Sulfur-Doped Graphene Derived from Cycled Lithium-Sulfur Batteries as a Metal-Free Electrocatalyst for the Oxygen Reduction Reaction

Heteroatom-doped carbon materials have been extensively investigated as metal-free electrocatalysts to replace commercial Pt/C catalysts in oxygen reduction reactions in fuel cells and Li-air batteries. However, the synthesis of such materials usually involves high temperature or complicated equipment. Graphene-based sulfur composites have been recently developed to prolong the cycling life of Li-S batteries, one of the most attractive energy-storage devices. Given the high cost of graphene, there is significant demand to recycle and reuse graphene from Li-S batteries. Herein, we report a green and cost-effective method to prepare sulfur-doped graphene, achieved by the continuous charge/discharge cycling of graphene-sulfur composites in Li-S batteries. This material was used as a metal-free electrocatalyst for the oxygen reduction reaction and shows better electrocatalytic activity than pristine graphene and better methanol tolerance durability than Pt/C.