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Statements

Subject Item
n2:RIV%2F00216208%3A11310%2F12%3A10119144%21RIV13-GA0-11310___
rdf:type
skos:Concept n17:Vysledek
rdfs:seeAlso
http://dx.doi.org/10.1021/ic202103v
dcterms:description
Three phosphinic acid 1,4,7-triazacyclononane (TACN) derivatives bearing methylphosphinic (TRAP-H), methyl(phenyl)phosphinic (TRAP-Ph), or methyl-(hydroxymethyl)phosphinic acid (TRAP-OH) pendant arms were investigated as members of a new family of efficient Ga3+ chelators, TRAP ligands (triazacyclononane phosphinic acids). Stepwise protonation constants of ligands and stability constants of their complexes with Ga3+, selected divalent metal, and Ln3+ ions were determined by potentiometry. These ligands exhibit high thermodynamic selectivity for Ga3+ over the other metal ions and a selective complexation of smaller Mg2+ over Ca2+. Stabilities of the Ga3+ complexes are dependent on the basicity of the donor atoms: [Ga(NOTA)] (log KGaL = 29.6) > [Ga(TRAP-OH)] (log KGaL = 23.3) > [Ga(TRAP-H)] (log KGaL = 21.9). The [Ga(TRAP-OH)] complex exhibits unusual reversible rearrangement of the %22in-cage%22 N3O3 complex to the %22out-of-cage%22 O6 complex. The in-cage complex is present in acidic solutions, and at neutral pH, Ga3+ ion binds hydroxide anion, induces deprotonation and coordination of the P-hydroxymethyl group(s), and moves out of the macrocyclic cavity; the hypothesis is supported by a combination of results from potentiometry, multinuclear nuclear magnetic resonance spectrometry, and density functional theory calculations. Isomerism of the phosphinate Ga3+ complexes caused by a combination of the chelate ring conformation, the helicity of coordinated pendant arms, and the chirality of the coordinated phosphinate groups was observed. All Ga3+ complexes are kinetically inert in both acidic and alkaline solutions. Complex formation studies in acidic solutions indicate that Ga3+ complexes of the phosphinate ligands are formed quickly (minutes) and quantitatively even at pH <2. Compared to common Ga3+ chelators (e.g., 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) derivatives), these novel ligands show fast complexation of Ga3+ over a broad pH range. Three phosphinic acid 1,4,7-triazacyclononane (TACN) derivatives bearing methylphosphinic (TRAP-H), methyl(phenyl)phosphinic (TRAP-Ph), or methyl-(hydroxymethyl)phosphinic acid (TRAP-OH) pendant arms were investigated as members of a new family of efficient Ga3+ chelators, TRAP ligands (triazacyclononane phosphinic acids). Stepwise protonation constants of ligands and stability constants of their complexes with Ga3+, selected divalent metal, and Ln3+ ions were determined by potentiometry. These ligands exhibit high thermodynamic selectivity for Ga3+ over the other metal ions and a selective complexation of smaller Mg2+ over Ca2+. Stabilities of the Ga3+ complexes are dependent on the basicity of the donor atoms: [Ga(NOTA)] (log KGaL = 29.6) > [Ga(TRAP-OH)] (log KGaL = 23.3) > [Ga(TRAP-H)] (log KGaL = 21.9). The [Ga(TRAP-OH)] complex exhibits unusual reversible rearrangement of the %22in-cage%22 N3O3 complex to the %22out-of-cage%22 O6 complex. The in-cage complex is present in acidic solutions, and at neutral pH, Ga3+ ion binds hydroxide anion, induces deprotonation and coordination of the P-hydroxymethyl group(s), and moves out of the macrocyclic cavity; the hypothesis is supported by a combination of results from potentiometry, multinuclear nuclear magnetic resonance spectrometry, and density functional theory calculations. Isomerism of the phosphinate Ga3+ complexes caused by a combination of the chelate ring conformation, the helicity of coordinated pendant arms, and the chirality of the coordinated phosphinate groups was observed. All Ga3+ complexes are kinetically inert in both acidic and alkaline solutions. Complex formation studies in acidic solutions indicate that Ga3+ complexes of the phosphinate ligands are formed quickly (minutes) and quantitatively even at pH <2. Compared to common Ga3+ chelators (e.g., 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) derivatives), these novel ligands show fast complexation of Ga3+ over a broad pH range.
dcterms:title
Complexation of Metal Ions with TRAP (1,4,7-Triazacyclononane Phosphinic Acid) Ligands and 1,4,7-Triazacyclononane-1,4,7-triacetic Acid: Phosphinate-Containing Ligands as Unique Chelators for Trivalent Gallium Complexation of Metal Ions with TRAP (1,4,7-Triazacyclononane Phosphinic Acid) Ligands and 1,4,7-Triazacyclononane-1,4,7-triacetic Acid: Phosphinate-Containing Ligands as Unique Chelators for Trivalent Gallium
skos:prefLabel
Complexation of Metal Ions with TRAP (1,4,7-Triazacyclononane Phosphinic Acid) Ligands and 1,4,7-Triazacyclononane-1,4,7-triacetic Acid: Phosphinate-Containing Ligands as Unique Chelators for Trivalent Gallium Complexation of Metal Ions with TRAP (1,4,7-Triazacyclononane Phosphinic Acid) Ligands and 1,4,7-Triazacyclononane-1,4,7-triacetic Acid: Phosphinate-Containing Ligands as Unique Chelators for Trivalent Gallium
skos:notation
RIV/00216208:11310/12:10119144!RIV13-GA0-11310___
n17:predkladatel
n18:orjk%3A11310
n3:aktivita
n16:Z n16:S n16:P n16:I
n3:aktivity
I, P(GA203/09/1056), P(OC 179), S, Z(MSM0021620857)
n3:cisloPeriodika
1
n3:dodaniDat
n15:2013
n3:domaciTvurceVysledku
n13:9695656 n13:5386381 n13:8447241 n13:8270392 n13:3978877
n3:druhVysledku
n22:J
n3:duvernostUdaju
n14:S
n3:entitaPredkladatele
n4:predkladatel
n3:idSjednocenehoVysledku
128199
n3:idVysledku
RIV/00216208:11310/12:10119144
n3:jazykVysledku
n21:eng
n3:klicovaSlova
potentiometry; stability; computational methods; 68-Ga; 1,4,7-triazanonane; macrocycle; phosphinates; gallium complexes
n3:klicoveSlovo
n7:potentiometry n7:4 n7:macrocycle n7:computational%20methods n7:7-triazanonane n7:gallium%20complexes n7:phosphinates n7:1 n7:68-Ga n7:stability
n3:kodStatuVydavatele
US - Spojené státy americké
n3:kontrolniKodProRIV
[DD537FA04598]
n3:nazevZdroje
Inorganic Chemistry
n3:obor
n9:CA
n3:pocetDomacichTvurcuVysledku
5
n3:pocetTvurcuVysledku
7
n3:projekt
n12:OC%20179 n12:GA203%2F09%2F1056
n3:rokUplatneniVysledku
n15:2012
n3:svazekPeriodika
51
n3:tvurceVysledku
Šimeček, Jakub Hermann, Petr Plutnar, Jan Schulz, Martin Havlíčková, Jana Kubíček, Vojtěch Notni, Johannes
n3:wos
000298712000074
n3:zamer
n20:MSM0021620857
s:issn
0020-1669
s:numberOfPages
14
n19:doi
10.1021/ic202103v
n6:organizacniJednotka
11310