Synthesis and detailed structural characterization of a new coordination compound [Sn(HL)2(NCS)2]·0.5MeOH (1·0.5MeOH), synthesised from a mixture of SnSO4 and KNCS with a bulky organic ligand phenyl(pyridin-2-yl)methylenepicolinohydrazide (HL) in MeOH, is reported. The metal is N6O2 octacoordinated by two tridentate ligands HL through the pyridyl-imine units and the carbonyl oxygen atoms, and its coordination sphere is completed by two N-bound isothiocyanate anions to form the mononuclear heteroleptic complex. The crystal packing of 1·0.5MeOH is strongly dictated by aromatic pyridine and benzene substituents in the structure of coordinated ligands HL. The pyridine rings are involved in intermolecular π(Py)···π(Py) stacking interactions, yielding a 2D supramolecular layer. These 2D layers are further interlinked in the orthogonal direction through intermolecular π(Ph)···π(Ph) stacking interactions, yielding a 3D supramolecular structure. The structure of 1·0.5MeOH is further stabilized by weak non-covalent interactions of the type C–H···S and C–H···π(Py). Latter interactions have been studied using density functional theory (DFT) and molecular electrostatic potential (MEP) surface calculations and characterized using the quantum theory of atoms-in-molecules (QTAIM).
