High-density graphene/single-walled carbon nanohorn composite supercapacitor electrode with high volumetric capacitance

Abstract

The low density of porous carbon nanomaterials for supercapacitor electrodes has limited their widespread application, despite their ultra-high gravimetric capacitance. In this work, we successfully prepared highly densified composite electrodes of graphene and single-walled carbon nanohorns (SWCNHs) using a simple spray-drying method that is suitable for mass production. To prepare the high-density composite electrodes, water-based mixtures of oxidized SWCNHs (NHOs) and graphene oxides (GOs) were spray-dried in heated air; after spray-drying, GOs dispersed in water were agglomerated in spherical clusters containing NHO nanoparticles. The reduced spray-dried GO/NHO (rS-GO/NHO) composite electrodes exhibited an extremely high bulk density of 1.23 g.cm(-3), which is almost double that of commercial activated carbon (AC) and reduced NHO (r-NHO) electrodes, and three times higher than that of rS-GO electrodes. Of the materials tested, the rS-GO/NHO composite electrode had the highest volumetric capacitance (80 F.cm(-3) at 1 mA.cm(-2)) and a low sheet resistance (0.005 Omega.sq.(-1)), which are far superior to those of commercial AC (57 F.cm(-3) at 1 mA.cm(-2) and 0.293 Omega.sq.(-1), respectively), without the need for a conductive material, such as carbon black. We expect that these high-density graphene/SWCNH composite electrodes with high volumetric capacitances can be substituted for commercial AC materials in energy storage devices, such as supercapacitors.