Abstract

A tetranuclear mixed-spin nickel(II) complex featuring two urea molecules in an unprecedented μ3-ĸN:ĸN′:ĸO coordination mode has been structurally characterized. The two central high-spin nickel(II) ions exhibit ferromagnetic coupling (J = +3.4 cm−1) mediated by the NH2–C–O linkages of the bridging urea. In solution the temperature dependence of the UV/Vis optical absorption and of the magnetic moment indicate that, upon cooling, additional solvent molecules bind to the terminal low-spin metal ions and a concomitant spin change occurs. In the solid state the coordinated urea ligands can be thermally degraded to cyanate within the grip of the multimetallic nickel(II) site.

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