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Predicting Glass-to-Glass and Liquid-to-Liquid Phase Transitions in Supercooled Water using Classical Nucleation Theory
Chemical Physics ( IF 2.3 ) Pub Date : 2017-11-13 , DOI: 10.1016/j.chemphys.2017.11.008
Robert F. Tournier

Glass-to-glass and liquid-to-liquid phase transitions are observed in bulk and confined water, with or without applied pressure. They result from the competition of two liquid phases separated by an enthalpy difference depending on temperature. The classical nucleation equation of these phases is completed by this quantity existing at all temperatures, a pressure contribution, and an enthalpy excess. This equation leads to two homogeneous nucleation temperatures in each liquid phase; the first one (Tn- below Tm) being the formation temperature of an “ordered” liquid phase and the second one corresponding to the overheating temperature (Tn+ above Tm). Thermodynamic properties, double glass transition temperatures, sharp enthalpy and volume changes are predicted in agreement with experimental results. The first-order transition line at TLL=0.833×Tm between fragile and strong liquids joins two critical points. Glass phase above Tg becomes “ordered” liquid phase disappearing at TLL at low pressure and at Tn+=1.302×Tm at high pressure.



中文翻译:

使用经典成核理论预测过冷水中的玻璃到玻璃和液体到液体的相变

在有或没有施加压力的情况下,在散装和承压水中观察到玻璃到玻璃和液相到液相的转变。它们是由两个液相的竞争所决定,这两个液相之间的焓差取决于温度。这些相的经典成核方程由在所有温度下存在的该量,压力贡献和焓过量来完成。该方程式在每个液相中导致两个均匀的成核温度。第一个温度(低于T m的T n-)是“有序”液相的形成温度,第二个温度对应于过热温度(T m +高于T m))。与实验结果一致地预测了热力学性质,双重玻璃化转变温度,急剧的焓和体积变化。易碎液体和强液体之间的T LL = 0.833×T m的一阶过渡线连接了两个临界点。高于T g的玻璃相变成“有序”液相,低压在T LL消失,高压在T n + = 1.302×T m消失。

更新日期:2017-11-13
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