Molecular Dynamics Simulation Reveals a Change in the Structure of Liquid Water Near 150?°C, which May Explain Apparent Anomalies in High-Temperature Water Radiolysis
Molecular Dynamics Simulation Reveals a Change in the Structure of Liquid Water Near 150?°C, which May Explain Apparent Anomalies in High-Temperature Water Radiolysis
复制标题
分子动力学模拟揭示了150°C附近液态水结构的变化，这可能解释了高温水辐射分解中的明显异常
DOI：
10.1007/s42250-022-00513-2
复制
发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Soldera A.
中科院分区：
文献类型：
--
作者：
Ndongo Assomo J. G. G.;Ebrahimi S.;Muroya Y.;Jay-Gerin J.-P.;Soldera A.
SPC/E分子动力学模拟被用来研究在25℃和350℃的恒压下，液态水的结构随温度的变化。对计算的氧-氧(O-O)和氧-氢(O-H)径向分布函数的分析表明，水在150℃左右经历了结构变化，其特征是O-O/O-H配位数大幅下降。这种结构变化可以解释在高温下实验观察到的水的辐解过程中的一些明显异常。这包括二次次激发电子的热化距离和两个水合电子的双分子反应速率常数，它们都在150℃附近经历了突然而急剧的下降。
SPC/E molecular dynamics simulations are used to examine the structure of liquid water as a function of temperature between 25 and 350 °C at a constant pressure of 25 MPa. Analysis of the calculated oxygen–oxygen (O–O) and oxygen-hydrogen (O–H) radial distribution functions shows that water undergoes a structural change around 150 °C, characterized by large drops in the O–O/O–H coordination numbers. This structural change could explain some apparent anomalies experimentally observed in the radiolysis of water at elevated temperatures. These include the thermalization distance of secondary subexcitation electrons and the rate constant of the bimolecular reaction of two hydrated electrons, both of which experience a sudden and sharp drop near 150 °C.