Polyoxometalate-Cyclodextrin-Based Cluster-Organic Supramolecular Framework for Polysulfide Conversion and Guest-Host Recognition in Lithium-sulfur Batteries

Developing polyoxometalate-cyclodextrin cluster-organic supramolecular framework (POM-CD-COSF) still remains challenging due to an extremely difficult task in rationally interconnecting two dissimilar building blocks. Here we report an unprecedented POM-CD-COSF crystalline structure produced through the self-assembly process of a Krebs-type POM, [Zn-2(WO2)(2)(SbW9O33)(2)](10-), and two & beta;-CD units. The as-prepared POM-CD-COSF-based battery separator can be applied as a lightweight barrier (approximately 0.3 mg cm(-2)) to mitigate the polysulfide shuttle effect in lithium-sulfur batteries. The designed Li-S batteries equipped with the POM-CD-COSF modified separator exhibit remarkable electrochemical performance, attributed to fast Li+ diffusion through the supramolecular channel of & beta;-CD, efficient polysulfide-capture ability by the dynamic host-guest interaction of & beta;-CD, and improved sulfur redox kinetics by the bidirectional catalysis of POM cluster. This research provides a broad perspective for the development of multifunctional supramolecular POM frameworks and their applications in Li-S batteries.