One-pot synthesis of graphene-sulfur composites for Li-S batteries: influence of sulfur precursors

Abstract

Lithium-sulfur (Li-S) batteries are postulated as next-generation electrochemical energy storage devices due to their increased storage capabilities. However, challenges persist from the polysulfide-shuttle effect at the cathode. Soluble sulfur-based species in the cathode cross over to the lithium anode through the separator leading to fading capacity with cycling. This has spurred continuous effort by the scientific community to develop novel cathodes where sulfur species can affix better. A conductive nanostructured graphene network is a suitable candidate that can serve as a scaffold for holding sulfur nanoparticles. Here, a one-pot synthesis of chemically reduced graphene oxide networks prepared from easily accessible graphene oxide is demonstrated. The solution-based method simply allows for impregnation of the graphene oxide network with sulfur nanoparticles through a careful manipulation of pH of the chemical environment. Two routes were chosen for the precipitation of such sulfur nanoparticles: firstly, the dissolution of sulfur in sodium hydroxide into polysulfides followed by acidification and secondly, the acidification of sodium thiosulfate from alkaline media into sulfur nanoparticles. Both graphene oxide materials from the two routes were treated with sodium borohydride to achieve conductive graphene. The second route, with the sulfur nanoparticles derived from the acidification of sodium thiosulfate with chemically reduced graphene oxide, demonstrated favorable electrochemical behavior, showing promise as electrode material for Li-S batteries.