Multifunctional Carbonized Polyimide‐Supported PEDOT:PSS/Ni‐TABQ Interlayer for Efficient Polysulfide Regulation in Lithium–Sulfur Batteries

A lightweight, flexible carbonized polyimide (C‐PI) membrane serves as the supporting backbone and is coated with a composite layer of nickel‐coordinated tetraaminobenzoquinone (Ni‐TABQ) and poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS, abbreviated as P:PSS). This architecture yields a multifunctional interlayer,denoted as (P:PSS/Ni‐TABQ)@C‐PI, which synergistically integrates physical barrier functionality, chemical adsorption, and catalytic activity. Positioned between the cathode and the separator, this interlayer also functions as an additional current collector. The dual catalytic sites derived from Ni‐TABQ on the P:PSS surface provide abundant nucleation sites for sulfur and lithium sulfide (Li 2 S), along with reactive interfaces for polysulfides, thereby substantially enhancing the utilization of active materials and the overall electrochemical performance. At 0.5 C, the cell incorporating the (P:PSS/Ni‐TABQ)@C‐PI interlayer delivers an initial specific capacity of 1237 mAh g −1 and retains 1133 mAh g −1 after 500 cycles, corresponding to a capacity retention of 91.59% and demonstrating its exceptional long‐term cycling stability.