Reaction of 2-hydroxy-acetophenone (HL) or 2-hydroxy-benzophenone (HL') with nickel(ii) acetate provides the tetrakis-[(μ3-methanolato-κ3 O:O:O)(methanol-κO)(2-oxyacetophenone-κ2 O,O')nickel(ii)], [Ni(L)(μ3-CH3O)(CH3OH)]4 (1) or tetrakis-[(μ3-methanolato-κ3 O:O:O)(aqua-κO)(2-oxybenzophenone-κ2 O,O')nickel(ii)] monohydrate, [Ni(L')(μ3-CH3O)(H2O)]4·H2O (2). Molecular structure determination demonstrates each nickel(ii) ion is six-coordinate with a distorted octahedral geometry defined by three oxygen atoms from three methoxide fragments, a methanol (1) or water (2) molecule, and two oxygen atoms from the acetophenonate (L-) or benzophenonate (L'-) ligand, such that the four nickel atoms and four methoxide groups represent a cubane-type structural topology with each methoxide fragment bridging three of the metal centers. Stabilization of the cubane core occurs via intramolecular O-H⋯O hydrogen bonds. Solid-state magnetic measurements along with computational modeling confirm dominant ferromagnetic interactions for the compounds, attributed to their cubane topology and the Ni-O-Ni angles adopting values lower than 100°. Thermogravimetric analysis (TGA) suggests thermal decomposition of the complexes with successive release of the lattice water, coordinated solvents (MeOH or H2O), OCH3 groups and fragmented ligand species, supported by differential scanning calorimetry (DSC) studies. Cyclic voltammetry reveals a quasi-reversible two electrons charge transfer process in N,N-dimethylformamide.

Department of Chemistry Jahangirnagar University Dhaka 1342 Bangladesh

Department of Chemistry University of Manitoba 144 Dysart Road Winnipeg Manitoba R3T 2N2 Canada

Department of Inorganic Chemistry Faculty of Science Palacký University Olomouc Olomouc 77146 Czech Republic

Institut für Anorganische Chemie und Strukturchemie Universität Düsseldorf Universitätsstr 1 D 40225 Düsseldorf Germany

Institute of Physics of Materials Czech Academy of Sciences Žižkova 22 61662 Brno Czech Republic

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