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Intermolecular, stepwise functionalization by BH bonds of a (triphosphine)MoIV–nitrido complex generated by N2 splitting is reported. The imido–hydride and di‐hydride–amido MoIV complexes have been isolated and characterized. Addition of PinBH to the [Mo(H)2(N(BPin)2)]+ complex at room temperature results in the liberation of borylamines from the metal center.
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