Healable, Recyclable, and Upcyclable Gel Membranes for Efficient Carbon Dioxide Separation

Abstract Ionic liquids (ILs) are prized for their selective dissolution of carbon dioxide (CO 2 ), leading to their widespread use in ionogel membranes for gas separation. Despite their advantages, creating sustainable ionogel membranes with high IL contents poses challenges due to limited mechanical strength, leakage risks, and poor recyclability. Herein, we leverage copolymerized and supramolecularly bound ILs to develop ionogel membranes with high mechanical strength, zero leakage, and excellent self‐healing and recycling capabilities. These membranes exhibit superior ideal selectivity for gas separation compared to other reported ionogel membranes, achieving a CO 2 /nitrogen selectivity of 61.7 and a CO 2 /methane selectivity of 24.6, coupled with an acceptable CO 2 permeability of 186.4 Barrer. Additionally, these gas separation ionogel membranes can be upcycled into ionic skins for sensing applications, further enhancing their utility. This research outlines a strategic approach to molecularly engineer ionogel membranes, offering a promising pathway for developing sustainable, high‐performance materials for advanced gas separation technologies.