Self‐Adaptive Adsorption of Zwitterionic Polymer in Self‐assembly Lithium‐Sulfur Battery Cathode with 3D Dynamical Networks

Lithium‐sulfur (Li‐S) system is an attractive candidate for next‐generation energy storage due to its high specific energy. However, its commercialization faces significant challenges due to its low cycle stability induced by the shuttle effect and the volume expansion. Herein, these problems are solved simultaneously in a deformable and robust cathode with self‐adaptive adsorption (SAA) capacity. The self‐assembly cathode has deformable and self‐healing capacity due to its dynamic cross‐linked network. Furthermore, ionic chains in the network prepared by sulfonating the chitosan can interconvert between separated and bonding states driven by the charges. So, the SAA effect on the polysulfides exhibits optimal performance. And the electrochemical performance and cycling stability of the Li‐S battery are significantly enhanced, achieving a high capacity of up to 1156 mAh·g −1 at 1C and 80.3% capacity retention rate after 1500 cycles. This work presents a promising solution to the challenge of commercialization of the Li‐S batteries.