The following coordination compounds derived from 2-guanidinobenzimidazole (2GB) (1); [Ni(2GB)2]C1 a" H20, (2); [Ni(2GB)z]BH.3H20, (3); [Ni(2GB)2 l-(NO3) 2, (4); [Ni(2GB); [Cu(2GB)2] (OAc)2-H2O , (t0); [Zn(2GB)C12]'H20, (tt); [Zn(2GB)Br2]" H20, (12); [Co(2GB)C12(H20)z]-5HzO, (13); [Co-(2GB)2C12]'3H20, (14);. [Co(2GB)2(H20)z](NO3) 2 4H20, (t5); and [Co(2GB)z(HzO)2](OAc) 2, (t6) have been synthesized and characterized by i.r. and electronic spectroscopy. In addition (6)-(10) were analysed by e.p.r. The X-ray diffraction structure of compound (4) was obtained. It crystallizes in the monoclinic system, C2/c (a=22.511 (7), b=6.735(6) arid c=15.345(5)A, /3 = 115.31(3) ~ Z = 4, final R =0.0360 and R W = 0.0388 for 1167 observed independent reflections). The nickel(II) atom coordinates two ligands in a square-planar geometry through the imidazolic N(3) and the guanidino N(12).The probable ligand isomers involved in the coordination were determined by theoretical calculations, and the possible structures of the coordination compounds were investigated in order to verify that the experimentally proposed structures were stable. Two different types of coordination compounds were found. One, where the ligand is chelating through the imidazolic N(3) and the guanidino N(12), which is the case for most of the complexes [(2)-(13)]. With only one ligand in the coordination sphere, the structure was either tetrahedral (copper and zinc chloride and bromide complexes) or octahedral (cobalt). With two chelating 2GB units a square-planar geometry was stabilized [(2)-(5) and (8)-(10)]. The second type of coordination behaviour was observed in the cobalt compounds [(I4)-(I6)]. Here the ligand coordinates monodentate through the imidazolic N(3); the structure is tetrahedral.

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