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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetic Isotope Effect in the Gas-Phase Reaction of Muonium with Molecular Oxygen
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Kinetic Isotope Effect in the Gas-Phase Reaction of Muonium with Molecular Oxygen

机译：Molecular与分子氧的气相反应中的动力学同位素效应

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摘要

The rate constant of the gas-phase addition reaction of the light hydrogen isotope muonium to molecular oxygen, Mu + O_2 -> MuO_2, was measured over a range of temperatures from 115 to 463 K at a pressure of 2 bar and from 16 to 301 bar at room temperature, using N_2 as the moderator gas. The reaction remains in the termolecular regime over the entire pressure range. At room temperature, the average low-pressure limiting rate constant is k_(ch)~o (Mu) = (8.0 +- 2.1) * 10~(-33) cm~6 s~(-1), a factor of almost 7 below the corresponding rate constant for the H+O_2 addition reaction, k_(ch)~o (H). In contrast to k_(ch)~o (H), which exhibits a clear negative temperature dependence, k_(ch)~o (Mu) is essentially temperature independent. At room temperature, the kinetic isotope effect (KIE) is strongly pressure (density) dependent and is reversed at pressures near 300 bar. The kinetics are analyzed based on the statistical adiabatic channel model of Troe using a Morse potential, which works well in reproducing the overall KIE. The major factors governing the isotope effect are differences in the moment of inertia and density of vibrational states of the addition complex.
机译：在2 bar和16至301的压力下，在115至463 K的温度范围内，测定了轻氢同位素mu与分子氧的气相加成反应速率常数Mu + O_2-> MuO_2室温下，使用N_2作为缓和气体。反应在整个压力范围内保持在分子状态。在室温下，平均低压极限率常数为k_（ch）〜o（Mu）=（8.0 +-2.1）* 10〜（-33）cm〜6 s〜（-1），几乎是在低于H + O_2加成反应的相应速率常数k_（ch）〜o（H）的条件下降低7。与表现出明显的负温度依赖性的k_（ch）〜o（H）相反，k_（ch）〜o（Mu）本质上与温度无关。在室温下，动力学同位素效应（KIE）很大程度上取决于压力（密度），并且在接近300 bar的压力下会逆转。基于特洛的统计绝热通道模型，使用莫尔斯电势对动力学进行了分析，在复制整个KIE时效果很好。控制同位素效应的主要因素是加成络合物的惯性矩和振动态密度的差异。

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