6-(6-methyl-1,2,4,5-tetrazine-3-yl)-2,2′-bipyridine: a N-donor ligand for the separation of lanthanides(III) and actinides(III)
Here, we report the synthesis of the 6-(6-methyl-1,2,4,5-tetrazine-3-yl)-2,2′-bipyridine (MTB) ligand that has been developed for lanthanide/actinide separation. A multimethod study of the complexation of MTB with trivalent actinide and lanthanide ions is presented. Single-crystal X-ray diffraction...
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| Hauptverfasser: | , , , , , , , , , , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
August 19, 2024
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| In: |
Inorganic chemistry
Year: 2024, Jahrgang: 63, Heft: 33, Pages: 15259-15269 |
| ISSN: | 1520-510X |
| DOI: | 10.1021/acs.inorgchem.4c01793 |
| Online-Zugang: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.inorgchem.4c01793
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| Verfasserangaben: | Gerlinde Greif, Fynn S. Sauerwein, Patrik Weßling, Tamara M. Duckworth, Michael Patzschke, Robert Gericke, Thomas Sittel, Juliane März, Andreas Wilden, Giuseppe Modolo, Petra J. Panak, and Peter W. Roesky |
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| 245 | 1 | 0 | |a 6-(6-methyl-1,2,4,5-tetrazine-3-yl)-2,2′-bipyridine |b a N-donor ligand for the separation of lanthanides(III) and actinides(III) |c Gerlinde Greif, Fynn S. Sauerwein, Patrik Weßling, Tamara M. Duckworth, Michael Patzschke, Robert Gericke, Thomas Sittel, Juliane März, Andreas Wilden, Giuseppe Modolo, Petra J. Panak, and Peter W. Roesky |
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| 520 | |a Here, we report the synthesis of the 6-(6-methyl-1,2,4,5-tetrazine-3-yl)-2,2′-bipyridine (MTB) ligand that has been developed for lanthanide/actinide separation. A multimethod study of the complexation of MTB with trivalent actinide and lanthanide ions is presented. Single-crystal X-ray diffraction measurements reveal the formation of [Ce(MTB)2(NO3)3], [Pr(MTB)(NO3)3H2O], and [Ln(MTB)(NO3)3MeCN] (Ln = Nd, Sm, Eu, Gd). In addition, the complexation of Cm(III) with MTB in solution was studied by time-resolved laser fluorescence spectroscopy. The results show the formation of [Cm(MTB)1-3]3+ complexes, which occur in two different isomers. Quantum chemical calculations reveal an energy difference between these isomers of 12 kJ mol-1, clarifying the initial observations made by time-resolved laser fluorescence spectroscopy (TRLFS). Furthermore, quantum theory of atoms in molecules (QTAIM) analysis of the Cm(III) and Ln(III) complexes was performed, indicating a stronger covalent contribution in the Cm-N interaction compared to the respective Ln-N interaction. These findings align well with extraction data showing a preferred extraction of Am and Cm over lanthanides (e.g., max. SFAm/Eu = 8.3) at nitric acid concentrations <0.1 mol L-1 HNO3. | ||
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| 700 | 1 | |a Weßling, Patrik |d 1992- |e VerfasserIn |0 (DE-588)1201055911 |0 (DE-627)1684202809 |4 aut | |
| 700 | 1 | |a Duckworth, Tamara M. |e VerfasserIn |4 aut | |
| 700 | 1 | |a Patzschke, Michael |e VerfasserIn |4 aut | |
| 700 | 1 | |a Gericke, Robert |e VerfasserIn |4 aut | |
| 700 | 1 | |a Sittel, Thomas |e VerfasserIn |4 aut | |
| 700 | 1 | |a März, Juliane |e VerfasserIn |4 aut | |
| 700 | 1 | |a Wilden, Andreas |e VerfasserIn |4 aut | |
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| 700 | 1 | |a Roesky, Peter W. |e VerfasserIn |4 aut | |
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