The refluxing of chloroacetamide derivatives with n-butyl imidazole resulted in their corresponding salt of composition 1-(n-butyl)-3-N-(2-Ar)acetamido-1, 3-imidazolium chloride (Ará=áfurylmethyl (1a); phenylmethyl (1b)). The latter salt on treatment with DBU followed by the addition of chalcogen atom resulted into a compound [(1-(n-butyl)-3-N-(2-Ar)acetamido-1,3-imidazol-3-ylidine)E] (Ará=áfurylmethyl; Eá=áS (2a); Ará=áphenylmthyl; Eá=áSe (2b)). Similarly, the reaction of the imidazolium salts with, excess K2CO3 and NiCl2E6H2O yielded compounds [(1-(n-butyl)-3-N-(2-Ar)acetamido-1,3-imidazol-3-ylidine)]2Ni (Ará=áfurylmethyl (3a); phenylmethyl (3b)). The latter complexes have also been isolated by using Ni(II) phosphine precursors [NiCl2(PP)] (PPá=áPPh3, dppf). The molecular structure of [(1-(n-butyl)-3-N-(2-furylmethyl)acetamido-1, 3-imidazol-3-ylidine)]2Ni and [(1-(n-butyl)-3-N-(2-phenylmethyl)acetamido