Heli Tian , Kunjie Li , Ruihong Zhao , Jiangze Han , Jingsi Yang , Zhengjie Li
{"title":"利用分子极性指数筛选和评估相变吸附剂:实验和量子化学计算研究","authors":"Heli Tian , Kunjie Li , Ruihong Zhao , Jiangze Han , Jingsi Yang , Zhengjie Li","doi":"10.1016/j.seppur.2024.130318","DOIUrl":null,"url":null,"abstract":"<div><div>Phase change absorbents have recently received increasing attention due to their potential to reduce the energy penalty of CO<sub>2</sub> capture. However, its complex composition makes the prediction of phase separation performance difficult. Phase separation behavior and phase separation rate have been investigated for the amine-aqueous 5.0 M amine blends by experimental and quantum chemical calculations (including MPI, hydrogen bonds and Gibbs free energy). The different phase behaviors upon CO<sub>2</sub> absorption were discussed and well explained by the polarity change of components and the reaction products. A defined MPI value of tertiary amines was recommended to predict the immiscible type (MPI > 10.55 Kcal/mol), phase separation type (9.00 Kcal/mol < MPI < 10.08 Kcal/mol), and miscible type (MPI < 6.74 Kcal/mol). The electron density at the critical point of hydrogen bonds and interaction region indicators were employed to visually evaluate the influence of intramolecular and intermolecular hydrogen bonds on phase separation behaviors. The results show that the presence of excessive hydrogen bonds decreased the phase separation capacity. Furthermore, the relationship between the MPI, the Gibbs free energy of the proton transfer process and the phase separation time were explored. The increase of MPI caused by the tertiary amines can enhance the stability of the final product, delay the appearance of the phase separation peak and reach a maximum phase separation time of 230 min. Therefore, this study is significant for the screening and evaluation of efficient phase change absorbents with good potential for industrial applications in CO<sub>2</sub> capture.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"358 ","pages":"Article 130318"},"PeriodicalIF":8.1000,"publicationDate":"2024-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Screening and evaluation of phase change absorbents by molecular polarity index: Experimental and quantum chemical calculation studies\",\"authors\":\"Heli Tian , Kunjie Li , Ruihong Zhao , Jiangze Han , Jingsi Yang , Zhengjie Li\",\"doi\":\"10.1016/j.seppur.2024.130318\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Phase change absorbents have recently received increasing attention due to their potential to reduce the energy penalty of CO<sub>2</sub> capture. However, its complex composition makes the prediction of phase separation performance difficult. Phase separation behavior and phase separation rate have been investigated for the amine-aqueous 5.0 M amine blends by experimental and quantum chemical calculations (including MPI, hydrogen bonds and Gibbs free energy). The different phase behaviors upon CO<sub>2</sub> absorption were discussed and well explained by the polarity change of components and the reaction products. A defined MPI value of tertiary amines was recommended to predict the immiscible type (MPI > 10.55 Kcal/mol), phase separation type (9.00 Kcal/mol < MPI < 10.08 Kcal/mol), and miscible type (MPI < 6.74 Kcal/mol). The electron density at the critical point of hydrogen bonds and interaction region indicators were employed to visually evaluate the influence of intramolecular and intermolecular hydrogen bonds on phase separation behaviors. The results show that the presence of excessive hydrogen bonds decreased the phase separation capacity. Furthermore, the relationship between the MPI, the Gibbs free energy of the proton transfer process and the phase separation time were explored. The increase of MPI caused by the tertiary amines can enhance the stability of the final product, delay the appearance of the phase separation peak and reach a maximum phase separation time of 230 min. Therefore, this study is significant for the screening and evaluation of efficient phase change absorbents with good potential for industrial applications in CO<sub>2</sub> capture.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"358 \",\"pages\":\"Article 130318\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-11-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624040577\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624040577","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Screening and evaluation of phase change absorbents by molecular polarity index: Experimental and quantum chemical calculation studies
Phase change absorbents have recently received increasing attention due to their potential to reduce the energy penalty of CO2 capture. However, its complex composition makes the prediction of phase separation performance difficult. Phase separation behavior and phase separation rate have been investigated for the amine-aqueous 5.0 M amine blends by experimental and quantum chemical calculations (including MPI, hydrogen bonds and Gibbs free energy). The different phase behaviors upon CO2 absorption were discussed and well explained by the polarity change of components and the reaction products. A defined MPI value of tertiary amines was recommended to predict the immiscible type (MPI > 10.55 Kcal/mol), phase separation type (9.00 Kcal/mol < MPI < 10.08 Kcal/mol), and miscible type (MPI < 6.74 Kcal/mol). The electron density at the critical point of hydrogen bonds and interaction region indicators were employed to visually evaluate the influence of intramolecular and intermolecular hydrogen bonds on phase separation behaviors. The results show that the presence of excessive hydrogen bonds decreased the phase separation capacity. Furthermore, the relationship between the MPI, the Gibbs free energy of the proton transfer process and the phase separation time were explored. The increase of MPI caused by the tertiary amines can enhance the stability of the final product, delay the appearance of the phase separation peak and reach a maximum phase separation time of 230 min. Therefore, this study is significant for the screening and evaluation of efficient phase change absorbents with good potential for industrial applications in CO2 capture.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.