Blocking Polysulfides and Facilitating Lithium-Ion Transport: Polystyrene Sulfonate@HKUST‑1 Membrane for Lithium–Sulfur Batteries

Minimizing the shuttle effect of polysulfides (PS) is crucial for practical applications of lithium–sulfur (Li–S) batteries. However, the trade-off between effective suppression of the shuttle effect and fast redox reaction kinetics is inevitable for separator-based Li–S batteries. Herein, via a self-confined solid-conversion process, we develop a polystyrene sulfonate (PSS)-threaded well-intergrown HKUST-1 (Cu3(BTC)2) (BTC: 1,3,5-benzenetricarboxylic acid)-coated Celgard separator (PSS@HKUST-1/Celgard, PHC) for high-performance Li–S batteries. The PHC membrane favors the interception and accommodation of long-chain PS. Notably, enormous sulfonate groups of the three-dimensional PSS networks in PSS@HKUST-1 membrane significantly facilitate lithium-ion transport, which guarantee fast redox kinetics. The PHC separator demonstrates efficient inhibition of PS (i.e., 4 orders of magnitude lower in PS permeation rate) with fast Li+ transportation (i.e., 71% higher in ionic conductivity) than the Celgard separator. When applying the PHC membrane in Li–S batteries with conventional sulfur/super P carbon cathode, highly reversible capacity with an average fading rate of 0.05% per cycle is maintained for 500 cycles at 0.5 C, excellent rate performance up to 5 C, and high areal capacity over 7 mA h cm–2 are also achieved. This work paves a new way for addressing the trade-off between suppressing the PS shuttle effect and fast kinetic reaction for separator-based Li–S batteries.