Three-dimensional mesoporous graphene-modified carbon felt for high-performance vanadium redox flow batteries

In our contribution, we study the synthesis of three-dimensional (3D) mesoporous graphene-modified carbon felt (MG-CF) via a facile self-assembly interaction method for the application of mesoporous graphene (MG) as an electrocatalyst for vanadium redox flow batteries (VRFBs). The MG loading on carbon felts (CFs) is systematically varied for optimal performance. Morphological and spectroscopic studies indicate that the MG exhibits a wrinkled configuration over the relatively smooth surface of the pristine CF (P-CF), and shows an increase in sp2/sp3 ratio. Nitrogen adsorption/desorption isotherms exhibit increase in specific surface area and porosity with increasing MG loading. Analysis of cyclic voltammetry and electrochemical impedance spectroscopy measurements reveal MG–CF–4 (4 wt% MG) possess the best electrochemical performance towards V2+/V3+ and VO2+/VO2+ redox couples, attributing to optimal 3D MG strongly anchoring on the CF, enhancing conductivity, specific surface area, and electrochemical activity. In addition, charge/discharge measurements exhibit a high energy efficiency (EE) of 76.5% at 100 mA cm−2 in MG–CF–4, compared to P-CF (66.2). Moreover, a higher energy efficiency (61.6%) and voltage efficiency (62.6) is obtained at a high current density of 175 mA cm−2 with MG–CF–4 electrode. Furthermore, MG–CF–4 shows excellent stability and rate capability (EE of 74.9% and VE of 77.5 after 100 charge/discharge cycles at 100 mA cm−2), demonstrating superior performance of the modified electrodes during the vanadium ions redox reaction under acidic conditions. •Self-assembly interaction to modify electrode with 3D mesoporous graphene.•Significant enhancement of V2+/V3+ and VO2+/VO2+ redox reversibility and kinetics.•Excellent performance attributed to 3D wrinkled mesoporous graphene structures.•Increased specific surface area, pore volume, and electrical conductivity.•MG–CF–4 (4 wt% MG) improves VRFB EE from (66.2–76.5) % at 100 mA cm−2.