Thermodynamic modeling with uncertainty quantification using the modified quasichemical model in quadruplet approximation: Implementation into PyCalphad and ESPEI
Thermodynamic modeling with uncertainty quantification using the modified quasichemical model in quadruplet approximation: Implementation into PyCalphad and ESPEI
复制标题
使用四重态近似中改进的准化学模型进行不确定性量化的热力学建模：在 PyCalphad 和 ESPEI 中的实现
DOI：
10.1016/j.calphad.2023.102618
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发表时间：
2023
期刊：
影响因子：
2.4
通讯作者：
Smith, Nathan D.
中科院分区：
文献类型：
--
作者：
Paz Soldan Palma, Jorge;Gong, Rushi;Bocklund, Brandon J.;Otis, Richard;Poschmann, Max;Piro, Markus;Shahbazi, Shayan;Levitskaia, Tatiana G.;Hu, Shenyang;Smith, Nathan D.
四重态近似下的修正准化学模型（MQMQA）考虑了第一和第二近邻的配位和相互作用，特别适用于描述复杂液体如熔盐、金属加工中的炉渣和电解质溶液中的短程有序（SRO）。目前的工作实现MQMQA到基于Python的开源软件PyCalphad的热力学计算。这一奋进促进了基于MQMQA的热力学数据库的开发，并使用开源软件ESPEI进行不确定性量化（UQ）和传播（UP）。提出了一种基于可扩展标记语言（XML）的MQMQA模型参数ESPEI评估数据库结构。我们以KF-NiF 2盐体系为例，通过吉布斯能、平衡四重态分数和相图的热力学计算，以及使用ESPEI使用UQ和UP进行数据库开发，展示了MQMQA在PyCalphad中的成功实施。此外，作为本实施方案的应用，LiFTbF 3和LiF-HoF 3体系都首次被MQMQA建模，这与实验吻合得很好。因此，本实施提供了一个开源的能力，执行复杂的液体与SRO使用MQMQA加上一个新的XML数据库结构的CALPHAD建模。
The modified quasichemical model in the quadruplet approximation (MQMQA) considers the first-and the second-nearest-neighbor coordination and interactions, particularly useful in describing short-range ordering (SRO) in complex liquids such as molten salts, slag in metal processing, and electrolytic solutions. The present work implements the MQMQA into the Python based open-source software PyCalphad for thermodynamic calculations. This endeavor facilitates the development of MQMQA-based thermodynamic database with uncertainty quantification (UQ) and propagation (UP) using the open-source software ESPEI. A new database structure based on Extensible Markup Language (XML) is proposed for ESPEI evaluation of MQMQA model parameters. Using the KF-NiF2 salt systems as examples, we demonstrate the successful implementation of MQMQA in PyCalphad through thermodynamic calculations of Gibbs energy, equilibrium quadruplet fractions, and phase diagram, as well as database development with UQ and UP using ESPEI. Furthermore, as an application of the present implementation, both the LiFTbF3 and LiF-HoF3 systems have been modeled by MQMQA for the first time, which are in good agreement with experiments. The present implementation hence offers an open-source capability for performing CALPHAD modeling for complex liquids with SRO using MQMQA plus a new XML database structure.