Synthesis, Crystal Structures and Magnetic Properties of Copper(II) Complexes with Nitronyl Nitroxide Radicals

Two new copper(II) compounds with imino nitroxide radicals [Cu(IM‐MeImz)2· (SCN)] 0.5[Cu(SCN)4] (1) and [Cu(IM‐MeImz)2· (SCN)]ClO4· H2O (2) (IM‐meImz = 2‐(5‐methylimidazol‐4‐yl)‐4,4,5,5‐tetramethyl‐2‐imidazoline‐1‐oxyl) have been synthesized and characterized structurally and magnetically. X‐ray analysis demonstrates that complex 1contains CuIIions in both square‐pyramidal and square planar coordination. There are complete charge separation into [Cu(IM‐MeImz)2(SCN)]+cations and 0.5[Cu(SCN)4]−anions, in a 2:1 ratio. The complex 1was connected as a one‐dimensional polymer by intermolecular interactions. In complex 2, the coordination around the copper atom is distorted square pyramidal and the apical position is occupied by one nitrogen atom of SCN−anion. The 2‐D network structure was formed and arranged through intermolecular H‐bonds interactions. The complex 1exhibits intramolecular weak ferromagnetic coupling between CuIIion and the radicals.