Utilize este identificador para referenciar este registo:
https://hdl.handle.net/10316/95710
Campo DC | Valor | Idioma |
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dc.contributor.author | Garda, Zoltán | - |
dc.contributor.author | Kócs, Tamara | - |
dc.contributor.author | Bányai, István | - |
dc.contributor.author | Martins, José A. | - |
dc.contributor.author | Kálmán, Ferenc Krisztián | - |
dc.contributor.author | Tóth, Imre | - |
dc.contributor.author | Geraldes, Carlos F. G. C. | - |
dc.contributor.author | Tircsó, Gyula | - |
dc.date.accessioned | 2021-09-09T10:53:32Z | - |
dc.date.available | 2021-09-09T10:53:32Z | - |
dc.date.issued | 2021-08-16 | - |
dc.identifier.issn | 1420-3049 | pt |
dc.identifier.uri | https://hdl.handle.net/10316/95710 | - |
dc.description.abstract | The thermodynamic, kinetic, and structural properties of Ln3+ complexes with the bifunctional DO3A-ACE4- ligand and its amide derivative DO3A-BACE4- (modelling the case where DO3A-ACE4- ligand binds to vector molecules) have been studied in order to confirm the usefulness of the corresponding Gd3+ complexes as relaxation labels of targeted MRI contrast agents. The stability constants of the Mg2+ and Ca2+ complexes of DO3A-ACE4- and DO3A-BACE4- complexes are lower than for DOTA4- and DO3A3-, while the Zn2+ and Cu2+ complexes have similar and higher stability than for DOTA4- and DO3A3- complexes. The stability constants of the Ln(DO3A-BACE)- complexes increase from Ce3+ to Gd3+ but remain practically constant for the late Ln3+ ions (represented by Yb3+). The stability constants of the Ln(DO3A-ACE)4- and Ln(DO3A-BACE)4- complexes are several orders of magnitude lower than those of the corresponding DOTA4- and DO3A3- complexes. The formation rate of Eu(DO3A-ACE)- is one order of magnitude slower than for Eu(DOTA)-, due to the presence of the protonated amine group, which destabilizes the protonated intermediate complex. This protonated group causes the Ln(DO3A-ACE)- complexes to dissociate several orders of magnitude faster than Ln(DOTA)- and its absence in the Ln(DO3A-BACE)- complexes results in inertness similar to Ln(DOTA)- (as judged by the rate constants of acid assisted dissociation). The 1H NMR spectra of the diamagnetic Y(DO3A-ACE)- and Y(DO3A-BACE)- reflect the slow dynamics at low temperatures of the intramolecular isomerization process between the SA pair of enantiomers, R-Λ(λλλλ) and S-Δ(δδδδ). The conformation of the Cα-substituted pendant arm is different in the two complexes, where the bulky substituent is further away from the macrocyclic ring in Y(DO3A-BACE)- than the amino group in Y(DO3A-ACE)- to minimize steric hindrance. The temperature dependence of the spectra reflects slower ring motions than pendant arms rearrangements in both complexes. Although losing some thermodynamic stability relative to Gd(DOTA)-, Gd(DO3A-BACE)- is still quite inert, indicating the usefulness of the bifunctional DO3A-ACE4- in the design of GBCAs and Ln3+-based tags for protein structural NMR analysis. | pt |
dc.description.sponsorship | Funding text 1 This research was funded by the Hungarian National Research, Development and Innovation Office (Projects NKFIH K-128201, K-134694, and FK-134551). Funding text 2 Funding: This research was funded by the Hungarian National Research, Development and Innovation Office (Projects NKFIH K‐128201, K‐134694, and FK‐134551). | pt |
dc.language.iso | eng | pt |
dc.publisher | MDPI | pt |
dc.rights | openAccess | pt |
dc.rights.uri | http://creativecommons.org/licenses/by/4.0/ | pt |
dc.subject | Bifunctional ligands (BFCs) | pt |
dc.subject | Complexes | pt |
dc.subject | Dynamic NMR | pt |
dc.subject | Equilibrium | pt |
dc.subject | Formation and dissociation kinetics | pt |
dc.title | Complexes of Bifunctional DO3A-N-(α-amino)propinate Ligands with Mg(II), Ca(II), Cu(II), Zn(II), and Lanthanide(III) Ions: Thermodynamic Stability, Formation and Dissociation Kinetics, and Solution Dynamic NMR Studies | pt |
dc.type | article | - |
degois.publication.firstPage | 4956 | pt |
degois.publication.issue | 16 | pt |
degois.publication.title | Molecules | pt |
dc.peerreviewed | yes | pt |
dc.identifier.doi | 10.3390/molecules26164956 | pt |
degois.publication.volume | 26 | pt |
dc.date.embargo | 2021-08-16 | * |
uc.date.periodoEmbargo | 0 | pt |
item.fulltext | Com Texto completo | - |
item.grantfulltext | open | - |
item.languageiso639-1 | en | - |
item.cerifentitytype | Publications | - |
item.openairetype | article | - |
item.openairecristype | http://purl.org/coar/resource_type/c_18cf | - |
crisitem.author.researchunit | CQC - Coimbra Chemistry Centre | - |
crisitem.author.parentresearchunit | Faculty of Sciences and Technology | - |
crisitem.author.orcid | 0000-0002-0837-8329 | - |
Aparece nas coleções: | I&D CIBIT - Artigos em Revistas Internacionais FCTUC Ciências da Vida - Artigos em Revistas Internacionais I&D CQC - Artigos em Revistas Internacionais |
Ficheiros deste registo:
Ficheiro | Descrição | Tamanho | Formato | |
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molecules-26-04956-v2.pdf | 30.73 MB | Adobe PDF | Ver/Abrir |
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