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The development of high-power density vanadium redox flow batteries (VRFBs)with high energy efficiencies (EEs) is crucial for the widespread disseminationof this energy storage technology. In this work, we report the production ofnovel hierarchical carbonaceous nanomaterials for VRFB electrodes with highcatalytic activity toward the vanadium redox reactions (VO2+/VO2+ and V2+/V3+).The electrode materials are produced through a rapid (minute timescale)low-pressure combined gas plasma treatment of graphite felts (GFs) in aninductively coupled radio frequency reactor. By systematically studying theeffects of either pure gases (O2 and N2) or their combination at different gasplasma pressures, the electrodes are optimized to reduce their kineticpolarization for the VRFB redox reactions. To further enhance the catalyticsurface area of the electrodes, single-/few-layer graphene, produced by highlyscalable wet-jet milling exfoliation of graphite, is incorporated into the GFsthrough an infiltration method in the presence of a polymeric binder. Dependingon the thickness of the proton-exchange membrane (Nafion 115 or Nafion XL), ouroptimized VRFB configurations can efficiently operate within a wide range ofcharge/discharge current densities, exhibiting energy efficiencies up to 93.9%,90.8%, 88.3%, 85.6%, 77.6%, and 69.5% at 25, 50, 75, 100, 200, and 300 mA cm-2,respectively. Our technology is cost-competitive when compared to commercialones (additional electrode costs < 100 euro m-2) and shows EEs rivalling therecord-high values reported for efficient systems to date. Our work remarks onthe importance to study modified plasma conditions or plasma methodsalternative to those reported previously (e.g., atmospheric plasmas) to improvefurther the electrode performances of the current VRFB systems.

Graphene-Based Electrodes in a Vanadium Redox Flow Battery Produced by Rapid Low-Pressure Combined Gas Plasma Treatments