Molecular magnet nickel(II) hexacyanoferrate(III), powder Ni3[Fe(CN)6]2ź15H2O, was prepared by coprecipitation method. The coprecipitated powder was annealed in vacuum at different temperatures of 80, 100, 120, and 140 graduate C. Water molecules contained in Prussian blue analogues were removed by heating. The effects of dehydration on its charge transfer properties were studied by Fourier-transform infrared and Mössbauer measurements. It was found that the FeIII–CN–NiII state is the major structure in the coprecipitated form, while the FeII–CN–NiIII bond is formed in the annealed samples. The dehydration of NiII ferricyanide above 80°C induces an inner charge transfer from NiII towards FeIII to form the mixed valence system Ni(II) Ni(III) ferri-ferro-cyanide.
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