Mechanistic Insight into the CO2 Capture by Amidophosphoranes: Interplay of the Ring Strain and the trans Influence Determines the Reactivity of the Frustrated Lewis Pairs

Abstract CO 2 capture has attracted increasing attention owing to its contribution to global warming and climate change as a greenhouse gas. As an alternative strategy to transition‐metal‐based chemistry and catalysis, frustrated Lewis pairs have been developed to sequester CO 2 efficiently under mild conditions. However, the mechanism of CO 2 sequestration with amidophosphoranes remains unclear. Herein, we present a thorough density functional theory study on a series of amidophosphoranes. Our results reveal that the interplay of the ring strain and the trans influence determines the reactivities, thus opening a new avenue to the design of frustrated Lewis pairs for CO 2 capture.