An optimised molecular model for ammonia
An optimised molecular model for ammonia
复制标题
氨的优化分子模型
DOI：
10.1080/00268970802112137
复制
发表时间：
2008
影响因子：
1.7
通讯作者：
H. Hasse
中科院分区：
文献类型：
--
作者：
Bernhard Eckl;J. Vrabec;H. Hasse
氨的优化分子模型，其基于Kristóf等人的先前工作[Mol. Phys.97，1129（1999）]。通过在第一模型中包括来自从头算量子力学计算的几何和静电学数据来实现改进。之后的Lennard-Jones势，建模分散和排斥相互作用的参数，优化实验纯氨的汽液平衡数据。由此产生的分子模型显示平均无符号偏差实验的0.7%的饱和液体密度，1.6%的蒸汽压，和2.7%的汽化焓在整个温度范围内从三相点到临界点。这种新的分子模型用于预测液体，蒸汽和超临界区域的热物理性质，这与高精度的状态方程非常吻合，该状态方程被优化为1147个实验数据集。此外，它还能够正确地预测径向分布函数，而在优化过程中不使用结构信息。
An optimised molecular model for ammonia, which is based on a previous work of Kristóf et al. [Mol. Phys. 97, 1129 (1999)], is presented. Improvements are achieved by including data on geometry and electrostatics from ab initio quantum mechanical calculations in a first model. Afterwards the parameters of the Lennard–Jones potential, modelling dispersive and repulsive interactions, are optimised to experimental vapour–liquid equilibrium data of pure ammonia. The resulting molecular model shows mean unsigned deviations to experiment of 0.7% in saturated liquid density, 1.6% in vapour pressure, and 2.7% in enthalpy of vapourisation over the whole temperature range from triple point to critical point. This new molecular model is used to predict thermophysical properties in the liquid, vapour and supercritical region, which are in excellent agreement with a high precision equation of state, that was optimised to 1147 experimental data sets. Furthermore, it is also capable of predicting the radial distribution functions properly, while no structural information is used in the optimisation procedure.