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. Two for one: A novel preorganization and cooperation strategy has been designed for a superior capacity (22 wt %, 1.65 mol mol−1) to capture low‐concentration CO2 (10 vol. % CO2 in N2) by imide‐based ionic liquids with excellent reversibility (16 cycles). Multiple‐site cooperative interactions between CO2 and active sites in the preorganized anion are operative.