In
this paper, we report a simple two-step approach for the synthesis
of large graphene oxide (GO) sheets with lateral dimensions of ≈10
μm or greater. The first step is a pretreatment step involving
electrochemical exfoliation of graphite electrode to produce graphene
in a mixture of H
2
SO
4
and H
3
PO
4
. The second step is the oxidation step, where oxidation of
exfoliated graphene sheets was performed using KMnO
4
as
the oxidizing agent. The oxidation was carried out for different times
ranging from 1 to 12 h at ∼60 °C. Prepared GO batches
were characterized using a number of spectroscopy and microscopy techniques
such as X-ray diffraction (XRD), field emission scanning electron
microscopy (FE-SEM), transmission electron microscopy (TEM), Fourier-transform
infrared spectroscopy (FTIR), and UV–visible spectroscopy.
Raman and thermogravimetric analysis techniques were used to study
the degree of oxidation in the as-synthesized GO batches. The UV–visible
absorption spectrum showed an intense peak at 230 nm and an adjacent
band at 300 nm corresponding to π–π* and n−π*
transitions in all samples. Normalized FTIR plots were used to calculate
the relative percentages of oxygen-containing functional groups, which
were found to be maximum in GO (6 h). Boehm titration was used to
quantify the functional groups present on the GO surface. Overall
GO sheets obtained after 6 h of oxidation, GO (6 h), were found to
be the best. XRD pattern of GO (6 h) revealed a characteristic peak
at 2θ = 8.88°, with the corresponding interplanar spacing
between the layers being 0.995 nm, which is among the best with respect
to the previous methods reported in the literature. Raman spectroscopy
showed that the degree of defect (
I
D
/
I
G
) area ratio for GO (6 h) was 1.24, which is
higher than that obtained for GO (1.18) prepared by widely used Marcano’s
approach.