Nitrogen fixation to cyanide at a molybdenum center

Facile methoxymethylation of N-2-derived nitride NMo(N-[Bu-t]Ar)(3) provided the imido cation [MeOCH2NMo(N-[Bu-t]Ar)(3)](+) as its triflate salt in 88% yield. Treatment of the latter with LiN(SiMe3)(2) provided blue methoxyketimide complex MeO(H)CNMo(N[Bu-t]Ar)(3) in 95% yield. Conversion of the latter to the terminal cyanide complex NCMo(N[Bu-t]Ar)(3), which was the subject of a single-crystal X-ray diffraction study, was accomplished in 51% yield upon treatment with a combination of SnCl2 and Me2NSiMe3.