Assessing Combinations of B(C₆F₅)₃ and N₂‐Derived Molybdenum Nitrido Complexes for Heterolytic Bond Activation

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(C 6 F 5 ) 3 . The stable adducts were assessed for frustrated Lewis pair‐type heterolytic E−H bond splitting of hydrosilanes (E=Si) and HB(C 6 F 5 ) 2 . Whereas Si−H bond activation was achieved, HB(C 6 F 5 ) 2 was shown to substitute B(C 6 F 5 ) 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.