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Mater. Res. Express 12 (2025)025305 https://doi.org/10.1088/2053-1591/adb2e0
PAPER
Fe
3
O
4
modified graphene epoxy composite materials via polyether
amine reduction with enhanced microwave absorption performance
Guangyuan Yang
1
, Jing Che
1
, Xiaokang Zhao
1
, Congxin Chen
1
, Sanwen Peng
1
, Heng Yang
2
and
Bin Zhang
2,3
1
China Tobacco Hubei Industrial Limited Liability Company, Wuhan, 430056, People’s Republic of China
2
School of Materials Science and Engineering, Wuhan Textile University, Wuhan, 430200, People’s Republic of China
3
School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430700, People’s Republic of China
E-mail: 13817345274@163.com (S Peng)and whutfrpzhangbin@163.com
Keywords: polyether amine reduced graphene oxide, polymer composites, impedance matching, microwave absorption performance
Abstract
The increasing complexity of electromagnetic environments demands the development of advanced
absorbers with superior performance. In this study, a novel magnetic Fe
3
O
4
-modified graphene-based
absorber (FARGO)is synthesized via an in situ reduction process using polyether amine. The resulting
FARGO composite exhibits excellent microwave absorption properties. When the filling content of
FARGO is 5 wt% in epoxy resin, the optimal reflection loss is −23.12 dB with a thickness of 4 mm and
a broad absorption bandwidth of 5.6 GHz can be achieved as the thickness changes to 2 mm. Polyether
amine efficiently reduces GO to rGO, significantly improving electrical conductivity. Simultaneously,
it grafts amine groups onto the graphene surface, enhancing dispersion and reactivity within the epoxy
resin matrix. These synergistic effects make it a promising candidate for high-performance microwave
absorbing materials.
1. Introduction
The rapid advancement of wireless communication and unmanned technologies has greatly improved our work
efficiency and everyday life. However, it has also led to increasingly severe electromagnetic pollution due to the
extensive use of wireless communication and detection devices. This pollution poses significant risks to human
health and the environment [1–3]. To address these challenges, microwave absorption materials (MAMs)with
low density, strong absorption capabilities, and minimal thickness have become a focal point of research in
recent years [4,5]. Among these, graphene-based MAMs have gained particular attention due to their unique
properties, such as high electrical conductivity, large specific surface area, and excellent mechanical strength
[6,7]. Nevertheless, the inherent large surface area and strong tendency of graphene to agglomerate significantly
limit its use and reduce its dispersion uniformity within matrices. This issue can be mitigated by incorporating
other organic functional groups or nanoparticles, which helps to improve the overall stability and dispersion of
graphene in the composite material [8,9]. Kowsari et al [10]have grafted imidazolium based dicationic ionic
liquid on the GO surface, which can effectively reduce the agglomeration of GO.
Designing effective MAMs requires overcoming several challenges, including achieving proper impedance
matching and incorporating multiple loss mechanisms to enhance microwave absorption [11]. Single-
component materials often fall short in these areas, as they typically suffer from poor impedance matching and
offer only a single loss source, which limits their absorption efficiency. On the other hand, hybrid composites,
which combine dielectric materials with magnetic materials in optimal ratios, can significantly improve
performance by leveraging multiple loss mechanisms, such as dielectric loss, magnetic loss, and interfacial
polarization [12,13]. This multifunctional approach enhances the material’s microwave absorption capabilities,
making hybrid composites a preferred choice in the development of advanced MAMs.
Graphene-based MAMs, modified with magnetic particles, have been extensively studied and shown to
deliver broadband absorption bandwidths and enhanced microwave absorption intensities [14,15]. These
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REVISED
31 December 2024
ACCEPTED FOR PUBLICATION
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PUBLISHED
18 February 2025
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modifications involve introducing magnetic nanoparticles such as iron oxides [16], cobalt [17], or nickel [18],
which contribute magnetic loss mechanisms to the composite. Cui et al [19]have reported single layer graphene
encapsulating FeCo alloy nanoparticles with strongest reflection loss value of −46 dB and excellent absorption
bandwidth covering the whole Ku-band. Sun et al [20]have synthesized NiCo
2
O
4
modified thermally reduced
graphene oxide three-dimensional composites at different calcination temperature, and the best absorption
bandwidth was 4.5 GHz obtained at 800 °C. Porous Graphene/Ni
0.5
Co
0.5
Fe
2
O
4
composite derived from
grapefruit peel was fabricated with adjustable carbonization temperature, and the optimal absorption
bandwidth was 5.14 GHz with a thin thickness of 1.7 mm [21]. The synergistic effect between graphene’s
dielectric properties and the magnetic characteristics of these particles enhances the overall electromagnetic
wave attenuation capability of the material.
However, the practical application of these materials is often limited by the type of matrix used. In many
research studies, paraffin is employed as the matrix due to its simplicity in thermal melting and mechanical
mixing processes. Although paraffin-based composites are convenient for laboratory experiments, they are not
suitable for real-world applications where more robust and durable materials are required. Polymer matrices are
preferred due to their superior mechanical properties, thermal stability, and ease of processing [22–25].
Nonetheless, increasing the loading of graphene-based MAMs in resin matrices presents its own set of
challenges, primarily related to maintaining good dispersion and achieving effective interaction between the
graphene and the resin matrix.
Based on the above analysis, this study aims to develop a high-performance microwave absorbing material
by employing alkaline polyetheramine to reduce GO and promote the uniform growth of Fe
3
O
4
nanoparticles
on graphene layers. Polyetheramine not only serves as a reducing agent for GO but also grafts amino groups onto
the graphene surface during the reduction process. This dual functionality significantly improves the dispersion
and reactivity of the composite within the epoxy resin, strengthening the interaction between the graphene-
based absorber and the resin matrix. Consequently, a Fe
3
O
4
modified polyether amine reduced graphene oxide
composite with excellent microwave absorption properties was successfully prepared, addressing the growing
demand for advanced materials in complex electromagnetic environments.
2. Experimental section
2.1. Synthesis of Fe
3
O
4
modified polyether amine reduced graphene oxide composite
GO was prepared by pressurized oxidation method [26]and dispersed in deionized water with a concentration
of 4 mg ml
−1
. With continuous vigorous mechanical stirring, 120 ml GO aqueous solution, 0.02 mol ferric
nitrate and 0.02 mol ferrous sulfate were mixed at 50 °C for 15 min. Then, 10 ml polyether amine
(D230, Aladdin, Co., Ltd)was slowly dropped into the mixture within 30 min and the pH value was adjusted to
11 with NaOH aqueous solution (1 mol/l). After 12 h reaction at 70 °C, black deposit was collected and washed
by deionized water, followed with vacuum drying procedure. Similar process was conducted to obtain polyether
amine modified reduced GO (ARGO)without the addition of ferrum source, so was the polyether amine
modified Fe
3
O
4
sample (AF). Finally, as-prepared FARGO was homogeneously mixed into epoxy resin
(Epikote 862, Hexion Inc.)with an addition amount of 1 wt%, 2 wt% and 5 wt%, marked as FARGO1, FARGO2
and FARGO3 respectively. Referring to our previous work [27], the maximum addition amount of pure rGO in
epoxy resin is about 1 wt%, which we use as the control group and name the absorption sample RGO. The
specific composition ratios are detailed in table 1. By reduction with polyether amine, the maximum amount of
FARGO that can currently be added is 5 wt% of the resin. This increase is likely ascribed to the amino segments
on the surface of FARGO improving fluidity and compatibility in resin. Scheme 1shows the fabrication
illustration of FARGO.
2.2. Characterization
Morphology and micro-structure of as-prepared FARGO was characterized by scanning electron microscope
(SEM, Zesis Sigma500 and Oxford X-MAX). The chemical composition, crystal structure and magnetic
Table 1. Sample ID and the
corresponding component content.
Sample ID Composition
RGO 1 wt% RGO in epoxy
FARGO1 1 wt% FARGO in epoxy
FARGO2 2 wt% FARGO in epoxy
FARGO3 5 wt% FARGO in epoxy
2
Mater. Res. Express 12 (2025)025305 G Yang et al
properties were conducted via Fourier Transform Infrared Spectroscopy (FTIR, Nicolet 6700), X-ray diffraction
(XRD, Bruker D8 Advance diffractometer)and vibrating sample magnetometry (VSM, LakeShore 7404)
respectively. Above mentioned FARGO/epoxy samples were processed into coaxial circular ring specimens for
electromagnetic parameter test by vector network analyzer (VNA, Agilent N5247A)with an outer diameter of
7 mm and an inner diameter of 3.04 mm, as shown in figure 1. The complex permittivity and complex
permeability within the range of 1 GHz to 18 GHz were recorded.
3. Results and discussion
Figure 2(a)shows the surface morphology of the FARGO sample with an apparent result that the surface of the
rGO sheets is covered with Fe
3
O
4
nanoparticles, which exhibit an aggregated state with particle diameters of
approximately 50 nm. Figures 2(b)and (c)are EDS mapping images of the FARGO sample, indicating the
presence of C, O, Fe, and N elements, in which C element originates from the rGO, Fe element is from Fe
3
O
4
,
N element is from the reducing agent polyether amine, and O element primarily comes from the partially
reduced GO and Fe
3
O
4
, confirming that Fe
3
O
4
is uniformly distributed on the rGO surface. Chemical
composition and functional groups characterized by FTIR spectrum are depicted in figure 2(d). GO samples
contain typical oxygen-containing functional groups, −OH (3450 cm
−1
),C=O(1630 cm
−1
), and C–O group
(1100 cm
−1
)[9,28]. After reduction with polyetheramine, some oxygen-containing functional groups disappear
in ARGO, while new nitrogen-containing groups, such as -NH and -CN [29,30], are generated. For the FARGO
sample, most of its infrared absorption peaks are consistent with those of ARGO and the diffraction peak at
594 cm
−1
corresponds to Fe-O groups [30].Infigures 2(e),(a)distinct diffraction peak for GO can be observed
around 10°. In contrast, ARGO only shows a peak near 20°, indicating that the polyether amine has successfully
reduced GO. In the case of FARGO, apart from the characteristic peak around 20°, there are additional
Scheme 1. Fabrication of Fe
3
O
4
modified polyether amine reduced graphene oxide composite.
Figure 1. Physical picture of coaxial ring sample.
3
Mater. Res. Express 12 (2025)025305 G Yang et al
distinctive Fe
3
O
4
characteristic peaks at 2θ=30.0°, 35.4°, 43.3°, 53.4°, 57.1°, and 62.7°[30]. This confirms that
Fe
3
O
4
has been successfully synthesized and attached to the RGO layers, consistent with the results of SEM and
FTIR. Additionally, the saturation magnetization (M
s
)of the AF sample is approximately 48.5 emu g
−1
, while
that of FARGO decreases to 20.3 emu g
−1
due to the incorporation of non-magnetic rGO. Due to the
significantly higher content of magnetic component in AF compared to FARGO, AF exhibits greater residual
magnetization (M
r
)and coercivity (H
c
)than FARGO, which can be observed in the inset figure in figure 2(f).
Despite this magnetic reduction, the ethanol suspension of FARGO is still easily attracted to a magnet,
demonstrating notable magnetic properties.
Since the introduction of magnetic Fe
3
O
4
into graphene layers, both the complex permittivity (ε
r
=ε′-jε″)
and complex permeability (μ
r
=μ′-jμ″)were variable during electromagnetic parameter measurement using a
vector network analyzer within the range of 1 GHz to 18 GHz, as shown in figure 3. Among them, the real parts
(ε′and μ′)represent the material’s capacity to store energy when subjected to a varying electric or magnetic field,
while the imaginary parts (ε″and μ″)stand for the corresponding energy loss intensity [31]. Comparing with the
RGO sample, the FARGO1, FARGO2, and FARGO3 samples exhibit significantly enhanced complex
Figure 2. SEM (a)and EDS (b),(c)of FARGO, FTIR (d)and XRD spectrum of as-prepared samples, hysteresis loop (f)of AF and
FARGO.
Figure 3. Electromagnetic parameters (a),(b),(d),(e)and corresponding loss angle tangent value (c),(f)of samples.
4
Mater. Res. Express 12 (2025)025305 G Yang et al
permittivity and permeability, primarily on account of the increased content of conductive rGO layers and
magnetic Fe
3
O
4
nanoparticles. Among these, the FARGO3 sample shows the highest values for both complex
permittivity and permeability, while FARGO1 and RGO have similar permittivity values. All electromagnetic
parameter curves display typical dispersion phenomena, with ε′value ranging from 5 to 10 and ε″value ranging
from 0.5 to 2.5. The ideal dielectric properties mainly originate from the incomplete reduction of GO, which
retains some defects and oxygen-containing functional groups. The complex permeability shows a similar trend
but is overall more consistent, with less variation compared to the complex permittivity. The real part μ′ranges
from 1.35 to 1.1, while the imaginary part μ″varies between 0.24 and 0.02. In contrast, the reference group RGO
exhibits real part μ′close to 1 and imaginary part μ″near 0, characteristic of a typical non-magnetic sample.
Besides, the tanδ
ε
values of these materials are higher than their tanδ
μ
values, indicating that dielectric loss
primarily contributes to electromagnetic wave absorption [32].
Based on transmission line theory and the previously measured electromagnetic parameters, the microwave
absorbing performance was calculated according to equations (1)and (2)[33].
/∣( ) ( )∣ ( )=-+RL ZZZZ20 log 1
in in
10 00
//() ()me p me=ZZ jfd ctanh 2 2
in 0
Figures 4(a)–(d)depict the 3D reflection loss (RL)maps of the four as-prepared samples at thicknesses
ranging from 1 to 5 mm. FARGO3 possesses the superior absorption intensity, followed by FARGO2 and
FARGO1, with the control group RGO showing the weakest performance. The RL values of the latter three
groups do not exceed −15 dB, specifically −10.83 dB, −9.49 dB, and −14.33 dB, respectively. For the FARGO3
sample, the optimal absorption peak is approximately −23.12 dB at 6.4 GHz with a given thickness of 4 mm.
While a matching thickness adjusted to 2 mm, a broadest absorption bandwidth of about 5.6 GHz, nearly
covering the entire Ku band, can be obtained. A in-depth analysis of the electromagnetic parameters yields the
normalized impedance ratio |Z
in
/Z
0
|and the microwave attenuation constant α(equation (3)) [33]. Generally,
when the characteristic impedance Z
in
of the absorber is closer to free space wave impedance Z
0
, the
electromagnetic waves can more easily penetrate the material, thus |Z
in
/Z
0
|closer to 1 is preferable. Next, a
higher αvalue indicates stronger dissipative capability for incident electromagnetic waves. FARGO3
demonstrates the best absorbing performance due to its optimal impedance matching and highest microwave
attenuation constant (figures 4(e)and (f)). The comparison of the two crucial indicators shows that FARGO3
performs the best, followed by FARGO2 and FARGO1, with RGO being the least favorable. This indicates that
the incorporation of magnetic Fe
3
O
4
nanoparticles can significantly enhance the impedance matching
performance of the MAMs, bringing its impedance value closer to that of free space. Moreover, the addition of
magnetic materials increases magnetic loss, thereby improving the material’s ability to attenuate
electromagnetic waves [34].
Figure 4. 3D reflection loss (a)–(d), impedance matching ratio (e)and microwave attenuation (f).
5
Mater. Res. Express 12 (2025)025305 G Yang et al
{ ( (( )( )) )} ( )apme me m m e e=-¢¢++¢+¢
f
c23
2 2 2 2 12 12
To further illustrate the microwave absorbing performance of the as-prepared samples, a single-station
radar cross section (RCS)simulation was performed for both a metal conductor plate and a metal plate coated
with a 2 mm thick layer of as-prepared MAMs with CST software [35]. The RCS results at a frequency of
14.5 GHz are shown in figure 5. The radar scattering signal indicates that the scattering intensity of the pure
metal plate significantly decreases after applying the as-prepared MAMs. FARGO3 coating reduces the RCS of
the metal plate from 14.82 dB•m
2
to 0.045 dB•m
2
at an angle of 0°, achieving the smallest RCS value, which is
consistent with the previously calculated RL value. Therefore, the prepared polyether amine reduced graphene
oxide/Fe
3
O
4
resin-based composite materials demonstrated excellent electromagnetic wave absorbing
properties, making them suitable for application as absorbing coatings to reduce radar scattering signals.
Scheme 2illustrates the potential wave absorption mechanism of the FARGO sample. Firstly, the rGO is
uniformly dispersed within the resin matrix, forming abundant interfaces among rGO, Fe
3
O
4
and resin, which
facilitates interfacial polarization [36]. Secondly, rGO exhibits excellent electrical conductivity, and after being
reduced and grafted with polyetheramine and attached with Fe
3
O
4
, it reduces the tendency to agglomerate. At
higher contents within the resin, it forms a well-connected conductive network, contributing to conductive loss.
The defects generated during the reduction of rGO, along with the residual oxygen-containing functional
groups and the incorporation of magnetic Fe
3
O
4
nanoparticles, further enhance dielectric and magnetic loss.
Additionally, electromagnetic waves undergo multiple reflections and scatterings within the three-dimensional
conductive network formed by rGO layers, which also dissipates electromagnetic energy [37]. Therefore, the
Figure 5. 3D radar wave scattering signal (a)–(f)and RCS values of as-prepared samples (g).
Scheme 2. Microwave absorption mechanism of FARGO composites.
6
Mater. Res. Express 12 (2025)025305 G Yang et al
polyether amine-modified magnetic Fe
3
O
4
-decorated graphene composite material proposed in this study
demonstrates excellent microwave absorption performance.
4. Conclusion
In summary, an ideal magnetic Fe
3
O
4
particle modified graphene MAMs was prepared via in situ reduction
using polyether amine. Compositional analysis and structural morphology tests confirmed the uniform
distribution of magnetic Fe
3
O
4
particles on the graphene sheets. The modified graphene contained amino
groups, which help alleviate the agglomeration tendency of graphene and enhance its bonding strength with
epoxy resin. Among all the samples, the FARGO3 sample exhibited optimal microwave absorption
performance, with a peak absorption intensity reaching −23.12 dB and an effective absorption bandwidth of
5.6 GHz. Electromagnetic parameters were conducted to calculate the characteristic impedance and microwave
attenuation constant of the as-prepared absorbers, further verifying that FARGO3 sample possessed the best
impedance matching and the highest microwave attenuation constant, resulting in superior microwave
absorption performance. Furthermore, RCS simulation results indicated that the graphene-based absorbing
coating significantly reduced the RCS of a metal plate, highlighting its potential for advanced stealth and
camouflage applications. These findings provide a solid foundation for the development of next-generation
microwave absorbing materials, with future work focusing on fine-tuning the composite structure and
exploring novel dopants to further enhance performance and broaden application scenarios.
Acknowledgments
None.
Conflicts of interest
The authors declare that they have no known competing financial interests or personal relationships that could
have appeared to influence the work reported in this paper.
Data availability statement
All data that support the findings of this study are included within the article (and any supplementary files).
ORCID iDs
Sanwen Peng https://orcid.org/0009-0002-6317-4123
Bin Zhang https://orcid.org/0000-0002-6287-8754
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