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In the title compound, [Ni(C15H14N3O2S)2], the NiII atom lies on a center of symmetry. The deprotonated ligands act as N,S-donors, forming five-membered metalla-rings. The NiII atom is four-coordinated in a slightly distorted square-planar environment. In the crystal, the discrete complex mol­ecules are linked by weak N—H...O hydrogen bonds, generating chains along [110]. The chains are further connected via weak O—H...N inter­actions into a layered network extending parallel to (001).

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In the title compound, [Ni(NCS)2(C5H5N)2]n, the Ni2+ cation is coordinated by four thio­cyanate anions (μ-1,3) and two pyridine ligands within a slightly distorted octa­hedral configuration. The Ni—N bond lengths to the pyridine rings are 2.1189 (17) and 2.1241 (17) Å, whereas those to the thiocyanate anions are 2.0299 (18) and 2.0359 Å. The Ni—S bond lengths are 2.5357 (6) and 2.5568 (6) Å. The Ni2+ cations are linked by N:S-bridging thio­cyanate ligands into chains extending along [010]. The Ni...Ni distance within the chains is 5.5820 (5) Å. The asymmetric unit contains two Ni2+ cations of which one is located on a centre of inversion, whereas the second is located on a general position.

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The conformation of the title mol­ecule, C17H17N3S, is stabilized by an intra­molecular N—H...N hydrogen bond involving the azometinic group. The dihedral angle between the two aromatic rings is 36.49 (06)°. The non-aromatic ring of the tetra­lone substituent adopts a sofa conformation. In the crystal, mol­ecules are linked by pairs of N—H...S hydrogen bonds related via centres of symmetry, forming dimers.

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In the title compound, C15H15N3O2S, the central C—N—N—C unit has an anti conformation [torsion angle = −170.17 (15)°]. The phenyl substituent is oriented perpendicular to this unit [dihedral angle of 89.2 (1)°], whereas the substituted ring is rotated out of this plane by only 18.86 (17)°. In the crystal, mol­ecules are linked by pairs of N—H...S hydrogen bonds into inversion dimers that are further connected via N—H...O and O—H...S hydrogen bonds into a three-dimensional network.

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There are two independent mol­ecules in the asymmetric unit of the title compound, C12H15N3S, both of which display disorder of several C atoms in the N-bound ring (occupancy ratios of 0.75:0.25 in the first independent mol­ecule and 0.50:0.50 in the second) with the methyl H atoms also being disordered in the first mol­ecule (occupancy ratio of 0.70:0.30). The planes of the benzene ring and the N—N—C—N fragment make dihedral angles of 12.92 (14)° in the first independent mol­ecule and 7.60 (13)° in the second. In the crystal, mol­ecules are linked by weak N—H...S hydrogen bonds into chains along the a-axis direction. The crystal packing ressembles a herringbone arrangement.

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Although the mol­ecular structure of the title compound, C22H32N4O8, displays a twofold symmetry of the mol­ecule including the meth­oxy and methyl substituents, no crystallographic twofold symmetry is observed in the X-ray structure analysis. The carbonyl O atoms alternately point to different sides of the plane defined by the carbonyl C atoms. Two meth­oxy groups are oriented inside the mol­ecules cavity. The H atoms of two methyl groups are disordered over two orientations and were refined using a split model.
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