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001-es BibID:BIBFORM103530
035-os BibID:(WOS)000541873600033 (Scopus)85084399701
Első szerző:Garda Zoltán (vegyész)
Cím:Unexpected Trends in the Stability and Dissociation Kinetics of Lanthanide(III) Complexes with Cyclen-Based Ligands across the Lanthanide Series / Zoltán Garda, Viktoria Nagy, Aurora Rodríguez-Rodríguez, Rosa Pujales-Paradela, Véronique Patinec, Goran Angelovski, Éva Tóth, Ferenc K. Kálmán, David Esteban-Gómez, Raphaël Tripier, Carlos Platas-Iglesias, Gyula Tircsó
Dátum:2020
ISSN:0020-1669 1520-510X
Megjegyzések:We report a detailed study of the thermodynamic stability and dissociation kinetics of lanthanide complexes with two ligands containing a cyclen unit, a methyl group, a picolinate arm, and two acetate pendant arms linked to two nitrogen atoms of the macrocycle in either cis (1,4-H(3)DO2APA) or trans (1,7-H(3)DO2APA) positions. The stability constants of the Gd3+ complexes with these two ligands are very similar, with log K-GdL values of 16.98 and 16.33 for the complexes of 1,4-H(3)DO2APA and 1,7-H(3)DO2APA, respectively. The stability constants of complexes with 1,4-H(3)DO2APA follow the usual trend, increasing from log K-LaL = 15.96 to log K-LuL = 19.21. However, the stability of [Ln(1,7-DO2APA)] complexes decreases from log K = 16.33 for Gd3+ to 14.24 for Lu3+. The acid-catalyzed dissociation rates of the Gd3+ complexes differ by a factor of similar to 15, with rate constants (k(1)) of 1.42 and 23.5 M(-1)s(-1) for [Gd(1,4-DO2APA)] and [Gd(1,7DO2APA)], respectively. This difference is magnified across the lanthanide series to reach a 5 orders of magnitude higher k(1) for [Yb(1,7-DO2APA)] (1475 M(-1)s(-1)) than for [Yb(1,4-DO2APA)] (5.79 x 10(-3)M(-1)s(-1)).The acid catalyzed mechanism involves the protonation of a carboxylate group, followed by a cascade of proton-transfer events that result in the protonation of a nitrogen atom of the cyclen unit. Density functional theory calculations suggest a correlation between the strength of the Ln-O-carboxylate bonds and the kinetic inertness of the complex, with stronger bonds providing more inert complexes. The H-1 NMR resonance of the coordinated water molecule in the [Yb(1,7-DO2APA)] complex at 176 ppm provides a sizable chemical exchange saturation transfer effect thanks to a slow water exchange rate of (15.9 +/- 1.6) x 10(3) s(-1).
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
folyóiratcikk
Megjelenés:Inorganic Chemistry. - 59 : 12 (2020), p. 8184-8195. -
További szerzők:Nagy Viktória Rodríguez-Rodríguez, Aurora Pujales-Paradela, Rosa Patinec, Véronique Angelovski, Goran Tóth Éva Kálmán Ferenc K. (1978-) (vegyész) Esteban-Gómez, David Tripier, Raphaël Platas-Iglesias, Carlos Tircsó Gyula (1977-) (vegyész, kémia tanár)
Pályázati támogatás:GINOP-2.3.2-15-2016-00008
GINOP
NKFIH-K-120224
Egyéb
NKFIH-K-128201
Egyéb
2019-2.1.11-TÉT-2019-00084
Egyéb
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2.

001-es BibID:BIBFORM103610
035-os BibID:(cikkazonosító)110978 (WOS)000522119300002 (Scopus)85077754827
Első szerző:Guillou, Amaury
Cím:Picolinate-appended tacn complexes for bimodal imaging: Radiolabeling, relaxivity, photophysical and electrochemical studies / Amaury Guillou, Margau Galland, Amandine Roux, Balázs Váradi, Réka Anna Gogolák, Patricia Le Saëc, Alain Faivre-Chauvet, Maryline Beyler, Christophe Bucher, Gyula Tircsó, Véronique Patinec, Olivier Maury, Raphaël Tripier
Dátum:2020
ISSN:0162-0134 1873-3344
Megjegyzések:Based on our previous works involving two 1,4,7-triazacyclononane (tacn)-based ligands Hno2py1pa (1-Picolinic acid-4,7-bis(pyridin-2-ylmethyl)-1,4,7-triazacyclononane) and Hno1pa (1-Picolinic acid-1,4,7-triazacyclononane), we report here the synthesis of analogues bearing picolinate-based rz-conjugated ILCT (IntraLigand Charge Transfer) transition antenna (HL1, HL2), using regiospecific N-functionalization of the tacn skeleton and their related transition metal complexes (e.g. Cu2+, Zn2+ and Mn2+). Coordination properties as well as their photophysical and electrochemical properties were investigated in order to quantify the impact of such antenna on the luminescent or relaxometric properties of the complexes. The spectroscopic properties of the targeted ligands and metal complexes have been studied using UV-Vis absorption and fluorescence spectrocopies. While the zinc complex formed with HL1 possesses a moderate quantum yield of 5%, complexation of Cu2+ led to an extinction of the luminescence putatively attributed to a photo-induced electron transfer, as supported by spectroscopic and electrochemical evidences. The [Mn(L2)](+) complex is characterized by a fluorescence quantum yield close to 8% in CH2Cl2. The potential interest of such systems as bimodal probes has been assessed from radiolabeling experiments conducted on HL1 and( 64)Cu(2+) as well as confocal microscopy analyses and from relaxometric studies carried out on the cationic [Mn(L2)](+) complex. These results showed that HL1 can be used for radiolabeling, with a radiochemical conversion of 40% in 15 min at 100 degrees C. Finally, the relaxivity values obtained for [Mn(L2)](+), r(1p) = 4.80 mM(-1).s(-1) and r(2p) = 8.72 mM(-1).s(-1), make the Mn(II) complex an ideal candidate as a probe for Magnetic Resonance Imaging.
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
folyóiratcikk
Megjelenés:Journal of Inorganic Biochemistry. - 205 (2020), p. 1-9. -
További szerzők:Galland, Margaux Roux, Amandine Váradi Balázs (1990-) (vegyész) Gogolák Réka Anna (kémia tanár) Le Saëc, Patricia Faivre-Chauvet, Alain Beyler, Maryline Bucher, Christophe Tircsó Gyula (1977-) (vegyész, kémia tanár) Patinec, Véronique Maury, Olivier Tripier, Raphaël
Pályázati támogatás:NKFIH-K-120224
Egyéb
GINOP-2.3.2-15-2016-00008
GINOP
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3.

001-es BibID:BIBFORM113922
035-os BibID:(WoS)001044538800001 (Scopus)85168325256
Első szerző:Marlin, Axia
Cím:H 3 nota Derivatives Possessing Picolyl and Picolinate Pendants for Ga 3+ Coordination and 67 Ga 3+ Radiolabeling / Axia Marlin, Angus Koller,Enikő Madarasi, Marie Cordier, David Esteban-Gómez, Carlos Platas-Iglesias, Gyula Tircsó, Eszter Boros, Véronique Patinec, Raphaël Tripier
Dátum:2023
ISSN:0020-1669 1520-510X
Megjegyzések:We synthesized, thanks to the regiospecific N-functionalization using an orthoamide intermediate, two tacn derivatives containing an acetate arm and either a methylpyridine or picolinic acid group, respectively Hnoapy and H2noapa, as new Ga3+ chelators for potential use in nuclear medicine. The corresponding Ga3+ complexes were synthesized and structurally characterized in solution by 1H and 13C NMR. The [Ga(noapy)]2+complex appears to exist in solution as two diasteroisomeric pairs of enantiomers, as confirmed by theorical DFT calculations, while for [Ga(noapa)]+ a single species is present in solution. Solid state investigations were possible for the [Ga(noapa)]+ complex, that crystallized from water as a pair of enantiomers. The average length of the N-Ga bonds of 2.090 ?A is identical to that found for the [Ga(nota)] complex, showing that the presence of the picolinate arm does not hinder the coordination of the ligand to the metal ion. Protonation constants of noapy- and noapa2 were determined by potentiometric titrations, providing an overall basicity ?log KiH (i = 1-4) that increases following the order noapy- < noapa2 < nota3 , as increases the negative charge of the ligand. Stability constants determined by pH-potentiometric titrations supplemented with 71Ga NMR data show that the stabilities of [Ga(noapy)]2+ and [Ga(noapa)]+ are lower when compared to [Ga(nota)], but higher than those of other standards as [Ga(aazta)]-. 67Ga radiolabeling studies were performed in order to demonstrate the potentiality of these chelators for 67/68Ga-based radiopharmaceuticals. The labeling of Hnoapy and H2noapa was nearly identical while outperforming H3nota. Stability studies were conducted in PBS and in presence of human serum transferrin, revealing no significant decomplexation of [67Ga][Ga(noapy)]2+, [67Ga][Ga(noapa)]+ compared to [67Ga][Ga(nota)]. Finally, all complexes were found to be highly hydrophilic, with calculated logD7.4 values of -3.42 ? 0.05, -3.34 ? 0.04, and -3.00 ? 0.23 for Hnoapy, H2noapa, and H3nota respectively, correlating with the charge of each complexes and the electrostatic potentials obtained with DFT.
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
folyóiratcikk
Ga(III) complexes
tacn derivatives
synthesis
structure
stability
labeling studies
Megjelenés:Inorganic Chemistry. - 62 : 50 (2023), p. 20634-20645. -
További szerzők:Koller, Angus Madarasi Enikő Cordier, Marie Esteban-Gómez, David Platas-Iglesias, Carlos Tircsó Gyula (1977-) (vegyész, kémia tanár) Boros Eszter Patinec, Véronique Tripier, Raphaël
Pályázati támogatás:Ministere de l·Enseignement Superieur et de la Recherche and the Centre National de la Recherche Scientifique
Egyéb
Brittany Region
Egyéb
"Service Commun" of NMR of the University of Brest
Egyéb
FEDER funds from the EU (grant PID2019-104626GB-I00)
Egyéb
Xunta de Galicia (ED431B 2020/52)
Egyéb
Centro de Supercomputación de Galicia (CESGA)
Egyéb
NKFIH K-128201
OTKA
NKFIH K-134694
OTKA
Hungarian-Spanish science and technology cooperation program (2019-2.1.11-TÉT-2019-00084)
Egyéb
Doctoral School of Chemistry at the University of Debrecen, Hungary
Egyéb
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4.

001-es BibID:BIBFORM057618
Első szerző:Molnár Enikő (vegyész)
Cím:Picolinate-Containing Macrocyclic Mn(II) Complexes as Potential MRI Contrast Agents / Enikő Molnar, Nathalie Camus, Veronique Patinec, Gabriele A. Rolla, Mauro Botta, Gyula Tircso, Ferenc K. Kalmán, Tamas Fodor, Raphael Tripier, Carlos Platas-Iglesias
Dátum:2014
ISSN:0020-1669
Megjegyzések:We report the synthesis of the ligand Hnompa (6-((1,4,7-triazacyclononan- 1-yl)methyl)picolinic acid) and a detailed characterization of the Mn2+ complexes formed by this ligand and the related ligands Hdompa (6-((1,4,7,10-tetraazacyclododecan-1- yl)methyl)picolinic acid) and Htempa (6-((1,4,8,11-tetraazacyclotetradecan-1-yl)methyl)- picolinic acid). These ligands form thermodynamically stable complexes in aqueous solution with stability constants of logKMnL = 10.28(1) (nompa), 14.48(1) (dompa), and 12.53(1) (tempa). A detailed study of the dissociation kinetics of these Mn2+ complexes indicates that the decomplexation reaction at about neutral pH occurs mainly following a spontaneous dissociation mechanism. The X-ray structure of [Mn2(nompa)2(H2O)2]- (ClO4)2 shows that the Mn2+ ion is seven-coordinate in the solid state, being directly bound to five donor atoms of the ligand, the oxygen atom of a coordinated water molecule and an oxygen atom of a neighboring nompa- ligand acting as a bridging bidentate carboxylate group (1 -carboxylate). Nuclear magnetic relaxation dispersion (1 H NMRD) profiles and 17O NMR chemical shifts and transverse relaxation rates of aqueous solutions of [Mn(nompa)]+ indicate that the Mn2+ ion is six-coordinate in solution by the pentadentate ligand and one innersphere water molecule. The analysis of the 1 H NMRD and 17O NMR data provides a very high water exchange rate of the innersphere water molecule (kex 298 = 2.8 x 109 s -1 ) and an unusually high value of the 17O hyperfine coupling constant of the coordinated water molecule (AO/ = 73.3 ± 0.6 rad s-1 ). DFT calculations performed on the [Mn(nompa)(H2O)]+ ·2H2O system (TPSSh model) provide a AO/ value in excellent agreement with the one obtained experimentally
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
MRI contrast agents
Mn(II) complexes
equilibrium
Kinetics
Structure
Megjelenés:Inorganic Chemistry. - 53 : 10 (2014), p. 5136-5149. -
További szerzők:Camus, Nathalie Patinec, Véronique Rolla, Gabriele A. Botta, Mauro Tircsó Gyula (1977-) (vegyész, kémia tanár) Kálmán Ferenc K. (1978-) (vegyész) Fodor Tamás (1987-) (vegyész) Tripier, Raphaël Platas-Iglesias, Carlos
Pályázati támogatás:Centro de Supercomputacion de Galicia (CESGA)
Egyéb
K-84291
OTKA
K-109029
OTKA
TÁMOP-4.2.2.A-11/ 1/KONV-2012-0043
TÁMOP
János Bolyai Research Scholarship of the Hungarian Academy of Sciences.
Egyéb
COST TD1004 "Theragnostics Imaging and Therapy: An Action to Develop Novel Nanosized Systems for Imaging-Guided Drug Delivery" Action.
Egyéb
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5.

001-es BibID:BIBFORM067424
035-os BibID:(WoS)000395753000022 (Scopus)85006969224
Első szerző:Rodríguez-Rodríguez, Aurora
Cím:Definition of the labile capping bond effect in lanthanide complexes / Aurora Rodríguez-Rodríguez, Martín Regueiro-Figueroa, David Esteban-Gómez, Teresa Rodríguez-Blas, Véronique Patinec, Raphaël Tripier, Gyula Tircsó, Fabio Carniato, Mauro Botta and Carlos Platas-Iglesias
Dátum:2017
ISSN:0947-6539
Megjegyzések:Two macrocyclic ligands containing a cyclen unit, a methyl group, a picolinate arm, and two acetate pendant arms attached to two nitrogen atoms of the macrocycle either in trans (1,7-H3Medo2?ampa = 2,2·-(7-((6-carboxypyridin-2-yl)methyl)-10-methyl-1,4,7,10-tetraazacyclododecane-1,4-diyl)diacetic acid) or in cis (1,4-H3Medo2?ampa) positions are reported. These ligands provide eight-coordination to the Ln3+ ions, leaving a coordination position available for a water molecule that occupies a capping position in the twisted square antiprismatic polyhedron (1,4-H3Medo2?ampa) or one of the positions of the square antiprism (1,7-H3Medo2?ampa). The charge neutral [Gd(1,7-Medo2?ampa)] complex presents an unprecedentedly low water-exchange rate (kex298=8.8?103?s?1), whereas water exchange in [Gd(1,4-Medo2?ampa)] is three orders of magnitude faster (kex298=6.6?106?s?1). These results showcase the labile capping bond phenomenon: A ligand occupying a capping position is hindered by the environment and thus is intrinsically labile.
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
folyóiratcikk
density functional calculations
gadolinium
magnetic resonance imaging
NMR spectroscopy
water exchange
Megjelenés:Chemistry - a European Journal. - 23 : 5 (2017), p. 1110-1117. -
További szerzők:Regueiro-Figueroa, Martín Esteban-Gómez, David Rodríguez-Blas, Teresa Patinec, Véronique Tripier, Raphaël Tircsó Gyula (1977-) (vegyész, kémia tanár) Carniato, Fabio Botta, Mauro Platas-Iglesias, Carlos
Pályázati támogatás:GINOP-2.3.2-15-2016-00008
GINOP
OTKA-109029
OTKA
OTKA-120224
OTKA
János Bolyai Research Scholarship
MTA
Internet cím:Szerző által megadott URL
DOI
Intézményi repozitóriumban (DEA) tárolt változat
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