Rare examples of trinuclear [Ni-N-M-N-Ni] core (M = Ca, Mg) with linear bridged dinitrogen ligands are reported in this work. The reduction of [PrNN]Ni(μ-Br)Li(thf) (1) (PrNN = 2,4-bis-(2,6-diisopropylphenylimido)pentyl) with elemental Mg or Ca in THF under an atmosphere of dinitrogen yields the complex {PrNNNi(μ-N)}M (thf) (M = Mg, complex 2 and M = Ca, complex 3). The bridging end-on (μ-N)M(thf) moiety connects the two [PrNNNi] nickelate fragments. A combination of X-ray crystallography, solution and solid-state spectroscopy have been applied to characterize complexes 2 and 3, and DFT studies have been used to help explain the bonding and electronic structure in these unique Ni-N-Mg and Ni-N-Ca complexes.
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