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Synthetic, structural and solution speciation studies on binary Al(III)–(carboxy)phosphonate systems. Relevance to the neurotoxic potential of Al(III) |
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| Authors: | V. Georgantas N. Kotsakis C.P. Raptopoulou A. Terzis L. Iordanidis M. Zervou T. Jakusch T. Kiss A. Salifoglou |
| Affiliation: | a Laboratory of Inorganic Chemistry, Department of Chemical Engineering, Aristotle University of Thessaloniki, Thessaloniki 54124, Greece b Department of Chemistry, University of Crete, Heraklion 71409, Greece c Institute of Materials Science, NCSR Demokritos, Aghia Paraskevi, 15310 Attiki, Greece d Department of Chemistry, Michigan State University, East Lansing, MI 48824-1322, USA e Laboratory of Molecular Analysis, Institute of Organic and Pharmaceutical Chemistry, National Hellenic Research Foundation, Athens 11635, Greece f Biocoordination Chemistry Research Group of the Hungarian Academy of Sciences, Department of Inorganic and Analytical Chemistry, University of Szeged, Szeged H-6720, Hungary |
| 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(C5H6NPO7)2(OH)2]·8H2O (1) and (NH4)2[Al2(C5H6NPO7)2(H2O)2]·4H2O (2), while reaction of Al(NO3)3·9H2O with NTA3P led to K8[Al2(C3H6NP3O9)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. |
| Keywords: | Neurotoxic aluminum Binary aluminum– (carboxy)phosphonate interactions Aqueous structural speciation X-ray crystal structure Solid state-solution property correlation |
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