Calixarene‐Functionalized Porous Carbon Aerogels for Polysulfide Capture: Cathodes for High Performance Lithium‐Sulfur Batteries

Abstract A cage‐type composite was successfully prepared by attaching p ‐sulfonatocalix[4]arene to a porous activated carbon aerogel (ACA). The resulting composite showed a high specific surface area of 1620.7 m 2 g −1 and a high sulfur loading of 2.5 mg cm −2 . The calixarene is uniformly dispersed on the carbon spheres and efficiently captures polysulfides by interaction with the sulfonate groups. Meanwhile, the cross‐linked porous structure of the composite restricts the migration of polysulfides. The cathode delivers an outstanding electrochemical performance with an initial capacity of 1304.7 mAh g −1 at 0.2 C. Furthermore, it displays excellent long‐term cycling stability, maintaining 884.7 mAh g −1 after 300 cycles at 0.5 C. Density functional theory (DFT) adsorption calculations support the strong interaction between the calixarenes and polysulfides and reveal the capture mechanism.