Carbon
paper electrodes are employed for different electrochemical
applications such as flow batteries and fuel cells. However, redox
reactions such as VO2+/VO2
+ in a
vanadium redox flow battery have been found to possess relatively
slow kinetics, resulting in significant activation losses during operation.
In this work, we demonstrate a facile and scalable method for nitrogen
doping of carbon paper electrodes, leading to superior electrocatalytic
activity. The effects of pyrolytic pretreatments under different conditions
on the performance of carbon paper were also studied to elucidate
their electrocatalytic activity from a material physics perspective,
using Raman spectroscopy. The 2D Raman signature, a specific feature
of the carbon structures, was employed to understand the effect of
different pretreatments on the Fermi level of the carbon papers, which
could help us elucidate their intrinsic electron transfer kinetics.
The full wave half-maximum of the 2D Raman band and the intensity
ratio I
2D/I
G were used to indicate changes in the Fermi level relative to the
untreated carbon paper, and hence the electrocatalytic properties,
which were confirmed using voltammetric techniques. Although heating
of carbon paper in air at around 500 °C (a widely used method
for activating carbon paper electrodes) increases the surface area
by about 16 times compared to untreated and nitrogen-doped carbon
paper, the latter exhibits superior electrocatalytic property for
VO2+/VO2
+, [Fe(CN)6]3–/4–, and the oxygen reduction reaction. This
study provides greater physical insights into different pretreatments
in terms of the energy barrier at the interface, which will aid the
pursuit for better carbon-based electrode materials and provide mechanistic
details about charge transfer processes at the interface.