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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >A Shock-Tube Study of the Rate Constant of PH3 + M reversible arrow PH2 + H + M (M = Ar) Using PH3 Laser Absorption
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A Shock-Tube Study of the Rate Constant of PH3 + M reversible arrow PH2 + H + M (M = Ar) Using PH3 Laser Absorption

机译：使用PH3激光吸收的PH3 + M可逆箭头PH2 + H + M（M = AR）的抗冲击管研究

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摘要

Phosphine (PH3) is a highly reactive and toxic gas. Prior experimental investigations of PH3 pyrolysis reactions have included only low-temperature measurements. This study reports the first shock-tube measurements of PH3 pyrolysis using a new PH3 laser absorption technique near 4.56 mu m. Experiments were conducted in mixtures of 0.5% PH3/Ar behind reflected shock waves at temperatures of 1460-2013 K and pressures of similar to 1.3 and similar to 0.5 atm. The PH3 time histories displayed two-stage behavior similar to that previously observed for NH3 decomposition, suggesting by analogy that the rate constant for PH3 + M reversible arrow PH2 + H + M (R1) could be determined. A simple three-step mechanism was assembled for data analysis. In a detailed kinetic analysis of the first-stage PH3 decomposition, values of k(1,0 )were obtained and best described by (in cm(3).mol(-1.)s(-1)) k(1,0) = 7.78 x 10(17 )exp(-80,400/RT), with units of cal, mol, K, s, and cm(3). Agreement between the 1.3 and 0.5 atm data confirmed that the measured k(1,0) was in the low-pressure limit. Agreement of the experimental k(1,0) with ab initio estimates resolved the question of the main pathway of PH3 decomposition: it proceeds as PH3 reversible arrow PH2 + H instead of PH3 reversible arrow PH + H-2.
机译：膦（pH3）是高度反应性和有毒的气体。 PH3热解反应的现有实验研究仅包括低温测量。本研究报告了使用新的PH3激光吸收技术在4.56 mu m附近的第一个震动管测量pH3热解。在0.5％pH3 / AR的混合物中进行实验，在反射冲击波的温度下，在1460-2013K的温度和类似于1.3的压力下，与0.5atm类似。 PH3时间历史显示出类似于先前对于NH3分解的两阶段行为，这通过类比可以确定PH3 + M可逆箭头PH2 + H + M（R1）的速率常数。组装了一个简单的三步机制，用于数据分析。在第一阶段PH3分解的详细动力学分析中，获得K（1,0）的值并最佳地描述（以cm（3）.mol（-1。）s（-1））k（1， 0）= 7.78 x 10（17）exp（-80,400 / RT），具有Cal，Mol，K，S和CM（3）单元。 1.3和0.5 ATM数据之间的协议确认测量的K（1,0）处于低压极限。实验k（1,0）与AB初始估计的同意解决了pH3分解的主要途径的问题：它作为pH3可逆箭头pH2 + h而不是pH3可逆箭头pH + H-2。

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