{"title":"Design and Synthesis of Novel Dual-Functional Protic Ionic Liquids with a Superior High CO<sub>2</sub> Absorption Efficiency.","authors":"Jing Ma, Yaxuan Du, Meizhe Liu, Yamei Zhou, Xiejun Wang, Baohe Wang, Jing Zhu, Mingxuan Zhu","doi":"10.1021/acs.jpcb.4c06299","DOIUrl":null,"url":null,"abstract":"<p><p>As a predictive tool, quantum chemical calculations can be used to design protic ionic liquids (PILs) and predict the result. By adding anionic negative potential sites, two dual-functional PILs diethylenetriamine-barbituric acid [C<sub>4</sub>H<sub>14</sub>N<sub>3</sub>]<sub>2</sub>[C<sub>4</sub>H<sub>2</sub>N<sub>2</sub>O<sub>3</sub>] and diethylenetriamine-ethylenolactonium [C<sub>4</sub>H<sub>14</sub>N<sub>3</sub>]<sub>2</sub>[C<sub>3</sub>H<sub>2</sub>N<sub>2</sub>O<sub>2</sub>] were designed. The simulation results indicated that multisite absorption of anions and cations resulted in an expected absorption ratio exceeding 3:1 (mol CO<sub>2</sub>:mol ILs). Furthermore, the Gibbs free energy and enthalpy barrier were calculated. Based on this, the two PILs were synthesized in a controlled manner, and the experimental results demonstrated that 0.25 mol/L [C<sub>4</sub>H<sub>14</sub>N<sub>3</sub>]<sub>2</sub>[C<sub>4</sub>H<sub>2</sub>N<sub>2</sub>O<sub>3</sub>] and [C<sub>4</sub>H<sub>14</sub>N<sub>3</sub>]<sub>2</sub>[C<sub>3</sub>H<sub>2</sub>N<sub>2</sub>O<sub>2</sub>] exhibited a superior CO<sub>2</sub> absorption capacity of 3.152 and 3.466 mol CO<sub>2</sub>/mol ILs, respectively. After five adsorption-desorption experiments, the regeneration rates of [C<sub>4</sub>H<sub>14</sub>N<sub>3</sub>]<sub>2</sub>[C<sub>3</sub>H<sub>2</sub>N<sub>2</sub>O<sub>2</sub>] were all higher than 90%. Finally, the reaction mechanism for CO<sub>2</sub> capture in these PILs was revealed that the significant increase in capacity could be attributed to the combined absorption of double negative potential N atoms on anions and primary and secondary amines on cations by using <sup>13</sup>C NMR.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.8000,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry B","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpcb.4c06299","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
As a predictive tool, quantum chemical calculations can be used to design protic ionic liquids (PILs) and predict the result. By adding anionic negative potential sites, two dual-functional PILs diethylenetriamine-barbituric acid [C4H14N3]2[C4H2N2O3] and diethylenetriamine-ethylenolactonium [C4H14N3]2[C3H2N2O2] were designed. The simulation results indicated that multisite absorption of anions and cations resulted in an expected absorption ratio exceeding 3:1 (mol CO2:mol ILs). Furthermore, the Gibbs free energy and enthalpy barrier were calculated. Based on this, the two PILs were synthesized in a controlled manner, and the experimental results demonstrated that 0.25 mol/L [C4H14N3]2[C4H2N2O3] and [C4H14N3]2[C3H2N2O2] exhibited a superior CO2 absorption capacity of 3.152 and 3.466 mol CO2/mol ILs, respectively. After five adsorption-desorption experiments, the regeneration rates of [C4H14N3]2[C3H2N2O2] were all higher than 90%. Finally, the reaction mechanism for CO2 capture in these PILs was revealed that the significant increase in capacity could be attributed to the combined absorption of double negative potential N atoms on anions and primary and secondary amines on cations by using 13C NMR.
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An essential criterion for acceptance of research articles in the journal is that they provide new physical insight. Please refer to the New Physical Insights virtual issue on what constitutes new physical insight. Manuscripts that are essentially reporting data or applications of data are, in general, not suitable for publication in JPC B.
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