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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ab initio molecular dynamics study of the reaction of U~+ and U~(2+) with H_2O in the gas phase: Direct classical trajectory calculations
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Ab initio molecular dynamics study of the reaction of U~+ and U~(2+) with H_2O in the gas phase: Direct classical trajectory calculations

机译：U〜+和U〜（2+）与H_2O在气相中反应的从头算分子动力学研究：直接经典轨迹计算

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摘要

The gas phase reactions of U~+ and U~(2+) with H_2O were investigated using an ab initio molecular dynamics method. All of the information along the minimum energy path were calculated with density functional theory (DFT) and coupled cluster methods. For U~+ with H_2O, the molecular dynamics simulations yield a branching ratio of 86% for the H2 elimination channel to 14% for the H atomic elimination channel in agreement with the quadruple ion trap mass spectrometry (QIT/MS) experimental ratio of 91% to 9%. In the case of U~(2+) + H_2O, there is a crossing of the potential energy surfaces (PES) after the first transition state. Crossing seams between the PES and possible spin inversion processes were studied by means of the intrinsic reaction coordinate (IRC) approach. For U~(2+) with H_2O, all trajectories are corresponds to H atom elimination channel, this is consistent with the Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) experimental results. The chemical bonding evolution along the reaction pathways was discussed by using topological methodologies of the electron localization function (ELF).
机译：采用从头算分子动力学方法研究了U〜+和U〜（2+）与H_2O的气相反应。沿最小能量路径的所有信息均使用密度泛函理论（DFT）和耦合聚类方法进行计算。对于具有H_2O的U〜+，分子动力学模拟得出H2消除通道的支化率为86％，H原子消除通道的支化率为14％，与四重离子阱质谱（QIT / MS）实验比率91一致％到9％。在U〜（2+）+ H_2O的情况下，在第一个跃迁状态之后势能面（PES）发生交叉。通过固有反应坐标（IRC）方法研究了PES与可能的自旋反演过程之间的交叉接缝。对于具有H_2O的U〜（2+），所有轨迹都对应于H原子消除通道，这与傅立叶变换离子回旋共振质谱（FTICR-MS）实验结果一致。通过使用电子本地化功能（ELF）的拓扑方法讨论了沿着反应路径的化学键演化。

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