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Article history: Graphene, a two-dimensional material, is now considered as a rewarding contestant for nanodevices due
Received 18 May 2017 to its morphology and novel properties. The chemical exfoliation and thermal annealing methods are
Received in revised form appraised as an inventive route towards the production of graphene at prodigious scale. This method is
28 August 2017
utilized for the oxidation of graphite flakes having an oxidizing specialist and thermally reduced the
Accepted 7 October 2017
graphene oxide into reduced graphene oxide. We have examined the samples through different char-
Available online 9 October 2017
acterization techniques. X-ray diffraction displayed the peaks of graphene oxide at 11.8 and reduced
graphene oxide at 25.5 . Scanning electron microscopy images revealed the single and multilayers
Keywords:
Graphene oxide (GO)
morphology. The optical microscopy examined the number of layers of graphene oxide through the
Reduced graphene oxide (rGO) various contrasts of light. UV-Vis spectroscopy showed the hills of graphene oxide and reduced graphene
Oxidizing agent oxide at 215 nm and 267 nm. Fourier transform infrared spectroscopy has been utilized to examine the
Chemical exfoliation method resonating modes.
Thermal annealing © 2017 Elsevier B.V. All rights reserved.
https://doi.org/10.1016/j.matchemphys.2017.10.020
0254-0584/© 2017 Elsevier B.V. All rights reserved.
2 H. Saleem et al. / Materials Chemistry and Physics 204 (2018) 1e7
be loaded to form graphite (3D), it can be rolled to form nanotubes 2.3. Thermal reduction of graphene oxide
(1D), and enfolded to form fullerenes (0D). p-conjugation of long
range in graphene produces amazing electrical, mechanical, and The GO was annealed in a Nabertherm Gmbh N17/HR-400V
thermal properties [2]. Muffle heating furnace at 500 C at a heating rate of 2 C min1
The different method to synthesis the graphene are: micro- for 2 h and allowed to cool in furnace till the temperature decreased
mechanical cleavage of natural graphite flakes using a Scotch Tape till 50 ± 5 C. The GO was completely converted into reduced gra-
[1], epitaxial growth of graphene on SiC [3], thermal or plasma phene oxide (rGO) [26,27].
enhanced chemical vapor deposition (CVD) of graphene [4e6],
chemical exfoliation of graphitic materials [7e10], bottom-up
synthesis from organic compounds, and electrochemical exfolia- 2.4. Characterization
tion of graphite [11]. Only the chemical exfoliation method is
considered as a typical way toward the generation of graphene with The X-Ray Diffraction STOE q-q was used with CuKa radiation
ease and in huge amount [12]. The ideal graphene sheets that can with wavelength 1.5406 Å and scintillation detector as sensor
be achieved by this mechanical exfoliation technique have proven equipment, scanning electron microscope (SEM) analysis in this
to be highly ordered, exhibit outstanding surface areas research was performed by JEOL scanning electron microscope
(2630 m2 g1), high Young's modulus (1 TPa), highest hardness, (JSM 6490LA), optical microscopy, UV-Vis spectroscopy (wave-
flexible elastic, ultra thickness, high thermal conductivity length 200 nm-1100 nm), Fourier transform infrared spectroscopy
(5000 W mK1), and strong chemical durability [13]. Having zero (FTIR) were used to investigate the structural, optical, and func-
rest mass of charge carriers, electrons travel with the speed of light tional properties of graphene oxide (GO) and reduced graphene
through the crystal. Such electron transport has never been prac- oxide (rGO).
tically seen in any semiconductor, and as a result graphene has
proved to be the most conductive non-superconducting material 3. Results and discussions
with a room temperature resistivity of just 106/cm.
The following potential applications of graphene are: (a) The 3.1. X-ray diffraction (XRD)
electronic devices contain graphene have ultrafast terahertz elec-
tron flexibility that gives smaller, quicker, less expensive digital XRD is used for the determination of crystal structure and lattice
products such as field transistors [14], spintronics [15], and opto- parameters. During the oxidation process, we observed that the
electronics [16], (b) Graphene loaded polymer composites have intense peaks of the (002) plane (d-space 3.4 Å at 26.23 ) of
high electrical and heat conductivity, good mechanical strength, graphite flakes gradually debilitated and vanished which increased
and low percolation threshold [17], (c) It is used in display pro- the inter-planar distance from 3.4 Å to 7.5 Å and shifted the
grams such as touch displays [18], (d) Graphene centered electro- diffraction peak of the plane (002) from 26.47 to 11.8 shown in
chemical storage space energy devices, (e) Graphene is used as Fig. 1 [28]. This enlargement of inter-planar distance is due to the
transport, performing electrodes [19], and (f) Many other applica- entrapping of oxygen functional groups between the graphene
tions in bio-, electrochemical, and chemical sensors [20], dye- oxide sheets [27,29]. This is confirmed by the Bragg's equation 2d
sensitized and organic solar panels, hydrogen storage, catalysts sin q ¼ n l, shows the inverse relation of inter planar ‘d’ to the
[21] and photo catalysts [22]. diffraction angle ‘2W’.
Here, we report the chemical and thermal synthesis routes to- After thermal reduction of graphene oxide, GO was reduced to
wards the massive production of reduced graphene oxide. We rGO and the ordered crystal structure of reduced graphene oxide
prepared high quality graphene nanosheets through this approach. (rGO) was restored. This is verified by the reappearance of the (002)
The crystal structure, morphology and optical properties were diffraction peak at 25.5 and disappearance of the diffraction peak
investigated by X-ray dffraction (XRD), scanning electron micro- (001) at 11.8 in XRD pattern in Fig. 2 [12,30]. During the reduction
scopy (SEM), optical microscopy, UV-Vis spectroscopy, and Fourier of GO, the yellow brown solution gradually transferred into black
transform infrared spectroscopy (FTIR). precipitate.
2. Experimental
3.2. Scanning electron microscope (SEM)
2.1. Chemical exfoliation method
In scanning electron microscopy, the surface of the specimen is
Oxidized the graphite flakes by chemical exfoliation method. analyzed by an electron beam. SEM samples of graphene oxide (GO)
Mixed 3 g of graphite flakes with 9:1 mixture of concentrated and reduced graphene oxide (rGO) were prepared by sonication of
H2SO4/H3PO4 (360:40 ml) and 18 g of KMnO4. Stirred the mixture GO in ethanol for 30 min. Dried the sample on a glass slide by
mechanically at 35-40 C for 4e5 h to produce the slightly heating under an incandescent lamp. SEM image of graphite flakes
exothermic reaction. Heated and stirred it at 50 C for 12 h. Then shows the flat surface with ordered layer structure [31]. Invariance,
cooled it to room temperature and poured 400 ml ice of distilled graphene oxide reveals randomly aggregated, thin, crumpled layers
water and 5 ml hydrogen peroxide H2O2 in a mixture to complete structure. It exhibits that the oriented layer structure of graphite
the reaction. The dark pink color was converted into mustard color. has been unbalanced due to its oxidation. In Fig. 3, the graphite
Washed the mixture with 1 M HCl and distilled water till the pH of sheets have exfoliated into mono or multi-layer graphene oxide
supernatant liquid reached 7 [23,24]. (GO) sheets [27,32].
Fig. 4 shows the SEM images of reduced graphene oxide ori-
2.2. Exfoliation of graphene oxide (GO) ented as randomly crumpled silk veil waves. The nanosheets are
rippled and entangled with each other. The lamella structure of
To exfoliate the GO, sonicated the GO dispersion under normal wrinkled rGO nanosheets is due to the van der Waal's interactions.
condition for 30 min. The homogeneous brown dispersion was They are transparent and the lateral dimensions of the sheets
produced which was utilized for reduction. Dried the solution in ranged from hundreds of nanometers to several micrometers
the vacuum oven at 40 C for 24 h [25]. [30,33].
H. Saleem et al. / Materials Chemistry and Physics 204 (2018) 1e7 3
3000 (001)
2000
Intensity (a.u.)
1000
GO
0
0 5 10 15 20 25 30 35 40 45 50 55 60 65 70 75 80 85
300
(002)
200
Intensity (a.u.)
100
rGO
0 5 10 15 20 25 30 35 40 45 50 55 60 65 70 75 80 85
2
Fig. 2. XRD of reduced graphene oxide (rGO).
4 H. Saleem et al. / Materials Chemistry and Physics 204 (2018) 1e7
shows the absorption peak at 215 nm. The absorption peak varies
on the oxidation of graphite [35].
When GO is being reduced, the absorption peak of oxidized
graphene shifts to a greater wavelength from 215 nm to 267 nm.
This is due to the desorption of the oxygen attached to the graphene
layers after the thermal annealing shown in Fig. 7. As an impact of
this, the color has changed from brownish to dark [35]. Graphene
oxide nanosheets are hydrophilic and reduced graphene oxide
(rGO) nanosheets are hydrophobic. We noticed that GO solution is
stable in the water while rGO can homogenously disperse in water
Fig. 3. SEM images of Graphene Oxide (GO) layers.
via ultrasonic vibrations but the dispersion can only be stable for
few hours due to their hydrophobic nature.
Absorption 4
GO
1
200 250 300 350 400
Wavelegth(nm)
Fig. 6. UV-Vis spectrum of Graphene Oxide (GO).
2.6
2.5
Absorption
rGO
2.4
2.3
270 280 290 300
Wavelength(nm)
Fig. 7. UV-Vis spectrum of Reduced Graphene Oxide (rGO).
6 H. Saleem et al. / Materials Chemistry and Physics 204 (2018) 1e7
65
GO
% Transmittance
60
C=O
55
75
rGO
70
% Transmittance
65
60
C-N C=C
C-H
55 O-H
50
0 500 1000 1500 2000 2500 3000 3500 4000 4500
Wavelength (nm)
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