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001-es BibID:	BIBFORM076235
035-os BibID:	(WoS)000436023800023 (Scopus)85048704903
Első szerző:	Le Fur, Mariane
Cím:	Expanding the Family of Pyclen-Based Ligands Bearing Pendant Picolinate Arms for Lanthanide Complexation / Mariane Le Fur, Enikő Molnár, Maryline Beyler, Olivier Fougère, David Esteban-Gómez, Olivier Rousseaux, Raphaël Tripier, Gyula Tircsó, Carlos Platas-Iglesias
Dátum:	2018
ISSN:	0020-1669 1520-510X
Megjegyzések:	We report a detailed characterization of lanthanide complexes with two azaligands based on the pyclen macrocycle containing two picolinate and one acetate pendant arms. The two picolinate arms are attached to either opposite (L3) or adjacent (L4) amine nitrogen atoms of the macrocyclic platform. The X-ray structures of the Yb3+ complexes show nine coordination of the ligand to the metal ion, a situation that is also observed for EuL4 in the solid state. The EuL3 complex forms centrosymmetric dimers in the solid state joined by ?2-?1:?1 carboxylate groups, which results in 10-coordinate Eu3+ ions. The emission spectra of EuL3 measured in H2O and D2O solution reveal the presence of a hydration equilibrium involving a nine-coordinate species lacking inner-sphere water molecules and a monohydrated 10-coordinate species. The Eu3+ complexes present modest emission quantum yields in buffered aqueous solution (? = 16 and 22% for EuL3 and EuL4, 0.1 M tris buffer, pH 7.4), while the corresponding Tb3+ complexes present very high emission quantum yields under the same conditions (?90%). 1H NMR studies show that the complexes of L3 present a fluxional behavior in D2O solution, while those of L4 are more rigid. The analysis of the Yb3+-induced NMR shifts of YbL4 indicates that the complex presents a structure in solution similar to that observed in the solid state. The Gd3+ complexes present very high thermodynamic stability constants (log KGdL = 23.56(2) and 23.44(2) for GdL3 and GdL4, respectively). The corresponding pGd values (pGd = ?log[Gd3+]free with cL = 1 ? 10?5 M and cGd = 1 ? 10?6 at pH 7.4) of 20.69 (GdL3) and 21.83 (GdL4) are higher than that of Gd(dota)? (pGd = 19.21). The Gd3+ complexes also show remarkable inertness with respect to their proton-assisted dissociation, with dissociation half-life times of 50 min (GdL3) and 20 h (GdL4) in 1 M HCl.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban folyóiratcikk Pyclen-Based Ligands Picolinate Lanthanide
Megjelenés:	Inorganic Chemistry. - 57 : 12 (2018), p. 6932-6945. -
További szerzők:	Molnár Enikő (1991-) (vegyész) Beyler, Maryline Fougère, Olivier Esteban-Gómez, David Rousseaux, Olivier Tripier, Raphaël Tircsó Gyula (1977-) (vegyész, kémia tanár) Platas-Iglesias, Carlos
Pályázati támogatás:	OTKA K-120224 OTKA Bolyai János Kutatási Ösztöndíj Egyéb U?NKP-17-3 Egyéb COST Action CA15209 Egyéb GINOP-2.3.2-15-2016-00008 GINOP GINOP-2.3.3-15-2016-00004 GINOP
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