Abstract
Two different dinitrogen-derived molybdenum nitrido complexes varying by their geometry, ligand spheres and oxidations states were shown to engage their N ligand in dative bonding with the strong Lewis acid B(C6F5)3. The stable adducts were assessed for frustrated Lewis pair-type heterolytic E–H bond splitting of hydrosilanes (E = Si) and HB(C6F5)2. Whereas Si–H bond activation was achieved, HB(C6F5)2 was shown to substitute B(C6F5)3 in a quantitative or equilibrated fashion, depending on the nature of the nitrido complex. No B–H bond splitting was observed. Thermodynamics of these reactions, computed by DFT, are in agreement with the experimental outcomes.