are in qualitative agreement with a recent T ≥ 1680 K shock tube study (D. F. Davidson, M. D. DiRosa, A. Y. Chang, and R. K. Hanson, ref 9) in that extrapolation of their results to the present temperatures indicates rate coefficients much larger than had been previously thought. However, though the results agree within error limits for such a long extrapolation, the present results are about a factor of 4 smaller. Combined with the results of the companion paper by Meagher and Anderson (ref 6, following paper in this issue), in which the prior literature is critically reevaluated, it is found that the O_2 + N_2 product channel dominates at the present temperatures.
机译：已经使用高温光化学技术在130至500 mbar的压力下测量了O原子与N_2O反应所消耗的速率系数。这些代表反应的k值的首次直接测量。基态氧原子是通过SO_2的激光光解或SO_2或O_2的快速光解产生的，并通过时间分辨共振荧光进行监测。结果产生k（1075-1140 K）= 3.2 * 10〜（-11）exp（-9686K / T）cm〜3分子〜（-1）s〜（-1），2σ精度极限为±12％，相应的2σ精度极限为±25％。文献中的几种来源的结果表明，O + N_2O反应系统对痕量的H_2O具有很高的敏感性，如果以污染物形式存在，则会提高速率。因此，对痕量的H_2O对结果的可能影响进行了建模。具有假定的H_2O污染物的模拟衰减曲线用作测试实验数据减少程序的测试。尽管显着影响结果所需的H_2O浓度很小，但可能存在的量甚至更少，而且显示出的影响微不足道。结果与最近的T≥1680 K激波管研究（DF Davidson，MD DiRosa，AY Chang和RK Hanson，参考文献9）的定性一致，因为将其结果外推到当前温度表明速率系数远大于以前被认为。然而，尽管对于这样长的外推结果在误差范围内是一致的，但是当前结果大约小4倍。结合Meagher和Anderson的伴随论文的结果（本期后继文献6），对现有文献进行了严格的重新评估，发现在当前温度下O_2 + N_2产物通道占主导地位。

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