2D crystal structure, magnetic behavior and theoretic analysis of two new molecular solids based on Ni(maleonitriledithiolate)2 monoanion with substituted 2-aminopyridinium

Two new molecular solids based on [Ni(mnt)2]− monoanion, [BzPyNH2][Ni(mnt)2](1) and [2-NpCH2PyNH2][Ni(mnt)2](2) (mnt2− = maleonitriledithiolate, [BzPyNH2]+ = 1-benzyl-2-aminopyridinium and [2-NpCH2PyNH2]+ = 1-(2′-naphthylmethylene)-2-aminopyridinium), form a 1D magnetic chain, 1 is weak antiferromagnetic coupling, while 2 exhibits a novel and interesting spin-gap transition.