The single-step electrochemical synthesis of neutral transition metal complexes of imidazole, pyrazole and their derivatives has been achieved at ambient temperature. The metal was oxidized in an MezCO solution of the diazole to yield complexes of the general formula: [M(Iz)2 ] (where M = Co, Ni, Cu, Zn; Iz = imidazolate); [M(MeIz)2 ] (where M = Co, Ni, Cu, Zn; MeIz = 4-methylimidazolate); [M(priIz)2] (where M = Co, Ni, Cu, Zn; priIz = 2-isopropylimidazolate); [M(pyIz).] (where M = Co m, Cu n, Znll; pyIz = 2-(2'-pyridyl)imidazolate); [M(PZ)n ] (where M = Co hI, Ni n, Cu n, Znn; Pz = pyrazolate); [-M(C1Pz)n ] and [M(IPz)~] (where M = Co m, Ni", Cu n, Zn"; CIPz = 4-chloropyrazolate; IPz = 4-iodopyrazolate); [M(Me2Pz),] (where M = Co n, Cu ~, Zn"; MezPz = 3,5-dimethylpyrazolate) and [M(BrMezPz)J (where M = Co n, Ni n, Cu I, Znn; BrM%Pz = 3,5-dimethyl-4-bromopyrazolate). Vibrational spectra verified the presence of the anionic diazole and electronic spectra confirmed the stereochemistry about the metal centre. Variable temperature (360-90 K) magnetic measurements of the cobalt and copper chelates revealed strong antiferromagnetic interaction between the metal ions in the lattice. Data for the copper complexes were fitted to a Heisenberg (S = 1/2) model for an infinite one-dimensional linear chain, yielding best fit values of J=-62--65cm -x and 9=2.02-2.18. Data for the cobalt complexes were fitted to an Ising (S = 3/2) model with J = --4.62---11.7 cm-z and g = 2.06-2.49.
