Rigidified Derivative of the Non-macrocyclic Ligand H OCTAPA for Stable Lanthanide(III) Complexation

A tétel rövid nézete
dc.contributor.authorLucio-Martínez, Fátima
dc.contributor.authorGarda, Zoltán
dc.contributor.authorVáradi, Balázs
dc.contributor.authorKálmán, Ferenc Krisztián
dc.contributor.authorEsteban-Gómez, David
dc.contributor.authorTóth, Éva
dc.contributor.authorTircsó, Gyula
dc.contributor.authorPlatas-Iglesias, Carlos
dc.contributor.authorLucio-Martínez, Fátima (1900-) (okl. vegyész)
dc.contributor.authorGarda Zoltán (1989-) (vegyész)
dc.contributor.authorVáradi Balázs (1990-) (Okleveles vegyész)
dc.contributor.authorKálmán Ferenc (1978-) (vegyész)
dc.contributor.authorEsteban-Gómez David (1900-) (okl. vegyész)
dc.contributor.authorTóth Éva (1960-) (kémikus)
dc.contributor.authorTircsó Gyula (1977-) (vegyész és kémia tanár)
dc.contributor.authorPlatas-Iglesias Carlos (1900-) (okl. vegyész)
dc.contributor.submitterdepKémiai Intézet -- 724
dc.contributor.submitterdepFizikai Kémiai Tanszék -- 726
dc.contributor.submitterdepTTK
dc.contributor.submitterdepCentro de Investigacións Científicas Avanzadas (CICA) and Departamento de Química, Facultade de Ciencias, Universidade da Coruña
dc.contributor.submitterdepDebreceni Egyetem
dc.contributor.submitterdepCentre de Biophysique Moléculaire, CNRS UPR 4301, Université d’Orléans
dc.date.accessioned2023-01-19T07:42:36Z
dc.date.available2023-01-19T07:42:36Z
dc.date.oa2024-03-21
dc.date.updated2023-01-19T07:42:36Z
dc.description.abstractThe 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 (kex 298 = 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 protonand metal-assisted pathways. The latter is relatively efficient at neutral pH, thanks to the formation of a heterodinuclear hydroxo complex.
dc.description.correctorLB
dc.identifier.citationInorganic Chemistry. -61 : 12 (2022), p. 5157-5171. -Inorg. Chem. -0020-1669. -1520-510X
dc.identifier.doi10.1021/acs.inorgchem.2c00501
dc.identifier.issn0020-1669. -
dc.identifier.issn1520-510X
dc.identifier.opachttps://ebib.lib.unideb.hu/ebib/CorvinaWeb?action=cclfind&resultview=long&ccltext=idno+BIBFORM106973
dc.identifier.urihttps://hdl.handle.net/2437/343982
dc.identifier.urlhttps://pubs.acs.org/doi/10.1021/acs.inorgchem.2c00501
dc.languageeng
dc.rights.accessopen access article
dc.subject.otheridegen nyelvű folyóiratközlemény külföldi lapban
dc.tenderK-128201 -- OTKA
dc.tenderK-134694 -- OTKA
dc.tenderFK-134551 -- OTKA
dc.tenderNKFIH -- Egyéb
dc.tender2019- 2.1.11-TET-2019-00084 -- Egyéb
dc.tenderÚNKP-21-4 -- Egyéb
dc.tenderJános Bolyai Research Scholarship of the Hungarian Academy of Sciences -- Egyéb
dc.titleRigidified Derivative of the Non-macrocyclic Ligand H OCTAPA for Stable Lanthanide(III) Complexation
Fájlok
Eredeti köteg (ORIGINAL bundle)
Megjelenítve 1 - 1 (Összesen 1)
Nincs kép
Név:
lucio-martínez-et-al-2022-rigidified-derivative-of-the-non-macrocyclic-ligand-h4octapa-for-stable-lanthanide(iii).pdf
Méret:
2.24 MB
Formátum:
Adobe Portable Document Format
Leírás:
Kiadói változat
Letöltés
Gyűjtemények
Publikációs Adatbázis