A comprehensive study on effect of carbon nanomaterials as conductive additives in EDLCs

Abstract

This study performs a comprehensive investigation to objectively analyze the effects of various carbon nanomaterials using as conductive additives (5 wt%) in activated carbon (AC) based electrodes for electrical double-layer capacitors (EDLCs). A variety of carbon nanomaterials including carbon black (CB), single-walled carbon nanotubes (SWCNT), graphene nanoplatelets (GNP), fullerenes (C60), and activated carbon nanofibers (ACNF) are considered in this work as they provide a diverse combination of intrinsic properties such as specific surface area, conductivity, micro-mesoporous structures, and geometry of nanomaterials. These additives are incorporated into freestanding carbon electrodes, and their EDLC performance in a neutral aqueous electrolyte is investigated by means of electrochemical measurements. The findings from this work provide useful insight into how the properties of various carbon nanomaterials influence EDLC performance in different aspects such as capacitive behavior, resistivity, performance at different current densities, charge propagation properties, and stability over long-term cycling. The results show that each carbon additive has its own strengths and limitations for different performance parameters considered. The unfavorable material properties of C60 cause a significant decrease in capacitance at high current density, leading to the lowest device performance incorporated with C60 as additives. While GNP and SWCNT show high crystallinity, low ID/IG ratios, the EDLCs still exhibit decreased specific capacitance and moderate energy densities due to their relatively limited specific surface area and high resistivity of the resultant composite electrodes compared to the pristine AC. The CB additives-based samples demonstrate the highest conductivity of dry electrodes and low equivalent series resistance (ESR) in EDLCs. On the other hand, a reduction in capacitance at high current densities and material degradation during long-term cycling are observed for CB samples, which could be attributed to the high dispersibility of CB causing limited interparticle voids and thus increasing diffusion resistance. In contrast, the use of ACNFs significantly reduces the diffusion resistance and improves the cyclic stability compared with CB based samples due to the advantages of larger specific surface area and superior micro-mesoporous structures of ACNFs. In particular, EDLCs with ACNFs demonstrate an increase in specific capacitance and energy density by 99 % and 76 %, respectively compared to CB based EDLCs at a current density of 20 A/g. This work elucidates the complex interplay between carbon nanomaterials using as additives and corresponding EDLC performance. These results provide important information to the community for future development of new energy conversion and storage devices.