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Multilayer polymeric nanocomposites for

electromagnetic interference shielding:
Cite this: New J. Chem., 2021,
45, 21488 fabrication, mechanisms, and prospects
Milad Kamkar, † Ahmadreza Ghaffarkhah,† Ehsan Hosseini, Majed Amini,
Saeed Ghaderi and Mohammad Arjmand *

Received 27th September 2021,
Accepted 2nd November 2021
DOI: 10.1039/d1nj04626h
rsc.li/njc
The ever-increasing proliferation of wireless communication systems and modern electronics arouses
concerns regarding electromagnetic pollution. Such concerns become even more vital considering the
rapid development of compact and flexible electronics. These concerns call for the integration of
lightweight EM shielding materials with enhanced thermal and mechanical characteristics in advanced
electronics. In this regard, multilayer polymer nanocomposites have been developed as a novel class of
functional electromagnetic interference (EMI) shielding materials. Up to now, this new class of EMI
shields has showcased several key features, including enhanced flexibility, thermal properties, and EMI
shielding effectiveness (EMI SE) that can meet the current demands of the industry. More interestingly, the
multilayer strategy is capable of transcending the EMI shielding mechanism from reflection to absorption. This
feature article provides a comparative and balanced discussion of recent advances in multilayer EMI shields.
The EMI shielding mechanisms, choice of materials, and the rationale behind the improved mechanical and
thermal properties of the multilayer shields are also highlighted. The outlook provided in this review points
out the promising properties and remarkable tunability of the multilayer shields that introduce them as
versatile substitutes for traditional metallic or even single-layer polymeric shields. This review paper promises
that the future of multilayer EMI shields is boundless, and soon, this novel class of EMI shields will be utilized
in various electronic devices and radiation source fields on a large scale.

Nanomaterials and Polymer Nanocomposites Laboratory, School of Engineering, University of British Columbia, Kelowna, BC, V1V 1V7, Canada.
E-mail: mohammad.arjmand@ubc.ca
† These authors contributed equally to this work.

Milad Kamkar received his PhD Ahmadreza Ghaffarkhah is a PhD

in chemical engineering from the student in the School of Engi-
University of Calgary (2020) and neering at the University of
was a guest researcher at British Columbia, Okanagan
Stanford University (2019). His Campus. His research interest
work is focused on structure includes synthesis of carbon-
property relationship of poly- based nanomaterials, polymer
meric nanocomposites. After his processing and forming, and
PhD, he worked on 3D printing intrinsically conductive polymers.
and liquid-in-liquid printing of
MXene- and graphene-based
hydrogels/inks at the University
Milad Kamkar of British Columbia (UBC) for Ahmadreza Ghaffarkhah
fabrication complex EMI shields.
Currently, he is a postdoctoral researcher at UBC Bioproducts
Institute, working on 3D printing of biomaterials (e.g., CNC,
CNF, chitin, etc.).

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1. Introduction
Humans in modern society have rapidly adopted digital techno-
logies for a multitude of purposes, including education, enter-
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tainment, and communications. Almost all these technologies,
ranging from mobile telecommunications networks to compact
electronics, create undesirable electromagnetic interference
(EMI).1–3 EMI is known to adversely affect the performance of
miniaturized electronics, communication systems, and modern
warfare.4–6 Besides, prolonged exposure to electromagnetic
waves causes severe human health problems such as nausea,
chronic headaches, cancer, and even abnormal brain develop-
ment of infants.3,7–10 These detrimental impacts of electro-
magnetic noise are even more noticeable considering the advent
Ehsan Hosseini holds a PhD in
Chemical Engineering from the
University of Calgary in Canada
and has worked as a post-
doctoral research associate in
Okanagan Microelectronics &
Gigahertz Applications (OMEGA)
lab and Nanomaterials and
Polymer Nanocomposites Labora-
tory (NPNL) at the University of
British Columbia-Okanagan. His
main areas of interest are mostly
Ehsan Hosseini focused on the charge transport
mechanisms in conductive
polymers and fabrication of innovative materials using
conductive polymers alone or in composite forms with nanofillers
to develop highly transparent thin films for printable organic
electronics applications, including de-icing, electromagnetic
interference shielding, and sensors.
Saeed Ghaderi is a PhD student
at the University of British
Columbia (UBC), Okanagan
Campus. He received his MSc
degree in Chemical Engineering-
Polymer Engineering from Sharif
University of Technology (SUT),
Tehran, Iran. He has been
working on developing rheo-
logical modifier copolymers and
corrosion protective inhibitors
and organic coatings. His inter-
Saeed Ghaderi ests are polymers and nano-
structures synthesis, characterization,
and processing. At the UBC, he is focusing on developing
intrinsically conductive polymers and nanocomposites for
organic electronic applications and wearable devices using 3D
printing techniques.
This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
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of the 5G era, the ever-increasing usage of compact and miniatur-
ized electronics, and the mass production of defense and medical
devices operating at high frequencies and long periods of
radiation.11,12 Therefore, the development of effective EMI shields
to mitigate the undesirable effects of EM noise is indispensable.
The mentioned detrimental impacts have propelled the growth of
the current market of EMI shielding materials. The global EMI
shielding market size is projected to grow from USD 6.8 billion in
2020 to USD 9.2 billion by 2025.13
Traditionally, metals such as Ag, Cu, Al, and stainless steel
are known as excellent barriers against electromagnetic waves
due to their exceptional electrical conductivity.3,4 However,
their limitations, including high density, difficult processability,
and susceptibility to corrosion, have limited their application in
Majed Amini is a PhD student in
the School of Engineering at the
University of British Columbia,
Okanagan Campus. His research
interest includes synthesis of
carbon-based nanomaterials for
fabrication of innovative 3D-
printed polymer nanocomposites
for EMI shielding applications.
Majed Amini
Mohammad Arjmand is an
assistant professor in the School
of Engineering at the University of
British Columbia, Okanagan
Campus. He is also the Canada
Research Chair in Advanced
Materials and Polymer Engi-
neering. Dr Arjmand directs the
Nanomaterials and Polymer
Nanocomposites Laboratory
(NPNL), which focuses on the
synthesis and development of
Mohammad Arjmand multifunctional nanomaterials
and polymer nanocomposites.
Research Website: https://npnl.
ok.ubc.ca/.
New J. Chem., 2021, 45, 21488–21507 | 21489

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wearable, portable, and miniaturized electronics.14,15 Thus, an
increasing number of studies have focused on lightweight and
easy-to-process shielding materials that can meet the current
demands of the electronics market. Until now, various EMI
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shields based on carbonaceous nanomaterials (e.g., carbon nano-
tubes (CNTs), graphene, reduced graphene oxide, and amorphous
carbon),16–19 intrinsically conductive polymers (e.g., poly(3,4-
ethylene dioxythiophene:polystyrene sulfonate) (PEDOT:PSS),
polypyrrole, and polyaniline),20–22 MXene (a large class of 2D
carbides, nitrides, and carbonitrides),23–25 and their nanocom-
posites have been developed to replace the metallic shields.
Furthermore, a variety of processing and coating technolo-
gies such as spin-coating,1,26 dip-coating27, spray coating,15,25
interfacial assembly28, blade coating,29,30 casting,31,32 and
inkjet printing33 have been exercised to fabricate various EMI
shields for a range of applications. As a result of this extensive
research attention, the literature has witnessed major break-
throughs in the field of EMI shielding, presenting practical
alternatives for conventional metal-based shields. Among these
innovative shielding solutions, we can refer to flexible, scalable,
and highly conductive micrometer-thick EMI shields that
can be used for flexible, wearable, and smart electronics.29
The ultra-light EMI shields based on conductive foams with
a density of as low as 0.1 g cm3,34, 35 the nanometer-thick
shields with exceptional transparency,1,14 and the conductive
polymer nanocomposites shields that can be prepared by
common polymer processing methods18,36,37 are among other
groundbreaking innovations in this realm.
Despite the aforementioned progresses, there are still sev-
eral core issues to be addressed and challenges to be overcome
in the field of EMI shielding. The first important challenge to
be addressed is fabrication of multifunctional EMI shields.
Industry demands EMI shields that not only mitigate the
negative effects of the electromagnetic waves but also feature
outstanding mechanical and thermal characteristics.38–40
Second, there is an urgent need for the development of EMI
shields that absorb a large portion of incoming electromagnetic
waves. To date, most studies have only focused on the fabrication
of highly conductive shields that primarily rely on the reflection
of electromagnetic waves.41,42 However, this approach is often
impractical for military and medical applications that require a
great degree of EMI absorption with minimal reflection.41–43
Indeed, the electromagnetic waves reflected from a conductive
shield may act as a secondary source of EMI and affect the
performance of nearby devices.44,45
Recently, the fabrication of multilayer EMI shields has been
introduced as a viable solution to address the above-mentioned
challenges. For example, a multilayer structure of appropriate
nanomaterials and polymers was employed to fabricate multi-
functional EMI shields with outstanding EMI shielding charac-
teristics and exceptional thermal properties.39 Besides, in
many studies, it was shown that a multilayer structure of
conductive and magnetic materials could enhance the absorp-
tion portion of the shielding and even, to a great extent,
the total EMI shielding effectiveness (EMI SE) of designed
structures.46–48 Despite these encouraging advances, there is
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no review article exclusively on multilayer EMI shields, their
EMI shielding mechanisms, and prospects. Furthermore, even
the most recent reviews on general perspective and choice of
materials have missed the concept of multilayer shields (refer to
Table 1). Herein, we aim to present a comparative and balanced
discussion on various perspectives of multilayer EMI shields.
In the following sections, we will provide the general concepts
of EMI shielding along with the underlying shielding mechanisms
of multilayer shields (Section 2) and, then, a comprehensive
review of the most exciting studies on the multilayer shields
(Section 3). Finally, we will cover the current challenges and
prospective trends of multilayer EMI shields in Section 4.
2. Mechanisms
The effectiveness of a shield is assessed based on the extent
of attenuation of electromagnetic (EM) waves incident on a
material. The mechanisms of shielding can be described
through the interaction of EM waves with a material. An EM
wave features both the electric (E) and magnetic (H) fields that
are perpendicular to each other and these fields are transverse
to the direction of wave propagation. When an EM wave reaches
the front interface of a material with air, part of the incident
electric field (Eo) and magnetic field (Ho) will be reflected (SER),
as a primary mechanism of EMI shielding (Fig. 1). Reflection is
a consequence of the interaction of EMI radiation with the free
electrons on the surface of the shield. This interaction causes
the charges to become excited and redistribute across the
shield, thereby creating an opposing electromagnetic field.
The electromagnetic field generated by the redistribution of
charges cancels out the external field. When the remaining part
of the EM wave penetrates through the material, it would be
absorbed and dissipated in the form of thermal energy (SEA),
undergone multiple internal reflections (SEM), and transmitted
through the shielding material (Et and Ht).
The overall (total) EMI shielding effectiveness (SET) of a
shield can be defined as the logarithmic ratios of the incident
EM wave power (Po), electric field (Eo), and magnetic field (Ho)
to the transmitted EM wave power (Pt), electric field (Et), and
magnetic field (Ht) (eqn (1)), respectively. It can also be
expressed in terms of the sum of the reflection, absorption,
and multiple internal reflections loss:
 
P0
SET ¼ SEA þ SER þ SEM ¼ 10 log
Pt
    (1)
E0 H0
¼ 20 log ¼ 20 log
Et Ht
The reflection loss intensity (SER) of a conductive monolithic
shield, such as metals, is a function of the electrical conductiv-
ity and magnetic permeability of the material in conjunction
with the frequency of the incident wave source:
   
sr 1
SER ¼ 168 þ 10 log ¼ 10 log (2)
mr f 1R
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Table 1 Summary of studies on recently published review papers on EMI shielding

Discussion on
Author(s) Main topic multilayer shields Ref.
1 Guo et al. (2021) Application of electrospun fiber-based materials for EMI shielding No 49
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2 Song et al. (2021) EMI shielding of MXene/polymer nanocomposites Briefly 50

3 Wang et al. (2021) Conductive polymer nanocomposites with multiple interfaces for EMI Briefly 51
shielding applications
4 Bhattacharjee Application of core–shell nanomaterials for microwave absorption and No 52
and Bose (2021) EMI shielding
5 Yao et al. (2021) Application and performance of polymer-based lightweight materials Briefly 53
for EMI shielding
6 Chen et al. (2021) Recent advances in graphene-based films for EMI shielding Briefly 12
7 Wang et al. (2021) Shielding mechanisms and structural design of EMI shielding Briefly 54
composites
8 Maruthi et al. (2021) Conducting polymer-based composites as efficient EMI shielding Briefly 55
materials
9 Liu et al. (2021) Lightweight carbon–polymer nanocomposites for EMI shielding No 56
10 Hema et al. (2021) Ferrite-based polymer nanocomposites as shielding materials No 57
11 Zhang et al. (2021) Advances in waterborne polymer/carbon material composites for EMI Briefly 8
shielding
12 Kumar (2021) Recent progress on carbon-based composite materials for microwave Briefly 4
EMI shielding
13 Wu et al. (2021) EMI shielding properties of carbon-based materials and No 58
nanocomposites
14 Wanasinghe et al. (2020) EMI shielding performance of polymeric nanocomposites No 59
15 Ahsan Nazir (2020) Application of polyvinylidene fluoride (PVDF), polyurethane (PU), and No 60
polyaniline (PANI) composites-based materials for EMI shielding
16 Sushmita et al. (2020) Polymer nanocomposites containing semiconductors as advanced No 61
materials for EMI shielding
17 Liu et al. (2020) Development of polymer-based EMI shielding materials Briefly 62
18 Panahi-Sarmad et al. (2020) Carbon-based polymer nanocomposite foams as EMI shields Briefly 63
19 Jiang et al. (2020) EMI shielding of polymers and nanocomposites Briefly 2
20 Abbasi et al. (2019) Recent advances in the EMI shielding of carbon-based polymer No 64
nanocomposites
21 Geetha et al. (2009) EMI shielding: methods and materials No 65
22 Thomassin et al. (2013) Design and characterization of polymer/carbon-based composites as Briefly 66
EMI shielding materials

where sr is the electrical conductivity of the shield relative to
that of copper (5.8  107) in S m1, mr is the magnetic
permeability of the shield relative to that of the free space
(4p  107) in H m1, f is the frequency of the source in Hz, and
R is the reflectance in percent. As implied from eqn (2), the
reflection loss is directly associated with the conductivity of the
material. Consequently, a material with high conductivity can
demonstrate greater overall shielding effectiveness (SET), owing
to its higher reflection loss. Similar to the reflection loss, the
absorption loss (SEA) of a monolithic material has a correlation
with the electrical conductivity and magnetic permeability of
the material, and the frequency of the incident wave source.
The absorption loss is defined as:
rffiffiffiffiffiffiffiffiffiffiffiffi  
sr omr t 1R
SEA ¼ 8:68t ¼ 8:68 ¼ 10 log (3)
2 d T
where t is the thickness of the shield in m, o is the angular
frequency in rad s1, d is the skin depth of the shield in m, and
T is the transmittance in percent. The skin depth d is the
distance through which the electric (E) and magnetic (H) field
intensities of the EM wave decrease to 1/e (37%) of the incident
value (Fig. 2) and can be calculated as:11
1 is insignificant when the absorption loss of the shield is more
d ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffi
pf mr sr
Eqn (2) and (3) both confirm the direct dependency of the
reflection and absorption loss on the conductivity of the
material; however, the enhancement of the conductivity will
be more manifested on the absorption loss rather than the
reflection loss. The reason rests beneath the square root
pffiffiffi
correlation of the absorption loss with conductivity ðSEA / sÞ
as opposed to the logarithmic relationship with the reflection loss
(SER p log s). According to eqn (3), the thickness of a shield (t)
plays a significant role in increasing the absorption loss and the
overall shielding effectiveness. This correlation has been the
cornerstone of the numerous latest studies to design multilayer
EMI shields that can provide more efficient shielding properties
but with lighter weights and smaller thicknesses. The challenge
remains in the direct impact of the material thickness on the
absorption characteristic of the shield. Although lightweight,
low cost, and thin EMI shields have recently attracted atten-
tion for many emerging applications in printable electronics,
reducing the thickness of the material impedes the absorption
loss considerably.
The multiple internal reflections, which consist of the sum
of the internal reflections of EM waves inside a material,
contribute to more transmission of EM waves and, thus, are
not desired. However, the effect of multiple internal reflections
(4)
than 10 dB, or the shield thickness is larger than its skin

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Fig. 1 The primary mechanisms of the interaction between an incident
EM wave and a shielding material.
Fig. 2 Schematic representation of the skin depth inside a shield.
depth.13 Above absorption loss values of 10 dB or for thick
films, the multiple internal reflections of EM waves are
absorbed inside the material. The multiple internal reflections
can be evaluated using the following equation:
 
2t
SEM ¼ 20 log 1  e d : (5)
Materials with multilayer structures involve all the EMI
shielding attenuation mechanisms in each layer (Fig. 3); never-
theless, the effectiveness of each layer is dependent on the
frequency of the incident EM source, the distance of the shield
from the source, the thickness (addition of more layers), and
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Fig. 3 Mechanisms of multilayer shields: materials with multilayer structures
encompass all the EMI shielding attenuation mechanisms in each layer.
the material of the shield. The electrical conductivity of the
forefront material layer can reflect a portion of the incident EM
waves. The remaining waves that pass the first layer and
penetrate towards the underneath layers will be repeatedly
attenuated via the mechanisms of reflection, absorption, and
multiple reflections both within each layer and between the
layers.
Recent studies are driven to fulfill the challenge of develop-
ing materials with high conductivity and small thickness in
order to generate layers with high reflection and/or absorption
loss features. In this regard, materials with both electric and
magnetic properties have been considered for multilayer struc-
tures to further add on the magnetic loss component to the
overall EMI shielding effectiveness, utilizing the absorption of
the magnetic part of the incident EM waves.
The ordering of layers and the choice of the materials, in a
multilayer structure, depend on the application of the shield,
which determines whether the reflection or absorption loss is
required to be the leading mechanism. In the military, for
instance, highly reflective objects can be traced, and thus
require absorbing shields to stay hidden. To determine the
dominance between the two major shielding mechanisms, it is
important to note that the reflection loss (SER) is correlated
with s/m based on eqn (2). However, as eqn (3) shows, the
absorption loss (SEA) is proportional to the product of the
conductivity and permeability (sm). Although both reflection
and absorption losses increase upon the enhancement of the
conductivity of the layers, any changes in the permeability have
an inverse effect on the reflection loss, whereas they are in
direct correlation with absorption loss. This indicates that
using materials with magnetic properties favors absorption
loss as the governing mechanism in the overall shielding.
In this regard, materials with no or low magnetic properties
should possess a high conductivity to compensate for their lack
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of permeability in order to govern the shielding effectiveness
via the reflection loss mechanism. In a multilayer structure
shield with different layers, both permittivity and permeability
can be defined as complex quantities:
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hybrids). In each subsection, we will discuss the multilayer
shields’ performance along with the role of non-conductive
layers in their structures.

3.1 Carbon nanotube-based multilayer shields

e = e 0 + ie00
m = m 0 + jm00
where e 0 (m 0 ) denotes the real part and e00 (m00 ) is the imaginary
part of the permittivity (permeability). e 0 (m 0 ) represents the
electric (magnetic) energy storage, whereas e00 (m00 ) relates to
ohmic (magnetic) losses similar to an electrical system. e 0 is
also known as dielectric constant and e00 as dielectric loss or
loss factor.
The mechanisms accounting for enhanced EMI shielding
performance of the multilayer shields will be further explained
in a more detailed manner in the next sections by giving
practical examples. We will also expound on the rationales
behind the improved mechanical and thermal characteristics
of the multilayer shields.
3. Multilayer EMI shields
The fabrication of multilayer EMI shields has drawn significant
attention over the last few years. This novel strategy is routinely
adopted for enhancing the mechanical and thermal properties
of the shields and/or transcending the EMI shielding mecha-
nism from reflection to absorption. The multilayer shields
consist of at least one conductive layer that ensures the
acceptable shielding effectiveness of the structures and a few
non-conductive layers containing magnetic, flame retardant, or
other types of functional fillers, depending on the final targeted
properties. Indeed, the inherent properties of the conductive
nanomaterials play a decisive role in defining the total EMI
shielding of the nanocomposites. Table 2 summarizes the
properties of the widely used conductive materials for EMI
shielding application. Herein, the studies on multilayer EMI
shields are categorized based on the type of nanofillers utilized
in their conductive layers (e.g., CNTs, graphene, MXene, or their
(6)
In this section, we review the multilayer shields with carbon
(7) nanotube (CNT)-incorporated layers as the primary conductive
layer. Since the discovery of CNT in 1991, it has been widely
used for various applications such as fabrication of conductive
polymer nanocomposites. Indeed, CNT stands out among
different nanofillers due to its unique geometrical features
(e.g., high aspect ratio), remarkable mechanical properties
(e.g., tensile strength of 100–600 GPa, and Young’s modulus
of 1–5 TPa), and extraordinary electrical conductivity. The
resistance of the metallic CNTs is zero, and due to the ballistic
transport, their electrical conductivity is several times greater
than copper.80 Thus, in a major portion of the existing works
on multilayer shields, at least one CNT-based layer has been
utilized. However, it should be borne in mind that the men-
tioned properties of the CNT significantly depend on the
structural and chemical features of the nanotubes, including
structural perfection, aspect ratio, doping, and so forth.81,82
In the case of conductive polymer nanocomposites, the final
properties also rely on the dispersion, distribution, and align-
ment of the CNTs in the polymeric matrix.37,83,84 Thus, the
inherent properties of the nanotubes conjugated with their
dispersion quality in polymeric matrices must be tuned to
achieve the highest electrical potential of the fabricated conduc-
tive nanocomposites.83
In order to address the emerging multifunctional needs (e.g.,
high EMI shielding with appreciable mechanical properties),
Zhang et al.85 fabricated hybrid systems integrating CNTs with
cellulose. The authors proposed a layered structure consisting of a
polymer/CNT layer as the EMI shield with a regenerated cellulose
layer as the supporting substrate. Poly(ethylene oxide) (PEO) was
used as the polymeric matrix in this study due to the favorable
interactions of PEO chains with cellulose chains, providing inter-
facial adhesion between the CNTs and cellulose layers. The
thickness of the PEO/CNTs layer was estimated to be in the range

Table 2 Widely used conductive materials for EMI shielding applications

Nanostructure Synthesis method Electrical conductivity (S cm1) Ref.

Graphene film Graphitization of graphene oxide (GO) 1000 67
Graphene paper Oxidative acid treatment and sonication of graphite 197 68
Graphene nanoplatelet Sonication and annealing 2200 69
Graphene foams Hydrazine-foaming and annealing GO 3.1 70
Graphene paper Chemical vapor deposition (CVD) 1136 71
Graphene sheets Hydrogen arc discharge exfoliation of GO 2000 72
Nitrogen doped-CNT Chemical vapor deposition 0.0001 17
SWNT bucky papers Dispersion and filtration 6200 73
CNT Chemical vapor deposition 22.9 74
MWCNT Direct amination of MWCNTs 860 75
Carbon nano fiber Nitrogen-doped CNF 15.4 76
Ti3C2Tx MXene Evaporated-nitrogen minimally intensive layer delamination (EN-MILD) 24 000 77
Ti3C2Tx MXene Minimally intensive layer delamination 5800 77
Ti3C2Tx MXene LiF/HCl etching 15 100 78
Ti3C2Tx MXene LiF/HCl etching 10 400 78
Ti3C2Tx MXene HCl/HF/LiCl etching and delamination 8000 79

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of 80–100 mm, and that of the cellulose layer was found to be
30–40 mm. The design of the CNT-based multilayer shields with
cellulose layers has proved to be very efficient in the simultaneous
enhancement of EMI SE and mechanical properties. The EMI SE
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waves. The waves that exit the conductive layer are further
attenuated progressively by multiple reflections and absorptions
between the conductive layers, leading to dissipation in the form
of heat within the material by prolonging the propagation path of

and Young’s modulus increased from 20 dB and 1274 MPa for
plain-structured nanocomposite (i.e., a mixture of the fillers in a
single-layered structure) to 35 dB and 2615.4 MPa, respectively, for
a 2-layer structure. The authors postulated that the higher EMI SE
of the layered structure is related to the formation of a more
extensively connected CNT network at a constant CNT loading in
the layered structure. They were able to further improve the EMI
SE of the layered structure to 65 dB by increasing the number of
layers to 6. It was mentioned that the outstanding EMI perfor-
mance of the layered structure is because of the conspicuous high
conductivity of the PEO/CNTs layer, which trapped most of the
the re-reflected wave. It was claimed that interfacial polarization
also contributes to this phenomenon.86,87 However, the literature
has shown that interfacial polarization relaxes significantly over
the X-band;16,37,88 as such, we believe that the contribution of the
interfacial polarization mechanism is negligible.
In another study,89 Fe3O4 was added to a cellulose-based
substrate to further enhance the EMI shielding performance by
absorption mechanism. To this aim, Li et al.89 prepared flexible
and tough nano-fibrillated cellulose (NFC)/Fe3O4&CNT/poly-
ethylene oxide (NFC/Fe3O4&CNT/PEO) films with alternating
multilayer structure (see Fig. 4a) via a facile vacuum-assisted

Fig. 4 (a) Schematic diagram for the preparation process of alternating multilayer films. (b) EMI SE of fabricated alternating multilayer films in figure (a).
(c) Schematic diagram for electromagnetic microwave dissipation across the alternating multilayered film. (d) Schematic representation of different
stacked films arranged in a specific order and the EMI SE of their multilayer structures. (e) Schematic of multilayer structure consisting of CNTs and FRs.
(f) PLM photographs of multilayer structure shown in figure (e). (g) A comparison of the combustion behavior of the 2-, 8- and 32-layer specimens.
(a), (b) and (c) Reprinted from ref. 89, Copyright (2021), with permission from Elsevier. (d) Reprinted from ref. 48, Copyright (2021), with permission from
Elsevier. (e), (f), and (g) Reprinted from ref. 90, Copyright (2021), with permission from Elsevier.

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filtration (VAF) method. In this method, separate NFC/Fe3O4
(15 ml) and CNT/PEO (15 ml) suspensions were alternatingly
filtered in a vacuum via a cellulose acetate filter membrane.
Similar to the previous study,85 the CNT layer in this structure
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acted as the main EMI shield and NFC/Fe3O4 played the role of
the supporting substrate. In terms of mechanical properties,
the alternating structure improved the toughness and ductility
of the nanocomposite films. The thicknesses of the CNT/PEO
and NFC/Fe3O4 layers were found to be in the range of 24.0–
28.8 and 11.1–14.3 mm, respectively. Fig. 4b shows the EMI SE
of the samples with different number of conductive CNT/PEO
layers from 1 to 4 (NFC/Fe3O4 was designed as the top
and bottom layers to protect the inner CNT/PEO layers).
As expected, the samples’ EMI SE increased by adding more
layers, which was attributed to the ‘‘zigzag’’ reflection mechanism
induced by the alternating multilayer structures (see Fig. 4c). The
authors also compared the results of the multilayer structure with
the plain structure. Although the thickness of both structures was
approximately the same, to eliminate the effect of thickness
the authors reported specific SE defined as SE/d, where d is the
thickness of the sample. It was observed that SE/d of the
alternating multilayer films was relatively higher than that of
the plain-structure films, revealing the superiority of the multi-
layer structure to the plain (single-layer) structure. In addition to
the mentioned mechanisms in the previous work,85 the existence
of the magnetic Fe3O4 nanoparticles in the NFC layer led to a
more pronounced EMI SE by absorption of the magnetic part of
the EMI waves.
Nallabothula et al.47 and Arief et al.48 also utilized magnetic
nanoparticle-incorporated layers for fabrication of multiwall
CNT (MWCNT)-based multilayer shields in an attempt to
increase the EMI SE by adsorption mechanisms. In the former
study, the authors used Fe3O4, while in the latter, the authors
used CoNi (cobalt–nickel) as the magnetic nanoparticles.
Nallabothula et al.47 achieved an EMI SE of 23 dB for a 4layer
structure of 3 wt% MWCNT (150 mm) – 1 wt% Fe3O4 + 1 wt%
MWCNT (300 mm) – 1.5 wt% MWCNT (150 mm) – 5 wt% Fe3O4 +
3 wt% MWCNT (300 mm). Arief et al.48 constructed a layer-wise
assembly with a total thickness of 0.9 mm by sandwiching a
reflector spacer (i.e., polyvinylidene fluoride (PVDF)/MWCNT
nanocomposites) between absorber layers (PVDF/CoNi (flower,
sphere, and rod)/MWCNT nanocomposites). Fig. 4d schemati-
cally shows the design of their multilayer shields along with
their EMI SE. They were able to achieve an EMI SE of 41 dB for a
7-layer structure. It was postulated that EM waves penetrate the
nanocomposite because of the top and bottom magnetic layers.
These waves are attenuated by coherent multiple reflections at
the internal interfaces of conductive and magnetic layers.91
It can be said that interlayer scattering (for high absorption)
and impedance matching between the inner and outer layers
are the main reasons researchers utilized highly conductive and
magnetic layers to fabricate multilayer EMI shields.
Bhattacharjee et al.46 used a combination of magnetic nano-
particles (Mn (manganese)–ferrite and Ni) to block the EMI
waves at small thicknesses. Following a precise layer-by-layer
(LbL) architectural assembly, they were able to achieve an
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excellent EMI SE of B50 dB at a thickness of 0.6 mm for a
3-layer architecture. The incoming EM radiation is absorbed
through a pseudo-network of Mn–ferrite and MWNTs in the
outer layer (PVDF/MWNT/Mn–Fe) and, then, the transmitted
waves are reflected back by the inner layer (Ni-deposited woven
carbon fiber (CF) mat). Hence, the outer layers also scavenged
the reflected waves from the highly conductive inner layer.
In this study, the authors46 used magnetic and conductive
components in all the layers to take advantage of electric and
magnetic dipole interactions in all layers. The rationale behind
the utilization of magnetic particles in the multilayer shield is
explained more in the next paragraph.
It is well known that EM radiation is the harmonized
perpendicular proliferation of electric and magnetic vector
components. Thus, the magnetic materials (Mn–Fe and Ni)
directly interact with the magnetic vector component, which
leads to magnetic hysteresis loss. That is, a considerable
portion of the waves would be dissipated by the re-orientation
of the magnetic domains of Mn–Fe and nickel nanoparticles
in all layers, which is in line with eqn (3) in Section 2. This
confirms that higher magnetic permeability leads to greater
EM wave absorption. The remainder of EM wave would be
transmitted, reflected, or absorbed by the conductive compo-
nents (CF and MWCNT). Moreover, Ni was deposited onto the
conductive mat via an electroless method, it was claimed that
the reflected waves from CF would be absorbed by interfacial
polarization, contributing toward the absorption mechanism.
However, we (the authors of this work) believe that the inter-
facial polarization plays an insignificant role in the absorption
of the microwaves due to relaxations.
Hence, based on the abovementioned discussions, magnetic
particles can absorb the EM waves. However, their efficiency in
absorption depends on their magnetic properties. Table 3
summarizes the properties of the different magnetic particles
along with their synthesis procedure, which can be used as a
roadmap to design EMI shield absorbers. In general, a higher
magnetization leads to higher EM absorption.
Recently, proper heat transfer management was found to
be of utmost importance in advanced EMI shields in compact
electronics. In this regard, heat accumulation in compact
electronics has become an increasingly serious problem. He
et al.90 and Ji et al.101 showcased that multilayer structuring
of EMI shields is an effective approach in simultaneously
improving the EMI shielding efficiency and enhancing the
flame safety of the electronic components. In both studies,
commercial flame retardants (FRs) and CNTs were used to
construct a synergistic flame-retarding shields. The conductive
layer consists of only CNTs, and the flame retarding layer
contains both CNTs and FRs (see Fig. 4e and f). It was observed
that both 8- and 16-layer specimens exhibit EMI SE of greater
than 30 dB. The acceptable EMI SE of the multilayer structures
was a direct result of the impedance mismatch (conductivity
difference) between the conductive polymer–CNT layers and
flame retardant polymer–FR–CNT layers. Electrical impedance
is the general concept of electrical resistance, and it is the
ratio of the electric and magnetic fields’ amplitudes (|E|/|H|).
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Table 3 Different magnetic particles along with their properties and synthesis methods

Saturation magnetization Coercivity Calcination

Magnetic particle (emu g1) (Oe) Synthesis method temperature (1C) Ref.
Fe3O4 74.9 B0 Solvothermal 180 92
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Fe3O4/AC 30 B0 Solution-precipitation — 93
Fe3O4/AC@SiO2 20 B0 Solution-precipitation —
Fe3O4/AC@SiO2@Sulfanilamide 14 B0 Solution-precipitation —
Ni nanowires 54.88 207.7 Solution-precipitation — 94
Ni@Co-MOF 22.81 234.5 —
Ni@Co/C 68.85 257.6 500
Ni@Co/C@PPy 11.64 165.0 —
ZnFe2O4 168.0 — Hydrothermal-precipitation 120 95
ZnFe2O4@SiO2 nanochains 35.04 B100 Solvothermal 500
NiCo2O4 0.19 67.5 Hydrothermal 120 96
0.54 — Hydrothermal 160
1.85 119.7 Hydrothermal 200
NiFe2O4 B50 B20 Sol–gel — 97
Ni@Co3O4 14.10 180.7 Dropping method — 98
ZnFe2O4 75.5 B0 Hydrothermal 700 99
ZnFe2O4@carbon 61.1
ZnFe2O4@carbon@MoS2/FeS2 8.8
Zn0.5Ni0.5Fe2O4 54.2 0.020 Precipitation 400 100
66.4 0.020 700
84.2 0.014 1000

When an electromagnetic wave strikes a conductive material
having a different intrinsic impedance than the domain in
which the EM plane wave propagates, two waves will be created
at the external surface: a reflected wave and a transmitted wave.
Generally, impedance mismatch occurs when the input impe-
dance of the input power (EM supply) is not equal to the source
impedance of jointing (our sample), and thus the reflection
will occur.
The authors also showed that the flammability greatly depends
on the number of layers. In this regard, the flame retardancy
increased by increasing the number of layers, and superior
flame retardancy with prompt self-extinguishment and anti-
dripping was achieved for the 8-layer structure (see Fig. 4g).
This was attributed to the production of continuous and
foaming carbonaceous structures among the layers during
burning. According to the intumescent flame-retarding mecha-
nism, the FRs in the nanocomposite layer undergo thermal
decomposition and dehydration during combustion. This
phenomenon conjugated with the formation of intumescent
carbonaceous char result in reducing heat and fuel delivery
between the heat source and the polymer matrix, limiting the
diffusion of oxygen as well as carbon-based gases into the
matrix and, thus, inhibiting the spread of fire.102,103 That is,
although the neat polymers used in these studies are classified
as inflammable materials, the multilayer structure of the EMI
shields made them flame retardant. Interestingly, a further
increase in the number of layers (i.e., more than 8 layers)
deteriorated the flame retardancy, meaning that there is an
optimum number of layers to achieve the best thermal proper-
ties. As can be seen in Fig. 4g, by increasing the number of
layers from 8 to 32, the flame retardancy decreased. This was
attributed to the limitation of the intumescent capacity of
chars, as the number of layers increases by more than 8. Hence,
the flame retardant layer is not cable of protecting the adjacent
inflammable layers when the number of layers is more than 8.
The results of this section verify that the final properties of
CNT-based incorporated multilayer shields have excellent
potential to tailor a combination of properties for electrical
applications. It was shown that the multilayer fabrication
strategy not only leads to a significant enhancement in EMI SE
but also, based on the type of filler used in the secondary layer,
mechanical and thermal properties can be drastically improved.
Layer gradient structuring (using similar conductive filler in
different layers but at different concentrations) is another
promising approach in enhancing the EMI SE of multilayer
structures with a dominant absorption mechanism,104 which
will be discussed in detail in the next section.
3.2 Graphene-based multilayer shields
Another important member of the conductive carbonaceous
nanomaterials family is graphene, including graphene oxide
(GO), reduced graphene oxide (rGO), expanded graphite, graphene
nanoplatelets, and graphene nanosheets. Graphene was first
produced by mechanical exfoliation (scotch taping) into single
layers in 2004. Among the mentioned materials, GO has the least
electrical conductivity as a direct consequence of basal and edge
functional groups, acting as a barrier to conductive pathways. The
differences between the other forms of graphene are related to the
degree of exfoliation and size of the nanoparticles/particles.105
For instance, in expanded graphite, exfoliation of graphite is not
throughout the entire plane between the adjacent carbon layers.
When the number of layers reduces to 3–10 by layer exfoliation
throughout the entire plane, then this piece is referred to as
graphene nanoplatelets.106 In other words, stacked graphene
nanosheets are the building unit of graphite nanoplatelets and
expanded graphite.
Expanded graphite and GO are more available and much
easier to prepare/synthesize compared to the graphene nano-
sheets. However, due to graphene nanosheets’ exceptional
mechanical and electrical properties, a higher content of

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expanded graphite and GO, compared to graphene nanosheets,
is required to achieve a certain property. Because of this trade-
off, all these materials have been used for the fabrication of
multilayer shields. Moreover, similar to CNT-based nanocom-
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In another study, Liang et al.111 designed a heterogenous
alternating multilayer structure (HAMS) containing highly-
aligned graphene nanosheets and Ni nanochain in a PVDF
matrix for EMI shielding and heat dissipation applications.

posites, not only do the physical and chemical structures of the
graphene-based materials play a major role in defining the
final properties but also their dispersion quality dictates their
efficiency in a property of interest.107,108
A GO-based multilayer shield was proposed by Zhang
et al.109 for simultaneously resolving the undesirable electro-
magnetic wave and heat emissions caused by an electronic
device. Boron nitride was utilized in this study in order to
improve the thermal conductivity of the shield. Although GO
can dissipate the heat to some extent, boron nitride was
added to further resolve the dissipating heat of the electronic
components. This is because the thermal and electrical
conduction mechanisms are different. In this regard, the
electrons, photons, and phonons are the heat carriers, while
the charge carriers are solely electrons and holes.110 Zhang
et al. reported an EMI SE of 38 dB and high thermal conductiv-
ity of 12.62 W m1 K1 by fabricating a multilayer shield
comprising graphene oxide/polymer and boron nitride/polymer
via a solution casting method. The authors also compared the
EMI SE of the multilayer shields by varying the number of
layers at a constant thickness of 233 mm. They observed that the
EMI SE increases from 30 dB for a 3-layer shield to 37 dB for
an 11-layer shield.
Effective electron and phonon conductive paths were formed in
the layers as a direct result of the highly aligned structure,
leading to an appreciable electrical and thermal conductivity.
The excellent electrical conductivity of the highly aligned
structure combined with multilevel EM multi-reflection and
magnetic loss of Ni chains resulted in an EMI SE of 43.3 dB for
an 8-layer shield with a thickness of 0.5 mm, found to be 98.6%
better than the homogenous film.
Im et al.112 prepared both monolayer and 3-layer graphene
nanoplatelet (GNP)/Ni/polymethyl methacrylate (PMMA) nano-
composites for EMI shielding applications. The monolayer and
multilayer nanocomposites were designed based on the same
average amount of GNP/Ni (30 wt%) at a thickness of 2.5 mm
(see Fig. 5a). The average amount of GNP/Ni in both structures
was kept constant (i.e., 30 wt%), while the loading of the filler
increased from 20 to 40 wt% from the top layer to the bottom
layer in the 3-layer shield (see Fig. 5b). Accordingly, the first
layer of the multilayer shield contains less amount filler (i.e.,
10 wt%) compared to the monolayer (30 wt%) shield, leading
to a lower impedance mismatch between the material’s surface
and air.
Minimizing the impedance mismatch between the materi-
al’s surface and the air maximizes the fraction of the incident

Fig. 5 Schematic of the (a) monolayered GNP/Ni/PMMA nanocomposite with 30 wt% GNP/Ni and (b) multilayer GNP/Ni/PMMA nanocomposite (20 wt%
GNP/Ni/30 wt% GNP/Ni/40 wt% GNP/Ni). Monolayer and multilayer nanocomposites have the same average amount of GNP/Ni (30 wt%) and total
specimen thickness (2.5 mm). (c) SER, (d) SEA, and (e) SET results of the monolayered and multilayer GNP/Ni/PMMA nanocomposites in figures (a) through
(e) Reprinted from ref. 112 copyright Royal Society of Chemistry.

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wave that enters the shields. Hence, gradient multilayer strategy
can enhance the total EMI SE by absorption mechanism. In this
regard, due to the penetrating capability of the first layer, most
portion of the waves enters the shields. As the waves enter deeper
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through the material, they will be more attenuated by both higher
reflection and absorption capability of the 2nd and 3rd layers.
Moreover, an abrupt concentration increase between the contact-
ing layers induces an additional internal reflection between layers
(see Fig. 5b). According to the fact that the thickness of each layer
is larger than the skin depth, the reflected waves between layers
turn into heat, adding to the SEA. That is, as can be seen in Fig. 5c
through Fig. 5e, although the SER of both shields is close to each
other, SEA of the multilayer structure is about 3 times greater than
that of the monolayer structure, resulting in an excellent EMI SE
of 61 dB. Thus, the gradient multilayer strategy can be deemed as
a promising technique to considerably increase the EMI SE at
a constant filler loading and a fixed thickness of the shield.
Li et al.113 used the same gradient concentration technique to
enhance the microwave-absorbing (MA) property of a multilayer
thermoplastic polyurethane/graphene (PUG) nanocomposite.
The results of this section prove that other than incorpora-
tion of various nanoparticles (e.g., conductive and magnetic
nanoparticles) in different layers of a multilayer shield, con-
structing a concentration gradient with the aid of the multilayer
strategy can significantly contribute to efficient EMI shielding
with dominant absorption mechanism. Hence, if the goal is
just to improve the EMI SE at a minimum cost, it is suggested
to follow the concentration gradient approach instead of incor-
porating a secondary nanoparticle.
3.3 MXene-based multilayer shields
MXenes are a unique family of two-dimensional (2D) transition
metal carbides and/or nitrides. The general formula of MXenes
is Mn+1XnTx, where M is an early transition metal (e.g., Ti, Zr, V,
Nb, Ta, or Mo), X is carbon and/or nitrogen, and Tx stands for
the surface terminations (OH, O, or F). This variety of composi-
tions and combinations has led to the formation of a large
number of 2D MXene materials, i.e., more than 30 types of
MXene so far.114 Due to this variety and unique features, since
the discovery of the first MXene in 2011,115 they have been
expanding rapidly by finding applications in different fields
(e.g., energy storage and conversion, environment and catalysis,
separation membranes, medicine, optics, and electronics).114
MXenes have also been widely used to fabricate high-performance
polymeric EMI shields, thanks to the unique electrical conduc-
tivity and mechanical properties of the transition metal carbides/
nitrides.116 In 2016, Shahzad et al.23 reported EMI SE of several
MXenes in a polymeric matrix, among which a 9 mm thick film of
Ti3C2Tx/polymer showed an excellent shielding of B55 dB. The
outstanding performance of Ti3C2Tx in shielding the EMI waves
was correlated to high electrical conductivity (4600 S cm1) and
multiple internal reflections from Ti3C2Tx flakes. Since then,
MXenes have been incorporated into different polymeric matrices
for the fabrication of EMI shields.
Since 2019, several authors have prepared multilayer EMI
shields with MXene/polymer as the primary layer. Jin et al.39
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fabricated alternating polyvinyl alcohol (PVA)/Ti3C2Tx films
synchronously with high EMI SE and thermal conductivity.
As MXenes form a stable suspension in water, most of the
MXene-based polymeric nanocomposites are based on water-
soluble PVA. The multilayer films were fabricated via the layer-
by-layer casting of an aqueous solution of PVA and an aqueous
suspension of MXene. The casting procedure was repeated 11
times to achieve a multilayer film with 5 layers of pure MXene
and 6 layers of pure PVA. The content of the MXene in the
multilayer shields was manipulated by the concentration of the
Ti3C2Tx in the casted suspension. The amount of MXene in
the final structure was found to be in the range of 7.5–19.5 wt%.
In these films, the continuous compact Ti3C2Tx network in the
pure MXene layers conducts heat and electron and the PVA
layers endow flexibility to the multilayer shield. The best EMI
SE achieved in this study was 44.4 dB with a SEA of 36.1 dB for a
27 mm-thick PVA/MXene multilayer film. The authors claimed
that the re-reflection of the waves between the MXene layers
dissipates the waves in the form of heat, resulting in a signi-
ficant enhancement in the absorption. Therefore, multiple
reflections at the interface of PVA and MXene layers triggered
the excellent EMI shielding performance of this multilayer
shield.
In other studies published in the last 3 years, clay nanoplatelets
(montmorillonite (MTM)),117 cellulose nanofiber (CNF),118
boron nitride (BN),119 and silver nanowires (AgNWs)120 were
used as the secondary filler for the fabrication of MXene-based
multilayer shields. In the first-mentioned study,117 PVA/MTM/
MXene (Ti3C2) multilayer films were fabricated by dipping a
pretreated glass slide into PVA/MXene aqueous suspension,
followed by dipping into MTM/MXene suspension after drying.
This process was repeated until the desired number of bilayers
were formed. The authors named this technique as ‘‘dip-LbL
technique’’. The thickness and density of the bilayer film
were found to be 272 nm and 2.16 g cm3, respectively. After
deposition of the desired number of the bilayers, an acid (hydro-
fluoric acid) treatment was used for delamination of the films
from the glass substrate to achieve free-standing films.
These films exhibited excellent mechanical properties and a
60-bilayer film withstood the weight of a 450 g book (see
Fig. 6a). The mechanical properties of the films were deeply
explored by uniaxial tensile testing. The excellent mechanical
properties of the films were attributed to the existence of MTM
in the systems. In this regard, interactions of MXenes and MTM
with the polymer matrix allow for the stress transfer from
the polymer to the high-strength nanomaterials. This stress
transfer along with the interactions between the platelets
themselves, in a manner similar to nacre, positioned these
multilayer films among prominent strong LbL films. Fig. 6b
shows the EMI SE of the 10–40 bilayer nanocomposites.
Expectedly, the EMI SE increased by increasing the number of
layers. However, interestingly, the EMI SE of the 40-bilayer
nanocomposite is slightly lower than the EMI SE of its
30-bilayer counterpart. This was attributed to the higher resis-
tance of the nanocomposites (i.e., higher resistance of the
shield) when the number of bilayers increases from 30 to 40
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Fig. 6 (a) Photograph of a 60-bilayer nanocomposite film supporting the weight of a 450 g book. The sample was attached to the book using a label
tape. (b) EMI SE of 10–40 bilayer nanocomposite film. (c) The plot of bilayer number versus thickness (left y-axis) and sheet resistance (right y-axis).
(d) Schematic illustration for the fabrication of the double-layer ANF-MXene/AgNW nanocomposite papers. (e and f) EMI SE of the double-layer and
homogeneously blended nanocomposite. (g) Digital images of the double-layer nanocomposite paper possessing ultra flexibility and withstanding a
weight of 500 g. Figure (a–c) reproduced from ref. 117 with permission from the Royal Society of Chemistry. (d–g) Reprinted with permission from ref.
120, Copyright (2021) American Chemical Society.

(see Fig. 6c). Thus, increasing the number of layers is not
always favorable to EMI SE.
Recently, Ma et al.120 utilized aramid nanofibers (ANFs) and
AgNW for the fabrication of high-performance double-layer
MXene-based films with excellent EMI shielding, ultra flexibility,
and outstanding mechanical properties. ANFs, also called nano-
scale Kevlar fibers and composed of aligned poly(paraphenylene
terephthalamide) (PPTA) chains, are a novel 1D nanomaterial
derived from the deprotonation of macroscopic Kevlar fabrics
or the bottom-up nanofiber synthesis.121–123 The double-layer
structures were fabricated via a facile two-step vacuum-assisted
filtration followed by a hot-pressing approach. In this process,
initially, a constant amount of the dispersion of ANF was
vacuum filtrated until a stable ANF hydrogel was formed on
the surface of a porous nylon membrane. Then, the aqueous
suspension of the mixture of the Ti3C2Tx/AgNW was vacuum
filtrated on top of the ANF hydrogel. Afterward, the whole
system was dried under hot-pressing conditions (Fig. 6d sche-
matically shows the entire process). The weight ratio of the
Ti3C2Tx and AgNW was fixed at 10 : 1 and the content of the

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MXene in the suspensions changes from 5 to 80 wt%. For
comparison, the authors also prepared a series of homoge-
neously blended ANF/MXene/AgNW nanocomposites with the
same solid contents as the bilayer nanocomposites.
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charge density. That is, local dipoles are generated, which can
rotate directionally toward the electromagnetic field. This
phenomenon caused polarization loss and thus improved the
overall EMI shielding performance. Fig. 6g shows the flexibility

The EMI SE of the bilayer and blended structures is shown
in Fig. 6e and f. Interestingly, despite the smaller thickness of
the bilayer structure compared to the blended structure at the
same solid contents, the bilayer nanocomposites showed a
higher EMI SE. For instance, at a MXene loading of 80 wt%,
the EMI SE of the bilayer structure at a thickness of 91 mm was
80 dB while the EMI SE was 50.9 dB for a 98 mm-thick blended
nanocomposite. The rationale behind the higher EMI SE of the
bilayer structure is the synergistic effect of MXene nanosheet
and Ag nanowires in the formation of a compact network
structure with a great electrical conductivity. Thus, due to
the facile electron transfer in the conductive network of
MXene/AgNW, the EM waves are depleted and transformed
into thermal energy. In this regard, the penetrated waves into
the highly conductive MXene/AgNW layer are attenuated by
massive ohmic loss upon the interaction of the waves with
the electron carriers (such as electrons, holes, and dipoles).
Multiple internal reflections between the adjacent nanosheets
also contributed to the shielding by absorption. Other than
the mentioned mechanisms, the presence of localized defects
of post-etched MXene combined with the existence of the
functional (–O–, –F, and –OH) groups on the edges and surface
of the nanosheets led to asymmetry in the distribution of
and mechanical strength of the fabricated bilayer films. The
excellent mechanical properties of these systems originate from
the presence of the ANF layer, withstanding the applied stress
on the nanocomposites. With regard to structure, the bilayer
nanocomposites exhibited better mechanical properties com-
pared to monolayer nanocomposites. Thus, it can be concluded
that the bilayer nanocomposites performed better in terms of
both mechanical and electrical properties. This is because the
co-existence of ANF and conductive fillers in one layer would
interfere with each other’s network destructively. In other
words, MXene/Ag nanoparticles disrupt the integrity of the
ANF network structure, negatively impacting the mechanical
properties. On the other hand, ANF also disrupts the 3D
interconnected network of MXene/Ag, leading to a lower elec-
trical conductivity and, thus, lower EMI SE results for the
blended structure.
3.4 Hybrid conductive fillers
Incorporation of more than one type of conductive filler in the
same or different layers of the multilayer shields is an effective
approach to take advantage of the geometrical and electrical
features of various nanomaterials. For instance, it is known that
the inherent electrical conductivity of graphene nanosheets is

Fig. 7 (a) Effect of order of layers: average SET, SEA, and SER of the three-layer PVDF/fillers nanocomposites. (b) Effect of the number of layers: EMI SE of
the different PVDF/GNP-Ni-CNT nanocomposites with a thickness of 0.6 mm. (c) Scheme of six-layer PVDF/filler nanocomposites with a sandwich
structure. Reprinted with permission from ref. 125, Copyright (2021) American Chemical Society.

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higher than CNTs, while CNTs are more effective in the formation
of 3D interconnected networks in polymeric matrices at low
concentrations, leading to superior electrical and rheological
properties.124 The mentioned differences in the final properties
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are also adjustable in the single-layer shields, the number, and
order of the layers are the additional controllable factors in
engineering the multilayer shields. Moreover, different types
and combinations of fillers can be incorporated in each layer,

of graphene-based and CNT-based polymer nanocomposites stem
from the geometrical features of the nanomaterials and the ability
of CNTs to form mechanical entanglements, extending the range
of tube–tube interactions.124
In a recent study in 2020, a three-layer sandwich structure
of PVDF-based nanocomposites consisting of graphene nano-
platelets (GNP)-, Ni-, and CNT-based layers was devised by
Qi et al.125 for the fabrication of advanced EMI shields. The
authors investigated the effect of shield thickness, the number
of layers, and order of the layers. Based on Fig. 7a, regardless of
the order and type of the layers, the multilayer structures
showed higher SE than the blended structure (single-layer
shield containing all types of fillers). The highest SE was
observed for the sample with layers containing all three types
of the nanofillers with the following order: first layer PVDF/
GNP, second layer PVDF/Ni, and third layer (PVDF/CNT). The
high SE was attributed to the conductivity gradient of the
layers, leading to propagation of the waves through the internal
layers and internal multiple reflections. More importantly, it
was shown that SE increases as the number of layers increases
(see Fig. 7b and c). In a similar study in 2015, Lin et al.126
investigated different three-layer shields containing CNTs and
graphene nanosheets in each layer. By manipulating the type
and order of the layers at a constant thickness of 1 mm, they
were able to achieve an EMI SE of B36 dB.
4. Conclusion and outlook
To recapitulate, the multilayer structure strategy provides
higher degree of freedom in designing EMI shields, making
them more tunable. In this regard, in addition to the thickness
of the shield and type and concentration of the fillers, which
expanding the applications of the multilayer EMI shields.
By regulating the number, thickness, and type of the layers,
tunable EMI SE for multilayer films can be obtained, surpassing
that of their monolayer counterparts. Moreover, in many research
studies, it has been shown that this approach intensifies the
absorption portion of the shielding, mainly attributed to the
multiple reflections and heterogeneous dielectric polarizabilities
between the layers, leading to the accumulation of virtual charges
at the interface.
More importantly, the demand for multifunctional EMI
shields has increased dramatically in the last few years,
owing to the fast technological developments in the electro-
nics industry. For advanced applications, for instance, it is
expected for a shield to be mechanically strong and flexible
with desired thermal properties (e.g., high heat dissipation
and flame retardancy). It has been shown that the multilayer
assembly of EMI shields is an effective approach for improving
the EMI shielding by absorption mechanism while enhan-
cing the other mentioned properties of the shield. Both
mechanical and thermal properties of the multilayer shields
have been found to be superior to those of their monolayer
counterparts, fulfilling the stringent requirements in practical
applications.
In this review, first, we discussed the EMI shielding mechan-
isms of multilayer polymeric shields. Then, the current devel-
opment status of multilayer EMI shields was presented, and the
research progress of EMI shielding composites with different
structures was detailedly illustrated. We also expounded on the
rationales behind the improved mechanical and thermal pro-
perties of the multilayer shields. Table 4 provides a summary of
the recent literature on multilayer EMI shields and their
enhanced properties. Based on this table, not only appreciable
EMI SE values have been reported for multilayered shields, but

Table 4 Summary of multilayer EMI shields

Nanofiller EMI SE (dB) Number of layers Remarks Ref.

CNT/regenerated cellulose 60 6 Improved total EMI SE and mechanical properties 85
CNT/nanofibrillated cellulose/Fe3O4 34 7 Improved total EMI SE and mechanical properties 89
CNT/FRs 32 32 Improved total EMI SE and flame retardancy 101
Graphene nanoplatelet/Ni/CNT 46 6 Improved total EMI SE and tensile elongation 125
CNT/graphene 36.85 3 Improved total EMI SE 126
CNT-flame retardant 32 16 Improved total EMI SE and flame retardancy 90
CNT/(cobalt–nickel) 41 7 Improved total EMI SE 48
CNT- Fe3O4 26 6 Improved total EMI SE 47
CNT/Mn-Fe/carbon fiber-Ni 50 3 Improved total EMI SE 46
Graphene/Ni nanochain 51 8 Improved total EMI SE and heat dissipation 111
Graphene 27 5 Improved total EMI SE 127
Graphene oxide/boron nitride 38 11 Improved total EMI SE and thermal conductivity 109
Graphene nanoplatelet/Ni 58–85 3 Improved total EMI SE 112
MXene 44 11 Improved total EMI SE, flam retardancy, and thermal conductivity 39
MXene/Ag nanowire 80 2 Improved total EMI SE, mechanical and thermal properties 120
Mxene/clay nanoplatelets 27 80 Improved total EMI SE and mechanical properties 117
MXene/PDMS/BN 33 11 Improved total EMI SE and heat dissipation 119
Fe3O4@rGO/MWCNT 36 4 Improved total EMI SE and mechanical properties 128

This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021 New J. Chem., 2021, 45, 21488–21507 | 21501

NJC
also these shields benefit from tunable mechanical and thermal
properties.
So far, to achieve a high EMI shielding efficiency, at least one
highly conductive layer, including carbonaceous or transition
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metal carbide nanofillers, has been incorporated into the
structure of the multilayer shields. The other layer/layers
included a wide range of nanoparticles with desired mechanical,
thermal, and magnetic properties. It was shown that reasonable
macroscale structural (number, thickness, and order of the layers)
design plays a vital role in dictating the final properties of the
multilayer shields, promoting the full replacement of single-layer
polymeric and metallic EMI shielding materials.
However, the number of publications in this field is very
limited and there is still plenty to be explored in this area. For
instance, recently, it has been shown that nanometer-thick
transparent filler-free conjugated polymers can provide an
EMI SE as high as 16 dB.1 However, the minimum required
EMI SE for most industrial applications is 20 dB, translated to
the shielding of 99% of the incident waves. We believe that via
utilization of layer-by-layer strategy by advanced processing
techniques (e.g., spin coating, extrusion 3D printing, and inkjet
printing), fabrication of transparent nanometer-thick shields
with improved EMI SE is feasible. Nevertheless, it should
be borne in mind that careful engineering of the interfaces
(e.g., proper interaction between different layers) and that
complex fabrication eprocess are indivisible challenges of such
multiphase systems.
As a final note, it has to be pointed out that the recent efforts
in the fabrication of multilayer EMI shield opens a creative
avenue for designing and constructing flexible and tough
nanocomposite films simultaneously featuring excellent EMI
shielding performance, fascinating heat removal ability, and
robust mechanical properties. Further advancement in the
generation of the multilayer shields enables the combination
of several multifunctional characteristics with the possibility of
a tailor-made control of the EMI shielding and final properties,
which would open new possibilities in a vast array of fields.
Conflicts of interest
There are no conflicts to declare.
References
1 E. Hosseini, M. Arjmand, U. Sundararaj and K. Karan,
Filler-free conducting polymers as a new class of trans-
parent electromagnetic interference shields., ACS Appl.
Mater. Interfaces, 2020, 28596–28606.
2 D. Jiang, V. Murugadoss, Y. Wang, J. Lin, T. Ding, Z. Wang
and N. Lu, Electromagnetic interference shielding poly-
mers and nanocomposites – A review, Polym. Rev., 2019,
59(2), 280–337.
3 A. Iqbal, P. Sambyal and C. M. Koo, 2D MXenes for
electromagnetic shielding: A review., Adv. Funct. Mater.,
2020, 30(47), 2000883.
21502 | New J. Chem., 2021, 45, 21488–21507 This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
Perspective
4 R. Kumar, S. Sahoo, E. Joanni, R. K. Singh, W. K. Tan, K. K.
Kar and A. Matsuda, Recent progress on carbon-based
composite materials for microwave electromagnetic inter-
ference shielding, Carbon, 2021, 177, 304–331.
5 R. Chen, R. Yu, X. Pei, W. Wang, D. Li, Z. Xu and H. Deng,
Interface design of carbon filler/polymer composites for
electromagnetic interference shielding, New J. Chem., 2021,
30(47), 2000883.
6 L. P. Mathew, N. Kalarikkal, S. Thomas and T. Volova,
An effective EMI shielding material based on poly(tri-
methylene terephthalate) blend nanocomposites with
multiwalled carbon nanotubes, New J. Chem., 2018, 42(16),
13915–13926.
7 G. Redlarski, B. Lewczuk, A. Żak, A. Koncicki, M. Krawczuk,
J. Piechocki and D. Ambroziak, The influence of electro-
magnetic pollution on living organisms: Historical trends
and forecasting changes, BioMed Res. Int., 2015, 1–18.
8 W. Zhang, L. Wei, Z. Ma, Q. Fan and J. Ma, Advances
in waterborne polymer/carbon material composites for
electromagnetic interference shielding, Carbon, 2021, 177,
412–426.
9 A. Christ, M. Douglas, J. Nadakuduti and N. Kuster, Asses-
sing human exposure to electromagnetic fields from wire-
less power transmission systems, Proc. IEEE, 2013, 101(6),
1482–1493.
10 R. Stam and S. Yamaguchi-Sekino, Occupational exposure
to electromagnetic fields from medical sources, Ind. Health,
2017.
11 E. Drakakis, E. Kymakis, G. Tzagkarakis, D. Louloudakis,
M. Katharakis, G. Kenanakis and E. Koudoumas, A study of
the electromagnetic shielding mechanisms in the GHz
frequency range of graphene based composite layers, Appl.
Surf. Sci., 2017, 398, 15–18.
12 Y. Chen, J. Li, T. Li, L. Zhang and F. Meng, Recent advances
in graphene-based films for electromagnetic interference
shielding: Review and future prospects, Carbon, 2021, 180,
163–184.
13 https://www.globenewswire.com/news-release/2020/03/02/
1993356/0/en/9-2-Billion-EMI-Shielding-Market-by-Material-
Method-Industry-and-Region-Global-Forecast-to-2025.html.
14 G.-M. Weng, J. Li, M. Alhabeb, C. Karpovich, H. Wang,
J. Lipton and M. Elimelech, Layer-by-layer assembly of
cross-functional semi-transparent MXene–carbon nano-
tubes composite films for next-generation electromagnetic
interference shielding, Adv. Funct. Mater., 2018, 28(44),
1803360.
15 M. Han, C. E. Shuck, R. Rakhmanov, D. Parchment,
B. Anasori, C. M. Koo and Y. Gogotsi, Beyond Ti3C2Tx:
MXenes for electromagnetic interference shielding, ACS
Nano, 2020, 14(4), 5008–5016.
16 M. Arjmand, M. Mahmoodi, G. A. Gelves, S. Park and
U. Sundararaj, Electrical and electromagnetic interference
shielding properties of flow-induced oriented carbon nano-
tubes in polycarbonate, Carbon, 2011, 49(11), 3430–3440.
17 M. Arjmand, K. Chizari, B. Krause, P. Pötschke and
U. Sundararaj, Effect of synthesis catalyst on structure of

Perspective
nitrogen-doped carbon nanotubes and electrical conduc-
tivity and electromagnetic interference shielding of their
polymeric nanocomposites, Carbon, 2016, 98, 358–372.
18 F. Sharif, M. Arjmand, A. A. Moud, U. Sundararaj and
Published on 02 November 2021. Downloaded by University of Science and Technology of China on 5/4/2024 5:35:17 PM.
E. P. L. Roberts, Segregated hybrid poly(methyl methacry-
late)/graphene/magnetite nanocomposites for electro-
magnetic interference shielding., ACS Appl. Mater. Inter-
faces, 2017, 9(16), 14171–14179.
19 K. Chizari, M. Arjmand, Z. Liu, U. Sundararaj and
D. Therriault, Three-dimensional printing of highly conduc-
tive polymer nanocomposites for EMI shielding applications,
Mater. Today Commun., 2017, 11, 112–118.
20 C. K. Madhusudhan, K. Mahendra, B. S. Madhukar, T. E.
Somesh and M. Faisal, Incorporation of graphite into iron
decorated polypyrrole for dielectric and EMI shielding
applications, Synth. Met., 2020, 267, 116450.
21 F. Qin, Z. Yan, J. Fan, J. Cai, X. Zhu and X. Zhang, Highly
uniform and stable transparent electromagnetic interfer-
ence shielding film based on silver nanowire–PEDOT: PSS
composite for high power microwave shielding, Macromol.
Mater. Eng., 2021, 306(2), 2000607.
22 H. Lai, W. Li, L. Xu, X. Wang, H. Jiao, Z. Fan and Y. Yuan,
Scalable fabrication of highly crosslinked conductive nano-
fibrous films and their applications in energy storage
and electromagnetic interference shielding, Chem. Eng. J.,
2020, 400, 125322.
23 F. Shahzad, M. Alhabeb, C. B. Hatter, B. Anasori, S. M.
Hong, C. M. Koo and Y. Gogotsi, Electromagnetic inter-
ference shielding with 2D transition metal carbides
(MXenes), Science, 2016, 353(6304), 1137–1140.
24 J. Lipton, J. A. Röhr, V. Dang, A. Goad, K. Maleski, F. Lavini
and J. Kong, Scalable, highly conductive, and micro-
patternable MXene films for enhanced electromagnetic
interference shielding, Matter, 2020, 3(2), 546–557.
25 W. Chen, L.-X. Liu, H.-B. Zhang and Z.-Z. Yu, Flexible,
transparent and conductive Ti3C2Tx MXene-silver nanowire
films with smart acoustic sensitivity for high-performance
electromagnetic interference shielding., ACS Nano, 2020,
16643–16653.
26 B. Zhou, M. Su, D. Yang, G. Han, Y. Feng, B. Wang and
C. Shen, Flexible MXene/silver nanowire-based transparent
conductive film with electromagnetic interference shielding
and electro-photo-thermal performance, ACS Appl. Mater.
Interfaces, 2020, 12(36), 40859–40869.
27 Y. Wang, H.-K. Peng, T.-T. Li, B.-C. Shiu, H.-T. Ren,
X. Zhang and J.-H. Lin, MXene-coated conductive compo-
site film with ultrathin, flexible, self-cleaning for high-
performance electromagnetic interference shielding, Chem.
Eng. J., 2021, 128681.
28 T. Yun, H. Kim, A. Iqbal, Y. S. Cho, G. S. Lee, M.-K. Kim and
S. O. Kim, Electromagnetic shielding of monolayer MXene
assemblies, Adv. Mater., 2020, 32(9), 1906769.
29 J. Zhang, N. Kong, S. Uzun, A. Levitt, S. Seyedin, P. A. Lynch
and J. Liu, Scalable manufacturing of free-standing, strong
Ti3C2Tx MXene films with outstanding conductivity,
Adv. Mater., 2020, 2001093.
This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
NJC
30 Y. Xu, Y. Yang, D.-X. Yan, H. Duan, G. Zhao and Y. Liu,
Flexible and conductive polyurethane composites for
electromagnetic shielding and printable circuit, Chem.
Eng. J., 2019, 360, 1427–1436.
31 C. Song, X. Meng, H. Chen, Z. Liu, Q. Zhan, Y. Sun and
Y. Dai, Flexible, graphene-based films with three-
dimensional conductive network via simple drop-casting
toward electromagnetic interference shielding, Compos.
Commun., 2021, 24, 100632.
32 B. Y. Wen, X. J. Wang and Y. Zhang, Ultrathin and
anisotropic polyvinyl butyral/Ni-graphite/short-cut carbon
fibre film with high electromagnetic shielding perfor-
mance, Compos. Sci. Technol., 2019, 169, 127–134.
33 M. Vural, A. Pena-Francesch, J. Bars-Pomes, H. Jung,
H. Gudapati, C. B. Hatter and Y. Gogotsi, Inkjet printing
of self-assembled 2D titanium carbide and protein electro-
des for stimuli-responsive electromagnetic shielding, Adv.
Funct. Mater., 2018, 28(32), 1801972.
34 J. Liu, H.-B. Zhang, R. Sun, Y. Liu, Z. Liu, A. Zhou and
Z.-Z. Yu, Hydrophobic, flexible, and lightweight MXene
foams for high-performance electromagnetic-interference
shielding., Adv. Mater., 2017, 29(38), 1702367.
35 M. Han, X. Yin, K. Hantanasirisakul, X. Li, A. Iqbal,
C. B. Hatter and Y. Soda, Anisotropic MXene aerogels with
a mechanically tunable ratio of electromagnetic wave reflec-
tion to absorption, Adv. Opt. Mater., 2019, 7(10), 1900267.
36 S. M. N. Sultana, S. P. Pawar, M. Kamkar and U. Sundararaj,
Tailoring MWCNT dispersion, blend morphology and EMI
shielding properties by sequential mixing strategy in
immiscible PS/PVDF blends, J. Electron. Mater., 2020, 49(3),
1588–1600.
37 M. Arjmand, T. Apperley, M. Okoniewski and U. Sundararaj,
Comparative study of electromagnetic interference shielding
properties of injection molded versus compression molded
multi-walled carbon nanotube/polystyrene composites,
Carbon, 2012, 50(14), 5126–5134.
38 S. Das, S. Sharma, T. Yokozeki and S. Dhakate, Conductive
layer-based multifunctional structural composites for elec-
tromagnetic interference shielding, Compos. Struct., 2021,
261, 113293.
39 X. Jin, J. Wang, L. Dai, X. Liu, L. Li, Y. Yang and S. Guo, Flame-
retardant poly(vinyl alcohol)/MXene multilayered films with
outstanding electromagnetic interference shielding and ther-
mal conductive performances, Chem. Eng. J., 2020, 380, 122475.
40 S. Zeng, Z.-X. Huang, H. Jiang and Y. Li, From waste to
wealth: A lightweight and flexible leather solid waste/
polyvinyl alcohol/silver paper for highly efficient electro-
magnetic interference shielding, ACS Appl. Mater. Interfaces,
2020, 12(46), 52038–52049.
41 R. Wilson, G. George and K. Joseph, An introduction
to materials for potential EMI shielding applications:
Status and future, in Materials for Potential EMI Shielding
Applications, 2020, Elsevier, pp. 1–8.
42 J. Kuruvilla, R. Wilson and G. Gejo, Materials for Potential
EMI Shielding Applications: Processing, Properties and
Current Trends, Elsevier, 2019.
New J. Chem., 2021, 45, 21488–21507 | 21503

NJC
43 M. Jaroszewski, S. Thomas and A. V. Rane, Advanced
Materials for Electromagnetic Shielding: Fundamentals, Proper-
ties, and Applications, 2018.
44 M. K. Aswathi, A. V. Rane, V. Ajay, A. R. Ajitha, S. Thomas,
Published on 02 November 2021. Downloaded by University of Science and Technology of China on 5/4/2024 5:35:17 PM.
and M. Jaroszewski, EMI shielding fundamentals. Advanced
Materials for Electromagnetic Shielding: Fundamentals,
Properties, and Applications, 2018, pp. 1–9.
45 S. B. Kondawar and P. R. Modak, Theory of EMI shielding, in
Materials for Potential EMI Shielding Applications, Elsevier,
2020, pp. 9–25.
46 Y. Bhattacharjee, V. Bhingardive, S. Biswas and S. Bose,
Construction of a carbon fiber based layer-by-layer (LbL)
assembly–a smart approach towards effective EMI shield-
ing, RSC Adv., 2016, 6(113), 112614–112619.
47 H. Nallabothula, Y. Bhattacharjee, L. Samantara and
S. Bose, Processing-mediated different states of dispersion
of multiwalled carbon nanotubes in PDMS nanocomposites
influence EMI shielding performance, ACS Omega, 2019, 4(1),
1781–1790.
48 I. Arief, Y. Bhattacharjee, O. Prakash, M. Sahu, S. Suwas
and S. Bose, Tunable CoNi microstructures in flexible
multilayered polymer films can shield electromagnetic
radiation, Composites, Part B, 2019, 177, 107283.
49 H. Guo, Y. Chen, Y. Li, W. Zhou, W. Xu, L. Pang and
S. Jiang, Electrospun fibrous materials and their applica-
tions for electromagnetic interference shielding: A review,
Composites, Part A, 2021, 106309.
50 P. Song, B. Liu, H. Qiu, X. Shi, D. Cao and J. Gu, MXenes for
polymer matrix electromagnetic interference shielding
composites: A review, Compos. Commun., 2021, 100653.
51 M. Wang, X.-H. Tang, J.-H. Cai, H. Wu, J.-B. Shen and
S.-Y. Guo, Construction, mechanism and prospective of
conductive polymer composites with multiple interfaces
for electromagnetic interference shielding: A review,
Carbon, 2021, 177, 377–402.
52 Y. Bhattacharjee and S. Bose, Core–shell nanomaterials for
microwave absorption and electromagnetic interference
shielding: A review, ACS Appl. Nano Mater., 2021, 4(2), 949–972.
53 Y. Yao, S. Jin, H. Zou, L. Li, X. Ma, G. Lv and Q. Shu,
Polymer-based lightweight materials for electromagnetic
interference shielding: A review, J. Mater. Sci., 2021, 1–32.
54 H. Wang, S. Li, M. Liu, J. Li and X. Zhou, Review on
shielding mechanism and structural design of electro-
magnetic interference shielding composites, Macromol.
Mater. Eng., 2021, 2100032.
55 N. Maruthi, M. Faisal and N. Raghavendra, Conducting
polymer based composites as efficient EMI shielding
materials: A comprehensive review and future prospects,
Synth. Met., 2021, 272, 116664.
56 S. Liu, S. Qin, Y. Jiang, P. Song and H. Wang, Lightweight
high-performance carbon-polymer nanocomposites for
electromagnetic interference shielding, Composites, Part
A, 2021, 106376.
57 S. Hema and S. Sambhudevan, Ferrite-based polymer
nanocomposites as shielding materials: A review, Chem.
Pap., 2021, 1–14.
21504 | New J. Chem., 2021, 45, 21488–21507 This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
Perspective
58 N. Wu, Q. Hu, R. Wei, X. Mai, N. Naik, D. Pan and Z. Shi,
Review on the electromagnetic interference shielding
properties of carbon based materials and their novel
composites: Recent progress, challenges and prospects,
Carbon, 2021, 176, 88–105.
59 D. Wanasinghe, F. Aslani, G. Ma and D. Habibi, Review
of polymer composites with diverse nanofillers for electro-
magnetic interference shielding, Nanomaterials, 2020,
10(3), 541.
60 A. Nazir, A review of polyvinylidene fluoride (PVDF), poly-
urethane (PU), and polyaniline (PANI) composites-based
materials for electromagnetic interference shielding,
J. Thermoplast. Compos. Mater., 2020, 0892705720925120.
61 K. Sushmita, G. Madras and S. Bose, Polymer nanocompo-
sites containing sEMIconductors as advanced materials for
EMI shielding, ACS Omega, 2020, 5(10), 4705–4718.
62 C. Liu, L. Wang, S. Liu, L. Tong and X. Liu, Fabrication
strategies of polymer-based electromagnetic interference
shielding materials, Adv. Ind. Eng. Polym. Res., 2020, 3(4),
149–159.
63 M. Panahi-Sarmad, M. Noroozi, M. Abrisham, S. Eghbalinia,
F. Teimoury, A. R. Bahramian and V. Goodarzi, A compre-
hensive review on carbon-based polymer nanocomposite
foams as electromagnetic interference shields and piezo-
resistive sensors, ACS Appl. Electron. Mater., 2020, 2(8),
2318–2350.
64 H. Abbasi, M. Antunes and J. Velasco, Ignacio, Recent
advances in carbon-based polymer nanocomposites for
electromagnetic interference shielding., Prog. Mater. Sci.,
2019, 103, 319–373.
65 S. Geetha, K. K. Satheesh Kumar, C. R. K. Rao, M. Vijayan
and D. C. Trivedi, EMI shielding: Methods and materi-
als—A review, J. Appl. Polym. Sci., 2009, 112(4), 2073–2086.
66 J.-M. Thomassin, C. Jerome, T. Pardoen, C. Bailly,
I. Huynen and C. Detrembleur, Polymer/carbon based
composites as electromagnetic interference (EMI) shield-
ing materials, Mater. Sci. Eng., R, 2013, 74(7), 211–232.
67 B. Shen, W. Zhai and W. Zheng, Ultrathin flexible gra-
phene film: An excellent thermal conducting material with
efficient EMI shielding, Adv. Funct. Mater., 2014, 24(28),
4542–4548.
68 W.-L. Song, L.-Z. Fan, M.-S. Cao, M.-M. Lu, C.-Y. Wang,
J. Wang and J. Liu, Facile fabrication of ultrathin graphene
papers for effective electromagnetic shielding, J. Mater.
Chem. C, 2014, 2(25), 5057–5064.
69 H. Wu and L. T. Drzal, Graphene nanoplatelet paper as a
light-weight composite with excellent electrical and ther-
mal conductivity and good gas barrier properties, Carbon,
2012, 50(3), 1135–1145.
70 B. Shen, Y. Li, D. Yi, W. Zhai, X. Wei and W. Zheng,
Microcellular graphene foam for improved broadband
electromagnetic interference shielding, Carbon, 2016,
102, 154–160.
71 D. Zhang, B. Chi, B. Li, Z. Gao, Y. Du, J. Guo and J. Wei,
Fabrication of highly conductive graphene flexible circuits
by 3D printing, Synth. Met., 2016, 217, 79–86.

Perspective
72 Z.-S. Wu, W. Ren, L. Gao, J. Zhao, Z. Chen, B. Liu and H.-
M. Cheng, Synthesis of graphene sheets with high elec-
trical conductivity and good thermal stability by hydrogen
arc discharge exfoliation, ACS Nano, 2009, 3(2), 411–417.
Published on 02 November 2021. Downloaded by University of Science and Technology of China on 5/4/2024 5:35:17 PM.
73 I.-W. P. Chen, R. Liang, H. Zhao, B. Wang and C. Zhang,
Highly conductive carbon nanotube buckypapers with
improved doping stability via conjugational cross-linking,
Nanotechnology, 2011, 22(48), 485708.
74 Y. Z. Keteklahijani, M. Arjmand and U. Sundararaj, Cobalt
catalyst grown carbon nanotube/poly(vinylidene fluoride)
nanocomposites: Effect of synthesis temperature on mor-
phology, electrical conductivity and electromagnetic interfer-
ence shielding., ChemistrySelect, 2017, 2(31), 10271–10284.
75 H. Yao, C.-C. Chu, H.-J. Sue and R. Nishimura, Electrically
conductive superhydrophobic octadecylamine-functionalized
multiwall carbon nanotube films, Carbon, 2013, 53, 366–373.
76 O. Y. Podyacheva, S. V. Cherepanova, A. I. Romanenko, L. S.
Kibis, D. A. Svintsitskiy, A. I. Boronin and Z. R. Ismagilov,
Nitrogen doped carbon nanotubes and nanofibers: Composi-
tion, structure, electrical conductivity and capacity proper-
ties, Carbon, 2017, 122, 475–483.
77 A. S. Zeraati, S. A. Mirkhani, P. Sun, M. Naguib, P. V. Braun
and U. Sundararaj, Improved synthesis of Ti3C2Tx MXenes
resulting in exceptional electrical conductivity, high synth-
esis yield, and enhanced capacitance, Nanoscale, 2021,
13(6), 3572–3580.
78 J. Zhang, N. Kong, S. Uzun, A. Levitt, S. Seyedin, P. A. Lynch
and J. Liu, Scalable manufacturing of free-standing, strong
Ti3C2Tx MXene films with outstanding conductivity, Adv.
Mater., 2020, 32(23), 2001093.
79 A. Sarycheva, A. Polemi, Y. Liu, K. Dandekar, B. Anasori
and Y. Gogotsi, 2D titanium carbide (MXene) for wireless
communication, Sci. Adv., 2018, 4(9), eaau0920.
80 O. Breuer and U. Sundararaj, Big returns from small fibers:
A review of polymer/carbon nanotube composites, Polym.
Compos., 2004, 25(6), 630–645.
81 M. Kamkar, S. Sadeghi, M. Arjmand, E. Aliabadian and
U. Sundararaj, Intra-cycle elastic nonlinearity of nitrogen-
doped carbon nanotube/polymer nanocomposites under
medium amplitude oscillatory shear (MAOS) flow, Nano-
materials, 2020, 10(7), 1257.
82 M. Kamkar, S. Sadeghi, M. Arjmand and U. Sundararaj,
Structural characterization of CVD custom-synthesized
carbon nanotube/polymer nanocomposites in large-amplitude
oscillatory shear (LAOS) mode: Effect of dispersion
Characteristics in Confined Geometries, Macromolecules,
2019, 52(4), 1489–1504.
83 M. Kamkar, S. M. N. Sultana, S. P. Pawar, A. Eshraghian,
E. Erfanian and U. Sundararaj, The key role of processing
in tuning nonlinear viscoelastic properties and microwave
absorption in CNT-based polymer nanocomposites, Mater.
Today Commun., 2020, 24, 101010.
84 E. Erfanian, M. Kamkar, D. Williams, K. Zamani, S. Yalda,
R. Reza, S. Sinha and U. Sundararaj, Dielectrorheology
of aspect-ratio-tailored carbon nanotube/polyethylene
composites under large deformations: Implications for
This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
NJC
high-temperature dielectrics, ACS Appl. Nano Mater.,
2021, DOI: 10.1021/acsanm.1c01698.
85 L.-Q. Zhang, B. Yang, J. Teng, J. Lei, D.-X. Yan, G.-J. Zhong
and Z.-M. Li, Tunable electromagnetic interference shield-
ing effectiveness via multilayer assembly of regenerated
cellulose as a supporting substrate and carbon nanotubes/
polymer as a functional layer, J. Mater. Chem. C, 2017,
5(12), 3130–3138.
86 M. Han, X. Yin, H. Wu, Z. Hou, C. Song, X. Li and L. Cheng,
Ti3C2 MXenes with modified surface for high-performance
electromagnetic absorption and shielding in the X-band,
ACS Appl. Mater. Interfaces, 2016, 8(32), 21011–21019.
87 M. Han, X. Yin, L. Kong, M. Li, W. Duan, L. Zhang and
L. Cheng, Graphene-wrapped ZnO hollow spheres with
enhanced electromagnetic wave absorption properties,
J. Mater. Chem. A, 2014, 2(39), 16403–16409.
88 M. Mahmoodi, M. Arjmand, U. Sundararaj and S. Park,
The electrical conductivity and electromagnetic interfer-
ence shielding of injection molded multi-walled carbon
nanotube/polystyrene composites, Carbon, 2012, 50(4),
1455–1464.
89 Y. Li, B. Xue, S. Yang, Z. Cheng, L. Xie and Q. Zheng,
Flexible multilayered films consisting of alternating nano-
fibrillated cellulose/Fe3O4 and carbon nanotube/polyethy-
lene oxide layers for electromagnetic interference
shielding, Chem. Eng. J., 2021, 410, 128356.
90 L. He, Y. Shi, Q. Wang, D. Chen, J. Shen and S. Guo,
Strategy for constructing electromagnetic interference shield-
ing and flame retarding synergistic network in poly(butylene
succinate) and thermoplastic polyurethane multilayered
composites, Compos. Sci. Technol., 2020, 199, 108324.
91 Y. Li, B. Shen, X. Pei, Y. Zhang, D. Yi, W. Zhai and
W. Zheng, Ultrathin carbon foams for effective electro-
magnetic interference shielding, Carbon, 2016, 100,
375–385.
92 D. Prokopiou, M. Pissas, G. Fibbi, F. Margheri, B. Kalska-
Szostko, G. Papanastasiou and E. Efthimiadou, Synthesis
and characterization of modified magnetic nanoparticles
as theranostic agents: In vitro safety assessment in healthy
cells, Toxicology in Vitro, 2021, 72, 105094.
93 M. -S. Ece, Synthesis and characterization of activated
carbon supported magnetic nanoparticles (Fe3O4/AC@
SiO2@ Sulfanilamide) and its application in removal of
toluene and benzene, Colloids Surf., A, 2021, 617, 126231.
94 Y. Bi, M. Ma, Z. Liao, Z. Tong, Y. Chen, R. Wang and G. Wu,
One-dimensional Ni@ Co/C@ PPy composites for superior
electromagnetic wave absorption, J. Colloid Interface Sci.,
2022, 605, 483–492.
95 G. Wu, H. Zhang, X. Luo, L. Yang and H. Lv, Investigation
and optimization of Fe/ZnFe2O4 as a wide-band electro-
magnetic absorber, J. Colloid Interface Sci., 2019, 536,
548–555.
96 X. Yang, X. Yu, Q. Yang, D. Zhao, K. Zhang, J. Yao and
X. Zuo, Controllable synthesis and magnetic properties of
hydrothermally synthesized NiCo2O4 nano-spheres, Ceram.
Int., 2017, 43(12), 8585–8589.
New J. Chem., 2021, 45, 21488–21507 | 21505

NJC
97 A. Tomitaka, H. Kobayashi, T. Yamada, M. Jeun, S. Bae and
Y. Takemura, Magnetization and self-heating temperature
of NiFe2O4 nanoparticles measured by applying ac mag-
netic field, J. Phys.: Conf. Ser., 2010, 200(12), 122010.
Published on 02 November 2021. Downloaded by University of Science and Technology of China on 5/4/2024 5:35:17 PM.
98 Z. Tong, Y. Bi, M. Ma, Z. Liao, W. Huang, K. L. Chung and
C. Pan, Fabrication of flower-like surface Ni@Co3O4 nano-
wires anchored on RGO nanosheets for high-performance
microwave absorption, Appl. Surf. Sci., 2021, 565, 150483.
99 Z. Liao, M. Ma, Z. Tong, Y. Bi, K. L. Chung, M. Qiao and
Z. Li, Fabrication of one-dimensional ZnFe2O4@ carbon@
MoS2/FeS2 composites as electromagnetic wave absorber,
J. Colloid Interface Sci., 2021, 600, 90–98.
100 T. Dippong, O. Cadar, I. G. Deac, M. Lazar, G. Borodi and
E. A. Levei, Influence of ferrite to silica ratio and thermal
treatment on porosity, surface, microstructure and mag-
netic properties of Zn0. 5Ni0. 5Fe2O4/SiO2 nanocompo-
sites, J. Alloys Compd., 2020, 828, 154409.
101 X. Ji, D. Chen, J. Shen and S. Guo, Flexible and flame-
retarding thermoplastic polyurethane-based electro-
magnetic interference shielding composites, Chem. Eng.
J., 2019, 370, 1341–1349.
102 C. Chen, X. Zhao, C. Shi and J. Chen, Synergistic effect
between carbon nanoparticle and intumescent flame
retardant on flammability and smoke suppression of
copolymer thermoplastic polyurethane, J. Mater. Sci.,
2018, 53(8), 6053–6064.
103 X. Ji, D. Chen, Q. Wang, J. Shen and S. Guo, Synergistic
effect of flame retardants and carbon nanotubes on flame
retarding and electromagnetic shielding properties of
thermoplastic polyurethane, Compos. Sci. Technol., 2018,
163, 49–55.
104 M. Y. Yablokov, V. G. Shevchenko, L. A. Mukhortov and
A. N. Ozerin, Electromagnetic interference shielding of
carbon nanotube-fluoropolymer elastomer composites
with layered structure, Fullerenes, Nanotubes Carbon Nanos-
truct., 2020, 28(4), 267–271.
105 A. Allahbakhsh and M. Arjmand, Graphene-based phase
change composites for energy harvesting and storage: state
of the art and future prospects, Carbon, 2019, 148,
441–480.
106 D. D. L. Chung, A review of exfoliated graphite, J. Mater.
Sci., 2016, 51(1), 554–568.
107 A. R. Moghaddam, M. Kamkar, Z. Ranjbar, U. Sundararaj,
A. Jannesari and B. Ranjbar, Tuning the network structure
of graphene/epoxy nanocomposites by controlling edge/
basal localization of functional groups, Ind. Eng. Chem.
Res., 2019, 58(47), 21431–21440.
108 A. R. Moghaddam, Z. Ranjbar, U. Sundararaj, A. Jannesari
and M. Kamkar, A novel electrically conductive water
borne epoxy nanocomposite coating based on graphene:
Facile method and high efficient graphene dispersion.,
Prog. Org. Coat., 2019, 136, 105223.
109 X. Zhang, X. Zhang, M. Yang, S. Yang, H. Wu, S. Guo and
Y. Wang, Ordered multilayer film of (graphene oxide/
polymer and boron nitride/polymer) nanocomposites: an
ideal EMI shielding material with excellent electrical
21506 | New J. Chem., 2021, 45, 21488–21507 This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
Perspective
insulation and high thermal conductivity, Compos. Sci.
Technol., 2016, 136, 104–110.
110 T. L. Li and S. L.-C. Hsu, Preparation and properties of
thermally conductive photosensitive polyimide/boron nitride
nanocomposites, J. Appl. Polym. Sci., 2011, 121(2), 916–922.
111 L. Liang, P. Xu, Y. Wang, Y. Shang, J. Ma, F. Su and C. Liu,
Flexible polyvinylidene fluoride film with alternating
oriented graphene/Ni nanochains for electromagnetic
interference shielding and thermal management, Chem.
Eng. J., 2020, 395, 125209.
112 H. J. Im, J. Y. Oh, S. Ryu and S. H. Hong, The design and
fabrication of a multilayered graded GNP/Ni/PMMA nano-
composite for enhanced EMI shielding behavior., RSC
Adv., 2019, 9(20), 11289–11295.
113 Y. Li, B. Shen, D. Yi, L. Zhang, W. Zhai, X. Wei and
W. Zheng, The influence of gradient and sandwich config-
urations on the electromagnetic interference shielding
performance of multilayered thermoplastic polyurethane/
graphene composite foams, Compos. Sci. Technol., 2017,
138, 209–216.
114 Y. Gogotsi and B. Anasori, The rise of MXenes, ACS
Publications, 2019.
115 M. Naguib, M. Kurtoglu, V. Presser, J. Lu, J. Niu, M. Heon and
M. W. Barsoum, Two-dimensional nanocrystals produced by
exfoliation of Ti3AlC2, Adv. Mater., 2011, 23(37), 4248–4253.
116 A. Ghaffarkhah, M. Kamkar, H. Riazi, E. Hosseini,
Z. A. Dijvejin, K. Golovin and M. Arjmand, Scalable man-
ufacturing of flexible and highly conductive Ti3C2/PEDOT:
PSS thin films for electromagnetic interference shielding,
New J. Chem., 2021, DOI: 10.1039/D1NJ04513J.
117 J. Lipton, G.-M. Weng, M. Alhabeb, K. Maleski, F. Antonio,
J. Kong and A. D. Taylor, Mechanically strong and electri-
cally conductive multilayer MXene nanocomposites, Nano-
scale, 2019, 11(42), 20295–20300.
118 B. Zhou, Z. Zhang, Y. Li, G. Han, Y. Feng, B. Wang and
C. Liu, Flexible, robust, and multifunctional electromag-
netic interference shielding film with alternating cellulose
nanofiber and MXene layers, ACS Appl. Mater. Interfaces,
2020, 12(4), 4895–4905.
119 H. Liu, R. Fu, X. Su, B. Wu, H. Wang, Y. Xu and X. Liu,
Electrical insulating MXene/PDMS/BN composite with
enhanced thermal conductivity for electromagnetic shield-
ing application, Compos. Commun., 2021, 23, 100593.
120 Z. Ma, S. Kang, J. Ma, L. Shao, Y. Zhang, C. Liu and J. Gu,
Ultraflexible and mechanically strong double-layered
aramid nanofiber–Ti3C2Tx MXene/silver nanowire nano-
composite papers for high-performance electromagnetic
interference shielding, ACS Nano, 2020, 14(7), 8368–8382.
121 Y. Wu, F. Wang and Y. Huang, Facile and simple fabrica-
tion of strong, transparent and flexible aramid nanofibers/
bacterial cellulose nanocomposite membranes, Compos.
Sci. Technol., 2018, 159, 70–76.
122 C. Xie, L. He, Y. Shi, Z.-X. Guo, T. Qiu and X. Tuo, From
monomers to a lasagna-like aerogel monolith: An assembling
strategy for aramid nanofibers, ACS Nano, 2019, 13(7),
7811–7824.

Perspective
123 W. Tian, T. Qiu, Y. Shi, L. He and X. Tuo, The facile
preparation of aramid insulation paper from the bottom-
up nanofiber synthesis, Mater. Lett., 2017, 202, 158–161.
124 S. Sadeghi, M. Arjmand, I. Otero Navas, A. Zehtab Yazdi
Published on 02 November 2021. Downloaded by University of Science and Technology of China on 5/4/2024 5:35:17 PM.
and U. Sundararaj, Effect of nanofiller geometry on net-
work formation in polymeric nanocomposites: Compari-
son of rheological and electrical properties of multiwalled
carbon nanotube and graphene nanoribbon, Macromole-
cules, 2017, 50(10), 3954–3967.
125 Q. Qi, L. Ma, B. Zhao, S. Wang, X. Liu, Y. Lei and C. B. Park,
An effective design strategy for the sandwich structure
of PVDF/GNP-Ni-CNT composites with remarkable electro-
magnetic interference shielding effectiveness, ACS Appl.
Mater. Interfaces, 2020, 12(32), 36568–36577.
This journal is © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique 2021
View Article Online
NJC
126 J.-H. Lin, Z.-I. Lin, Y.-J. Pan, C.-L. Huang, C.-K. Chen and
C.-W. Lou, Polymer composites made of multi-walled
carbon nanotubes and graphene nano-sheets: Effects of
sandwich structures on their electromagnetic interference
shielding effectiveness, Composites, Part B, 2016, 89, 424–431.
127 W.-L. Song, M.-S. Cao, M.-M. Lu, S. Bi, C.-Y. Wang, J. Liu
and L.-Z. Fan, Flexible graphene/polymer composite films
in sandwich structures for effective electromagnetic inter-
ference shielding, Carbon, 2014, 66, 67–76.
128 A. Sheng, W. Ren, Y. Yang, D.-X. Yan, H. Duan, G. Zhao and
Z.-M. Li, Multilayer WPU conductive composites with
controllable electro-magnetic gradient for absorption-
dominated electromagnetic interference shielding, Compo-
sites, Part A, 2020, 129, 105692.
New J. Chem., 2021, 45, 21488–21507 | 21507