Hexanuclear zirconium clusters of coordination supramolecular network with abundant catalyst sites for...

Lithium‑sulfur (LiS) batteries hold greater development potential than lithium-ion batteries because of their high theoretical specific capacity. Nevertheless, lithium‑sulfur batteries are severely limited by the lithium polysulfides (LiPSs) shuttle effect. Herein, a zirconium coordination supramolecular network (Zr₆-CSN) with hexanuclear zirconium clusters as metal nodes interconnected by 2,5-furandicarboxylate linkers is synthesized as a host for sulfur cathodes. The inherent mesoporous structure of Zr₆-CSN provides abundant exposed catalytic sites from zirconium clusters, enables rapid Li⁺ transport, and promotes uniform Li⁺ flux. This dual functionality effectively traps polysulfides and greatly enhances the kinetics of sulfur conversion reactions. Leveraging these synergistic advantages, lithium‑sulfur batteries with Zr₆-CSN-based cathodes exhibit a minimal capacity fading rate of 0.05 % per cycle over 1000 cycles at 1C. Under conditions of high sulfur loading (4 mg cm^-2) and lean electrolyte, the battery maintains excellent electrochemical stability (over 150 cycles). This research highlights the importance of incorporating multinuclear metal clusters with numerous active sites into coordination supramolecular networks to catalyze polysulfides reactions, opening new avenues for the future development of lithium‑sulfur batteries cathodes.