Interface Engineering of MOF Nanosheets for Accelerated Redox Kinetics in Lithium‐Sulfur Batteries

Abstract Modifying the separator is considered as an effective strategy for achieving high performance lithium‐sulfur (Li‐S) batteries. However, most modification layers are excessively thick, with catalytic active sites primarily located within the material′s interior. This configuration severely impacts Li + transport and the efficient catalytic conversion of polysulfides. Therefore, there is an urgent need to develop a multifunctional separator that integrates ultrathin design, catalytic activity, and ion sieving capabilities. Herein, we successfully linked TCPP(Ni) as a secondary ligand with Zr‐BTB nanosheets to create an ultra‐thin separator modification layer (Zr‐TCPP(Ni)) with efficient ion sieving and catalytic properties. The resultant multifunctional separators provide robust ion sieving capabilities that promote rapid Li + transport and intercept polysulfides shuttling. Therefore, The Zr‐TCPP(Ni)@PP cell maintains 70.0 % of its initial capacity after 600 cycles at a high rate of 3 C, while achieving an impressive areal capacity of 4.55 mA h cm −2 even with high sulfur content of 80 wt% at 0.5 C. This work provides valuable insights for rational design of MOF interface engineering in high energy density Li‐S batteries.