Ionically Cross-Linked Polymers as Asymmetric Gel Polymer Electrolytes for Enhanced Cycle Performance of Lithium-Sulfur Batteries.

Two thermoplastic triblock copolymers of poly(ε-caprolactone)-based acidic (PCL-A) and basic (PCL-B) polymers are synthesized by atom transfer radical polymerization. PCL-A and PCL-B are sequentially electrospun on a sulfur electrode and then ionically cross-linked by an acid-base reaction via hot pressing at 70 °C, which is confirmed by infrared (IR) spectroscopy. The cross-linked PCL-A/PCL-B-electrospun sulfur electrode is assembled as a lithium-sulfur battery with an asymmetric gel polymer electrolyte. The cross-linked polymer is swollen by a liquid electrolyte to form an asymmetric gel polymer electrolyte. The cyclic voltammetry results indicate that the asymmetric gel polymer electrolyte can suppress the dissolution of lithium polysulfides (Li2Sn) into the electrolyte. Furthermore, the lithium-sulfur battery with the asymmetric gel polymer electrolyte exhibits enhanced cycle-life performance.