Graphene-containing flowable electrodes for capacitive energy storage

High conductivity and extended particle contacts are required for rapid charge percolation in flowable electrodes. In this study, carbon spheres (CS) were wrapped by highly conductive reduced graphene oxide sheets (rGO) to address these issues. Various compositions of the conductive, 3D interconnected hybrid materials (rGO@CS) were synthesized by a hydrothermal method. Synergistic effects of both materials were utilized where CS served to minimize the sheet stacking for better flowability of the suspensions, and wrapped rGO sheets enabled higher conductivity for fast charge transport throughout the suspension network. When tested as flowable electrodes, the composition with a 1:2 ratio of GO to CS exhibited the highest capacitance of 200 F/g and an improved rate performance. The improved performance is attributed to the fast charge transport in the suspension network due to higher conductivity and enhanced connectivity of the active material particles. Optimized electrodes were also examined in a flow mode which yielded a capacitance of 45 F/g.