Applied Materials Today 7 (2017) 246–254

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Applied Materials Today

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Review

A short review on preparation of graphene from waste and bioprecursors

Nivea Raghavan a , Sakthivel Thangavel a , Gunasekaran Venugopal b,∗
a
Department of Nanosciences and Technology, School of Engineering and Technology, Karunya University, Coimbatore 641114, Tamil Nadu, India
b
Department of Materials Science, School of Technology, Central University of Tamil Nadu, Thiruvarur 610 005, Tamil Nadu, India

a r t i c l e i n f o a b s t r a c t

Article history: Herein an overview of the graphene preparation from waste and bio-precursors is given which is simple
Received 13 February 2017 yet adaptable approach excluding usual hydrocarbon or graphite as graphene precursor. Recently precur-
Received in revised form 8 April 2017 sors such as paper cups, glucose, hemp, rice husk, cockroach legs, cookies, and grass has been identified for
Accepted 10 April 2017
graphene production. We believe this review facilitates researchers in the better use of biomass and other
waste as precursor material and so it can expectantly paves the way for the exploration of untouched
Keywords:
biomass and other waste for graphene preparation.
Graphene
© 2017 Elsevier Ltd. All rights reserved.
Waste
Bioprecursors
Biomass
Glucose
Rice husk
Hemp

1. Introduction Graphene plays an important role in optic based devices such as

Graphene is unanimously called as a 21st-century wonder mate-
rial as plastic in the 20th century. It is a single-atom thick sheet of
sp2 hybridized carbon atoms arranged in a honeycomb lattice struc-
ture with outstanding properties such as high surface area, high
electrical conductivity, good chemical stability, and strong mechan-
ical strength [1–4]. A great tribute to Noble laureates Prof. Andre
K. Geim and Prof. Konstantin Novoselov, because in the year 2007
the team unveiled the immense potential of graphene in various
application by perceiving its electrical property. Also commented
that “Graphene is a rapidly rising star on the horizon of materials
science and condensed matter physics”, in their pioneer article on
graphene [1]. It is indeed a true statement, graphene started revo-
lutionizing every sector from energy, environment to health [5–8].
Its electrical, optical, and mechanical properties [9–11] are amazing
which makes graphene a highly desirable material for any applica-
tion. Some of the application highlight is as follows; graphene is
fluorescent over a broad range of wavelength owing to its hetero-
geneous electronic structure. Optical transparency, flexibility and
high mobility are attributes of graphene, which is a prerequisite
for superior optoelectronic devices. Nowadays graphene became
an attractive replacement for ITO and other transparent conductor.
∗ Corresponding author.
E-mail address: pvsguna@gmail.com (G. Venugopal).
terahertz devices, optical frequency convertors, optical frequency
convertors and flexible smart windows into next level. Further the
optical absorption of graphene can be changed by adjusting the
Fermi level. Also graphene has been recently recognized as a mul-
tifaceted nanomaterial for cutting edge biomedical application. It
supports biological application from cell scaffolds, drug delivery to
neural interface. Graphene has no untouched field, even in the field
of ultra filtration it has started revolutionizing owing to its high
surface area and 2D sheet morphology. Also it is so far a best mem-
brane for water treatment application. Ultrathin nature of graphene
makes it an attractive candidate for water purification [12]. It has
great potential to treat real waste water. Further it has become
a best candidature for photocatalysis treatment in which it acts
as an electron scavenger, so electron-hole recombination has been
tremendously decreased. Thus improving the overall efficiency of
the catalyst. Therefore graphene is being explored for ultra-fast
transistor [13], supercapacitor [14], memory devices [15], flexi-
ble display [16], light emitting diode [17], battery [18], solar cell
[19], fuel cell [20], water treatment [21] and biological application
[22]. In every venture, the researchers could able to obtain a good
outcome.
Generally, there are two fundamental sources for the prepa-
ration of graphene: graphite and organic molecules. Conversely,
there are several approaches to prepare graphene which are as fol-
lows, CVD on metallic films (Chemical Vapor Deposition, bottom up
approach) [23] and top-down approach includes liquid exfoliation

http://dx.doi.org/10.1016/j.apmt.2017.04.005
2352-9407/© 2017 Elsevier Ltd. All rights reserved.
 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254
Fig. 1. Four typical methods for the mass production of small graphene sheets by exfoliation of bulk graphite.
“Reprinted with permission from W. Ren, H.-M. Cheng, The global growth of graphene, Nat. Nanotechnol. 9 (2014) 726–730, Copyright © 2014, Nature Publishing Group”.
of graphite crystal [24], epitaxial growth on silicon carbide [25],
mechanical cleavage [26], chemical reduction of graphene oxide
[27]. Wen-Cai Ren and Hui-Ming Cheng have demonstrated the
detailed strategy of each method which is shown in Fig. 1 [28].
These are usual approaches to prepare graphene. Every method
has its own merits and demerits; CVD uses organic molecules as
carbon source often in the form of hydrocarbon gas or solid. This
technique needs high operating temperature and expensive sub-
strate like the epitaxial method and its yield is low. Further the
hydrogen released to atmosphere has the tendency to react with
ozone which eventually depletes the ozone layer. The microcleav-
age method is a simple process, the adhesive tape is used in order to
produce graphene from graphite, though it produces good quality
of graphene, yet it is not a not feasible method for mass produc-
tion. On the other hand liquid exfoliation of graphite crystal and
chemical reduction uses graphite as precursor to generate graphene
(reduced graphene oxide), the method is generally known as Hum-
mers’ method. This method often liberates toxic gases. Further
the electrical conductivity of the produced graphene is of several
order less than the pristine graphene since the chemical exfoliation
involves complex chemical process which leads to destruction of
the basal plane structure. Bulk production of graphene is a universal
challenge because depending on the strategy there are considerable
differences in yield, cost, and other properties. Preparation of uni-
form monolayer graphene sheets with high yield and efficiency is a
great challenge. Recently graphene from different sources exclud-
ing graphite also received great attention.
The present review mainly focus on graphene preparation using
different precursor instead of above mentioned precursors. The
waste generation and accumulation has become inevitable, so wise
use of any waste is a commendable approach. Further converting
247
the waste into advance material like graphene is an appreciable
act. Bio-precursor such as chitosan, glucose and alginate etc also
supports the preparation of graphene. Even coal has been used
to prepare graphene quantum dots. The entire review deals with
study of preparation of graphene via different unusual precursors
which is discussed in later section with reference to literature.
Every approach has its own merit and demerit nevertheless each
approach is admirable and novel. If graphene is successfully and
economically produced using biomass or other waste it can be used
for several applications from energy to environment.
1.1. Importance to prepare graphene from different sources
Herein unconventional, inexpensive and biomass related
sources has been identified from literature and discussed. The
chief aim of the review is to bring the attention of environmen-
talist and chemist toward the preparation of graphene in a sensible
way to ease remediation and to augment the innovative approach.
In recent days, the hunt for the graphene preparation with high
yield and good quality has started. Hence, this review will certainly
enable the readers to ponder over other sources which are yet to
be disclosed. Ultimately pose challenges to the researchers to pre-
pare economically viable graphene and enables the researchers for
further improvement of existing preparation strategy.
The requirement of the sustainable resource is inevitable for
any application, so renewable biomass is a sensible entrant for
graphene precursor. In addition, coal has been used as a starting
material, though it is not a renewable resource yet we included due
the innovative and sensible approach involved in the production of
graphene quantum dots. This review illuminates the use of various
precursors such as rice husk, glucose, hemp, disposable paper cups,
248 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254
Table 1
Comparison of different graphene preparation method against parameters such as density, surface area, and conductivity.
Precursor/Method Density (g cm−3 )
Glucose 0.0077
Glucose 3D strutted graphene 0.003
Organic gas/CVD [Ni foam] 0.005
Table 2
Summarized table of different precursors properties and application.
S. No. Novel precursor Thickness of sheet (nm) Specific surface area (m2 g−1 )
1 Rice husk – 2200
2 Glucose 0.35–0.39 820
3 Hemp – 325
4 Paper cups 10–30 – 470
6 Food – 1315
7 Chitosan 1–5 nm 523
and cookies in detail including synthesis approach, mechanism,
and potential application. The resulting graphene material has been
used for diverse application; which is summarized in Table 2. Fur-
ther, Table 3 given at the rear briefly demonstrates the precursor
and approach used to prepare graphene with its respective yield.
2. Different precursors
2.1. Glucose
Glucose is a sugar molecule with formula C6 H12 O6 . It is copi-
ous and renewable carbon source. Most researchers are employing
graphene to detect the presence of glucose non-invasively due to its
exquisite sensitivity to environmental changes [29]. On the other
hand, researchers started using glucose as preparatory material
to prepare graphene. Recently a research team employed glucose
as a starting material to produce graphene with the aid of ferric
chloride [30]. The brief preparation method is given below. Firstly,
the glucose and FeCl3 were dissolved in water and then heated to
80 ◦ C. In which carbonized glucose and FeCl2 (H2 O2 ) was formed.
Subsequent calcination at 700 ◦ C (argon atmosphere) leads to the
formation of graphene and Fe0 . Finally, with the aid of HCl, the Fe
was removed. The author’s claim its electrical conductivity is on a
par with graphene synthesized using the CVD technique. Therein
FeCl3 plays a vital role in producing high-quality graphene because
it acts as template and catalyst. From above method, the mass pro-
duction of graphene from glucose becomes a plausible way. This
simple method can be adopted for graphene preparation from any
biomass. The schematic representation of preparation of graphene
from glucose is given in Fig. 2.
Xin-Hao Li and co-workers also synthesized graphene using
glucose and named with a term “patched graphene” [31]. In
this approach dicyandiamide (DCDA) was added into glucose in
the presence of nitrogen for the temporary in-situ formation of
the layered graphitic carbon nitride (g-C3 N4 ), the DCDA acted as
a sacrificial template. The as-formed g-C3 N4 undergoes a com-
plete thermolysis at 750 ◦ C. Thus, the graphene-like sheets were
generated at higher temperatures. The obtained graphene was
claimed to be highly crystalline and atomically clean graphene.
Further experimentation unveiled the influence of the DCDA addi-
tion to the number of graphene layers. The nitrogen content was
also controlled by heating temperature and reaction time. This
method seems to be good to obtain nitrogen doped graphene since
the nitrogen content is tunable. In modified Hummers’ method,
the substantial aggregation of graphene-oxide into thick flakes
takes place. In this novel approach, the monoliths of continu-
ous entangled thin graphene sheets were created without any
post purification or separation process. The bulk is found to be
Surface area (m2 g−1 ) Conductivity (S m−1 ) Ref.
820 785 [31]
1005 20,000 [36]
850 10 [35]
Electrical conductivity (S m−1 ) Application studies (Ref.)
– Electrochemical performance [41]
785 General [31]
226 Supercapacitor [44]
Fuel cells [45]
– General [47]
– H2 evolution [48]
Fig. 2. Schematic representation of graphene preparation with aid of ferric chloride
solution.
“Reprint with permission from B. Zhang, J. Song, G. Yang, B. Han, K.S. Novoselov, A.K.
Geim, S. V. Morozov, D. Jiang, Y. Zhang, S.V. Dubonos, I.V. Grigorieva, A.A. Firsov, K.S.
Novoselov, et al. Large-scale production of high-quality graphene using glucose and
ferric chloride, Chem. Sci. 5 (2014) 4656–4660, Copyright © 2014, Royal Society of
Chemistry”.
785 S m−1 which agrees well with a CVD technique based prepared
graphene. Yet, calcination at 1000 ◦ C contains 4.3% atom of nitrogen
in graphene. So the complete elimination of nitrogen is difficult. So
this method can be adopted to prepare nitrogen-doped graphene,
which has versatile application in many fields from energy to envi-
ronment [32].
Recently 3D graphene has received great attention because
restacking issue can be significantly resolved in 3D graphene [33].
3D graphene can be prepared via freeze drying method, hydrother-
mal method and CVD technique, each method have its own
advantages and disadvantages. Except the hydrothermal method,
other methods require sophisticated instruments. Yet in hydrother-
mal approach, the yield is too low and unstable approach [34]. The
Ni foam, which is essential in CVD technique is quite costly [35].
Also, freeze drying is essential to obtain 3D graphene. Collectively
the above-mentioned approach is tedious and tiresome. Further,
these methods undoubtedly use graphite and other precursor gases
in order to realize 3D graphene. In addition, conductivity is low
due to poor contact between graphene sheets. Recently, Xuebin
Wang and his co-worker innovatively adapted an old technique
known as “blown sugar” inspired by ancient food art to prepare
3D graphene [36]. This technique is being used to prepare sugar
 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254
Fig. 3. Pictorial illustration on conversion of glucose to graphene.
“Reprinted with permission from Xuebin Wang, Yuanjian Zhang, Chunyi Zhi, Xi Wang, Daiming Tang, Yibin Xu, Qunhong Weng, Xiangfen Jiang, Masanori Mitome, Dmitri
Golberg Yoshio Bando, Three-dimensional strutted graphene grown by substrate-free sugar blowing for high power-density supercapacitors, Nature Commun. 4 (2013),
Copyright © 2013, Nature Publishing Group”.
Table 3
Approach used to prepare graphene and its respective yield.
S. No. Method Graphene
1 Sugar blowing 3D strutted graphene
2 Thermolysis Patched graphene
3 Combustion Graphene sheets
4 Hydrothermal Interconnected carbon nanosheets
5 Chemical treatment N-doped and undoped Graphene sheets
6 CVD Monolayer Graphene
7 Pyrolysis N-doped graphene
balloon for the edible and decorative purpose. In this approach
mere table sugar has been used as a source in order to prepare 3D
graphene and coined a name “strutted 3D graphene” also known as
a 3D graphene bubble network. Therein, the team formed a solution
containing NH4 Cl. Then heated the solution to obtain melanoidin,
which is a glucose-based polymer. The gas generated from NH4 Cl
aided the formation of bubbles. The challenge occurs in balancing
the optimum proportion of glucose and NH4 Cl to obtain a superior
product. Under continuous heating, the syrup drains out along the
bubble wall as the bubble grew. Deoxidation and dehydrogena-
tion gradually transforms the graphitized melanoidin to strutted
graphene. The diagrammatic synthetic protocol is given in Fig. 3.
The estimated cost was found to be $0.5 per gram (laboratory). Also,
realized into high power density supercapacitor (893 kW g−1 at
100 mg−1 ) and the team asserted the structural interconnect hier-
archical porous channel, and huge accessible surface area. Further,
the team demonstrated its high photon/electron transfer ability,
high surface area, and robust mechanical strength. The parameters
such as surface area, density and conductivity graphene against
other precursor based graphene are compared in Table 1. So 3D
graphene via above approach is sensible and robust with good
electrical conductivity compared to the existing method.
2.2. Rice husk
Rice husk is the outer covering of rice kernels. The annual rice
production is in huge million tons. So the rice husk is considered as
a massive agricultural waste. The potential of rice husk has been
recently tapped for the graphene preparation though rice husk
acted as a starting material for the production of activated car-
bon [37]. Due to presence of more amount of Si concentration in
rice husk, it is used to prepare silica and its derivatives [38,39].
Excluding Si the rice husk contains large amount of organic carbon
which is being wasted [40]. Recently researcher’s started deriving
nanocarbon from the same. Luyi and his team prepared biocom-
patible graphene quantum dot from rice husk with the yield of 15%
and confirmed its biocompatibility using cell viability test which
could be suitable for bio-imaging and bio probing. Further, silicon
nanoparticles with huge surface area with the inorganic content
249
Precursor and treatment Yield (wt%) Ref.
Glucose/Chemical treatment and carbonization at Ar atmosphere 16 ± 5 [36]
Glucose/Aid of dicyandiamide 28–60 [31]
Rice husk/chemical activation with KOH 10 [41]
Hemp/Activation with KOH – [44]
Paper cups/with the aid of Fe2+ catalyst – [45]
Food, insect. . ./grown at Cu foil under inert atmosphere – [47]
Chitosan/Chemical treatment under inert atmosphere 30 [48]
were prepared simultaneously [40]. It seems to be a comprehen-
sive utilization of rice husk. The pictorial representation is given in
Fig. 4 as provided in the manuscript. It was prepared by adopting
both top-down and bottom-up approach. The detailed strategy can
be obtained from the manuscript.
Hiroyuki and co-workers adopted a new synthetic method for
the preparation of corrugated graphene via activation of rice husk
with potassium hydroxide (KOH) and substantial calcinations was
done at 1123 K [41]. Therein the KOH has two key roles (i) it assists
in the formation of high purity graphene material containing sta-
ble and clean edges and (ii) induces porosity in carbon materials.
Also, KOH is a strong alkali to remove Si impurities. Herein the
KOH activation creates a continuous 3D network so high volumet-
ric capacitance can be achieved. The hydrogen storage ability of
graphene was demonstrated and found to be excellent owing to
high porosity and enriched active edge. Yet, the team failed to
explain the detailed mechanism of graphene formation.
Further, as mentioned above another researcher used rice husk
to prepare silicon based high capacity lithium battery anode
owing to interconnected nanoporous structure of rice rusk [42].
So before employing rice husk as a starting material for the
mass graphene production, the issues regarding purity should be
answered. Another research team recently prepared graphenated
CNT’s from rice husk by one step microwave plasma irradiation and
demonstrated the electrochemical performance [43]. Graphene
from rice husk seems to be an adoptable approach, yet the qual-
ity of graphene seems to be uncertain due to the formation of CNT
and other carbon product along with graphene. A comprehensive
strategy is required to prepare graphene and other material such Si
and CNT from rice husk. After resolving above points, the rice husk
can be a good option for mass production.
2.3. Hemp
Hemp fiber can be derived from cannabis plant often known as
bast. This plant can withstand varied climatic condition and can be
nourished without fertilizer and pesticides. The fibrous part of the
plant is utilized to prepare products such as rope, clothing, oil and
plastics. Huanlei Wang and his team converted fibrous hemp waste
250 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254

Fig. 4. Comprehensive utilization of rice husks for high quality graphene quantum dots and mesoporous silica nanoparticles.
“Reprinted with permission from Z. Wang, J. Yu, X. Zhang, N. Li, B. Liu, Y. Li, Y. Wang, W. Wang, Y. Li, L. Zhang, S. Dissanayake, S. L. Suib, and L. Sun, Large-scale and controllable
synthesis of graphene quantum dots from rice husk biomass: a comprehensive utilization strategy, ACS Appl. Mater. Interfaces 8 (2016), Copyright © 2016, American Chemical
Society”.

Fig. 5. Schematic of the synthesis process for the hemp-derived carbon nanosheets, with the three different structural layers S1, S2, and S3.
“Reprinted with permission from Huanlei Wang, Zhanwei Xu, Alireza Kohandehghan, Zhi Li, Kai Cui, Xuehai Tan, Tyler James Stephenson, Cecil K. King’ondu, Chris M. B. Holt,
Brian C. Olsen, Jin Kwon Tak, Don Harfield, Anthony O. Anyia, David Mitlin, Interconnected carbon nanosheets derived from hemp for ultrafast supercapacitors with high
energy, ACS Nano 7 (2013) 5131–5141, Copyright © 2013, American Chemical Society”.

into a graphene-like nanomaterial [44]. Hemp waste is an inex- made up of layers of lignin, hemicellulose, and crystalline cellulose.
pensive feedstock material for the commercial use. David Miltin, a If you process it the right way, it separates into nanosheets similar
researcher in the same team stated “Hemp bast is a nanocomposite to graphene”. Fig. 5 depicts the preparation highlights schemat-
 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254
Fig. 6. The formation mechanism of Fe/graphene sheets, graphene sheet and Pt/graphene sheets from disposable paper cups.
“Reprinted with permission from Hong Zhao and T. S. Zhao, Graphene sheets fabricated from disposable paper cups as a catalyst support material for fuel cells, J. Mater.
Chem. A 1 (2013) 183, Copyright © 2013, Royal Society of Chemistry”.
ically; hemp is composed of three layers namely S1, S2 and S3
i.e. inner, middle and outer respectively. The S1 and S3 are com-
posed of semi-cellulose and lignin the middle layer is primarily
crystalline cellulose. Therein a hydrothermal method was used in
order to obtain carbonaceous product and KOH activation was used
to induce porosity. Briefly the fibers were heated for 24 h at around
180 ◦ C in order to dissolve the cellulose and lignin components
and then the resulting material was treated with KOH to create
porous graphene. The sheets obtained are crumpled and contains
holes which is ideal for supercapacitor application. The final prod-
uct was named as “unique interconnected partially graphitic carbon
nanosheets”.
Therein prepared graphene was used for supercapacitor applica-
tion and achieved a power density (a measure of how much power
a given mass of material can produce) of 49 kW kg−1 at 60 ◦ C and
whereas the power density of activated carbon is 17 kW kg−1 at the
same temperature [44]. Graphene from hemp waste outperformed
standard supercapacitor around 200%. This method seems to be the
simple and suitable approach for supercapacitor application due to
crumpled holey nature of graphene sheets.
2.4. Disposable paper cups
The paper cups are mainly made of wood, which is composed of
lignin and hemicelluloses. The disposable paper cup is an extrane-
ous material; however a research team perceived disposable paper
cups differently. Hong Zhao et al. made a novel endeavor by using
the disposable paper cups as a precursor for graphene preparation
with the aid of iron catalyst [45].
The author highlighted three remarkable advantages of this
approach, which are as follows (i) graphene from waste, (ii) higher
yield than conventional approach, (iii) good quality. The brief mech-
anism is as follows, during the activation treatment of paper cups
using KOH, K+ ions get adsorbed into the structure of paper pulp.
Introducing Fe catalyst eventually results in the exchange of Fe2+
ions and K+ ion. Finally, Fe3 C layers are formed when heated at high
251
temperature in a fashion similar to graphitization process. The car-
bon atom diffuses out to form a multiple layers of graphene over the
Fe during the gradual reduction of temperature, thus Fe/graphene
was formed. Finally, the etching process can be utilized in order
to remove Fe ions from graphene. Pt/graphene can be prepared
by replacing Fe ions with Pt ion via galvanic displacement. The
mechanism is given in Fig. 6 as in the research article. The team
demonstrated the fuel cell application of prepared Pt/graphene.
The limiting current density of the Pt/graphene is higher than the
commercial Pt/C electrode [45]. So good catalytic activity is exhib-
ited for ORR (oxygen reduction in a fuel cell). Graphene preparation
from a disposable paper cup is a suitable economical approach since
it uses a cheap starting material. Further, the method seems to be
good due to high yielding. Graphene preparation using a disposable
paper cup is a pioneer work, so further optimization is essential.
2.5. Coal
Coal is a non-renewable source used for energy production
for several decades. Though it is a non renewable energy, yet we
would like to bring under the canopy of graphene preparation
owing to the immense potential graphene quantum dots (QD’s).
QD’s has been prepared using various carbon materials including
fullerene, graphene, graphene-oxide, and CNT, etc. For instance,
the lithography technique has the tendency to etch the graphene
to ∼20 nm width. Yet, lithography is expensive and not plausi-
ble for the bulk quantity production. Recently Rugyan ye et al.
unveiled the potential of coal in graphene QD’s preparation and
claims as, “the exceptional structure of coal is beneficial in prepa-
ration of graphene QD’s by utilizing various types of coal, namely
anthracite, bituminous and coke as the precursor to generate tun-
able graphene quantum dots” and demonstrated the unique coal
structure has an advantage over pure sp2 -carbon allotropes for the
generation of quantum dots [46]. The comprehensive synthesis and
essential characterization is given in Fig. 7. The author claims the
above method of graphene preparation as a facile approach since
252 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254

Fig. 7. b-GQDs (bituminous coal quantum dot) synthesis and characterization. (a) Macro-scale image and simplified illustrative nanostructure of coal. (b) SEM image of
ground bituminous coal with sizes ranging from 1 to hundreds of microns in diameter. Scale bar, 50 mm. (c) Schematic illustration of the synthesis of b-GQDs. Oxygenated
sites are shown in red. (d) TEM image of b-GQDs showing a regular size and shape distribution. Scale bar, 20 nm. (e) HRTEM image of representative b-GQDs from (d); the
inset is the 2D FFT image shows the crystalline hexagonal structure of these quantum dots. Scale bar, 2 nm. (f) AFM image of b-GQDs showing height of 1.5–3 nm. Scale bar,
100 nm.
“Reprinted with permission from R. Ye, C. Xiang, J. Lin, Z. Peng, K. Huang, Z. Yan, P. Cook Errol, L.G. Samuel, C. Hwang, G. Ruan, G. Ceriotti, A. Rahman O. Raji, A. James, M. Tour,
Coal as an abundant source of graphene quantum dots, Nature Commun. 4 (2013), Copyright © 2013, Nature Publishing Groups”.

the crystalline carbon within the coal structure is easier to oxida- ration approach is interesting and sensible, the yield is a matter of
tively displace than when pure sp2 -carbon structures are used. concern.
Graphene quantum dots prepared using coal can be realized for
several applications by impregnating it with structural composite
material. 2.7. Chitosan

Chitosan is an N-containing renewable biopolymer. It is

2.6. Food, insect, and waste
Gedeng Ruan and his team developed an economic approach for
graphene preparation from strange inexpensive raw carbon con-
taining material without pre-purification (cookies, chocolate, grass,
plastics, cockroaches and dog feces) [47]. CVD technique was used
in order to grow graphene directly on the backside of a Cu foil at
1050 ◦ C for 15 min under H2 /Ar flow. Later the Cu foil was removed
by etching. The residual particles were found on the front side of a
Cu foil and no residual particles were observed on the back side of
the coil. The diagrammatic representation (Fig. 8) is given below.
Therein XPS data clearly reveals the purity of the carbon. In raw
carbon source, the presence of O, N, Fe, S, and P were observed but
in obtained graphene, none of this element were present, which
confirmed the pristine graphene composition. Though the prepa-
obtained from the hard outer skeleton of crustacean. It is a fibrous
substance used to treat high cholesterol. Ana Primo and team
demonstrated the N-doped graphene preparation from chitosan
using pyrolysis technique [48]. Chitosan film was heated at 800 ◦ C
under argon gas atmosphere to give high quality single layer N-
doped graphene film with 99% transmittance. Also, the team used
the same as photocatalyst to generate hydrogen under stimulated
sunlight illumination. Recently Pin Hao et al. demonstrated the
preparation of graphene based self doped nitrogen aerogels derived
from chitosan [49]. A detailed formation is also given, which can
be derived from the manuscript. Initially carbonized aerogel com-
posed of graphene framework was prepared. Then the residual
amorphous carbon was etched away by increasing the activation
temperature. The prepared nitrogen based carbon was realized
into supercapacitor which displayed the specific capacitance of
 N. Raghavan et al. / Applied Materials Today 7 (2017) 246–254 253

Fig. 8. (A) Diagram of the experimental apparatus for the growth of graphene from food, insects, or waste in a tube furnace. On the left, the Cu foil with the carbon source
contained in a quartz boat was placed at the hot zone of a tube furnace. The growth was performed at 1050 ◦ C under low pressure with a H2 /Ar gas flow. On the right is a
cross view which represents the formation of pristine graphene on the backside of the Cu substrate. (B) Growth of graphene from a cockroach leg. (a) One roach leg on top
of the Cu foil. (b) Roach leg under vacuum. (c) Residue from the roach leg after annealing at 1050 ◦ C for 15 min.
“Reprinted with permission Gedeng Ruan, Zhengzong Sun, Zhiwei Peng, James M. Tour, Growth of graphene from food, insects, and waste, ACS Nano 5 (2011) 7601–7607.
Copyright © 2011, American Chemical Society”.

197 F g−1 at a current density of 0.2 A g−1 . An extensive study of
graphene derivatives preparation exclusively from polysaccharides
has been reviewed by Terzopoulou et al. [50].
3. Future prospective of different precursors in graphene
production
Bulk Graphene preparation using different precursor is a sen-
sible approach. Successful and economical preparation leads to
the utilization of graphene in several applications from energy to
environment. The improvement of material constantly presents
surpassing effect in any field. Graphene preparation is a vital field
for material scientists due to its extensive property. So the ratio-
nal graphene preparation will always receive its due salutation in
the scientific community. More investigation is needed to opti-
mize the preparation method. For instance, the optical absorption
of graphene can be varied by tuning the Fermi level [51]. So an
extensive study on Fermi level of graphene is highly required
for any optical and electronic application. In field effect transis-
tor application, the polycrystallinity nature of graphene greatly
affects the transconductance [52]. Further, the quality level of the
resulting graphene is not plainly discussed for any intended appli-
cation. Therefore the performance metrics of graphene prepared via
unconventional method is vague. Detailed study of quality aspects
will pave way for the use of graphene in specific application. It is
believed each precursor based graphene has its own unique appli-
cation based on its properties and quality. For instance graphene
prepared from waste dry cell has been extensively for electronic
applications and it seems to be good for the mentioned application
[53].
4. Conclusion
In conclusion, all the above-discussed graphene preparation
routes are sensible and innovative. Yet, most of the studies have
not dealt systematic characterization at atomic level, inherent
property and application. For instance, calcination and alkaline
treatment makes the process intricate to assess the detailed growth
mechanism of graphene. Further the edges and defect distri-
bution of graphene obtained using different precursor has not
been addressed plainly. As already mentioned, the Fermi level of
graphene aspects was not dealt. Further light is required on mate-
rial purity aspects. On the other hand we believe this review will
open a window of opportunity for a breakthrough in the develop-
ment of graphene from different precursor. Because all the methods
dealt in this review seems to be rapid, reliable, efficient, scalable and
cost effective for several useful applications such as supercapacitor,
next generation water filter, fuel cell, H2 generation, etc.
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