Interlayer of Lithium‐Ion‐Sieving Spodumene Nanosheets Coupled with Co‐Loaded CNFs Enables High‐Performance Li‐S Batteries

Abstract A novel strategy combining Li + sieve nanosheets with cobalt‐loaded carbon fibers as interlayer is proposed to synergistically address the shuttle effect and slow reaction kinetics in Li‐S batteries. Natural spodumene nanosheets act as Li + sieves, enabling selective Li + transport while blocking lithium‐polysulfides (LiPSs). Carbon nanofibers enhance conductibility, while the Co nanoparticles adsorb and catalytically convert LiPSs. The cathode by using the modified separator displays an initial discharge‐capacity of 1265 mAh g −1 at 0.2 C, and 647 mAh g −1 at 4.0 C as a result of the synergy among the above‐designed favorable factors. Under conditions of high‐sulfur‐loading and low‐electrolyte‐content, the cathode retains 79.16% of its incipient capacity after 100 cycles. The adsorbed, catalytic, and blocking effects of this strategy on LiPSs are proved by Density Functional Theory and Bond Valence Sum approach. This research provides insights into designing novel, cost‐effective, and sustainable modified separators for Li‐S batteries with high stability.