  Frustrated Lewis pairs (FLPs) are known for its ability to capture CO2.
Although many FLPs have been reported experimentally and several theoretical
studies have been carried out to address the reaction mechanism, the individual
roles of Lewis acids and bases of FLP in the capture of CO2 is still unclear.
In this study, we employed density functional theory (DFT) based metadynamics
simulations to investigate the complete path for the capture of CO2 by
tBu3P/B(C6F5)3 pair, and to understand the role of the Lewis acid and base.
Interestingly, we have found out that the Lewis acids play more important role
than Lewis bases. Specifically, the Lewis acids are crucial for catalytical
properties and are responsible for both kinetic and thermodynamics control. The
Lewis bases, however, have less impact on the catalytic performance and are
mainly responsible for the formation of FLP systems. Based on these findings,
we propose a thumb of rule for the future synthesis of FLP-based catalyst for
the utilization of CO2.
