A COMPUTER SIMULATION STUDY ON LEWIS ACID–BASE INTERACTIONS AND COOPERATIVE C-H⋯O WEAK HYDROGEN BONDING IN VARIOUS CO2 COMPLEXES

Abstract

The Lewis acid–base interaction and cooperative C-H⋯O weak hydrogen bonding have been widely suggested as two key factors in the solubility of CO2 -philic materials. In this work, both ab initio and Monte Carlo simulations were performed to investigate the properties of the two important interactions between CO2 and several common organic molecules. Binding energies, geometries and charge transfer were calculated by ab initio method, showing that the mutual enhancement between the two sorts of interactions plays an important role in the stability of the CO2 complexes. Monte Carlo simulations were employed to investigate the effect of many-body interactions in real solutions. The results show that the many-body interactions also have a significant impact on the energetic and geometric properties of the CO2 complexes. Moreover, the self-aggregation of strong polar molecules will greatly weaken the effective Lewis acid–base interaction due to the zone overlapping, which needs to be taken into account in the design of future CO2 -philes.