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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. (en)
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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 (en)
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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 (en)
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skos:notation
| - RIV/00216208:11310/12:10119144!RIV13-GA0-11310___
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http://linked.open...avai/riv/aktivita
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http://linked.open...avai/riv/aktivity
| - I, P(GA203/09/1056), P(OC 179), S, Z(MSM0021620857)
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http://linked.open...iv/cisloPeriodika
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http://linked.open...vai/riv/dodaniDat
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http://linked.open...aciTvurceVysledku
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http://linked.open.../riv/druhVysledku
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http://linked.open...iv/duvernostUdaju
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http://linked.open...titaPredkladatele
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http://linked.open...dnocenehoVysledku
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http://linked.open...ai/riv/idVysledku
| - RIV/00216208:11310/12:10119144
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http://linked.open...riv/jazykVysledku
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http://linked.open.../riv/klicovaSlova
| - potentiometry; stability; computational methods; 68-Ga; 1,4,7-triazanonane; macrocycle; phosphinates; gallium complexes (en)
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http://linked.open.../riv/klicoveSlovo
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http://linked.open...odStatuVydavatele
| - US - Spojené státy americké
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http://linked.open...ontrolniKodProRIV
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http://linked.open...i/riv/nazevZdroje
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http://linked.open...in/vavai/riv/obor
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http://linked.open...ichTvurcuVysledku
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http://linked.open...cetTvurcuVysledku
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http://linked.open...vavai/riv/projekt
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http://linked.open...UplatneniVysledku
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http://linked.open...v/svazekPeriodika
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http://linked.open...iv/tvurceVysledku
| - Hermann, Petr
- Kubíček, Vojtěch
- Plutnar, Jan
- Havlíčková, Jana
- Notni, Johannes
- Šimeček, Jakub
- Schulz, Martin
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http://linked.open...ain/vavai/riv/wos
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http://linked.open...n/vavai/riv/zamer
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issn
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number of pages
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http://bibframe.org/vocab/doi
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http://localhost/t...ganizacniJednotka
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