The [Ni(S 2 COCH 2 CH 2 CH 3 ) 2 (C 6 H 4 N 2 ) 2 ] adduct of 4-cyanopyridine with [Ni(S 2 COCH 2 CH 2 CH 3 ) 2 ] was synthesized and characterized by elemental analysis, magnetic susceptibility measurement, IR, electronic spectral data, Thermogravimetric analysis/DTA techniques and X-ray diffraction analysis. The Ni atom in the title complex is octahedrally coordinated within a trans-N 2 S 4 donor set, with the Ni atom located on a centre of inversion. The title complex crystallizes in the monoclinic space group P2 1 /c with unit cell parameters a = 11.75(4), b = 11.62(3), c = 9.20(2) Å , b = 104.99(3)°. Crystal structure was solved by direct methods and refined by full matrix least squares procedures to a final R-value of 0.0294 for 1895 observed reflections. The packing of layers of molecules is stabilized by weak C-HÁÁÁN and C-HÁÁÁp interactions.

The Ni2+ ion in the title complex, [Ni(C3H5OS2)2(C6H4N2)2], is in a strongly distorted octa­hedral coordination environment formed by an N2S4 donor set, with the Ni2+ ion located on a centre of inversion. In the crystal, weak C—H⋯S and C—H⋯N inter­actions are observed.

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The [Ni(S2CO-n-C5H11)2(C6H4N2)2] adduct of 4-cyanopyridine with [Ni(S2CO-n-C5H11)2] was synthesized and characterized by elemental analysis, magnetic susceptibility measurement, IR, electronic spectral data, and X-ray diffraction analysis. The Ni atom in the title complex is octahedrally coordinated within a trans-N2S4 donor set, with the Ni atom located on a centre of inversion. The title compound exhibits magnetic moment value (3.20 B.M) which is in agreement with magnetic moment values observed for paramagnetic octahedral complexes of nickel(II). The title complex crystallizes in the orthorhombic space group Pbca with unit cell parameters a = 11.455(5), b = 9.602(4), and c = 26.374(1) Å. Crystal structure was solved by direct methods and refined by full matrix least-squares procedures to a final R value of 0.0499 for 2004 observed reflections. The amyl chain is disordered over two sets of sites, with occupancy ratios of 0.595 : 0.405. Infinite long chains of molecules are formed with the help of C–H⋯N hydrogen bond.