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Vapour- and solvent-mediated crystalline transformations in Mo(vi) hydrazone complexes controlled by noncovalent interactions

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Abstract

The synthesis and structures of the Mo(VI) coordination polymer [MoO2(L)]n (1), mononuclear complexes [MoO2(L)(MeOH)] (2α, 2β, and 2γ), and salts [MoO2(HL)(MeOH)]X, where X = Cl (3), Br (4), NO3 (5), and MeOSO3 (6), and L = 4-methoxysalicylaldehyde isonicotinoylhydrazonato ligand, are described. Polymer 1 can be quantitatively self-assembled from the neutral mononuclear complex upon vapour-mediated desolvation. The efficiency of the solid-state transformation is driven by the proximity of reaction centres due to O–H⋯N interactions. Additionally, the conversion seems to be sensitive to solvent polarity and can be achieved only in the presence of polar non-coordinating solvents. In the case of salts 3–6, an examination of the crystal structures shows that two architecturally different supramolecular assemblies are obtained. When anion X is Cl or Br, hydrogen bonded dimers are constructed while in the case of NO3 or MeOSO3 infinite hydrogen-bonded 1D chains are achieved. In the deprotonation reactions with Et3N, crystals of 3 or 4 and 5 or 6 serve as heteronuclear templates, affording polymorphic forms 2α and 2γ, respectively. A common feature of 2α and 2β forms is the association of the molecules into discrete dimers, whereas in the case of 2γ, 1D chains are formed as a consequence of O–H⋯N hydrogen bonding interactions. The non-porous complex 2α is shown to undergo a single-crystal-to-single-crystal transformation when crystals are exposed to moisture, thus yielding chains of hydrogen bonded dimers of [MoO2(L)(H2O)] (2w-α). The potent and broad-spectrum activity of 2–6 was established against selected Gram-positive and Gram-negative bacteria. The cytotoxicity of the compounds was evaluated on HepG2 and THP-1 cell lines.

Graphical abstract: Vapour- and solvent-mediated crystalline transformations in Mo(vi) hydrazone complexes controlled by noncovalent interactions

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Publication details

The article was received on 13 Aug 2019, accepted on 27 Sep 2019 and first published on 27 Sep 2019


Article type: Paper
DOI: 10.1039/C9CE01273G
CrystEngComm, 2019, Advance Article

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    Vapour- and solvent-mediated crystalline transformations in Mo(VI) hydrazone complexes controlled by noncovalent interactions

    M. Mandarić, B. Prugovečki, D. Cvijanović, J. P. Vuković, J. Lovrić, M. Skočibušić, R. Odžak, M. Cindrić and V. Vrdoljak, CrystEngComm, 2019, Advance Article , DOI: 10.1039/C9CE01273G

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