Realizing High-Performance Sulfur Cathodes through a Self-Healing and Confining Strategy

Shuttling effect and mechanical pulverization are main challenges impeding the practical application of sulfur cathodes for high energy-density Li–S batteries. Here we demonstrate that such issues can be effectively addressed by embedding sulfur microparticles into a self-healable and polysulfide-confining binder comprising of trithiocarbonate, carboxylic acid, and amino functionalities. In the charge/discharge process, the binder autonomously integrates the pulverized sulfur particles together via its excellent self-healability and good extendibility, but also effectively confines the generated polysulfides by its polar functionalities. Consequently, the resulting sulfur cathodes deliver high reversible capacity, excellent rate capability, and good cycling stability. This self-healing and confining strategy provides a novel insight into the structural collapse and shuttle effect of sulfur cathodes.