Preorganization and Cooperation for Highly Efficient and Reversible Capture of Low‐Concentration CO2 by Ionic Liquids

A novel strategy based on the concept of preorganization and cooperation has been designed for a superior capacity to capture low-concentration CO₂ by imide-based ionic liquids. By using this strategy, for the first time, an extremely high gravimetric CO₂ capacity of up to 22 wt % (1.65 mol mol^-1 ) and excellent reversibility (16 cycles) have been achieved from 10 vol. % of CO₂ in N₂ when using an ionic liquid having a preorganized anion. Through a combination of quantum-chemical calculations and spectroscopic investigations, it is suggested that cooperative interactions between CO₂ and multiple active sites in the preorganized anion are the driving force for the superior CO₂ capacity and excellent reversibility.