Cyanide-bridged MnIIMIII coordination polymers, [Mn(dien)]3[M(CN)6]2·2H2O (M = Cr (1), Mn (2); dien = diethylenetriamine), have been prepared by using [M(CN)6]3- building units and a tridentate dien as a coligand. Single crystal and powder X-ray diffraction results of 1 and 2 proposed that the compounds are isomorphous and form a highly symmetric 3D network based on M8Mn12 cubes consist of [Mn(dien)] 2+ cations and μ6-, μ4-, and unbridged [M(CN)6]3- anions. Both compounds exhibited a ferrimagnetic ordering at 63.4 K (1) and 24.8 K (2) with coercive field of ∼0 G (1) and 1 kG (2). Their magnetic properties were compared with other cyanide-bridged MnIIMIII ferrimagnets and the differences were discussed based on the structure and the electric configuration.
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