Theoretical insights into the activation of N2O by a model Frustrated Lewis Pair. An ab-initio metadynamics study

Abstract

Frustrated Lewis Pairs (FLPs) are a prominent class of substances capable of activation of small molecules. Albeit several experimental and theoretical studies devoted to the activation of greenhouse gases were recently published, activation of N2O are yet scarce. In present study we employed Density Functional Theory based metadynamics to reconstruct the Free Energy Landscape of the activation of N2O by the model [t-Bu3P][B(C6F5)(3)] FLP. Similarly to the mechanism observed in the activation of CO2, Lewis acid promotes the thermodynamic requirements of the reaction by stabilizing key intermediates. Regioselectivity of the activation of N2O as well as the effect of phosphine basicity are also discussed.