Trapping of Polysulfides with Sulfur-Rich Poly Ionic Liquid Cathode Materials for Ultralong-Life Lithium-Sulfur Batteries.

Sulfur-rich polymers synthesized by inverse vulcanization are promising cathodes for Li-S batteries and can suppress the shuttle effect to improve the cycling properties of Li-S batteries. However, developing a sulfur-rich copolymer with new chemical functionality to enhance performance of Li-S batteries remains a huge challenge. In this report, a sulfur-rich polymer cathode containing ionic liquid segments named poly(sulfur-co-1-vinyl-3-allylimidazolium bromide) [poly(S-co-DVIMBr)] was obtained by the inverse vulcanization of S with DVIMBr and used as cathode for the first time. This sulfur-rich poly ionic liquid cathode showed effective suppression of the shuttle effect through joint effects of the stable chemical bonding of C-S and strong cation absorption for lithium polysulfides, which was confirmed by DFT calculations. In particular, the Li-S cell with poly(S-co-DVIMBr) cathode delivered high capacity retention of 90.22 % even over 900 cycles. Developing sulfur-rich poly ionic liquids may provide a new strategy of introducing the functional groups with cations into the cathode materials for suppressing the shuttle effect and improving the performance of Li-S batteries.