(Pyridin‐2‐ylmethyl)triel Derivatives as Masked Frustrated Lewis Pairs. Interactions and CO₂‐Sequestration

Abstract

The isolated (pyridin‐2‐ylmethyl)triel derivatives (triel = B, Al and Ga) show an intramolecular N···Tr triel bond as shown by compounds found in the Cambridge Structural Database and DFT calculations. The possibility to use them as masked frustrated Lewis pairs (mFLP) has been explored theoretically concerning their reaction with CO2. The adduct formation proceeds in two steps. In the first one, the (pyridin‐2‐ylmethyl)triel derivatives break the intramolecular N···Tr bond assisted by CO2 and in the second step the adduct is formed with Tr‐O and N‐C covalent bonds. The corresponding energy minima and transition states (TS) of the reaction have been characterized and analyzed. The distortion/interaction model analysis of the stationary points indicates that the whole process can be divided in two parts: reorganization of the mFLP in the first steps of the reaction while the reaction with CO2 (associated to the distortion of this molecule) is more important in the formation of the final adduct. In all cases studied, the final products are more stable than the starting molecules that combine with reasonable TS energies indicate that these reactions can occur.