Synthetic, structural and solution speciation studies on binary Al(III)-(carboxy)phosphonate systems. Relevance to the neurotoxic potential of Al(III)

V. Georgantas, N. Kotsakis, C. P. Raptopoulou, A. Terzis, L. Iordanidis, M. Zervou, T. Jakusch, T. Kiss, A. Salifoglou

Research output: Contribution to journalArticle

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Abstract

Efforts to delineate the interactions of neurotoxic Al(III) with low molecular mass substrates relevant to neurodegenerative processes, led to the investigation of the pH-specific synthetic chemistry of the binary Al(III)-[N-(phosphonomethyl) iminodiacetic acid] (Al-NTAP), Al(III)-[nitrilo-tris(methylene-phosphonic acid)] (Al-NTA3P), and Al(III)-[1-hydroxy ethylidene-1,1-diphosphonic acid] (Al-HEDP) systems, in correlation with solution speciation studies. Reaction of Al(NO3)3·9H2O with NTAP at pH 7.0 and 4.0 afforded the new species (CH6N3)4[Al2(C5H 6NPO7)2(OH)2]·8H 2O (1) and (NH4)2[Al2(C5H6NP O7)2(H2O)2]·4H 2O (2), while reaction of Al(NO3)3·9H2O with NTA3P led to K8[Al2(C3H6NP3O 9)2(OH)2]·20H2O (3). Complexes 1-3 were characterized by elemental analysis, FT-IR, 13C, 31P, 1H NMR (for 1-2 solid state and solution NMR where feasible), and X-ray crystallography. The structures of 1-3 reveal the presence of uniquely defined dinuclear complexes of octahedral Al(III) bound to fully deprotonated phosphonate ligands, water and hydroxo moieties. The aqueous solution speciation studies on the aforementioned binary systems project a clear picture of the binary Al(III)-(carboxy)phosphonate interactions and species under variable pH-conditions and specific Al(III):ligand stoichiometry. The concurrent solid state and solution work (a) exemplifies essential structural and chemical attributes of soluble aqueous species, reflecting well-defined interactions of Al(III) with phosphosubstrates and (b) strengthens the potential linkage of neurotoxic Al(III) chemical reactivity toward O,N-containing (carboxy)phosphate-rich cellular targets.

Original languageEnglish
Pages (from-to)1530-1541
Number of pages12
JournalJournal of Inorganic Biochemistry
Volume103
Issue number11
DOIs
Publication statusPublished - Nov 2009

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Organophosphonates
Nuclear magnetic resonance
Ligands
Chemical reactivity
X ray crystallography
X Ray Crystallography
Molecular mass
Stoichiometry
Acids
Water
Substrates
Chemical analysis

Keywords

  • Aqueous structural speciation
  • Binary aluminum-(carboxy)phosphonate interactions
  • Neurotoxic aluminum
  • Solid state-solution property correlation
  • X-ray crystal structure

ASJC Scopus subject areas

  • Biochemistry
  • Inorganic Chemistry

Cite this

Synthetic, structural and solution speciation studies on binary Al(III)-(carboxy)phosphonate systems. Relevance to the neurotoxic potential of Al(III). / Georgantas, V.; Kotsakis, N.; Raptopoulou, C. P.; Terzis, A.; Iordanidis, L.; Zervou, M.; Jakusch, T.; Kiss, T.; Salifoglou, A.

In: Journal of Inorganic Biochemistry, Vol. 103, No. 11, 11.2009, p. 1530-1541.

Research output: Contribution to journalArticle

Georgantas, V. ; Kotsakis, N. ; Raptopoulou, C. P. ; Terzis, A. ; Iordanidis, L. ; Zervou, M. ; Jakusch, T. ; Kiss, T. ; Salifoglou, A. / Synthetic, structural and solution speciation studies on binary Al(III)-(carboxy)phosphonate systems. Relevance to the neurotoxic potential of Al(III). In: Journal of Inorganic Biochemistry. 2009 ; Vol. 103, No. 11. pp. 1530-1541.
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AU - Raptopoulou, C. P.

AU - Terzis, A.

AU - Iordanidis, L.

AU - Zervou, M.

AU - Jakusch, T.

AU - Kiss, T.

AU - Salifoglou, A.

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N2 - Efforts to delineate the interactions of neurotoxic Al(III) with low molecular mass substrates relevant to neurodegenerative processes, led to the investigation of the pH-specific synthetic chemistry of the binary Al(III)-[N-(phosphonomethyl) iminodiacetic acid] (Al-NTAP), Al(III)-[nitrilo-tris(methylene-phosphonic acid)] (Al-NTA3P), and Al(III)-[1-hydroxy ethylidene-1,1-diphosphonic acid] (Al-HEDP) systems, in correlation with solution speciation studies. Reaction of Al(NO3)3·9H2O with NTAP at pH 7.0 and 4.0 afforded the new species (CH6N3)4[Al2(C5H 6NPO7)2(OH)2]·8H 2O (1) and (NH4)2[Al2(C5H6NP O7)2(H2O)2]·4H 2O (2), while reaction of Al(NO3)3·9H2O with NTA3P led to K8[Al2(C3H6NP3O 9)2(OH)2]·20H2O (3). Complexes 1-3 were characterized by elemental analysis, FT-IR, 13C, 31P, 1H NMR (for 1-2 solid state and solution NMR where feasible), and X-ray crystallography. The structures of 1-3 reveal the presence of uniquely defined dinuclear complexes of octahedral Al(III) bound to fully deprotonated phosphonate ligands, water and hydroxo moieties. The aqueous solution speciation studies on the aforementioned binary systems project a clear picture of the binary Al(III)-(carboxy)phosphonate interactions and species under variable pH-conditions and specific Al(III):ligand stoichiometry. The concurrent solid state and solution work (a) exemplifies essential structural and chemical attributes of soluble aqueous species, reflecting well-defined interactions of Al(III) with phosphosubstrates and (b) strengthens the potential linkage of neurotoxic Al(III) chemical reactivity toward O,N-containing (carboxy)phosphate-rich cellular targets.

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