Abstract
Two new molecular solids, [BzPyNH 2][Ni(mnt) 2]( 1) and [2-NpCH 2PyNH 2][Ni(mnt) 2]( 2) (mnt 2− = maleonitriledithiolate, [BzPyNH 2] + = 1-benzyl-2-aminopyridinium and [2-NpCH 2PyNH 2] + = 1-(2′-naphthylmethylene)-2-aminopyridinium) have been characterized structurally and magnetically. The Ni(Ш) ions of 1 and 2 form a 1D magnetic chain within a [Ni(mnt) 2] − column through Ni⋯N or π⋯π interactions. Some weak interactions observed in 1 and 2 give further rise to a 2D structure. The overlapping fashions of the [Ni(mnt) 2] − anions are different when the 2-aminopyridine ring was fixed and the phenyl ring changed into the naphthyl ring of the cation. Magnetic susceptibility measurements in the temperature range 2–300 K show that 1 is weak antiferromagnetic coupling, while 2 exhibits a novel and interesting spin-gap transition around 140 K with Δ/ k b = 381.4 K.
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