The present investigation describes the synthesis and structural study of the ligand 2-((1H-imidazol-2-yl)methyleneamino)phenol, which was used to generate three dimensio-nal supramolecular complex formulated as {[Ni(HL)2]2.[Ni(H2L)2]2.(Cl)4.(H2O)5}. The title compound crystallizes in the orthorhombic space group Fddd with the following unit cell parameters: a = 13.9269(4) Å, b = 29.5295(16) Å, c = 43.1739(15) Å, V = 17755.5(12) Å3, Z = 8, R1 = 0.043 and wR2 = 0.129. For this compound, the structure reveals that one neutral mononuclear unit [Ni(HL)2] and one cationic mononuclear unit [Ni(H2L)2]2+. In the neutral unit, the organic molecule acts as a tridentate through one imino nitrogen atom, one nitrogen atom from the imidazole ring and one phenolate oxygen atom. In the cationic unit, it acts as tridentate through one imino nitrogen atom, one nitrogen atom from the imidazole ring and one oxygen atom of non-deprotonated phenol group. In both units the nickel(II) ion is hexacoordinated and the coordination environment can be described as distorted octahedral geometry. Numerous hydrogen bonds link the molecules into three dimensional network.
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