Enhancing the reactivity of uranium(vi) organoimido complexes with diazoalkanesElectronic supplementary information (ESI) available: experimental, including general procedures, materials and synthesis of complexes 2 and 3. See http://www.rsc.org/suppdata/cc/b1/b109455f/

Diphenyldiazomethane effects a two-electron oxidation of the uranium(IV) monoimido complex (C5Me5)2U(=N-2,4,6-t-Bu3C6H2) to give the uranium(VI) mixed bis(imido) complex, (C5Me5)2U(=N-2,4,6-t-Bu3C6H2)(=N-N=CPh2), which undergoes a rare cyclometallation reaction upon mild thermolysis to afford a uranium(IV) bis(amide) complex that results from net addition of a C-H bond of an ortho tert-butyl group across the N=U=N core.