Developing A “Polysulfide‐Phobic” Strategy to Restrain Shuttle Effect in Lithium–Sulfur Batteries

Inspired by hydrophobic interface, a novel design of "polysulfide-phobic" interface was proposed and developed to restrain shuttle effect in lithium-sulfur batteries. Two-dimensional VOPO4 sheets with adequate active sites were employed to immobilize the polysulfides through the formation of a V-S bond. Moreover, owing to the intrinsic Coulomb repulsion between polysulfide anions, the surface anchored with polysulfides can be further evolved into a "polysulfide-phobic" interface, which was demonstrated by the advanced time/space-resolved operando Raman evidences. In particular, by introducing the "polysulfide-phobic" surface design into separator fabrication, the lithium-sulfur battery performed a superior long-term cycling stability. This work expands a novel strategy to build a "polysulfide-phobic" surface by "self-defense" mechanism for suppressing polysulfides shuttle, which provides new insights and opportunities to develop advanced lithium-sulfur batteries.