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Statements

Subject Item
n2:RIV%2F00216208%3A11310%2F12%3A10127259%21RIV13-GA0-11310___
rdf:type
n13:Vysledek skos:Concept
rdfs:seeAlso
http://dx.doi.org/10.1002/ejic.201101335
dcterms:description
The lanthanide (Ln3+) complexes of three cyclen-based ligands containing three methylphosphonate pendant arms were studied, the ligands being 1,4,7,10-tetraazacyclododecane-1,4,7-triyltris(methylphosphonic acid) (H6do3p), 3-[4,7,10-tris(phosphonomethyl)-1,4,7,10-tetraazacyclododec-1-yl]propanoic acid (H7do3p1pr), and 10-(3-hydroxypropyl)-1,4,7,10-tetraazacyclododecane-1,4,7-triyltris(methylphosphonic acid) (H6do3p1ol). The three macrocyclic ligands form complexes of very high thermodynamic stability with all studied Ln3+ ions. Kinetic studies showed that the acid-assisted dissociation of Ce3+ complexes of these ligands is much faster than for the complex of the related ligand H8dotp [1,4,7,10-tetraazacyclododecane-1,4,7,10-tetrayltetrakis(methylphosphonic acid)]. The number of water molecules coordinated to the Eu3+ and Gd3+ complexes was estimated to be < 1 for the do3p1ol ligand but ca. 1 for the other two ligands, as obtained by time-resolved luminescence spectroscopy and by 1H and 17O relaxometric measurements. The NMR spectroscopic data indicate the existence of a considerable contribution from second-sphere water molecules to the relaxivity of all the Gd3+ complexes studied. The 1H and 31P NMR spectra of the Eu3+, Yb3+ and Lu3+ complexes showed that the propionate arm in the [Ln(do3p1pr)]4 complexes and the propanol arm in the [Ln(do3p1ol)]3 complexes are not bound to the Ln3+ ion. The [Ln(do3p)]3 and [Ln(do3p1pr)]4 complexes have a clear preference for the TSAP (twisted square antiprismatic) isomer, while both SAP (square antiprismatic) and TSAP isomers are present in solutions of the [Ln(do3p1ol)]3 complexes. The lanthanide (Ln3+) complexes of three cyclen-based ligands containing three methylphosphonate pendant arms were studied, the ligands being 1,4,7,10-tetraazacyclododecane-1,4,7-triyltris(methylphosphonic acid) (H6do3p), 3-[4,7,10-tris(phosphonomethyl)-1,4,7,10-tetraazacyclododec-1-yl]propanoic acid (H7do3p1pr), and 10-(3-hydroxypropyl)-1,4,7,10-tetraazacyclododecane-1,4,7-triyltris(methylphosphonic acid) (H6do3p1ol). The three macrocyclic ligands form complexes of very high thermodynamic stability with all studied Ln3+ ions. Kinetic studies showed that the acid-assisted dissociation of Ce3+ complexes of these ligands is much faster than for the complex of the related ligand H8dotp [1,4,7,10-tetraazacyclododecane-1,4,7,10-tetrayltetrakis(methylphosphonic acid)]. The number of water molecules coordinated to the Eu3+ and Gd3+ complexes was estimated to be < 1 for the do3p1ol ligand but ca. 1 for the other two ligands, as obtained by time-resolved luminescence spectroscopy and by 1H and 17O relaxometric measurements. The NMR spectroscopic data indicate the existence of a considerable contribution from second-sphere water molecules to the relaxivity of all the Gd3+ complexes studied. The 1H and 31P NMR spectra of the Eu3+, Yb3+ and Lu3+ complexes showed that the propionate arm in the [Ln(do3p1pr)]4 complexes and the propanol arm in the [Ln(do3p1ol)]3 complexes are not bound to the Ln3+ ion. The [Ln(do3p)]3 and [Ln(do3p1pr)]4 complexes have a clear preference for the TSAP (twisted square antiprismatic) isomer, while both SAP (square antiprismatic) and TSAP isomers are present in solutions of the [Ln(do3p1ol)]3 complexes.
dcterms:title
Tris(phosphonomethyl)cyclen Derivatives: Thermodynamic Stability, Kinetics, Solution Structure, and Relaxivity of Ln(3+) Complexes Tris(phosphonomethyl)cyclen Derivatives: Thermodynamic Stability, Kinetics, Solution Structure, and Relaxivity of Ln(3+) Complexes
skos:prefLabel
Tris(phosphonomethyl)cyclen Derivatives: Thermodynamic Stability, Kinetics, Solution Structure, and Relaxivity of Ln(3+) Complexes Tris(phosphonomethyl)cyclen Derivatives: Thermodynamic Stability, Kinetics, Solution Structure, and Relaxivity of Ln(3+) Complexes
skos:notation
RIV/00216208:11310/12:10127259!RIV13-GA0-11310___
n13:predkladatel
n20:orjk%3A11310
n3:aktivita
n4:I n4:S n4:P n4:Z
n3:aktivity
I, P(ED1.1.00/02.0068), P(GAP207/11/1437), P(ME09065), S, Z(MSM0021620857)
n3:cisloPeriodika
15
n3:dodaniDat
n5:2013
n3:domaciTvurceVysledku
n16:3978877
n3:druhVysledku
n10:J
n3:duvernostUdaju
n22:S
n3:entitaPredkladatele
n21:predkladatel
n3:idSjednocenehoVysledku
175212
n3:idVysledku
RIV/00216208:11310/12:10127259
n3:jazykVysledku
n9:eng
n3:klicovaSlova
relaxivity; kinetics; thermodynamics; lanthanide complexes; macrocyclic ligands
n3:klicoveSlovo
n7:thermodynamics n7:relaxivity n7:macrocyclic%20ligands n7:lanthanide%20complexes n7:kinetics
n3:kodStatuVydavatele
GB - Spojené království Velké Británie a Severního Irska
n3:kontrolniKodProRIV
[7592363C3BAD]
n3:nazevZdroje
European Journal of Inorganic Chemistry
n3:obor
n19:CA
n3:pocetDomacichTvurcuVysledku
1
n3:pocetTvurcuVysledku
9
n3:projekt
n17:ME09065 n17:GAP207%2F11%2F1437 n17:ED1.1.00%2F02.0068
n3:rokUplatneniVysledku
n5:2012
n3:svazekPeriodika
neuveden
n3:tvurceVysledku
Delgado, Rita Martins, André F. Hermann, Petr Geraldes, Carlos F. G. C. Lima, Luís M. P. Ševčík, Radek Carvalho, Henrique F. Tóth, Éva Lubal, Přemysl
n3:wos
000303987800009
n3:zamer
n11:MSM0021620857
s:issn
1434-1948
s:numberOfPages
12
n8:doi
10.1002/ejic.201101335
n14:organizacniJednotka
11310