Permselective SPEEK/Nafion Composite-Coated Separator as a Potential Polysulfide Crossover Barrier Layer for Li–S Batteries

Minimizing the shuttle effect by constraining polysulfides to the cathode compartment and activating the passive layer between cathode and separator are highly important for improving the Li–S cell performance, Coulombic efficiency, and cycle life. Here, we report a submicron thin coating of permselective sulfonated poly(ether ether ketone) (SPEEK) composite layer on the separator that would reduce polysulfide crossover, imparting a significant improvement in cycle life. It is observed that SPEEK increases the stability, and adding Nafion improves the capacity value. Among different ratios of Nafion and SPEEK (25:75, 50:50, and 75:25), the composite with a SPEEK/Nafion ratio of 50:50 showed a controlled shuttle effect with a stable cell capacity of 600 mA h g–1 up to 300 cycles. This modified separator with permselective coatings not only reduces the polysulfide shuttle but also improves the wettability and interfacial contact, which results in an improvement in average cell potential and lithium diffusivity. It is demonstrated here that the combination of functional (ionomer coating on separator) and nonfunctional (extra cathode layer) physical barriers effectively suppresses the polysulfide crossover and improves the electrochemical performance of Li–S batteries. The cell shows an initial capacity of 1300 mA h g–1 and a capacity retention of 650 mA h g–1 over 500 cycles with a 6 mg/cm2 sulfur loading.