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j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 0 ; 9 ( 6 ) : 1 5 9 2 4 e1 5 9 5 1
Available online at www.sciencedirect.com
journal homepage: www.elsevier.com/locate/jmrt
Review Article
Advances in synthesis of graphene derivatives

using industrial wastes precursors; prospects and
challenges
Rabia Ikram a,*, Badrul Mohamed Jan a, Waqas Ahmad b

a
Department of Chemical Engineering, University of Malaya, 50603, Kuala Lumpur, Malaysia
b
Institute of Chemical Sciences, University of Peshawar, Peshawar, 25120, Pakistan
article info abstract
Article history: Graphene, a two-dimensional single layered carbon atoms crystal lattice has grabbed much
Received 2 September 2020 attention due to its unique electronic, surface, mechanical and optoelectronic character-
Accepted 17 November 2020 istics. Owing to its unique structure and properties, graphene has opened new opportu-
Available online 23 November 2020 nities for the future systems and devices, which has led to increase its demand in
numerous applications. However, scaling up its production is still a challenging job.
Keywords: Although there is a huge body of literature on the graphene synthesis using various
Graphene synthetic routes techniques but eco-friendly and costeeffective processes for mass scale production are still
Waste precursors needed. In order to conceptualize and develop the processes fulfilling the growing con-
Carbon sources cerns, it is important to overview the existing literature. The current review summarizes
Materials processing the production of graphene using several approaches as well as the potential of various
Mass production waste materials as graphene precursors. The methods used for graphene synthesis have
been categorized into top down techniques such as chemical exfoliation, mechanical
exfoliation and chemical fabrication processes, and bottom up techniques including py-
rolysis, plasma synthesis, epitaxial growth and chemical vapor deposition (CVD) processes.
Conversely, several limitations are considerate for an individual procedure such as toxicity
of chemicals, high-cost, time consumption or inadequate quality of the product. Further-
more, mass production of graphene derivatives under low-cost can also be considered by
utilizing a variety of wastes precursors such as plastic and batteries waste, newspaper,
biomass, chitosan, coal, insects waste etc. This review designates the current advances in
wastes-derived graphene synthesis to relief synthetic difficulties as well as predicts the
future development in this area.
© 2020 The Authors. Published by Elsevier B.V. This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
* Corresponding author.
E-mail address: [email protected] (R. Ikram).
https://doi.org/10.1016/j.jmrt.2020.11.043
2238-7854/© 2020 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 0 ; 9 ( 6 ) : 1 5 9 2 4 e1 5 9 5 1 15925
down method [28] have been successfully utilized for gra-

1. Introduction phene synthesis.
Likewise, various strategies have been designed for the
Recycling wastes precursors to synthesize graphene-based synthesis of graphene derivatives. Earlier studies have
materials into value-added products has inspired re- demonstrated conventional methods which has grabbed
searchers for industrial applications [1]. Waste materials enormous attention of scientific community [26,29,30]. For
ranging from household to various industries create destruc- example, synthesis of graphene 2D-heterostructures was
tive effects on environmental and hygiene factors [2]. Based discovered for scale-up production [31,32]. Furthermore, syn-
on earlier assessments, global cities have produced 1.3 billion thesis of 3D nanostructured graphene was reported in the
tons of wastes per annum with Asia responsible for 1 million form of nanoshells, hydrogels, graphene foams, aerogels and
tons per day. With current developments and population encapsulates with improved properties for biomedical and
growth rate, the worldwide wastes generation has been esti- environmental applications [33]. Other methods such as laser
mated to rise to 2.2 billion tons by 2025 [3]. It is a known fact induced synthesis [34], nitrogen-doped synthesis [35,36] and
that wastes conversion significantly varies due to the type and nanoparticles-assisted quartz substrate synthesis [37] and
composition of waste precursors. For instance, conversion of exfoliation with alkali halide salts [38] have been examined for
biomass such as cellulose, chitosan or rice husk depends on graphene preparation.
their variety of sources [4,5]. Conversely, none of the above-mentioned studies have
In 2007, the real journey of graphene has revealed by Nobel reported the impact of waste precursors into graphene de-
laureates by observing its electrical characteristics and huge rivatives. In recent studies, Kong et al. have evaluated biomass
potential in various applications. They stated that “Graphene precursors into graphene derivatives using pyrolysis process
is considered as a rising star on the horizon of condensed for various industrial applications [28,39]. Besides, grafting of
matter physics and materials science”, in their pioneer significant graphene derived nanocomposites have been
research on graphene [6,7]. Graphene, a solidly known wonder reinforced by metal oxides for highly selective energy storage
material of 21st century has obtained from a single sheet of applications [36,40e43]. For better engineering perspectives,
graphite (Gr). This single sheet contains a single-atom of sp2 effects of graphene derivatives through their morphology,
hybridized carbon atoms organized in a structure of honey- structure and properties such as electrical [44], mechanical
comb lattice with exceptional characteristics such as strong [45], and optical [46] have been thoroughly emphasized.
mechanical strength, high electrical conductivity, chemical Prior to graphene synthesis, conversion of industrial
stability, and improved surface area [8e10]. Over the years, wastes into graphene-based materials is an emerging concern
graphene has revolutionized from nanotechnology, health, of current era. However, fabrication of eco-friendly tech-
and energy to environment [11]. Potential characteristics of niques to produce high-quality and scale-up production of
graphene such as optical transparency, flexibility, high graphene is challenging. We aim to abridge the state of the art
mobility, fluorescent over a wide range of wavelength due to knowledge of waste precursors to convert graphene. Bio-
its heterogeneous electronic structure are desired features for wastes, plastic wastes and other low-cost industrial sources
the optoelectronic devices [12,13]. Graphene has also been have been considered from the literature. Since recent ap-
lately identified as a multifaceted nanomaterial for advanced proaches are concerned for synthesis of fine and uniform
biomedical applications [14]. Newly, conversion of batteries graphene sheets. Herein, inexpensive and unconventional
waste into graphene has conveyed an essential role for sources have brought attention of scientists to disclose un-
advanced devices including optical frequency convertors, used precursors and improvement of graphene preparation
smart conductive films and terahertz devices [15]. Similarly, for fundamental applications. Renewable bio-sources can find
value-added reuse of tyre wastes into graphene has examined sensible graphene precursors. This review will pave a way for
for cost-friendly and scalable production [16]. researchers to discover unusual waste precursors for
Graphene has begun revolutionizing due to its 2D sheet economical and commendable production of graphene into
morphology that has a high surface area even in ultra- several biological, environmental and other industrial
filtration area. Typically, 3D materials consist of 100 layers applications.
of thick sheets stacked over each other [17]. Gr as a 3D mate-
rial formed multiple monolayers of carbon atoms as building
blocks in a 2D honeycomb lattice [18]. Additionally, mono- 2. Methodology
layered, bi-layered and multi-layered graphene ranged be-
tween 3 and <10 layers have reported significant and unique The objective of the current literature review was to compile,
properties for desired applications [19,20]. Multiple ap- analyze and identify the current investigations pertaining to
proaches have been implemented to produce required gra- graphene synthesis processes in order to provide wide-
phene layers. Primarily, mechanical exfoliation (high oriented ranging information to the research groups working into
pyrolytic Gr) has been presented as a reliable method [21]. Due divergent fields. In this study, systematic literature review
to lack of qualitative production of graphene, it paved a way to methodology was adopted [47]. The protocol consisted of
look forward to other methods. Later, graphitization process three main steps; search process, selection of the study fol-
using SiC [22], laser-induced graphene [23], calcination [24], lowed by analyzing and reporting. An organized search pro-
solvothermal [25], and hummers method [26] were reported as cess was conducted to collect all the digitally available
chemical methods. In addition, chemical vapor deposition information on the sources and techniques for graphene
(CVD) as a bottom-up approach [27], and pyrolysis as a top- synthesis. Relevant sources of literature i.e. journal articles,
15926 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 0 ; 9 ( 6 ) : 1 5 9 2 4 e1 5 9 5 1
review papers, books, conference proceedings etc. were product. After many attempts, graphene synthesis was con-
collected from digital libraries. The libraries searched ducted again in 1999 [49,50]. Though Novoselov et al. [51]
included the, Web of Science, Science Direct, Elsevier, credited for the discovery of graphene in 2004. They have first
Springer, Taylor and Francis, Google scholar, American revealed the synthesis of graphene using exfoliation process.
Chemical society (ACS), Wiley Online Library, Royal society of The method was followed with efforts to develop new tech-
Chemistry etc. niques for effective and large-scale production of graphene.
After collecting a large number of literature sources, most In the last decade, several methods were established and
relevant sources were screened by filtering less relevant utilized to synthesize graphene. The most commonly used
literature. The focus of selection remained the techniques for graphene synthesis methods are mechanical exfoliation [52],
synthesis of graphene derivatives and graphene synthesis chemical exfoliation [53], chemical synthesis [54], and CVD
from different waste materials. The most closely related pa- method [55]. During chemical exfoliation route, Gr dispersed
pers were picked by its relevance form the title, abstract and into solution was chemically exfoliated by introducing large
contents and irrelevant sources were excluded. Moreover, the amount of alkali ions between the layers of Gr. Later, chemical
collected literature was sorted out based on the reported type exfoliation applied for the synthesis of graphite oxide (GrO) as
of techniques and the nature of product (graphene and its well. Other commonly used graphene synthetic routes are
derivatives) formed. It was also focused on the starting ma- presented such as unzipping process of carbon nanotubes
terial used for synthesis along with experimental conditions (CNTs) [56] and microwave process [57]. Despite the ability of
utilized during each process. All the data and concerned in- mechanical exfoliation route to synthesize graphene into few-
formation was analyzed for comparisons after compilation. layers, the limitation of this method has provided variation
Advantages and shortcomings are presented in the form of between graphene layers. A thickness of up to 10 nm has been
tables, graphics and typescript. Finally, recommendations, found which is 30 times thicker than normal graphene layer.
future prospects and conclusions were presented. The design Thermal chemical vapor deposition (TCVD) has demonstrated
of followed methodology in this study is displayed in Fig. 1. as most substantial route for the production of large-scale
graphene [58]. TCVD is a modified type of CVD route which
has been conducted in a resistive heating furnace. Further-
3. Graphene synthetic routes more, plasma enhanced CVD or PECVD is another reliable
route which includes plasma-assisted growth due to reacting
Graphene synthesis refers to any method used to synthesize gases [59].
or fabricate graphene depending on the desired purity and On the other hand, all of these synthesis routes also exhibit
size of the product. The first attempt of monolayer Gr syn- some limitations and challenges based on the desired gra-
thesis was investigated in early 1975. Lang et al. [48] revealed phene applications. For example, the mechanical exfoliation
the formation of Gr with mono and multi-layers by using route has the ability to produce monolayer and few-layers
carbon thermal decomposition process on single platinum graphene. However, producing a consistent graphene struc-
substrates. Nevertheless, due to inconsistency between Gr ture using this route is too difficult. Besides, chemical syn-
sheets formed on different platinum crystal surfaces, failure thesis route has been conducted in low temperature
was exposed to recognize the valuable applications of the condition. It has been emerged as a suitable process to
Fig. 1 e Methodology adopted for literature survey and review in this study.
synthesize graphene on multi-types of substrates at ambient comprising van der Waals forces among stacking of sheets.
temperature, specifically on polymeric substrates [19,52]. Exfoliation has been considered as a reverse step of
Furthermore, graphene has been converted to reduced gra- stacking which caused poor bonding and big lattice
phene oxide (rGO) through chemical synthesis due to incom- spacing in the perpendicular direction. During the lattice
plete GrO reduction. This process has caused a successive plane with hexagonal formation, it leads to tiny lattice
debasement of the electrical characteristics based on its spacing and better bonding [81]. In mechanical exfoliation
reduction degree [58]. Epitaxial graphene growth is another technique, graphene has been detached from a Gr crystal
route used to synthesize graphene by applying thermal using adhesive tape. By means of repeated taking off,
decomposition on the surface of Silicon carbide (SiC). Addi- multi-layers of graphene were cleaved into single layers
tionally, this route has been presented strong limitations to and flakes. Further, acetone was used to detach the gra-
produce graphene such as the requirement of high tempera- phene from the tape. Therefore, various types of graphitic
ture as well as the incapability to transfer on other substrates materials such as mono-crystal Gr [82], highly ordered
[60]. Graphene has been synthesized using two diverse pyrolytic Gr [83], natural Gr [84], and synthesis of graphene
methods, either top-down method or bottom-up method [61]. sheets with different thickness have been observed using
The process flow chart is shown in Fig. 2. A brief summary of mechanical exfoliation technique. This exfoliation method
graphene synthetic routes is displayed in Table 1. has been conducted using agents like transfer printing
technique [85], ultra-sonication [86], electric field [87], and
3.1. Top-down methods scotch tape [88].
The limitation of mechanical exfoliation comprises low
3.1.1. Mechanical exfoliation yield of graphene. Also, the flakes of graphene need to be
Mechanical exfoliation has been considered as an inex- found on the surface of the substrate which has observed as
pensive way to synthesize graphene. It is one of the com- labor exhaustive. The characteristics and the quality of gra-
mon approaches used to synthesize monolayer graphene phene has been utilized to produce field electric transistor
flakes on favored substrates. It has been one of the earliest devices [89]. Nevertheless, synthesis of graphene has required
recognized method to produce graphene. This method has improvement for high purity and large scale production using
been applied in nanotechnology where the superficial mechanical exfoliation.
layered materials experience either longitudinal or trans-
verse stress [62]. Gr formation was occurred when the 3.1.2. Chemical reduction of graphite oxide
single carbon atoms of graphene stacking via van der Another top-down method to produce big amount of gra-
Waals forces for the interlayer data followed by the bond phene is chemical reduction of GrO. It is one of the conven-
energy value and distance at 2 eV/nm2 and 3.34 A respec- tional techniques used to synthesize graphene in large
tively [79]. Nonetheless, mechanical cleaving requires up amounts [90]. GrO has been commonly obtained from the
to 300 nN/mm2 of external force to separate single atomic oxidation process of Gr using some oxidants comprising po-
layer from Gr [80]. Perpendicular overlapping of partially tassium permanganate, nitric acid, and concentrated sulfuric
filled p orbital onto the plane of sheet have been occurred acid as reported in hummers method [91], Staudenmaier
Fig. 2 e Schematic flow of graphene synthetic routes [61] (With permission from Elsevier).
Table 1 e Summary of graphene synthetic routes.

Synthesis routes No. of layers Advantages Limitations Ref.
Top-down methods
Mechanical exfoliation Multiple layers Uniform and large size of Small amount of prepared [61,62]
layers graphene
Gr sonication Mono/multiple layers Fine layers of graphene, Small amount of prepared [63,64]
Low-cost graphene,
Separation issues
Graphene Mono/multiple layers One step functionalization High cost, [65e68]
functionalization/ and exfoliation, Require ionic liquids
electrochemical Functionalized graphene
exfoliation with high electrical
conductivity
Gr acid dissolution Mono layer Modified layers of graphene Use of toxic acids, [69,70]
for high scale-up Requires removal of acids,
production Additional cost
Bottom-up methods
CVD Multi-layers High amount, Difficult to scale up [61,71]
Large size
Epitaxial growth on Silicon Multi-layers Large surface area Time consuming process [61,72]
Carbide
Arc discharge Mono, bi and multi-layers Generates about *10 g h1 of Presence of carbonaceous [61,73]
graphene impurities,
Low graphene yield
GO Reduction Multi-layers Un-oxidized graphene Graphene was [74]
layers contaminated by
aluminium sulfide/oxide
CNTs Unzipping Multi-layers Controlled thickness by Oxidized graphene [75]
selecting nanotubes High-priced raw material
Confined self-assembly Monolayer Measurement control of Low yield [76e78]
thickness
method [92], and Brodie method [93]. Another technique used step method [105]. Initially, increase of Gr interlayer spacing
for graphene synthesis includes reduction of graphene oxide triggered reduction of van der Waals forces between the in-
(GO) and sonication. H2 addition occurred using alkenes terlayers. Then, sonication or fast heating process has been con-
together with the nitrogen gas extrusion, excess of NaBH4 was ducted to exfoliate Gr into single and few layers. Ultra-sonication
utilized as a reducing agent [94]. Another reducing agent uti- process is usually required to extract monolayer graphene.
lized contains hydroquinone [95], ascorbic acid [96], glucose Subsequently, the development of hummers method led to
[97], hydroxylamine [98], phenyl hydrazine [99], pyrrole and the establishment of modified and improved hummers
alkaline solutions [100]. method [106]. To compare these developments, type of oxi-
Electrochemical reduction has considered as another route dants, and significant disadvantages and advantages are dis-
to produce graphene in large amounts. Primarily, production cussed in Table 2. Recent reviews have summarized the
of rGO monolayer was reported in year 1962 [101]. The solution performance of improved hummers method and other
of GrO was sonicated for GO formation. Then, the functional appropriate approaches due to toxic free capability and uni-
groups like oxygen were removed using hydrazine as a form structure of graphene synthesis [17,61,62,107].
reducing agent. In addition, the process of reduction found to The process of chemical exfoliation consists of two main
be imperfect due to remaining oxygen group [101]. GO is a steps. The first step reduces the interlayer forces to produce
valuable material due to its hydrophilic nature. GO was sus- graphene-intercalated compounds [113]. Later, it exfoliates Gr
pended in water by using sonication process by subsequent to graphene with mono to multi-layers by applying sonication
deposition on to surfaces by filtration or spin coating to pro- or fast heating. Usually, mono-layer graphene or GO utilize
duce mono- or bi-layer GO [102]. Later, graphene films formed ultrasonication process [114], while multi-layer graphene/GO
by reducing the GO either chemically or thermally. One-step utilize density gradient ultracentrifugation [115]. Graphene
solvothermal reduction process generated the dispersion of has been usually synthesized using hummers method
reduced GO in organic solvent [103]. A schematic flow of gra- including oxidation process of Gr/GrO with strong oxidizing
phene platelets synthesis into Gr functionalization through agents like NaNO3 and KMnO4 in H3PO4/H2SO4 [116]. A mixture
ball milling is presented in Fig. 3. of water/dimethyl formamide (DMF) (1:9) also utilized ultra-
sonication to synthesize monolayer graphene. Thus, spacing
3.1.3. Chemical exfoliation of interlayer increases up to 9.5 A. Monolayer graphene has
Chemical exfoliation has been considered as the best top-down been distributed by chemical reduction with hydrazine for
approach used to synthesize graphene. It carried out in a two- functional group reduction [117].
Fig. 3 e Surface-functionalized graphene platelets through ball milling of Gr in the presence of an aryl diazonium salt [104]
(With permission from Elsevier).
3.2. Bottom-up techniques for lithium ion capacitors [119], production of lignin-based
graphene through pyrolysis at 900 C for 3 h and 5 C/min
3.2.1. Pyrolysis for energy storage applications [120], synthesis of elephant
Pyrolysis has been reported as a friendly procedure to derive grass into graphene-derived materials through pyrolytic
highly graphitic carbon materials (HGCM). Principally, it is a optimization (350/600/900 C) for waste-water treatment [121],
bottom-up technique for preparation of Gr derivatives under and pyrolytic synthesis of numerous types of plastic wastes
high temperature and non-oxidizing atmosphere. Designed into graphene nanosheets have been outlined for industrial
pyrolysis of various waste precursors have testified produc- applications [122]. In some cases the pyrolysis has been
tion of graphene-derived materials [28]. Recent studies have assisted by solvothermal techniques [123]. For example, using
narrated conversion of industrial wastes into graphenaceous a 1:1 of molar ratio of sodium and ethanol has been used in the
materials. Wang et al. have prepared graphene following one- reactor vessel during thermal reaction. Sodium ethoxide py-
step AC arc plasma pyrolysis. The method involved a mixture rolysis via sonication have improved the performance of
of hydrogen and methane gas under carrier gas (Ar) to produce graphene sheets detachment. The produced graphene sheets
few-layered graphene at optimum conditions for lithium are measured up to 10 mm [124]. Likewise, sodium ethoxide
battery applications [118]. More interestingly, other recent has been directly used for thermal pyrolysis under nitrogen
sources of wastes using pyrolysis have been used for scale-up atmosphere [125]. Lately, researchers have reported an
production of graphene. For example, conversion of coffee- extensive summary of graphene-derivatives production used
waste into graphene at 800 C for 1 h under Ar atmosphere for a wide range of applications [126].
Table 2 e Overview of Chemical exfoliation methods for graphene synthesis.

Method Year Oxidizing agents Toxicity Advantages Limitations Ref.
Brodie 1859 Nitric acid, Potassium Yes Large surface area of Unsafe process, Time [108]
chlorate graphene consuming,
Structural defects in
graphene, Limited
thickness & small size, Easy
diffusion in alkali solutions
Staudenmaier 1898 Sulfuric acid, Yes Easier than Brodie process Unsafe process, Time [109]
Nitric acid, consuming
Sodium chlorate, Potassium
chlorate
Hummers 1958 Sodium nitrate, No Increased level of oxidation Time consuming, [110]
Sulfuric acid, as compared to Brodie and Slow separation and
Potassium permanganate Staudenmaier method. purification,
Inadequate oxidation
Modified 2008 Sodium nitrate, No Enhancement in level of Time consuming, [111]
Hummers Sulfuric acid, Potassium oxidation level which Slow separation
permanganate improves graphene
performance
Improved 2010 Phosphoric acid, No Large surface area of Time consuming, [112]
Hummers Sulfuric acid, graphene as compare to Slow synthesis
Potassium permanganate conventional methods,
Less number of defects in
the basal plane, Higher
amount of GrO formed,
attained better production
of graphene/GO,
Environmentally friendly
3.2.2. Epitaxial growth substrate, ultra-high vacuum annealing produces small areas,
Epitaxial growth on the surface of silicon carbide (SiC) is one of about 30e100 nm of graphene [132]. Graphene prepared at a
the common bottom-up techniques used for graphene pro- very high temperature (<1000 C) in ultra-high vacuum
duction. The epitaxial term has been derived from the Greek, graphitization due to silicon evaporation by SiC thermal
the first part “epi” refers to upon or over word, while second decomposition [133].
part “taxial” refer to arrange or order word. During this pro- Epitaxial growth process of graphene using SiC substrate
cess, a single crystalline SiC film has been deposited on the has been found as a promising technique for graphene
substrate which creates a new film. Thus, this method is commercialization as well as graphene production in large-
called epitaxial growth. It generates high-crystalline film of scale for electronics applications. Graphene on the substrate
graphene onto single-crystalline substrates of SiC [127]. of SiC can generate high-frequency electronics [134], radiation
Generally, there are two processes types of epitaxial hard devices (RHD) [135], and light emitting devices (LED) [136].
growth based on the type of the substrate, either homo- or High-frequency transistors were also fabricated with cut-off
hetero-epitaxial growth. During the process, the film is frequency at 100 GHz [137]. Graphene on SiC was recognized
deposited on a same material of substrate material which is as a unique resistance standard based on the quantum hall
known as homo-epitaxial. When the substrate and film are effect (QHE) [138]. However, it has been considered as an
different materials, it is known as a hetero-epitaxial. The first expensive process.
application of silicon carbide SiC was used in electrical mea-
surements on patterned epitaxial. Later in year 2004, SiC was 3.2.3. Chemical vapor deposition
used as a wide band gap semiconductor (3 eV). The heat CVD is another technique excessively utilized to synthesize
treatment was carried out in the temperature range between graphene. CVD has been known as the deposition of gaseous
1000 and 1500 C in a vacuum pressure (about 1010 mbar) reactants onto a substrate [139]. This technique has been
produced Gr on both of the SiC polar planes (0001) [128]. operated using mixture of gas molecules in a reaction cham-
Studies have proved to synthesize ultrathin Gr containing ber under optimum conditions. A material film has been
mono to few layers of graphene on Si completed (0001) face of formed on exterior substrate when the mixed gases touched
single-crystal 6HeSiC substrate to investigate its electronic the substrate in heated reaction chamber. Subsequently, the
characteristics [129]. The graphene growth rate on the SiC waste gases discharged from the reaction chamber. Though
substrate has been based on the specific polar SiC crystal face the substrate temperature has been considered an important
[130]. The formation of graphene on the C-face was much condition to confirm the reaction occurrence. During the
faster than the graphene formation on the Si-face. On the C- process of CVD, coating has been conducted on the substrate
face substrate, bigger areas (about 200 nm) of multi-layered in a very small amount with extremely low speed as in mi-
graphene are synthesized [131]. While on the Si-face crons/hour. This process is analogous to the physical vapor
Fig. 4 e Schematics of CVD graphene grown on (a) metals with high carbon solubility, (b) Cu foil, (c) Cu enclosure, and (d)
sapphire [144] (With permission from Elsevier).
deposition (PVD) and a simple difference has been found due Thus, the sputtered atoms diffusion occurs through plasma
to the precursors in solid phase [140]. The vaporization of solid and release impure atoms while graphene synthesis.
substances and solids deposition onto a substrate by Whereas, ICP-PECVD has been known as a process that ap-
condensation has been conducted as presented in Fig. 4 [141]. plies wave heating and produces plasma without electrodes
There are two main processes used to conduct CVD, [148].
which are ultra-high vacuum chemical vapor deposition Plasma constraints application comprised of gas flow rate,
(UHVCVD), and low pressure chemical vapor deposition temperature, and pressure in the reaction cavity which car-
(LPCVD) [142]. LPCVD has been known as operated under ried out via ICP-PECVD. Hence, the growth period and power
sub-atmospheric pressures to prevent needless reactions of generated plasma has been adjusted accurately. However,
and increased production of same coating thickness on this process has been considered as less effective, yet envi-
substrate. Whereas, UHCVD has been operated under ronmentally friendly and scalable. In MW-PECVD, the wave
extremely low atmospheric pressures which is about heating is used to generate plasma. During the process, wet
6e10 Pa [143]. etching and transfer are not included and therefore, none of
the remaining metallic impurities, polymer pollution, and
3.2.4. Plasma synthesis metal catalysts are found on generated graphene films [149].
Other than UHVCVD and LPCVD, plasma synthesis is another Table 3 summarizes graphene synthesis and its significant
method of graphene synthesis. It includes both plasma doping characteristics by CVD technique.
and plasma-enhanced chemical vapor deposition (PECVD) to
exfoliate graphene [145]. Numerous plasma types such as 3.2.5. Unzipping method
electrons, highly reactive radicals, energetic ions, a fraction of Plasma-etched and chemical process have been used in
associated source gas and photons tend to vary the synthesis CNTs unzipping. Graphene nanoribbon has been designated
progressions. Nonetheless, they achieved more actively as as a thin elongated strip of graphene that reveals straight
compared to the ground-state types and consequently high edges. It has exposed an electronic state change from
temperatures found necessary in order to conduct chemical semimetal to semiconductor which was based on the
reactions. PECVD method has been divided into three routes, nanotube width [158]. Mono or multi-layers of graphene
which are direct current plasma-enhanced chemical vapor have been synthesized through single or multi-walled CNTs.
deposition (DC-PECVD), induced coupled plasma-enhanced These carbon nanoribbons width formed grounded on the
chemical vapor deposition (ICP-PECVD), and microwave CNTs dimensions (i.e., diameter). Multi-walled nanotubes
plasma-enhanced chemical vapor deposition (MW-PECVD) recognized by ammonia (NH3) and lithium (Li). Dry tetra-
[146]. During DC-PECVD, plasma sustainability has been hydrofuran (THF) with liquid ammonia (NH3) has used in the
depended on secondary electrons produced by accelerated formation of multi-walled nanotubes [159]. It was observed
ions attacked by electrodes [147]. For example, when the that about 60% of these nanotubes were completely exfoli-
plasma ions and atoms attack cathode, atoms tend to release. ated while about 5% of multi-walled nanotubes were
Table 3 e Brief illustration of graphene synthesis and its characteristics by CVD methods.
CVD Type Pressure Temp. Graphene Characteristics Ref.
Synthesis of Graphene on polycrystalline 1 atm 1000 C Few layer of Graphene [150]
Nickel substrate
Gr thin layer on Nickel substrate 40e80 mT 950 C DC current discharge was 0.5 A cm2 [151]
Graphene layer in nm thickness
Synthesis of Graphene on polycrystalline Nill 900e1000 C Nil [152]
Nickel substrate by wet-etching
Growth of Graphene sheet on e-beam Nill 1000 C The transmittance was about 80% [153]
evaporated Nickel The resistance was 280 U sq1
Large-scale of Graphene monolayer
Deposition of catalytic graphene on 40 mT 1000 C The range of thickness from mono to few [154]
Copper foil 500 mT 1000 C layers graphene
Gram-scale graphene using Magnesium 40 mT 1000 C No substrate [155]
Oxide compound Few layers of graphene
Graphene roll-to-roll synthesis on a 90 mT 1000 C Nill [156]
polymer substrate 460 mT 1000 C Nill
Growth of Graphene on rectangular Nill 1000 C Nill [157]
Copper foil (15 5 cm)
partially exfoliated. Oxidizing agents such as hydrogen 3.3. Other methods

peroxide (H2O2), potassium permanganate (KMnO4), and
sulfuric acid (H2SO4) were used for the oxidation of CNTs Other than top-down and bottom-up techniques, several
[160]. Researchers stated the diameter of multi-walled other techniques presented to produce graphene. One of these
nanotubes between 40 and 80 nm and expanded up to techniques is Arc discharge which synthesized graphene with
100 nm. The conversion of multi-walled nanotubes to gra- rapid heating process and 1 atm pressure. The best conditions
phene nanoribbon is illustrated in Fig. 5. applied in order to form graphene are high hydrogen pressure,
In unzipping method, the suspension of multi-walled voltage and current (above 200 torr, 50 V, and 100 A respec-
nanotubes with diameter between 4 and 18 nm was reac- tively) [164]. On the other hand, graphene has mechanically
ted through silicon substrate and treated with C9H23NO3Si synthesized by rubbing multi-walled CNTs bulk sample on
[162]. Another technique of converting multi-walled nano- glass micro-blades [165]. This technique has offered a unique,
tubes to graphene nanoribbon utilized as electric field which effective and convenient way to synthesize high quality
was applied to multi-walled nanotubes using a tungsten sheets of graphene. Furthermore, this technique allowed
electrode and perceived multi-walled nanotubes unzipping graphene sheets to form easily on any type of substrates by
established into graphene nanoribbon. The synthesis rubbing [166].
method attained to a defect-free with high-purity graphene In the last decade, a new approach known as photo-
nanoribbon [163]. irradiating related process was applied for GrO reduction. It
includes laser conversion of GrO to graphene [167], direct laser
writing for GrO reduction [168], photo/thermal reduction
using a pulsed xenon flash [169], and UV- induced photo-
catalytic reduction [170]. One of the advantages of the photo-
irradiating has been consuming no high temperatures and
chemicals during the process.
Another process entails femtosecond laser that applied
for GrO reduction without using any reducing agent. This
technique reported a short duration of laser pulse and
transferred minimum heat into the sample [171]. Newly,
water-based graphene exfoliation into nanosheets [172],
ultrasonic graphene exfoliation in aqueous media [173], Liþ/
Naþ intercalated ultrasonic synthesis into nanosheets [174],
shear force-based exfoliation through electro-spinning
technique [175], green and large-scale fluorinated gra-
phene exfoliation via ionic liquid crystals [176], CO2-assisted
supercritical exfoliation of graphene nanoplatelets [177],
two-step microwave-assisted exfoliation of Gr into gra-
phene [178], and facile electrochemical exfoliation of Gr into
graphene using aqueous solution [179] have been testified
Fig. 5 e A schematic diagram of multi-walled CNTs and considered as promising techniques employed for
converted into graphene nanoribbons [161] (With large-scale graphene production and opened up new ap-
permission from Elsevier). proaches for industrial applications.
Table 4 e Summary of bottom-up and top-down techniques used for graphene synthesis.
Techniques Pressure Temp. Graphene Characteristics Ref.
Mechanical Exfoliation
Ball milling Atmospheric 400 C Mono-layers Graphene [21]
Deposition of Gr on silicon z1000 N m2 700 C Graphene monolayers with high yield [79]
wafer using tape peeling
process
Metal layer deposition on Si Gentle 25 C 40 types of graphene monolayers [80]
substrate
Interfacial peeling and e e Single and multi-layers graphene [81]
intralayer tearing process
Facile exfoliation e 40 C Multi-layers of graphene [84]
Micromechanical 10 MPa 650 C Bi and tri-layers of graphene [88]
exfoliation
Pyrolysis
Salt-based method, 2e5 h 800e1000 C Single to multi-layered graphene sheets [48]
Chemical blowing,
Template based
confinement, Coupled
with hydrothermal, post-
exfoliation
Activation of coffee waste 2h 950 C Multi-layers of graphene [119]
using pyrolysis
Catalytic pyrolysis of lignin 3h 900 C Single layered graphene [120]
Two step pyrolysis of plastic e 400e750 C Graphene nanosheets [122]
waste
Vacuum pyrolysis 1h 1088e1103 K Single-layer graphene [123]
Pyrolysis of sodium 4h 850 C Graphene foams [125]
ethoxide
Epitaxial growth
Thermal decomposition of e 2000 C Multiple graphene layers [127]
SiC
Ultra-high vacuum epitaxial Frequency of vacuum 1500 C Multi-layers of graphene [129]
growth furnace ~106 torr
Epitaxial growth of Surface energy 300 erg/cm2 1800e2000 C Multi-layers of graphene [130]
graphene on carbon face
of SiC
Graphene on Si-face of 6H Growth period 3 min 1450 C Monolayer graphene [131]
eSiC
In situ process e 1100 C Monolayer graphene [134]
Unzipping method
Nanowire lithography narrow width of graphene 350 C Few layers of graphene [158]
up to ~50 nm
Flash light irradiation of Flash light for 1 h, X-ray source e Few layered stacking of graphene [160]
carbon nanotubes from Cu Ka 1.54 A
In situ oxidative unzipping 2h 65 C GO nanoribbons [161]
Electric unzipping 24 h, Voltage of 20 kV 25 C Graphene nanoribbons [162]
Controlled reduction 24 h 90 C GO nanoribbons [163]
unzipping of carbon
nanotubes
Table 4 displays a summary of most commonly used

bottom up and top down techniques such as mechanical 4. Industrial wastes precursors for graphene
exfoliation, epitaxial growth, pyrolysis and unzipping synthesis
methods. It can be seen that all these techniques lead to
produce variety of graphene derivatives. However, the In view of the wide increase in significant applications of
choice of any approach depends on several factors including graphene, the developments of its synthetic routes have been
the quality of graphene required for specific application, discussed extensively. In this regard, various carbonaceous
nature of precursor material, cost of the process and avail- industrial wastes are progressively drawing attention to
ability of particular facility. Additionally, a graphical repre- transform into graphene-derived materials in order to cater its
sentation of graphene synthetic routes and their growing demands and low production cost. Depending upon
comparison is illustrated in Fig. 6. the nature and compositions of carbonaceous wastes, several
agricultural waste per annum. Chemically, rice husk repre-

sents cellulose (50%), lignin (25e30%) and silica (15e20%) [182].
Due to its high silica contents, rice husk ash is used to produce
amorphous and crystalline silica into variety of silicon prod-
ucts [183e185]. Although, effective recovery of silica from rice
husk has been carried out, besides, its carbonaceous compo-
nents constitutes more than 70% of its mass which has un-
employed in this practice [186].
The utilization of rice husk as a raw material for production
of activated carbon, meso, nano, microporous carbon, and
graphene derivatives have gained enormous attention of re-
searchers [187e189]. Likewise, synthesis of graphene from rice
husk was first reported by Muramatsu et al. [190] in the
presence of KOH and carbon black to inhibit the air oxidation
of rice husk. Later, Singh et al. [191] upgraded this method by
Fig. 6 e Comparative analysis of various graphene annealing rice husk ash (RHA) in the presence of KOH at 900 C
synthetic routes. for 2 h. Sankar et al. [192] also used similar method to prepare
ultrathin graphene nanosheets from rice husk for electro-
processing steps are required to produce graphene analogues. chemical energy storage electrode applications. Similarly,
Comprehensive literature reports are available on utilizing Cheng and his group [193] developed a method for preparation
various types of industrial wastes for graphene production of graphene by successive intercalation through sulfate ions,
[180], on the basis of which these wastes are classified into followed by thermal dispersion with N, N-dimethylacetamide
different classes which are discussed below. (DMAC), microwave and ice splashing treatments of rice husk.
Although rice husk presents a potential source of carbon,
4.1. Bio-wastes but silica supposed to be the major impurity which should be
removed prior to its conversion into carbon materials. Alter-
On an annual basis, a wide range of bio-wastes produced by nately, silica and carbon have been simultaneously obtained
massive scale animals or agricultural origins are dumped into from the rice husk. For example, Luyi et al. reported the syn-
the environment. Although these wastes are effectively thesis of high surface area mesoporous silica nano particles,
biodegradable and produced on large tonnage, their utiliza- as well as biocompatible graphene quantum dots (GQDs) with
tion as bio-waste precursors into graphene accounts for their 15% yield, using rice husk as primary material. The GQDs were
value-added consumption and potential applications. analyzed for the biocompatibility through cell viability in-
vestigations, which improved its suitability for bio-probing
4.1.1. Rice husk and bioimaging [194]. Fig. 7 indicates the conversion of
Globally, rice is the third abundantly cultivated crop [181]. various graphene-derived materials obtained from rice husk.
Therefore, large tonnage of rice husk or hull which is the Similarly, Rhee et al. [196] presented the synthesis of
exterior shell of the rice grain has been produced as an corrugated graphene through KOH activation of rice husk
Fig. 7 e Preparation of graphene-derived materials from rice husk [195] (With permission from Elsevier).
Fig. 8 e Production of graphene like interconnected Gr-knitted sheets from hemp fibers [206] (Courtesy of ACS Publisher).
followed by its calcination at 1123 K. The authors suggested sustainable application for the same purpose. Therefore, this
that the KOH activation of rice husk assisted to produce high area of research needs to be explored to develop product-
porosity in the activated carbon, which in turn led to produce oriented techniques for high-quality graphene production
pure graphene having stable and smooth edges. Additionally, from rice husk. Recently, an efficient method was advised by
being a strong base, KOH activation also helped in leaching of Mahmoud et al. [200] for the preparation of GQDs with 2D
Si impurities. Due to its high porosity, the resulting graphene morphology from rice husk (RH) in two steps. In first step RH
was found to show high H2 storage capacity. However, in this was carbonized at 700 C for 2 h. Silica was removed from the
study, mechanism of graphene synthesis was not explained. RH based carbon by treatment with NaOH solution. In second
Another study reports the preparation of graphenated step the carbon was refluxed with a mixture of HNO3 and
carbon nanotubes (GCNTs) through single step microwave H2SO4 to obtain GQDO’s. The GQDOs were converted to
plasma irradiation using rice husk as precursors [197]. The GQDOs-Ba by treatment with BaCl2 solution and was used as
authors also characterized the electrochemical properties of adsorbent for the removal of Pb(II) and La(III) from aqueous
GCNTs. Seitzhanova et al. [198] reported the preparation of GO medium.
from rice husk in a four step process, consisting of carbon-
ization of rice husk to producing carbonized rice husk (CRH), 4.1.2. Hemp fiber
followed by its desilication using KOH solution, activation at The hemp or cannabis is an annual herbaceous plant, which
850 C for 2 h and finally exfoliation and oxidation to obtain can grow in different climatic conditions. The hemp bast has
GO. Preliminary characterization of GO prepared presented been used to derive hemp fibers which are used in textile in-
that graphene material with 70% carbon content was pro- dustry since ages. The hemp plants are also used to make
duced, but it also consisted of some inorganic impurities bioplastic, biofuels, animal feed, various phytochemical and
including K, Fe and Si (up to 20%). Raman and FTIR analysis paper [201,202]. Due to the increased demand, hemp fibers are
confirmed the presence of graphene layers and amorphous cultivated on large scale. However, stem of the hemp has been
carbon. Ismail et al. [199] used a very simple approach to often discarded as waste or burnt after cultivation [203]. The
prepare graphene from rice husk by activation of rice husk hemp stem contains high quantity of hemicellulos, crystalline
impregnated with KOH (1:2 ratio) at 800 C for 2 h, the gra- cellulose and lignin [203]. Therefore, these precursors have
phene mass was confirmed through Raman investigations. been utilized to obtain carbon materials and minimize bio-
These studies suggest that rice husk has been efficiently used wastes.
to prepare graphene and its derivatives using different ap- A number of studies have reported the preparation of high-
proaches. Although the purity of the product limits its quality carbon materials from hemp stems for various
Fig. 9 e Preparation of graphene sheets, Fe-graphene and Pt-graphene from disposable paper cups [211].
applications. For example, Yang and his co-workers [204] ob- waste for the preparation of activated carbon via carboniza-
tained the activated carbon with high surface area for tion at 500 C. The activated carbon was magnetized and
adsorption through phosphoric acid activation from hemp successfully used for adsorption of dyes from wastewater
stem. Similarly, Wang et al. [205] obtained porous carbon [209]. Likewise, the preparation of graphene from waste paper
spheres through hydrothermal and KOH activation of hemp, have also been reported through carbonization at 850 C in the
which was used for energy related applications. presence of urea [191].
Likewise, hemp materials can also be utilized as a low-cost The utilization of disposable wastepaper cups for synthesis
graphene production. Wang and his team prepared graphene of graphene derivatives has been scarcely studied. Zhao et al.
like interconnected carbon nanosheets for capacitance mea- [210] successfully derived Fe-graphene from disposable waste
surement by hydrothermal and KOH activation processes paper cups with high yield and enhanced quality which
[206]. The authors revealed that the hemp consisted of three exhibited superior efficiency as support for catalyst (Pt) in fuel
layers composite, (as shown in Fig. 8), the outer (S1) and inner cell application as presented in Fig. 9. The synthesis process
layers (S3) were made of semi-cellulose and lignin, while the involved the treatment of paper cup wastes with KOH solution
middle layer was composed of crystalline cellulose. During the to form the pulp. During this process, the Kþ cations were also
hydrothermal treatment of fibers at 180 C for 24 h in the incorporated to eOH and eC]O groups of the cellulose and
presence of dil. H2SO4, the cellulose and lignin layers were lignin structures. The pulp was treated with Fe solution to
dissolved to produce biochar. Further, the biochar was acti- replace the Kþ cations with Fe2þ in the pulp. It was graphitized
vated with 1:1 KOH at 700e800 C under argon flow to obtain at high temperature during which multiple graphene layers
highly porous carbon nanosheets. The synthesized graphene were produced leading to formation Fe/graphene. Fe could be
like carbon nanosheets were found to have desired properties removed by itching. Nevertheless, Fe was replaced by Pt
for supercapacitor applications. A patent also reported on the through galvanic replacement in graphene. The Pt/graphene
similar process and production of graphene nanosheets from displayed enhanced efficiency as a catalyst in fuel cell as
hemp bast for various applications [207]. compared to commercial Pt/C [210].
4.1.3. Disposable paper cups 4.1.4. Glucose

Nowadays, disposable paper cups are used on large scale Glucose is a monosaccharide carbohydrate which is abun-
throughout the world. As these cups are discarded soon after dantly produced by various plants through photosynthesis.
being used, therefore, constituting a major portion of the solid Hence, it is a major renewable source of carbon in nature. Due
waste produced on daily basis. These cups chemically indicate to it renewability and large abundance in nature, researchers
lignin and hemicellulose from paper pulp [180]. Although, it is also utilized it as a raw material for production of graphene.
a biodegradable waste material but rich in carbon content in For example, Li et al. [212] reported the synthesis of graphene
the form of carbohydrates, it can also be viewed as raw ma- from glucose in the presence of dicyandiamide (DCDA) by
terial for production of carbon materials. Like other paper/ sacrificial template, the produced graphene was called as
pulp-based waste materials e.g. laboratory tissue papers and patched graphene. In this process, glucose and DCDA were
hard board wastes reported for obtaining good quality acti- heated together under nitrogen atmosphere at 600 C, which
vated carbon for supercapacitors and adsorption applications resulted to produce layered graphitic carbon nitride (g-C3N4).
[208]. Similarly, Shukla et al. utilized disposable paper cups Moreover, heating of above 750 C fragmented carbon nitride
Fig. 10 e Preparation of graphene from Glucose in the presence of DCDA as template through pyrolysis [212].
and crystalline GO was formed. However, nitrogen was not glucose and melamine by one step hydrothermal method at
eliminated completely. After oxidation by modified hummers low temperature. Their experiment narrated that during
method, graphene sheets were aggregated into thick layers of hydrothermal treatment, glucose carbonization induced
GO. This method was helpful in production of N-doped gra- polymerization with melamine to form graphene nitride
phene for specific applications. Also, the nitrogen content was and GO nanochips, which assembled to form microsphere.
tuned easily and graphene was produced without pretreat- The nanochips having sandwiched morphology, wherein,
ment as displayed in Fig. 10 [212]. the outer layer made of GO and inner layer of carbon nitride
Similarly, Zhang et al. produced graphene using glucose as linked through p-p linkage. The nanocomposite micro-
raw material in the presence of FeCl3 as a template and sphere has been assumed to show efficient photocatalysts
catalyst [213]. The glucose and FeCl3 were dissolved together as well as a suitable catalyst support.
as heated to 80 C, wherein carbonized carbon and FeCl2(H2O2)
were formed. On calcination at 700 C under argon atmo- 4.1.5. Chitosan
sphere, zerovalent iron (Fe0) and graphene were formed, Fe Chitosan is a polysaccharide carbohydrate which is comprised
was removed from graphene by leaching with HCl. Graphene of glucosamine and N-acetyl-glucosamine units randomly
produced by this method was found with high conductance linked together. It is produced by alkaline treatment of chitin,
than produced through CVD method. Wang et al. developed a which is obtained from the shells or exoskeleton of various
convenient method for production of 3-D graphene from crustaceans such as crab, lobster, and shrimp [220,221]. It is
glucose [214]. The method found convenient as compared to the second largely occurring biopolymer and due to its use in
other methods such as hydrothermal or CVD process assisted new drugs development, biomedical applications, and other
by foaming and freeze drying [215,216]. In this process, 3D areas of research [222]. Like other renewable carbohydrate
graphene was formed by bubbling or foaming sugar followed sources, chitosan is also a potential raw material for synthesis
by its graphitization. The formed graphene was termed as of graphene. The chitosan molecule conveniently links
strutted graphene or 3D graphene bubble network. The solu- together forming large polymer, which on carbonization
tion of glucose and NH4Cl was heated to form glucose-based easily converts into graphene. However, the presence of ni-
polymer called melanoidin during heating bubbles or foam trogen in the structure of chitosan hinders the production of
was formed by release of gas from NH4Cl. The polymer mass pure graphene. Alternately, the production of N-doped gra-
underwent de-oxidation, dehydration and graphitization, phene derivatives has been reported from chitosan. For
leading to the formation of strutted graphene by heating example, Kumar et al. [223] produced N-doped GQDs on Al foil
around 1350 C. Finally, produced 3D graphene was shown to by CVD process using chitosan as sole precursor.
have high surface area, mechanical strength, density, con- Primo et al. reported the synthesis of single layer N-doped
ductivity and photon/electron transfer [214]. graphene by making a thin sheet (100 mm) of chitosan fol-
Hallaj et al. [217] prepared GQDs by thermal pyrolysis of lowed by its pyrolysis at 800 C under argon atmosphere [224].
powder glucose, which were stabilized for about 30 days at The produced N-doped graphene was used as catalysts for
4 C. GQDs were synthesized successfully and used for photocatalytic generation of hydrogen. However, because of
quantitative analysis of free chlorine in water through the complexity of the process, it was not scaled up. Similarly,
chemiluminescent reactions. Similarly, Shehab et al. [218] Hao and his team [225] presented a process for synthesis of
also synthesized GQDs from glucose by thermal pyrolysis. The graphene-based nitrogen aerogels using chitosan as precur-
quantum dots (QDs) were functionalized by phenylboronic sor. In this method, the chitosan aerogel was formed by freeze
acid and utilized for glucose sensing. These QDs exhibited drying the acetic acid solution of chitosan at 80 C for 12 h.
enhanced photoluminescence, high water solubility and high The aerogel was carbonized by using pyrolysis at 800 C under
sensing efficiency. nitrogen. Furthermore, the carbonized aerogel was activated
Recently, Hu et al. [219] reported the synthesis of with 3:1 ratio of KOH under various temperatures ranging
graphitic carbon nitride and GO nanocomposite from from 700 to 900 C. The synthesized N-doped graphene which
Table 5 e Overview of graphene derivatives synthesized from various bio-wastes.

Source Method and conditions Graphene type Remarks Ref.
Rice husk KOH activation and High Graphene, graphene High quality graphene synthesized [191e193,196]
temperature pyrolysis or nanosheets
microwave treatment
Rice Husk Single step microwave plasma GCNTs Electrochemical properties of GCNTs [197]
irradiation
Rice Husk Carbonization @ 700 C 2 h, reflux 2-D GQDOs Prepared nano-bioadsorbent GQDOs-Ba [200]
with mixture of HNO3 and H2SO4 with high adsorption capacity for the
for 24 h removal of Pb(II) and La(III) from water.
Sugar Pyrolysis, 1000 C, 1 h. N-doped graphene Efficient electro-catalyst NG, obtained at [226]
high annealing temperature.
Disposable KOH treatment, Fe2þ exchange, Fe/graphene High yield, good quality, superior [210]
paper cups graphitization efficiency as support for catalyst (Pt) in
fuel cell application
Glucose Heating glucose and DCDA at graphitic carbon nitride (g- nitrogen contents were tuned easily, [212]
600 C, followed by heating to C3N4). graphene produced without pretreatment
above 750 C,
Glucose Heating glucose and FeCl3 to 80 C, Graphene The produced graphene by this method [213]
calcination at 700 C leaching with was found to show higher conductance
HCl. than produced through CVD method
Glucose (Sugar blowing), Chemical 3D strutted graphene 3D graphene has high surface area, [214]
treatment and carbonization mechanical strength, conductivity and
photon/electron transfer
Glucose Thermal pyrolysis GQDs GQDs exhibit enhanced [217,218]
photoluminescence, high water solubility
and high sensing efficiency
Chitosan Making a thin sheet (100 mm) of Monolayer N-doped Single layer N-doped graphene, but [224]
chitosan followed by its pyrolysis graphene procedure complex
at 800 C under argon atmosphere
Chitosan CVD process: Annealing @ 250 N-doped GQDs QD with 10e15 nm dia, 2e5 nm thickness [223]
e300 C, Growth steps on Al foil @ and 4.2% N2 content
250e300 C (H2þ Ar flow), Cooling,
Ar flow
exhibited high specific capacitance and current density was Large hexagonal crystals were formed, and its rate of forma-
used for supercapacitor applications [225]. tion was found as proportional to the rate of injection for
A detailed overview of the graphene synthesis from products decomposition.
various waste biomass materials is presented in Table 5. Gong et al. [228] examined a simple method for obtaining
high yield of graphene flakes using waste propylene as a raw
4.2. Plastic wastes material in the presence of catalysts such as organo-
montmorillonite (OMMT). The waste propylene was obtained
Plastic is used in every sector of life as the huge tonnage of from scrape bumpers and panels consisted of PP (89%) and
plastics produced worldwide which ultimately leads to gen- additives (11%) with major constituent as talcum. About 15 g
eration of massive solid wastes. To safeguard the environ- of waste PP granules and OMMT were carbonized by heating in
ment, handling of plastic solid wastes has become a a crucible at 700 C. The carbonized mass was leached with HF
challenging issue for the researchers [47]. Being a rich carbon to remove impurities and clay to oxidize with HNO3. El Essawy
source, sustainable recycling of the plastic wastes has been and his team reported a simple method for synthesis of gra-
suggested its conversion into graphene-derived materials for phene from waste PET bottles [229]. They pyrolyzed the
variety of applications. Most of literature have focused on shredded waste PET bottles in stainless steel and autoclaved
transformation of single type or mixtures of plastic sources at 800 C for 1 h, which converted into graphene sheets. The
into graphene. For example, Sharma and his group reported successful synthesis of the graphene sheets was confirmed by
the preparation of high-quality crystalline graphene from various instrumental analysis. It was used as an adsorbent for
solid plastic waste, a mixture of PE (86%) and PS (14%) using the treatment of dyes in contaminated water as presented in
CVD process [227]. The process involved the growth of gra- Fig. 11.
phene on Cu foil by two heating stages and furnaces. In first Similarly, Rendo n-Patin
~ o obtained graphene sheets and 3D
furnace, the waste plastic was loaded in ceramic boat and graphene sponge from waste polystyrene precursors [230].
heated to about 500 C under flow of Ar and H2 (98:2) gases. They applied the dichloromethane solution of PS as a thin film
The decomposition products were carried by the gaseous on quartz and Cu substrate by spin coating, and pyrolyzed it at
stream to the second furnace maintained at 1020 C, wherein 900 C in argon atmosphere for 2 h to obtain graphene sheets.
the growth of crystalline graphene occurred over the Cu foil. Whereas, the graphene sponge was prepared by dispersing
Fig. 11 e Preparation of graphene form waste PET bottles [229] (With permission from Elsevier).
silica nanospheres (80 nm) in DCM solution of PS, which was was synthesized. Further, the TiO2 decorated rGO was used as
subjected to pyrolysis under conditions used in the former a photocatalyst for degradation methylene blue dye in
method. Silica spheres were dissolved by HCl solution to wastewater. Table 6 presents a summary of graphene prepa-
obtain graphene sponge. ration from various types of waste plastics.
Recently, Pandy et al. prepared bulk scale graphene nano-
sheets from mixed waste plastic by pyrolysis [122]. The mixed 4.3. Other low-cost sources
plastic wastes were consisted of PE, PP and PS and collected
from local municipality and flea market, washed and dried. Apart from various waste biomass and industrial wastes dis-
The plastic waste was exposed to slow pyrolysis at 400 C in cussed above, recently some other wastes and low-cost as
the presence nano bentonite, converted plastic waste into well as abundantly available sources are also under spotlight
carbonized mass. During the process, some volatile hydro- for production of graphene. Some common sources are dis-
carbons were also removed. The carbonized mass was grinded cussed as under.
to fine powder, and subjected into second step pyrolysis at
750 C to obtain graphene nanosheets under nitrogen atmo- 4.3.1. Domestic wastes
sphere. The clay materials were washed from graphene by HCl Being low-cost carbonaceous materials, variety of domestic
leaching. and vegetation wastes are gaining attention as potential raw
Takami et al. used polymethylmethacrylate (PMMA) film as materials for the synthesis of graphene and its derivatives.
a raw material to grow graphene sheets on sapphire substrate Recently, Ruan et al. synthesized single layered graphene
and Cu catalysts through CVD technique [231]. In this process, from PS and other carbonaceous waste materials including
PMMA film was loaded on sapphire substrate by spin coating, grass, dog excrements, chocolate, waste cookies and cock-
followed by deposition of Cu layer in order to inhibit the roach legs [234]. These wastes were loaded on Cu substrate in
evaporation and deposition of Cu. The multi-layer assembly quartz boat and converted into graphene materials by CVD
was the heated in the CVD reactor to 1000 C under Ar and H2 techniques at 1050 C for 15 min at low pressure under inert
flow, resulting in growth of graphene films on sapphire. atmosphere, leading to formation of graphene sheets.
Lately, Hu and his team [232] prepared multi-layers graphene Newly, Panahi-Kalamuei and his group came up with the
sheets from waste expanded polystyrene using Fe cluster idea of recycling waste bread leftover to produce graphene
analysis. The polystyrene waste was expanded using FeCl3 as derivatives by hydrothermal synthesis [235]. The group ob-
catalyst and subjected to high temperature carbonization at tained a gel by mixing bread waste with water at 70e80 C. The
900 C under nitrogen. Graphene layers were characterized to gel was subjected to hydrothermal treatment in Teflon lined
show that it consisted of 3 layers with micron level size. These steel autoclaved at 180 C under different conditions of pH and
layers also presented high crystallinity and electrical reaction time. Then, the suspension was filtered to recover the
conductance. precipitate formed.
Waste car bumper was utilized to produce rGO by pyrolysis
in the presence of TiO2 nanoparticles [233]. After cleaning, the 4.3.2. Agro wastes
waste pumper pieces were loaded in a pyrex glass reactor Similarly, Akhavan et al. utilized various natural and indus-
along with TiO2 nanoparticles enclosed in a steel reactor. The trial waste materials for synthesis of graphene and GO. These
steel reactor was placed in the furnace and heated to about wastes included wood, bagasse, leaves, fruit wastes, powder
700 C for 1 h, which produced shiny black powder of rGO. soot collected from exhaust of diesel engine and waste
Results indicated that in the presence of TiO2 catalyst, rGO newspapers [236]. Similarly, Adolfsson et al. demonstrated a
Table 6 e Summary of graphene derivatives prepared from plastic waste sources.

Waste plastics mixture PE (86%)þPS CVD process (graphene grown on crystalline graphene high-quality crystalline graphene [227]
(14%) Cu foil)
Waste PP scrape Carbonized at 700 C in presence of graphene flakes (GFs) high yield of graphene flakes (GFs) [228]
organo-MMT þ acid treatment formed
Waste PET bottles Pyrolysis 800 C, 1 h Graphene sheets successful synthesis of the [229]
graphene sheets
Waste polystyrene Pyrolysis (@ 900 C) of DCM solution Graphene sheets and 3 D High quality graphene nanosheets [230]
of PS coated on quartz and Si graphene sponge and graphene sponge produced
nanosphere in solution
Mixed plastic wastes Pyrolysis @ 400 C and graphene nanosheets Easy process for making graphene [122]
carbonization at 450 C nanosheets
Expanded polystyrene hyper crosslinked with FeCl3 as Few layers graphene FLG consisted of 3 layers with [232]
catalyst, Carbonization @ 900 C sheets (FLG) micron level size, high crystalline
and electrical conductance
Waste car bumper rGO Pyrolysis @ 700 C for 1 h, TiO2 TiO2 decorated rGO TiO2 decorated rGO used as a [233]
catalyst photocatalyst for degradation of
methylene blue dye
process for synthesis of graphene oxide quantum dots all these three wastes i.e., tricomposite agro waste (TAW) by
(GOQDs) from waste newspapers. The cellulose obtained from pyrolysis in the presence of ferrocene which provides electron
waste newspaper was utilized to prepare carbon nanospheres transfer reactions [242]. The dried powder of these agro
(CN) through microwave assisted hydrothermal process in the wastes (about 0.3e0.5 g) were loaded in a crucible with known
presence of H2SO4 as catalyst. The 3D CN were transformed amount of ferrocene (0.1e0.3 g) and carbonized in muffle Kiln
into 2D GOQDs through sonication and HNO3 treatment [237]. at 300e400 C for 15 min. The as synthesized GO, i.e. orange
Likewise, Faiz et al. reported the synthesis of GO from waste peel GO (OPGO), Rice bran GO (RBGO), Sugarcane bagasse GO
tea leaves. The tea leaves were carbonized twice at tempera- (SBGO) and tricomposite agro waste GO (TAWGO) were char-
ture range of 650e850 C under inert atmosphere, followed by acterized by XRD, SEM, HRTEM, FTIR spectroscopy and TGA/
its oxidation through hummers method [238]. DTA analysis.
Sujiono and his team [239] reported a method for the Tahir et al. [243] reported the synthesis of graphene from
preparation of GO from coconut shells, in this method fruit cover plastic waste (FCPW) and oil palm fibre (OPF)
powdered coconut shells were fist carbonized at 600 C for 3 h through CVD process. In this process the graphene layers were
to obtain charcoal, which was oxidized to GO by modified grown on copper (Cu) sheets in two stage furnaces, in the
hummers method. Various characterization tools were used presence of argon and hydrogen gases. The preheat time from
to confirm the successful synthesis of GO. 27 to 1000 C was 60 min, annealing time at 1020 C was
Long et al. reported [240] the preparation of densely porous 30 min, growing time was 90 min at 1020 C under only Ar
graphene-like carbon (PGC) materials form the fungus flow. The tribological performance of synthesized graphene
(Auricularia) by hydrothermal treatment in the presence of were tested. It has been indicated that these products were
KOH followed by carbonization process (Fig. 12). The PGC was used as best type of coating materials due to their potential
found to show interconnected porous framework and was friction reduction. In a study, Gr waste obtained from spent
successfully used as supercapacitor electrode. The PGC elec- lithium batteries was used as a source for producing rGO [244].
trode shown ultra-high volumetric capacitance and excellent Conversion of batteries Gr waste was carried out by one pot
cycling stability with 99% capacitance retention after 10,000 redox reaction using H2SO4, KMnO4 and peroxyacetic acid
cycles. (Fig. 13). The synthesis pf rGO was confirmed by TEM, SEM,
Pulping black liquid, a waste biomass resource produced by XPS, FTIR, XRD and Raman spectroscopy. The morphology of
pulping industry is rich in alkaline lignin which has also been the rGO synthesized from waste batteries Gr was found to be
utilized successfully as a source to prepare micron sized gra- similar to that of commercial rGO.
phene sheets [241]. The liquor was hydrothermally treated in
Teflon lined autoclave at 180 C for 6e12 h, the graphene 4.3.3. Coal as a source of graphene
synthesized was called black liquor graphene (BL-G), was Coal being a fossil fuel is widely used for power generation
collected and purified. The authors proposed that the syn- and industrial heating. However, due to its abundant avail-
thesis of graphene from aromatic rings of lignin occurs ability, low price and close structural resemblance to gra-
through aromatic rebonding, refusion and deoxygenation re- phene materials, it has been a spotlight precursor for
action, whereas the alkaline species act as situ-activation graphene derivatives. Ye et al. developed an easy method for
agent. The BL-G was used to prepare conductive films on synthesis of nanometer sized GQDs from coal [245]. In this
PET subtract by electrospinning for flexible electrode material. method, the coal sample was sonicated with a mixture of
A recent study reports the cost effective and green prepa- conc. H2SO4 and HNO3, and heated to 120 C for 2 h. The
ration of GO from various agro wastes, including rice bran mixture was neutralized by addition of NaOH, followed by
(RB), sugarcane bagasse (SB), orange peel (OP), and mixture of filtration through PTFET membrane. The filtrate was dialyzed
Fig. 12 e Shows the conversion of fungal wastes into PGC [240] (With permission from Elsevier).
and concentrated to obtain GQDs. Also, Vijapur and his team technique [248]. The coal suspension in ethanol was ablated
developed a convenient and economical route of synthesis. by a pulsed laser beam (35 nm) at room temperature and in air.
They yielded high quality few layer graphene sheets using The suspension was centrifuged to harvest the GOQDs, which
coal as a raw material through CVD technique [246]. The revealed excellent optoelectronic properties and potential
graphene films were produced with high transparency and usage in bioimaging applications. Potential characteristics
uniform structure for energy storage and other electronic and processing details of graphene derivatives using various
applications. low-cost and abundant waste precursors are summarized in
In addition, Zhang and his team also derived GQDs from Table 7.
coal by sonication of coal with DMF, followed by high effi- The researcher shown that under different conditions,
ciency filtration, and 3 days dialysis [247]. The GQDs were different graphene derivatives are formed including single
employed for detection of Cu2þ in aqueous system. However, layer graphene, few layers’ graphene and GQDs. This present
Kang and his team came up with a new techniques for fabri- a very economic and convenient synthesis route of graphene
cation of GOQDs from coal, using ND:YAG laser ablation and its derivatives. From the above-mentioned studies, it can
Fig. 13 e Preparation rGO from waste Gr of spent Li-batteries [244].

Table 7 e Summary of low-cost waste materials into graphene derivatives.

Other low-cost sources
Food, grass, insects, Dog CVD, Monolayer graphene High-Quality monolayer graphene [234]
feces, 1050 C obtained without pre-treatment.
Plastic 15 min
Newspapers Microwave assisted hydrothermal GOQDs Low cost raw materials produced [237]
process, followed by Sonication high quality of GOQDs
and HNO3 treatment
Tea Leaves Double thermal pyrolysis (at 650 GO Successful oxidation of graphitized [238]
e850 C), followed by oxidation by carbon
hummers method.
Industrial and vegetation Thermal pyrolysis Mono and multi-layer Good quality mono-and multi- [236]
wastes graphene layer graphene formed
Waste bread Hydrothermal treatment at 180 C, single layer, few layers Under different conditions, [235]
and different pH and time graphene and GQDs. different graphene derivatives
were produced by economic and
convenient route
Coconut shells Carbonization @ 600 C, 3 h, 2-D single layer graphene Presence of granular particles, [239]
followed by oxidation by hummers sufficient optical properties
method
Fungus (Auricularia) hydrothermal treatment followed PGC Interconnected porous network, [240]
by carbonization used as supercapacitor electrode
delivers high volumetric energy
density
Black liquor (Pulp waste) Hydrothermal synthesis Micron sized graphene Hexagonal honeycomb lattice, 1e3 [241]
180 C for 6e12 h atomic carbon layers thick, coated
on PET film to make transparent
conductive film for flexible
electrodes
Rice bran, Sugarcane Pyrolysis in presence of Ferrocene GO Synthesis of GO confirmed by XRD, [242]
bagasse, Orange peel, as electron transfer agent at 300 SEM, HRTEM and FTIR analysis
Tricomposite agro waste e500 C for 15 min
Fruit cover plastic waste CVD process, graphene grown on Single and multi-layer Good tribological performance, [243]
(FCPW) and Oil palm fiber Cu sheet Graphene proposed and coating material
(OPF)
Spent Li-batteries Gr One pot redox synthesis using rGO The morphology of the rGO [244]
H2SO4, KMnO4 and peroxyacetic synthesized was similar to
acid. commercial rGO
Coal Sonication with acids, heating at GQDs nanometer sized GQDs [245]
120 C for 2 h, filtration and dialysis
Coal CVD technique Few-layer graphene Graphene with large-area, [246]
1050 C conductive, and transparent (95%)
Coal Sonication with DMF, filtration and GQDs GQDs was used for electrochemical [247]
dialysis detection Cu2þ ions
Coal ND:YAG laser ablation of coal GOQDs GOQDs shows excellent [248]
suspension optoelectronic properties, suitable
for bioimaging application
be concluded that using waste precursors, the cost of bulk 1. Graphene synthesis is a well explored theme and the
level synthesis of graphene and its derivatives should be literature space is filled with studies on this topic. In light
curtailed. Additionally, these studies also suggest minimizing of this review, there has been a compelling rationale
the environmental pollution by utilizing solid wastes in a very offered for the need of modern tailoring of graphene and its
productive way. However, further studies are necessary to derivatives from unused waste materials such as eco-
cover the cost effectivity of techniques and enhancement for friendly, biodegradable, non-degradable and toxic types
the quality and yield of these graphene-derived products. of waste materials.
2. Utilization of eco-friendly and biodegradable waste mate-
rials into graphene fabrication will bring novel and green
5. Recommendations electronic devices, environmental protection as well as
global E-waste management system.
Based on foregoing global concerns on graphene synthesis, 3. This review paves the way for research studies for the
there are noteworthy recommendations that can be drawn conversion of waste precursors not only into graphene but
from this study; also graphene related materials including GO, rGO, porous
carbon sheets, graphene quantum dots, graphene-based One of the noteworthy challenges comprise optimization of
aerogels etc. process parameters and methods to control the size, quality
4. These waste derived graphene-based materials can also be and morphology of graphene-derivatives from waste mate-
used as functional nanofillers to improve considerable rials. Calibration of these synthetic methods should be
mechanical and electrical properties of various devices. accomplished. The usage of eco-friendly and green processes
5. Although waste derived materials are emphasized in the is crucial for scale-up production. However, improved syn-
current study, sustainability concerns posed by the actual thetic ideas and approaches are remarkably motivating and
synthetic routes should be focused in future research di- requires commercial investigations using biodegradable and
rection. For example, sustainable waste materials and renewable waste materials. Another lingering encounter has
their proper usage to lessen environmental damages been temperature effects which changes the morphological
should be concerned. Similarly, synthesis of graphene properties of graphene derivatives. More importantly, future
derivatives using greener processes is the requirement of studies should be established to deploy consistency of waste
current era. materials fabrication into graphene-based structures with
6. Moreover, other significant factors such as renewable en- improved and noticeable surface area and functionalities.
ergy, choice of appropriate solvents and other features Future evaluations require careful and precise analysis as
with reduced impact on the planet and its resources should presented in Fig. 15.
be considered for future prospects. Newly, numerous ways have been outlined for the
7. From an application-oriented point of view, purity and fabrication of graphene derivatives such as graphene
quality of the synthesized graphene is important. The quantum dots or metal oxide doped graphene with wide-
future studies should tangentially refer to this point. This ranging structures and characteristics. However, selective
may lead the scale-up production of graphene and its de- and rare greener or sustainable synthetic methods have
rivatives for various industrial applications. been utilized for graphene derivatives which requires elab-
orative research works. In this regard, precise and distinct
We hope that this review will bring the scientific commu- studies are needed to unlimited the insightful examination
nity adjoining to the opportunities and benefits of using low- and relationships between divergent structures and prop-
cost unused waste materials as a tool in the synthesis of erties. Furthermore, detailed and regulatory assessments
graphene-based materials as reported in Fig. 14. are required for innovative synthetic methods and
applications.
Overall, the appraisal of this work has examined the cur-
6. Future prospects & challenges rent focus of researchers in defining and innovating novel
sources of graphene along with synthetic methods. The
Although graphene has shown a surge in scientific activities mechanism of using cheap and unused waste materials have
for various applications, there are several key challenges extensive potential for industrial applications. An all-
which are yet to be conveyed. As long as major challenges are inclusive attention towards the usage of these waste mate-
connected, one of the vital issues includes the reproducibility rials is needed; additional hypothetical market research and
of waste materials into graphenaceous materials. Cost- improved understanding of systematic features are very
effective and scalable procedures should be established with crucial.
high consistency along with improved morphological prop-
erties. Excitedly, cumulative interest of graphene-based ma-
terials synthesis in assessment of their production and
combination with other materials is sustainable. Although,
recent studies are focused on waste precursors but none of
them are capable to mark into commercialized products yet.
Fig. 14 e Opportunities & Limitations of using waste Fig. 15 e Future challenges in graphene synthesis
precursors for graphene synthesis. techniques.
references
7. Conclusion
Realizing the industrial importance of graphene, there is

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synthesis of graphene from waste graphite of spent lithium chapter. He is currently the Energy Education Chairperson in SPE
ion batteries with peracetic acid assistance. Mater Chem KL Section and the Energy4me advisory team for SPE Asia Pacific.
Phys 2020;241:122397. Jan was the recipient of the 2016 SPE Distinguished Achievement
[245] Ye R, Xiang C, Lin J, Peng Z, Huang K, Yan Z, et al. Coal as an Award for Petroleum Engineering Faculty for the Northern Asia
abundant source of graphene quantum dots. Nat Commun Pacific Region. He has also served as the deputy director of Uni-
2013;4(1):2943. versity Malaya Center of Innovation & Commercialization for
[246] Vijapur SH, Wang D, Botte GG. Raw coal derived large area and about 3 years. His responsibilities include providing an environ-
transparent graphene films. ECS Solid State Lett 2013;2(7):M45. ment at the University of Malaya conducive to researchers
[247] Zhang Y, Li K, Ren S, Dang Y, Liu G, Zhang R, et al. bringing their research outputs to a commercialization-ready
Coal-derived graphene quantum dots produced by level. He received his Chartered Engineer (CEng) award from the
ultrasonic physical tailoring and their capacity for Institute of Engineering Technology (IET), United Kingdom.
Cu(II) detection. ACS Sustainable Chem Eng
2019;7(11):9793e9.
[248] Kang S, Kim KM, jung K, Son Y, Mhin S, Ryu JH, et al.
Dr. Waqas Ahmad received his PhD degree
Graphene oxide quantum dots derived from coal for
in Chemistry from University of Peshawar in
bioimaging: facile and green approach. Sci Rep
2013. He has carried out a part of his research
2019;9(1):4101.
work at Department of Chemical and Mate-
rial Engineering, University of Alberta, Can-
ada. Presently, he is working as Assistant
Dr. Rabia Ikram has received her PhD de- Professor at Institute of Chemical Sciences,
gree in Analytical Chemistry from Univer- University of Peshawar. His research in-
sity of Malaya (2018). Currently, she is terests include Petroleum & coal processing
working as a Research Fellow at Depart- and upgrading, Material synthesis and
ment of Chemical Engineering, University Characterization, Catalysis and water pollu-
of Malaya. Her research interests include tion. He is an author of over 36 Research publications and has
Green Synthesis, Separation Techniques, contributed chapters in several renown books.
Method Development, and Chemometrics.
At present, her research focuses on various
synthetic approaches and characterization
of Nanomaterials for industrial applica-
tions. She has published around 30 ISI paper and has partici-
pated in numerous National & Internal Conferences as an
Invited Speaker.
Badrul Mohamed Jan, SPE, CEng (UK), is an

Associate Professor and researcher
attached to the Department of Chemical
Engineering, University of Malaya (UM),
Malaysia. He holds a BS, MS and PhD de-
grees in petroleum engineering from New
Mexico Institute of Mining and Technology.
Jan’s research areas and interest include
the development of super lightweight
completion fluid for underbalance perfo-
ration, ultra low interfacial tension micro-
emulsion for enhanced oil recovery and extraction of graphene
form unwanted industrial waste for drilling fluid application. He
has published numerous technical conference and journal pa-
pers. Jan is also an active SPE members; he has participated in
SPE Mentor/Mentee volunteers program for several years. He is

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j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 0 ; 9 ( 6 ) : 1 5 9 2 4 e1 5 9 5 1

Available online at www.sciencedirect.com

journal homepage: www.elsevier.com/locate/jmrt

Advances in synthesis of graphene derivatives

Rabia Ikram a,*, Badrul Mohamed Jan a, Waqas Ahmad b

article info abstract

down method [28] have been successfully utilized for gra-

Table 1 e Summary of graphene synthetic routes.

Table 2 e Overview of Chemical exfoliation methods for graphene synthesis.

partially exfoliated. Oxidizing agents such as hydrogen 3.3. Other methods

Table 4 displays a summary of most commonly used

agricultural waste per annum. Chemically, rice husk repre-

4.1.3. Disposable paper cups 4.1.4. Glucose

Table 5 e Overview of graphene derivatives synthesized from various bio-wastes.

Table 6 e Summary of graphene derivatives prepared from plastic waste sources.

Fig. 13 e Preparation rGO from waste Gr of spent Li-batteries [244].

Table 7 e Summary of low-cost waste materials into graphene derivatives.

Realizing the industrial importance of graphene, there is

Badrul Mohamed Jan, SPE, CEng (UK), is an

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