Optimizing the Energetics of FLP-Type H₂ Activation by Modulating the Electronic and Structural Properties of the Lewis Acids: A DFT Study.

ABSTRACT: The great potential of frustrated Lewis pairs (FLPs) as metal-free catalysts for activation of molecular hydrogen has attracted increasing interest as an alternative to transition-metal catalysts. However, the complexity of FLP systems, involving the simultaneous interaction of three molecules, impedes a detailed understanding of the activation mechanism and the individual roles of the Lewis acid (LA) and Lewis base (LB). In the present work, using density functional theory (DFT) calculations, we examine the reactivity of 75 FLPs for the H₂ splitting reaction, including a series of experimentally investigated LAs combined with conventional phosphine-based (tBu₃P) and oxygen-based (i.e., ethereal solvent) Lewis bases. We find that the catalytic activity of the F

SUBMITTER: Heshmat M 

PROVIDER: S-EPMC8279552 | biostudies-literature | 2020 Aug

REPOSITORIES: biostudies-literature