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Half-sandwich type rhodium(III)–aminohydroxamate complexes: the role of the position of the amino group in metal ion binding.

Autoři: Parajdi-Losonczi P.L., Buglyo P., Skakalova H., Kasparkova J., Lihi N., Farkas E.Publikováno : New Journal of Chemistry 42(10), 7659-7670Rok: 2018

Complex formation equilibria between [(η⁵-Cp*)RhIII(H2O)3]2+ and aminohydroxamic acids (2-amino-N-hydroxyacetamide (α-alahaH), 3-amino-N-hydroxypropanamide (β-alahaH) and 4-amino-N-hydroxybutanamide (GABAha, γ-abhaH)) having the primary amino group in different chelatable position to the hydroxamic function were studied by pH-potentiometric, 1H NMR and ESI-MS methods and formation constants of the complexes present in aqueous solution are reported. Relative order of the pH-dependent conditional stability of the hydroxamate type (O,O) and (Namino, Nhydroxamato) chelates was found to determine in high extent the coordination modes both in the mono- and various dinuclear species formed. While with α-alaha–, the 5-membered (N,N) chelated mononuclear complex predominates, with β-alaha–, in a wide pH-range, very stable dinuclear cluster ions exist. With γ-abha–, in the most stable complexes, two ligands (in reverse variation) link two half-sandwich cations, coordinating each ligand via the hydroxamate chelate to one metal centre, while via the amino-N to the other one. This arrangement seems to be further stabilized by a hydrogen bond as DFT calculations support the extra stabilization effect of an internal H-bonding in [{(η⁵-Cp*)RhIII}2H–1(γ-abha)2]⁺. Synthesis, spectral (NMR, IR) and MS characterization of a novel complex with the iridium analogue, [(η⁵-Cp*)IrIII(α-alaha)Br] (1) is also described. This complex was tested for its in vitro cytotoxicity using human-derived cancer cell lines (A2780, HeLa, DU-145, A549, and MCF-7) and showed insignificant anti-proliferative activity in the micromolar concentration range.


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