The crystal structures and magnetic properties of compounds [MII(apo)(N(CN)2)2], where M = Co (1), Ni (2) or Mn (3), apo = 2-aminopyridine N-oxide, have been determined. The structural analyses revealed that they are isomorphous, and all belong to monoclinic space group P21/n. The metal(II) ions display distorted octahedral co-ordination, with four terminal N atoms of different [N(CN)2]− ligands and two O atoms of different apo ligands. Two ions are bridged by two μ-O atoms to form a dimer subunit. Those dimers are further linked to each other by [N(CN)2]− resulting in a three-dimensional structure. The magnetic properties of the compounds were investigated in the temperature range 2–300 K for 1 and 2 and 4–300 K for 3. The values for the intradimer spin coupling constant J were estimated to be −17.8, −40, −1.3 cm−1 for 1–3, respectively, indicative of antiferromagnetic interaction.
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