Three complexes [Ni(Him)4(3,4-NCNsq)(H2O)]·H2O 1, {[Ni2(Him)2(3,4-NCNsq)2(H2O)6]·8H2O}n2 and [Ni(tren)(3,4-NCNsq)]n3, where 3,4-NCNsq2−
= 3,4-bis(cyanamido)cyclobutane-1,2-dione dianion and Him = imidazole, have been synthesized and characterized by electronic absorption and IR spectroscopies. The structures of the three complexes have been determined by X-ray crystallography and, for the first time, two conformations of the ligand 3,4-NCNsq2− have been evidenced. Complex 1 consists of mononuclear entities and complexes 2 and 3 are made of infinite chains with nickel(II) atoms bridged by the bis monodentate 3,4-NCNsq2− ions. The magnetic properties of the three complexes have been investigated in the 2–300 K temperature range (μeff
= 2.84 to 3.12 μB for 1, μeff
= 2.32 to 3.46 μB for 2 and μeff
= 2.74 to 3.13 μB for 3). Their redox properties are discussed and compared to those of the free 3,4-NCNsq2− dianion.
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