Cleavage of dihydrogen is an important step in the industrial and enzymatic transformation of N into ammonia. The reversible cleavage of dihydrogen was achieved under mild conditions (room temperature and 1 atmosphere of H ) by the molecular uranium nitride complex, [Cs{U(OSi(O Bu) ) } (μ-N)] 1, leading to a rare hydride-imide bridged diuranium(IV) complex, [Cs{U(OSi(O Bu) ) } (μ-H)(μ-NH)], 2 that slowly releases H under vacuum. This complex is highly reactive and quickly transfers hydride to acetonitrile and carbon dioxide at room temperature, affording the ketimide- and formate-bridged U species [Cs{U(OSi(O Bu) ) } (μ-NH)(μ-CH CHN)], 3 and [Cs{U(OSi(O Bu) ) } (μ-HCOO)(μ-NHCOO)], 4.

Cleavage of dihydrogen is an important step in the industrial and enzymatic transformation of N 2 into ammonia. The reversible cleavage of dihydrogen was achieved under mild conditions (room temperature and 1atmosphere of H 2 ) by the molecular uranium nitride complex, [Cs{U(OSi-(O t Bu) 3 ) 3 } 2 (m-N)] 1, leading to ar are hydride-imide bridged diuranium(IV) complex, [Cs{U(OSi(O t Bu) 3 ) 3 } 2 (m-H)(m-NH)], 2 that slowlyr eleases H 2 under vacuum. This complex is highly reactive and quickly transfers hydride to acetonitrile and carbon dioxide at room temperature,a ffording the ketimide-and formate-bridged U IV species [Cs{U(OSi-(O t Bu) 3 ) 3 } 2 (m-NH)(m-CH 3 CHN)], 3 and [Cs{U(OSi-(O t Bu) 3 ) 3 } 2 (m-HCOO)(m-NHCOO)], 4.