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001-es BibID:	BIBFORM118019
035-os BibID:	(cikkazonosító)e202300784 (WoS)001153927400001 (Scopus)85183623079
Első szerző:	Laine, Sophie
Cím:	Structural, stability and relaxation features of lanthanide-complexes designed for multimodal imaging detection of enzyme activities / Sophie Laine, Rémy Jouclas, Célia S Bonnet, PascalRetailleau, Vincent Steinmetz, Agnès Pallier, Zoltán Garda, Gyula Tircsó, Philippe Durand, Éva Tóth
Dátum:	2024
ISSN:	1434-1948
Megjegyzések:	Lanthanide complexes of DO3A-derivative ligands bearing a pyridine-carbamate (L1) or pyridine-amine (L2) arm have potential interest in the design of enzymatically activated imaging probes. Solid-state X-ray structures for CeL1 and YbL2 both demonstrate twisted square antiprismatic geometry, with the metal ion in a nine- or an eight-coordinate environment, respectively. As assessed by pH-potentiometry, in solution lanthanide ions form more stable complexes with the nonadentate L1 than with the octadentate L2 ligand (logKML = 18.7-21.1 vs. 16.7-18.6, respectively), while stability constants are similar for L1 and L2 chelates of Mg2+, Ca2+, Zn2+ or Cu2+. The kinetic inertness of GdL1 is exceptionally high with an estimated dissociation half-life ~108 h at pH 7.4, while LnL2 (Ln = Ce, Gd, Yb) complexes have 3-4 orders of magnitude faster dissociation, related to the presence of the protonatable, non-coordinating amine function. The water exchange rate determined for the monohydrated GdL2 (kex298 = 1.3x106 s-1) shows a threefold decrease with respect to GdDOTA, as consequence of a reduction in the negative charge and in the steric crowding around the water binding site, both important in dissociatively activated water exchange processes.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban folyóiratcikk Lanthanide complexes macrocyclic ligands structure stability inertness
Megjelenés:	European Journal Of Inorganic Chemistry. - [Epub ahead of print] (2024), p.1-13. -
További szerzők:	Laine, Sophie Jouclas, Rémy Bonnet, Célia S. Retailleau, Pascal Steinmetz, Vincent Pallier, Agnes Garda Zoltán (1989-) (vegyész) Tircsó Gyula (1977-) (vegyész, kémia tanár) Durand, Philippe Tóth Éva (1967-) (koordinációs kémia)
Pályázati támogatás:	PD-138064 OTKA K-128201 OTKA K-134694 OTKA
Internet cím:	Szerző által megadott URL DOI Intézményi repozitóriumban (DEA) tárolt változat
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001-es BibID:	BIBFORM076229
035-os BibID:	(WoS)000434245500055 (Scopus)85047091952
Első szerző:	Laine, Sophie
Cím:	Mn complexes of open-chain ligands with a pyridine backbone: less donor atoms lead to higher kinetic inertness / Sophie Laine, Célia S. Bonnet, Ferenc K. Kálmán, Zoltán Garda, Agnès Pallier, Fabien Caillé, Franck Suzenet, Gyula Tircsó, Éva Tóth
Dátum:	2018
ISSN:	1144-0546 1369-9261
Megjegyzések:	The kinetic inertness of Mn2+ complexes is an important parameter for the in vivo safety of potential MRI contrast agents. Rigidifying the ligand structure typically leads to reinforced kinetic inertness. In this context, we studied the Mn2+ complexes of three linear poly(amino carboxylate) ligands containing a pyridine moiety in their skeleton and bearing four (L1, L2) or three carboxylates (L3). The thermodynamic stability constants of the complexes formed with Mn2+, Ca2+, Mg2+, Zn2+ and Cu2+ have been determined using pH-potentiometry, 1H relaxometry and UV/Vis spectrophotometry and are close to those of the EDTA analogues. In contrast, and despite the presence of the pyridine in the ligand backbone, the dissociation rates of the complexes are several orders of magnitude higher than that of [Mn(EDTA)]2?, resulting from a very efficient dissociation pathway catalyzed by the direct attack of Cu2+ or Cu(OH)+. Due to the fewer carboxylate functions, ligand L3 is less favorable for metal-assisted dissociation and provides higher kinetic inertness for its Mn2+ chelate than the L1 and L2 analogues. The water exchange of the monohydrated MnL3 complex has been studied in a variable temperature 17O NMR study. The exchange rate is very high, k298ex = 2.8 ? 109 s?1, which is among the highest values reported for a Mn2+ complex. The NMRD profiles are typical of small molecular weight Mn2+ chelates (r1p = 2.44 mM?1 s?1 at 25 ?C and 20 MHz).
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban folyóiratcikk
Megjelenés:	New Journal Of Chemistry. - 42 : 10 (2018), p. 8012-8020. -
További szerzők:	Bonnet, Célia S. Kálmán Ferenc K. (1978-) (vegyész) Garda Zoltán (1989-) (vegyész) Pallier, Agnès Caillé, Fabien Suzenet, Franck Tircsó Gyula (1977-) (vegyész, kémia tanár) Tóth Éva
Pályázati támogatás:	OTKA K-120224 OTKA Bolyai János Kutatási Ösztöndíj Egyéb GINOP-2.3.2-15-2016-00008 GINOP GINOP-2.3.3-15-2016-00004 GINOP COST CA15209 Egyéb
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