EPR, NMR relaxation methods, and DFT calculations were jointly used to investigate the structural and dynamical characteristics of solvation shells of copper(II) complexes with iminodiacetic acid, glycylglycine, and glycyglycylglycine in comparison with the copper(II) bis-glycinate studied previously. A strong trans influence of deprotonated peptide nitrogen was revealed in EPR spectra parameters of copper(II) complexes with oligopeptides. With models of the experimental NMRD data and literature X-ray structural information, it was suggested that only one water molecule coordinates in axial position of copper(II) complexes with glycine and di- and triglycine (Cu(Gly)2, Cu(GGH(-1)), and Cu(GGGH(-2))(-)), and the copper ion in these complexes is pentacoordinated, while in the iminodiacetate complex, Cu(IDA), both apical positions can be occupied by solute molecules.
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