基于团簇结构模型的Na_2O-Al_2O_3-SiO_2三元体系熔体吉布斯混合摩尔自由能计算  

Molar Gibbs Mixing Free Energy Calculation for a Na_2O-Al_2O_3-SiO_2 Ternary Melt Based on the Cluster Model

作　　者：李永康 尤静林[1] 王建[1] 王敏[1] 马楠 魏广超 

机构地区：[1]省部共建高品质特殊钢冶金与制备国家重点实验室,上海市钢铁冶金新技术开发应用重点实验室,上海大学材料科学与工程学院,上海200072

出　　处：《物理化学学报》2016年第3期631-637,共7页Acta Physico-Chimica Sinica

基　　金：国家自然科学基金重点项目(50932005);国家自然科学基金(20973107,40973046);上海科学技术委员会(12520709200);澳大利亚Flagship的科学与工业研究组织CSIRO资助项目~~

摘　　要：以三元硅酸盐熔体团簇结构模型为基础,选取了Na_2O-Al_2O_3-SiO_2体系不同成分的团簇结构,采用半经验量子化学方法MNDO/d分别计算该三元体系熔体中不同结构的团簇基元在1473、1873、2000 K温度下的熵、焓、热容和自由能等热力学数据,计算得出不同团簇结构基元的混合自由能,并根据统计热力学波尔兹曼分布定律,推导计算得出Na_2O-Al_2O_3-SiO_2三元体系各成分下的混合摩尔自由能。三元硅酸盐熔体的热力学性质与该熔体的微观结构密切相关。Based on the cluster model of molten ternary silicates, the thermodynamic properties, including entropy, enthalpy, and heat capacity of Na_2O-Al_2O_3-SiO_2 at 1473, 1873, and 2000 K were calculated by the modified neglect of differential overlap（MNDO/d） semi-empirical method based on the primitive assumption of clusters in the melt. The mixing free energies of the Na_2O-Al_2O_3-SiO_2 ternary system were derived. The mixing free energy of the Na_2O-Al_2O_3-SiO_2 ternary system is the sum of all the cluster units that exist according to the Boltzmann distribution law. The thermodynamic properties of this ternary silicate melt depend on its microstructure.

关 键 词：Na2O-Al2O3-SiO2 团簇结构模型 熔体 混合摩尔自由能 

分 类 号：O611.2[理学—无机化学]