Composites Part C: Open Access 13 (2024) 100434

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Composites Part C: Open Access

journal homepage: www.sciencedirect.com/journal/composites-part-c-open-access

Critical review on the characterization, preparation, and enhanced

mechanical, thermal, and electrical properties of carbon nanotubes and
their hybrid filler polymer composites for various applications
Zulfiqar Ali a, Saba Yaqoob a, Jinhong Yu b, Alberto D’Amore c, *
a
Department of Mathematics and Physics, Università degli Studi della Campania “Luigi Vanvitelli”, Caserta 81100, Italy
b
Key Laboratory of Marine Materials and Related Technologies, Zhejiang Key Laboratory of Marine Materials and Protective Technologies, Ningbo Institute of Materials
Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China
c
Department of Engineering, Università degli Studi della Campania “Luigi Vanvitelli”, Via Roma 29, Aversa 81031, Italy

A R T I C L E I N F O A B S T R A C T

Keywords: Carbon nanotube (CNT) reinforced hybrid polymer composites offer multi-functional and sustainable materials
Carbon nanotube due to fascinating mechanical, electrical and thermal properties. However, many studies reported the impact of
Hybrid polymer composites CNTs orientation and synergistically enhanced properties of hybrid polymer composites but only a few review
Synergistic effects
literatures are published. This review provides a comprehensive overview of published research by addressing
Mechanical properties
Thermal-electrical conductivity
CNT classification, preparation methods, mechanical, thermal, and electrical properties, and potential applica­
Applications tions, as due to high strength, high young’s modulus, higher thermal and electrical conductivity these nano-
dimensional hybrid composites find many applications in aerospace, automotive, electronics, energy storage,
sensors, electromagnetic interference (EMI) shielding, engineering, and biomedical fields.

1. Introduction CNTs, being a one dimensional (1D) cylindrical, rolled up single-

With the increasing technology, the demand for multi-functional,
smart, lightweight, flexible, and cheaper materials is increasing
rapidly. This is why traditional materials, e.g., metals, cannot serve in
the industries. However, polymers are in abundance and able to replace
traditional materials with fascinating properties, e.g., low specific
weight, high corrosion resistance, low cost, easier molding, smart opti­
cal properties, and good electrical and thermal insulation, but due to
amorphous structure, low mechanical, thermal and electrical properties
are the bottleneck to their industrial applications. Thus, researchers
presented polymer composites as a replacement with desired properties.
Composite is a different materials (filler and matrix) amalgamation with
unique properties without losing the individuality of constituent mate­
rials in the combination. Usually, three types of polymer matrix are used
in making polymer composites, i.e., thermoplastic, thermosetting poly­
mers, and elastomers [1–4]. Fillers are specific materials mostly used to
enhance the stiffness and strength of polymers. Among others, Carbon
fillers, e.g., Carbon fiber (CF), Carbon nanotubes (CNTs), and Graphene
(G), efficiently enhanced the desired properties in polymer matrices
[5–7].
layered sheet of carbon atoms, are an ideal candidate for polymer
composites due to high tensile strength, high chemical stability, higher
elastic modulus, good thermal and electrical conductivity, stiffness and
light weight [8–10]. The excellent mechanical, thermal and electrical
properties of CNTs are due to their strong sp2 bonds between carbon
atoms, providing an accurate self-supporting atomic structure with
exceptional phonon-dominated thermal conductivity and high tensile
strength in axial direction [11]. Currently, CNTs reinforced hybrid filler
polymer composites have greatly attracted researchers due to adapt­
ability with multiple fillers (e.g., graphene, carbon fiber, silica, carbon
black, fullerene etc.), impressive network structures, and synergistically
enhanced interfacial strength, electrical and thermal properties. Carbon
nanomaterials, with high aspect ratios and lower density of CNTs (1D)
added with graphene (2D) deliver well-organized 3D structured
nano-sized hybrid filler and offer highly conductive polymer composites
with high tensile strength [12].
Indeed, when considering CNT hybrid filler polymer composites,
which involve the presence of multiple fillers alongside carbon nano­
tubes (CNTs) in polymers, it is essential to examine the potential limi­
tations of cost, scalability, safety, and regulatory challenges that are

* Corresponding author.
E-mail address: alberto.damore@unicampania.it (A. D’Amore).

https://doi.org/10.1016/j.jcomc.2024.100434

Available online 6 January 2024

2666-6820/© 2024 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
Z. Ali et al.
specific to this composite type. Due to CNTs production cost and in­
clusion in polymers with exotic fillers can considerably raise the mate­
rial cost. Thus, balancing the expenditure is crucial to achieving high-
performing complex filler combinations. These complex combinations
refer to ambiguities to maintain consistent quality at a larger scale with
new safety risks and regulatory challenges associated with using mul­
tiple reinforcing fillers. Specialized equipment, effective regulatory
policies, and material optimization could help resolve these issues.
Fig. 1 shows key features and advantages of CNTs as a hybrid filler
with multiple fillers to produce polymer composites with highly con­
nected structural configurations. In another study, MWCNTs/Epoxy
composites were produced with ultrahigh filler aspect ratios 10–68 wt.%
by hot-press infiltration technique. The MWCNTs were wrapped around
a semi-permeable membrane and epoxy resin was injected during the
processing. The aligned and randomly orientated CNTs composites were
produced, and the results were analyzed. The characterization results
revealed that at ultrahigh aspect ratio (68 wt.%), aligned CNTs com­
posites showed higher Young’s modulus (36 GPa) with enhanced elec­
trical conductivity [17].
The efficiency of CNTs-reinforced polymer composites is highly
related to the distribution of CNTs through polymer solutions. Pristine
CNTs are highly rigid, chemically inert, and have strong π–π in­
teractions, resulting in difficulties in obtaining advanced reinforced
composites with homogeneously dispersed CNTs. However, size, shape,
and high surface area highly aid CNTs’ distribution and adjustment of
polymers on CNTs’ surface, but high loading of CNTs leads to higher
viscosity due to high surface area and agglomeration phenomena. Ag­
gregation and solvent chemistry regulate the CNTs particle size distri­
bution and dispersion to resolve the above issue. For this purpose, CNTs
are chemically functionalized, which highly intrigues homogeneous
dispersion, adsorption energy, and interfacial adhesion between CNTs
and polymer matrices by hydrogen bonding interaction [18].
It can be concluded that the performance of CNTs relies on geometry
(size, shape) and fabrication techniques to attain adequate dispersion
and sufficient bonding through polymer matrices [19]. Li et al. [20]
fabricated CNT–graphene nanoplatelet GNP/epoxy composite via CVD
method and achieved ~40 % increased tensile modulus and ~36 %
enhanced tensile strength at merely 0.5 wt.% hybrid filler loading. Wu
et al. [21] prepared micro-structured MWCNTs-CFs/ methylphenyl sil­
icone resin (MPSR) composites by chemical grafting with enhanced
interfacial properties, impact toughness, and heat resistance. In another
Fig. 1. Key features of CNTs as a hybrid filler to fabricate polymer composites. Reproduced with permission from Refs. [13–16].
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Composites Part C: Open Access 13 (2024) 100434
study, Zhou et al. developed polyamide 6 (PA6)/ functionalized gra­
phene (FG)/functionalized (FCNTs) composites by electrospinning and
at loading of FG (0.2 wt%)/FCNTs (0.3 wt%) the mechanical properties
were increased unto 2.4 times of pure PA6, with 132 % enhanced
Young’s modulus. Additionally, there are many references to disclose
the potential of CNT composites and methodologies employed [22–27].
This study encapsulates the classification of CNTs and mainly focuses
on currently adopted techniques and preparation methods for CNTs and
hybrid polymer composites. The impacts of filler aspect ratios, disper­
sion effects, and geometrical configurations on mechanical, electrical,
and thermal properties reported in published research are discussed in
detail. Moreover, to better introduce the multifunctionality of CNTs
hybrid filler polymer composites, applications in macro-level industries
(aerospace, automotive, electronics, energy storage devices, and wind
turbine blades) are also reviewed. In the last part, the conclusion and
prospects will be briefly discussed.
2. Classification of CNTs
CNT is a hollow 1D carbon tube with a nanometer diameter range,
obtained by rolling a 2D graphite sheet into a cylindrical shape. These
structures were accidentally discovered by Japanese physicist Sumio
Iijima (1991) during the fullerene synthesis by the electric arc discharge
method [28,29]. Based on structure, CNTs are classified into two major
categories: single-walled carbon nanotubes (SWCNTs) and multiwalled
carbon nanotubes (MWCNTs). SWCNTs, also called graphene nanotubes
(GNTs), consist of only one graphene layer rolled cylindrically with
one-atom thickness, two micrometers length, 0–2 electron volts (eV)
bandgap, and a diameter of two nanometers. While synthesis, the
cap-like closed-end SWCNTs are obtained with C-C bond, forming a ring
at both corners. Due to the variable arrangement of carbon atoms,
SWCNTs possess three configurations: armchair, zigzag, and chiral
structure. Depending upon the arrangement of chiral vectors, SWCNTs
show exceptional electronic properties and can also be employed as
semiconductors, like in transistor applications [30–32]. Fig. 2 shows the
formation of CNTs and the classification of SWCNTs and MWCNTs.
However, MWCNTs are based on multiple (2–10) concentric gra­
phene layers, cylindrically rolled into a tube shape with one atom
thickness, 0.5–50 µm length, and internal diameter of more than ten
nanometers. Based on structural arrangement, MWCNTs can be
described by two main models. First, the Russian doll model, where
Z. Ali et al.
Fig. 2. Overview of SWCNTs’ and MWCNTs’ formation and different configurations of both types of CNTs. Reproduced with permission from Refs. [33–35].
individually rolled graphite sheets are settled in concentric cylinders.
Secondly, the Parchment model, where a single graphite sheet is rolled
around itself consistently like a jellyroll or rolled newspaper. Third,
mixed MWCNTs based on the Russian doll and Parchment models
[30–32,35–37]. MWCNTs come in different complex arrangements in
which each concentric tube can have different sequential structures and
thus possess unique properties. Hence, MWCNTs have high aspect ratios
and are far stronger than SWCNTs, so practically, these are preferred for
high mechanical applications [32].
3. Preparation methods for CNTs
Many impurities and side reactions always accompany the synthesis
of CNTs, while the type and amount of these impurities rely on the
adopted preparation technique. Hence, purity is a crucial factor in
determining a material’s actual ability and properties; thus, much
research was made to explore innovative preparation methods for CNTs
to attain maximum purity with the least side reactions. Several tech­
niques to develop CNTs are reported in different literature listed below
[38].
3.1. Electric/plasma arc discharge method
Electric arc discharge is an extreme temperature (>1700 ◦ C) based
technique first employed for CNTs synthesis by Sumio Iijima in 1991. It
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Composites Part C: Open Access 13 (2024) 100434
is the easiest and most used method to attain CNTs with fewer structural
defects than other techniques. This technique is based on a vacuum
chamber with two water-cooled graphitic electrodes detached by 1–2
mm, with a diameter (6–12 mm), and the chamber filled with an inert
gas Helium (He) or Argon (Ar) at high pressure about 500 torr (inert gas
can also be replaced by methane or hydrogen) [39,40]. During the
process, the two graphite electrodes (anode, cathode) approach each
other, making an arc, and temperature increases (3000–4000 ◦ C) suffi­
cient to sublimate the carbon-contained anode. This vaporized carbon is
accumulated at a 1 mm/min rate on the cathode (negative electrode) in
the form of a black soot, and the remaining carbon is deposited (hard
gray shell) on the chamber’s walls. The scanning electron microscopy
(SEM) images showed the formation of MWCNTs and also fullerene,
amorphous carbon, and graphite sheets [38,40].
The arc discharge method can be employed to obtain both SWCNTs
and MWCNTs. The key difference between both types of synthesis is the
use of a catalyst, as in the synthesis of MWCNTs, there is no need for a
catalyst precursor, while SWCNTs can be achieved by using metallic
catalysts, e.g., Nickel (Ni), Cobalt (Co), Iron (Fe), Silver (Ag), Palladium
(Pd), Platinum (Pt) and alloys. The catalyst (metal powder) is packed
into a hole in the anode, and thus, small-diameter SWCNTs are achieved
using a complex anode. However, a Nickel-Yttrium (Ni-Y) graphite
mixture is mostly used to get a high yield (about 90 %) of SWCNTs with
an average diameter of 1.4 nm [41]. Fig. 3 represents the schematic
framework of the arc discharge method.
Z. Ali et al.
Fig. 3. Schematic electric/plasma-arc discharge technique setup for CNTs synthesis. Adopted with permission from Ref. [42].
The main advantages of this technique are the ability to produce
CNTs in large quantities, the simple procedure, and the lack of need for
multi-step purification. The disadvantages are a high-temperature
requirement, the need for a metallic catalyst, purification of the ob­
tained product, and no control over the alignment (chirality) of pro­
duced CNTs [41,43]. Moreover, this method primarily consumes a
substantial amount of energy, so high-power levels are used, resulting in
increased carbon emissions. Also, the reliance on inert gases, e.g., heli­
um or argon, waste generation and use of catalyst materials in this
process can cause serious environmental issues. Greener gases can be
explored to address these concerns, and effective strategies for catalyst
recycling and waste reduction can be developed to boost energy effi­
ciency and prevent environmental and health hazards.
3.2. Laser evaporation method
The laser ablation/evaporation process is like an electric arc
discharge method in many aspects e.g., high temperature, inert gas-
filled chamber, water-cooled surface, and use of metallic catalyst
(mostly Ni or Co in this method) for SWCNTs synthesis. The key dif­
ference is that unlike producing a graphite electrode arc by electric
current, a pulsed and continuous laser beam (Nd: YAG) with wavelength
(355 or 1064 nm) is used to evaporate the graphite target [44]. In this
method, a quartz tube containing the graphite block is placed in the
chamber filled with He or Ar gas and high-power laser vaporizes the
graphite billet at the temperature (1200 ◦ C), and CNTs are obtained with
few impurities. It was also observed that the diameter of produced CNTs
is highly dependent on laser power, i.e., by increasing the power of the
laser, smaller diameter CNTs can be attained [45]. Fig. 4 briefly
Fig. 4. Schematic representation of laser evaporation/ ablation method. Adopted with permission from Ref. [46].
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Composites Part C: Open Access 13 (2024) 100434
indicates the working setup of the laser ablation method.
This method is advantageous for producing CNTs with fewer metallic
impurities and thus less need for purification processes. However, it is
not beneficial for the economical production of CNTs because of the
need for high-purity graphite rods and high laser power. Moreover, the
produced CNTs are not necessarily uniform, and high-temperature
control is needed because the structure obtained below 1200 ◦ C has
many defects, and below 200 ◦ C, CNTs are not produced [40,41].
Additionally, the high-energy laser used in this method results in
significant energy consumption and carbon emissions. Also, operating in
an inert gas environment and using metal nanoparticles as catalyst
materials with waste production can emit airborne nanoparticles,
causing severe environmental impact. Thus, using greener gases, recy­
cling catalysts, employing waste reduction and management policies,
and ensuring safety measures can improve energy efficiency and reduce
environmental concerns.
3.3. Chemical vapor deposition method (CVD)
Chemical vapor deposition (CVD) is the most used technique
commercially producing CNTs. The key difference between CVD and
other methods is that, here, the CNTs are obtained by the decomposition
of carbon-containing compounds, while in prior methods CNTs were
produced by sublimation of graphite. However, researchers currently
employ many CVD types, e.g., catalytic CVD, plasma enhanced oxygen
assisted CVD, radiofrequency assisted CVD, water-assisted CVD, mi­
crowave plasma-enhanced CVD, and hot filament CVD. Moreover, the
CVD method may vary based on reactor pressure (high, low or atmo­
spheric), reactor type (hot wall or cold wall CVD), and carbon source
Z. Ali et al.
(solid, liquid or gas) [47–49].
Apart from others, catalytic chemical vapor deposition (CCVD) is
currently popular for highly pure and large-scale CNT production of
CNTs. In this method, a gaseous precursor reacts and makes a solid
coating on a heated (500–1000 ◦ C) substrate placed in the reactor,
producing CNTs. The schematic process is as follows: a substrate with a
catalytic metal (Ni, Co, Fe, or combined) layer is placed and heated in
the reactor, and a gaseous precursor (usually consisting of inert gas and
hydrocarbons) enters the chamber at room temperature [50,51]. The gas
is heated as it approaches the heated substrate, chemical reactions
occur, and CNTs start growing at the corners of catalytic metal particles
on the substrate (based on adhesion between catalytic particles and
substrate, the catalytic metal particles can be on the top or bottom of
growing CNTs). In contrast, waste gases are removed by gas outlets. This
technique can produce both MWCNTs and SWCNTs. However, the type
of CNTs (MWCNTs, SWCNTs) production is based on temperature and
gas precursor. Usually, MWCNTs are produced at 600–800 ◦ C and
SWCNTs at 900–1000 ◦ C. The diameter of CNTs depends on the size of
catalytic metal particles [52,53].
The advantages of the CVD technique are more significant control of
CNTs production parameters, no need for expensive graphite rods, lower
temperature requirement (500–1000 ◦ C), and highly pure large-scale
production of CNTs [54]. The disadvantages are structural defects in
CNTs, chances of non-compatibility of materials for chemical reaction,
and chemical and safety threats due to toxic, combustible, explosive,
and corrosive gas precursors used in some cases [55]. Reactor configu­
rations for CVD synthesis typically include a reaction chamber with
tubes containing an inert gas and specific hydrocarbons, as shown in
Fig. 5(a). SWCNT production commonly employs methane, while
MWCNTs use ethylene or acetylene. The process involves heating the
substrate to temperatures between 850 and 1000 ◦ C (for SWCNTs) or
550 and 700 ◦ C (for MWCNTs). During thermal decomposition, carbon is
generated from the hydrocarbons and dissolves into the metal nano­
particle catalyst. A semi-fullerene cap forms once a critical carbon
concentration is reached, serving as the initial structure for cylindrical
shell nanotube growth (Fig. 5b and c). This growth occurs through a
continuous flow of carbon from the hydrocarbon source to the catalyst
particle. The schematic steps of the CVD process are shown in Fig. 5.
However, the CVD method often relies on hydrocarbon gases, and
maintaining high temperatures for CNT growth may result in green­
house gas emissions and air pollution. To break the limit, research is
ongoing to develop sustainable precursor gases, like methane from
renewable sources or captured carbon dioxide. Additionally, efficient
Fig. 5. Schematic process of catalytic chemical vapor deposition (CCVD) (a) Representation of CVD process and CNTs growth (b) CNT base growth mechanism (c)
CNT tip growth mechanism. Adopted with permission from Ref. [56].
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reactor designs and recycling of precursor gases and catalyst materials
can reduce the energy requirements and help mitigate the CVD process’s
environmental effect.
In conclusion, there are challenges in the traditional production
methods of CNTs. Although different approaches e.g., arc discharge in
liquid media (water or ionic liquids lowers the requirement of inert
gases), bacterial synthesis (micro-organisms used to produce CNTs,
lowering the demand for high temperatures and toxic chemicals), solar
thermal synthesis (CNT synthesis using solar energy, reduces carbon
emissions and the need for traditional energy sources, green solvents,
hydrothermal synthesis, and plasma enhanced CVD offer environment-
friendly production of CNTs but lack in commercial production.
4. Preparation methods for CNTs/Polymer composites
The processing method, orientation, and CNTs dispersion signifi­
cantly impact the performance of CNT/polymer composites. Thus, many
techniques have been adopted in practice to integrate CNTs into the
polymer matrix, and CNTs’ dispersion was a major issue. Without
appropriate dispersion the CNTs tend to accumulate and, as a structural
defect, restrict composites’ mechanical and physical properties. How­
ever, the alignment of CNTs through the polymer composites provides
effective routes for phonon transmission. Thus, orientation improves the
thermal and electrical properties of CNT/polymer composites [57–59].
Traditionally, there are three major techniques for preparing CNT/
polymer composites.
4.1. Conventional approaches
4.1.1. Solution blending
Solution mixing is a versatile technique for large-scale production of
nanocomposites without losing the properties of nano-sized fillers. It is
also a widely used for fabricating CNT/polymer composites in labora­
tories [57,60]. In this method, CNTs and polymer matrix are dispersed
separately in (similar or different) solvents with good miscibility and
then mixed. The process is followed by intensive agitation, e.g.,
ultra-sonication, magnetic stirring, strong shaking, and high-speed ho­
mogenization. Finally, a CNT/polymer composite film is formed by
solvent vaporization (with or without vacuum assist).
However, CNT/polymer composite can also be produced by directly
mixing CNTs into the polymer solution, followed by intense ultra-
sonication and shear homogenization for a long time. However, it
damages the CNTs (shortening of length), causing the lower
Z. Ali et al.
performance of resultant composites. However, surface functionalized
CNTs offer better dispersion and interfacial bonding with polymer ma­
trix, improving composites’ mechanical, thermal, and electrical prop­
erties. The selection of solvent is also an essential parameter for the
production of composites. Usually, low boiling point solvents are
preferred because evaporation of high boiling point solvents is complex,
and it may get trapped during the solidification of composites, causing
structural defects. The low-viscosity solvents allow better dispersion
[61–64].
The main advantage of this method is the probability of de-bundling
of CNTs to provide quality dispersion [65]. Nevertheless, this technique
has some disadvantages, such the possibility of leaching of added con­
stituents and possible environmental contamination due to the large
amount of solvent, and it provides no solution for insoluble polymers
[58].
4.1.2. Melt blending
Melt blending is a simple, environmentally friendly, low-cost alter­
native method for insoluble thermoplastic polymers to produce com­
posites. Thermoplastic polymers become soft when heated at elevated
temperatures and hard when cooled. Thus, polymer pellets are melted in
this method, and viscous liquid is mixed with additives, e.g., CNTs,
followed by shear forces using Banbury mixer and extruder machines. At
the end, the sample is air dried or passed by a water bath to solidify and
cut into desired dimensions and shapes. In this way, a high sample
volume can be produced [58,60,66,67].
This method is fast and industrially friendly, and no solvent is needed
for processing [68,69]. However, this technique has some drawbacks, e.
Fig. 6. (a) Schematic representation of the LBL film-deposition. Steps 1 and 3 show the adsorption of polyanion and polycation, steps 2 and 4 represent washing
steps. (b) Two adsorption paths, LBL deposition for polymers and polymers with nanoparticles. Adopted with permission from Ref. [73].
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g., CNTs and polymer chains may be disrupted, and thus, intrinsic
properties might diminish due to high shear forces and temperature [58,
70].
4.1.3. In situ polymerization/ reaction processing
In situ polymerization is another efficient approach for CNT distri­
bution in insoluble and unstable polymers that cannot be handled by
solution blending and melt processing methods. During its processing,
dispersed CNTs are first mixed with a monomers solution, and finally,
CNT/polymer composites are achieved followed by certain conditions
[62,71,72]. The polymerization of thermosetting material, e.g., Epoxy,
unsaturated polyester (PET) is initiated by a curing agent/hardener as a
catalyst. Polymerization occurs in thermoplastics by temperature raising
or adding an initiator [60].
This technique is beneficial for homogenous and uniform distribu­
tion and compatibility of filler-matrix and provides a strong interaction.
However, there are some disadvantages, as this processing involves
expensive equipment and requires a large volume of solvent [58].
4.2. Modern approaches
4.2.1. Layer by layer (LBL) assembling method
The LBL is a simple, cheap, and effective technique to fabricate
molecular assemblies of multi-functional tailored materials with nano­
meter thickness, which can be used in high-scale production of highly
integrated micro-sensors.
The processing of this method, Fig. 6(a) and (b), is followed by
dipping a substrate into the dispersed solution of CNT and
Z. Ali et al.
polyelectrolyte. A thin composite film is created on the substrate and
washed with pure water to remove weakly bonded polyelectrolytes. The
substrate is first dipped into the positively charged polyelectrolyte so­
lution and later into the negatively charged polyelectrolyte solution to
achieve a double-layered composite film [74,75]. This approach can also
be employed in the fabrication of inorganic nanoparticles (nano-wires
and nano-sheets) into organic polymers, and it is easier to control the
CNT ratio and thickness of prepared composites [73,74].
4.2.2. Swelling method
The swelling technique is an efficient approach to producing high-
strength and robust CNT/polymer composites. It allows us to intro­
duce CNTs in temperature-sensitive and insoluble polymer products.
This approach allows CNTs to be dispersed even in very small-thickness
polymer film and produce composites with high mechanical, thermal,
and electrical properties. Ian et al. [76] produced CNT-reinforced Kevlar
composites using the swelling method. While processing, MWCNTs and
commercially available Kevlar fiber-based suspension was produced
using N-methylpyrrolidone (NMP) as solvent under ultra-sonication.
The Kevlar fiber swells, and CNTs diffuse into the fiber during the pro­
cess. Finally, the sample was dried and characterized, resulting in
improved mechanical properties of Kevlar-CNT composite. In another
report, conductive CNT-based polyethylene (PE) composites were pre­
pared by utilizing the same strategy i.e. MWCNTs were dispersed into
the swelled thin PE film using tetrahydrofuran (THF) as a solvent and
the process was followed by ultra-sonication [74].
4.2.3. Bucky paper (BP) based method
Bucky paper (BP) is a porous and very thin sheet of CNTs incorpo­
rated by filtration of CNTs dispersed in a suitable solvent. In this
approach, the BP is filled with a polymer matrix or introduced between
laminates and polymer composites, producing excellent mechanical and
electrical properties [74,77,78]. Besides Buchner filtration, BP can also
be produced by the domino-pushing effect. The MWCNTs are vertically
aligned in this method on a silicon substrate (10 cm diameter). Later, a
microporous membrane is placed on the top and pressed by constant
pressure. This process is repeated several times, and finally, the silicon
substrate is detached, and BP is peeled off from the porous membrane by
ethanol. This BP is strong and flexible with improved electrical (2.0 ×
104 S/m) and thermal (153 W m− 1 K− 1) properties [79].
Teotia et al. [80] prepared BP-based phenolic resin composites. The
MWCNTs were dispersed in acetone and then added to phenolic resin.
The suspension was stirred for 5 min by a high-speed mixer (3000 rpm)
to get a homogeneous amalgamation. Later, the mixture was filtered by
a specially designed filtration system. The filtered material was dried
and compression molded, resulting in BP-phenolic resin composite
paper. In another study, Kim et al. [81] introduced MWCNT BP and
electro-spun polyacrylonitrile (PAN) nanofibers based ultrathin, light­
weight composite membranes using electrospinning, thermal-rolling,
and vacuum filtration. As a result, smooth surfaces, high surface en­
ergy, and impressive mechanical strength of 19 MPa were achieved with
an enhanced interfacial network between the buckypaper and nanofiber
Fig. 7. Schematic representation for synthesis of BP-based nanofiber (BP/NF) composite. Adopted with permission from Ref. [81].
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Composites Part C: Open Access 13 (2024) 100434
substrates by thermal rolling at 130 ◦ C. Remarkably, a 100 μm thick
composite membrane showed a specific shielding efficiency of 13,734
dB cm2 g− 1, surpassing previous MWCNT/polymer composites. Several
studies have reported excellent mechanical, electrical, and thermal
properties of polymer composites produced by the BP-based approach
[82–86]. Fig. 7 shows the whole schematic process of the experiment.
However, conventional and current preparation methods of CNTs
hybrid polymer composites suffer significant limitations concerning
scalability, advanced apparatus requirements, and expenditure. For
example, traditional methods like solution blending, melt blending, and
in situ polymerization are effective at smaller scales but do not suffice for
industrial production. Ensuring bulk production with greater control
over quality requires specialized equipment, which results in extended
costs and compact practicality. While modern techniques, e.g., LBL
assembling, swelling method, and BP approach, are effective but
complicated and laborious. Such issues can be resolved by advanced
automation and process optimization. Thus, there is a need to explore
cost-effective equipment by recognizing sustainable material resources.
5. CNTs hybrid filler polymer composites
CNTs are a promising candidate for fabrication of polymer compos­
ites due to higher strength, high elastic modulus, surface area, stiffness,
porosity, corrosion resistance, mechanical and chemical stability, and
remarkable mechanical, thermal, and electrical properties [87]. Due to
exceptional nanostructure and properties, CNTs are an ideal precursor
for polymers, metal/alloys, and ceramic composites [88]. The bulk
production of composites by using primary filler, e.g., CNT, is inflated.
Thus, secondary filler is introduced to reduce the cost.
However, due to the nano-sized structure and reacting ability of
CNTs, there is a higher probability of health risks during the production
and execution of nanocomposites. Mainly, handling the airborne and
disposal of CNTs is problematic, and it causes severe toxic effects if
inhaled, e.g., lung cancer, pleural malignant mesothelioma, and respi­
ratory issues. Research is ongoing to make CNTs ecologically sustainable
and reduce harmfulness through surface modifications.
Currently, graphene oxide [89], silica [90], carbon black (CB) [91],
zinc oxide (ZnO) [92], nano-clay (NC) [93], conductive carbon black
(CCB) [94] and graphite [95] are used as secondary filler to produce
CNT hybrid filler. Graphene has incredible properties, e.g., flexibility,
lightweight, fire resistance, exceptional electrical and thermal conduc­
tivity, higher modulus, and strength. CNT and Graphene particles (GP)
hybrid filler-based natural rubber (NR) composites were prepared, and it
was observed that a combination of 3 phr CNT and 30 phGP showed
excellent performance in relaxation modulus and thermal stability of
CNT/GP-NR composites as compared to CNT-NR and GP-NR composites.
The characterization showed that CNT networks improved GP disper­
sion and prevented agglomeration, facilitating electron tunneling. Due
to the connected filler network, the conductive properties and dielectric
constant of NR composites was significantly improved [96].
Luo et al. [97] introduced pristine CNTs and functionalized f-CNTs in
polymethyl methacrylate (PMMA)/GNP composite to produce a hybrid
Z. Ali et al.
composite (PMMA/GNP/f-CNT) with three-dimensional (3D) structure
with different ratios. The investigation of these composites showed 3D
networks inside, and due to synergistic effects, the thermal and electrical
conductivity was significantly improved in the perpendicular direction.
Skórczewska et al. [98] prepared poly-vinyl chloride, carbon
fiber/multiwalled-carbon nanotube (PVC/CF/MWCNT) hybrid com­
posites with hybrid filler ratios 1 wt.%, 5 wt.% and 8 wt.%, respectively.
The Processing of composites was followed by coating of CNTs onto CFs
using polyvinyl acetate (PVAc) as an adhesive for better dispersion. It
was demonstrated that with increase of filler content the electrical
properties improved, while elastic modulus, rigidity and impact strength
of composites was significantly increased and thermal stability slightly
enhanced. Nabinejad et al. [99] developed pristine MWCNTs and oil
palm shell (OPS) powder-based unsaturated polyester (UP) composites
using a solvent mixing technique with ultrasonication. Initially, the
MWCNTs were precisely dispersed in four different solvents, e.g.,
acetone, styrene, ethanol, and methanol. Secondly, polyester resin was
added by shear mixing and ultrasonication. Later, the solution was
heated to evaporate the solvent. Lastly, the natural filler OPS was added
and prepared composite solution was passed through molding and
casting process. The investigation of these hybrid composites revealed
that, increasing the MWCNTs content (0.2–0.4) phr leads to maximum
tensile and flexural strength, while increasing the MWCNTs content (>
0.4 phr) the viscosity increases, and tensile modulus starts decreasing
due to structure abnormalities.
Liu et al. [100] introduced CNT/CF hybrid filler to prepare epoxy
composites for industrial scale. While preparing, the CNT was initially
functionalized with an amine monomer by a chemical modification
process to achieve better dispersion in a sizing agent. Later, the CNT
accompanying sizing agent was uniformly dispersed on the CF surface.
After drying, the epoxy-containing hardener was infused through a
hybrid filler. The process was followed by solution blending and soni­
cation methods. FTIR and XPS characterized the specimen, and it was
observed that integration of CNT at the interface highly improved the
interfacial shear strength of the prepared material.
CNT hybrid composites offer many real-world industrial applica­
tions, such as in the automotive sector, utilization of CNT composites in
Ford’s GT supercar wheels greatly enhanced fuel efficiency and perfor­
mance. CNT composites are applied in tennis rackets HEAD and Babolat
to achieve rigidity and reduced vibration. In electronics, CNT-based 3D
printed filaments offer electrically conductive components, which assist
in the prototyping of electrical devices. In textiles, CNTs are utilized in
smart fabric brands, e.g., Under Armour, for moisture, odor, and per­
formance control of sportswear. Moreover, CNT composites are used in
Boeing 787 Dreamliner for reduced weight and enhanced fuel efficiency.
6. Mechanical properties of CNT hybrid filler polymer
composites
CNTs own high mechanical properties, e.g., higher modulus
(270–950) GPa, higher tensile strength (11–63) GPa, and lower density
(2.1) gcm− 3, due to unique structure with regular arrangement of sp2
covalently bonded carbon atoms making it suitable filler for polymer
composites. Moreover, CNTs synergize with other potential fillers and
provide extraordinary mechanical properties [62,101–103]. Effective
distribution and homogeneous dispersion of CNTs through the polymer
matrices play a key role in constructing interconnected 3D structures,
which lead to outstanding mechanical properties [104].
Park et al. [103] reported MWCNTs and CFs hybrid filler-based
alkali-activated slag (AAS) composites using a solution blending tech­
nique. The investigation results revealed synergistic effects due to the
formation of bridging structures. The hybrid composite formation was
followed by diverse proportions (0, 0.1, 0.5, 1.0, and 2.0) wt.% of hybrid
fillers, and it was noted at 0.5 wt.% of MWCNTs and CFs, a highly
connected structure was produced which showed enhanced mechanical
and electrical properties.
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Composites Part C: Open Access 13 (2024) 100434
Dehrooyeh et al. [105] fabricated glass fiber/CNT/epoxy hybrid
composite to obtain higher mechanical properties. The experiment was
carried out in two significant steps. Firstly, the CNT/Epoxy composites
were prepared using CNT aspect ratios 0.1, 0.5 and 1.0 wt.% by solution
blending method and tested for mechanical properties. It was observed
that a composite with 0.5 wt.% of CNT showed higher Young’s modulus
of 1.8 GPa and a tensile strength of 61 MPa.
In the second step, the glass fiber/CNT/epoxy hybrid composite was
prepared by a hand-layup approach using a 45:55 filler-to-matrix ratio.
The investigation showed that hybrid composite followed the same
trend, i.e., at 0.5 wt.% CNT loading the ultrahigh Young’s modulus of
24.9 GPa and a tensile strength of 300 MPa were achieved.
Fig. 8(a) shows SEM images for CNT dispersion in the epoxy with
various ratios of 0.1, 0.5, and 1.0 wt.% and at 0.1 wt.% there are few
CNTs with uniform distribution and no agglomeration. Moreover, at 0.5
wt.%, the structure is more organized, and dispersion is homogeneous
with no accumulation of CNTs. Meanwhile, with 1.0 wt.%, the viscosity
increases, and CNT agglomeration causes structural defects and abnor­
malities, decreasing the mechanical properties. Fig. 8(b) shows stress-
strain curves of CNT/Epoxy composite with CNT aspect ratios (0.1,
0.5 and 1.0) wt.%, and Fig. 8(c) shows stress-strain curves for glass
fiber/CNT/epoxy hybrid composite with CNT loading (0, 0.5 and 1.0)
wt.%.
In another research, Xu et al. [106] fabricated Graphene oxide/­
carbon nanotube aerogel-based polystyrene (GOCA/PS) hybrid com­
posites by hot pressing and in-situ polymerization processes and
explored the compressive, flexural, tensile, and impact strengths with
different filler loadings (0, 0.8, 0.9, 1.0, 1.1 and 1.2) wt.%. In the
fabrication process, the GOCA large-size sheet was prepared and sub­
merged in a solution containing a 40 g PS mixture and 0.18 g of azo­
bisisobutyronitrile (AIBN) (analytical reagent). Later, the samples were
passed through different temperature ranges for 12 h, hot pressed, and
molded. Finally, the prepared GOCA/PS composites were tested for
mechanical properties.
As shown in Fig. 9, all four properties improved with increasing filler
content. The calculated increased values compared to pure PS were as
follows: tensile strength (103.29 %), flexural strength (60.30 %),
compressive strength (177.03 %) and impact strength (611.38 %).
However, in Fig. 9(a) at loading 0.8 wt.%, the curve line followed the
same trend as pure PS. This is due to a very low aspect ratio, and the
GOCA was probably destroyed during the in-situ polymerization process.
The results were excellent at 1.1 wt.% compared to 1.2 wt.% due to
increased density and porosity with increasing content ratio causing
structural defects and deprivation of mechanical properties. Fig. 9(b)
presents flexural stress-strain curves, Fig. 9(c) impact strength, and
Fig. 9(d) compression stress-strain curves. These graphs provide concise
and essential information about the material’s mechanical behavior
under different loading conditions.
7. Thermal properties of CNTs hybrid polymer composites
With the increasing demand for multi-functional and smart mate­
rials, overheating of devices is inevitable, and thus, the fabrication of
high thermal conductive, heat dissipative polymer composite materials
can resolve this issue. CNTs possess unique and strong configurations
with high in-plane thermal conductivity (3000–3500 Wm− 1 K− 1) [107],
which makes them ideal fillers for polymer matrices. CNTs are highly
effective in the thermal conductivity enhancement of hybrid polymer
composites due to synergistic behavior with other fillers by the forma­
tion of 3D bridge networks, which facilitates phonon transmission [108,
109].
Li et al. [110] designed hexagonal boron nitride (h-BN), reduced
graphene oxide (rGO), and CNTs based epoxy (EP) composite using a
layer-by-layer technique. In the fabrication process, the h-BN was
modified with tannic acid (TA) for better dispersion in EP coatings and
later blended with rGO and CNTs. The prepared TA@BN-rGO-CNT/EP
Z. Ali et al. Composites Part C: Open Access 13 (2024) 100434

Fig. 8. (a) Dispersion of CNTs in epoxy matrix at 0.1 wt%, 0.5 wt%, and 1 wt%. (b) Stress-strain curve of CNT/epoxy nanocomposites at different CNT weight
percentages. (c) Stress-strain curve of glass fiber/CNT/epoxy hybrid composites. Adopted with permission from Ref. [105].

Fig. 9. Mechanical properties (a) typical stress-strain curves, (b) stress-strain curves of flexural, (c) impact strength, (d) stress-strain curves of compression. Adopted
with permission from Ref. [106].

composite were investigated for higher thermal conductivity. It was reported the role of CNTs as a hybrid filler in the thermal conductivity
demonstrated that a well-defined interconnected hybrid structure was enhancement of polymer composites [111–114]. However, some refer­
produced and at 46 Vol% filler loading the thermal conductivity reached ences are added and explained in this study.
5.65 Wm− 1 K− 1 (22.6 times higher than pure EP). Numerous articles Wang et al. [115] successfully developed siloxane (SiO) and

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Z. Ali et al. Composites Part C: Open Access 13 (2024) 100434

MWCNTs core-shell hybrid epoxy resin (EPR) composite to attain high
thermal conductivity. In the preparation process, initially, MWCNTs
were treated with several surfactants and reagents, Cetyl­
trimethylammonium bromide (CTAB) to achieve surface polarity and
later reacted with tetraethoxysilane (TEOS) via hydrolysis condensation
reaction and other saline coupling agents; 3-methacryloxypropyl tri­
methoxy silane (MPS), 3-glycidoxypropyltrimethoxysilane (GPTMS) to
produce core-shell hybrids. Finally, these core-shell hybrid fillers are
impregnated with epoxy resin to produce SiO/MWCNT/EPR composite.
The characterization results showed precise dispersion through the
structure, and it was observed that with 1 wt.% content loading
SiO/MWCNT/EPR achieved 0.55 Wm− 1 K− 1 thermal conductivity.
Figure shows different graphs related to thermal variations. Fig. 10(A)
shows that the thermal conductivity of each composite is enhanced with
increasing filler content. Fig. 10(B) represents the thermal conductivity
enhancements (TCE%) for all prepared composites, and core-shell hy­
brids with saline coupling agents showed enhanced thermal conduc­
tivity as compared to MWCNT/EPR composite. Fig. 10(C) shows the
surface temperature variations for SiO/MWCNT-MPS/EPR and
MWCNT/EPR composites in the 20–80 ◦ C temperature range, captured
via infrared camera. Fig. 10(D) represents a brief comparison of thermal
conductivity enhancement with increasing filler volume (%) between
virgin MWCNT/EPR (red) and SiO/MWCNT-MPS/EPR (black) com­
posites. The improved thermal conductivity is due to connected surface
and inter-links between core-shell hybrid fillers.
In another article, Xiao et al. [116] introduced poly (vinylidene
fluoride) (PVDF)/GNP and PVDF/CNT composites to produce further
ternary PVDF/CNT/GNP and PVDF/GNP/CNT composites. The process
was carried out using a solvent method using N, N-dimethylformamide
(DMF) as a solvent, and the solution was passed through sonication and
stirring for 2 h at 55 ◦ C for homogeneity. Finally, the specimens were hot
compressed and molded for investigation. The investigation results
revealed that the addition of CNT and GNP greatly enhanced the
nucleation effects in the crystallinity of the PVDF matrix. However, it
was observed that the addition of CNT into the PVDF/GNP composite
exhibited excellent 3D conductive pathways rather than the addition of
GNP into PVDF/CNT composite. Thus, due to the higher synergistic ef­
fect, the thermal conductivity of PVDF/CNT/GNP composite was highly
enhanced. Fig. 11(a) shows the improvement in thermal conductivity
with increasing filler loading. The thermal conductivity of all
PVDF/CNT/GNP-x specimens is higher than PVDF/GNP-x with the same
GNP loading. At 20 wt.%, the PVDF/GNP-20 composite presented only
1.64 W m− 1 K− 1 thermal conductivity, while PVDF/CNT/GNP-20
showed 1.92 W m− 1 K− 1. Fig. 11(c) shows the thermal conductivity
enhancement for PVDF/CNT-x and PVDF/GNP/CNT-x specimens with
increasing filler loading. The graph shows that at CNTs loading 20 wt.%,
the thermal conductivity of PVDF/CNT-20 was 0.56 W m− 1 K− 1 and
PVDF/GNP/CNT-20 achieved 0.69 W m− 1 K− 1. Fig. 11(b) and (d)
represent the thermal enhancement factor (%) related to filler aspect
ratios.
Besides the increased thermal performance, inspecting the long-term
stability and aging effects of CNT hybrid composites cannot be over­
looked. To address this issue, the precise control over CNT loading,
particular selection, and processing parameters plays a decisive role in
the assembly of a characteristic composite material. After fabrication,
the composite behavior over time and performances were analyzed by
various characterization techniques such as thermogravimetric analysis
(TGA), differential scanning calorimetry (DSC), dynamic mechanical
analysis (DMA), and infrared spectroscopy (FTIR). Herein, TGA reveals
the shifts in decomposition temperature and weight loss and shows the
composite aging process. Meanwhile, mechanical properties, e.g., ten­
sile strength, flexural properties, and impact resistance, can affect the
composite’s ability to conduct heat effectively. Moreover, the study in­
volves ecological influences, like UV radiation, moisture, and chemical
exposure, which can stimulate degradation in CNT-polymer composites.

Fig. 10. (A) Thermal conductivities and (B) thermal conductivity enhancements of different MWCT/EPR composites as the functions of filler contents. (Black:
MWCT/EPR, red: MPS/MWCT/EPR, blue: GPTMS/MWCT/EPR, olive: SiO/MWCT-MPS/EPR, pink: SiO/MWCT-GPTMS/EPR) (C) The surface temperatures of
MWCT/EPR and SiO/MWCT-MPS/EPR composites vary over time under the heating state. (D) EMA model fitting results of experimental data for MWCT/EPR (red)
and SiO/MWCT-MPS/EPR (black) composites at different filler loadings. Adopted with permission from Ref. [115].

10
Z. Ali et al.
Fig. 11. (a and c) Variations of thermal conductivity versus the content of fillers in the PVDF composites, and (b and d) the comparison of the thermal enhancement
factor between binary and ternary composites as indicated in the graphs. Adopted with permission from Ref. [116].
8. Electrical properties of CNT hybrid filler polymer composites
CNTs are ideal electrical conductors with high current carrying ca­
pacity due to high bonding strength between carbon atoms in the
nanostructure. High electrical conductivity 106–107 Sm− 1 [117], lower
density, and other excellent properties make it a perfect reinforcing
material for polymer composites.
Saleh et al. [118] developed CNT and carbon black (CB)/polystyrene
(PS) nanocomposites via melt mixing technique. During preparation
CNT/PS, CB/PS and CNT: CB/PS composites were produced and inves­
tigated for electrical conductivity enhancement. It was observed that
CNT: CB/PS composite with CNT: CB (75:25) showed excellent electrical
conductivity as compared to other composites due to synergistic effects
through the well-organized structure.
Yu et al. [119] reported expanded graphite (EG)-CNT/EP hybrid
composites with enhanced electrical conductivity. In the preparation
process, the EG was loaded with a metal catalyst, and hybrid EG/CNT
filler was produced by direct CNT growth onto EG via modified com­
bustion and thermal chemical vapor deposition (CVD) technique. Then,
EG/CNT filler was impregnated with EP resin, and the prepared com­
posite was hot pressed (80 ◦ C) and molded for 2 h. The characterization
results revealed that EG-CNT/EP achieved remarkable electrical con­
ductivity compared to separate EG and CNT or simply mixed EG-CNT
fillers. There are many references to demonstrate the fabrication of
hybrid polymer composites with increased electrical properties using
CNTs as reinforcing material [120–122]. Here, we report a detailed
analysis of a few articles.
Zhang et al. [123] prepared and investigated the synergistic effects in
poly (ether sulfone) (PES) composites reinforced with functionalized
multiwalled carbon nanotubes (f-CNTs) and functionalized graphene
(f-G) for electrical conductivity enhancement. Composite preparation
was followed by solution casting and sonication techniques. The char­
acterization results showed that the electrical conductivity of hybrid
composite with merely 5 wt.% of f-G-f-CNTs /PES was 2.2 and 8.9 times
higher than 5 wt.% of f-G/PES and f-CNTs/PES composites.
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Composites Part C: Open Access 13 (2024) 100434
Incorporating f-G-f-CNTs in PES composites significantly enhanced
electrical conductivity compared to composites filled with individual f-G
and f-CNTs fillers, owing to the synergistic effect. Fig. 12(a) illustrates
the experimental data, showing a notable peak at a f-G:f-CNT filler ratio
of 1:3. Notably, the electrical conductivity of σf-G-f-CNTs (Wf-G/Wf-CNTs =
1:3) was 3.45 times higher than σf-G and 10.6 times higher than σf-CNTs.
Fig. 12(b) portrays the variation in electrical conductivity of f-G-f-CNTs
(Wf-G/Wf-CNTs = 1:1)/PES composites as a function of f-G-f-CNT content
while maintaining a fixed Wf-G:Wf-CNTs ratio of 1:1 in the mixed fillers.
The conductivity behavior of this composite, combining a conductor and
an insulator, can be effectively elucidated through the application of the
modified classical percolation theory.
σ = σ0 [(Φ − Φc )/(1 − Φc )]t (1)
The symbol σ represents the composite’s conductivity, while the
filler material’s conductivity is denoted by “σ0”. The volume fraction of
the mixed filler is expressed as “Ф” and “Фc” refers to the volume
percolation concentration. Moreover, the parameter “t” corresponds to
the universal critical exponent. The conductivity behavior of the f-G-f-
CNTs (Wf-G/Wf-CNTs = 1:1)/PES composites exhibited excellent agree­
ment with the predicted percolation characteristics described by Eq. (1).
The log-log plot of σ versus (Ф− Фc) in the inset figure displayed the best
linear fit, yielding Фc = 0.22 vol%, t = 3.36, and a correlation factor R =
0.972. Notably, the volume percolation concentration for these com­
posites was significantly lower than that of the f-G/PES composite.
Hu et al. [124] synthesized CNTs and graphite (Gr) hybrid
filler-based polypropylene (PP) composites via Pickering emulsion
technique with different wt.% filler loadings. During the experimenta­
tion, three different network structures PP@Gr, PP@(CNTs/Gr), and
(CNTs/PP) @Gr were fabricated and characterized to investigate elec­
trical conductivity. The investigation revealed that (2 wt.%-CNT/PP)
@Gr at 13.01 wt.% Gr presented the maximum electrical conductivity
(1.45 Sm− 1) compared to all other composites. The structural analysis
demonstrated that CNTs performed as a bridge, and a dense 3D structure
was produced, resulting in superior electrical conductivity. Fig. 13(a and
Z. Ali et al. Composites Part C: Open Access 13 (2024) 100434

Fig. 12. (a) The DC conductivity of the f-G-f-CNTs/PES composites as a function of the weight ratio of f-G and f-CNTs in the mixed fillers at a mixed filler loading of 5
wt%. (b) Log (DC conductivity) as a function of the f-G-f-CNT content for the f-G-f-CNTs (Wf-G/Wf-CNTs = 1:1)/PES composites. The inset shows a log–log plot of the
conductivity σ as a function of Ф− Фc with an exponent t = 3.36 and a critical volume content Фc = 0.22 vol.% with a correlation factor of R = 0.972. Adopted with
permission from Ref. [123].

Fig. 13. (a) TGA thermograms of PP@Gr microparticles, (a1) the residual mass of the microparticles, and (b) the conductivity of composites. Adopted with
permission from Ref. [124].

a1) represents the TGA results for thermal stability of PP composites with
different Gr content and shows PP decomposition starts at 380 ◦ C and
completely decomposes at 800 ◦ C, but Gr is not decomposed. Fig. 13(b)
compares electrical conductivity enhancement for different composites
with different CNTs loading related to increasing Gr content (wt.%).
Owing to terrific electrical properties, CNT composites find wide­
spread employment in electronics. Conversely, the attributes come with
safety challenges mainly linked with long and rigid airborne CNTs cause
skin and eye irritation, and breathing of these nanoparticles can result in
lung infections. Moreover, the toxic behavior of CNT triggers oxidative
damage in biological systems and affects the central nervous system.
Careful safety procedures involving engineering controls to monitor the
airborne CNT levels, worker training, and personal protective equip­
ment are essential to tackle these concerns. Moreover, risk management
strategies, emergency response procedures, and regular safety assess­
ments are essential to utilize the potential of CNTs in industrial appli­
cations fully.
Beyond the realization of synergistically enhanced electrical con­
ductivity, the large-scale production of CNT hybrid composites is highly
influenced by cost-effectiveness, scalability, and quality control. Pro­
duction of CNTs and integration into polymer matrices can significantly
increase the overall cost of the composite materials. Thus, finding cost-
effective methods is crucial to make these composites commercially
feasible. Furthermore, maintaining consistent quality and properties at a
large scale is a complex assignment that demands sensible control and
optimization of various factors. Composite quality and performance
depend highly on CNT dispersion variations, polymer/CNT bonding,
and homogeneity. Thus, the execution of strict quality control measures
is essential to validate the reliability of the final product.
9. Applications
In recent eras, the need for multi-processing and smart materials has
been increasing rapidly, which is a bottleneck to traditional materials.
Polymer composites are good alternatives. However, multi-functional
operations require all good properties on the same page, and some in­
dividual filler composites still have limitations. Consequently, extensive
studies were conducted, and hybrid polymer composites were found
outstanding with multiple properties fit for aerospace applications due
to synergistic 3D structures, easy Processing, low density, strength-to-
weight ratio, and inexpensive. CNT hybrid polymer composites offer
high mechanical, thermal, and electrical properties using structural
geometry, making them suitable for multi-functional operations and
engineering applications [102,125]. This article summarizes some
top-notch applications of CNT polymer composites.
9.1. Aerospace
Aerospace industries design, produce, and maintain aircraft, engines,
space vehicles, missiles, and other propulsion units at large scale and
thus require very high strength and durable materials. Due to easier
molding, substantial strength, stiffness, and reduced weight, CNT
polymer composites are preferred for aerospace applications. Much
research was conducted to explore the properties and usage of CNT/
polymer composites in aerospace industries [126–129].
Zhang et al. [130] developed ultrathin CF-reinforced CNT/EP com­
posites by ultrasonic tow-spreading technique for aerospace applica­
tions. The composites were prepared with different CNT loadings, and it
was observed that, at 0.2 wt.% CNT and 24 wt.% CF loading, the
CF/CNT/EP composite achieved high tensile strength, compressive
strength, and interlaminar shear strength with improved electrical,

12
Z. Ali et al.
thermal, and electromagnetic interference (EMI) shielding efficiency.
Bellucci et al. [131] designed Gr-CNT/EP composites and examined
the electrical resistivity at different pressure and temperature ranges. It
was demonstrated that even a small change in CNT content highly
changes the resistivity values suitable for circuits used in aerospace
applications. CNT/ polymer composites are effective in weight reduction
and thus preferably used in aircraft manufacturing. Most parts in Boe­
ings 767 and 747 are CNT and aluminum alloy composites, e.g., eleva­
tors, flaps, tips, rudders, and spoilers.
Along with other challenges, weight reduction is essential in space
vehicles, commercial and military aircraft, and considerable cost is
devoted to quick and safe travel. During flights, there is a considerable
risk of lightning strikes, and the weight of aircraft also considerably
increases due to ice accumulation on aircraft surfaces for long flights.
Alemour et al. [132] demonstrated that lightning strikes and ice accu­
mulation on aircraft during flights reduce aircraft efficiency and cause
serious accidents. Thus, high thermal conductive CNT/polymer com­
posites are used to modify aircraft surfaces to resolve the ice accumu­
lation issues and reduce weight and fuel consumption. Fig. 14(a) shows
the lightning strike in and out of the mechanism through the aircraft
structure and the significance of using composite materials in the
aircraft exterior. Fig. 14(b) shows the effect of lightning strikes on
aircraft structures without composite materials.
Parveez et al. [133] and Lu et al. [134] reported that the Boeing 787
was the first commercial aircraft with the main structure 50 % composed
of carbon-reinforced nanocomposite material. The details are high­
lighted in Fig. 15. The percentage of materials used are 50 % carbon
composite, 20 % aluminum, 15 % titanium, 10 % steel and 5 % other
materials. A 20 % weight reduction was achieved using composite ma­
terial. In comparison, the structure of Boeing 777 is composed of 50 %
aluminum and merely 12 % composite material.
CNTs possess a bright future in aerospace applications, e.g., vehicle
weight reduction, enhanced self-healing properties, energy production,
improved controls with superior tolerance facilities and improved
thermal protection. Iqbal et al. [135] reported that CNT/EP nano­
composites can play a substantial role in artificial intelligence and
telecommunication, especially for un-manned spaceships, and are
highly effective in weight reduction, aircraft wirings, ice protection, and
fuel consumption.
However, aerospace materials are exposed to various stressors,
including extreme temperatures, high altitudes, and varying pressure
conditions. Thus, long-term stability under environmental impact and
extreme conditions is a crucial aspect and subject of exploration. Hence,
studies are ongoing to evaluate competent CNT composites with high
thermal stability, erosion resistance, and resistance to radiation. Also,
environmental impact, search for sustainable and recyclable composites
and safety in extreme conditions are under consideration.
9.2. Automotive
The automotive industry’s quest for low-weight, efficient vehicles
with innovative designs and color schemes is headed to CNT/polymer
composites. It was determined that polymer composites reduce
Fig. 14. (a) The continuous conductive path of low resistance over the entire aircraft exterior. (b) Lightning strike effects. Adopted with permission from Ref. [132].
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Composites Part C: Open Access 13 (2024) 100434
approximately 50 % of the weight of automobile and fuel utilization.
Moreover, CNT/polymer composites are used in fuel consumption fields,
braking systems, exhaust systems, vehicle carcasses, and body parts
[136]. In traditional vehicles, the fuel system is mainly based on metal
parts, and it was risky to replace them with plastics due to the possibility
of electrostatic discharge. It is estimated that future vehicles will operate
via hydrogen fuel cells. A hydrogen fuel cell is a fuel system with
renewable compressed hydrogen that operates the vehicle by conversion
of chemical energy to electrical energy without emitting hazardous CO2
gas. Currently, CNT composites are utilized to improve the efficiency of
hydrogen fuel cells, and their availability is expected soon in developing
countries [137]. CNTs are flexible, anti-corrosive, more transparent and
less brittle, making it a suitable coating material for automobile surfaces
compared to traditional and expensive Indium Tin Oxide. CNT coating
shows higher resistance against rust and extreme weather conditions
and attributes higher strength and stiffness to the surface. The me­
chanical properties of materials for vehicle manufacturing are crucial in
automobile industries. For a long time, steel alloys served for vehicle
body manufacturing and other parts despite their heavier weight and
corrosivity. Then, industries preferred aluminum because of its lighter
weight and corrosion resistance to replace steel. However, the usage of
aluminum is expensive and non-economical. Thus, CNT and its com­
posite are the best alternatives to previous materials due to their flexi­
bility, remarkable mechanical properties, and low cost [138]. While
selecting the material, Young’s modulus is the standard parameter for
industries to measure the material strength and hardness, and it was
found that Young’s modulus of CNTs is far better than steel and
aluminum.
Moreover, CNT composites are considerably resistant to weathering
conditions, e.g., temperature variations, moisture, and pressure, making
them suitable for experiments. Due to flexibility and structural integrity,
CNT composites are more favorable than traditional materials for the
experimentation and molding of different structural designs for vehicles
[139]. Fig. 16 summarizes the use of CNT composites in automobiles
reported by Cambridge Nanomaterials Technology Limited [140].
CNTs possess large bending constants due to their high strength and
straight structure. However, bending is essential to manufacture vehi­
cles of the desired shape. To make it possible, the points are marked at
specific locations where bending is required, and structural faults are
introduced to obtain sharp bending. Such a facility is highly suitable for
producing geometric and intricate automobiles [141].
Although these composites hold great potential in the aerospace and
automotive industries, they struggle with scalability and affordability on
a large scale due to cost-effectiveness because recent production pro­
cedures are expensive and laborious. Thus, scaling of production
methods, e.g., improvements in solution-based processing and roll-to-
roll manufacturing, can reduce costs and ease accessibility for world­
wide applications. In comparison, affordability can be addressed
through various factors, including developing cost-effective production
processes, sourcing raw materials, and economies of scale. Moreover,
recycling and sustainability aspects must be considered to ensure long-
term cost-effectiveness. The aerospace and automotive industries are
increasingly focusing on environmental sustainability, and CNT
Z. Ali et al. Composites Part C: Open Access 13 (2024) 100434

Fig. 15. Overall distribution of composite materials used in Boeing 787 aircraft. Adopted with permission from Ref. [132].

Fig. 16. Possible applications of CNT composites in automobiles. Adopted with permission from Ref. [140].

composites can contribute to this goal by reducing weight and
improving fuel efficiency.
9.3. Electronics
Currently, the tendency towards smart electronic devices is over­
whelming in the marketplace. Thus, the world’s research and engi­
neering community always looks for innovative, attractive, and smaller
designs for multi-functional electronic devices. Moreover, this minia­
turization leads to device heating problems, which affects device effi­
ciency and lifetime. So, there is a need for multi-functional materials to
reduce the device weight, cost, and size and establish attractive designs
with thermal heat dissipation at a time [142]. CNT polymer composites
are ideal for flexible and wearable electronic applications due to the
substantial flexibility, mechanical strength, and thermal and electrical
properties of CNTs [143,144]. The fabrication of CNTs composite

Fig. 17. Schematic of a typical module for thermoelectric generators (TEGs). Adopted with permission from Ref. [146].

14
Z. Ali et al.
networks plays a significant role in thermoelectric devices due to their
excellent thermal properties. These devices utilize waste heat to elec­
tricity using the Seebeck effect [145]. Fig. 17 depicts a representative
thermoelectric (TE) device that requires both n-type and p-type TE
materials. These materials are assembled using electrodes, bonding
materials, and insulators to create thermoelectric generators (TEGs)
[146].
Wang et al. [147] developed Piezoelectric poly(vinylidene
fluoride-trifluoroethylene) P(VDF-TrFE) nanofibers and Poly­
dimethylsiloxane (PDMS)/MWCNT thin composite membrane-based
flexible nanogenerator for finger motion detector application, working
under hybrid triboelectric and piezoelectric processes. While Processing,
the electrospinning technique formed the triboelectric and piezoelectric
functional layers, and nanogenerator triboelectric performance was
improved by increasing the initial capacitance of PDMS/MWCNT com­
posite by doping of MWCNTs as a flexible frictional layer into PDMS
films. The investigations showed that under 5 N pressure in open cir­
cuits, the nanogenerator’s triboelectric and piezoelectric output peak
voltages were 25 V and 2.5 V, respectively. Moreover, under 5 MΩ
matched resistance, the triboelectric output power and power density
were 98.56 μ W and 1.98 mW/cm3, respectively, and with 30 MΩ
matched resistance, the piezoelectric output power and power density
were 9.747 μ W and 0.689 mW/cm3 respectively.
Lin et al. [148] exhibited PP/MWCNT coated PET conductive com­
posite yarns with variable loadings (0 wt%, 0.5 wt%, 1 wt%, 2 wt%, 4 wt
%, and 8 wt%) of MWCNTs using melt extrusion technique. The pre­
pared specimens were investigated for morphology, tensile properties,
and electrical conductivity. A continuously connected structure was
formed at 8 wt% MWCNTs, and electrical conductivity reached 0.8862
S/cm with the highest tensile strength, making it useful for wearable
electronics applications, e.g., battery-heated armor and others. Kar et al.
[149] proposed MWCNTs and silica-contained poly-vinylidene-fluoride
(MWCNT@SiO2/PVDF) nanocomposite films with improved piezoelec­
tric, dielectric, and ferromagnetic properties for cheap and flexible en­
ergy harvester nanogenerator. While investigating, the flexible
nanogenerator showed high output voltage (45 V), high current density
(1.2 μA/cm2), and high power density (5400 W/m3), and power effi­
ciency is so high that it can directly power 55 commercial LEDs.
Wang et al. [150] fabricated fluorinated CNTs/nano fibrillated cel­
luloses (FCNTs/NFCs) composites using vacuum-assisted filtration.
Composites were explored for thermal conductivity enhancement to
resolve heat dissipation issues in electronic circuits. The investigations
showed that with 35 wt.% FCNT loading, the ultrahigh thermal con­
ductivity of 14.1 W m− 1 K− 1 was achieved with an efficient mechanical,
flexible, and tough structure.
Kozak et al. [151] developed in situ filled interconnected poly­
urethane/CNT composites, polymer blend (polyurethane and linear poly
(methylmethacrylate))/CNT composites and polymer blend/CNT/Ni
composites with 1.5 wt.% and 3 wt.% filler loading and transformed
with Fe(3+)acetylacetonate or Cr(3+)acetylacetonate coordination
compounds to investigate the EMI shielding properties. The character­
ization showed that chromium-modified composite showed better re­
sults, i.e., shielded efficiency at 25.8–37.5 GHz, which was about 25 dB
in the isolated polymer. Several other references are reporting the mir­
acle of CNTs and polymer composites in electronics for EMI-shielding
[152–155] heat dissipation, field emission, transistors [156], touch
screens, sensors [157–159], antennas, electric motor brushes, and
conductive coatings [160–166].
9.4. Energy storage
The energy consumption rate is increasing rapidly, and unfortu­
nately, the large-scale energy production sources are not environmen­
tally friendly, causing terrible climate change. Thus, there is a need to
store green energy to reduce the high energy demand and cost savings
for the future. Due to high surface area and optimized electrical and
15
Composites Part C: Open Access 13 (2024) 100434
thermal properties, CNTs and their polymer composites are promising
materials for energy storage devices. SWCNT composites are favorable
for photovoltaic applications as it can absorb light with a wide range of
wavelengths, i.e., visible to infrared, and contain both (electrons and
holes) charge carriers [167,168]. In batteries, CNT polymer composites
are utilized as an active anode or cathode material due to higher elec­
trical conductivity while, in solar cells decrease the need of noble metals
traditionally used as catalysts to enhance fuel cells’ performance [169,
170].
Chen et al. [171] reported a CNT/PPy composite based on a flexible,
high-performing super-capacitor. In preparation, primarily CNT flexible
freestanding films were fabricated via a vacuum filtration approach, and
then CNT/PPy electrodes were synthesized through the electrodeposi­
tion process of PPy. It was observed that mechanical and electro­
chemical properties were significantly enhanced and a robust device
with higher flexibility, longer lifetime, lightweight, and higher volu­
metric capacitance (4.9 F/cm3 at 0.05 A/cm3) was achieved. The per­
formance analysis revealed that the device can light up 53 LEDs and a
digital watch. Fracowiak et al. [172] developed supercapacitor elec­
trode materials using three different electrically conducting polymers
(ECPs) namely polyaniline (PANI), polypyrrole (PPy) and poly-(3,
4-ethylenedioxythiophene) (PEDOT) with MWCNTs. The prepared
composites were analyzed, and it was demonstrated that MWCNTs
played a substantial role in polymers distribution through the compos­
ites, higher conducting and mechanical properties, improved charge
transfer properties. It was stated that 20 wt.% CNTs loading in ECPs can
provide special electrodes i.e., with appropriate configurations, the
capacitance values can reach (100–330 F g− 1) with capacitor voltage
(0.6–1.8 V).
Muralidharan et al. [173] demonstrated ion-conducting epoxy elec­
trolyte composites’ mechanical and energy storage properties reinforced
with aligned CNTs grown on stainless steel mesh. It was observed that
energy storage composites also showed high mechanical strength (> 85
MPa), elastic modulus (5 GPa) and energy density (> 3 mWh/kg).
Fig. 18(a) shows the structural concept of a supercapacitor and its
fabrication in a vehicle framework. Fig. 18(b) represents the Optical and
SEM images of CNT-steel mesh. Fig. 18(c) shows images of fiberglass and
Kevlar, two different layering materials in the composite. Fig. 18(d)
refers to epoxy-IL (ion liquid) electrolyte photographs compared to in­
dividual epoxy and IL components.
Su et al. [174] formulated polytriphenylamine (PTPAn)/MWCNTs
and PTPAn/super-p carbon composites to test and compare the effect of
CNTs as cathode material in Li-ion batteries. The in-situ polymerization
process and the mechanical mixing of super-p carbon followed the
preparation of the composite. Both composites were analyzed for per­
formance, and it was observed that PTPAn/MWCNT composite presents
higher discharge capacity, lower charge transfer resistance (Rct) and
cycle stability as compared to PTPAn/ super-p carbon composite.
Park et al. [175] proposed a sea urchin (SU) shaped CNT bimetallic
composite such that MWCNTs were grown radially onto Ni and Al and
later precisely dispersed in an active polymer layer. The specimen in­
vestigations confirmed that SU-CNTs doped solar cells showed better
performance as compared to pristine solar cell, the calculated current
density (7.5 to 9.5 mA/cm2), and power conversion efficiency (2.1 ±
0.1 % to 2.2 ± 0.2 %). Many studies have explored the role of CNTs
polymer composites in energy storage devices e.g., batteries [176–178],
solar cells [179–181], fuel cells [182,183], supercapacitors [184,185],
hydrogen storage and presented satisfactory results [186,187].
However, integrating CNT hybrid composites in solar panels and
energy storage systems can greatly improve efficiency and present sus­
tainable energy solutions for a greener future. However, cost-
effectiveness, production methods, and ecological impact must be
focused on making a significant influence. As high-quality CNTs are
expensive, integrating them into existing energy technologies can
further increase the overall cost. Thus, innovative, cost-effective
methods should be introduced by improving synthesis techniques and
Z. Ali et al.
Fig. 18. Application of CNT in supercapacitor (a) Strategic module of CNT reinforced structural supercapacitor in a vehicle framework. (b) SEM and optical pictures
of a CNT/steel mesh. (c) Images of fiberglass and Kevlar separators. (d) Representation of the epoxy-IL electrolyte (on the left) and individual components (on the
right). Adopted with permission from Ref. [173].
scaling up production. However, achieving production methods that
yield consistent and reliable CNT quality of CNTs with zero ecological
impact is also challenging. To resolve these concerns, research should
focus on recycling methods by removing harmful byproducts by
employing green chemistry principles for CNT composites and calcu­
lating their environmental affect via comprehensive life cycle studies.
9.5. Wind turbine blade
The energy demand is rapidly increasing, and efficient green energy
sources are needed extensively to fulfill the demand. The wind turbine is
among the best green energy sources with its sturdy blades rotating and
producing electricity. However, severe weather conditions highly affect
the structural behavior of blades, and structural damage reduces effi­
ciency. In current designs, CNT thermoplastic polymer composites have
replaced the traditional classical fibers to maximize the blade’s perfor­
mance with high surface area, extraordinary strength and stiffness,
weight reduction, and physicochemical, thermal, and electrical prop­
erties. Moreover, CNT composites are impressive in sensor-making and
are utilized to examine internal variations in wind turbine blades [188].
Due to their nanoscale dimensions and diameter ranging from 180 nm
(Fig. 19b and c), CNTs possess an exceptionally high aspect ratio char­
acterized by a substantial length-to-diameter ratio. These distinctive
Fig. 19. Application of CNTs in a wind turbine blade. (a,b,c,d) CNT types micro-macro scale overview and its implementation effect in wind turbine blade,
respectively. Adopted with permission from Ref. [189].
16
Composites Part C: Open Access 13 (2024) 100434
properties significantly enhance the durability of blade structures.
Fig. 19 shows the application of continuous CNT fibers in the future
structure of ultra-mega wind turbine blades [189].
Boncel et al. [190] stated that a large-scale wind turbine blade is
typically a three-blade rotor rotating on a horizontal axis with two-face
suction and pressure construction, joining faces via shear webs
combining upper and lower parts. While operating, the wind turbine
blade faces flap-wise load (due to wind pressure) and edgewise load (due
to gravity and torque), and thus flap-wise, the operation should be in
compression-compression/tension-tension mode while edgewise in
compression-tension mode. Considering the variable load effects
through the blades, CNTs reinforced polymer composites are the best
candidates for sandwich structures due to the feasibility of polymer
adhesion with the electrochemical and mechanical properties of CNTs.
Fig. 20 shows different wind turbine blade components and
load-carrying sections.
Elhenawy et al. [191] proposed f-CNT/Ep composites via resin
impregnation technique to design a small vertical axis wind turbine
blade. The investigation results were performed by finite element
analysis (FEA) and the prepared composites were also investigated for
mechanical properties. Results showed that CNT/Ep composites signif­
icantly improved deflection and mechanical properties. Moreover, the
implementation and effectiveness of prepared CNT/Ep composites in the
Z. Ali et al.
Fig. 20. Wind turbine blade simplified cross-section with an indication of working loads with their directionalities (left); major elements of a wind turbine blade,
based on linking of two aeroshells and shear webs (grey color indicates the primary load-carrying composites) (right). Adopted with permission from Ref. [190].
movement of wind turbine blades under variable loads were analyzed by
ANSYS code package, confirming that introducing CNTs into Ep com­
posites highly influences the efficiency of the wind turbine blade.
The ice formation on wind turbine blades causes imbalances, reduces
lifetime, and results in 20 % energy loss annually. Due to substantial
thermal properties, CNT composites greatly reduce the problem. Zheng
et al. [192] established CNT-reinforced waterborne polyurethane (WPU)
composite films via roll-roll gap coating and hot-press method for highly
flexible, durable, lightweight in situ deicing system. It was disclosed that
electrothermal composite film heaters can endure 100,000 times 240◦
bending at 3.17 % resistance fluctuation, and in length direction, the
repeated 2.0 % stretching without any influence on their temperature
dispersal with impact strain of 10 %. Many references reported CNT
composites’ impact in advancing wind turbine blades [193–196].
10. Conclusion and outlook
The addition of CNTs in polymers with multiple fillers has opened a
new corridor for structural applications. Based on existing studies, the
better dispersion of CNTs with other fillers in polymer matrices produces
hybrid polymer composites with highly connected synergistically
enhanced 3D structures, significantly increasing the mechanical, ther­
mal, and electrical properties. However, the dispersion of CNTs is
challenging as they tend to agglomerate and have poor dispersion while
processing, which deteriorates the overall performance of the composite
material. This study reported different preparation methods of CNTs
hybrid polymer composites from previous research to resolve CNTs
agglomeration issues and its effects on mechanical, thermal, and elec­
trical properties and uses in heavy industries (aerospace, automotive,
electronics, and other engineering fields). Although many references
presented CNTs hybrid polymer composites with excellent properties,
some limitations exist to get optimum results. Certain vital factors
significantly contribute to fabricating highly organized stress-induced
synergistic structures, e.g., aspect ratios, filler size, homogeneous dis­
tribution, and surface modification. It is challenging to balance these
parameters to get ultimate properties. Thus, forthcoming investigations
can provide a better insight to scale up these crucial factors and obtain
optimized results.
Funding
The authors gratefully acknowledge the financial support from the
University of Campania Luigi Vanvitelli. The University of Campania
Luigi Vanvitelli participates in the transformative national contract
managed by CARE-CRUI for access to the electronic journals of the
publisher Elsevier.
17
Composites Part C: Open Access 13 (2024) 100434
CRediT authorship contribution statement
Zulfiqar Ali: Data curation, Writing – original draft. Saba Yaqoob:
Investigation, Writing – original draft. Jinhong Yu: Conceptualization,
Writing – original draft. Alberto D’Amore: Supervision, Writing – re­
view & editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
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