| Summary: | In the crystal structure of the title compound, {[Ni(NCS)2(C6H7N)2]·CH3CN}n, the NiII cation is octahedrally coordinated by two N-bonding and two S-bonding thiocyanate anions, as well as two 3-methylpyridine coligands, with the thiocyanate S atoms and the 3-methylpyridine N atoms in cis-positions. The metal cations are linked by pairs of thiocyanate anions into chains that, because of the cis–cis–trans coordination, are corrugated. These chains are arranged in such a way that channels are formed in which disordered acetonitrile solvate molecules are located. This overall structural motif is very similar to that observed in Ni(NCS)2[4-(boc-amino)pyridine]2·CH3CN reported in the literature. At room temperature, the title compound loses its solvent molecules within a few hours, leading to a crystalline phase that is structurally related to that of the pristine material. If the ansolvate is stored in an acetonitrile atmosphere, the solvate is formed again. Single-crystal X-ray analysis at room-temperature proves that the crystals decompose immediately, presumably because of the loss of solvent molecules, and from the reciprocal space plots it is obvious that this reaction, in contrast to that in Ni(NCS)2[4-(boc-amino)pyridine]2·CH3CN, does not proceed via a topotactic reaction.
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