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We report the formation and N(2) reactivity of novel cobalt hydride complexes supported by bulky beta-diketiminate ligands (L). Addition of KHBEt(3) to LCoCl gives [LCo(mu-H)](2) (1) or K(2)[LCoH](2) (2), depending on the amount of borohydride used. Compound 2 is the first example of a crystallographically characterized hydride complex in which a transition metal is three-coordinate. Both 1 and 2 react with N(2) at room temperature to give dinuclear N(2) complexes with loss of H(2).

Three-Coordinate and Four-Coordinate Cobalt Hydride Complexes That React with Dinitrogen