Halogen‐Bonded Co‐Crystals Containing Mono‐ and Dinuclear Metal‐Organic Units: Three‐Component One‐Pot Mechanosynthesis, Structural Analysis and Magnetic Properties

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Abstract We provide a systematic investigation of three‐component one‐pot mechanochemical reactions which combine the formation of coordination bonds and halogen bonds to obtain crystal structures based on halogen‐bonded metal‐organic units. Grinding CuCl2 ⋅ 2H2O or CuCl2, 2‐benzoylpyridine (bzpy) and perfluorinated iodobenzenes as halogen bond donors in different stoichiometric ratios has shown that one‐pot mechanosynthesis is a useful approach in the preparation of halogen‐bonded co‐crystals containing mononuclear or dinuclear copper(II) complexes as halogen bond acceptors. This study has yielded a series of seven new co‐crystals: five co‐crystals containing the mononuclear complex [CuCl2(bzpy)2] and two co‐crystals containing the dinuclear complex [Cu2Cl4(bzpy)2]. All solid products were also obtained by crystallization from the solution. Single‐crystal X‐ray diffraction revealed that the co‐crystals display different crystal packing governed by Cu−Cl⋯I halogen bonds. Magnetization measurements revealed that all co‐crystals are paramagnetic in the entire measured temperature range.

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