Complexation and extraction of trivalent actinides over lanthanides using highly soluble phenanthroline diamide ligands with different side chains
Although phenanthroline diamide ligands have been widely reported, their limited solubility in organic solvents and poor performance in the separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) at high acidity are still clear demerits. In this study, we designed and synthesized three...
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| Published in | Journal of hazardous materials Vol. 465; p. 133508 |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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Netherlands
Elsevier B.V
05.03.2024
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| Abstract | Although phenanthroline diamide ligands have been widely reported, their limited solubility in organic solvents and poor performance in the separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) at high acidity are still clear demerits. In this study, we designed and synthesized three highly soluble phenanthroline diamide ligands with different side chains. By introducing alkyl chains and ester groups, the ligands solubility in 3-nitrotrifluorotoluene is increased to over 600 mmol/L, significantly higher than the previous reported phenanthroline diamide ligands. Based on anomalous aryl strengthening, benzene ring was incorporated to enhance ligand selectivity toward Am(III). Extraction experiments demonstrated favorable selectivity of all the three ligands towards Am(III). The optimal separation factor (SFAm/Eu) reaches 53 at 4 mol/L HNO3, representing one of the most effective separation of An(III) over Ln(III) under high acidity. Slope analysis, single crystal structure analysis, as well as titration of ultraviolet visible spectroscopy, mass spectrometry, and nuclear magnetic resonanc confirmed the formation of 1:1 and 1:2 complex species between the metal ions and the ligands depending on the molar ratio of metal ions in the reaction mixture. The findings of this study offer valuable insights for developing phenanthroline diamide ligands for An(III)/Ln(III) separation.
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•The multi-modified phenanthroline diamide ligands were synthesized for An(III)/Ln(III) separation.•The solubility of ligands was clearly improved by introducing alkyl and ester groups.•Benzene ring was incorporated to enhance ligand selectivity toward Am(III) under high acidity.•The ligands achieve one of the most effective separation of An(III) over Ln(III) at 4 mol/L HNO3. |
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| AbstractList | Although phenanthroline diamide ligands have been widely reported, their limited solubility in organic solvents and poor performance in the separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) at high acidity are still clear demerits. In this study, we designed and synthesized three highly soluble phenanthroline diamide ligands with different side chains. By introducing alkyl chains and ester groups, the ligands solubility in 3-nitrotrifluorotoluene is increased to over 600 mmol/L, significantly higher than the previous reported phenanthroline diamide ligands. Based on anomalous aryl strengthening, benzene ring was incorporated to enhance ligand selectivity toward Am(III). Extraction experiments demonstrated favorable selectivity of all the three ligands towards Am(III). The optimal separation factor (SFAm/Eu) reaches 53 at 4 mol/L HNO3, representing one of the most effective separation of An(III) over Ln(III) under high acidity. Slope analysis, single crystal structure analysis, as well as titration of ultraviolet visible spectroscopy, mass spectrometry, and nuclear magnetic resonanc confirmed the formation of 1:1 and 1:2 complex species between the metal ions and the ligands depending on the molar ratio of metal ions in the reaction mixture. The findings of this study offer valuable insights for developing phenanthroline diamide ligands for An(III)/Ln(III) separation.
[Display omitted]
•The multi-modified phenanthroline diamide ligands were synthesized for An(III)/Ln(III) separation.•The solubility of ligands was clearly improved by introducing alkyl and ester groups.•Benzene ring was incorporated to enhance ligand selectivity toward Am(III) under high acidity.•The ligands achieve one of the most effective separation of An(III) over Ln(III) at 4 mol/L HNO3. Although phenanthroline diamide ligands have been widely reported, their limited solubility in organic solvents and poor performance in the separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) at high acidity are still clear demerits. In this study, we designed and synthesized three highly soluble phenanthroline diamide ligands with different side chains. By introducing alkyl chains and ester groups, the ligands solubility in 3-nitrotrifluorotoluene is increased to over 600 mmol/L, significantly higher than the previous reported phenanthroline diamide ligands. Based on anomalous aryl strengthening, benzene ring was incorporated to enhance ligand selectivity toward Am(III). Extraction experiments demonstrated favorable selectivity of all the three ligands towards Am(III). The optimal separation factor (SFAm/Eu) reaches 53 at 4 mol/L HNO3, representing one of the most effective separation of An(III) over Ln(III) under high acidity. Slope analysis, single crystal structure analysis, as well as titration of ultraviolet visible spectroscopy, mass spectrometry, and nuclear magnetic resonanc confirmed the formation of 1:1 and 1:2 complex species between the metal ions and the ligands depending on the molar ratio of metal ions in the reaction mixture. The findings of this study offer valuable insights for developing phenanthroline diamide ligands for An(III)/Ln(III) separation. Although phenanthroline diamide ligands have been widely reported, their limited solubility in organic solvents and poor performance in the separation of trivalent actinides (An(III)) and lanthanides (Ln(III)) at high acidity are still clear demerits. In this study, we designed and synthesized three highly soluble phenanthroline diamide ligands with different side chains. By introducing alkyl chains and ester groups, the ligands solubility in 3-nitrotrifluorotoluene is increased to over 600 mmol/L, significantly higher than the previous reported phenanthroline diamide ligands. Based on anomalous aryl strengthening, benzene ring was incorporated to enhance ligand selectivity toward Am(III). Extraction experiments demonstrated favorable selectivity of all the three ligands towards Am(III). The optimal separation factor (SF ) reaches 53 at 4 mol/L HNO , representing one of the most effective separation of An(III) over Ln(III) under high acidity. Slope analysis, single crystal structure analysis, as well as titration of ultraviolet visible spectroscopy, mass spectrometry, and nuclear magnetic resonanc confirmed the formation of 1:1 and 1:2 complex species between the metal ions and the ligands depending on the molar ratio of metal ions in the reaction mixture. The findings of this study offer valuable insights for developing phenanthroline diamide ligands for An(III)/Ln(III) separation. |
| ArticleNumber | 133508 |
| Author | Ye, Guoan Shehzad, Hamza Liang, Yuanyuan Jiao, Caishan Yuan, Liyong Shi, Weiqun Zhang, Meng Xiu, Taoyuan Liu, Likun Liu, Siyan |
| Author_xml | – sequence: 1 givenname: Taoyuan surname: Xiu fullname: Xiu, Taoyuan organization: College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China – sequence: 2 givenname: Likun surname: Liu fullname: Liu, Likun organization: China Institute of Atomic Energy, Beijing 102413, China – sequence: 3 givenname: Siyan surname: Liu fullname: Liu, Siyan organization: College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China – sequence: 4 givenname: Hamza surname: Shehzad fullname: Shehzad, Hamza organization: School of Chemistry and Materials Science, East China University of Technology, Nanchang 330013, China – sequence: 5 givenname: Yuanyuan surname: Liang fullname: Liang, Yuanyuan organization: Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China – sequence: 6 givenname: Meng surname: Zhang fullname: Zhang, Meng organization: College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China – sequence: 7 givenname: Guoan surname: Ye fullname: Ye, Guoan email: yeguoan@ciae.ac.cn organization: College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China – sequence: 8 givenname: Caishan surname: Jiao fullname: Jiao, Caishan email: jiaocaishan@hrbeu.edu.cn organization: College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China – sequence: 9 givenname: Liyong surname: Yuan fullname: Yuan, Liyong email: yuanly@ihep.ac.cn organization: Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China – sequence: 10 givenname: Weiqun surname: Shi fullname: Shi, Weiqun email: shiwq@ihep.ac.cn organization: Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China |
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| Keywords | Phenanthroline diamide ligand High solubility Americium Solvent extraction Europium |
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| Title | Complexation and extraction of trivalent actinides over lanthanides using highly soluble phenanthroline diamide ligands with different side chains |
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