Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution

doi:10.1016/j.cjche.2023.10.002

中国化学工程学报 ›› 2024, Vol. 66 ›› Issue (2): 125-135.DOI: 10.1016/j.cjche.2023.10.002

• Full Length Article • 上一篇下一篇

Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution

Hongwei Jin, Yun Teng, Kangkang Li, Zhou Feng, Zhonghao Li, Shiqi Qu, Hongzhi Xia, Huanong Cheng, Yugang Li, Xinshun Tan, Shiqing Zheng

College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China

收稿日期:2023-07-26 修回日期:2023-10-06 出版日期:2024-02-28 发布日期:2024-04-20
通讯作者: Huanong Cheng,E-mail:chn@qust.edu.cn
基金资助:
Financial support from the National Natural Science Foundation of China (21775081) and Shandong Province Natural Science Foundation (ZR2020MB145) is gratefully acknowledged.

Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution

Hongwei Jin, Yun Teng, Kangkang Li, Zhou Feng, Zhonghao Li, Shiqi Qu, Hongzhi Xia, Huanong Cheng, Yugang Li, Xinshun Tan, Shiqing Zheng

College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China

Received:2023-07-26 Revised:2023-10-06 Online:2024-02-28 Published:2024-04-20
Contact: Huanong Cheng,E-mail:chn@qust.edu.cn
Supported by:
Financial support from the National Natural Science Foundation of China (21775081) and Shandong Province Natural Science Foundation (ZR2020MB145) is gratefully acknowledged.

摘要/Abstract

摘要： The solubility of H₂S was measured in solutions of N-butyl-N-methylmorpholine acetate ([Bmmorp][Ac]) containing 20 %–40 % (mass) water at experimental temperatures ranged from 298.15 to 328.15K and pressures up to 320kPa. The total solubility of H₂S increased with higher temperatures, lower pressures, and reduced water content. The reaction equilibrium thermodynamic model was used to correlate the solubility data. The results indicate that the chemical reaction equilibrium constant decrease with increasing water content and temperature, whereas Henryconstant increase with increasing water content and temperature. Compared with other ionic liquids, H₂S exhibits a higher physical absorption enthalpy and a lower chemical absorption enthalpy in [Bmmorp][Ac] aqueous solution. This suggests that [Bmmorp][Ac] has a strong physical affinity for H₂S and low energy requirement for desorption. Quantum chemical methods were used to investigate the molecular mechanism of H₂S absorption in ionic liquids. The interaction energy analysis revealed that the binding of H₂S with the ionic liquid in a 1:2 ratio is more stable. Detailed analyses by the methods of the interaction region indicator and the atoms in molecules were conducted to the interactions between H₂S and the ionic liquid.

关键词: Ionic liquid, Hydrogen sulfide, Model, Solubility, Molecular mechanism

Abstract: The solubility of H₂S was measured in solutions of N-butyl-N-methylmorpholine acetate ([Bmmorp][Ac]) containing 20 %–40 % (mass) water at experimental temperatures ranged from 298.15 to 328.15K and pressures up to 320kPa. The total solubility of H₂S increased with higher temperatures, lower pressures, and reduced water content. The reaction equilibrium thermodynamic model was used to correlate the solubility data. The results indicate that the chemical reaction equilibrium constant decrease with increasing water content and temperature, whereas Henryconstant increase with increasing water content and temperature. Compared with other ionic liquids, H₂S exhibits a higher physical absorption enthalpy and a lower chemical absorption enthalpy in [Bmmorp][Ac] aqueous solution. This suggests that [Bmmorp][Ac] has a strong physical affinity for H₂S and low energy requirement for desorption. Quantum chemical methods were used to investigate the molecular mechanism of H₂S absorption in ionic liquids. The interaction energy analysis revealed that the binding of H₂S with the ionic liquid in a 1:2 ratio is more stable. Detailed analyses by the methods of the interaction region indicator and the atoms in molecules were conducted to the interactions between H₂S and the ionic liquid.

Key words: Ionic liquid, Hydrogen sulfide, Model, Solubility, Molecular mechanism

Hongwei Jin, Yun Teng, Kangkang Li, Zhou Feng, Zhonghao Li, Shiqi Qu, Hongzhi Xia, Huanong Cheng, Yugang Li, Xinshun Tan, Shiqing Zheng. Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution[J]. 中国化学工程学报, 2024, 66(2): 125-135.

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Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution

Absorption characteristics, model, and molecular mechanism of hydrogen sulfide in morpholine acetate aqueous solution

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