Switchable encapsulation of polysulfides in the transition between sulfur and lithium sulfide

Abstract Encapsulation strategies are widely used for alleviating dissolution and diffusion of polysulfides, but they experience nonrecoverable structural failure arising from the repetitive severe volume change during lithium−sulfur battery cycling. Here we report a methodology to construct an electrochemically recoverable protective layer of polysulfides using an electrolyte additive. The additive nitrogen-doped carbon dots maintain their “dissolved” status in the electrolyte at the full charge state, and some of them function as active sites for lithium sulfide growth at the full discharge state. When polysulfides are present amid the transition between sulfur and lithium sulfide, nitrogen-doped carbon dots become highly reactive with polysulfides to form a solid and recoverable polysulfide-encapsulating layer. This design skilfully avoids structural failure and efficiently suppresses polysulfide shuttling. The sulfur cathode delivers a high reversible capacity of 891 mAh g −1 at 0.5 C with 99.5% coulombic efficiency and cycling stability up to 1000 cycles at 2 C.