Zwitterionic Separator Featured with Superdesolvating Properties for High Performance Lithium–Sulfur Batteries

Lithium–sulfur chemistry has greatly expanded the boundaries of lithium batteries, but the persistent parasitic reaction of soluble sulfur intermediates with lithium anode remains a primary challenge. Understanding and regulating the solvation structures of lithium ions (Li + ) and polysulfides (LiPSs) are critical to addressing the above issues. Herein, inspired by the natural superhydrophilic resistance to contamination, we developed a zwitterionic nanoparticles (ZWP) separator capable of modulating the solvated of Li + and LiPSs. The dense solvated layer induced by ZWP effectively prevents the movement of LiPSs without compromising Li + transport. Moreover, the high electrolyte affinity of the ZWP effectively results in minimizing the deposition of LiPSs on the separator. Furthermore, the structure of the solvated Li + and LiPSs is also unveiled by molecular simulation and nuclear magnetic resonance (NMR). In addition, in situ UV setup proved the ZWP separator can effectively suppress the shuttle of LiPSs. The restricted space formed by the tightly packed ZWP stabilizes the lithium deposition and regulates dendrite growth. Consequently, the performance of lithium–sulfur batteries is significantly improved and good cycle stability is maintained even at high sulfur loadings (5 mg cm –2 ). This contribution provides a new insight into the rational design of lithium–sulfur battery separators.