Green functionalization for chelating ligand-like and π-conjugated active sites on carbon nanotubes and its use for vanadium redox flow batteries

Abstract

An imide bond-based functional group is proposed for the catalyst's active site in vanadium redox flow batteries (VRFBs). Based on the functional group's inherent property produced by the optimized process, the catalytic activity toward vanadium ion redox reaction (VIRR) on both sides was increased sixfold without adversely affecting VIRR reversibility in comparison to the raw material, carboxylic acid-functionalized carbon nanotubes. These advantages were attributed to the imide bond-based functional groups acting as a chelating ligand to form strong interactions with vanadium redox couples while also inducing facile electron transfer by the π-conjugated bonds, resulting in increased catalytic activity and reversibility. Moreover, the treatment used an eco-friendly process comprising low-cost precursors (citric acid and urea) and mild conditions (80 °C, 2 h), thereby improving the commercial availability of VRFBs. In VRFB driving tests, the fabricated electrode outperformed the electrode with a polymer-like structure in terms of catalytic activity and long-term stability due to leaching of the active sites from the latter. Overall, the proposed catalyst could be a practical option for enhancing VRFB performance based on a low-cost and eco-friendly treatment method.