Rational design of self-supporting graphene - Polypyrrole/sulfur - Graphene sandwich as structural paper electrode for lithium sulfur batteries

Lithium sulfur batteries have been regarded as next-generation battery technology due to its high energy density, environmental benignity and abundance. However, the poor electric/ionic conductivity of sulfur limits the practical use of sulfur in an electrode. The main problem is the high solubility of long-chain polysulfides, which are the intermediates of the electrochemical processes in the liquid electrolyte. The dissolved polysulfide ions shuttle between the cathode and anode, thus causing precipitation of insulating Li 2 S 2 /Li 2 S on the surface of the electrode. The unavoidable phenomenon results in loss of active materials and fast capacity fading. In this regard, we show one simple method to prepare free-standing paper electrode used as cathode material for lithium sulfur batteries. Binder-free graphene-polypyrrole (PPy)/S-graphene (G-PPy/S-G) paper-like sandwich structural electrode was prepared by using the vacuum filtration method. In this structure, the unique graphene layers of sandwich-like framework not only serve as a conductive film, but also effectively block the diffusion of polysulfides, leading to suppression of the shuttle effect and low self-discharge behaviour. In addition, the middle layer, the PPy nanofibers can limit the diffusion of dissolved polysulfides due to the special bond with sulfur, and furthermore maintain the structural stability of the paper electrode because the nanofibers can serve as elastic springs to accommodate the huge volume changes in charging-discharging processes. When tested as cathode for Li-S batteries, the as-prepared sample G-PPy/S-G exhibits excellent electrochemical performance. We believe that our strategy could provide a useful pathway towards commercial utilizing of sulfur.