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A TRLFS study on the complexation of novel BTP type ligands with Cm(III)

Two BTP-type N-donor ligands with different numbers of aromatic nitrogen atoms (2,6-bis(4-ethyl-pyridazin-1-yl)pyridine, Et-BDP and 2,6-bis(4-npropyl-2,3,5,6-tetrazine-1-yl)pyridine, nPr-Tetrazine) have been synthesized and characterized by NMR and MS techniques. The complexation with Cm(III) in 2-p...

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Hauptverfasser: Beele, Björn B. (VerfasserIn) , Rüdiger, Elias (VerfasserIn) , Schwörer, Felicitas (VerfasserIn) , Müllich, Udo (VerfasserIn) , Geist, Andreas (VerfasserIn) , Panak, Petra (VerfasserIn)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: 25 Mar 2013
In: Dalton transactions
Year: 2013, Jahrgang: 42, Heft: 34, Pages: 12139-12147
ISSN:1477-9234
DOI:10.1039/C3DT50536G
Online-Zugang:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1039/C3DT50536G
Verlag, lizenzpflichtig, Volltext: https://pubs.rsc.org/en/content/articlelanding/2013/dt/c3dt50536g
Volltext
Verfasserangaben:Björn B. Beele, Elias Rüdiger, Felicitas Schwörer, Udo Müllich, Andreas Geist and Petra J. Panak

MARC

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520 |a Two BTP-type N-donor ligands with different numbers of aromatic nitrogen atoms (2,6-bis(4-ethyl-pyridazin-1-yl)pyridine, Et-BDP and 2,6-bis(4-npropyl-2,3,5,6-tetrazine-1-yl)pyridine, nPr-Tetrazine) have been synthesized and characterized by NMR and MS techniques. The complexation with Cm(III) in 2-propanol-water (1 : 1, vol.) is studied for both ligands using time resolved laser-induced fluorescence spectroscopy (TRLFS) and the complexation properties are compared to nPr-BTP. With increasing the ligand concentration three different species, the 1 : 1-, 1 : 2- and 1 : 3-complex, were found. Log β3 values of 7.6 for the formation of Cm(Et-BDP)3 and 9.2 for the formation of Cm(nPr-Tetrazine)3 are determined. The complexation with nPr-Tetrazine shows slow kinetics. Thermodynamic data of the complexation reactions are determined in a temperature range of 25 °C-60 °C. The complexation with Et-BDP is exothermic (ΔH = −16.3 ± 1.2 kJ mol−1) and exergonic (ΔG = −43.8 ± 2.6 kJ mol−1) whereas the complexation with nPr-Tetrazine is endothermic (ΔH = 43.9 ± 3.1 kJ mol−1) and exergonic (ΔG = −51.7 ± 2.2 kJ mol−1). In the case of the latter the complexation is driven by a highly positive reaction entropy change (ΔS = 320.6 ± 15.4 J mol−1 K−1). In comparison to nPr-BTP, less negative ΔG values were found for the complexation of Cm(III) with both ligands. 
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