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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Isotopic self-exchange reactions of water: Evaluation of the rule of the geometric mean in liquid-vapor isotope partitioning
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Isotopic self-exchange reactions of water: Evaluation of the rule of the geometric mean in liquid-vapor isotope partitioning

机译：水的同位素自交换反应：液-汽同位素分配中几何均值规则的评估

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摘要

Deviations from the random distribution of hydrogen isotopes among isotopic species of liquid and vapor water (the rule of the geometric mean) were critically assessed theoretically and experimentally from the triple to critical point of water. A third-order polynomial equation of the classical near-critical expansion was used to accurately describe the liquid-vapor isotope fractionation of H2O and D2O on the basis of their equations of state. It was found that experimental data for the enthalpy of mixing of H2O-D2O can be used to calculate accurately the deviation from the rule of the geometric mean in liquid and vapor water, 1n(K-D(v)/K-D(l)). A new equation obtained in this study shows that the value of 1n(K-D(v)/K-D(l)) smoothly decreases from +0.009 to 0 with increasing temperature from the triple to critical temperature of water. In contrast, the equation available in the literature and that derived from mass spectrometric measurements of liquid-vapor partitioning of H2O and HDO show complex behavior, including maximum, minimum, and crossover.
机译：从水的三重点到临界点，从理论和实验上严格评估了氢同位素在液体和蒸气水的同位素物种之间的随机分布的偏差（几何平均值的规则）。使用经典近临界膨胀的三阶多项式方程式，根据状态方程，精确描述了H2O和D2O的液汽同位素分馏。已经发现，H 2 O-D 2 O的混合焓的实验数据可以用来精确地计算与液体和蒸气水中的几何平均值的规则的偏差1n（K-D（v）/ K-D（l））。在这项研究中获得的新方程式表明，随着温度从水的三重温度升高到临界温度，1n（K-D（v）/ K-D（l））的值从+0.009平稳地减小到0。相反，文献中可用的方程式以及从质谱测量H2O和HDO的水蒸气分配得出的方程式显示出复杂的行为，包括最大，最小和交叉。

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