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001-es BibID:BIBFORM106968
035-os BibID:(Wos)000779822100036 (Scopus)85126557192
Első szerző:Lucio-Martínez, Fátima
Cím:Rigidified Derivative of the Non-macrocyclic Ligand H4OCTAPA for Stable Lanthanide(III) Complexation / RFátima Lucio-Martínez, Zoltán Garda, Balázs Váradi, Ferenc Krisztián Kálmán, David Esteban-Gómez, Éva Tóth, Gyula Tircsó, Carlos Platas-Iglesias
Dátum:2022
ISSN:0020-1669 1520-510X
Megjegyzések:he stability constants of lanthanide complexes with the potentially octadentate ligand CHXOCTAPA4?, which contains a rigid 1,2-diaminocyclohexane scaffold functionalized with two acetate and two picolinate pendant arms, reveal the formation of stable complexes [log KLaL = 17.82(1) and log KYbL = 19.65(1)]. Luminescence studies on the Eu3+ and Tb3+ analogues evidenced rather high emission quantum yields of 3.4 and 11%, respectively. The emission lifetimes recorded in H2O and D2O solutions indicate the presence of a water molecule coordinated to the metal ion. 1H nuclear magnetic relaxation dispersion profiles and 17O NMR chemical shift and relaxation measurements point to a rather low water exchange rate of the coordinated water molecule (kex298 = 1.58 ? 106 s?1) and relatively high relaxivities of 5.6 and 4.5 mM?1 s?1 at 20 MHz and 25 and 37 ?C, respectively. Density functional theory calculations and analysis of the paramagnetic shifts induced by Yb3+ indicate that the complexes adopt an unprecedented cis geometry with the two picolinate groups situated on the same side of the coordination sphere. Dissociation kinetics experiments were conducted by investigating the exchange reactions of LuL occurring with Cu2+. The results confirmed the beneficial effect of the rigid cyclohexyl group on the inertness of the Lu3+ complex. Complex dissociation occurs following proton- and metal-assisted pathways. The latter is relatively efficient at neutral pH, thanks to the formation of a heterodinuclear hydroxo complex.
Tárgyszavak:Természettudományok Kémiai tudományok idegen nyelvű folyóiratközlemény külföldi lapban
folyóiratcikk
Megjelenés:Inorganic Chemistry. - 61 : 12 (2022), p. 5157-5171. -
További szerzők:Garda Zoltán (1989-) (vegyész) Váradi Balázs (1990-) (vegyész) Kálmán Ferenc K. (1978-) (vegyész) Esteban-Gómez, David Tóth Éva Tircsó Gyula (1977-) (vegyész, kémia tanár) Platas-Iglesias, Carlos
Pályázati támogatás:K-134694
OTKA
K-128201
OTKA
FK-134551
OTKA
Bilateral Hungarian-Spanish Science and Technology Cooperation Program (2019-2.1.11-TET-2019-00084 supported by NKFIH).
Egyéb
Gedeon Richter's Talentum Foundation
Egyéb
Cooperative Doctoral Program of the Ministry of Innovation and Technology financed from the National Research, Development and Innovation Fund (NKFIH)
Egyéb
ÚNKP-21-4 new national excellence program of the Ministry of Human Capacities
Egyéb
János Bolyai Research Scholarship of the Hungarian Academy of Sciences
MTA
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