物理化学学报 >> 2016, Vol. 32 >> Issue (3): 631-637.doi: 10.3866/PKU.WHXB201512281

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基于团簇结构模型的Na2O-Al2O3-SiO2三元体系熔体吉布斯混合摩尔自由能计算

李永康,尤静林*(),王建,王敏,马楠,魏广超   

  • 收稿日期:2015-09-28 发布日期:2016-03-04
  • 通讯作者: 尤静林 E-mail:jlyou@163.com
  • 基金资助:
    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

Molar Gibbs Mixing Free Energy Calculation for a Na2O-Al2O3-SiO2 Ternary Melt Based on the Cluster Model

Yong-Kang LI,Jing-Lin YOU*(),Jian WANG,Min WANG,Nan MA,Guang-Chao WEI   

  • Received:2015-09-28 Published:2016-03-04
  • Contact: Jing-Lin YOU E-mail:jlyou@163.com
  • Supported by:
    the Key Project of National Natural Science Foundation of China(50932005);National Natural Science Foundation ofChina(20973107, 40973046);Shanghai Committee of Science and Technology, China(12520709200);CSIRO Minerals Down Under Flagship of Australia

摘要:

以三元硅酸盐熔体团簇结构模型为基础,选取了Na2O-Al2O3-SiO2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Na2O-Al2O3-SiO2三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。

关键词: Na2O-Al2O3-SiO2, 团簇结构模型, 熔体, 混合摩尔自由能

Abstract:

Based on the cluster model of molten ternary silicates, the thermodynamic properties, including entropy, enthalpy, and heat capacity of Na2O-Al2O3-SiO2 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 Na2O-Al2O3-SiO2 ternary system were derived. The mixing free energy of the Na2O-Al2O3-SiO2 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.

Key words: Na2O-Al2O3-SiO2, Cluster model, Melt, Molar mixing free energy

MSC2000: 

  • O642