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The binary and ternary systems formed by VIVO and CuII ions with ligands (L) based on the pyridine ring (1,10-phenanthroline (phen), 2,2′-bipyridine (bpy), 2,2′:6′,2′′-terpyridine (terpy), 2,2′-bipyrimidine (bpm) and 2,3-bis(2-pyridyl)pyrazine (bpp)) were studied, combining spectroscopic (EPR and UV-vis), pH-potentiometric and computational (DFT calculations) methods. In the systems with VIVO, the formation of mono-chelated complexes with equatorial–equatorial and equatorial–axial (phen, bpy, bpm and bpp) or equatorial–equatorial–equatorial and equatorial–axial–equatorial coordination (terpy) and bis-chelated species with cis-octahedral geometry, with a water or a hydroxido ion in the fourth equatorial position, is demonstrated. Phen, bpy, bpm and bpp form also a dinuclear [(VO)2L2(H2O)2(OH)2]2+ complex with an anti-coplanar arrangement of the two VIVO ions and a ferromagnetic coupling …