Ceramics International xxx (xxxx) xxx–xxx

Contents lists available at ScienceDirect

Ceramics International
journal homepage: www.elsevier.com/locate/ceramint

The effect of Ag nanoparticles content on dielectric and microwave

absorption properties of β-SiC
Bo Weia,b,c, Jintang Zhoua,b,c,∗, Zhengjun Yaoa, Azhar Ali Haidrya, Xinlu Guoa, Haiyan Linc,
Kun Qiana, Wenjing Chena
a
College of Materials and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 211100, China
b
Key Laboratory of Material Preparation and Protection for Harsh Environment (Nanjing University of Aeronautics and Astronautics), Ministry of Industry and
Information Technology, Nanjing, 211100, China
c
Research Institute of Aerospace Special Materials & Technology, Beijing, 100074, China

ARTICLE INFO ABSTRACT

Keywords: In the present work, high purity cubic silicon carbide (β-SiC) was synthesized by using resorcinol-formaldehyde
Microwave absorption aerogel coated silica as precursor at high temperature. Subsequently, β-SiC was coated with various con-
Dielectric property centrations of silver nanoparticles (Ag NPs) by tin sensitization electroless plating. Thereafter, the effect of
β-SiC various Ag NPs contents on the dielectric and microwave absorption properties of β-SiC was investigated in
Nano Ag
detailed. It is found that the Ag NPs can significantly increase the overall complex permittivity, reduce the
Electroless plating
thickness of the absorber and increase the absorption bandwidth to some extent. Despite, the improvement of the
attenuation ability of electromagnetic wave with increasing contents of Ag NPs also has an adverse effect on
impedance matching. The improvement in the microwave absorption of β-SiC coated with Ag NPs mainly comes
from the enhancement of dipole polarization, interface polarization and conductivity loss. In the 2–18 GHz band,
Ag@SiC (1.0 g/L) can achieve an effective bandwidth of 4.99 GHz at a thickness of 1.6 mm, and it is a kind of
lightweight, high-temperature microwave absorbent with excellent performance.

1. Introduction and pressure, strong acid and strong alkali. However, the SiC absorbing
frequency band is relatively narrow, which cannot meet the require-
In recent years, the rapid development of communication devices ments of modern absorbing composite materials [7,8]. Therefore, it is
working within electromagnetic (EM) radiation has a great impact on necessary to do intensive research to improve its microwave absorption
human life and environment as well. On the one hand, it is true that all properties. At present, advanced researche on the doping of B, N and P
kinds of communication products have brought great convenience to elements is ongoing and until now the dielectric loss is increased by
people [1,2], but On the other hand, electromagnetic pollution has improving the dielectric performance, or depositing magnetic elements
shown detrimental effect on living species, especially on human health on the SiC surface to increase magnetic losses. For instant, Zhao et al.
[3]. Meanwhile, the development of radar technology greatly threatens [9] prepared N-doped nano-SiC particles by using a laser-induced gas-
the survival environment of aircraft, other weapons and equipment in phase reaction. The found that adjusting the content of SiC could be
military war [4,5], the use of absorbing materials provides an effective used to control the complex dielectric constant of N–SiC particles with
way to solve several problems such as electromagnetic pollution. The high dielectric constant imaginary part and electrical loss factor. The
research and development of absorbing agents has recently become a particles have an effective absorption bandwidth of 6 GHz at a thickness
research hotspot as the core of absorbing materials is to realize im- of 2.96 mm, with a maximum reflection loss of −63.41 dB at
proved absorbing functionality [6]. 12.17 GHz. Li et al. [10] plated nickel-cobalt film on the surface of SiC
Silicon carbide (SiC) absorbents have large loss angle tangent and particles by chemical plating method and shown that adjusting the Ni
can attenuate electromagnetic wave effectively in a certain microwave and Co content ratios of Ni–Co can lead to obtain Ni–Co films with
band. Meanwhile, excellent physical properties and chemical corrosion different conductive and ferromagnetic characteristics. When the initial
resistance make silicon carbide a potential candidate for better micro- atomic ratio of Ni and Co is 1.5 and the material thickness is 2.5 mm
wave absorption under extreme conditions, such as high temperature and the maximum reflection loss of −32 dB was obtained at 6.3 GHz.

∗
Corresponding author. College of Materials and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 211100, China.
E-mail address: imzjt@nuaa.edu.cn (J. Zhou).

https://doi.org/10.1016/j.ceramint.2019.11.029
Received 3 October 2019; Received in revised form 30 October 2019; Accepted 4 November 2019
0272-8842/ © 2019 Elsevier Ltd and Techna Group S.r.l. All rights reserved.

Please cite this article as: Bo Wei, et al., Ceramics International, https://doi.org/10.1016/j.ceramint.2019.11.029
B. Wei, et al. Ceramics International xxx (xxxx) xxx–xxx

Among other conductive materials (e.g., Ni, Cu and Fe), silver is 2.3. Preparation of Ag NPs
widely used owing to its stable physical and chemical properties and
low oxidation tendency [11,12]. However, Ag is rarely coated on SiC to For the sensitization treatment, SnCl2 sensitizing solution (1 g SnCl2,
obtain improved wave absorbers due to its high preparation cost. The 3 mL hydrochloric acid, 30 mL deionized water) was prepared and 0.5 g
strong skin effect of silver can also lead to form a conductive network, SiC powder was added into the sensitizing solution under rigorous
which results in the reflection of electromagnetic wave and thus poor stirring for 15 min at 60 °C. After centrifuging, washing and vacuum
absorption performance. To address such issues, Ag nanoparticles (Ag drying at 60 °C, Sn2+ coated sensitized SiC powder was obtained.
NPs) were coated on the β-silicon carbide instead of a single silver filler, Thereafter, two solutions were prepared, namely solution-A (Ag salt
which reduces the cost, improved the overall dielectric performance solution) and solution-B reducer solution, various compositions of these
and hence improved microwave absorption performance. solutions is shown in Table 2.
In this work, innovative Ag@SiC absorbent was prepared by carbon Both the solutions A and B were then mixed under rigorous stirring
thermal reduction and subsequent electroless plating. The influence of followed by the addition of sensitized SiC powder. The composite Ag@
the content of Ag NPs on the dielectric and absorbing properties of the SiC powder with silver-gray coating was obtained after stirring at a
SiC was investigated by changing the concentration of silver precursor constant temperature of 30 °C for 90 min.
in electroless plating. It is found that the Ag NPs coating significantly
improves the real and imaginary parts of the overall complex permit- 2.4. Characterization
tivities, and the resistive loss mechanism changes to the dielectric loss
mechanism. Ag NPs have an adverse effect on impedance matching Analysis of the lattice structure and element composition of the
performance, but significantly improves the attenuation performance, products in each stage were performed by a powder X-ray diffractometry
which we believe can be correlated with the enhancement of dipole (XRD, Bruker, D8 Advance) and a fourier transform infrared spectro-
polarization, interface polarization and conductivity loss. meter (FT-IR, Nicolet, Nexus 670) respectively. The thermodynamic
stability, the microstructural morphologies were obtained by thermo-
2. Experimental gravimetric analysis (TG, NETZSCH, TA), scanning electron microscopy
(SEM, Hitachi, S4800) and transmission electron microscopy (TEM,
2.1. Reagent and raw materials JEOL, JEM-2100F). Moreover, the element composition of surface
coating was observed by an X-ray photoelectron spectroscopy (XPS,
The related specifications of chemical reagents and raw materials Thermo Scientific, ESCALAB 250XI). Last but not the least, the electro-
used in this work are shown in Table 1. magnetic parameters were tested by a vector network analyzer (VNA,
Ceyear, 3672B), during this testing a mold was used to mix the sample
with paraffin in a 1 : 1 ratio of mass and compactness to get a annular
2.2. Preparation of high-purity β-SiC specimen with a thickness of about 2 mm. We also used the coaxial
method to test the electromagnetic performance of the annular specimen.
5 mL ethyl orthosilicate was weighed in a beaker and subsequently
40 mL ethanol, 40 mL deionized water, 2.5 mL ammonia and 1.5 g PVP 3. Results and discussion
(k-30) was added under rigorous stirring (150 rpm) at 30 °C for 20 h.
Then, the solution was filtered and SiO2 was obtained after roasting at 3.1. Preparation mechanism and basic characterization
650 °C for 3 h.
The prepared SiO2 was mixed evenly with an appropriate amount of The typical synthesis process of Ag@SiC is shown in Fig. 1. Firstly,
resorcinol/formaldehyde solution with a molar ratio of 1 : 2, the pH SiO2 was prepared by ethyl orthosilicate-sol-gel method and the im-
value was adjusted to 8–9 by ammonia solution. Then, 2.5 ml nickel purities were removed by calcining at high temperature to obtain
chloride hexahydrate and 0.01 g anhydrous sodium carbonate was evenly dispersed SiO2 powder. Then aerogel was prepared in the system
added for 5 h reaction at 60 °C followed by solidifying for 1 h at 85 °C containing resorcino-formaldehyde (RF) sodium carbonate and then
and drying. The crude product was obtained after two step heating- coated on SiO2 to obtain the precursor of RF aerogel@SiO2. High purity
treatment of the mixture in argon atmosphere of, at 650 °C for 1 h and SiC with β-SiC as the main crystal type was obtained by carbon thermal
1450 °C for 4 h. Thereafter, the powder was annealed in static-air at reduction in Ar atmosphere. The prepared SiC powder was then sensi-
650 °C for 3 h to remove carbon followed by pickling and drying to tized with Sn2+ ions to add target sites for Ag coating [13]. The fol-
obtain high-purity β-SiC. lowing chemical reactions will occur during the plating process:

Table 1 CH2 OH (CHOH ) 4 CHO + 2Ag (NH3)2 OH CH2 OH (CHOH ) 4

Reactant properties.
COONH4 + 2Ag + 3NH3 + H2 O
Reactant Manufacture Purity, %
The essence of electroless silver plating is the silver-mirror reaction of
Tetraethyl orthosilicate Macklin, China 99.0 glucose solution and silver salt solution. Finally, SiC coated by Ag NPs were
Ammonia solution Nanjing Reagent, China 99.7 prepared by AgNO3-glucose electroless silver plating system by adjusting
Ethanol absolute Sinopharm Chemical ReagentCo., Ltd 99.7
the Ag content (controlling the concentration of Ag) in the main salt.
Resorcinol Energy Chemical, China 99.0
Formaldehyde solution Nanjing Reagent, China 99.7 The advantage of SiC as a wave absorbent is not only due to its high
Sodium carbonate anhydrous Nanjing Reagent, China 99.7 dielectric loss, but also due to its excellent physical and chemical sta-
Nickel chloride hexahydrate Macklin, China 99.0 bility. Although the use of ordinary Ni and Cu metal coating can im-
Polyvinyl Pyrrolidone(K-30) Sinopharm Chemical Reagent Co., 99.7
prove the microwave absorption performance to a certain extent, the
Ltd
D(+)-Glucose Sinopharm Chemical ReagentCo., 99.0 properties of these metals are more active with poor thermal stability
Ltd, China and chemical corrosion resistance, which will have an adverse effect on
Tin(Ⅱ) chloride Energy Chemical, China 98.0 the comprehensive properties of SiC absorbent. As a stable metal, Ag
Silver nitrate Aladdin, China 99.0 can not only significantly change the overall dielectric property of SiC,
Ethanol absolute Sinopharm Chemical ReagentCo., 99.7
but also have little influence on other properties of SiC. The crystal
Ltd, China
Hydrochloric acid Aladdin, China 99.5 structure, surface functionality and thermally mass loss are firstly dis-
cussed, as can be seen in Fig. 2. The XRD patterns of the sample can be

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Table 2
Formulation composition.
Ag salt solution/1L AgNO3(g) ammonia solution deionized water pH
0.25, 0.5, 0.75, 1 5 mL 50 mL 11.5–12.5
Reducer solution/1L D(+)-Glucose(g) ethanol absolute deionized water temperature
15 100 mL 900 mL 30 °C

seen in Fig. 2-(a) showing the characteristic absorption peaks of 3C–SiC in the sensitization process. With the increase of Ag concentration, the
(111), (200), (220), and (311) crystal planes appeared at 2 particle size and number of Ag particles increased significantly. For Ag@
theta = 35.597°, 41.383°, 59.977°, and 71.777°, respectively. The ob- SiC (1.0 g/L), Ag NPs adhered to each other and tended to become
tained patterns are in good agreement with standard PDF. No. 04-29- membranes. The EDS spectrum also shows that with the increase of Ag
1129, indicating that the synthesized SiC mainly existed in β-crystal. concentration the intensity of characteristic absorption peak at 2.98 keV
For Ag coated samples, with the increase of Ag content, clutter and fine increases, confirming the increase of Ag content on SiC surface.
peak shape became more and more prominant, which is probably due to Fig. 4 shows the TEM image of Ag@SiC (0.75 g/L) and the SAED
the influence of partial poor crystallinity and defective Ag lattice. diffraction pattern. The crystal plane fringe has been calibrated in the
Meanwhile, (111), (200), (220), and (311) crystal planes of 3C–Ag HRTEM image. The coating of Ag NPs is basically uniform, and there is a
appeared at 2 theta = 38.116°, 44.277°, 64.426°, and 77.472°, respec- certain space between the particles to avoid the reflection caused by skin
tively, consistent with PDF. No. 04-04-0783. The peak intensity in- effect, as shown in Fig. 4-(a). From SAED pattern in Fig. 4-(b), the poly-
creased with the increase of Ag content, i.e., the Ag prepared by elec- crystalline diffraction rings of the (111) and (220) crystal planes from β-
troless plating was mainly 3C crystal. SiC are clearly visible, while the (111) and (200) crystal planes from the
From the FT-IR spectra shown in Fig. 2-(b), one can notice the ab- Ag single crystal speckle group are present. From HRTEM images of Fig. 4-
sorption peaks at 3423 cm-1 and 1628 cm-1 originating from the (c) and Fig. 4-(d), the lattice fringes show the (111) crystal faces of SiC and
stretching vibration of the H–O bond, the characteristic absorption peak Ag, respectively, the crystal grows mainly along the (111) crystal face.
of SiC appeared at 928 cm-1 and 810 cm-1, and the curve has almost no Fig. 5 shows the XPS spectrum of Ag@SiC (0.75 g/L). The composition
stray peaks. No other absorption peaks were observed, which proves that of the sample elements is shown in Fig. 5-(a), mainly including C, Si and
the prepared samples are highly pure. The possible absorption peak of Ag elements. It can be seen from the high resolution Ag XPS spectrum in
Ag–O bond at 753 cm-1 is almost unnoticeable in the figure, indicating Fig. 5-(b) that the characteristic absorption peak of Ag0 appears in
that wet and warm electroless plating will not oxidize the generated Ag 368.10 eV and 374.27 eV. Ag is mainly in the form of Ag elementary
NPs. Moreover, from the Tg curves of samples obtained in the tem- substance in 3d orbit, reflecting the strong antioxidant performance of Ag.
perature range of 50–800 °C, as shown in Fig. 2-(c), at the quantity
hardly changed; indicating that Ag has excellent thermal stability and 3.3. Electromagnetic performance analysis
will not affect the high temperature absorbent properties of SiC.
It is aknown fact that Ag has very low contact resistance compared
3.2. Micro morphology and crystal lattice structure with the semiconductor properties of β-SiC. When Ag is coated on the
surface of SiC, the overall dielectric property will change significantly,
The microstructural morphology of the samples obtained by SEM is which will increase a series of dielectric loss and affect the absorption
shown in Fig. 3. SiC prepared in this work mainly consists of irregular performance. However, excessive Ag content is easy to form a con-
block with particle size ranging from 1 to 10 μm. These structures with ductive network on the surface of the wave absorber, causing sig-
different particle sizes and shapes can provide more reflection, scattering nificant skin effect, skin depth reduction, and ultimately leading to a
points and attenuation times for electromagnetic waves. When Ag con- strong reflection of electromagnetic waves. Therefore, it is of great
centration was low, nano-sized Ag particles were formed on SiC surface significance to find an appropriate Ag content to suppress the reflection
and dispersed evenly, which was related to the pretreatment of Sn2+ ions effect of electromagnetic wave and increase the attenuation capacity at

Fig. 1. Preparation mechanism of Ag@SiC. Including four parts: (1) SiO2 prepared by hydrolysis of TEOS; (2) RF aerogel@SiO2 prepared by Sol-Gel method; (3) SiC
prepared by high temperature calcination; (4) Ag@SiC prepared by electroless plating.

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the same time. Microwave absorbing properties of the absorbent de-

pends on its electromagnetic parameters, including complex permit-
tivities (εr, εr = ε' - jε'') and complex permeabilities (μr, μr = μ' - jμ''),
where the real part represents its ability to store electromagnetic en-
ergy, and the imaginary part represents its ability to attenuate elec-
tromagnetic energy [14]. Reasonable combination of real part and
imaginary part of electromagnetic parameters can obtain good ab-
sorbing performance.
Fig. 6 shows the electromagnetic parameters of Ag@SiC prepared
with different Ag NPs concentrations. Fig. 6-(a) shows the real part of
the complex permittivities in the range of 2–18 GHz, the real part of the
complex permittivities of SiC prepared in this work fluctuates with
frequency from 9.2–6.1. With the increase of Ag content, the peak value
of the real part increases significantly and shows a dependence on Ag
content. The higher the Ag content leads the higher the real part, which
indicates that Ag is beneficial to enhance the material charge storage
property. Meanwhile, Ag@SiC shows a more obvious electrical dis-
persion effect, indicating that the dielectric property of Ag@SiC is more
responsive to the change of frequency. Fig. 6-(b) shows the imaginary
part of the complex permittivities and it can be seen that the value of
the imaginary part after Ag coating is significantly improved in the
whole frequency band. For Ag@SiC (1.0 g/L), the peak value increased
from 3.1 to 4.6, indicating that the dielectric attenuation performance
of electromagnetic wave has been significantly improved. Fig. 6-(c) and
Fig. 6-(d) show the real part and imaginary part of the complex per-
meabilities of samples, respectively. SiC as a nonmagnetic material, μ′ is
close to 1 and μ′′ is close to 0 in the whole frequency band. When the
surface of SiC is coated with different content of Ag, μ′ and μ′′ hardly
changes. Compared with dielectric loss, the contribution of magnetic
loss is negligible. Therefor, this work mainly discusses the influence of
Ag on the dielectric properties of SiC.
A good absorber should meet the requirements of electromagnetic
wave absorption and attenuation [15], which requires consideration of
the impedance matching and attenuation performance of the absorber.
Impedance matching rate can be expressed by equations (1)–(3) [16]:
Z0 Zin
R=
Z0 + Zin (1)

µr µ 0
Zin =
r 0 (2)

µ0
Z0 =
0 (3)

here R is the reflection coefficient, Z0 is the impedance of air, Zin is the

wave impedance at interface, μ0 and ε0 are vacuum permeability and
vacuum permittivity, respectively. It is generally recognized that the
impedance matching rate of the absorber should be greater than 0.3, so
that more electromagnetic waves can enter into the absorber for better
attenuation [17]. Fig. 7-(a) shows the relationship between impedance
matching rate and frequency of samples. The impedance matching ratio
of SiC is higher (~0.3) in the whole frequency band, which has a good
ability to allow electromagnetic wave to enter. The impedance matching
ratio reduces gradually with increasing contents of Ag NPs. For example,
for Ag@SiC (1.0 g/L), the peak value decreased from 0.42 to 0.32, and
the impedance matching ratio was less than 0.3 in a large range. This
result indicates that good conductor Ag would have an adverse effect on
the impedance matching performance of the absorber, which was more
obvious in the low frequency range with lower electromagnetic energy.
Further, the attenuation characteristics of the material can be
evaluated by attenuation coefficient α, as shown in equation (4) [18]:

2 f 2 2
= × (µ µ )+ (µ µ ) + (µ +µ )
Fig. 2. Basic performance characterization: (a) XRD patterns, (b) FT-IR spectra c (4)
and (c) Tg curves of samples.
here c is the speed of light in a vacuum. Fig. 7-(b) shows the relation-
ship between attenuation factor α and frequency of samples. The value

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Fig. 3. The micromorphology and element composition of samples. SEM images of (a) β-SiC; (b) Ag@SiC (0.25 g/L); (c) Ag@SiC (0.50 g/L); (d) Ag@SiC (0.75 g/L);
(e) Ag@SiC (1.0 g/L). (f) EDS spectra of all samples.

Fig. 4. Tem analysis and lattice fringe calibration of Ag@SiC (0.75 g/L): (a) TEM images; (b) SAED pattern; (c) HRTEM image of SiC; (d) HRTEM image of Ag.

Fig. 5. Element analysis of surface coating of Ag@SiC (0.75 g/L): (a) XPS spectra and (b) high resolution Ag XPS spectrum.

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Fig. 6. Electromagnetic parameters of samples: (a) Real part of permittivity (ε′); (b) Imaginary part of permittivity (ε′′); (c) Real part of permeability (μ′); (d)
Imaginary part of permeability (μ′′).

of the α peak of intrinsic SiC is about 156, which increases significantly interface polarization and dipole polarization [21]. Among them, the
specifically for higher Ag NPs contents. For example, for Ag@SiC degree of dipole polarization can be characterized by Cole-Cole semi-
(1.0 g/L) sample the peak value can reach 216. For nonmagnetic SiC circle.
and diamagnetic Ag, this attenuation of electromagnetic waves is due to According to debye relaxation model, the dielectric properties of
dielectric losses. Due to the poor dielectric performance of ordinary SiC, materials are characterized in the plural form [22]:
the loss mechanism generally comes from resistance loss and the at-
s
tenuation of electromagnetic wave is mainly caused by dielectric po- r = + = j
1 + j2 f (5)
larization and leakage conductivity loss [19,20]. The coating of Ag
significantly improves dielectric properties, enhances dielectric polar- here f is the microwave frequency; εr is the static permittivity, ε∞ is the
ization effect and conduction current intensity, and thus improves at- optical permittivity at the high frequency limit; τ is the relaxation cycle.
tenuation ability. The dielectric polarization effect can be divided into The expression of ε′, ε'' and tan δε can be derived from equation (5):

Fig. 7. Analysis of absorption and attenuation of electromagnetic wave: (a) Impedance matching ratio and (b) attenuation constant α of samples.

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= + s Ag coating can be seen visually from Fig. 8-(f), with the increase of Ag
1 + (2 f )2 2
(6) content, the value of tanδε first increases and then decreases. Moreover,
the peak value shifts towards the high frequency direction, indicating
2 f (s )
= that there is a limit to the increase of dielectric loss caused by Ag, and is
1 + (2 f ) 2 2 (7) not that the higher Ag content is beneficial to dielectric loss.
In addition to dipole polarization, Ag coating uniformity and Ag
( s )2 f lattice defects or impurities will significantly affect the Ag@SiC inter-
tan = =
s + (2 f )2 2
(8) face, enhancing the interface polarization effect. In addition, due to the
Equations (6) and (7) are known as Debye equations. The tanδε in greatly different dielectric properties of Ag and SiC, Maxwell-Wagner
equation (8) represent the dielectric loss. The expression of Cole-Cole effect [24] is significantly enhanced at the interface where the two are
semicircle can be obtained by canceling 2πf in equation (6) and equa- connected, leading to an increased degree of space charge accumula-
tion (7): tion. When the charge accumulates to a certain extent, an electric
current will be formed, and the pyroelectric transducer process will
( )2 + ( )2 = ( s ) (9) occur to promote the loss of electromagnetic energy. At the same time,
the good conductor property of Ag increases the overall conductivity,
In the Cole-Cole model, each semicircle represents a debye relaxa-
which provides favorable conditions for the conduction of current. In
tion process [23]. According to equations (8) and (9), tanδε and Cole-
conclusion, the improvement of dielectric loss ability with Ag@SiC
Cole semicircle of samples are plotted as shown in Fig. 8.
originates from the enhancement of dipole polarization, interface po-
As mentioned above, an increase in Ag content will lead to an in-
larization and conductivity loss.
crease in the real part of the complex permittivities. In the Cole-Cole
model, an increase in the real part will cause the range appearing in the
circular model to shift toward the high-frequency direction, as shown in 3.4. Reflection loss and absorption mechanism
Fig. 8-(a) ~ (e). The Cole-Cole model is similar in shape, indicating that
the dependence of SiC on electromagnetic wave absorption and fre- The properties of absorbing materials can be directly reflected by
quency does not change due to Ag coating. At the same time, the fre- reflection loss value (RL). The reflection loss of single-layer absorbing
quency range of Cole-Cole circle will increase significantly with the materials can be calculated by equation (10), (11) [25]:
increase of Ag content, that is, Ag coating makes dipole polarization
RL = 20 log (Zin 1)/(Zin + 1) (10)
increase in the region of 2–18 GHz band. The effect on dielectric loss of

Fig. 8. Typical Cole-Cole semicircles (a) ~ (e) and dielectric tangent loss (tanδε) (f) of samples.

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Fig. 9. Three-dimensional representation and two-dimensional representation of the values of reflection loss for samples: (a) ~ (b): SiC; (c) ~ (d) Ag@SiC (0.25 g/L);
(e) ~ (f) Ag@SiC (0.5 g/L); (g) ~ (h): Ag@SiC (0.75 g/L); (i) ~ (j) Ag@SiC (1.0 g/L).

Zin = µr / r tan h [j (2 fd )/c ] µr r (11) (a), (c), (e), (g) and (i) in Fig. 9, it can be found that Ag coating can
expand the absorption region of SiC to a certain extent. Furthermore the
where Zin is normalized input impedance of absorbing agent; d is the maximum reflection loss (RL) and effective absorption bandwidth are
thickness of the absorbing layer. It can be seen from equations (10) and also increased. At the same time, several peaks with excellent absorbing
(11) that the reflection loss has a quantitative relationship with the properties appear in the range of sufficient thickness. The higher the Ag
complex permittivities and complex permeabilities. content, the more the number of peaks appear, and the RL value in-
Fig. 9 shows two-dimensional as well as three-dimensional re- creased slightly. For instance, RL value can reach to −58.2 dB for Ag@
presentation of the values of reflection loss for samples. By comparing SiC (1.0 g/L) sample.

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Fig. 9. (continued)

Table 3 effective bandwidth and corresponding thickness of each sample are

Maximum effective bandwidth and corresponding thickness of each sample. shown in Table 3.
Ag@SiC /c (Ag) (g/L) 0 0.25 0.50 0.75 1.0 For Ag@SiC prepared in this work, the increase of εr is beneficial to
Tickness (mm) 2.5 2.4 2.3 1.8 1.6 decrease the thickness of the absorber, which is of great significance for
Effective bandwidth (GHz) 5.01 5.33 4.97 4.61 4.99 the lightweight of the absorber.
Fig. 10-(a) shows the relationship between RL value and frequency
of samples at a thickness of 2 mm. With the increase of Ag content, the
By comparing (b), (d), (f), (h) and (j) parts in Fig. 9, Ag coating can peak value of RL moved towards the low-frequency direction. Among
increase the effective absorption bandwidth, while a narrow area of them, Ag@SiC (0.25 g/L) has the maximum effective absorption
RL < −10 dB appears at the same time, which reflects the position of λ bandwidth of 4.68 GHz, and Ag@SiC (0.50 g/L) has the maximum RL
/4 wavelength. According to transmission line theory, a strong standing value of −41.62 dB. Considering RL and effective absorption band-
wave at λ /4 can form inside the absorbent resulting in interference and width, Ag@SiC (0.50 g/L) has the best performance at a thickness of
canceling out with the incident electromagnetic wave and thus creating 2 mm. Fig. 10-(b) shows the relationship between the RL value and
a significant attenuation effect. In addition, it can be concluded from frequency at different thickness of Ag@SiC (0.50g /L). In contrast to
two-dimensional model that the general law of reflection loss changes other reports [27,28], this work demonstrates a larger effective ab-
with frequency and thickness. This suggests that when the thickness of sorption bandwidth for lower the thickness of the wave absorber, which
absorbing layer increases, the peak value of reflection loss moves to- is due to the improvement of dielectric properties by Ag. It is easy to
wards the low frequency band. This peak displacement can be ex- form a conductive network in the inner part when the absorber is more
plained by the λ /4 equation [26]: thick, leading to the increase of electromagnetic wave reflection effect.
tm = n /4 = nc /4fm ( r µr )1/2 (12) At the same time, according to the analysis of equation (12) and Fig. 9,
the λ /4 wavelength of Ag@SiC appears at a lower thickness, which has
where λ is the wavelength; tm is the absorbent's matching thickness at a stronger attenuation effect on electromagnetic waves.
the best wave absorption performance; fm is the frequency corre- Fig. 11 shows the microwave absorption mechanism of Ag@SiC
sponding to permittivity and permeability. According to equation (12), structure. Under the electromagnetic field, Ag@SiC has a series of di-
the frequency fm of the same absorbent material decreases with the electric behaviors such as conductance loss, interface polarization and
increase of tm. In addition, the large values of εr is favorable for the dipole polarization. The coating of Ag NPs improves the dielectric
decrease of absorbent thickness; the estimated values of maximum

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Fig. 10. Performance comparison between different samples with the same thickness: (a) Reflection loss of samples at a thickness of 2.0 mm; Performance com-
parison of the same sample with different thickness: (b) Reflection loss of Ag@SiC (0.50 g/L) at different thickness.

properties and further enhances these attenuation effects, so as to ef- Table 4

fectively attenuate the incident electromagnetic wave. By adjusting the Reported microwave absorption properties of some recent absorbing compo-
content of silver, a balance between impedance matching and at- sites.
tenuation can be found to obtain the best absorption performance. Sample Optimal RL Absorption Thickness Ref.
In comparison to recent reports, the Ag@SiC (1.0 g/L) prepared in value (dB) bandwidth (mm)
this work achieves an effective absorption bandwidth of 4.99 GHz at (GHz)
1.6 mm, with optimal RL value of −36.3 dB, see Table 4. From this we
Co0.2Ni0.4Zn0.4Fe2O4/GN −53.5 4.8 3.1 [17]
can infer that Ag@SiC has obvious advantages on the matching thick- Ni(OH)2/biomass carbon −23.6 2.1 6.0 [29]
ness and it is a kind of light absorbent with good microwave absorption rGO/Ni −59.7 4.8 2.7 [30]
performance. Fe@Ni −22.7 5.5 2.0 [31]
Graphene/CoFe2O4/ −36.1 2.0 3.5 [32]
Y3Fe5O12
4. Conclusion NiFe2O4 −22.5 1.8 3.5 [33]
rGO/Ni0.5Zn0.5Fe2O4 −37.71 3.68 2.0 [34]
Carbon nanotube/Silica 22.0 4.2 4.0 [35]
In this work, we successfully prepare high purity β-SiC, Ag@SiC Ag@SiC −36.3 4.99 1.6 This
wave absorbers with different Ag contents aided with Sn2+ ion elec- work
troless silver plating. It was found that Ag NPs were mainly in 3C crystal
form with excellent thermal stability and oxidation resistance.

Fig. 11. Absorption mechanism of Ag@SiC. Ag coating leads to three improvements: Conductivity loss, interfacial polarization and dipole polarization.

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B. Wei, et al. Ceramics International xxx (xxxx) xxx–xxx

Meanwhile, Ag can improve the dielectric properties of SiC obviously. 4399–4403.

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Declaration of competing interest (2018) 385–389.
[17] P. Liu, Z. Yao, J. Zhou, Z. Yang, L.B. Kong, Small magnetic Co-doped NiZn ferrite/
graphene nanocomposites and their dual-region microwave absorption perfor-
The authors declare that they have no known competing financial
mance, J. Mater. Chem. C 4 (2016) 9738–9749.
interests or personal relationships that could have appeared to influ- [18] E.Q. Huang, J. Zhao, J.W. Zha, L. Zhang, R.J. Liao, Z.M. Dang, Preparation and
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