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A new supramolecular Pb(II) complex [PbL(NO 2 )]  n   was synthesized from Pb(NO 3 ) 2 , N' -(1-(pyridin-2-yl)ethylidene)isonicotinohydrazide ( HL ) and NaNO 2 . [PbL(NO 2 )]  n   is constructed from discrete [PbL(NO 2 )] units with an almost ideal N 2 O 3 square pyramidal coordination environment around Pb(II). The ligand L -  is coordinated through the 2-pyridyl N-atom, one aza N-atom, and the carbonyl O-atom. The nitrite ligand binds in a κ  2 -O,O coordination mode through both O-atoms. The Pb(II) center exhibits a hemidirected coordination geometry with a pronounced coordination gap, which allows a close approach of two additional N-atoms arising from the N=C(O) N-atom of an adjacent molecule and from the 4-pyridyl N-atom from the another adjacent molecule, yielding a N 4 O 3 coordination, constructed from two Pb-N and three Pb-O covalent bonds, and two Pb⋯N tetrel bonds. Dimeric units in the structure of [PbL(NO 2 )]  n   are formed by the Pb⋯N=C(O) tetrel bonds and intermolecular electrostatically enforced π + ⋯π - stacking interactions between the 2- and 4-pyridyl rings and further stabilized by C-H⋯π intermolecular interactions, formed by one of the methyl H-atoms and the 4-pyridyl ring. These dimers are embedded in a 2D network representing a simplified uninodal 3-connected fes (Shubnikov plane net) topology defined by the point symbol (4∙8 2 ). The Hirshfeld surface analysis of [PbL(NO 2 )] revealed that the intermolecular H⋯X (X = H, C, N, O) contacts occupy an overwhelming majority of the molecular surface of the [PbL(NO 2 )] coordination unit. Furthermore, the structure is characterized by intermolecular C⋯C and C⋯N interactions, corresponding to the intermolecular π⋯π stacking interactions. Notably, intermolecular Pb⋯N and, most interestingly, Pb⋯H interactions are remarkable contributors to the molecular surface of [PbL(NO 2 )]. While the former contacts are due to the Pb⋯N tetrel bonds, the latter contacts are mainly due to the interaction with the methyl H-atoms in the π⋯π stacked [PbL(NO 2 )] molecules. Molecular electrostatic potential (MEP) surface calculations showed marked electrostatic contributions to both the Pb⋯N tetrel bonds and the dimer forming π + ⋯π - stacking interactions. Quantum theory of atoms in molecules (QTAIM) analyses underlined the tetrel bonding character of the Pb⋯N interactions. The manifold non-covalent interactions found in this supramolecular assembly are the result of the proper combination of the polyfunctional multidentate pyridine-hydrazide ligand and the small nitrito auxiliary ligand.

Tetrel Bonding and Other Non-Covalent Interactions Assisted Supramolecular Aggregation in a New Pb(II) Complex of an Isonicotinohydrazide