Sulfonated covalent organic framework modified separators suppress the shuttle effect in lithium-sulfur batteries

Lithium-sulfur batteries (LSBs) have gained intense research enthusiasm due to their high energy density. Nevertheless, the 'shuttle effect' of soluble polysulfide (a discharge product) reduces their cycling stability and capacity, thus restricting their practical application. To tackle this challenging issue, we herein report a sulfonated covalent organic framework modified separator (SCOF-Celgard) that alleviates the shuttling of polysulfide anions and accelerates the migration of Li⁺ ions. Specifically, the negatively charged sulfonate can inhibit the same charged polysulfide anion through electrostatic repulsion, thereby improving the cycle stability of the battery and preventing the Li-anode from being corroded. Meanwhile, the sulfonate groups may facilitate the positively charged lithium ions to pass through the separator. Consequently, the battery assembled with the SCOF-Celgard separator exhibits an 81.1% capacity retention after 120 cycles at 0.5 C, which is far superior to that (55.7%) of the battery with a Celgard separator. It has a low capacity degradation of 0.067% per cycle after 600 cycles at 1 C, and a high discharge capacity (576 mAh g⁻¹) even at 2 C. Our work proves that the modification of a separator with a SCOF is a viable and effective route for enhancing the electrochemical performance of a LSB. (paper)