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Extended lead(II) architectures engineered via tetrel bonding interactions

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The evaluation of N′-(pyridin-2-ylmethylene)nicotinohydrazide (HLI) and N,N′′′-bis(1-(pyridin-2-yl)-ethylidene)carbazide (H2LII) as linker precursors in the synthesis of novel PbII extended structures is described. An equimolar one-pot reaction of PbX2 (X = NO3, CH3COO) salts with HLI and H2LII in MeOH at 60 °C in a branched tube apparatus leads to heteroleptic complexes [Pb(HLI)(NO3)2]n (1), [Pb(LI)(CH3O)]n (2), [Pb2(H2LII)(NO3)4] (3) and [Pb2(HLII)(CH3COO)3]n (4), respectively. The nature of the anion in the parent PbII salt also influences the final structure. In all complexes, the PbII center exhibits a hemidirected coordination geometry with all the covalent bonds being concentrated on one hemisphere of the coordination sphere. The sterically available PbII ion participates in Pb⋯O/N tetrel bonding or Pb⋯Cg interaction as evidenced from the detailed structural and topological analysis of the described complexes. As a result of these interactions, the structures of all four compounds can be extended to a higher dimensional framework, which is further stabilized by hydrogen N–H⋯O/C–H⋯O and dihydrogen C–H⋯H–C bonds and/or π⋯π stacking interactions. The complementary Hirshfeld surface analysis of the discrete complex 3, considering covalent bonds, showed that the structure is highly dominated by H⋯X (X = O, H and C) and O⋯Y (Y = O, Pb, C and N) contacts, of which the O⋯Pb/H/N/C contacts are highly favoured. DFT based charge and energy decomposition (ETS-NOCV) calculations are performed in order to shed light on the nature of the non-covalent interactions that determine the stability of the obtained structures.

Graphical abstract: Extended lead(ii) architectures engineered via tetrel bonding interactions

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Publication details

The article was received on 30 Jan 2018, accepted on 21 Feb 2018 and first published on 23 Feb 2018

Article type: Paper
DOI: 10.1039/C8NJ00525G
Citation: New J. Chem., 2018, Advance Article
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    Extended lead(II) architectures engineered via tetrel bonding interactions

    G. Mahmoudi, E. Zangrando, M. P. Mitoraj, A. V. Gurbanov, F. I. Zubkov, M. Moosavifar, I. A. Konyaeva, A. M. Kirillov and D. A. Safin, New J. Chem., 2018, Advance Article , DOI: 10.1039/C8NJ00525G

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