A cyanide-bridged bimetallic compound, [Ni(1,1-dmen)2]2[Fe(CN)6] (BPDS)0.5·4H2O (1) (1,1-dmen = 1,1-dimethylethylenediamine, BPDS2- = biphenyl-4,4′-disulfonate), has been prepared. It has a pseudo 2-D network structure based on a Fe4Ni4 square unit with two Fe-CN-Ni-NC-Fe and two Fe-CNH2O-Ni-NC-Fe linkages and shows a metamagnetic ordering with Tc = 3.3 K. The dehydration of 1 at 150 °C has afforded [Ni(1,1-dmen)2]2[Fe(CN)6] (BPDS)0.5 (1a). It has a definite 2-D network structure based on a Fe4Ni4 square unit with four Fe-CN-Ni-NC-Fe linkages and shows essentially a ferromagnetic ordering with Tc = 10.7 K under weak applied field (> 250 G). 1a is hygroscopic and adsorbed atmospheric moisture to afford [Ni(1,1-dmen)2]2[Fe(CN)6] (BPDS)0.5·2H2O (1b), which has a pseudo 2-D network structure similar to that of 1 and shows a metamagnetic ordering with Tc = 4.0 K. 1a and 1b can be interconverted by dehydration at 150 °C and hydration in open air at room temperature, producing a unique molecular magnetic system exhibiting a reversible ferromagnetism/metamagnetism modulation.
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