Preferred Electric Field Mechanism for Frustrated Lewis Pair Reactivity

Abstract This study employs computational methods to investigate the mechanism of H 2 activation by frustrated Lewis pair (FLP) species, including both intermolecular and intramolecular nitrothane/borane FLP systems. Previous studies have proposed two qualitative reactivity mechanism models to explain the facile cleavage of H 2 by FLPs. The findings of this study support the electric field mechanism as the favorable pathway for H 2 cleavage. Utilizing frontier molecular orbital theory and energy decomposition analysis, the study explores the electronic structure and nature of the reactions under an external electric field (EEF). Analysis using the activation strain model highlights the significant influence of geometrical deformation energies of FLPs on the activation barriers of H 2 activation reactions. Computational results suggest that H 2 activation by FLP molecules follows the electric field mechanism, indicating the potential of the FLP/EEF combination as an effective activator for inert molecules.