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REVIEW

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Carbon-Based Radar Absorbing Materials toward Stealth


Technologies
Seong-Hwang Kim, Seul-Yi Lee, Yali Zhang, Soo-Jin Park,* and Junwei Gu*

enhancing survivability in electronic


Stealth technology is used to enhance the survival of military equipment in warfare.[1–7] In response to an ever-
the field of military surveillance, as it utilizes a combination of techniques to increasing range of high-performance
render itself undetectable by enemy radar systems. Radar absorbing materials radar-guided missiles and interceptors on
(RAMs) are specialized materials used to reduce the reflection (or absorption) the modern battlefield, the so-called stealth
technology (or low observable technology)
of radar signals to provide stealth capability, which is a core component of
has recently begun to be incorporated into
passive countermeasures in military applications. The properties of RAMs can the great majority of new aircraft, ship,
be optimized by adjusting their composition, microstructure, and surface missile, satellite, and submarine designs
geometry. Carbon-based materials present a promising approach for the to render them invisible to infrared, radar,
fabrication of ultrathin, versatile, and high-performance RAMs due to their and other detection methods.[8–15] Radar
primarily detects aircraft when they enter
large specific surface area, lightweight, excellent dielectric properties, high
monitored airspace, i.e., the emitted radar
electrical conductivity, and stability under harsh conditions. This review signal is reflected off the aircraft back to
begins with a brief history of stealth technology and an introduction to the radar. Especially for military aircraft, all
electromagnetic waves, radar systems, and radar absorbing materials. This is new designs take low observable principles
followed by a discussion of recent research progress in carbon-based RAMs, and techniques into account, while existing
including carbon blacks, carbon fibers, carbon nanotubes, graphite, graphene, jet fighters are considered for modification
in order to reduce their radar signatures.
and MXene, along with an in-depth examination of the principles and
The development of stealth technol-
strategies on electromagnetic attenuation characteristics. Hope this review ogy begun before World War I (1914–
will offer fresh perspectives on the design and fabrication of carbon-based 1918). At the time, because radar was not
RAMs, thereby fostering a deeper fundamental understanding and promoting yet invented, visibility was the primary
practical applications. concern.[16,17] It dates back to 1912 in Ger-
many. Where researchers produced mono-
planes in which the fuselage was covered
by a transparent material derived from cel-
lulose, and this was painted them with
1. Introduction bright colors to further reduce visibility. As a result, the aircraft
With the advancement in military surveillance systems, stealth was invisible from the ground when flown at or above 900 ft and
technology has attracted significant interest with regard to only slightly visible at low altitudes. Soviet aircraft designers in
the 1930s also attempted to design transparent aircraft, and radar
was invented in 1939. In 1944, a German bomber (Horten Ho
S.-H. Kim, S.-Y. Lee, S.-J. Park 229) was designed, where its wings were made of carbon black-
Department of Chemistry impregnated plywood held together by a mixture of sawdust and
Inha University charcoal. Being one of the earliest radar-stealth aircraft designed
100 Inharo, Incheon 22212, South Korea by Germans, it absorbed electromagnetic waves and had a small
E-mail: sjpark@inha.ac.kr
radar cross section. At the same time, Germans used graphite
Y. Zhang, J. Gu
Shaanxi Key Laboratory of Macromolecular Science and Technology dispersed in a rubber matrix, next to ordinary paper, in a three-
School of Chemistry and Chemical Engineering layer material called the chimney-sweeper and swamp.[18–20] Ap-
Northwestern Polytechnical University plication of this rubber-based composite enabled a reduction in
Xi’an, Shaanxi 710072, P. R. China the reflectivity of radio waves. Throughout the 1960s and 1970s,
E-mail: gjw@nwpu.edu.cn
the development of true stealth aircraft continued primarily in
The ORCID identification number(s) for the author(s) of this article
the United States (U.S.), with several stealth prototypes being
can be found under https://doi.org/10.1002/advs.202303104 studied. Here, Americans applied similar solutions, but replaced
© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH. graphite with carbon black (CB) and carbon nanotubes (CNTs)
This is an open access article under the terms of the Creative Commons to obtain the Halpern anti-radiation paint (HARP) used in the
Attribution License, which permits use, distribution and reproduction in aircraft.[21,22] With the discovery and development of graphite,
any medium, provided the original work is properly cited. CB, CNTs, graphene, graphite nanoplatelets, carbon aerogels,
DOI: 10.1002/advs.202303104 carbon fibers (CFs), and other new macro- or nano-scale carbon

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Figure 1. A statistical survey of the number of literature publications per year between 2010 and 2022 based on the keyword “stealth” and other keywords
relating to the field of stealth (e.g., “carbon materials”) using the scientific database Web of Science (as of Nov 2022).

Figure 2. A schematic visualization of the stealth jamming and survival equipment.

allotropes, the carbon family has come to play an irreplaceable Radar Absorbing Structure (RAS) stealth across the world, they
role in stealth technology.[23–29] Now, 50 years later, various stud- mainly focus on the use of Radar Absorbing Materials (RAMs)
ies on carbon materials have proved to be important for the future such as carbon materials as fillers.[30–35] On the “battlefield” of
of stealth systems (Figure 1). stealth technology itself, the development of RAMs has been ac-
Advanced multispectral compatible stealth materials are in- companied by continuous advances in the construction of in-
creasingly needed due to the rapid development of detector and creasingly sophisticated radar as a natural countermeasure.[36–38]
precision guidance technology, which has made the threat to mili- As shown in Figure 3, all radar systems use microwaves (MWs)
tary targets and weapons more serious (Figure 2). Although many to detect, locate, and determine the velocity of the target object,
research articles are available on the successful realization of and can work across a wide range of transmission frequencies

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Figure 3. Radar frequency bands according to the Institute of Electrical and Electronics Engineers (IEEE) standards. Reproduced with permission
from,[43] Copyright Elsevier 2018.

Table 1. Radar frequency bands (Reproduced with permission from,[43] Copyright Elsevier 2018).

Radar frequency Radar range Wavelength Used


bands (IEEE)

TLF <3 Hz >100000 km Frequency of neural activity.


ELF 3–30 Hz 100000–10000 km Neural activity, communication with submarines.
SLF 30–300 Hz 10000–1000 km Communication with submarines.
ULF 300–3000 Hz 1000–100 km Communication with submarines, Communications in mines across the land.
VLF 3–30 kHz 100–10 km Radio help, underwater communication, wireless pulse gauges, time signals, geophysics.
LF 30–300 kHz 10–1 km Radio help, AM broadcasting (long wave), RFID, amateur radio, time signals.
MF 300–3000 kHz 1000–100 m AM broadcasting (medium wave), avalanche beacon, amateur radio.
HF 3–30 MHz 100–10 m Over the horizon surveillance; low range and low resolution.
VHF 30–300 MHz 10–1 m Long-range surveillance, counter stealth, ground-penetrating; low/medium resolution.
UHF 300–1000 MHz 1–0.3 m Long-range surveillance, FOPEN: low/medium resolution.
L 1–2 GHz 30–15 cm Long-range air traffic control; medium resolution, small weather effects.
S 2–4 GHz 15–7.5 cm Terminal air traffic control, long-range weather observation, moderate weather effect in heavy
precipitation.
C 4–8 GHz 7.5–3.75 cm Long-range tracking, weather observation, weapon location; increased weather effect in
light/medium rain.
X 8–12.5 GHz 3.75–2.4 cm Short-range tracking, missile guidance, mapping marine radar, airborne intercept, battlefield
surveillance, weapon location.
Ku 12.5–18 GHz 2.4–1.7 cm High-resolution mapping, satellite altimetry, short-range due to water vapor absorption.
K 18–26.5 GHz 1.7–1.1 cm Police radar; very limited use due to high water vapor absorption.
Ka 26.5–40 GHz 1.1–0.75 cm Short-range very high-resolution mapping, airport surveillance; short range due to water
vapor absorption.
V 40–75 GHz 0.75–0.4 cm Scientific remote sensing; high water vapor absorption.
W 75–110 GHz 0.2–0.1 cm Automobile crusie control (77 GHz), missile seekers, very high-resolution imaging (94 GHz).

from 3 MHz to 300 GHz and their corresponding wavelengths (12.5–18.0 GHz), the K band (18.0–26.5 GHz), and the KA band
from 1 mm up to tens of meters depending on the optimum (26.5–40.0).[42,43] For example, Zhao et al. have explored the pos-
operating conditions.[39–41] The Institute of Electrical and Elec- sibility of using CNTs as RAMs.[44] They observed when the CNT
tronics Engineers (IEEE) provides additional information on the content reaches 10 wt%; the epoxy-based composites containing
radar frequency which, in most cases, corresponds to the IEEE CNTs achieved a reflection loss (RL) below –10 dB (90% absorp-
standard, as listed in Table 1. The major frequency bands for tion) over 3.0 GHz in the range of 10.1–13.1 GHz, and the maxi-
long-range surveillance, aerospace, military, and aircraft radars mum value was –22.89 dB at 11.4 GHz. Additionally, Chen et al.
include the L band (1.0–2.0 GHz), the S band (2.0–4.0 GHz), the studied the radar-absorbing effects of graphene in the interlayers
C band (4.0–8.0 GHz), the X band (8.0–12.5 GHz), the Ku band of Fe-doped nanocomposites and found that when the graphene

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Figure 4. A schematic visualization of the radar operating principle.

content reached 20 wt% and the film thickness was 2.5 mm, the by an object.[51–53] The visualization factors relating to the detec-
effective bandwidth was determined to be 14.2 GHz, yielding a tion of a target are shown in Figure 4. The main component of the
maximum RL of −31.5 dB.[45] Meanwhile, Wu et al. fabricated radar system is the transmitter, which can transmit electromag-
polyaniline-based composites with a 30 wt.% of CBs to obtain a netic waves in the intended directions. The waves in the trans-
maximum absorption of −40 dB for the frequency range of 9.0– mitter travel through free space, interact with the target under
13.0 GHz (the X-band).[46] Similarly, Zou et al. reported a band- observation, and return to the receiver. Thus, radar measures the
width below –10.0 dB at 12.2 GHz with a CF content of 0.76 wt.%. interval of time between the generation of the electromagnetic
Consequently, more and more carbon-based materials are being waves and the return of the waves to the radar after reflecting
used as RAMs in the fabrication of stealth equipment.[47] from the target. It uses the radar Equations (1) and (2) to deter-
Stealth technologies have improved rapidly over the past 100 mine the distance between the target and radar as follows.[54–56] :
years, and will probably continue to develop at a greater speed
during the future 100 years if universal properties permit. To the ct
R = (1)
best of the present author’s knowledge, the utilization of carbon- 2
based materials for stealth technologies is still a relatively new
topic. Thus, the present review aims to highlight the recent ad- where R is the range between the target and the radar, c is the
vances in carbon-based materials as the best feasible option for speed of light, and t is the time taken by the energy pulse to move
the development of stealth technologies. To this end, after provid- from the radar and back after striking the target, and
ing an introduction of electromagnetic waves, frequency bands,
radar systems, radar cross section, and radar absorbing materials, Pt Gt 𝜎
a comprehensive discussion of the recent research progress in Pr = × × Ae (2)
4𝜋R2 4𝜋R2
carbon-based RAMs, including carbon blacks, carbon fibers, car-
bon nanotubes, graphite, graphene, and MXene, in terms of elec- where Pr is the returned power, Pt is the transmitted power, Gt is
tromagnetic attenuation characteristics are provided. Last, this the antenna gain, 𝜎 is the radar cross section (RCS) of the target
review article addresses the desirable feature of the next gener- (m2 ), and Ae is the effective aperture of the receiving antenna
ation of carbon-based RAMs for practical stealth technology. (m2 ). All these variables are used in the detection of an object, but
the RCS plays an important role in the detection of the target.
2. Radar Stealth
Radar absorption is a basic and most important requirement for 3. Radar Cross Section (RCS)
stealth technologies. Radar stands for the “Radio Detection and
Ranging”, first patented by Christian Hulsmeyre in Germany The RCS is the virtual size of the object or target as seen by the
(1904).[48–50] Radar systems were developed during World War II radar, which is the core detection parameter at radar frequencies.
and their advance continues to the present day. The operating Detailed research on the RCS began in the early 1930s, shortly
principle of a radar is to send electromagnetic energy pulses in after the invention of radar.[57–60] The RCS measures the intensity
the direction of the target. These pulses move at the speed of light, of the waves returning to the radar after reflecting from the object
almost unobstructed, through space until they are encountered or target. The RCS (𝜎) can be calculated in square meters using

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Figure 5. The RCS values of various object or target in square meter and decibel square meter.

Equation (3):[61] ments). It acts to reduce the reflected electromagnetic radiations


by absorbing a considerable part of the incident electromagnetic
lEs l2 energy. It works to reduce the reflected electromagnetic radiation
𝜎 = lim 4𝜋R2 ⋅ (3)
R→∞ lEi l2 by absorbing a significant portion of the incident electromagnetic
energy. This can be achieved by employing one of the following
where Es is the scattered electric field, and Et is the field incident methods. Accepting the signals and subsequently lowering their
at the target. Alternatively, the RCS can be calculated in terms of intensity. This type of action is appropriate for a broad spectrum
decibel square meters (dB sm) by using Equation (4): of radar frequencies. Creating internal reflections of received sig-
𝜎m 2 𝜎 2 nals that impede the reflected signals from the outer surface. This
𝜎(dB sm) = 10log10 = 10log10 m 2 (4) action is effective when dealing with a specific frequency.
𝜎R 1m

where 𝜎 R is the RCS of a reference object or target with area of 4.2. Radar Abosorbing Mechanism
1 m2 . The typical RCS values of certain objects or targets such
as aircraft and ships according to Equations (3) and (4) are indi- The RAMs use two mechanisms to reduce, or eliminate the re-
cated in Figure 5. If the RCS is low, then the probability of detec- flected waves, as detailed below: i) absorption of the electromag-
tion by an enemy during a combat mission is also low, and the netic wave by the materials, thereby reducing the intensity via
capacity for penetration into enemy territory is high. Conversely, dielectric, resistive, and/or magnetic losses, and ultimately con-
a high RCS means that the object or target is likely to be detected verting it to heat energy, and ii) multiple internal reflections of
by the radar. The factors that influence the RCS of an object or the incident wave from the back and front interior faces of the
target include:[62] i) the size of the target, with a larger target hav- material.[63–67] These mechanisms are shown schematically in
ing greater RCS, ii) the material construction and, hence, the re- Figure 6.
flectivity, of the target, and iii) the geometric shape of the target, In detail, when electromagnetic energy is incident on a flat
which can be designed to prevent the reflection of waves toward lossy material, the reflectivity of the transverse electrically (TE)
the detection system. Among all the factors described above, care- polarized wave (RTE ) is equal to the square of the magnitude of
ful selection of construction materials would be a more viable way the reflection coefficient (r), and is given by Equation (5):[68–70]
for RCS reduction.
| √ |2
| cos 𝜃 − 𝜇r−1 n2 − sin 𝜃 2 |
4. Radar Absorbing Materials (RAMs) RTE |2
= ||rTE | = || √ |
| (5)
| cos 𝜃 + 𝜇 −1 n2 − sin 𝜃 2 |
| r |
4.1. Radar Abosorbing Theory
where 𝜖 r and μr are the relative complex permittivity and perme-
The RAMs are composites composed of an insulating binder ability of the lossy material, respectively, and 𝜃 is the incident an-
(matrix) along with conductive and magnetic fillers (reinforce- gle. Similarly, the reflectivity of the transverse magnetically (TM)

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Figure 6. A schematic diagram showing the mechanisms of electromagnetic attenuation by the RAM (i.e., absorption and multiple internal reflections).

and polarized wave (RTM) are also equal to the square of the mag- where 𝜖 0 and μ0 are the relative complex permittivity and perme-
nitude r, and is given by Equation (6): ability of free space, respectively. Because the impedance (Zin ) of
a metallic aircraft is close to zero, a signal that strikes the metal-
| √ |2 lic surface is mostly reflected. Meanwhile, the energy absorbed
| 𝜀r cos 𝜃 − 𝜇r−1 n2 − sin𝜃 2 |
RTM |2
= ||rTE | = || √ |
| (6) by the RAM depends on the thickness of the coating, the angle
| 𝜀r cos 𝜃 + 𝜇 −1 n2 − sin 𝜃 2 | of the incident wave, and the specific material properties. Hence,
| r |
an RAM must have an impedance value close to that of air and
For normal incidence, the reflectance of the TE and TM wave must be able to absorb the energy of the electromagnetic radi-
decreases as indicated by Equation (7): ation rapidly as it passes through the material. To achieve this
goal, the surface of the aircraft must be coated with dielectric or
| 𝜇 − n |2 magnetic materials.
R = || r |
| (7)
| 𝜇r + n |
5. RAMs Based on Carbon Materials and their
Additionally, the absorptivity (A) may be used, as calculated Composites
from Equation (8):
5.1. Carbon Black (CB)
|𝜇 − n |2
A = 1 − R = −|| r |
| (8) Carbon black (CB) is an amorphous allotrope of carbon with a
| 𝜇r + n | low density, high conductivity, and high mechanical strength,
and is generally derived from the combustion of petroleum
Generally, electromagnetic absorption performance can be
products.[72–75] In particular, it contains more than 90% pure el-
characterized by the waveguide, coaxial line, and free space meth-
emental carbon, and is made up of tiny, mostly spherical carbon
ods. The values of 𝜖 r and μr for a given material can then be ob-
atoms fused together in clusters known as aggregates. Due to its
tained from the vector network analyzer based on the tested scat-
favorable properties, CB has been the most commonly applied
tering parameters.[71] According to transmission line theory, the
reinforcing carbon filler in the manufacture of composites since
reflection loss (RL) can be calculated using Equation (9):
the First World War, and is used in applications such as a rein-
√ [ ( )] forcing agent to provide mechanical strength to absorber mate-
𝜇r 2𝜋fd √
Zin = Z0 tanh j 𝜀r 𝜇r (9) rials. Moreover, the electrical properties of a composite can be
𝜀r c enhanced by adding CB with a low particle density (high poros-
ity), small particle size (large surface area), low volatility (few oxy-
where Zin is the impedance of the absorber, given by Equa- gen groups), and favorable structure (better aggregation). This
tion (10): section covers some examples of CB-based RAMs as composites,
single- and multi-layer composites.
| Z − Z0 |
RL (dB) = 20 log || in |
| (10) Kwon et al. investigated the reinforcing effects of varying com-
| Zin + Z0 | positions (5, 10, 20, and 30 wt.%) of CB (Vulcan XC-72) fillers in
the silicone rubber matrices of single-layer composites.[76] The
where f and d are the microwave frequency and thickness, re- optimum CB content was identified as 10 wt.%, giving a maxi-
spectively, and c is the velocity of light. Meanwhile, Z0 is the mum RL of −22.2 dB in the frequency range of 11.6 GHz at a
impedance of free space (≈377 Ω), and is given by Equation (11): sample thickness of 1.9 mm (Figure 7a). Similarly, Oh et al. stud-
√ ied the effects of various contents (5, 6, 7, 8, 10, 15, and 20 wt.%)
𝜇0 of CB (Vulcan XC-72) filler in the grass fabric/epoxy prepreg
Z0 = ≈ 377Ω (11)
𝜀0 of multi-layer composites to conclude that the incorporation of

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Figure 7. The microwave absorbing properties of various CB-based RAMs: a) the calculated RL curves for single-layer silicone rubber composites with
CB (Vulcan XC-72) (Reproduced with permission from,[76] Copyright Wiley 2002), b) the calculated RL curve and microwave absorption mechanism
of polypropylene-based composites with various contents of CB (Xyui Zongze) (Reproduced with permission.[78] Copyright 2020, Elsevier), and c) the
geometry and RL curve of an absorber with a honeycomb sandwich structure (Reproduced with permission.[80] Copyright 2019, Elsevier).

7 wt.% CB significantly enhanced the microwave absorbing prop- waves via multi-scattering and reflection. Meanwhile, Luo et al.
erties of the composite, giving an RL of less than 10 dB in the fre- used a dipping process to prepare honeycomb cores with distinct
quency range of 2.4 GHz with a 0.6 mm thick sample.[77] Mean- pore sizes coated with epoxy resin and filled with conductive CB
while, Lee et al. reported the fabrication of polypropylene-based (Tianjing Ebory), as shown schematically in Figure 7c to obtain a
composites with inner diameters of 3 and 7 mm and various con- sandwich structure with an RL of up to –2.5 dB within the range
tents of CB (Xyui Zongze) via fused deposition modeling technol- of 8.7–16.4 GHz.[80]
ogy, as shown in Figure 7b.[78] The optimal CB content was found As discussed, an addition of CB alone is instructive to en-
to be 10 wt.%, giving a maximum RL of –62.6 dB at 10.6 GHz hancing microwave absorbing properties. Hence, future studies
with a 2.8-mm thick sample. The authors concluded that the mi- should focus more on the effects of particle size uniformity, film
crowave attenuation capacity was mainly due to conductive loss, thickness, dispersion, and roughness, while further refining the
interfacial polarization, dipole polarization, and multiple internal amount of CB. In addition, methods for skillfully controlling the
reflections, and that these properties were affected by the distri- nano-scale structure and design of single- and multi-layer ma-
bution of the CB particles. In addition, Mehdizadeh et al. inves- terials need to be investigated. Further, the performance of the
tigated the effects of various CB contents (2, 5, 7, and 10 wt.%) stealth system could be optimized by enabling the material to ab-
upon the microwave absorbing properties of single- and multi- sorb radiation without significantly increasing the emissivity.
layer epoxy-based composites with film thicknesses of 1, 2, and
3 mm in the frequency range of 8.0–12.0 GHz.[79] As a result, a
maximum RL of –32.1 GHz was obtained in the frequency range 5.2. Carbon Fibers (CFs)
of 8.2-8.8 GHz with a 3-mm thick multi-layer sample contain-
ing 10 wt.% CB. The authors concluded that a higher content of Carbon fibers (CFs) consist of carbon atoms linked in long,
CB per unit volume enables the attenuation of electromagnetic thin filaments with diameters in the range of micrometers.

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Since the 1960s, CFs have been recognized as the most impor- obtain excellent microwave absorbing properties. In addition, the
tant industrial materials in science and technology.[81] They are CFs can be shaped or arranged to further enhance the electro-
the preferred material for fiber-reinforced composites (FRPs) magnetic absorption.
in a wide range of fields, including the automotive industry,
mechanical engineering, civil construction, aviation, aerospace,
and offshore applications, due to their outstanding properties, 5.3. Carbon Nanotubes (CNTs)
such as high specific strength and stiffness, performance-to-
weight ratio, electrical conductivity, thermal stability, and corro- Carbon nanotubes (CNTs) are 1D nano-scale materials that can
sion resistance.[82,83] Most importantly, the use of CFs allows a re- be categorized as either amorphous or crystalline on the basis
duction in the weight of the product or equipment due to its high of their structures. Many previous studies have demonstrated
strength to weight ratio. Due to these properties, CFs are widely that CNTs are 100 times stronger than steel, and one-sixth as
used in many applications, including electromagnetic absorber dense.[91–94] In addition, the CNTs have higher thermal conduc-
materials.[84,85] In this regard, a significant amount of work has tivities of ≈2000–6000 W m−1 K−1 , while their electrical con-
been performed on CF-reinforced polymer composites (CFRPs) ductivities are much higher than that of copper.[95–97] These ad-
and CF/magnetic nanoparticles. vantages will become the key to multi-walled carbon nanotubes
For example, Zhao et al. studied the microwave absorbing (MWCNTs) and single-walled carbon nanotubes (SWCNTs) in
properties of composites containing inductive activated carbon the field of RAMs.[98–103] This section covers some examples of
fiber felt screens (IACFFSs) and vertically-arranged carbon fibers CNT-based RAMs as composites, metal-filled or magnetically
(VACFs).[86] As shown in Figure 8a, a block design method was coated CNTs, core-shell CNTs, and CNT/bimetallic metals.
applied to fabricate the composites with enhanced RAM perfor- Zhao et al. investigated the effects of Co-filled CNTs (10 and
mances. In this approach, the spacing between the adjacent fibers 20 wt.%) upon the microwave absorbing properties of epoxy-
is important for the microwave absorbing properties of the com- based composites with thicknesses of 2.22–2.26 mm in the fre-
posite, giving a maximum RL of –30.0 dB in the frequency range quency range of 2.0–12.0 GHz.[104] The results in Figure 9a re-
of 11.8–18.0 GHz when the interval between strips, the width of vealed that the optimum content of Co-filled CNTs was 20 wt.%,
the strips, and the fiber space are 5, 8, and 10 mm, respectively. giving a maximum RL of –21.8 dB at 12.2 GHz. In addition, the
In addition, Ling et al. prepared linear low-density polyethylene effects of various contents (10 and 20 wt.%) of Ag-filled CNTs
(LLDPE)/ethylene-octene copolymer composites filled with short upon the epoxy-based composites were examined, giving a maxi-
CFs via melt blending. The optimum content of short CFs was mum RL of –19.2 dB at 7.8 GHz with 10 wt.% Ag-filled CNTs and
found to be 30 wt.%, giving maximum RL values of –15.6 dB at a sample thickness of 1.0 mm.[105] In a similar study, Zou et al.
4.6 GHz and –17.4 dB at 16.4 GHz.[87] Meanwhile, Ye et al. inves- studied the effect of different contents (5 and 10 wt.%) of Ni-filled
tigated the effects of coating the CFs with various concentrations CNTs in the epoxy-based composites.[106] They concluded that the
of magnetic FeCoNi particles, and reported a maximum RL of incorporation of Ni-filled CNTs at 10 wt.% significantly enhanced
–30.6 dB at 11.7 GHz, with an effective bandwidth of 7.4 GHz the microwave absorbing properties of epoxy-based composites,
(from 8.7 to 16.1 GHz) due to the dielectric loss from the mag- which the RL less than –23.1 dB could be obtained in the fre-
netic particles.[88] In addition, Quan et al. presented the in situ quency range of 4.6 GHz from the samples at 2.0 mm of thick-
horizontal growth of Co3 O4 nanoparticles embedded in an N- ness.
doped carbon array on the surface of the CFs in carbon paper The coating of magnetic metals onto the CNT surface is widely
to fabricate low-thickness RAMs (NC-Co3 O4 /CP) (Figure 8b).[89] used in stealth technology due to the enhancement in the mi-
Here, maximum RL values of –16.1 and –34.3 dB were achieved crowave absorbing properties.[107–110] For example, Li et al. pre-
at thicknesses of 1.1 and 1.5 mm, respectively. The authors at- pared Fe3 O4 -coated CNTs to achieve a maximum RL of –43.0 dB
tributed the enhanced microwave absorbing properties of these and an effective frequency bandwidth of up to 8.5 GHz with a
RAMs to the internal reflections due to dielectric and magnetic sample thickness of 1.5 mm (Figure 9b).[111] In addition, the au-
losses, the shortened impedance matching gap, the dipolar polar- thors reported that a high surface area in the Fe3 O4 -coated CNTs
ization, and the thickness effect. Moreover, Chen et al. reported provides more active sites than the bare CNTs for dissipating
the successful fabrication of FeCo/CoFe2 O4 /CF hybrid compos- and scattering microwaves. Consequently, the composites with
ites via an electrospinning method to obtain a significant mi- the magnetic particle-coated structures are ideal for achieving a
crowave absorbing performance, with a maximum RL of –52.3 dB high microwave absorption performance due to the high inci-
at 5.0 GHz at a sample thickness of only 1.95 mm (Figure 8c).[90] dence probability and multiple reflection and absorption of mi-
In addition, the RCS contribution of as-prepared composites for crowaves. Li et al. also deposited CoFe2O4 onto the surface of
EM waves can reach 34.5 dB m2 . The authors concluded that the CNTs to achieve a maximum RL of –30.7 dB and an effective fre-
EM wave attenuation originates from polarization loss and con- quency bandwidth of up to 12.9 GHz with a sample thickness of
ductivity loss of the carbon material itself as well as the magnetic 2.0 mm.[112] The authors concluded that the enhancement in the
loss of the magnetic metal particles. absorbing properties of the nanocomposite can be attributed to
In brief, a magnetic loss-based absorbent such as a magnetic the improved impedance matching and the synergetic effects of
metal or metal oxide can be combined with CFs to prepare low- the multiple dielectric and magnetic losses.
density composites with strong absorption properties. In this ap- Alternatively, due to their core-shell structures and large sur-
proach, a layer of magnetic powder is deposited on the surfaces face areas, the filling of CNTs with magnetic metals can prevent
of the CFs by chemical doping or surface modification in order to the metal nanoparticles from being oxidized and, thus, main-
enhance the magnetic permeability of the composites and, thus, tain better stability in practical applications.[113–115] For example,

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Figure 8. The microwave absorbing properties of CF-based RAMs: a) a cross section (left) and calculated RL curves (right) of a vertically-arranged carbon
fiber (VACF)/epoxy composite (Reproduced with permission.[86] Copyright 2006, Elsevier), b) the schematic fabrication (left) and calculated RL curves
(right) of NC-Co3 O4 /CF composites (Reproduced with permission.[89] Copyright 2018, ACS), and c) the calculated RL curves (left) and RCS simulated
curves (right) of the FeCo/CoFe2 O4 /CF composites (Reproduced with permission.[90] Copyright 2021, ACS).

Qi et al. prepared core/shell structured Fe/CNT nanohybrids via frequency range of 2.0–18.0 GHz. In addition, Wu et al. prepared
a chemical vapor deposition (CVD) method, to obtain a maxi- a high-performance microwave absorbent by dispersing a consid-
mum RL of –40.2 dB at 17.1 GHz with a sample thickness of erable amount of Co magnetic nanoparticles within a dandelion-
1.5 mm.[116] Due to the high attenuation constant and good com- like CNT assembly, as shown schematically in Figure 9c.[117] Due
plementarity between the dielectric and magnetic losses, an ex- to the decent dispersion and controlled spatial distribution of
cellent microwave absorption performance was obtained in the the Co magnetic nanoparticles inside the CNTs, the composite

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Figure 9. The microwave absorbing properties of CNT-based RAMs: a) the calculated RL curves of pristine and Co-filled CNTs (Reproduced with
permission.[104] Copyright 2010, Elsevier), b) the calculated RL curves (top) and microwave absorbing mechanism (bottom) of magnetic Fe3 O4 -coated
CNTs (Reproduced with permission.[111] Copyright 2017, ACS), and c) the schematic preparation of core-shell (Co/CNT) composites (left) and the
calculated RL curves (right) (Reproduced with permission.[117] Copyright 2020. RSC).

achieved its full potential for microwave absorption, with an RL chemical compositions, densities, and lengths of CNTs were
of –52.9 dB at 9.3 GHz at a sample thickness of 2.4 mm. In detail, prepared with various Ni2+ /Co2+ ratios of 4:0, 3:1, 2:2, and 1:3,
the in situ electric holography and simulation results indicated to find that the composite with the 2:2 ratio exhibited an RL
that the dispersion of the Co nanoparticles at narrow intervals of −58.8 dB at 14.0 GHz with a sample thickness of 2.6 mm.
provided a high magnetic loss capacity due to their dynamic cou- The mechanisms behind the outstanding microwave absorbing
pling network. properties of these NiCo/carbon nanorod@CNT composites are
In recent years, CNT/bimetallic metals have gained shown schematically in Figure 10b. Thus, the porous structure
widespread attention in the design of microwave absorbing of the NiCo/carbon nanorod@CNT composite facilitates mul-
materials.[110,118–120] For example, Xu et al. reported the in situ tiple reflections and scattering of the electromagnetic waves,
growing CNTs on the prismatic nickel-cobalt (NiCo) clusters thereby extending the propagation pathway and enhancing the
derived from Ni-Co layered double hydroxides (NiCo-LDH) via electromagnetic energy attenuation. In addition, the higher
catalytic carbonization of ethyl acetate.[121] The maximum RL aspect ratio of the carbon nanorods generates conductive losses,
of the NiCo/CNT composite was –46.2 dB and the effective while the larger coating density of CNTs provides multiple
absorption bandwidth was 5.8 GHz, with a sample thickness polarization relaxation processes such as dipole polarization
of only 1.5 mm (Figure 10a). In addition, the RCS values of due to the residual oxygen-containing functional groups (C-OH
NiCo/CNT composites with metal plate are almost lower than and –C(═O)OH), thus further attenuating the electromagnetic
–20 dB m2 in the whole range and the RCS reduction can reach energy. Finally, the bimetallic NiCo causes natural and exchange
27.5 dB m2 . Similarly, Wang et al. reported on the fabrication resonances, which also play effective roles in electromagnetic
of hierarchical NiCo/carbon nanorod@CNT structures via a wave dissipation. Meanwhile, Shu et al. reported the successful
carbonization process under an argon (Ar) flow by using Ni-Co- fabrication of 3D net-like ZnFe2 O4 /CNT hybrid composites via
MOF-75 nanorods as precursors.[122] Composites with various a facile one-step solvothermal method to obtain a significant

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Figure 10. The microwave absorbing properties of CNT/bimetallic metal RAMs: a) the calculated RL curves (left) and RCS simulated curves (right)
of the NiCo/CNT composites (Reproduced with permission.[121] Copyright 2023, Elsevier), b) a schematic representation of the microwave absorbing
mechanism (top) and the calculated RL curves (bottom) of NiCo/carbon nanorod@CNT composites (Reproduced with permission.[122] Copyright 2019,
ACS), and c) the calculated RL curves (top) and absorbing mechanism (bottom) of ZnFe2 O4 /CNT hybrid composites (Reproduced with permission.[123]
Copyright 2018, Elsevier).

microwave absorbing performance, with a maximum RL of microwave absorption. These advantages will become the key to
–55.5 dB at 13.4 GHz at a sample thickness of only 1.5 mm the use of CNTs in the field of stealth technology.
(Figure 10c).[123] The authors demonstrated that the hybridiza-
tion of magnetic ZnFe2 O4 microspheres with dielectric CNTs
influenced both the dielectric and magnetic losses, which de- 5.4. Graphite
termine the impedance matching and electromagnetic wave
attenuation. First, the abundant defects and oxygen-containing Graphite is a 3D carbon structure with high conductivity, easy
functional groups provide a significant quantity of dipoles, production, low cost, and high stability. These properties have
which generate polarization relaxation loss in the incident led to numerous investigations on the application of graphite
electromagnetic waves. Second, the magnetic microspheres act in RAMs. For example, Ismail et al. synthesized single and
as bridges for electron-hopping between neighboring CNTs, as double-layer doped CoFe2 O4 /graphite composites, and charac-
well as generating the magnetic loss via the eddy current loss terized their electromagnetic performances in the frequency
and natural resonance. Finally, the multiple reflection in the 3D range of 8.0–18.0 GHz.[124] The CoO and FeO2 O3 precursors
conductive network, and multiple scattering among the inter- were mechanically alloyed and sintered at 800, 900, 1000, and
faces, also play considerable roles in the electromagnetic wave 1100 °C in order to synthesise various particle sizes and shapes.
attenuation. The as-prepared double-layer composites revealed significant
In summary, the CNTs with multifunctional properties have microwave absorbing performances, with a maximum RL of
become highly favored among researchers. Consequently, CNTs –15.0 dB at 10.3 GHz at a sample thickness of 2.0 mm. Mean-
and CNT-based composites remain much more attractive than while, Rusly et al. studied the microwave absortion properties
other materials for the fabrication of efficient RAMs. The high of single- and double-layer doped SrCoZnFe16 O27 /graphite
specific surface area and high aspect ratio can be very beneficial to nanocomposites in the frequency range of 8.0–18.0 GHz.[125]
the attenuation of microwaves. In addition, the outstanding elec- Here, the SrCoZnFe16 O27 nanoparticles were prepared via
trical conductivities of the CNTs in the large-scale composite can solid-state reaction using high-energy ball milling, and then
translate into significant conduction-driven losses for enhanced sintered at various temperatures (800–1100 °C). As a result,

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Figure 11. The microwave absorbing properties of graphite-based RAMs: a) the calculated RL curves (left) and absorption mechanism (right) of
SrCoZnFe16 O27 /graphite nanocomposites (Reproduced with permission.[125] Copyright 2018, Springer), and b) the schematic synthesis (left) and mi-
crowave absorption mechanism (right) of graphite nanosheets decorated with core-shell Fe3 O4 @PPy hybrids (Reproduced with permission.[130] Copy-
right 2019, Elsevier).

the double-layer material consisting of SrCoZnFe16 O27 as the scattering and interfacial polarization, along with the improve-
absorbing layer and graphite as the matching layer provided a ment in the electromagnetic impedance matching of the graphite
high RL of –19.5 dB at 12.8 GHz with a matching-layer thickness nanoflakes.[131] The typical carbonaceous material graphite is
of 1.0 mm (Figure 11a). The authors attributed this result to considered as one of the most important simple substances, with
the combined effects of material losses and multiple internal wide availability in nature. Currently, the graphite is still a hot
reflections at the boundaries. spot in the field of RAMs where the modification of graphite flake
Graphite materials derived from graphite flakes have also been is mainly studied at home and abroad, which nano-scale graphite
used in RAMs.[126–129] For example, Su et al. reported the study and then prepares high-performance RAMs in combination with
of a RAM-based on graphite nanosheets decorated with core- other kinds of absorbers.
shell Fe3 O4 @PPy hybrids, as shown in Figure 11b.[130] The as-
prepared composites exhibited a maximum RL of –49.3 dB at
9.9 GHz at a sample thickness of 2.0 mm. Here, the com- 5.5. Graphene
bined effects of dielectric and magnetic losses could result in en-
hanced impedance matching, while the introduction of graphite Graphene is a carbon-based material with a variety of extraor-
nanosheets generated more interfaces, thereby increasing the dinary properties such as an interconnected porous structure,
interfacial polarization and extending the pathways of the elec- a large specific surface area, good thermal conductivity, strong
tromagnetic waves via multiple reflections. Similarly, Zhong et chemical resistance, and outstanding electrical conductivity due
al. fabricated a hexagonal boron nitride nanocrystal/graphite to its unique band structure.[132,133] Graphene-based materials
nanoflake composite via the wet-chemistry coating of graphite can solve electromagnetic wave problems with great efficiency,
nanoflakes to achieve a remarkable enhancement in the mi- and their microwave absorbing properties give them outstand-
crowave absorption properties due to the increases in multiple ing potential in the field of RAMs.[134–136] This section covers

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some examples of graphene-based RAMs as composites, mono- cles on graphene is a very promising approach to the design of
lithic 3D graphene, graphene/dielectric heterostructures, and lightweight and high-efficiency RAMs. Meanwhile, Li et al. fab-
graphene/dielectric multi-heterostructures. ricated CoFe2 O4 /graphene oxide hybrid composites via a facile
Although the unique structure of 2D graphene provides a one-pot polyol route, and then chemically converted them un-
number of excellent electrical properties, the most challenging der H2 /NH3 atmosphere into FeCo/graphene hybrid composites
issue is that of maintaining these properties at the macroscopic with enhanced attenuation ability for electromagnetic waves in
scale. This is mainly hindered by the restacking of the graphene, frequency range of 2.0–18.0 GHz (Figure 12b).[140] As a result,
which leads to destructive aggregation, such that the desired the maximum RL of the FeCo/graphene composite was −40.2 dB
properties cannot be completely realized. Recently, considerable at 8.9 GHz with a matching layer thickness of only 2.5 mm. They
progress has been made toward the fabrication of monolithic concluded that the FeCo/graphene composites exhibited signifi-
3D interconnected graphenes while maintaining the outstand- cant microwave absorbing performance enhancement due to re-
ing properties of single-layer graphene as well as exhibiting sev- markable complex permeability from FeCo nanocrystals and per-
eral unique properties. For example, Zhang et al. studied the mi- mittivity from graphene. In addition, the metallic nature of the
crowave absorbing properties of monolithic 3D graphene foam FeCo alloy may also contribute to the enhanced permittivity of
(GF) in the frequency range of 2.0–18.0 GHz.[137] Here, the the FeCo/graphene composites. In addition, Cao et al. reported
GF obtained from graphene oxide (GO) solution was divided the N-doping graphene/Fe3 O4 composites was prepared by a sim-
into five small batches, four of which were annealed at 200, ple hydrothermal method, where GO was reduced into rGO,
400, 600, or 800 °C. Thus, the optimal annealing temperature along with the formation of Fe3 O4 nanoparticles.[141] As shown
was found to be 600 °C, giving a maximum RL of –34.0 dB in Figure 12c, the as-prepared GFe composite provided a maxi-
at 13.1 GHz with a sample thickness of 10.0 mm. The depen- mum RL of –59.0 dB in the frequency range 0–4.14 GHz with a
dance of the microwave absorption performance upon the mono- thickness of 1.17 mm. The authors concluded that the benefiting
lithic 3D structure revealed that the GF with a suitable chem- from the synergy between the dielectric genes and the magnetic
ical composition and physical structure provides a balance be- medium to the enhancement in microwave absorbing properties.
tween excellent impedance matching and a high loss character- To further increase the tunability of the microwave absorb-
istic. Meanwhile, Shang et al. reported that the large-scale fab- ing performance, the construction of graphene/dielectric multi-
rication of 3D graphene-like networks (3D-GLNs) with hierar- heterostructures has been a widely adopted strategy.[129] For ex-
chical porous structures by employing an ion-exchange resin as ample, Du et al. studied the microwave absorbing properties
a carbon precursor.[138] The microwave absorbing properties of of FeCo/graphene composites in the frequency range of 2.0–
the Fe3 O4 -loaded 3D-GLNs were investigated in the frequency 18.0 GHz.[142] The results in Figure 13a revealed that the op-
range of 2.0–18.0 GHz to reveal a maximum RL of –46.8 dB at timum content of FeCo-filled graphene was 20 wt.%, giving a
11.8 GHz with a sample thickness of only 3.0 mm (Figure 12a). maximum RL of –71.63 dB at 10.8 GHz ith a sample thick-
This excellent microwave absorbing performance can primarily ness of 2.68 mm. In addition, the RCS of FeCO/graphene
be attributed to the hierarchical structure of the 3D-GLN/Fe3 O4 composite is less than –10 dB m2 , which provides evidence
composite. First, the 3D network of graphene-like pore walls pro- that the samples have good radar wave attenuation capabili-
vided a certain resistance, which generated induction currents ties when the scattering angle is between 0 and 60°. In ad-
upon electromagnetic incidence, thereby attenuating and trans- dition, Liu et al. investigated the effect of CuS and NiFe2 O4 -
forming the electromagnetic wave energy into thermal energy. filled graphene upon the microwave absorbing properties of
Second, the defects and functional groups of the 3D-GLN not graphene-based composites in the frequency range of 2.0–
only enhanced the impedance matching, but also introduced 18.0 GHz.[143] As shown in Figure 13b, the as-prepared com-
electronic dipole polarization relaxation, defect polarization relax- posites exhibited a maximum RL of –54.5 dB at 11.4 GHz
ation, and a reduction in the Fermi level, all of which contributed with a layer thickness of 2.5 mm. The authors suggested that
to electromagnetic wave penetration and absorption. Finally, the the introduction of magnetic particles into the graphene sheets
introduction of Fe3 O4 particles could induce considerable inter- and CuS nanoflakes played an important role in increasing
facial polarization losses, which originated from the interfaces the microwave absorbing properties, not only providing bet-
between the Fe3 O4 and graphene-like walls. ter impedance matching, but also strengthening the ion polar-
Typically, the development of graphene/magnetic hybrids is ization, dipole polarization, and interfacial polarization. Mean-
a more direct strategy than the above-mentioned method be- while, Manna et al. reported the fabrication of a graphene/iron
cause it directly affects the RL values of the composites. For (II/III) oxide/polyaniline (graphene/Fe3 O4 /PANI) composite via
instance, Wang et al. used the atomic layer deposition (ALD) a hydrothermal method.[144] As shown in Figure 13c, the as-
method to fabricate graphene/Fe3 O4 and graphene/Ni hybrid prepared composite provided a maximum RL of −64.0 dB in
RAMs.[139] The results indicated that the graphene/Fe3 O4 com- the frequency range 2.0–8.0 GHz with a thickness of 0.45 mm.
posite fabricated by the application of 100 cycles of Fe2 O3 de- This outstanding response was attributed to the good impedance
position followed by hydrogen reduction provided an optimal matching between permittivity and permeability values, as
RL of –46.4 dB at 15.6 GHz with a sample thickness of only well as magnetic and dielectric losses. Moreover, the high RL
1.4 mm. This enhancement in absorption performance can be of the graphene/Fe3 O4 /PANI composite suggested the pres-
attributed to the effective impedance matching, increased mag- ence of more interfacial polarization, relaxations, and multiple
netic loss, and multiple interfacial polarization due to the addi- reflections.
tion of magnetic constituents. The authors concluded that the The graphene-based RAMs have demonstrated their capa-
ALD-based nano-scale surface modification of magnetic parti- bilities for high microwave absorbing performance due to

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Figure 12. The microwave absorbing properties of graphene-based RAMs: a) the calculated RL curves (left) and microwave absorbing mechanism (right)
of the 3D-GLN/Fe3 O4 composites (Reproduced with permission.[138] Copyright 2021, MDPI), b) the schematic synthesis (left) and calculated RL values
(right) of FeCo/graphene composites (Reproduced with permission.[140] Copyright 2015, RSC), and c) the microstructure (left) and calculated RL values
(right) of N-doping graphene/Fe3 O4 composites (Reproduced with permission.[141] Copyright 2021, Wiley).

the hierachical structure and distinctive electrical properties 5.6. MXene


of graphene and other components. These two properties en-
dow the graphene-based composites with the greatest poten- To further enhance the electromagnetic wave absorption capac-
tial to achieve high-performance RAMs. Thus, graphene offers ity and construct an efficient RAM, researchers have explored
great opportunities for further enhancing the performance of the use of new materials such as the family of 2D structures
RAMs. known as the MXenes, which were discovered by Yury Gogotsi

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Figure 13. The microwave absorbing properties of graphene/dielectric multi-heterostructure RAMs: a) the calculated RL curves (left) and RCS simulated
curves (right) of the FeCO/graphene composites (Reproduced with permission.[142] Copyright 2022, ACS), b) schematic representation of the microwave
absorbing mechanism for magnetically decorated graphene/CuS composites (Reproduced with permission.[143] Copyright 2016, ACS), and c) calculated
RL curves and absorbing mechanism of the graphene/Fe3 O4 /PANI composites (Reproduced with permission.[144] Copyright 2021, ACS).

in 2011.[145] These have the general formula Ti3 C2 Tx , where Tx ture via the treatment of Ti3 AlC2 powders in hydrogen fluoride
represents an abundant fuctional group such as OH, O, and F, (HF) and subsequent ultrasonication, and investigated their elec-
and are considered to be hugely promisng materials for RAMs tromagnetic wave absorptions in the frequency range of 12.4–
due to their accordion-like structures, surface defects, and plen- 18.0 GHz.[156] The results indicated a maximum RL of –17.0 dB at
tiful surface termination groups. Due to its unique layered struc- 14.6 GHz with a matching layer thickness of 1.4 mm, which was
ture, hydrophilic surface, high conductivity and good mechan- mainly attributed to the proper matching of the electromagnetic
ical properties, MXene is widely applied in catalysts,[146–148] en- impedances and suitable dielectric losses. In addition, the high
ergy storage,[149,150] optics,[151,152] desalination,[153] film,[154] and specific surface area and low thicknesses of the Ti3 C2 nanosheets
other fields in addition to RAMs. This section covers some ex- also enhanced the propagation pathway of the incident wave in-
amples of MXene-based RAMs as composites, pure MXene, MX- side the sample. Meanwhile, Zhang et al. investigated the rein-
ene/dielectric materials, MXene/magnetic materials and MX- forcing effects of Ti3 C2 Tx upon the microwave absorbing proper-
ene/multiple loss materials. ties of paraffin-based composites in the frequency range of 2.0–
For example, Ting et al. prepared MXene nanosheets to achieve 18.0 GHz.[157] The composites were prepared by adding 40, 50,
a maximum RL of −54.8 dB and an effective frequency band- and 60% Ti3 C2 Tx into a paraffin matrix with thicknesses of be-
width of up to 3.0 GHz with a sample thickness of 2.0 mm tween 1.4 and 2.8 mm. The results indicated a maximum RL of
(Figure 14a).[155] In addition, the cartesian plot of RCS values –34.4 dB at 12.0 GHz with a thickness of 1.7 mm (Figure 14b).
that good microwave absorbing performance is exhibited over The authors concluded that the high dielectric loss and multiple
a wide range of incident angles ranging from –90° to 90°. The reflections between the Ti3 C2 Tx layers contributed greatly to the
authors demonstrated that the MXene nanosheets to tune their enhancement in microwave absorbing properties.
EM response properties, a multifunctional MXene which can The microwave absorbing performances of the MXenes can
serve EM wave absorption and shielding performance. Qing be further enhanced via integration with other dielectric loss
et al. prepared Ti3 C2 nanosheets with a typical MXene struc- materials such as carbon-based materials. For example, Li et

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Figure 14. The microwave absorbing properties of MXene-based RAMs: a) the calculated RL curves (left) and RCS simulated curves (right) of the MXene
nanosheets (Reproduced with permission.[155] Copyright 2023, Elsevie), b) the calculated RL curves of various MXenes (Reproduced with permission.[157]
Copyright 2020, IOPscience), c) a schematic illustration of the possible mechanisms of electromagnetic wave absorption in CNT/MXene composites
(Reproduced with permission.[158] Copyright 2017, RSC), d) the calculated RL curves (left) and computational micromagnetic simulation (right) of
MXene/Fe3 O4 composites (Reproduced with permission.[160] Copyright 2020, AC), and e) a schematic diagram of preparation of RGO/MXene/Fe3 O4
microspheres (Reproduced with permission.[161] Copyright 2021, Elsevier).

al. reported the in situ growth of carbon nanotubes (CNTs) on stance, Liang et al. reported the in situ growth of uniform and
MXenes via a simple catalytic CVD process.[158] The resulting size-controllable Ni nanoparticles on the surface of MXenes via
hierarchical CNT/MXene sandwich structure exhibited outstand- a novel, facile, and moderate co-solvothermal method.[159] The
ing microwave absorbing performance (RL max = –52.9 dB at optimum Ni content was found to be 10 wt.%, giving a maxi-
7.15 GHz) in the 2.0–18.0 GHz frequency range with a low mum RL of –52.6 dB in the frequency range of 8.4 GHz with
CNT loading of only 35 wt.% and a thickness of only 1.55 mm. a sample thickness of 3.0 mm. In addition, Li et al. reported the
As shown in Figure 14c, the CNTs were uniformly distributed study of a simple spray-drying routine to reshape the MXene into
on the surface of the MXene flakes, bridging the gap between a confined and magnetized microsphere with tightly embedded
various MXene particles to form the overall network. The authors Fe3 O4 nanospheres, contributing to the enhanced specific inter-
reported that this bridging effect provided high conductivity, faces and strong dielectric polarization.[160] The maximum RL of
along with a decrease in the number of surface functional the MXene/Fe3 O4 composite was –50.6 dB and the effective ab-
groups, thereby creating more conductive pathways for charge sorption bandwidth was 4.6 GHz, with a sample thickness of only
carriers and enhancing the conductivity loss. 2 mm (Figure 14d). The authors concluded that the above result
Some examples of magnetic loss materials that have been in- can be attributed to the advantages of the specially designed ar-
troduced into MXenes include magnetic metals (Fe, Co, Ni), their chitecture, especially the synergetic effect between the magnetic
alloys, and their metal oxides. The high permeability of the mag- units (Fe3 O4 ) and the dielectric framework (MXene).
netic loss material enhances the impedance matching, which The multi-components in the MXene-based composites can
is beneficial for the microwave absorbing performance. For in- introduce excellent impedance matching degree and interfacial

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Table 2. A summary of Carbon-based RAMs.

Carbon-based RAMs Features Limitations

Carbon blacks - Low cost - Difficult to dispersion in matrix


- Simple substances - Low microwave absorbing performance
- Easy to single-layer and multi-layer structures - Complex and difficult for optimization process
- Uniform particles
Carbon fibers - Easy to single-layer and multi-layer structures - Difficult to dry
- Moderate microwave absorbing performance - High cost
- Difficult to use for large-scale
Carbon nanotubes - High microwave absorbing performance - High cost
- High electrical conductivity - Difficult to use for large-scale
- Requires a deep understanding of the interface of multiple structures
Graphite - Low cost - Possibility of decomposition and mass loss
- Excellent stability - Low microwave absorbing performance
- Easy to use for large-scale
Graphene - High microwave absorbing performance - High cost
- High electrical conductivity - Harmful chemicals
- Easy to single-layer and multi-layer structures - Cost for refining
- large specific surface area - Difficult to use for large-scale
MXene - High microwave absorbing performance - High cost
- Easy to single-layer and multi-layer structures - Difficult to use for large-scale
- Excellent dielectric properties - Cost for refining
- High electrical conductivity - Complex and difficult for optimization process

polarization, and the morphology also has an important influ- isolation for the protection of product or equipment, subjects of
ence on microwave absorbing performance. For example, Cui interest in the civil and military surveillance fields (Figure 15).
et al. successfully fabricated 3D pleated RGO/MXene/Fe3 O4 mi- In this review, the recent progress in the uses of these carbon-
crospheres via a simple and rapid ultrasonic spray techonogy to based materials for RAMs were comprehensively reviewed. The
achieve a maximum RL of –51.2 dB at 11.1 GHz with a thickness underlying theories of the radar system, the attenuation of elec-
of 2.9 mm (Figure 14e).[161] The synergistic effects between the di- tromagnetic waves, the radar cross section, and radar absorb-
electric elements (RGO, MXene) and magnetic element (Fe3 O4 ) ing material were described. Then, the most recent advances in,
resulted in good impedance matching and enhanced microwave and responses of, each type of material and its composites were
absorbing properties within the composites. At the same time, listed, along with the effects of their fabrication and formation
the increase in the pore size was conducive to the entry of elec- processes, functionalization, and number and thickness of layers
tromagnetic waves, thereby increasing the probability of electro- upon the electromagnetic attenuation. In addition, the various
magnetic wave reflection loss in the material pores. microwave attenuation mechanisms, such as absorption, dielec-
The MXenes are novel 2D materials with many advantages for tric loss, magnetic loss, multiple reflection and scattering, dipole
use as RAMs, including unique layered structures, high electri- and/or interfacial polarization, and relaxation effects, were dis-
cal conductivities, and high specific surface areas. The synergistic cussed and related to the composition and structure of each ma-
effects between MXenes and the added dielectric or magnetic ma- terial, and to its overall attenuation performance. Thus, strategies
terials result in additional loss mechanisms, which can improve for using various types of metallic or magnetic particles and/or
microwave absorbing performance. As with graphene, MXenes conductive polymers to enhance the microwave absorption prop-
can be ideal substrates for coupling with other loss materials to erties via electric and/or magnetic losses were discussed. In par-
further enhance microwave absorbing performance. Thus, the ticular, the synergies among the various components of the com-
MXenes have wide application prospects in the field of RAMs. posite materials were shown to enable the tailoring of the per-
mittivity/permeability values, as well as the impedance matching
6. Summary and the Perspectives and electromagnetic absorption.
Different strategies for enhancing the microwave absorption
With the increasing interest on stealth materials and tech- properties with magnetic loss using different types of metallic
nologies, the carbon-based materials, such as carbon blacks, or magnetic particles, as well as conductive polymers have
carbon fibers, carbon nanotubes, graphite, and graphene, are been listed. In addition, the synergies within components that
great promising candidates for various radar absorbing materi- allowed tailoring the permittivity/permeability values, as well as
als (RAM) applications as a result of their extremely large specific the impedance matching and then the electromagnetic absorp-
surface area, low density, excellent dielectric properties, high elec- tion, was emphasized. The role of the composition and structure
trical conductivity, and excellent stability under harsh conditions of the carbon-based materials that lead to different microwave
(Table 2). absorbing mechanisms, such as absorption, dielectric loss,
The application of these RAMs could range from the reduction magnetic loss, multiple reflection and scattering microwaves,
of the radar cross section of the targets, protection and isolation besides dipole or interfacial polarization and relaxation effects,
of personnel exposed to electromagnetic waves, electromagnetic was related to the microwave absorbing performance of the

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Figure 15. Summary of electromagnetic applications according to carbon-based materials.

carbon-based materials. Based on these recent advances and scale fabrication can limit the modularization of these RAMs.
representative results, the following conclusions and trends for Hence, these aspects also need to be considered in order to
future developments can be noted: achieve a better microwave absorbing performance.
4) With the development of national defense and the rise
1) Although the excellent electrical conductivities and large sur- of environmental problems, the use of lightweight materi-
face areas of the carbon-based materials make them promis- als is becoming increasingly popular. In this respect, the
ing candidates for RAMs, the 3D carbon networks are pre- lightweight natures of the carbon-based materials ensure a
ferred over the 0D, 1D, and 2D carbon networks. This is be- balance between stealth and modularization. Nevertheless,
cause the multiple reflections in the 3D carbon network, along while carbon-based RAMs are being prepared at the present
with multiple scattering among the numerous interfaces, play time, their high preparation costs remain an important obsta-
considerable roles in enhancing the electromagnetic wave at- cle that limits their application. This requires expertise from
tenuation. Moreover, the optimal microwave absorption per- multiple teams and thus needs proper coordination among
formance depends on the physical structure of the 3D car- multi-disciplinary researchers (material science, nanotech-
bon network, which can provide a balance between excellent nology, and chemical engineering) and industrialists. The so-
impedance matching and high loss characteristics to deliver lution to this problem requires expertise from multiple teams
excellent microwave absorbing properties. and proper coordination between industrialists and multi-
2) The microwave absorbing performances of multi-layer struc- disciplinary researchers in fields such as materials science,
tured materials can be limited by disadvantages such as un- nanotechnology, and chemical engineering.
even material cross sections or surfaces, non-uniform parti-
cle sizes or dispersions, and incompatibilities between the To summarize, the past years have witnessed outstanding ad-
various layers. Hence, various fabrication strategies such as vancements in stealth materials and technologies, which have
chemical vapor deposition, magnetron sputtering, or atomic built a firm foundation. Consequently, the carbon-based RAMs
layer deposition have been explored, along with the genera- have become a topic of interest for future development and prac-
tion of core-shell structures, block structures, or foams via tical application via well-established or novel materials. Carbon-
wet-chemistry (e.g., hydrothermal or solvothermal) coating, based RAMs will play an increasingly important role in many
with some success. fields in the future. They have great potential for development
3) At present, the majority of reports have focused on the nano- in areas such as electronic device, artificial intelligence, and mil-
or micro-structure design of RAMs, which has proven to be itary industries. Carbon-based RAMs, as the newest and fastest
effective in considerably enhancing the attenuation of elec- growing, will open new avenues for realizing various classes of
tromagnetic waves. However, the lack of technology for large- electromagnetic protection devices.

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Seong-Hwang Kim joined as a Ph.D. student in Prof. Soo-Jin Park’s group at Inha University since
2018, where he is currently working on interfacial chemistry of the hybrid composites materials includ-
ing carbon and ceramic materials.

Seul-Yi Lee received her Ph.D. degree in the Department of Chemistry from Inha University, South
Korea (2013) where her research topics included the synthesis and characterization of carbonaceous
nanomaterials. She then joined as a research associate at the Institute for Critical Technology and Ap-
plied Science (ICTAS) and the Department of Mechanical Engineering at Virginia Tech (2014–2021).
She is now working as a research scientist in the Department of Chemistry at Inha University. Her cur-
rent research interests focus on hybrid composites toward meeting the grand challenges in the areas
of energy and sustainability for the future.

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Yali Zhang obtained her Bachelor degree from Northwestern Polytechnical University in 2019. Cur-
rently she is a Ph.D. candidate majoring in chemistry at Northwestern Polytechnical University. Her
research interests include microstructure design, performance regulation, and mechanism research
of MXenes-based electromagnetic interference shielding composite films.

Soo-Jin Park received his Ph.D. in materials chemistry from Institut de Chimie des Surfaces et Inter-
faces, CNRS, France (1992), under the supervision of Professor J. B. Donnet. He joined Korea Re-
search Institute of Chemical Technology (KRICT) as a principal research scientist, South Korea (1996).
Currently, he serves as a full professor in the Department of Chemistry at Inha University, since 2005.
His research has focused on the surfaces and interfaces of carbon, ceramic, polymer, and composite
materials. In particular, his group has worked on developing various nanoporous materials and their
composites for Energy, Electronics, and Environments.

Junwei Gu is a full professor and leader of the structure/function polymer composites group in the
School of Chemistry and Chemical Engineering at Northwestern Polytechnical University. He received
his Ph.D. degree of materials science from Northwestern Polytechnical University in 2010. His current
research focuses on the thermally conductive polymer composites, fibers/polymeric matrix wave-
transparent composite materials as well as electromagnetic interference shielding polymer compos-
ites.

Adv. Sci. 2023, 10, 2303104 2303104 (22 of 22) © 2023 The Authors. Advanced Science published by Wiley-VCH GmbH

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