REVIEW

Carbon nanotubes from renewable feedstocks: A move toward

sustainable nanofabrication
Singaravelu Vivekanandhan,1,2 Makoto Schreiber,3 Sankaralingam Muthuramkumar,4
Manjusri Misra,2,5 Amar Kumar Mohanty2,5
1
Sustainable Materials and Nanotechnology Lab, Department of Physics, VHNSN College, Virudhunagar, Tamilnadu, 626 001, India
2
Bioproducts Discovery and Development Centre, Department of Plant Agriculture, University of Guelph, Crop Science Building,
Guelph, Ontario, N1G 2W1, Canada
3
Okinawa Institute of Science and Technology (OIST), Tancha, Onna-son, 1919-1, Okinawa, Japan
4
Department of Botany, VHNSN College, Virudhunagar, Tamilnadu, 626 001, India
5
School of Engineering, University of Guelph, Thornbrough Building, Guelph, Ontario, N1G 2W1, Canada
Correspondence to: S. Vivekanandhan (E-mail: svivekan@vhnsnc.edu.in) or M. Misra (E-mail: mmisra@uoguelph.ca)

ABSTRACT: A recent development in the manufacturing of carbon nanotubes is the usage of renewable feedstocks as a carbon source.
This new development is receiving much support and is a source of excitement among the global research communities due to the
positive environmental impacts, reduced carbon footprints, and economic benefits. Various types of renewable feedstocks such as veg-
etable oils, plant derivatives, and other types of biomasses have been used for the green synthesis of carbon nanotubes by employing
conventional fabrication techniques. As the global demand increases for green manufacturing, efforts to synthesize carbon nanotubes
from renewable resources are receiving immense attention while also strengthening the concept of biorefinery. This also enables the
efficient use of resources as well as improved waste management. The present review summarizes the recent developments and current
status of the synthesis of carbon nanotubes using renewable feedstocks along with technical discussions, opportunities for novel pre-
cursors, and future directions. V C 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 44255.

KEYWORDS: fullerenes; graphene; nanotubes; non-polymeric materials and composites; synthesis and processing techniques

Received 17 May 2016; accepted 28 July 2016

DOI: 10.1002/app.44255

INTRODUCTION onions, and nanotubes).7,8 The structural classification of car-

Carbon nanostructures, which include fullerenes, carbon nano-
tubes, nanodiamonds, graphenes, and other particulates as well
as fibrous structures, receive remarkable attention because of
their unique structure dependent physiochemical properties.1–6
Such a diverse range of structures (allotropes) is possible
because elemental carbon can exist with sp3, sp2, and sp hybrid
orbitals: corresponding examples being diamond, graphite, and
carbine, respectively. The remaining other carbon structures are
classified into two major categories: (i) Mixed short-range order
carbons in which there is an arrangement of carbon atoms with
different hybridization states: examples being carbon blacks,
soot, and diamond-like carbon. (ii) Intermediate carbons in
which the carbons have intermediate hybridization states spn
with 1 < n < 2 (monocyclic carbon structures) or 2 < n < 3
(closed-shell carbon structures such as fullerenes, carbon
bons is summarized in Figure 1. Carbon nanostructures have
found a wide range of applications in almost all fields of mod-
ern science and technology9 including electronics,10 catalysts,
composites,11 sensors,12 photovoltaic solar cells,13 fuel cells,14
super capacitors,15 lithium ion batteries,16 medicine, and bio-
technology.17 Since the discovery of carbon nanotubes (CNTs)
by Iijima in 1991,18 CNTs have been among the most studied
carbon nanostructures. The study of CNTs has in fact become a
new field of materials research and is widely explored by the
global research community in various aspects such as fabrica-
tion/purification techniques, investigations into their structure
and size dependent physicochemical properties, and their scien-
tific and technological applications.11,19–21 This is made possible
due to their unique physical and chemical properties22,23 in
addition to their compatibility with other systems including

This article was published online on 23 September 2016. An error was subsequently identified in the spelling of the Corresponding
Author name. This notice is included in the online and print versions to indicate that both have been corrected 22 October 2016.

C 2016 Wiley Periodicals, Inc.

V

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Dr. S. Vivekanandhan, Assistant Professor at Department of Physics, VHNSN College,

received his PhD from Pondicherry University in 2007 and pressured his Post-Doctoral
Research at School of Engineering, University of Guelph between 2008 and 2011. Further,
he served as Research Scientist at Department of Plant agriculture, University of Guelph
during 2011–2013. He has more than 50 publications to his credit including 32 peer-
reviewed journal articles, 4 Book Chapters and 13 conference proceedings.

Makoto Schreiber is a recent graduate student from Okinawa Institute of Science and
Technology (OIST), Okinawa, Japan. He was the recipient of a University of Guelph
Entrance Scholarship and was awarded an Undergraduate Student Research Awards by
NSERC. His research has included work in the fabrication of lignin nanofibers for green
carbon fibers and green methods of synthesizing functionalized semiconductor nanopar-
ticles. He has coauthored 8 peer journal publications and one book chapter.

Dr. S. Muthuramkumar earned his PhD degree in Ecology and Environmental Sciences
from Pondicherry University in the year 2002. Since December 2007, he is working as an
Assistant Professor at Department of Botany, VHNSN College, Virudhunagar. He has coau-
thored over 10 publications in the peer reviewed internationals. He contributed two book
chapters in Ecology of Lianas and one book chapter in Biodiversity of Lianas. His current
research focuses on sustainable utilization biomass.

Dr. Manju Misra is a professor in the School of Engineering and holds a joint appointment
in the Dept. of Plant Agriculture at the University of Guelph. Dr. Misra’s current research
focuses primarily on novel biobased composites and nanocomposites from renewable
resources. She has authored more than 400 publications, including 2501 peer-reviewed
journal articles, 25 book chapters, and 15 granted patents. Dr. Misra received the presti-
gious “Jim Hammer Memorial Award” from the BioEnvironmental Polymer Society.

Dr. Amar K Mohanty, a Full Professor and Premier’s Research Chair in Biomaterials and
Transportation is the Director of Bioproducts Discovery & Development Centre at Universi-
ty of Guelph, Ontario, Canada. Dr. Mohanty has more than 600 publications to his credit
with 265 peering reviewed journal articles, 40 patents (awarded/filed) and four edited
books. He received the Andrew Chase Forest Products Division Award from the AIChE and
Jim Hammer Memorial Service Award from the BioEnvironmental Polymer Society.

nanostructured materials (metals/oxides/chalcogenids),24 chemi-
cal and biochemical molecules,25,26 and natural and synthetic
polymers.27,28 CNTs have been characterized as single, double,
and multiwall carbon nanotubes (SWCNTs, DWCNTs, and
MWCNTs); depending on the number of graphite sheets rolled
to form its structure. In general, they have diameters on the
order of nanometers and lengths up to millimeters. Peng et al.29
reported the fabrication of the thinnest energetically stable car-
bon nanotube with a diameter of 0.4 nm.
Synthesis methods play a vital role in the creation of carbon
nanotubes with desired properties. The experimental setup used
by Iijima was an arc discharge kit kept in 100 torr argon which
resulted in MWCNTs with 2–50 walls. In addition to arc dis-
charge methods, various other techniques including laser abla-
tion and chemical vapor deposition (CVD) have also been
established and investigated.30 The challenge is to establish these
technologies for large scale synthesis in order to meet the pro-
jected demand for CNTs in various technological applications.
Among the above mentioned processes, the CVD method
involving the pyrolysis of hydrocarbons in the presence of tran-
sition metal catalysts has received attention due to its ability to
produce CNTs on a larger scale.31 Wang et al.32 have developed a
fluidized bed CVD reactor for the large scale synthesis of CNTs.

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Figure 1. Schematic representation of structural classifications with
respect to sp3, sp2, and sp bonding states of carbon. (Reproduced from
Ref. 7). [Color figure can be viewed at wileyonlinelibrary.com]
They were successfully able to produce 50 kg/day with a purity of
approximately 80%. Precise control of the synthesized CNT struc-
ture and properties has been achieved by manipulating various
synthesis parameters such as the operating temperature, precursor
carbon source composition, precursor feed rate, growth duration,
and the catalysts used. The characteristic features of carbon nano-
tubes are highly dependant on their atomic arrangements and
size. Depending on the helicity and diameter of a carbon nano-
tube, its electrical properties can change between metallic and
semiconducting.33 Thus, precise control of the atomic arrange-
ments, tube diameter, and number of walls are challenging issues
in the synthesis of carbon nanotubes. Control over the synthesis
process can generate carbon nanotubes with the desired structural
and morphological features.33 Thus, a wide range of synthetic
processes have been explored and demonstrated for the synthesis
of carbon nanotubes, which are schematically shown in Figure 2.
Apart from the synthesis techniques, the carbon precursors and
the catalysts used are also key parameters which will determine
the type of CNTs which can be obtained. Numerous research and
development works have been patented for the production of car-
bon nanotubes.34–37
Carbon Sources for CNTs
Feedstocks for the synthesis of carbon nanotubes can be catego-
rized into three major group bases on their physical nature as a
solid, liquid, or gas.38 Examples of traditionally and commonly
used precursors include: solid—coal, mesophase carbon, graph-
ite, camphor, and naphthalene39,40; liquid—benzene, n-hexane,
thiophene, ferrocene, ethanol, cyclohexanol, xylene, and dime-
thylformamide;41,42 and gaseous—acetylene, methane, ethylene,
and pyrene.41,43,44 All these carbon precursors are petroleum
based and non-renewable in nature.
Solid precursors of coal and graphite have been widely used in
arc-discharge and laser ablation techniques for the synthesis of
carbon nanotubes. These processes deal with the vaporization of
carbon from the carbon sources at very high temperatures
(thousands of 8C) and their growth as nanotubes.45 These
processes have been widely explored for the synthesis of high-
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quality carbon nanotubes with structural purity. However,
significant amounts of byproducts are also produced. In the
arc-discharge method, pure graphite rods are employed as a car-
bon source and electrodes. The evaporation of anode then leads
to the formation of fullerenes.45 Fine tuning this process by
introducing helium gas with an optimum temperature and pres-
sure, MWCNTs have been produced on a large-scale.46 Optimal
doping with metals such as Fe, Co, Ni, Fe, etc., into the anodic
graphite act as the effective catalyst and caused the formation of
SWCNTs.47 These metal catalysts act as the nucleation site,
where the hydrocarbon decomposes and converts into carbon
atoms, which result in the growth of carbon nanotubes.47,48 In
the laser vaporization method, pelletized metal-doped graphite
powders are used as the target.
Solid, liquid, and gaseous precursors have been extensively used
in chemical vapor deposition (CVD), which employs metal or
metal oxide catalyst particles as “seeds” for the growth of car-
bon nanotubes from the thermally decomposed hydrocarbon
vapors at relatively low temperatures between 500 and 1000 8C
and at ambient pressure.49 The versatility afforded in the ability
to use solid, liquid, and gaseous precursors as well as various
substrates and catalysts enables CVD to grow CNTs in different
macroscopic morphologies such as powders and films (thick or
thin) and with different microscopic architectures such as
straight, aligned, entangled or coiled on predefined sites of pat-
terned substrates.50 In the case of liquid precursors, the purge
gas passes through a tank with the heated liquid to carry the
vapor into the heated reaction furnace. For solid precursors, a
high-temperature reaction furnace as well as another furnace
maintained at a lower temperature is essential to vaporize the
solid carbon sources.45 Stability of the hydrocarbons at higher
temperatures effectively affects the formation of MWCNTs or
SWCNTs. Precursors like CO and CH4 which exhibit reasonable
stability in the 900–1200 8C range result in the formation of
SWCNTs.45 Hydrocarbons such as acetylene and benzene which
are less stable at higher temperatures lead to the formation of
MWCNTs. The CNTs, both single wall and multiwalled,
Figure 2. Different processes that have been widely employed for growth of
carbon nanotubes. [Color figure can be viewed at wileyonlinelibrary.com]
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REVIEW WILEYONLINELIBRARY.COM/APP
synthesized from these processes contain amorphous carbon
and catalytic metal impurities. The amorphous contaminants
can be effectively removed through oxidation by employing hot
air at 400–500 8C or some oxidizing chemicals such as H2O2 as
the dangling bonds present on the amorphous carbon oxidize
easily.51
Traditional precursors used for the synthesis of CNTs originate
from petroleum resources. Increasing environmental concerns,
depleting fossil fuel resources, uncertainty in crude oil prices, and
the demand for the alternate precursor carbon sources has moti-
vated researchers toward the search for renewable resource based
green-carbon sources for the synthesis of CNTs. Recently, Deng
et al.,52 reviewed the research accomplishment on the effective
transformation of waste into carbon-based nanomaterials such
nanotubes and graphenes. Similarly Kumar et al.53 reviewed the
research work on the synthesis of graphene and CNTs from natu-
ral and waste precursors. Advances in this research would allow
manufacturers of CNTs to reduce their carbon foot print and
strengthen the field of sustainable nanofabrication. The aim of
this review article is to gather the work and knowledge obtained
till now on the fabrication of CNTs from renewable resources.
This article will describe how traditional processing methods and
equipment have been utilized for the fabrication of CNTs from
renewable precursor materials and the specific renewable carbon
sources which have been successfully utilized.
A MOVE TOWARD SUSTAINABLE CARBON MATERIALS
As the global population continues to grow, materials innovation
and their effective utilization can partially aid in allowing a larger
population to have improved living standards.54 These innovative
materials should critically address the issues pertaining to the
current dependence on finite resources as well as emerging threats
to our planet’s ecosystems. The main challenges associated with
implementing suitable sustainable solutions in any manufactur-
ing sector are the upgrading of processing facilities, added costs,
and reduced financial benefits as sustainable manufacturing
requires process developments, new equipment usage, and novel
designs for performance retention.55 Thus, Nidumolu et al.56
attributed sustainability to be the driving factor for innovation.
According to them, sustainable development consists of four
stages: (i) viewing compliances as opportunities, (ii) making the
value chain sustainable, (iii) designing sustainable products, and
(iv) developing new business models. The material aspects of a
sustainable value chain begin with the identification of new clas-
ses of environmental friendly feedstocks and finding methods to
effectively convert them into technologically important prod-
ucts.57 The sustainability of feedstocks or raw materials depends
on their origin (renewable vs. non-renewable), availability (abun-
dant vs finite), impact on the environment (carbon footprint),
and the energy input during processing. Thus, renewable resource
based feedstocks such as biopolymers (including cellulose, starch,
lignin, and other proteinaceous materials)58–60 and other chemi-
cals (including ethanol, glycerol, syngas, and methane)61–64
receive immense attention for the fabrication of various commer-
cial products. Product diversification is essential and also a key
factor in creating a successful move toward a sustainable future.
Thus, such renewable materials have been widely explored for the
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development of many advanced industrial products such as dura-
ble polymers/blends/composites, coatings/adhesives, energy stor-
age and conversion materials, sensor/catalytic products, and
medicinal implants.65–69 These sustainable materials have
received enormous benefits from nano science and technology;
improving their functionality and durability. As the global
demands increases for sustainable products, novel renewable
resources based nanostructured materials have been introduced
and investigated for many applications. These include cellulose
and protein based nanofibers, starch nanostructures, silica nano-
particles, and various types of carbon nanomaterials.58,70–72 In
addition to that, a variety of metal nanoparticles and metal-
nanoparticle functionalized materials have been produced using
plant-extract mediated bioreduction processes.73–75 Carbon
nanomaterials (such as spheres, fibers, carbon dots, graphenes,
and carbon nanotubes) synthesized from renewable resources has
also attracted many researchers around the globe.76–82
Renewable Resources for Carbonaceous Materials
Finite petroleum resources, unstable crude oil prices, ever
increasing global concern on environmental challenges (CO2
emissions, and climate change), and emerging demand for sus-
tainable materials requires a change in the fabrication of carbon
nanomaterials by using renewable resource based precursor
materials with a smaller carbon footprint than traditional petro-
leum resource based materials.72,83,84 Many types of carbon
nanomaterials such as tubes, particles, fibers, sheets, dots,
onions, and graphenes have been synthesized with renewable
precursors.85–88 Likewise, a wide variety of renewable precursors
have been used for the fabrication of carbonaceous nanomateri-
als and include raw biomasses (grass and leaf),89 juices (orange,
banana, grape and strawberry juice),79,90–92 seeds (sunflower,
grape),93,94 shell (chestnut, coconut, cashew nut),93 oils (palm,
neem), industrials coproducts (lignin, glycerol, DDGS), aqua/
marine products (chitin, algae), fruit peals (orange, banana),95
bioderived hydrocarbons (ethanol, biodesel) and other biobased
materials (silk, natural proteins).96 However, the synthesis of
carbon nanotubes (single/multiwalled) using renewable precur-
sors as the carbon source has received the most attention. The
renewable resource derived carbon nanotubes exhibit similar
properties to conventional CNTs and thus, in this review, we
focus mainly on the growth of CNTs from renewable feedstocks.
Carbon Nanotubes from Renewable Precursors
The first reported renewable feedstock used for the synthesis of
CNTs was a crystallized latex product from the Cinnamomum
camphora tree.97 Since then, many different products have been
used such as plant oils,98,99 biodiesel, and solid biomasses like
grass and leaves among other sources.100,101 Recently, in addi-
tion to plant-sourced materials, animal-sourced materials such
as chicken fat and feathers have been employed as an effective
carbon source for the fabrication of CNTs.102,103 Though they
are not renewable, they are biobased and available as byproducts
during the processing of poultry products. From a sustainability
perspective, using these resources can address issues related to
the disposal of these byproducts as well as offer an economic
return to the poultry industries. Chemical vapor deposition and
spray pyrolysis have been extensively used for the processing of
liquid feedstocks. Using solid precursors such as leaf, grass, and
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Figure 3. Structural features of carbon nanotubes grown from the fallen leaves of poplar (a) and hyperaccumulator plant of Brassica juncea L (b).
(Reproduced from Refs. 81,105). [Color figure can be viewed at wileyonlinelibrary.com]
other biomasses, thermal pyrolysis has been employed repeated-
ly for the condensation of biomass as well as the formation of
nanotube structures.81,101 By manipulating the type of catalysts
one can easily achieve the desired structure of carbon nanotubes
by employing renewable precursors. The following section sum-
marizes the recent developments in the production of CNTs
from different biosourced feedstocks.
RENEWABLE FEEDSTOCKS FOR CARBON NANOTUBES
Hydrocarbons with lower hydrogen contents can be effectively
used as suitable precursors for carbon nanotubes. It has been
identified that many renewable resource based biochemicals,
which can be used as precursors for the production of high
quality CNTs possess low C:H ratios (C:H ratio for palm oil
with the chemical formula of C55H100O is 1:2). The choice for
renewable resource based carbon precursors for the effective
synthesis of carbon nanotubes is vast, which includes a diverse
range of plant biomasses, vegetable oils, extracted biochemicals,
and other animal bioproducts. The challenges in using renew-
able precursors for CNT synthesis are (i) selection and purity of
the precursors and (ii) optimizing the experimental conditions
for every feedstock. At the optimum processing conditions and
catalysts/substrate combination, it is possible to synthesize the
carbon nanotubes with desired morphological features such as
wall number and bundle alignment. This section summarizes
the influences of various renewable feedstocks for the synthesis
of structure controlled carbon nanotubes under various
categories.
Biomasses
Various biomasses such as grass, leaves, and hyperaccumulating
plants have been explored for the synthesis of carbon nano-
tubes. Kang et al.101 reported the synthesis of MWCNTs by
decomposing grass in the presence of an optimal amount of
oxygen. First, a few grams of grass samples were crumbled and
dried at 250 8C for 1 h. The obtained black colored powder was
then washed with alcohol and repeatedly heated between room
temperature and 600 8C where it was held for 20 min in an oxy-
gen environment. The resulting MWCNT products were collect-
ed for further characterization. TEM analysis confirmed the
formation of MWCNTs with the diameter ranging between 30
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and 50 nm. In general, grass biomass contains quite a large con-
centration of vascular bundles composed mainly of cellulose,
hemicellulose, and lignin. The repeated heating process causes
the vascular bundles to dehydrate and be converted into carbon
nanotubes.101 In plants, vascular bundles exhibit tubular struc-
tures with the composition of cellulose, hemicellulose, and lig-
nin. During the carbonization process, the existing oxygen
environment causes rapid pyrolytic reactions and forms carbon
double bonds. This leads to the retention of tubular structures
even after repeated carbonization process at higher tempera-
tures.101 Qu et al.81 demonstrated the synthesis of CNTs from
the fallen leaves of poplar by employing a simple thermal
decomposition process under ambient air conditions. They
implemented a similar protocol as reported by Kang et al. The
collected leaves were dried, crumbled, and preheated at 250 8C
for 1 h in air. The charred particles adhered on the surface of
the shoots were removed with water. The collected black prod-
ucts were then washed with alcohol, rapidly heated to 500 8C in
air for 5 min, then cooled to room temperature. CNTs were
obtained after repeating the heating and cooling process 10
times. The synthesized CNTs were open at one end, had good
crystallinity, and inner and outer diameters of approximately 40
and 77 nm, respectively, which is shown in Figure 3(a). The
grown CNTs were also found to contain many defects in their
walls which have potential for catalytic applications.
Qu et al.104 reported a novel method of producing carbon
nanotubes using metal hyperaccumulator plants as the green
renewable source. Metal hyperaccumulator plants have been
receiving significant interest due to their ability to accumulate
unusually high levels of toxic metals in their stems and leaves.
Thus, they have been used for the purpose of phytoremediation
to clean contaminated soil. However, care must be taken in
order to prevent the plants from being ingested by animals and
other living organisms; which would eventually transfer the tox-
ic metals back into the ecosystem. It has been identified that
the Cu and Zn accumulation in the stems of Brassica juncea
plants on a dry weight basis are 3725 6 289 and 2573 6
237 mg/kg, respectively.104 These can be effectively converted
into Cu/ZnO nanoparticles. In order to synthesize CNTs, first
the biomass of B. juncea plants were collected, dried, and crum-
bled. The treated biomass of B. juncea plants was mixed with
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90% ethanol at 70 8C for 120 min and filtered. The treated bio-
mass was then further mixed with 250 mL of HNO3 (1.00 mol/L)
and shaken at 85 8C for 360 min. Reaction of biomass with
nitric acid caused the formation of Zn/Cu (NO3) and charred
biomass. The resulting black-colored biomass was rapidly heated
to 400 8C and held for 5 min. The heating/cooling process was
then repeated 20 times; resulting in the formation of carbon
nanotubes with an outer diameter of 80 nm as shown in Figure
3(b). In another reaction, the filtrate of the biomass which was
treated with alcohol and converted into C32H30ON4H2(CO2H)2
was reacted with Zn/Cu (NO3) solution to form C32H30ON4Cu/
Zn(CO2H)2.105 Mixing of this solution and the synthesized
CNTs in an ultrasonic bath along with the appropriate quantity
of NaOH and ethanol resulted in intermediate structures of
CNTs with Cu/Zn functionalization. Further thermal treatment
of these intermediate residues at 350 8C for 2 h and reduction
in a hydrogen and nitrogen environment at 260 8C for 30 min
resulted in CNTs-Cu/ZnO nanocomposites being synthesized.105
Qu et al.106 also reported a similar procedure for the synthesis
of CNTs/Cu0.05Zn0.95O nanocomposites without employing a
reduction process.106 The synthesized carbon nanotubes and
CNTs/Cu0.05Zn0.95O nanocomposites have been explored for the
photodegradation of bisphenol A (BPA).106 In addition, Cong
et al.,107 reported the effective fabrication of CNTs, ZnO nano-
particles, and CNTs/ZnO nanocomposites using Physalis alke-
kengi L. biomass as feedstock. They adopted a similar process as
Qu et al.106 for the synthesis of these nanoparticles. The outer
diameter of the synthesized CNTs and CNTs/ZnO nanocompo-
sites were found to be 70 and 120 nm, respectively. They also
found excellent catalytic activity for the CNTs and CNTs/ZnO
nanocomposites in photodegrading BPA in aqueous media.
Vegetable Oils
Vegetable oils are chemically known as triglycerides and are
commonly extracted from plants using two different methods:
(i) mechanical extraction and (ii) solvent extraction. It has been
found that various types of vegetable oil precursors such as tur-
pentine oil, eucalyptus oil, neem oil, castor oil, soy oil, coconut
oil, and palm oil can be used for the synthesis of SWCNTs as
well as MWCNTs with the various microstructures. Research on
the exploration of waste precooked vegetable oils for the synthe-
sis of carbon nanotubes has also been reported; aiming to
address issues related to their disposal. Many processing techni-
ques including CVD and spray pyrolysis have been used for the
synthesis of CNTs from vegetable oils. The vegetable oils which
have been used for the synthesis of CNTs and their applications
are discussed in this section.
Turpentine oil was the first renewable resource based oil precur-
sor used for the synthesis of CNTs and has been used extensive-
ly by many researchers in order to optimize experimental
conditions. Turpentine oil is derived from oleoresin of Pinus
palustris of the pinaceae family; wide spread in Asia, Europe,
and the United States.108 The oil is a mixture of terpenes and
other essential oils whose propositions varies with many factors
including the species of tree the oil is extracted from and the
extraction process used.108 Chatterjee et al.109 first reported the
synthesis of carbon nanotubes from Turpentine oil as a renew-
able carbon source using the CVD process. Decomposing the
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turpentine oil on Co catalysts at 675 8C resulted in the forma-
tion of MWCNTs with a diameter range of 10–50 nm. The
obtained nanotubes have been used for the fabrication of elec-
trochemical supercapacitors. Afre et al.108 reported the synthesis
of CNTs from Turpentine oil as the carbon source and using
Fe/Co as bimetallic catalysts in CVD. They were able to produce
MWCNTs starting at 500 8C. However, a maximal yield of 33%
was achieved at 700 8C. TEM images of the CNTs grown from
turpentine oil at various temperatures are shown in Figure 4.
Synthesis of single-walled carbon nanotubes has been successful-
ly reported by Ghosh et al.110 by using a spray pyrolysis process.
Through this process, they were able to produce SWCNTs with
approximately 57% purity with significant graphitization. In
addition, Afre et al.111 reported the fabrication of vertically
aligned carbon nanotubes from Turpentine oil using spray
pyrolysis techniques. Silicon and quartz have been used as the
substrates for the vertical growth of CNT bundles. Ghosh and his
research team112 also explored the synthesis of aligned carbon
nanotubes from Turpentine oil as well as eucalyptus oil using the
spray pyrolysis technique. The obtained products were critically
compared in order to understand precursor–product relationships.
Scanning electron microscopic (SEM) investigation revealed that
the length of the synthesized CNT from turpentine oil is greater
than the nanotubes synthesized from eucalyptus oil; which influ-
ences their field emission properties significantly. Similar spray
pyrolysis processes have also been employed by Awasthi et al.31
for the large scale fabrication of aligned CNT bundles from tur-
pentine oil using ferrocene as catalysts at 800 8C in an argon envi-
ronment. The bulk synthesized CNTs exhibit outer diameters in
the range of 15–40 nm with improved graphitization.
Kumar et al.99 reported the synthesis of carbon nanotubes by
using neem oil and ferrocene as the carbon and Fe catalyst
sources, respectively, using the spray pyrolysis techniques. Neem
oil, commonly known as Margoaa oil, is extracted from the
seeds of the neem (Azadirachta indica) tree. TEM analysis of the
synthesized carbon nanotubes indicates the formation of multi-
walled structures with a bare central core and 15–20 nm diame-
ter. It has also been reported that the obtained carbon
nanotubes contain negligible amounts of Fe catalyst impurities.
Ghosh et al.113 reported the synthesis of single-walled carbon
nanotubes (SWCNTs) by using spray pyrolysis techniques from
eucalyptus oil as a carbon source with a Fe/Co impregnated
silica-zeolite catalytic support. The processing temperature used
was 850 8C. Eucalyptus oil is a colorless to pale-yellow liquid
with a chemical formula of C10H18O and boiling point of 176–
177 8C. The resulting SWCNTs exhibit very low levels of amor-
phous carbon which is thought to be due to the presence of
one oxygen atom per eucalyptus oil molecule. During the synthe-
sis process, this oxygen plays a vital role in oxidizing amorphous
carbon. Angulakshmi et al.114 reported the synthesis of CNTs
from soy oil as a carbon source through the spray pyrolysis tech-
nique using Fe/Co catalysts at an operating temperature of
650 8C in Ar. The obtained MWCNTs were investigated for their
ability to absorb basic brown 4 from aqueous solutions.
A key component in the fabrication of CNTs is the heating
source. Incorporation of microwave energy in processing system
leads to many technical benefits including reduction in
J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44255
REVIEW WILEYONLINELIBRARY.COM/APP

Figure 4. TEM images of the CNTs grown from turpentine oil employing different temperatures: (a) 500 8C, (b) 600 8C, (c) 700 8C, (d) 800 8C and (e)
900 8C. (Reproduced from ref. 108). [Color figure can be viewed at wileyonlinelibrary.com]

processing time, energy and cost savings, improved product
quality, and improving the ecofriendliness of the proce-
dure.115,116 Thus, microwave technologies have already been
explored by many researchers toward the synthesis of CNTs
using traditional carbon sources.117–119 However, very few
researchers have applied microwave heating sources for the syn-
thesis of CNTs using vegetable oil precursors. Raziah et al.120
reported the successful synthesis of CNTs with multiwalled
bamboo-like microstructures synthesized using a microwave-
assisted CVD method using castor oil as the renewable carbon
source. In their studies, they have used Fe/Co as a catalyst with
very low operational temperatures of 300–400 8C. They found
the resulted CNTs contained very low levels of metal impurities.
In addition, Tripathi et al.121 also demonstrated the synthesis of
CNTs using castor oil as a carbon precursor by using the ther-
mal CVD method. They have explored various transition metal
based catalysts such as Ni, Zn, and Co in order to investigate
their effect in synthesizing CNTs. They found that the Co cata-
lysts result in the formation of CNTs and spherical carbon par-
ticle mixtures, whereas Ni caused the generation of only
spherical particles. The synthesized CNTs have been effectively
used for the removal of arsenic contaminants dissolved in water.
Azmina et al.122 reported the synthesis of CNTs using five
different types of plant oils (coconut, corn, olive, palm, and

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REVIEW WILEYONLINELIBRARY.COM/APP
sesame) as the carbon source for thermal chemical vapor depo-
sition (TCVD) with a ferrocene catalyst. They were able to com-
pare the structure of CNTs synthesized from different resources
to determine a precursor–product relationship. Their research
findings revealed that the CNT produced from coconut oil
results in a better surface morphology, phase purity, and
enhanced crystallinity compared with the CNTs synthesized
from other resources. The density of the precursor oils was
found to play a vital role in the morphology and diameter of
the synthesized CNTs. In addition to this work, Sharma et al.123
also successfully demonstrated the synthesis of CNTs using olive
oil as carbon source for CVD. The synthesized CNTs were used
for the fabrication of dye sensitized solar cells.
Maryam et al.124 performed extensive research on the fabrica-
tion of CNTs from palm oil with a ferrocene catalyst through
aerosol-assisted catalytic CVD. The resultant MWCNTs con-
tained Fe, O, and Si with the O content being significantly high.
Thus, further adjustments of parameters were necessary in order
to enhance the carbon content in the final product. Their group
has also investigated the effects of processing temperature on
the synthesis of MWCNTs by employing a floating catalyst
TCVD method with Fe and Co catalysts.125 The structural and
other physicochemical properties of the obtained MWCNTs
were compared with their synthesis temperature which was
between 600 and 1000 8C. Increasing the deposition temperature
caused the formation of well aliened straight nanotube bundles
with high crystallinity as well as a higher carbon content; 900 8C
being the optimal temperature. Suriania et al.126 explored the
research on the effect of Fe and Co metallic catalysts on the
growth mechanism of carbon nanotubes, while using Palm oil
as a carbon source. Between the Fe and Co catalysts, Fe was
found to be the more suitable catalysts for the fabrication of
CNTs, whereas Co resulted in the formation of CNTs with big-
ger diameters and greater number of impurities.
Cooking the vegetable oils at the temperatures between 80 and
300 8C, lead to two major reactions: lipid peroxidation and
polymerization which causes a steep increase in the viscosity of
the oils. Repeated heating of these oils can cause the generation
of carcinogenic free radicals and toxins which lead to health dis-
orders.127 Thus, a major challenge for cooked vegetable oils is
their safe disposal. One of the possible solutions is to use them
as feedstock for the production of biodiesel. In addition, many
efforts have been made to convert the waste oils into carbon
nanostructures for various industrial applications. Suriani
et al.128 successfully reported the synthesis of vertically aligned
carbon nanotubes using precooked palm oil as the carbon
source. They used the floating-catalyst thermal CVD method at
750 8C under argon with a ferrocene catalyst. The obtained
CNTs were a combination of MWCNTs and SWCNTs which
may be due to the complex composition of the pre-cooked veg-
etable oils. Recently, Datta et al.129 reported the effective fabrica-
tion of one dimensional carbon nanowhiskers from pre-cooked
vegetable oils of mustard, soybean, sesame, and castor using a
dry autoclaving method. These initial results indicate the possi-
bility for various other precooked oils from vegetable and ani-
mal sources to be used for the fabrication of different carbon
nanostructures.
WWW.MATERIALSVIEWS.COM 44255 (8 of 15)
Plant Derivatives
Biobased materials or biochemicals derived from renewable
plant resources have been widely investigated as the carbon
source for the fabrication of different carbon materials. Kumar
and Ando130 reported the fabrication of CNTs from Camphor,
an extract from the latex of Cinnamomum camphora tree. The
CNTs were synthesized using CVD with Fe-Co-impregnated
zeolite catalysts at 650 8C. The camphor was vaporized at 200 8C
and fed into a small reaction tube along with argon gas. The
catalytically decomposed camphor turned into CNTs with a
source-to-CNT conversion efficiency around 50%, which is
much higher compared with most other reported values. A
CNT array was also produced using camphor and used as an
efficient field emitter.131 The research work has been extended
by Kumar and researchers for the synthesis of a nanotube gar-
den containing SWCNTs and MWCNTs.97 They have also con-
ducted extensive research into the various parameters such as
the vapor pressure of camphor, catalyst concentration, and tem-
perature of the reaction furnace on the diameter distribution of
the grown CNTs.132 At lower reaction temperatures between 600
and 700 8C, they found high yields of MWCNTs with uniform
diameters of approximately 10 nm, while increasing the furnace
temperature between 850 and 900 8C, significant quantities of
SWCNTs (30%) were formed with average diameters ranging
from 0.86 to 1.23 nm.132 From these investigations, it was found
that when camphor is used as a biofeedstock for CNT synthesis,
only extremely low catalyst concentrations are required and thus
the final CNTs contain extremely low catalyst impurities. Addi-
tionally, the formation of undesired amorphous carbons is also
almost non-existent and thus heating post-treatments for purifi-
cation are not required. Figure 5 shows the molecular structure
of camphor as well as the TEM and SEM images of various
morphologies of camphor grown carbon nanotubes; isolated
fibers (b), well-aligned CNTs (c), and garden of carbon nano-
tubes (d).97,130–132
Karthikeyan and Mahalingam100 reported the synthesis of
MWCNTs from biodiesel oil of Jatropha curcas through a spray
pyrolysis process employing Fe/Co/Mo catalysts well dispersed
on a silica/alumina substrate. The synthesized MWCNTs were
found in individual fibers with the diameters of 16–24 nm.
They have also investigated the fabrication of carbon nanotubes
from methyl ester of Pongamia pinnata oil by employing a
pyrolysis process.133 They used a similar Fe, Co, and Mo sup-
ported silica substrate catalysis system and employed different
processing temperature for the synthesis of the CNTs. The mor-
phological features of the carbon structures obtained at different
pyrolysis temperatures of 550, 650 and 750 8C were investigated
and it was found that the formation of MWCNTs occurred only
at 750 8C. They also reported the formation of vertically aligned
carbon nanotubes when the catalyst was changed to ferrocene
[Fe(C5H5)2]. Figure 6 indicates the structural evaluation of
CNTs from methyl ester of Pongamia pinnata oil with different
temperatures. Kumar et al.134 have also explored the spray
pyrolysis of jatropha-derived biodiesel as a green carbon source
for the synthesis of CNTs and carbon–nitrogen (CAN) nano-
tubes by employing ferrocene and ferrocene–acetonitrile cata-
lysts, respectively. The synthesized CNTs were found to be
J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44255
REVIEW WILEYONLINELIBRARY.COM/APP
Figure 5. Molecular structure of camphor (a) and the various morphologies of camphor grown Carbon nanotubes; isolated fibers (b), Well-aligned
CNTs (c) and garden of carbon nanotubes (d). (Reproduced from refs. 97, 130–132]). [Color figure can be viewed at wileyonlinelibrary.com]
20 mm in length with the average diameter of 20–50 nm. A bun-
dled morphology was found for the CAN nanotubes with
lengths of approximately 30 mm and average diameters of 30–
60 nm. It was found that increasing the reaction temperature
decreased the nitrogen concentration in CAN nanotubes which
is due to the enhanced graphitization in higher temperatures.134
The nanotubes grown from jatropha-derived biodiesel employ-
ing spray pyrolysis were clean from amorphous carbon impuri-
ties. Angulakshmi et al.135 were able to grow vertically aligned
CNT arrays on a silicon substrate using methyl ester of Helian-
thus annuus oil as a carbon source and ferrocene as a catalyst
for spray pyrolysis. It was identified that Fe nanoparticles were
formed on the silicon substrate through decomposition of the
ferrocene precursor. The produced CNTs had diameters between
10 and 30 nm and contained negligible catalyst impurities
Dubrovina et al.136 investigated a one-pot synthesis of CNTs
from polyisocyanate crosslinked cellulose acetate as a renewable
carbon resource. The synthesis was carried out along with a
NiCl2 catalyst and fumed silica as a template or a one-pot
pyrolysis process. The reaction mixture was carbonized in a
tube furnace under nitrogen at 750 8C with a 10 8C/min ramp
rate and 20 min holding time. The synthesized carbon nano-
tubes were found to be 24–38 nm in diameter with the wall
thickness ranging from 9 to 11 nm. Goodell et al.137 reported
the production of carbon nanotubes from wood fibers employ-
ing a two stage heating process: holding at 240 8C for several
WWW.MATERIALSVIEWS.COM 44255 (9 of 15)
hours and then cycling between room temperature and 400 8C
for 35 cycles. The resultant NTs had inner diameters of 4–5 nm
and outer diameters of 10–20 nm. The thermal ablation con-
verted components in the secondary cell wall into CNTs.131
Poultry Products
The increased global chicken meat consumption has led to the
formation of significant quantities of related by-products such
as feathers and waste fats which creates problems for their prop-
er disposal. It has been reported that the annual global chicken
feather production has increased to up to more than 5 million
tonnes.138 Chicken feathers can make up 5–7% of the chicken’s
body weight and are composed of 90–92% protein, namely
keratin, and 1–8% lipids.139 The common disposal mechanism
of poultry feathers is in landfills and the chemical resistive
properties of keratin due to its a-helix and b-sheet structural
packaging makes their biodegradation very slow; creating envi-
ronmental concerns.140,141 Recently, efforts have been made to
create applications for chicken feathers in biobased materials
such as polymer composites142–144 and pyrolyzed products for
hydrogen adsorption/catalytic applications.145,146 Senoz et al.147
have reported the effective fabrication of carbon fibers from the
pyrolysis of chicken feathers. They investigated the physico-
chemical changes to the chicken feathers through various tem-
perature ranges between 25 and 600 8C. The synthesized carbon
fibers exhibit an unique microporous architecture and exhibit
strong H2 adsorption at low pressures.148 Gao et al.149
J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44255
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Figure 6. Structural evaluation of CNTs from methyl ester of Pongamia pinnata oil with different temperatures. (Reproduced from ref. 133). [Color fig-
ure can be viewed at wileyonlinelibrary.com]

investigated the pyrolysis of waste chicken feathers using a with diameters of 1–5 lm and significant quantities (26%) of
supercritical carbon dioxide system. The pyrolysis process ammonium bicarbonate [(NH4)HCO3]. Following this, Gao
resulted in the formation of well-shaped carbon microspheres et al.102 reported the effective generation of nitrogen doped

Figure 7. Schematic representation of various stages involve in the production of CNTs from chicken feathers. (a) photograph of chicken feathers; (b)
and (c) the white and black products formed in the autoclave; FESEM images of Ni3S2@C (d) and N-CNTs (e); (f) the catalytic reaction of the synthe-
sized Ni3S2@ C or N-CNTs. (Reproduced from ref. 102). [Color figure can be viewed at wileyonlinelibrary.com]

WWW.MATERIALSVIEWS.COM 44255 (10 of 15) J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44255
REVIEW WILEYONLINELIBRARY.COM/APP
Figure 8. FESEM images of VACNTs generated from waste chicken fat employing Si substrate with ascending magnification. (Reproduced from ref. 103).
[Color figure can be viewed at wileyonlinelibrary.com]
carbon nanotubes. N-doped carbon nanotubes were generated
through two steps: first, the chicken feathers were autoclaved
with NiAcTa (C4H14NiO8) and dry ice in a small pressure vessel
and heated to 650 8C for 2 h. This resulted in the formation of
Ni3S2-carbon coaxial nanofibers (Ni3S2@CNF). In the second
step, the synthesized Ni3S2@CNF were treated with hydro-
choloric acid at room temperature for 12 h for the removal of
Ni3S2 particles, which resulted in the formation of N-doped car-
bon nanofibers. Schematic representation of various stages
involve in the production of CNTs from chicken feathers are
shown in Figure 7.
Chicken fat possesses a similar chemical structure to vegetable
oil and results in high C contents with lower C:H ratios.103 It
can be considered as a zero cost biofeedstock since it is dis-
carded during poultry processing. Unhygienic disposal of waste
fat lead to the contamination of water and creates harm to eco-
systems. Significant efforts have been devoted to convert chick-
en fat into biodiesel and biogas.103 However, biodiesel produced
from chicken fat contains high amounts of sulfur, which cause
technical challenges and the energy derived from chicken fat
biogas is not economically viable. As an alternative, Suriani
et al.103 investigated the effective utilization of the oil obtained
from waste chicken fat for the synthesis of carbon nanotubes. A
mixture of chicken fat oil with 5.33 wt% ferrocene catalyst was
converted into CNTs with CVD at 750 8C. The reported CNTs
were of high quality with a purity of 88.2% and tube diameters
ranging between 18 and 78 nm. They concluded that the physi-
cochemical features of the CNTs produced from chicken fat oil
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is comparable to those obtained using traditional feedstocks.103
Figure 8 shows the FESEM images of VACNTs generated from
waste chicken fat employing Si substrate. Following this, Dalila
et al.150 made systematic investigations on the effects of process-
ing temperatures on the structural and morphological features
of the CNTs from waste chicken fat. The synthesis process was
performed in a tubular furnace equipped with two heating
zones. First, the waste chicken fat was vaporized at a fixed tem-
perature of 470 8C and the second heating zone (reactive zone)
was been varied between 650 and 900 8C. No CNTs were pro-
duced within the reaction temperature range of 600–650 8C.
Increasing the reaction temperature to be between 750 and
800 8C resulted in the formation of vertically aligned CNTs.
800 8C treatments produced the highest yield with the smallest
diameters of 19.8–31.7 nm, 91% purity, and higher crystallinity.
Further increases to the reaction temperature (850–900 8C),
reduced the quality of the CNTs and increasing nanotubes
diameters were obtained.
EMERGING OPPORTUNITIES
An increased number of research articles in the field of renew-
able carbon indicate the possibility of sustainable materials in
future technologies. Renewable precursors have been used in the
fabrication of a wide range of carbon materials including, but
not limited to CNTs, graphenes, quantum dots, nanospheres,
fibers, and foams. For example, lignin has been widely explored
for the synthesis of carbon nanofibers. Also, significant impact
has been made by the spray pyrolysis process, which utilizes
J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44255
REVIEW WILEYONLINELIBRARY.COM/APP
liquid precursors, as an alternative to CVD for the synthesis of
CNTs from renewable resources. This has created more oppor-
tunities for a wider range of renewable precursors to be used as
CNT carbon sources. A wide range of renewable resources
including agro, forestry, and marine are available as precursors
for the synthesis of diversified carbon nanostructures. Reviewing
the research work already conducted on renewable resource
based CNTs clearly indicates emerging opportunities for
employing a wider range and variety of feedstocks. Only a limit-
ed amount of bioresources have been explored so far and thus
more research efforts must be devoted to extend this laboratory
research into real world application for a sustainable future.
CONCLUSIONS
This review article discussed the effective utilization of renew-
able resources as carbon sources for the fabrication of carbon
nanotubes as alternatives to traditionally used precursors.
Renewable precursors can be converted into CNTs using the
same technologies as with traditional precursors such as pyroly-
sis, CVD, and spray pyrolysis with no further modifications.
Although, traditional CNTs have been extensively used for many
device applications, the applicability of bioresourced CNTs have
not yet been heavily explored. During the conversion of biomass
into carbon nanotubes, there is a possibility for the formation
of a mixture of the various carbon products such as particles,
onions, and graphene. In order to address this challenge, efforts
needs to be made to not only avoid the formation of these
unwanted products but also to establish newer separation pro-
tocols. A wide range of applications need to be investigated and
correlated with the properties and structural features of CNTs
synthesized from renewable resources. Some additional renew-
able precursors which have, at the current point in time, not
been explored toward CNT synthesis were suggested for further
investigation. We believe that the synthesis of CNTs with differ-
ent controllable structural and morphological features from
renewable resources will attract many researchers globally as the
demand expands for sustainable and high-quality materials. The
present review can act as a resource, particularly for interdisci-
plinary researchers with interests in sustainable materials and
future technologies, hoping to get basic information on the cur-
rent state of green CNT synthesis and the types of investigations
which have been performed.
ACKNOWLEDGMENTS
The authors are thankful to the Ontario Ministry of Agriculture,
Food and Rural Affairs (OMAFRA)—New Directions & Alterna-
tive Renewable Fuels Research Program (Project # 049528); OMA-
FRA- University of Guelph Bioeconomy-Industrial uses Research
Program; the Ministry of Economic Development and Innovation
(MEDI), Ontario Research Fund - Research Excellence Round—4
program (Project # 200283); the Ministry of Research and Innova-
tion (MRI), Ontario Research Fund - Research Excellence Round—7
program (Project # 052644 and 052665); the Natural Sciences and
Engineering Research Council (NSERC), Canada for the Discovery
grants (Project # 400320 and 401111) and NSERC NIPMMP
NETWORK (Project # 400489) for the financial support to carry out
this study.
WWW.MATERIALSVIEWS.COM 44255 (12 of 15)
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