Fullerenes, Nanotubes and Carbon Nanostructures

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Managing the degree of exfoliation and number of

graphene layers using probe sonication approach

Amanpreet Kaur & Ravi Chand Singh

To cite this article: Amanpreet Kaur & Ravi Chand Singh (2017) Managing the degree of
exfoliation and number of graphene layers using probe sonication approach, Fullerenes, Nanotubes
and Carbon Nanostructures, 25:5, 318-326, DOI: 10.1080/1536383X.2017.1292254

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FULLERENES, NANOTUBES AND CARBON NANOSTRUCTURES
2017, VOL. 25, NO. 5, 318–326
http://dx.doi.org/10.1080/1536383X.2017.1292254

Managing the degree of exfoliation and number of graphene layers using probe
sonication approach
Amanpreet Kaur and Ravi Chand Singh
Department of Physics, Guru Nanak Dev University, Amritsar, Punjab, India

ABSTRACT ARTICLE HISTORY

We have demonstrated a fast, versatile, and scalable approach to synthesize high-quality few layer Received 1 February 2017
graphene sheets with low defect ratio and high crystallinity produced from exfoliation of graphite flakes in Accepted 3 February 2017
DMF by using probe sonication. The effect of sonication time on degree of exfoliation and number of KEYWORDS
graphene layers has been fully investigated. The degree of exfoliation of graphene sheets as a function of Graphite flakes; Graphene;
sonication time has been successfully analyzed by XRD, UV-Vis spectroscopy, TEM, and BET studies. The Liquid phase exfoliation;
morphological changes at different sonication times have also been observed by SEM. A structural and Probe sonication
defect characterization of graphene sheets has been discussed in detail by Raman spectroscopic
technique. The shift in position of 2D Raman band and its de-convolution provided information about
formation of multi to few layer graphene sheets with sonication. Moreover, Raman results are highly
consistent with TEM studies as per number of graphene layers is concerned.

1. Introduction
Graphene, a two-dimensional carbon-based material having hex-
agonal lattice structure of sp2-bonded carbon atoms owing to its
unique nanostructure (1), electrical (2), and thermal properties
(3) combined with its elasticity (4,5) and mechanical stiffness (6)
has set the research and development sectors ablaze with interest
in the recent times (7). Basically, there are two different
approaches i.e. Top–down and bottom up for the synthesis of
graphene sheets. Bottom up methods can be accomplished by
high temperature reduction of SiC substrates under ultra-high
vacuum and chemical vapor deposition (CVD) (6). But, there
are some drawbacks of these methods. First, the synthesized gra-
phene samples prepared by above mentioned methods are sub
micrometer in scale and composed of multitude of domains (8).
Second, they demand high temperature, a vacuum environment
and expensive equipment which increase fabrication cost (6).
Therefore, the most efficient and inexpensive method for gra-
phene synthesis should be highly encouraged.
Alternatively, top–down approach can be realized by mechan-
ical cleavage of graphite using scotch tape to produce graphene.
Though, graphene obtained by this method is free from struc-
tural defects, but it is difficult to scale up this method for mass
production due to its low yield and fragmentation effects (8).
A large volume of literature is available on dispersion and
exfoliation of GO (graphene oxide) which possesses graphene
like sheets, but chemical functionalization of GO sheets with
epoxides and hydroxyl groups deprives its similarity with gra-
phene. Although graphene oxide (GO) had been reduced by
using various reducing agents in order to remove oxygen func-
tional groups, still it leaves a significant number of structural
defects which are introduced by oxidation of graphite using
Hummers method (10). These type of structural defects
degrade the original conjugated structure of graphene, band
structure, and hence it‘s electronic properties (8).
Recently, various studies of surfactant assisted liquid phase
exfoliation via mild ultrasonication technique has been
reported to synthesize graphene dispersions. But, there are
some issues such as use of expensive surfactants, prolonged
sonication periods and stability of dispersions which limit the
production of defect free graphene (9).
Herein, we have followed another top–down approach i.e.
sonication-assisted liquid phase exfoliation of graphite which is
considered as the promising route for synthesis of high-quality
graphene sheets with good crystallinity and low defect densities
(11). This method is the most viable approach for utilizing
excellent properties of graphene for composite synthesis, thin
film coatings, energy storage materials, catalysis, and gas sens-
ing applications (12–15).
In the present report, we have adopted a simple, efficient, and
surfactant-free approach to exfoliate graphite flakes by the appli-
cation of mechanical forces achieved through a high intensity
probe-sonication in diprotic solvent DMF(N,N-dimethylforma-
mide) to produce graphene sheets. The effect of sonication time
on the degree of exfoliation and number of graphene layers has
been investigated. Further, optimization of sonication time for
the synthesis of high quality few layered graphene sheets has
been studied in detail. Also, we have elaborated the mechanism
of solvent-assisted mechanical exfoliation of bulk graphite into
graphene sheets. In addition, time taken to exfoliate one gra-
phene layer has been calculated in this report.

CONTACT Ravi Chand Singh ravichand.singh@gmail.com Department of Physics, Guru Nanak Dev University, Amritsar, Punjab, India.
Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lfnn.
© 2017 Taylor & Francis Group, LLC

1.1. Mechanism of organic solvent-assisted exfoliation via
probe sonication
The detailed mechanism of exfoliation of graphene layers is as
follows:
Vander Waals (VdW) attractions are the most predominant
forces between stacked layers of graphite. These VdW interac-
tions must be overcome in order to exfoliate layers completely.
This can be accomplished by intercalation of organic solvent
(super critical fluid) into graphitic layers followed by introduc-
tion of mechanical forces which are achieved through probe
sonication (11). As the ultrasonic waves travel through
medium, solvent molecules compress and stretch i.e. starts
oscillating about their mean positions resulting into formation
of high pressure regions (compression) and negative pressure
regions (stretching). At a certain point, when negative pressure
is not large enough to hold liquid molecules intact, then break-
down of liquid takes place forming voids or cavitation bubbles.
These cavitation bubbles will collapse violently in high pressure
regions and behave like micro reactors, produce local tempera-
ture of several thousand degrees, and high pressure of several
hundred atmosphere which is sufficient to overcome the inter-
sheet attractive forces and hence induces exfoliation (16). The
schematic representation of exfoliation of graphite flakes into
graphene sheets using probe sonication is depicted in Figure 1.
1.2. Choice of solvent
The key requirement for suitable solvent is that interactions
between solvent and graphene must be comparable to interactions
between stacked layers of graphite (17). Mostly, the solvents whose
surface tension matches with that of graphene i.e. g D 40 m J m¡2
are the ideal solvents for well dispersion of graphite flakes and gra-
phene, as they minimize the interfacial tension between solvent
and graphene (8). That is why we have adopted DMF whose g D
37.1 m J m¡2 as a solvent to disperse graphite flakes.
If ET is total energy required for exfoliation, E vwf is Vander
Waal forces between layers of graphite and d E is change in sur-
face energies of graphene (or graphite) and solvent. Then, the
Figure 1. The schematic representation of exfoliation of graphite in DMF using
probe sonication.
FULLERENES, NANOTUBES AND CARBON NANOSTRUCTURES 319
total energy required to exfoliate graphite is the sum of Vander
Waal forces and change in surface energies expressed as (18):
ET D Evwf C .EG ¡ ES / (1)
ET D Evwf C dE (2)
2. Experimental
Three samples have been prepared by dispersing 1.0 gm graphite
flakes (purchased from Sigma-Aldrich) in 30 mL of DMF (by Loba
Chemie) solvent followed by probe sonication, using probe sonica-
tor PKS - 750 F has working frequency 20-25 kHz, probe diameter
0.5 inches, at different sonication times of 30, 60, and 90 min
labeled as PS-30, PS-60, and PS-90, respectively. The total amount
of energy delivered to the dispersions was calculated as E D P £ T,
where P is power used which is 40% of total power and T is sonica-
tion time (in sec). The energy delivered to dispersions comes out to
be 0.54 £ 106 J, 1.08 £ 106 J, and 1.62 £ 106 J for sample PS-30,
PS-60, and PS-90, respectively. The dispersions were kept for
30 days at ambient conditions in order to allow the settlement of
large particles. The supernatant was carefully collected for further
microscopy characterizations. X-ray diffraction (XRD) patterns
were recorded on X-ray diffractometer (D8 Focus, Bruker, Ger-
many) in the 2u range of 10 ¡ 50
using Cu Ka radiation (λ »
0.154 nm). The Raman spectra were recorded using an In Via
Reflex micro-Raman spectrometer (Renishaw) with a 50 £ objec-
tive lens using argon laser excitation of 514.5 nm operating at
0.1 m W. The UV- visible spectra were obtained on Shimadzu UV
3600 spectrophotometer using quartz cuvettes. Transmission elec-
tron microscopy (TEM) was carried out on a JEOL JEM 2100
microscope operated at 200 kV by using a holey carbon coated cop-
per grid. Carl Zeiss SUPRA 55 apparatus operating at 15- 30 kV
under vacuum was used to record SEM images of sheets.
For XRD, Raman and SEM studies the liquid dispersions (of
supernatant) were made to deposit on glass substrates by drop
casting method and allow them to dry at 154
C (b.pt of DMF).
Brunauer–Emmett–Teller (BET) surface area of synthesized
graphene samples was obtained by N2 adsorption / desorption
isotherms using Micromeritics ASAP 2020.
3. Results and discussions
3.1. XRD characterization
Figure 2 shows the diffraction patterns of (a) PS-30 (b) PS-60
(c) PS-90. The XRD patterns of all the exfoliated graphene sam-
ples show a characteristic peak of (002) which confirms the for-
mation of graphene (19). It is noticed that 2u value of (002)
reflection of sample PS-90 is slightly shifted towards smaller
angle relative to PS-60 and PS-30 which is attributed to increase
in inter-layer spacing of graphene.
The inter-layer d spacing has been calculated using Bragg‘s
diffraction law (20):
2d sin u D nλ (3)
Where u is diffraction angle and l is wavelength employed. The
measured values of inter-layer spacing d are 0.298, 0.308, and
0.313 nm for graphene samples PS-30, PS-60, and PS-90,
320 A. KAUR AND R. C. SINGH
Figure 2. XRD patterns of graphene samples sonicated at different sonication
times (a) 90 min (b) 60 min, (c) 30 min.
respectively. It is clear from above observation that as the soni-
cation time increases, the spacing between adjacent layers of
graphene increases. Consequently, the higher degree of exfolia-
tion is achieved in sample PS-90 relative to others.
3.2. Optical characterization
Figure 3 represents the photographs of synthesized gra-
phene dispersions which are probe sonicated at different
sonication times of 30, 60, and 90 min. It is clear from
these photographs that color of dispersions turns darker
with increase in sonication time which demonstrates the
higher degree of exfoliation in a sample sonicated at
90 min. UV-Vis absorption spectra were recorded for the
Figure 3. Photographs of graphene dispersions at different sonication times.
different graphene dispersions in order to examine the
degree of exfoliation as shown in Figure 4(a). The absorp-
tion peak centered at 278 nm, a characteristic peak of gra-
phene corresponds to p ¡ p transitions of C D C bonds
of graphitic structure (21). In addition, absorbance of gra-
phene dispersions increases with increase in sonication time
which clearly shows that the higher sonication energy leads
to higher degree of exfoliation of graphene layers (22).
Another noticeable observation is increase in the optical
transmittance of graphene samples from 95% to 99% at 550 nm
with increase in exfoliation time as depicted in Figure 4(b).
The sheets like morphology of exfoliated graphene samples
has been confirmed by its SEM images illustrated in Figure 5.
Figure 5(a) pronounced the stacked sheets of graphene of bulk
graphite. It is obvious from Figures 5(b)–(d) that degree of
exfoliation increases with increase in sonication time.
3.3. Raman characterization
The Raman spectra of graphite flakes and synthesized graphene
samples are shown in Figure 6(a) and (b). The prominent
Raman scattering features of graphene samples lie in the range
of 1000-3000 cm¡1: the D, G, and 2D bands at 1350 cm¡1,
1580 cm¡1, and 2700 cm¡1, respectively (23). The Raman D
band is attributed to the presence of disorder in graphene and
it depends on the breathing modes of sp2 atoms in aromatic
rings. This band arises from transverse optical (TO) phonons
around the K point of Brillouin zone (BZ) and it reflects the
stacking between adjacent layers of graphene, edges in finite
crystallite sites and atomic defects within layers (24). The G
band originates from in-plane vibration of sp2 carbon atoms
and it is a doubly degenerate (TO and LO phonon mode: E2g
symmetry) at the Brillouin zone center (25).
The signature of graphene, 2D band: the second order
overtone of D band arises from a two phonon double reso-
nance Raman process is the most important band of gra-
phitic materials after G band (25). The apparent variation
in position, shape and intensity of 2D band marks the vari-
ation in number of graphene layers (26). Figure 6(a) shows
the presence of D and G band at 1352 cm¡1 and 1582
cm¡1, respectively. The D band manifests folded graphene
sheets with curled edges (24). No significant shift in G posi-
tion has been observed which depicts that synthesized gra-
phene samples are free from strain and doping (23). The
additional peak at 1105 cm¡1 [indicated with arrow in
Figure 6(a)] has been noticed in sample PS-30 which corre-
sponds to sp3 hybridized carbon (27).
It is well known that defect ratio ID/IG gives the measure of
disorder in graphene. In the present case, ID/IG of synthesized
graphene layers decreases with increase in sonication time indi-
cating that lesser defects are pronounced in sample PS90 which
favors the formation of highly ordered graphene layers (ref to
Table 1). Therefore, it is evident from defect ratio that high
quality of graphene sheets has been synthesized at sonication
time of 90 min.
At this point, we are in position to measure the average crys-
tallite size of sp2 domain (or average inter-defect distance) LD
and defect density nD using intensity ratio ID / IG by well-
 FULLERENES, NANOTUBES AND CARBON NANOSTRUCTURES 321

Figure 4. (a) UV-Visible absorption spectra (b) Transmittance spectra of synthesized graphene samples.

established Tuinstra and Koenig relation (25). Another parameter of interest is the intensity ratio of 2D
and G band, I2D / IG which reflects the number of graphene
C ðλÞ layers (23). The values of I2D / IG for samples PS-30, PS-60,
LD D (4) and PS-90 is found to be 0.45, 1.04, and 1.17 (shown in
ID =I G
Table 1), respectively, which confirms the formation of
multi to few layered graphene. This increase in value of I2D
Where λ is excitation source of 514 nm and C.λ) is propor-
/ IG signifies reduction in the number of graphene layers
tionality constant i.e. 4.4 nm
(23). The plot of I2D / IG and sonication time is depicted in
Figure 7(b). The 2D band position of sample PS-30, PS-60,
1014 p and PS-90 was red shifted (towards lower wave number) by
nD .cm ¡ 2/ D (5)
L2D 9 cm¡1, 10.96 cm¡1, and 18 cm¡1, respectively, with respect
to bulk graphite as shown in Figure 6(b). It is clear from
The values of LD and n D of graphene samples are summa- above observation that the number of graphene layers
rized in Table 1. decreases with increase in sonication time. The plot between
It is clear from table, sp2 domain size LD increases with position of 2D band and sonication time is represented in
increase in sonication time whereas defect density n D decreases. Figure 7(a).

Figure 5. SEM images of (a) graphite flakes (b) PS-30 (c) PS-60, (d) PS-90.
322 A. KAUR AND R. C. SINGH

Figure 6. (a) Raman spectra of graphene samples at different sonication times (b) Enlarged view of 2D band.

Table 1. The values of ID/IG, I2D/IG, LD and nD are listed. (b) PS-60, and (c) PS-90 is found to be 34.35 cm¡1, 31.77
cm¡1, and 28 cm¡1, respectively. This decrease in wave number
Sample ID /IG I2D /IG LD (nm) nD £ 1023 (cm¡ 2)
separation between two sub peaks of 2D Raman band indicates
PS–30 0.62 0.45 27.02 43.62 the reduction in number of graphene layers which in turn
PS–60 0.31 1.04 54.03 10.9 depends upon sonication time.
PS–90 0.29 1.17 57.76 9.545

3.4. TEM characterization

Apart from I2D / IG, another noticeable parameter which is
sensitive to number of graphene layers is the wave number sep-
aration between two sub peaks of 2D band (27). The de-convo-
lution of 2D Raman band of all the prepared samples (shown
in Figure 8) has been done by Lorentzian multipeak fit using
Origin 8.0 software. The wave number separation between two
sub peaks of 2D Raman band of graphene samples (a) PS-30
Transmission electron microscopy is the most versatile and
powerful technique to examine the state of material in nanore-
gime. We measured the average length of graphene flakes `L’
(dimension along long axis of flake) of different samples from
their respective TEM images. It comes out to be 0.845, 1.165,
and 1.45 mm for sample PS-30, PS-60, and PS-90, respectively.
Folded edges of graphene sheets are clearly seen in TEM

Figure 7. (a) Plot between 2D band position and sonication time (b) Plot between I2D / IG and sonication time.

Figure 8. De convolution of 2D band: (a) PS-30 (b) PS-60, (c) PS-90.
images. The thickness of graphene flakes has been estimated
from HR-TEM images by using edge counting method i.e.
counting the number of monolayers per flake (28). The average
thickness of flakes is measured as 3.60, 3.28, and 1.917 nm for
sample PS-30, PS-60, and PS-90, respectively, corresponding to
approximate 10-11, 9, and 5-6 graphene layers, respectively, as
shown in Figures (9–11).
Figure 9. TEM images of: (a) graphene flakes of PS-30 (b) HR-TEM image of corresponding graphene sheet (plot profile is shown in inset) (c) SAED pattern of correspond-
ing graphene sheet.
FULLERENES, NANOTUBES AND CARBON NANOSTRUCTURES 323
The interlayer d spacing‘s has been measured from HRTEM
using Image J software. The measured values of d are 0.346, 0.363,
and 0.367 nm for PS-30, PS-60, and PS-90, respectively. Conse-
quently, exfoliation of graphene layers has been successfully
achieved in PS-90. Both the number of graphene layers and values
of d spacing’s are well consistent with their respective plot profile
shown in inset. These TEM results are in close agreement with
324 A. KAUR AND R. C. SINGH

Figure 10. TEM images of: (a) graphene flakes of PS-60 (b) HR-TEM image corresponding graphene flake (plot profile is shown in inset) (c) SAED pattern of corresponding
graphene sheet.

observation made in XRD and Raman spectra. We have also
observed bi-layer graphene sheet in few layered graphene sample
i.e. PS-90 which is confirmed by intensity profile diagram and elec-
tron diffraction pattern as shown in Figure 12.
3.4.1. Identification of graphene layers by selected area
electron diffraction (SAED)
SAED (selected area electron diffraction) pattern of each gra-
phene sample has been recorded. A clear six-fold hexagonal
pattern of sample PS-90 has been observed which proves the
higher crystallinity of few layer graphene sheets and light dif-
fraction spots of samples PS-30 and PS-60 corresponds to
multi-layer graphene. SAED pattern of bi-layer graphene sheets
(which are formed in few layer graphene sample i.e. PS-90)
clearly shows a hexagonal pattern in which outer diffraction
spots are more intense than inner ones. These clearly visible
hexagonal diffraction spots allow us to label the spots with the
Miller–Bravais (hkil) indices shown in Figure 12(b). The
inspection of number of layers can be achieved by plotting a
line section through (1-210), (0-110), (¡1010), and (¡2110)
axis in order to determine intensity ratio I{1100} / I{2110} (8).
The intensity profile has been recorded along (1-210) to
(¡2110) axis for SAED pattern of bi-layer graphene sheet
depicted in Figure 12(b). In the present case, the ratio of

Figure 11. TEM images of: (a) graphene flakes of PS-90 (b) HR-TEM image of corresponding graphene flake (plot profile is shown in inset) (c) SAED pattern of correspond-
ing graphene sheet.
 FULLERENES, NANOTUBES AND CARBON NANOSTRUCTURES 325

Figure 12. TEM images of: (a) bi-layer graphene sheet (HR-TEM image of sheet is shown in inset) (b) SAED pattern of corresponding bi-layer sheet (c) The intensity profile
of the line passing through (1-210) and (-2110) diffraction spots.

intensity of {1100} to the {2110} peaks comes out to be » Table 2. Exfoliation of graphite flakes into graphene sheets as a function of sonica-
0.45 (see Figure 12(c)) and this value is close to the tion time.
reported value of intensity ratio of bilayer graphene (8). Thickness of graphene No. of exfoliated Texf Remaining
Interestingly, the absence of bi-layer graphene character in Sample flake (nm) layers (sec) layers
our Raman spectra has been observed which might be PS–30 3.60 2930 0.624 10–11
ascribed to re-aggregation of graphene layers during film PS–60 3.28 2931 1.23 9–10
formation on substrate (22). PS–90 1.917 2936 1.84 5–6

3.5. Estimation of sonication time for exfoliation of

graphite into graphene sheets
Initially, thickness of graphite flakes » 1000 nm
For sample: PS-90
The exfoliated thickness at 90 min D 1000ðnmÞ

¡ ðReduced thicknessðnmÞafter probe sonicationÞ

D 1000 ¡ 1:917
D 998:083 nm

{ Distance between graphite layers is 0.34 nm.

998:083
Thus; the number of layers exfoliated at 90 min D D 2936
0:34
90£60
The time takenðsecÞto exfoliate one layer.Texf / D D 1:84 s
2936

1:917
Therefore; remaining layers at 1:917 nm D D5¡6
0:34

Similar calculations have been done with sample PS-60 and Figure 13. Nitrogen adsorption/desorption isotherms of: (a) PS-30 (b) PS-60 (c) PS-
PS-30 whose values are summarized in Table 2. 90 at 1 atm and 77 K.
326 A. KAUR AND R. C. SINGH
3.6. BET studies
The specific surface area for the synthesized graphene samples
has been estimated as 158, 257, and 273 m2 / g for PS-30, PS-
60, and PS-90, respectively, as shown in Figure 13. As expected,
these BET studies confirm the higher degree of exfoliation in a
sample which is sonicated for 90 min.
4. Conclusions
Graphene sheets have been successfully synthesized by using
probe sonication approach. Multi to few layered exfoliated gra-
phene sheets have been investigated with increase in sonication
time. XRD, UV-Visible, TEM, and BET studies provided infor-
mation regarding the degree of exfoliation of graphene sheets.
The sonication time affected the morphology of graphene
sheets as confirmed by its SEM studies. The Raman and TEM
studies pronounced the formation of highly ordered exfoliated
few layered graphene sheets in a sample which is sonicated for
90 min. Moreover, we were successful in synthesizing bi- layer
graphene sheets in few layered graphene sample i.e. PS-90. In
short, the enhanced degree of exfoliation and reduction in
number of graphene layers in sample PS-90 has been attributed
to longer sonication period relative to others.
Acknowledgements
Financial support from UGC (University Grants Commission) is highly
acknowledged. We are thankful to UGC-UPE and DST-FIST for providing
Raman Spectrophotometer, XRD, TEM, BET, SEM, and UV-Visible spec-
trophotometer facilities.
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