When the ligand 1,4,5-triazanaphthalene (abbreviated as tan) is reacted with Cu(II) BF4− and ClO4− salts, a variety of mononuclear compounds has been found, all with the [Cu(tan)4] unit and varying amounts of weakly coordinating axial ligands and lattice solvents. Reproducible compounds formed include two purple compounds, analyzing as [Cu(tan)4](ClO4)2(CH3OH)2(H2O) (1) and [Cu(tan)4](BF4)2(CH3OH)1.5(H2O) (3), and two blue compounds, analyzing as [Cu(tan)4](ClO4)2(H2O)2 (2) and [Cu(tan)4]2(BF4)2(H2O)2 (4). Upon standing at room temperature, red-coloured, mixed-valence dinuclear-based 3D coordination polymers are formed by conversion of the purple/blue products, of which [Cu2(tan)4]n(BF4)3n (5) and the isomorphic methanol–water adduct [Cu(tan)4]n(BF4)3n(CH3OH)n(H2O)5n (5A) are presented in this paper. In addition a fully reduced dinuclear Cu(I) compound of formula [Cu2(tan)3(ClO4)2] (7) has been observed, and structurally characterized, as a rare three-blade propeller structure, with a Cu–Cu distance of 2.504 Å.
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