Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model

doi:10.1016/j.cjche.2023.05.014

中国化学工程学报 ›› 2023, Vol. 64 ›› Issue (12): 250-258.DOI: 10.1016/j.cjche.2023.05.014

• Full Length Article • 上一篇下一篇

Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model

Xiao-Bin Zhang^1,2, A. Rajendran³, Xing-Bao Wang^1,2, Wen-Ying Li^1,2

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
3. Department of Chemistry, Mepco Schlenk Engineering College (Autonomous), Sivakasi 626005, Tamil Nadu, India

收稿日期:2023-03-22 修回日期:2023-05-04 出版日期:2023-12-28 发布日期:2024-02-05
通讯作者: Xing-Bao Wang,E-mail:wangxingbao@tyut.edu.cn;Wen-Ying Li,E-mail:ying@tyut.edu.cn
基金资助:
The authors are very grateful for the financial support from the National Key Research and Development Program of China (2022YFB4101302-01), the National Natural Science Foundation of China (22178243) and the science and technology innovation project of China Shenhua Coal to Liquid and Chemical Company Limited (MZYHG-22-02).

Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model

Xiao-Bin Zhang^1,2, A. Rajendran³, Xing-Bao Wang^1,2, Wen-Ying Li^1,2

1. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China;
2. College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China;
3. Department of Chemistry, Mepco Schlenk Engineering College (Autonomous), Sivakasi 626005, Tamil Nadu, India

Received:2023-03-22 Revised:2023-05-04 Online:2023-12-28 Published:2024-02-05
Contact: Xing-Bao Wang,E-mail:wangxingbao@tyut.edu.cn;Wen-Ying Li,E-mail:ying@tyut.edu.cn
Supported by:
The authors are very grateful for the financial support from the National Key Research and Development Program of China (2022YFB4101302-01), the National Natural Science Foundation of China (22178243) and the science and technology innovation project of China Shenhua Coal to Liquid and Chemical Company Limited (MZYHG-22-02).

摘要/Abstract

摘要： Direct coal liquefaction (DCL) is an important and effective method of converting coal into high-value-added chemicals and fuel oil. In DCL, heating the direct coal liquefaction solvent (DCLS) from low to high temperature and pre-hydrogenation of the DCLS are critical steps. Therefore, studying the dissolution of hydrogen in DCLS under liquefaction conditions gains importance. However, it is difficult to precisely determine hydrogen solubility only by experiments, especially under the actual DCL conditions. To address this issue, we developed a prediction model of hydrogen solubility in a single solvent based on the machine-learning quantitative structure–property relationship (ML-QSPR) methods. The results showed that the squared correlation coefficient R² = 0.92 and root mean square error RMSE = 0.095, indicating the model’s good statistical performance. The external validation of the model also reveals excellent accuracy and predictive ability. Molecular polarization (α) is the main factor affecting the dissolution of hydrogen in DCLS. The hydrogen solubility in acyclic alkanes increases with increasing carbon number. Whereas in polycyclic aromatics, it decreases with increasing ring number, and in hydrogenated aromatics, it increases with hydrogenation degree. This work provides a new reference for the selection and proportioning of DCLS, i.e., a solvent with higher hydrogen solubility can be added to provide active hydrogen for the reaction and thus reduce the hydrogen pressure. Besides, it brings important insight into the theoretical significance and practical value of the DCL.

关键词: Hydrogen solubility, Liquefied solvents, Predictive model, Density generalized function theory, Quantitative structure–property relationship

Abstract: Direct coal liquefaction (DCL) is an important and effective method of converting coal into high-value-added chemicals and fuel oil. In DCL, heating the direct coal liquefaction solvent (DCLS) from low to high temperature and pre-hydrogenation of the DCLS are critical steps. Therefore, studying the dissolution of hydrogen in DCLS under liquefaction conditions gains importance. However, it is difficult to precisely determine hydrogen solubility only by experiments, especially under the actual DCL conditions. To address this issue, we developed a prediction model of hydrogen solubility in a single solvent based on the machine-learning quantitative structure–property relationship (ML-QSPR) methods. The results showed that the squared correlation coefficient R² = 0.92 and root mean square error RMSE = 0.095, indicating the model’s good statistical performance. The external validation of the model also reveals excellent accuracy and predictive ability. Molecular polarization (α) is the main factor affecting the dissolution of hydrogen in DCLS. The hydrogen solubility in acyclic alkanes increases with increasing carbon number. Whereas in polycyclic aromatics, it decreases with increasing ring number, and in hydrogenated aromatics, it increases with hydrogenation degree. This work provides a new reference for the selection and proportioning of DCLS, i.e., a solvent with higher hydrogen solubility can be added to provide active hydrogen for the reaction and thus reduce the hydrogen pressure. Besides, it brings important insight into the theoretical significance and practical value of the DCL.

Key words: Hydrogen solubility, Liquefied solvents, Predictive model, Density generalized function theory, Quantitative structure–property relationship

Xiao-Bin Zhang, A. Rajendran, Xing-Bao Wang, Wen-Ying Li. Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model[J]. 中国化学工程学报, 2023, 64(12): 250-258.

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Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model

Solubility study of hydrogen in direct coal liquefaction solvent based on quantitative structure–property relationships model

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