An integrated flexible film as cathode for High-Performance Lithium-Sulfur battery

Poor cycling stability and low volumetric capacity of sulfur cathode prevents practical application of Lithium-sulfur (Li-S) batteries. Herein, we demonstrate a strategy to address the two drawbacks of sulfur cathode by synthesizing a compact and flexible film cathode with bilayer structure using a two-step vacuum filtration method. Two layers make up the sulfur cathode, active layer (sulfur-acethlene black (SC) spheres) and barrier layer (three dimensional MnO₂-graphene oxide-multi-walled carbon nanotubes (MnO₂-GO-CNTs) composites), which are integrated together by reduced graphene oxide (rGO) through self-binding. The rGO sheets provide an electrical conductive framework and a stable architecture to accommodate volume changes of sulfur. SC spheres stacked orderly between the rGO layers facilitate fast Li⁺ storage and energy release. Polar MnO₂-GO-CNTs composites with large specific surface area have not only afforded efficient sites for chemically binding polysulfides, but also provided fast electron transfer for accelerating polysulfides redox reaction. Consequently, the integrated film cathode exhibits an unprecedented cycling stability of ~0.0279% capacity decay per cycle over more than 600 cycles at 1C and high volumetric capacity of 1021.9 Ah L^-1 at 2C. Meanwhile, a foldable Li-S battery based on this flexible cathode is fabricated and shows excellent mechanical and electrochemical properties. The integrated flexible sulfur cathode of this study sheds light on the design strategies for application in flexible high volumetric capacity system.