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001-es BibID:	BIBFORM118635
035-os BibID:	(WoS)001166508700001
Első szerző:	Nizou, Gwladys
Cím:	Exploring the Limits of Ligand Rigidification in Transition Metal Complexes with Mono-Functionalized Pyclen Derivatives / Gwladys Nizou, Zoltán Garda, Enikő Molnár, David Esteban-Gómez, Mariane Le Fur, Olivier Fougere, Olivier Rousseaux, Carlos Platas-Iglesias, Raphaël Tripier, Gyula Tircsó, Maryline Beyler
Dátum:	2024
ISSN:	0020-1669 1520-510X
Megjegyzések:	We report the synthesis of the new family of side-bridged pyclen ligands. The incorporation of an ethylene bridge between two adjacent nitrogen atoms was reached from the pyclen-oxalate described previously in the scientific literature. Three new side-bridged pyclen macrocycles were obtained: Hsb-3-pc1a, sb-3-pc1py and Hsb-3-pc1pa, with the aim to assess their coordination properties toward Cu2+ and Zn2+ ions. We also prepared their non-reinforced analogues H3-pc1a, 3-pc1py and H3-pc1pa as comparative benchmarks. The two series of ligands were characterized and their coordination properties were investigated in detail. The Zn2+ and Cu2+ complexes with the non-side-bridge series H3-pc1a, 3-pc1py and H3-pc1pa were successfully isolated and their structures were assessed by X-ray diffraction studies. In the case of the side-bridged family, the synthesis of the com-plexes was far more difficult and, in some cases, unsuccessful. The results of our studies demonstrate that this difficulty is related to the extreme stiffening and basicity of such side-bridged pyclens.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban folyóiratcikk Macrocyclic ligands rigidification transition metal complexes N-functionalized pyclen derivatives syntheis stability
Megjelenés:	Inorganic Chemistry. - 63 : 8 (2024), p. 3931-3947. -
További szerzők:	Garda Zoltán (1989-) (vegyész) Molnár Enikő (1991-) (vegyész) Esteban-Gómez, David Le Fur, Mariane Fougère, Olivier Rousseaux, Olivier Platas-Iglesias, Carlos Tripier, Raphaël Tircsó Gyula (1977-) (vegyész, kémia tanár) Beyler, Maryline
Pályázati támogatás:	PD-138064 NKFIH K-128201 NKFIH 134694 NKFIH 2019-2.1.11-TET-2019-00084 Egyéb
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001-es BibID:	BIBFORM067433
Első szerző:	Rodríguez-Rodríguez, Aurora
Cím:	Stable Mn2+, Cu2+ and Ln3+ complexes with cyclen-based ligands functionalized with picolinate pendant arms / Aurora Rodríguez-Rodríguez, Zoltán Garda, Erika Ruscsák, David Esteban-Gómez, Andrés de Blas, Teresa Rodríguez-Blas, Luís M. P. Lima, Maryline Beyler, Raphaël Tripier, Gyula Tircsó, Carlos Platas-Iglesias
Dátum:	2015
ISSN:	1477-9226
Megjegyzések:	In this study we present the results of the equilibrium, dissociation kinetics, DFT and X-ray crystallographic studies performed on the complexes of metal ions of biomedical importance (Mn2+, Cu2+ and Gd3+) formed with octadentate ligands based on a cyclen platform incorporating two picolinate pendant arms (dodpa2? and Medodpa2?). The stability constants of the complexes were accessed by multiple methods (pH-potentiometry, direct and competition UV-vis spectrophotometry and 1H-relaxometry). The stability constants of the complexes formed with dodpa2? and Medodpa2? do not differ significantly (e.g. log K[Mn(dodpa)] = 17.40 vs. log K[Mn(Medodpa)] = 17.46, log K[Cu(dodpa)] = 24.34?25.17 vs. log K[Cu(Medodpa)] = 24.74 and log K[Gd(dodpa)]+ = 17.27 vs. log K[Gd(Medodpa)]+ = 17.59), which indicates that the steric hindrance brought by the methyl groups has no significant effect on the stability of the complexes. The stability constants of the Mn2+ complexes formed with the cyclen dipicolinates were found to be ca. 3 log K units higher than those determined for the complex of the cyclen monopicolinate (dompa?), which indicates that the second picolinate moiety attached to the backbone of the macrocycle is very likely coordinated to the Mn2+ ion. However, the stability of the [Cu(dodpa)] and [Cu(Medodpa)] complexes agrees well with the stability constant of [Cu(dompa)]+, in line with the hexadentate coordination around the metal ion observed in the X-ray structure of [Cu(Medodpa)]. The [Gd(dodpa)]+ and [Gd(Medodpa)]+ complexes display a fairly high kinetic inertness, as the rate constants of acid catalysed dissociation (k1 = 2.5(4) ? 10?3 and 8.3(4) ? 10?4 M?1 s?1 for [Gd(dodpa)]+ and [Gd(Medodpa)]+, respectively) are smaller than the value reported for [Gd(do3a)] (k1 = 2.5 ? 10?2 M?1 s?1). The [Mn(dodpa)] complex was found to be more inert than [Mn(Medodpa)]. The results of the diffusion-ordered NMR spectroscopy (DOSY) and DFT calculations of diamagnetic [La(dodpa)]+ and [Lu(dodpa)]+ complexes indicate the formation of a trinuclear entity of the La complex in aqueous solution.
Tárgyszavak:	Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban cyclen-based ligand transition metal lanthanide picolinate pendant thermodynamic stability kinetic inertness
Megjelenés:	Dalton Transactions 44 (2015), p. 5017-5031. -
További szerzők:	Garda Zoltán (1989-) (vegyész) Ruscsák Erika (1989-) (vegyész) Esteban-Gómez, David Blas, Andrès de Rodríguez-Blas, Teresa Lima, Luís M. P. Beyler, Maryline Tripier, Raphaël Tircsó Gyula (1977-) (vegyész, kémia tanár) Platas-Iglesias, Carlos
Pályázati támogatás:	OTKA-84291 OTKA OTKA-109029 OTKA TÁMOP 4.2.2.A-11/1/KONV-2012-0043 TÁMOP János Bolyai Research Scholarship MTA COST TD1004 " Theragnostics Imaging and Therapy: An Action to Develop Novel Nano-sized Systems for Imaging-Guided Drug Delivery " Egyéb CM1006 European F-Element Network (EUFEN) Actions Egyéb
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