Composites Science and Technology 200 (2020) 108402

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Composites Science and Technology

journal homepage: http://www.elsevier.com/locate/compscitech

Microwaves heating strategy to synthesize few layer graphene for polymer

composites towards thermal and electrical applications
Muhammad Maqbool, Muhammad Asif, Muhammad Yousaf, Ya-Fei Zhang, Waseem Aftab,
Imran Ali, Haichang Guo, Adeel Y. Abid, Shulin Bai *
Department of Materials Science and Engineering HEDPS/CAPT/LTCS, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, College of
Engineering, Peking University, Beijing, 100871, China

A B S T R A C T

The few-layer graphene (FLG) with tailorable microstructure for macro-properties is prepared from graphene oxide (GO) by simple, fast and inside microwave (Mw)
heating strategy. The effects of varying power, environment and time on FLG are studied throughout Mw treatment. The investigations based on microscopic and
spectroscopic results confirm the formation of FLG having much less oxygen-containing functional group with an average layer thickness of ~1.378 nm. The pa­
rameters related to the excellence of graphene such as carbon/oxygen (C/O) and Id/Ig ratios are calculated approximately to be ~2.99 and ~0.43 respectively. In
addition, thermal interface materials (TIMs) and electrodes are fabricated to check their efficiencies. The highest thermal conductivity of 0.25 W m− 1 K− 1 is achieved
by adding just 1 wt% FLG, which is ~278% that of the fluoropolymer being used. In electrochemical impedance spectroscopy (EIS), the Mw treated GO shows the
maximum charge transfer resistance of around 100 Ω, displaying almost 12 times lower than that of the pristine GO. Thermally reduced graphene oxide (rGO) at
1000 ◦ C is also prepared for comparison and it is concluded that FLG by Mw treatment is significantly better than rGO for such kind of real-life applications.

1. Introduction having less interlayer van der Waals forces in various structural forms, to
name a few are, nanosheets, nanoplates, and nanofibers, etc. [3,17,18].
Among carbon allotropes, graphene is the durable, free-standing and Many ways are explored to attain FLG at low cost; some of them are
2-dimensional (2D) crystal material coined in 2004 [1]. It provides based on bottom-up and top-down synthesis. In bottom-up method such
outstanding physio-chemical properties thus making it a potential as chemical vapor deposition (CVD) [19,20] wherein carbon (methane
candidate for its direct and indirect usage in different scientific disci­ gas, ethyl alcohol, acetylene. etc.) is added as a starting source and
plines ranging from engineering and material science to biomedicine graphene is developed directly from monomers [5]. In this technique,
and electronics [2–8,48–51]. However, the strong van der Waals inter­ the shape [5,21] even the thickness and size of graphene sheets can be
action [9] among graphene layers suppresses its usage in a few potential manipulated. However, this method is lacking to produce FLG at the
applications such as thermal interface materials (TIMs) and batteries. bulk scale as well as expensive because of used equipment that restricts
These intermolecular forces usually provide difficulty in dispersion and the role of graphene in the above mentioned potential applications [21].
separation that is the prime factor for the above-mentioned applications On the other hand, FLG is prepared also by using the top-down tech­
[10]. Because of poor dispersion and stacking of graphene sheets, pho­ nique. This technique further splits into two categories such as chemical
nons offer massive challenges while traveling through them [11–13]. or thermal treatment based reduction of GO for preparing graphene [22,
Attributed to high pressure and excessive attraction among layers, 23]. The chemical based reduction seems to be a very good approach to
graphite (a building block of many layers) possesses much less interlayer synthesize graphene in huge quantity at low cost, but the use of toxic and
spacing of 0.34 nm [14]. It can be overcome by reducing the number of harsh chemicals changes its electronic properties as well as makes it
layers in graphite to make them single or few-layer graphene. For unfriendly for the environment. Environmental friendly (EF) graphene
example, it is noticed that interlayer spacing is somewhat larger like 0.6 has been synthesized in an earlier study by using Lycium barbarum [24]
nm and 0.8 nm for thermally reduced graphene oxide (rGO) and gra­ to reduce GO, but the quality of graphene in respect of thickness still
phene oxide (GO), respectively due to less forces and functional groups remains a challenging task. Hence, implementing this, it is very difficult
[15,16]. Hence, adoption of a unique methodology is essential that can to get an EF approach and good quality graphene simultaneously. In
provide a serious breakthrough in developing few layer graphene (FLG) addition, thermal annealing based methods enhance the quality of

* Corresponding author.
E-mail address: [email protected] (S. Bai).

https://doi.org/10.1016/j.compscitech.2020.108402
Received 10 June 2019; Received in revised form 23 March 2020; Accepted 7 August 2020
Available online 14 August 2020
0266-3538/© 2020 Elsevier Ltd. All rights reserved.
M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Fig. 1. Schematic diagram of MwrGO synthesis and composite fabrication.

graphene by removing oxygen-related functional groups, however it heating strategy to fabricate FLG by using ordinary house hold micro­
needs high temperature and also requires a long time for annealing [13]. wave (Mw) oven. Thanks to graphene Mw absorption capability that
In spite of this, investigators have also discovered to make dispersed provides inside heat which is very favorable in producing dramatically
suspensions of graphene by using various inorganic and organic chem­ disperse-able FLG. Further, prepared material is used in developing TIMs
icals to overcome van der Waals interaction [25–27]. During this kind of and assembling Li-ion battery half-cells which reveal benefits of inside
treatment, organic solvents interact with pi-electronic clouds of gra­ heating technique over traditional methodologies. While annealing in
phene through covalent or non-covalent bonding. Consequently, the Mw oven, the effects of different powers, environments and time on the
electronic properties of graphene are altered and phonon traveling paths quality of graphene are examined in detail. In order to achieve this, a
are changed. Within this, it is also very hard to remove organic solvent novel and simple “balloon fixed Pyrex-tube” technique is developed for
or chemicals which are being used during processing. the treatment of GO. The rGO is prepared also to differentiate the per­
In this study, we introduce a simple, EF, time-saving and inside formance of our materials in these potential applications.

Fig. 2. (a) Digital images showing an arc maturing in a few seconds. (b) Schematic representation of Mw annealing with different time duration. (c) Original digital
images of balloon fixed Pyrex-tube while increasing time.

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M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Table 1 Elaborately, Mw radiations are directly associated with energy

Detail description of all developed samples. originating from non-ionizing (non-destructive) electromagnetic radia­
Sample name Power Time Environment tions. These radiations have a frequency lower than infra-red (IR) but
higher than ordinary radio waves, so it is highly desirable and necessary
MwrGO200 (microwave) 200 W 3s Ar
MwrGO600 (microwave) 600 W 3s Ar to give numerous powers for different annealing ability during the
MwrGO800 (microwave) 800 W 3s Ar treatment of mrGO. Various powers such as 200 W, 600 W, 800 W, and
MwrGO1000/S1 (microwave) 1000 W 3s Ar 1000 W are given through an ordinary house hold Mw oven at a constant
S2 (microwave) 1000 W 30s Ar time of 3 s. After getting superiority among powers, the focus was put on
S3 (microwave) 1000 W 60s Ar
S4 (microwave) 1000 W 120s Ar
time effect while keeping power constant. Numerous times, 3s, the 30s,
rGO (thermal annealing) 1000 ◦ C 1h Ar + H2 60s and 120s (Fig. 2b) were investigated also by using “balloon fixed
GO (as-received) - - - Pyrex-tube” technique to avoid the explosion. While treatment in Mw
oven, it is a worth mentioning step to provide a closed environment to
ensure the inert atmosphere. However, the closed environment can
2. Experimental
cause an explosion due to the pressure of CO2, CO and other gases
removing during annealing under Mw irradiation. The pressure of these
2.1. Materials
gases is high enough to break the vial at long time heating. To avoid this,
here a simple “balloon fixed Pyrex-tube” technique is developed, which
Fluoropolymer [Co-polymer of vinylidene difluoride (VDF) and
helps allot while studying at a long time annealing. In Fig. 2c as can be
chlorotrifluoroethylene (CTFE)] powder was provided by Beijing Yili
seen, the inside pressure of these gases results in blowing a balloon
Fine Chemical Co. Ltd., China. Ethyl acetate, lithium hexa­
which is fixed at the end of the Pyrex tube. Besides, the direct heating
fluorophosphate (LiPF6), ethanol, ethylene carbonate (EC) and dimethyl
approach was also adopted to fabricate rGO by direct annealing (heating
carbonate (DMC) were bought from Beijing Chemical Reagent Factory.
furnace) at 1000 ◦ C under inert atmosphere (Ar + H2) for comparison.
The GO powder (purity of >95 wt%) having lateral size 10–50 μm was
The sample’s names are listed in Table 1.
supplied by Shanghai Zhongwei Materials Co. Ltd. All suspensions and
solutions were made in distilled water and all other chemicals were used
2.3. Fabrication of composites
as received.
The FLG based TIMs were fabricated by using a simple solution
2.2. Synthesis of microwave reduced graphene oxide (MwrGO) method at 1 wt % filler loading. Concisely, 5 g fluoropolymer was
weighted and dissolved in vinyl acetate to get a clear solution at 50 ◦ C
Two-step reduction technique was used to fabricate FLG by reducing and then 0.05 g MwrGO1000 was measured and dispersed in the same
GO. In the first step, the heating furnace (direct heating) was used to get solvent by sonication process for 30min. Afterward, the prepared
mild reduced GO (mrGO) at 400 ◦ C for 1 h in an inert atmosphere (Ar + MwrGO1000 dispersion was added slowly into the polymer solution and
H2). Afterward, the achieved mrGO was tightened in a Pyrex-tube and a stirred while mixing both dispersions. Subsequently, this mixture was
balloon was fixed at the end of this tube. The latter process was done in kept in a sonication bath for 1 h and then transferred back to a me­
the glove box to ensure an inert (Ar) atmosphere in it. The second chanical stirrer for 2 h at 60 ◦ C. In the long run, the mixture was poured
heating step was conducted in Mw (indirect heating) oven where the in polytetrafluoroethylene dish and kept in a heating oven at 80 ◦ C for
study of varying power, time and environment was explored to acquire 24 h as shown in Fig. 1. The weight fraction of FLG in composites is
high-quality FLG. The complete schematic is shown in Fig. 1. When 0.99%, approximating 1 wt %. The same procedure was adopted to
mrGO was microwaved, an arc was produced and matured within a few synthesize GO and rGO based TIMs for comparison.
seconds as can be seen in Fig. 2a. For simple GO, no such kind of arc was
observed due to its non-electronic properties.

Fig. 3. HRTEM (a, b) images showing the transparent and crystalline nature of S1. (c–f) TEM images of FLG at 3s, 30s, 60s and 120s, respectively. SEM images (g–i)
illustrating 1 wt% GO, MwrGO1000, and rGO composites respectively.

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M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Fig. 4. Raman spectroscopy of (a) annealed samples by using various powers while keeping time (3s) constant and (b) samples annealed under 1000 W with different
time duration.

2.4. Assembling Li-ion battery half-cells few seconds assisting to remove functional groups [28]. TEM and
HRTEM images of FLG made at 1000 W for 3s in the Ar environment are
To context the potential applicability in batteries, electrodes were shown in Fig. 3(a–c), illustrating clear creases and wrinkles which
manufactured by using prepared materials. The active material slurry belong to crystalline graphene [29–31]. Moreover, under the same
was prepared by mixing the active material and carbon black in poly­ conditions (1000 W, Ar), graphene sheets are exfoliated initially (Fig. 3c
vinylidene fluoride (PVDF) binder solution at a weight ratio of 7:2:1. and d), then start to aggregate with an increase in time due to long-time
The slurry was coated on copper foil and dried overnight at 70 ◦ C under annealing as shown in Fig. 3e and f. Transparency of FLG sheets can be
vacuum. Half-cells were assembled using 8 mm diameter active material observed at 3s and 30s while getting opaque at longer time annealing
electrode, 14 mm Li disk as a counter electrode, 1 M LiPF6 as electrolyte due to the welding of graphene sheets with each other (Fig. 2b).
dissolved in EC and DMC (1: 1 in volume), and Celgard as a separator. Meanwhile, Mw belongs to non-destructive nature, but electrically
Electrochemical Impedance Spectroscopy (EIS) measurements were conductive materials can get defected in respect of shape and mor­
carried out in a frequency range from 1 mHz to 1 MHz at a voltage phologies at a long time annealing. Further, all trapped air was removed
amplitude of 10 mV. from the Pyrex-tube by using a vacuum pump to ensure pure vacuity.
Treatment was carried out once again at 1000 W for a different time, the
quality of graphene is still an issue for vacuum environment and
2.5. Characterizations
considered similar to the highly oxidized form of graphene made in the
air as displayed in supporting information (Fig. S1). Hence, Mw radia­
Quality of GO, FLG, and rGO for concerning defects, crystallinity and
tions help to fabricate FLG, but the environment and power of Mw oven
grain boundaries was seasoned by micro Raman imaging spectrometer
have a distinguished impact on its quality.
(DRxi U.S.A) under the visible wavelength of 532 nm. The chemical
The TIMs based on MwrGO1000, rGO and GO were fabricated as
composition was measured by X-ray photoelectron spectroscopy (XPS:
discussed in the experimental section. The inside or non-contacting
Axis Ultra, Kratos Analytical Ltd.) with Al (mono) Kα X-ray source.
heating strategy enables us to synthesize FLG which is found well
Thermogravimetric analysis (TGA-SDT-Q600 from TA) was made to test
compatible with polymer chain (fluoropolymer). In Fig. 3h, one can also
the stability of graphene at a heating rate of 10◦ /min under an inert
evaluate that MwrGO1000 is not aggregated likewise GO based polymer
atmosphere. Morphologies were visualized by field emission scanning
composite (Fig. 3g), suggesting that Mw annealing is quite beneficial to
electron microscopy (FE-SEM, S-4800, HITACHI, Japan) which operated
prepare FLG for such kind of application. On the other hand, rGO shows
at 10 kV and transmission electron microscopy (TEM: JEM-2100 F,
also aggregation in the same matrix as can be seen in Fig. 3i. Blue and
JEOL). Thermal conductivity was perceived by a simple hot wire
red arrows symbolize matrix and graphene sheets respectively.
(TC3010) method by considering the average of the three values for each
From the Raman spectra shown in Fig. 4, it is noted that MwrGO1000
sample. Electrochemical impedance spectroscopies (EIS) were per­
has sharp as well as intense 2D (2670 cm− 1), G (1570 cm− 1) and rela­
formed at Biologic VSP-300 electrochemical workstation in the fre­
tively less intense D (1348 cm− 1) peak ascribing to the coupling of
quency range of 1 MHz–1 mHz with an amplitude of 10 mV. Tensile tests
phonons with two opposite wave vectors, sp2 carbon and sp3 carbon
were undertaken by Instron 5980 instrument under a loading rate of 1
atoms respectively [32]. The number of layers depends upon the in­
mm/min. The dimensions of tensile samples are 20 × 2 × 1 mm3.
tensities ratio of 2D and G peaks. For single or bilayer graphene, the 2D
peak is equal or double to the G peak. Hence, comparing with similar
3. Results and discussions
previous studies, this trend is direct evidence of good reduction and
formation of FLG [5,29]. Conversely, large intense D peak (belongs to
3.1. Microscopic and spectroscopic investigations
defects) and very small 2D peak are observed in rGO attributing to large
defects due to the removal of oxygen which is located at the basal plane
The surface morphologies of prepared FLG and TIMs are visualized
[33,34]. Generally, defects related to oxygen-containing functional
by TEM and SEM imaging (Fig. 3). The Mw heating phenomenon is
groups decrease between 200oC-800 ◦ C, but later heating (up to 1200
found very fast and amicable to get several thousand degrees Celsius in a

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M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Fig. 5. (a) XPS analysis showing carbon contents in S1. (b) Oxygen constituents of S1 by fitting into two components. (c) Oxygen concentrations in various samples
(S1–S4). (d) Weight losses of different samples.

◦
C) causes an increase in defects [33,35]. oxygen peak of S1 (Fig. 5b) into two constituents, it is observed that
More importantly, when the time is increased while keeping power some of the oxygens are doubly bonded “ = O” around 531 eV and
constant (1000 W), more defects are produced wherein Id/Ig ratio in­ remaining singly bonded “O-” at 533 eV. For comparative analysis,
creases up to 1.22 (Fig. 4b) entailing agglomeration (already revealed in carbon and oxygen percentages in samples S1–S4 are calculated as shown
Fig. 3e and f). Some additional peaks such as D + D′ and D + D’’ are also in Table S1. It is noticed in Fig. 5c and Table S2 that oxygen percentage
apparent for the same annealing at the 60s and 120s (Fig. S2a). These decreases with increasing annealing time. Most essentially, all oxygen
over tonic peaks belong to acoustic and in-plane longitudinal phonons, peaks appear in the range of 531–536 eV which is the general range of
which were found in defective graphite or graphene [32]. Further, the this element in graphene related materials. Consequently, the intensity
effects of vacuum and air environment are also studied by using 1000 W ratio of carbon-oxygen (C/O) is observed to be ~2.7 for the S1 sample
at a different time as shown in Fig. S2b. From the results, it seems that (Fig. S3a), afterward this ratio gets higher at long time annealing which
prepared FLG is approximately similar to a highly oxidized form GO. illustrates again a decrease in oxygen content. Full surveys of S1–S4
It is noticed from XPS analysis in Fig. 5, these defects do not belong to samples are recorded to check the electronic behavior with increasing
oxidation of graphene because oxygen contents remain less even though time at constant power as shown in Fig. S3. Generally, some defects of
annealing at 120s in Mw oven. Therefore, these defects might be basal plane arise because of these peaks (C–H, C–O, O-, O = ) in the XPS
ascribed to change in shape and structural defects (due to annealing for a and D peak of Raman. In the current study, we successfully achieved the
long time) as explained in both TEM and Raman results. To distinguish possible lowest contents of these defects by using the inside heating
FLG in aspects of sp2 and sp3 contents, the carbon element of sample S1 is approach, matching well and somewhere better as compared with
deconvoluted in Fig. 5a. The characteristic peak of sp2 carbon content is earlier reported XPS and Raman results while adopting the top-down
observed at 284.6 eV. The other peaks having less intensity associated synthesis [24,36–38].
with C–H and C–O are established at 285.2 eV and 285.1 eV, respec­ Further TGA analysis (Fig. 5d and Table S2) shows that the huge
tively. Further, an oxygen component is deconvoluted also by fitting weight loss happened in the range of 100–300 ◦ C for GO due to the

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M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Fig. 6. (a) Thermal conductivities of fluoropolymer and its composites, (b) comparison with earlier reported results.

removal of oxygen-containing groups [39] and then it is approximately

Table 2
constant up to 1000 ◦ C. Moreover, a weight loss for MwrGO1000 is
Summary of TCE and TCE factor of MwrGO1000 as compared to results of
identified slightly low as compared to rGO indicating Mw irradiation is a
different fillers based composites.
quite superior and fast annealing method that helps to reduce GO almost
completely in a few seconds. On the other hand, the fluoropolymer is Filler Matrix FC TC (W TCE TCE Ref.
(wt. m− Factor
used to make TIMs is an amorphous polymer possessing no melting point %)< 1 − 1
k ) TCE/FF
and it is directly decomposed around 450 ◦ C.
Graphene Epoxy 10 5 2300 230 [40]
Graphene Epoxy 30 4.9 1900 63 [41]
3.2. Thickness of graphene sheets GNP Epoxy 25 6.44 3000 120 [42]
Graphite Epoxy 20 5 2400 120 [43]
SWCNT PMMA 7 0.35 55 7.86 [44]
Surface topography in taping mode is performed using atomic force
SWCNT Polystyrene 1 0.25 50 50 [45]
microscopy (AFM), as shown in Fig. S4. Images of all samples are ob­ SWCNT PVDF 1 0.3 129 129 [46]
tained by depositing them at the silicon substrate after sonication for 40 GNP Silicon 20 2.3 752 37.6 [47]
min. It is seen that graphene sheets are well separated from each other FLG Fluoropolymer 1 0.25 177 177 This
work
and consist of relatively smooth, planar and folded (at the ends) struc­
ture in case of smaller time annealing such as 3s and 30s (Figs. S4a and
d). The average thickness of ~1.378 nm and ~0.715 nm are observed for Fig. 6a, the highest in-plane TC (0.25 W m− 1 K− 1) is achieved for
3s and 30s respectively. It is approximately ascribing to a thickness of MwrGO1000 which is approximately 278% that of the neat fluoropol­
2–4, layer graphene. For a clear and better understanding, an area ymer. It is to note here that this polymer has a very low TC of 0.09 W
around 817 × 817 nm2 is taken under investigation wherein three sheets m− 1 K− 1 because of its amorphous nature. Due to poor dispersion and
laying on each other can be clearly seen in Fig. S4b. The thicknesses of
these sheets are ~0.59 nm, ~0.58 nm, and ~0.66 nm, respectively for
blue, red and green mark lines. These thicknesses are moderately higher
than pristine graphene (0.34 nm), on the other hand, comparatively
lower than a highly oxidizing form of graphene having a thickness of
~0.80 nm. Such kind of increase in thickness attributed to lower in “π
–π” interactions and functional group [14] that still present on the sur­
face of MwrGO1000, already discussed in XPS results for S1. TEM
(Fig. 3c) image also shows some folds at the edges of graphene sheets,
which are very helpful for graphene to have a planar hexagonal struc­
ture because they can decrease the surface tension of graphene sheets
[29]. Further, graphene sheets possess intertwined and wrinkled fea­
tures as can be seen in Fig. 3c and d. As time increases up to 120s,
graphene sheets look somewhat thicker like welding of graphene sheets
with each other. It can be clearly seen in Figs. S4e-f that graphene sheets
are not in disperse form but showing the bulk characteristics having a
large thickness. Here, some white spots are prominent they may be
because of impurities coming during handling or solvents remnants.

3.3. Thermal and electrical performances

Thermal conductivity (TC) was measured on MwrGO1000, GO and Fig. 7. EIS analysis showing electrical resistance of GO, rGO, and MwrGO1000
rGO filled fluoropolymer TIMs with the same loading of 1 wt%. From by assembling Li-ion battery half-cells.

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M. Maqbool et al. Composites Science and Technology 200 (2020) 108402

Fig. 8. (a) Stress-strain curves and (b) Young modulus and yield strength of studied materials.

stacking of GO and rGO sheets in a polymer matrix, their composites Among all, the highest Young’s modulus for MwrGO1000 is found to be
show less enhancement in TC. On the other hand, MwrGO1000 illus­ ~4.03 MPa, which is about 7.1, 3.2 and 1.1 times that of pure fluo­
trates complete homogeneous dispersion in the polymer matrix as ropolymer, GO and rGO filled composites, respectively. Consequently,
highlighted by black arrows in Fig. S5. The TIMs with desired TC value MwrGO1000 composite exhibits better compatibility with the polymer.
can be manufactured by increasing the fraction of MwrGO1000. More­ All samples underwent more than 100% deformation without any
over, thermal conductivity enhancement (TCE) and TCE factor are possible failure, proving good ductility of composites. Besides, the ten­
calculated to compare our results with earlier reported results as pre­ sile behavior of rGO and MwrGO1000 below 10% strain is much
sented in Table 2. TCE is defined as (TCcomposite-TCmatrix)/TCmatrix, while different from that of neat polymer and GO filled composite. A sharp
the TCE factor is obtained by dividing TCE with filler contents (FC). stress drop at about 5% strain is observed for rGO and MwrGO1000
From Fig. 6b, it can be concluded that the inside heating approach is composites. This phenomenon is probably caused by abrupt exfoliation
significantly better to develop TIMs as compared to other methodolo­ of the interface between graphene and fluoropolymer. At this moment,
gies. This kind of heating phenomenon does not affect the properties of the stress is relaxed, resulting in rapid dropping. Then the load-bearing
graphene sheets and reduces them without producing any additional ability is recovered with continuous deformation because the interfacial
defects [28]. Consequently, MwrGO1000 has good compatibility with cracks are not interconnected (due to low filler loading) and graphene
the matrix due to uniform dispersion that gives more and better paths for can still play the role of restricting the movement of molecular chains of
traveling of phonons. the fluoropolymer. For GO filled composite, even though the rein­
Moreover, the Nyquist plots in Fig. 7 comprise of three regions: (1) a forcement effect of filler appears, but its tensile behavior is somewhat
low frequency region that is characterized by an inclined line along the similar to a neat polymer with continuous strain hardening during the
Z′ axis which shows capacitive behavior; (2) a high frequency region primary plastic deformation period. Another important factor that af­
characterized by a partial semicircle which displays the blocking fects the tensile properties is filler dispersion which is best for
behavior (in this region, the resistance values determines the charge MwrGO1000 composite, resulting in quite better performance than GO
transfer resistance of the electrode); and (3) a middle frequency region and rGO composites.
that illustrates the effect of electrode thickness and the porosity on the
diffusion of ions from an electrolyte to the electrode. Herein, just high 4. Conclusion
frequency region’s semicircles were taken as a comparison of charge
transfer resistance of three electrodes, which reflect the improved In a nutshell, a fast, simple and inside heating strategy by micro­
electric conductivity of our prime material. The Nyquist plot depicts waves (Mw) to synthesize few-layer graphene (FLG) is explored in this
very low internal resistance of the MwrGO1000. The rGO reduced using work. This technique does not only develop FLG in a very short time but
direct thermal treatment shows double charge transfer resistance, while also environment friendly as well as applicable on an industrial scale.
the pristine GO illustrating much higher internal resistance compared to Employing this strategy, the synthesized FLG shows less concentration
the other two. This suggests that inside heating (Mw) facile to reduce of oxygen-containing functional groups, which in our best knowledge
defects does not only relate to functional groups but also help to attain has never been reported in any top-down synthesis method. Long-time
the planar shape of the graphene sheets as we discussed in the thickness annealing under inert environment is also achieved by a novel
section. “balloon fixed Pyre-tube” approach, which helps to understand the Mw
heating mechanism for a long time. Furthermore, the effects of various
3.4. Mechanical properties of composites power and time on the quality of FLG are demonstrated to give an idea
about the best condition and parameters while using Mw treatment. In
The mechanical behavior under the tension of the composites is addition, prepared FLG is used to fabricate fluoropolymer-based thermal
investigated at room temperature. From Fig. 8a, it is noted that the interface materials (TIMs) to record performance in the field of elec­
plastic deformation of the studied fluoropolymer increases continu­ tronics for heat dissipation. The obtained results explicitly entail that
ously, while stress almost remains constant after maximum stress is our technique is significantly better for the development of materials in
reached. As GO, rGO and MwrGO1000 were added in it, there is a such kind of applications. To examine this material in batteries appli­
dramatic increase in both strength and Young’s modulus (Fig. 8a and b). cation, the electrodes are manufactured also with prepared FLG thus

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