The value of mixed conduction for oxygen electroreduction on graphene-chitosan composites

Graphene-based electrocatalysts have been widely investigated for their excellent performance in electrocatalytic oxygen reduction. The surface chemistry of graphene-based electrocatalysts is important for developing more efficient fuel cells and metal-air batteries. In addition, the nanostructured gas-diffusion electrode (GDE) on which the electrocatalysts are loaded needs to be carefully tailored to facilitate mass transport (reactants and products). A polymer binder is often used to fabricate the GDE which means there is a need to optimize the ratio of binder to electrocatalyst. Herein we demonstrate the impacts of graphene-based GDE nanostructures on the efficiency of oxygen electroreduction by comparing a series of graphene/chitosan composites with varying compositions. In these nanostructured GDEs graphene acts as the electrocatalyst and chitosan as the binder. Our results illustrate a critical ratio of graphene to chitosan for enhanced electrocatalytic surface area and facilitated mass transport, while a continuous network for electron conduction is effectively established. We believe this work is an important piece of the puzzle to better understanding the electrode behavior of electrocatalysts consisting of graphene-like two-dimensional materials in oxygen reduction reaction.