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Developing the family of picolinate ligands for Mn2+ complexation

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EstebanGomez_David_2017_Developing_family_picolinate_ligands_Mn2+_complexation.pdf (1.359Mb)
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http://hdl.handle.net/2183/19672
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  • Investigación (FCIE) [1259]
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Título
Developing the family of picolinate ligands for Mn2+ complexation
Autor(es)
Forgács, Attila
Pujales-Paradela, Rosa
Regueiro-Figueroa, Martín
Valencia, Laura
Esteban-Gómez, David
Botta, Mauro
Platas-Iglesias, Carlos
Data
2016-12-22
Cita bibliográfica
Developing the family of picolinate ligands for Mn2+ complexation. A. Forgács, R. Pujales-Paradela, M. Regueiro-Figueroa, L. Valencia, D. Esteban-Gómez, M. Botta and C. Platas-Iglesias, Dalt. Trans., 2017, 46, 1546–1558.
Resumo
[Abstract] We have reported here a series of ligands containing pentadentate 6,6′-(azanediylbis(methylene))dipicolinic acid units that differ in the substituent present at the amine nitrogen atom (acetate: H3DPAAA; phenyl: H2DPAPhA; dodecyl: H2DPAC12A; 4-hexylphenyl: H2DPAC6PhA). The protonation constants of the hexadentate DPAAA3− and pentadentate DPAPhA2−ligands and the stability constants of their Mn2+ complexes were determined using pH-potentiometry (25 °C, 0.15 M NaCl). The mono-hydrated [Mn(DPAAA)]− complex (logKMnL = 13.19(5)) was found to be considerably more stable than the bis-hydrated [Mn(DPAPhA)] analogue (logKMnL = 9.55(1)). A detailed 1H and 17O NMR relaxometric study was carried out to determine the parameters that govern the proton relaxivities of these complexes. The [Mn(DPAC12A)] complex, which contains a dodecyl lipophilic chain, forms micelles in solution characterized by a critical micellar concentration (cmc) of 96(9) μM. The lipophilic [Mn(DPAC6PhA)] and [Mn(DPAC12A)] derivatives form rather strong adducts with Human Serum Albumin (HSA) with association constants of 7.1 ± 0.1 × 103 and 1.3 ± 0.4 × 105 M−1, respectively. The X-ray structure of the complex {K(H2O)4}{[Mn(DPAAA)(H2O)]}2 shows that the Mn2+ ion in [Mn(DPAAA)]− is coordinated to the six donor atoms of the ligand, a coordinated water molecule completing the pentagonal bipyramidal coordination environment.
Palabras chave
Magnetic resonance imaging
Manganese complexes
Picolinate ligands
Relaxivity
DFT calculations
 
Versión do editor
https://doi.org/10.1039/C6DT04442E
ISSN
1477-9226
1477-9234
 

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