Exquisitely constructing hierarchical carbon nanoarchitectures decorated with sulfides for high-performance Li-S...

The sluggish reaction kinetics and notorious shuttle effect of polysulfides significantly hinder the practical application of lithium-sulfur batteries (LSBs). Therefore, polysulfides are anchored and their conversion reactions are catalyzed to enhance the performance of LSBs. Herein, an exquisite hierarchical carbon nanoarchitecture decorated with sulfides is designed and introduced into LSBs. Systematic experiments show that the nanoarchitecture not only enables rapid electron/ion migration but also functions as an active catalyst to increase polysulfide conversion, thus effectively reducing the shuttle effect. As a result, LSBs with the nanoarchitecture modified separator exhibited outstanding rate capacity (724.9 mA h g^-1 at 5C), low self-discharge capacity loss (4.1% capacity loss after 72 h), and exceptional reversible capacity (1518.3 mA h g^-1 at 0.1C and 25.6% capacity loss after 100 cycles). Through the design of a multifunctional separator, this study offers an effective way to minimize the shuttle effect and speed up redox conversion. The strategy of constructing nanoarchitectures provides an innovative route for hierarchical heterocatalyst design for LSBs.