The development of
high-power density vanadium redox flow batteries
(VRFBs) with high energy efficiencies (EEs) is crucial for the widespread
dissemination of this energy storage technology. In this work, we
report the production of novel hierarchical carbonaceous nanomaterials
for VRFB electrodes with high catalytic activity toward the vanadium
redox reactions (VO
2+
/VO
2
+
and V
2+
/V
3+
). The electrode materials are produced through
a rapid (minute timescale) low-pressure combined gas plasma treatment
of graphite felts (GFs) in an inductively coupled radio frequency
reactor. By systematically studying the effects of either pure gases
(O
2
and N
2
) or their combination at different
gas plasma pressures, the electrodes are optimized to reduce their
kinetic polarization for the VRFB redox reactions. To further enhance
the catalytic surface area of the electrodes, single-/few-layer graphene,
produced by highly scalable wet-jet milling exfoliation of graphite,
is incorporated into the GFs through an infiltration method in the
presence of a polymeric binder. Depending on the thickness of the
proton-exchange membrane (Nafion 115 or Nafion XL), our optimized
VRFB configurations can efficiently operate within a wide range of
charge/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 commercial ones (additional electrode
costs < 100 € m
–2
) and shows EEs rivalling
the record-high values reported for efficient systems to date. Our
work remarks on the importance to study modified plasma conditions
or plasma methods alternative to those reported previously (e.g.,
atmospheric plasmas) to improve further the electrode performances
of the current VRFB systems.