J Mater Sci: Mater Electron (2024) 35:572

Effect of nitrogen‑doped reduced graphene oxide

on the wave‑absorbing properties of hollow ­ZnFe2O4
Hui Liu1, Jianfeng Dai1,2,* , Danqiang Huang1, and Rui Yu1

1
School of Science, Lanzhou University of Technology, Lanzhou 730050, Gansu, China
2
State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals, Lanzhou University of Technology,
Lanzhou 730050, Gansu, China

Received: 2 November 2023 ABSTRACT

Accepted: 5 March 2024
© The Author(s), under
exclusive licence to Springer
Science+Business Media, LLC,
part of Springer Nature, 2024
The mitigation of electromagnetic wave pollution is a pressing concern that can
be addressed by the effective utilization of microwave-absorbing materials char-
acterized by low density, thin thickness, wide absorption bandwidth, and robust
absorption strength. This work used a two-step solvent-thermal and hydrother-
mal approach to create nitrogen-doped reduced graphene oxide (NRGO)/ZnFe2O4
hollow-structured composite microwave absorbent materials. The study of its
microstructure reveals that the flaky NRGO is well adhered to the hollow ­ZnFe2O4
with a rough surface. The findings indicate that the electromagnetic wave absorp-
tion characteristics of NRGO/ZnFe2O4 are influenced by the variable contents of
NRGO. At the NRGO doping level of 15%, the NRGO/ZnFe2O4 composites exhibit
the best electromagnetic wave absorption capabilities. With the matching thick-
ness of 4.91 mm, the minimum reflection loss (RLmin) can approach − 59.95 dB.
This study serves as a significant point of reference for the development of highly
effective electromagnetic wave absorption materials using graphene.

1 Introduction In electromagnetic wave absorption, spinel-struc-

With the accelerated development of information
technology in the twenty-first century has come the
emergence of electromagnetic radiation pollution, an
issue of the utmost importance [1–3]. The develop-
ment of highly efficient microwave-absorbing (MA)
materials that can provide sustainable and advanced
electromagnetic energy conversion is also essential to
address such pollution [4, 5]. In order to be deemed
suitable, the material must possess specific attributes,
including low density, thin thickness, a broad absorp-
tion bandwidth, and a high absorption strength [6–8].
tured semiconducting metal oxides are frequently
employed due to their more stable chemical charac-
teristics and less expensive preparation [9, 10]. Its gen-
eral structure formula is ­AB2O4, where B is generally
Fe and the A position can be replaced by Mg, Cu, Co,
Ni, Zn, and so on [11–15]. Among them, ­ZnFe2O4 has
a low cost, is relatively simple to prepare, and is often
used as an electromagnetic wave absorber [16]. In fact,
it also has certain disadvantages that limit its use as
an efficient microblogging absorber, such as that the
loss is too low and the density is too large. Therefore,
rational design of microstructures with unique mor-
phology is particularly important for electromagnetic

Address correspondence to E-mail: daijf@lut.edu.cn

https://doi.org/10.1007/s10854-024-12327-8

Vol.:(0123456789)
 572 Page 2 of 16
wave attenuation [17]. Hollow structure has a wide
range of application prospects in the fields of wire-
less communication, radar technology, and electro-
magnetic shielding due to its low density and wide
band absorption characteristics. The cavity inside the
hollow structure can make electromagnetic waves
reflect and refract many times, increase the interaction
between electromagnetic waves and materials, and
optimize the impedance matching [18]. The hollow
open structure of ­ZnFe2O4 studied in this paper can
increase the effective electromagnetic wave absorption
cross-section by introducing openings in its exterior.
This allows more electromagnetic waves to enter the
interior of the structure, thereby increasing the absorp-
tion efficiency. Composites of carbon-based materials
with metal oxides introduce a variety of attenuation
mechanisms that effectively address the shortcomings
of ferrite materials.
Novel carbon-based materials, such as reduced
graphene oxide (RGO) [19] and graphite nanoparti-
cles (GNPs) [20, 21], are highly promising due to their
unique and distinctive physical and chemical proper-
ties [22]. In recent years, carbon-based materials have
been used as highly efficient absorbers for effective
microwave absorption by converting the energy of
incident electromagnetic waves into heat through die-
lectric and conductive losses [23]. Hybridizing RGO
with it is an excellent approach [24–31]. Good chemical
stability, low density, and significant dielectric loss are
all advantages of RGO as an efficient microblogging-
absorbing material [32–39]. For instance, a straight-
forward one-pot hydrothermal process was used to
create the reduced graphene oxide (RGO)/nickel-iron
oxide alloy ­(NiFe2O4) composites reported by Zong
et al. An absorption bandwidth of 5.0 GHz (from 12.7
to 17.7 GHz) was reached at a thickness of 1.9 mm with
RL below − 10 dB. The greatest RL of the RGO/NiFe2O4
composite with a thickness of 3.0 mm was − 39.7 dB at
9.2 GHz [28]. Using a straightforward, one-step hydro-
thermal process, Yang et al. created nanohybrids made
of zinc ironate ­(ZnFe2O4) and reduced graphene oxide
(RGO). The findings validate the existence of nano-
hybrids containing 20.4% reduced graphene oxide
(RGO). The ­ZnFe2O4/RGO nanohybrids have a RLmin
of − 29.3 dB at a frequency of 16.7 GHz and a thick-
ness of 1.6 mm [24]. Heidari used a one-pot solution
combustion synthesis to create ­MgFe2O4/RGO nano-
composites. Multi-region absorption properties were
demonstrated by ­MgFe2O4/RGO nanocomposites. The
composite of ­MgFe2O4 and 17-wt% RGO exhibited a
J Mater Sci: Mater Electron (2024) 35:572
robust absorption of − 35.5 dB at 12.5 GHz, whereas
the larger RGO concentrations resulted in a broad
effective bandwidth of 1.6 GHz in the Ku band [25].
Doping N atoms between carbon and magnetic
metal materials can effectively solve the deficiency of
ferrite materials [40]. Meanwhile, nitrogen doping can
modulate the electronic structure of graphene, thus
changing its conductivity and dielectric properties.
This makes it possible to optimize the electromagnetic
properties of composites by adjusting the degree of
nitrogen doping to meet the absorption needs in a spe-
cific frequency range. Nitrogen-doped graphene oxide
(NRGO) typically has good conductivity and electro-
magnetic properties, which helps to improve the capa-
bility of materials to absorb electromagnetic waves.
Therefore, in this experiment, we prepared composite
microwave-absorbing materials with a hollow open-
ended structure composed of nitrogen-doped reduced
graphene oxide/ZnFe2O4 by solvothermal and hydro-
thermal methods. Then, the effects of adding different
amounts of nitrogen-doped reduced graphene oxide
on the wave-absorbing ability of hollow ­ZnFe2O4 were
compared. The produced ­ZnFe2O4/NRGO exhibits
good absorption of electromagnetic waves at 4.91 mm
in thickness, the composite doped with 15% NRGO
has a RLmin of − 55.95 dB.
2 Experimental
2.1 Materials
Zinc acetate (Zn(Ac) 2 ⋅2H 2 O) and iron nitrate
(Fe(NO3)3⋅9H2O) were purchased from Sinopharm
Chemical Reagent Co. Ethylenediamine (EDA) and
glycerol were produced by Chengdu Jinshan Chemical
Reagent Co. Isopropanol was purchased from Alad-
din Industrial Company. Graphene oxide (GO) was
provided by the China Graphene Research Institute.
This experiment uses just analytical polar substances
that are all readily usable.
2.2 Process of material synthesis
The synthesis of ­Z nFe 2 O 4 /NRGO composites is
schematically shown in Fig. 1. To a mixture of
isopropanol and glycerol were added 0.0987 g of
Zn(Ac)2⋅2H2O and 0.3636 g of Fe(NO3)3⋅9H2O. After
complete dissolution by magnetic stirring, the solu-
tion was held at 180 °C for 8 h by solvent heating.
J Mater Sci: Mater Electron (2024) 35:572
Fig. 1  Schematic synthesis of ­ZnFe2O4/NRGO composites
This was followed by centrifugation, washing several
times with anhydrous ethanol and deionized water,
and drying in a desiccator at 60 °C for 24 h. Then, it
was calcined in the air at 500 °C for 2 h. The sample
was then dried in an oven at 60 °C for 24 h and then
calcined in the air at 500 °C for 2 h. It is then calcined
in the air at 500 °C for 2 h. The reaction principle of
this process is that after the metal salt is dissolved in
the organic solvent, the corresponding metal alcohol
salt will be formed first under the solvent heat con-
ditions of high temperature and high pressure, and
the metal alcohol salt precipitates into nucleation
and forms primary particles rapidly. As the reaction
proceeds, the primary particles grow slowly. During
the subsequent heat treatment, large nanocrystals of
­ZnFe2O4 are gradually formed and oriented by self-
assembly and organic matter to form ­ZnFe2O4 with a
hollow, open-ended morphology [41]. The prepared
­ZnFe2O4 microspheres and graphite oxide (GO) were
ultrasonically mixed in 80 mL of deionized water,
followed by the addition of ethylenediamine (EDA)
as a nitrogen dopant and reducing agent, which was
stirred thoroughly until complete dissolution and
then subjected to a hydrothermal reaction at 180 °C
for 6 h. Finally, the NRGO/ZnFe2O4 composites were
made by freeze-drying for 48 h. The pure ­ZnFe2O4
was named S1. The composites with 10%, 15%, and
20% NRGO doping were named S2, S3, and S4,
respectively.
Page 3 of 16 572
2.3 Characterization
The phase structure and crystallographic details of the
samples were assessed using Cu-Kα radiation X-ray
diffraction (XRD). Using Hitachi-Su8020 scanning
electron microscopy (SEM) and JEM-2100 F transmis-
sion electron microscopy (TEM), the morphology of
the produced samples was examined. Thermo Fisher
K-Alpha X-ray photoelectron spectroscopy (XPS) was
used to evaluate the chemical bond states. Using a
MicroSense EV-9 vibrating sample magnetometer
(VSM) at room temperature, the magnetic performance
of the samples was assessed. Peak carbon intensity and
location were obtained using the Renishaw RM2000
Raman spectrometer. Using an Agilent E5071C vector
network analyzer (VNA), the sample was filled with
paraffin, and the electromagnetic characteristics were
measured at the coaxial ring.
3 Results and discussion
Figure 2a displays the x-ray diffraction (XRD) patterns
of the four samples and NRGO. The characteristic
peaks associated with ­ZnFe2O4 are evident in samples
S1–S4. Specifically, the primary peaks at 2θ = 29.9°,
35.2°, 42.8°, 53.1°, 56.6°, and 62.1° correspond to the
crystal planes of Z
­ nFe2O4 (JCPDS No. 86–0507) (220),
(311), (400), (422), (511), and (440), respectively. The
 572 Page 4 of 16
Fig. 2  a XRD patterns of S1–S4. b Raman spectra of S1–S4
diffraction peaks of NRGO monomers at 2θ = 24.2° and
43° in the figure are attributed to the (002) and (100)
crystal planes of graphite, respectively [42]. The origi-
nal (001) diffraction peak disappears after GO reduc-
tion by ethylenediamine, and the (002) diffraction peak
reappears, and the (002) diffraction peak is a broad
front after the introduction of the N source. All these
confirm that GO is reduced and successfully doped
with N atoms [43, 44]. Nevertheless, it is challenging to
identify the NRGO diffraction peaks in S2–S4, which is
probably due to the much weaker diffraction intensity
of NRGO in NRGO/ZnFe2O4 composites compared to
­ZnFe2O4, a spinel-structured material.
Figure 2b illustrates the Raman spectra of S2–S4
samples and NRGO monomers, which are usually
used to detect their graphitization. The two observed
Raman scattering peaks, located at approximately
1586 and 1360 ­cm−1, are commonly referred to as the
G and D peaks, respectively. The G peak, a prominent
feature in the Raman spectrum of graphene, arises
from the in-plane vibrational motion of ­sp2 carbon
atoms. This peak serves as a reliable indicator of the
graphene’s layer count; however, it is notably influ-
enced by external stressors. The D peak is commonly
recognized as the manifestation of disordered vibra-
tional modes in graphene. The precise positioning
of this peak is contingent upon the laser wavelength
employed, and it arises from lattice vibrations occur-
ring away from the central region of the Brillouin
zone. Consequently, it serves as a means to character-
ize structural imperfections or boundaries present in
graphene specimens [45, 46]. In the Raman spectrum
of graphene, ID/IG can be used to characterize the ­sp3/
J Mater Sci: Mater Electron (2024) 35:572
sp2 bond ratio [47, 48]. The results show that the ID/IG
values become higher and higher with the increase in
the amount of NRGO, indicating that nitrogen dop-
ing causes disorders or structural defects [49]. Fur-
thermore, the presence of a scattering peak at around
633 ­cm−1 aligns with the previously documented peaks
observed in the Raman spectra analysis of ­ZnFe2O4
[24].
Scanning electron microscopy (SEM) was employed
to investigate the microscopic morphologies of the S1
and S3 samples, as depicted in Fig. 3. Among them,
Fig. 3a, b, and c shows that pure ­ZnFe2O4(S1) exhibits
a hollow, open, small spherical shape, and the hollow
structure helps to optimize the impedance matching
behavior. In Fig. 3d, NRGO completely encapsulates
­ZnFe2O4, and in Fig. 3e, f, NRGO exhibits multilayered
and single-layered structures, indicating that ­ZnFe2O4
is well bonded to the NRGO sheet, and the utilization
of a composite material consisting of three-dimen-
sional hollow ­ZnFe2O4 and NRGO exhibits the ability
to extend the transmission channel of electromagnetic
waves through the provision of numerous reflections
and scattering.
Only the open structure can be seen from the SEM
image, and the hollow structure also needs to be
observed by TEM. Figure 4a and b can better show that
pure ­ZnFe2O4 (S1) is a unique hollow, open spheri-
cal structure, which leads to multiple relaxation pro-
cesses and good impedance matching. Figure 4d, e,
and f can correspond to the previous SEM images,
where ­ZnFe2O4 creates an interface with NRGO, which
facilitates interfacial polarization, increases multiple
reflections and scattering, and provides excellent
J Mater Sci: Mater Electron (2024) 35:572
Fig. 3  a, b, c SEM images of S1. d, e, f SEM images of S3
Fig. 4  a, b TEM images of S1. c Selected-area electron diffraction (SAED) pattern of S1. d, e, f TEM images of S3
wave-absorbing properties and a wider absorption
range. Figure 4c shows the diffraction rings of the S1
sample, corresponding to the (220), (400), (331), and
(511) crystal planes of ­ZnFe2O4.
As shown in Fig. 5, we examined the surface ele-
ments of the S3 sample and electronic valence struc-
tures using XPS. The S3 sample contains Zn, Fe, O,
N, and C elements, according to the overall spectrum
(Fig. 5a). The C 1s spectra split peaks were fitted with
four peaks that corresponded to C–C, C–O, C=O, and
C–C=O bonds, as shown in Fig. 5b [31, 39], where no
Page 5 of 16 572
significant C–N bond synthesis was detected, mainly
because the nitrogen doping was too trace and did
not bind to C. However, it is evident from Fig. 5d that
the N 1s spectra may be classified into three distinct
nitrogen species, namely pyridine nitrogen, pyridine
nitrogen, and graphite nitrogen [39, 50, 51]. Fe–O and
Fe–O–C bonds are represented by the two peaks in
the O 1s spectra (Fig. 5c). Figure 5e illustrates the Fe
2p spectrum, where the peak observed at 710.7 eV
is assigned to Fe ­2p3/2, while the peak observed at
724.8 eV is assigned to Fe ­2p1/2, and the rest of the
 572 Page 6 of 16 J Mater Sci: Mater Electron (2024) 35:572

Fig. 5  XPS spectra of S3 include the following: a total spectrum, b the carbon 1s spectrum, c the oxygen 1s spectrum, d the nitrogen 1s
spectrum, e the iron 2p spectrum, and f the zinc 2p spectrum

IV-type isotherm can be observed in the figure,

indicating that the S1 sample possesses mesoporous
characteristics with a specific surface area of 35.4524
­m2/g. From the inserted pore size distribution image,
it can be seen that the pore size of the material has
reached the mesoporous range, with an average pore
size of 24.4487 nm. Combined with the TEM image,
this hollow open mesoporous material contributes
to the interfacial polarization and scattering sites,
which enhance the microwave absorption. By tuning
the pore structure and geometry of the hollow part,
we can optimize the electromagnetic properties. Its
light weight, low density, and broad band absorption
are also characteristics we are looking for [18, 54, 55].
The hysteresis loop (VSM) graphs of four samples
Fig. 6  N2 adsorption–desorption isotherms and pore size distri- at 300 K are displayed in Fig. 7. Every sample exhib-
butions of S1 its typical ferromagnetism with obvious hysteresis.
It is noteworthy that the saturation magnetization
intensities of samples S2 and S3 are basically the
peaks are satellite peaks [39, 52]. The Zn ­2p1/2 and Zn same as compared to sample S1, which is due to the
­2p3/2 peaks are represented by the two peaks in Fig. 5f, lower content of nonmagnetic NRGO. When more
so ­Zn2+ is present in the S3 material [53]. NRGO is added, the saturation magnetization inten-
The prepared pure ­Z nFe 2O 4 (S1) samples were sity of S4 decreases significantly compared with that
characterized by BET. The nitrogen adsorption–des- of S1 because the magnetic reaction is delayed by
orption method was used to calculate its specific sur- the addition of nonmagnetic NRGO. The coercivity
face area and porosity, as shown in Fig. 6. A typical of S1–S4 is almost the same, which indicates that the
J Mater Sci: Mater Electron (2024) 35:572
Fig. 7  Magnetization hysteresis loops of samples S1, S2, S3, and
S4
addition of nonmagnetic NRGO has no effect on the
coercivity [56, 57].
Figure 8 illustrates the electromagnetic param-
eters of the four samples. Dielectric loss materials
used to absorb microwaves depend on the relation-
ship between the complex dielectric constant and the
conductivity. The capability of the material to absorb
electromagnetic energy is determined by this interac-
tion. The complex dielectric constant is composed of
Fig. 8  ε′ (a) and ε″ (b), µ′ (d) and µ″ (e), tanδε (c), and tanδµ (f) of all samples
Page 7 of 16 572
two parts: real (ε′) and imaginary (ε″) components.
The real part involves the storage of electrical energy,
while the imaginary part involves its conversion to
heat [58]. Figure 8a and b shows the relationship
between ε′ and ε″ of S1–S4 and frequency (f). The val-
ues of ε′ and ε″ increase as the NRGO increases over
the entire frequency range. The larger value of ε″ indi-
cates that the conductivity is also higher and the mate-
rial is better able to absorb microwaves and convert
them into heat. The connection between conductivity
(σ) and ε″ is shown below:
𝜎
𝜀�� = 𝜀0 𝜔 , (1)
where ε0 is the vacuum permittivity and ω is the
angular frequency of the applied electromagnetic
field. Essentially, an increase in σ leads to an increase
in ε″, which enhances the microwave absorption of the
material. This is because higher conductivity means
greater energy loss, allowing these materials to con-
vert electromagnetic energy into heat more efficiently
[59, 60]. With an increase in f, the ε′ values of S1 and
S2 remain essentially unchanged, while the ε′ values
of S3 and S4 decrease from 5.9 to 4.2 and from 9.4 to
5.7. The ε″ values of S3 and S4 decreases from 2.8 to
1.6 and from 4.2 to 3.2, which are both decreasing and
therefore a dispersion phenomenon occurs, which can
better help the electromagnetic wave to be attenuated.
The sample will relax under an applied electric field,
 572 Page 8 of 16 J Mater Sci: Mater Electron (2024) 35:572

mostly as a result of interfacial and dipole polariza- permeability and complex permittivity are repre-
tion. Graphene serves as the source of the polariza- sented by µr and εr, respectively, and are computed
tion center, wherein dipole polarization manifests in as follows:
response to an applied electric field [61]. The applied
electric field is generated by an electromagnetic wave
𝜀r = 𝜀� − j𝜀�� , (4)
incident on the surface of the material. These are
responsible for the decrease in the complex dielectric 𝜇r = 𝜇� − j𝜇�� . (5)
constant with f.
It goes without saying that the closer Zin is to 1,
The magnetic dissipation capacity of an absorber
the less RL, which indicates that the electromagnetic
depends to a large extent again on the magnetic per-
wave absorption ability is stronger. In Fig. 9a, d, g,
meability. The magnetic permeability consists of two
and j, we displayed the two-dimensional reflection
parts, the real part (µ′) and the imaginary part (µ″).
loss of S1–S4. The reflection loss in three dimensions
The real part of the permeability represents the stor-
is depicted in Fig. 9b, e, h, and k, while the related
age capacity of the magnetic field energy, while the
contour plots may be observed in Fig. 9 c, f, i, and
imaginary part of the permeability represents the
l. According to the data presented in Fig. 9a, it can
dissipation capacity of the magnetic field energy.
be observed that the S1 sample does not exhibit any
Figure 8d and e illustrates the correlation between
RL values below − 10 dB. Additionally, the effective
µ′ and µ″ components of the complex permeability of
absorption bandwidth (EAB) is measured to be 0 GHz,
samples S1–S4 and f. The µ′ and µ″ of the S2–S4 sam-
suggesting that the microwave absorption capabili-
ples exhibit a consistent trend with frequency follow-
ties of pure ­ZnFe2O4 are inadequate. Consequently,
ing the addition of NRGO. Figure 8d demonstrates
we conducted an observation in order to ascertain the
a distinct correlation between µ′ and f at approxi-
alterations in the wave-absorbing characteristics of the
mately 3.4 GHz and 5.2 GHz, respectively. Simi-
composites subsequent to the introduction of varying
larly, Fig. 8e displays a clear relationship between
quantities of NRGO. Figure 9(d) shows that there is
µ″ and f for the S2-S4 samples at around 6.3, 14.5,
an S2 absorption peak, and the corresponding RLmin
and 16.5 GHz. Figure 8f exhibits distinct resonance
at the thickness of 5 mm is − 10.66 dB, which indicates
peaks at around 6.3, 14.5, and 16.5 GHz. These peaks
that the microwave absorption rate of NRGO doping
mostly arise from the establishment of electrode cou-
is about 90% when the amount of NRGO doping is
pling induced by the magnetic field applied. The
10%, and the EAB is 0.6 GHz, which is a too narrow
graphs of tanδε and tanδµ with f (Fig. 8c, f) provide a
absorption band. And in Fig. 9g, S3 has two absorp-
more comprehensive representation of the dielectric
loss and magnetic loss characteristics. The variation tion peaks at two different matching thicknesses.
of the curves is basically the same for all the samples. When the equivalent matching thickness is 4.96 mm,
In order to more thoroughly examine how much the best RLmin is − 51.8 dB; when it is 4.91 mm, the
best RLmin is − 59.95 dB, and both EABs are 4 GHz,
NRGO is characterized in relation to NRGO/ZnFe2O4
which indicates that the microwave absorption is best
composites’ wave absorption, the following formula
when the NRGO doping amount is 15%. And in Fig. 9j,
can be used to calculate reflection loss (RL), which
RLmin is − 56.41 dB and EAB is 3.5 GHz for 4.46 mm
is a measure of a material’s ability to absorb micro-
matching thickness. Matching thickness 2.09 yields
waves [62, 63].
RLmin − 50.28 dB. When the NRGO doping level is 20%,
| Z −1 | the microwave absorption effect is favorable for the
RL(dB) = 20 log|| Zin +1 || , (2)
| in | more thinly matched thickness. Figure 9b, e, h, and
k shows the three-dimensional diagrams correspond-
�𝜇 �
2𝜋fd √
� ing to S1–S4, which are more intuitive than the two-
Zin = 𝜀r
r
tan h j c 𝜀 r 𝜇r , (3) dimensional diagrams. Figure 9c, f, i, and l shows its
corresponding contour plot. We can see that the black
where Zin represents the normalized input impedance,
line is in the range of RL < − 10 dB, and the difference
f denotes the frequency of the electromagnetic wave,
in wave-absorbing performance can be judged from
d signifies the thickness of the absorbed layer, and c
the color depth; the deeper represents the better, and
represents the speed of light. The material’s complex
the deepest for Fig. 9i reaches − 59.95 dB. Finally, we
J Mater Sci: Mater Electron (2024) 35:572 Page 9 of 16 572

Fig. 9  Reflection losses for four different scenarios: S1, S2, S3, and S4 are shown in (a), (d), (g), and (j), 3D maps: S1, S2, S3, and S4
are shown in (b), (e), (h), and (k) and related contour maps: (c), (f), (i), and (l)

find that pure ­ZnFe2O4 is not a good electromagnetic
wave-absorbing material and with the individual sub-
stances that we have described earlier as the electro-
magnetic wave-absorbing material. A high-efficiency
electromagnetic wave absorber should not only meet
the wide effective absorption bandwidth but also meet
the low RL. Therefore, the amount of NRGO directly
affects the electromagnetic wave absorption ability of
­ZnFe2O4/NRGO and more is not better [64], and the
RL value varies as a result. The composites doped with
15% NRGO and doped with 20% NRGO have good
electromagnetic wave absorption. However, the effec-
tive bandwidth of composites doped with 15% NRGO
has a wider effective bandwidth and smaller RL val-
ues, so it is more in line with the conditions of the
electromagnetic wave-absorbing materials we want.
 572 Page 10 of 16
This magnetic experiment loss should be the result
of eddy current loss, which is determined by observ-
ing the variation of C0 with frequency with the fol-
lowing equation [39, 65, 66]:
2𝜋𝜇0 (𝜇 � ) 𝜎d2
2 tion frequency. When the relationship between tm
𝜇�� ≈ , (6)
3
( )−2
C0 = 𝜇�� 𝜇� f −1 ,
where σ represents electrical conductivity and µ 0
indicates vacuum permeability. The C0 value of the
sample varies between 2 and 18 GHz, as illustrated in
Fig. 10a, and the presence of exchange resonance and
natural resonance is often represented in the C0 and
frequency plot with significant peaks, at which time
the frequency is 3.0–8.0 GHz or 14.0–17.0 GHz. When
the frequency reaches 8 GHz, the C0 value tends to be
stabilized, which suggests that eddy current loss is the
source of this magnetic loss. The attenuation constant
α, which is determined by the following formula, can
be used to typically reflect the electromagnetic loss
capabilities of a microwave absorber [39, 67, 68]:
� wave absorber due to its small thickness, low density,
�
√
2𝜋f
𝛼= × (𝜇 �� 𝜀�� − 𝜇� 𝜀� ) + (𝜇 �� 𝜀�� − 𝜇� 𝜀� )2 + (𝜇𝜀 + 𝜇 � 𝜀� )2 .
c
The microwave loss capability is gradually
enhanced, as shown by Fig. 10b, where the value of
α is larger than that of pure ­ZnFe2O4 at 10% NRGO
doping, larger than that of 10% NRGO doping at 15%
NRGO doping, and the largest value of the four sam-
ples at 20% NRGO doping [69, 70].
Fig. 10  a C0 of S1–S4. b Decay constant of S1–S4
J Mater Sci: Mater Electron (2024) 35:572
(9)
n𝜆 nc
tm = = √ (n = 1, 3, …) .
4 4fm 𝜀r 𝜇r
The variable “tm” represents the thickness of the
absorber, whereas “f m” denotes the peak absorp-
and fm adheres to the aforementioned equation, the
phase difference between the two reflected micro-
waves, namely at the interfaces of air-absorber and
(7)
absorber-metal, amounts to 180°. Figure 11 illustrates
the RL − tm − ||Zin − 1|| plot for S3. A decrease in the
RL value corresponds to a decrease in the magnitude
of ||Zin − 1||, indicating an increased electromagnetic
wave absorption capability. The simulated thickness
sim ) is shown by the black line in the t figure, while
( tm
m
the experimental thickness ( tm ) is represented by
exp
the blue star, where all lie on the modeled λ/4 curve,
and the λ/4 rule can be satisfied by the impedance
matching.
Table 1 lists the ­ZnFe2O4-based and NRGO-based
electromagnetic wave absorbers reported in this
work and previously, and the results show that the
prepared ­ZnFe2O4/NRGO is a better electromagnetic
wide absorption width, and high absorption capacity.
The wave absorption mechanism of the ­ZnFe2O4/
(8)
NRGO composite wave-absorbing material is shown
in Fig. 12. Firstly, this pure ­ZnFe2O4 (S1) shows a hol-
low open blob shape, and the hollow structure helps to
optimize the impedance matching behavior [18]. Elec-
tromagnetic waves entering the interior of ­ZnFe2O4
undergo multiple reflections and scattering, and while
some of them dissipate heat, others are absorbed [71].
Second, the composite material consisting of hollow
J Mater Sci: Mater Electron (2024) 35:572 Page 11 of 16 572

the molecular polarization process. When an alter-

nating electric field is present, the molecular dipoles
try to align themselves with the electric field, but the
speed of molecular motion is finite and they do not
change fast enough, so the energy is dissipated as
heat. Electrons accumulate at defects and interfaces
in the presence of the electric field, promoting micro-
wave absorption [72]. At the same time, electrons
migrate and jump with conductive losses, converting
the absorbed electromagnetic energy into heat, while
higher conductivity can also enhance microwave
absorption by promoting resistive heating [49]. Fourth,
when elemental N is successfully doped into RGO, the
­sp2 hybridization of C atoms that would have been
broken means that there will be structural defects and
oxygen-containing functional groups that can act as
polarization centers to form a dipole polarization and
make the dipole moment unbalanced, which results in
a stronger attenuation of electromagnetic waves [73,
74]. Finally, the source of magnetic loss in ­ZnFe2O4/
NRGO composite wave absorbers is the natural loss
of eddy current. These reflect the electromagnetic loss
capability of the microwave absorber.

Fig. 11  RL, tm, and impedance matching curves of S3
­ nFe 2O 4 and NRGO in turn generates interfacial
Z of NRGO and hollow ­ZnFe2O4 by solvothermal and
polarization that extends the transmission chan-
nel of electromagnetic waves by providing multiple
reflections and scattering. Third, when electromag-
netic waves are incident on the material surface, the
directional motion of carriers on the NRGO creates an
oscillating current, and the boundary charge induces
dielectric relaxation. The relaxation loss is related to
4 Conclusion
In summary, we have prepared composite microwave-
absorbing materials consisting of different amounts
hydrothermal two-step methods. Through microscopic
morphology analysis, it is observed that ­ZnFe2O4 exhib-
its hollow open spheres, which helps to optimize the
impedance matching behavior. ­ZnFe2O4 is well attached
to the NRGO sheets, and the composite of three-
dimensional hollow ­ZnFe2O4 and NRGO can prolong
the transmission path of electromagnetic waves. An

Table 1  Previously reported

Absorber Operation frequency RLmin Thickness EAB (GHz) References
­ZnFe2O4-based and NRGO-
(dB) (mm)
based electromagnetic wave
absorbers ZnFe2O4 2–18 GHz − 30.90 8.00 5.66 [61]
ZnFe2O4/RGO 2–18 GHz − 29.30 1.60 2.60 [21]
ZnFe2O4@C 2–18 GHz − 51.38 2.00 4.10 [52]
MWCNTs/ZnFe2O4 2–18 GHz − 55.50 1.50 3.60 [62]
CuFe2O4/NRGO 2–18 GHz − 34.18 1.98 5.92 [18]
NiFe2O4/NRGO 2–18 GHz − 54.40 2.20 4.50 [28]
MgFe2O4/NRGO 2–18 GHz − 55.70 1.98 5.36 [50]
ZnFe2O4/NRGO 2–18 GHz − 59.95 4.91 4.00 This work
 572 Page 12 of 16
Fig. 12  Schematic diagram of microwave absorption mechanism of ­ZnFe2O4/NRGO composites
interface is created between the two, which facilitates
interfacial polarization and increases multiple reflec-
tion and scattering, leading to excellent wave-absorb-
ing properties. The composites of NRGO and ­ZnFe2O4
demonstrate superior electromagnetic wave absorption
characteristics when the doping level of NRGO is 15%.
The composites achieve a minimum reflection loss of
− 59.95 dB with an optimal thickness of 4.91 mm. This
study offers a significant point of reference for the devel-
opment of graphene-based materials with electromag-
netic wave absorption properties. These materials are
distinguished by their low density, thin thickness, wide
absorption bandwidth, and high absorption strength.
Author contributions
HL contributed to Conceptualization and Writing of
the original draft. JD contributed to Supervision and
Conceptualization. DH contributed to Editing of the
manuscript and Revision. RY contributed to Visualiza-
tion and Investigation.
Funding
We declare that no funds, grants, or other sup-
port were received during the preparation of this
manuscript.
J Mater Sci: Mater Electron (2024) 35:572
Data availability
We state that our manuscript is original and unpub-
lished, and all data are true in the original manuscript
and is not considered for publication elsewhere. We
would be grateful if our paper could be reviewed and
considered for publication in the Journal of Materials
Science.
Declarations
Conflict of interest The authors declare that they
have no known competing financial interests or per-
sonal relationships that could have appeared to influ-
ence the work reported in this paper.
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