Ceramics International 47 (2021) 18246–18251

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

Ferrite ceramic filled poly-dimethylsiloxane composite with enhanced

magnetic-dielectric properties as substrate material for flexible electronics
Fang Xu a, *, Yan Yang b, c, Yonggang Liu a, Jing Yang a, d, Yulong Liao c, Xueying Wang c,
Xiaolei Shi c, Jianbo Hu a, d, **
a
State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang, 621010, China
b
College of Communication Engineering, Chengdu University of Information Technology, Chengdu, 610225, China
c
State Key Laboratory of Electronic Thin Film and Integrated Devices, University of Electronic Science and Technology of China, Chengdu, 610054, China
d
Laboratory for Shock Wave and Detonation Physics, Institute of Fluid Physics, China Academy of Engineering Physics, Mianyang, 621900, China

A R T I C L E I N F O A B S T R A C T

Keywords: Improving magnetic-dielectric properties of polymer materials, through filler of functional ceramics, provides
Flexible electronics feasibility to develop high-frequency flexible electronics. Poly-dimethylsiloxane (PDMS), an inert silicone with
High-frequency low elasticity modulus and high transparency, has been considered a promising candidate for flexible electronics.
PDMS matrix
Current PDMS matrix used in high-frequency devices suffers from unsatisfactory properties due to very low
Magnetic ferrite
dielectric constant. In this study, using ultrasonic stirring and vacuum-pumping process, we prepare a series of
xCo2Z/PDMS (x = 2; 4; 6; 8; 10) composite films, which are consisted of PDMS matrix and different quantity of
micro-sized ferrite particles. XRD pattern indicates that the obtained ferrite particles include Co2Z main phase
and BaM second phase. We demonstrate that 4Co2Z/PDMS film has improved magnetic-dielectric properties at
800 MHz (μ’ = 1.49; ε’ = 4.54 tanδμ = 0.058; tanδε = 0.008). Also, the film has high saturation magnetization (σ s
= 17.51 emu/g). Furthermore, SEM micrographs show that using ultrasonic stirring and fast curing, the micro-
sized ferrite particles are well dispersed in PDMS matrix. Our study, which provides a simple method to improve
high-frequency magnetic and dielectric properties of PDMS matrix, could pave the way for development of high-
frequency flexible electronics.

1. Introduction
Inspired by the noticeable magnetoelectricity of ferrite ceramics,
studies of magnetic material have given rise to the spring up of polymer
composites, which is used as candidates of flexible electronic [1–3].
Among the diverse ferrite ceramics, hexagonal ferrite is a key material
for microwave/GHz electronic components, due to excellent magnetic
and dielectric properties [4,5]. For instance, the permeability (μ′ ) and
cut-off frequency of Z-type Ba3Co2Fe24O41 (Co2Z) hexaferrite can be
controlled through different methods, such as microstructure modula­
tion, ceramic doping and templated grain growth [6–8]. Motivated by
these researches, experimental studies have demonstrated that the Co2Z
ferrite particles have positive influences on high-frequency properties of
some polymer materials [8–10]. For example, Cheng et al. using
micron-sized Co2Z particles to adjust magnetic and dielectric properties
of polyimide (PI) via in-situ polymerization process [9]. Results indi­
cated that the obtained Co2Z/PI composites possessed good perfor­
mances at MHz, which are new candidates for antenna applications.
That is to say, the hexaferrite ceramic is an alternative material to
improve magnetic properties of polymer materials.
To date, flexible electronics fabricated through a stretchable sub­
strate or matrix have attracted much interest for next generation elec­
tronics [11,12]. However, for flexible polymer materials, the
disadvantages of low permeability (μ′ ) and permittivity (ε′ ) seriously
limit their high-frequency applications, especially for flexible GHz an­
tenna. In our previous experiment, we have fabricated and demon­
strated a transient antenna on PVA/TiO2 film substrate [13]. Although
the antenna presents good radiation performance, the antenna has large
size at working frequency (~2.5 GHz) due to very low permittivity and
miniaturization factor. To solve this problem, Inui et al. have proved

* Corresponding author.
** Corresponding author. State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang, 621010,
China.
E-mail addresses: fxu2331@gmail.com (F. Xu), jianbo.hu@caep.cn (J. Hu).

https://doi.org/10.1016/j.ceramint.2021.03.144
Received 14 December 2020; Received in revised form 25 January 2021; Accepted 15 March 2021
Available online 18 March 2021
0272-8842/© 2021 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
F. Xu et al. Ceramics International 47 (2021) 18246–18251

Table 1
Mass ratio of ferrite particles and PDMS in xCo2Z/PDMS composite films.
Sample PDMS precursor(g) curing agent(g) ferrite particles(g)

2Co2Z/PDMS 5.0 0.5 2.0

4Co2Z/PDMS 5.0 0.5 4.0
6Co2Z/PDMS 5.0 0.5 6.0
8Co2Z/PDMS 5.0 0.5 8.0
10Co2Z/PDMS 5.0 0.5 10.0

that using high-dielectric-constant filler could enhance dielectric prop­

erties of substrate and reduce antenna size [14]. In a word, improving
permittivity and permeability has great significance for extended ap­
plications of polymer matrix, especially for high-frequency electronics.
In this work, we use poly-dimethylsiloxane film as matrix due to its
good elastic property [15–17]. To improve its dielectric and magnetic
properties, the micron-sized Co2Z particles synthesized by solid phase
method are dispersed uniformly through ultrasonic stirring and fast
curing treatment. Strikingly, our measurements directly reveal the
magnetic ferrite particles have great effects on permittivity of PDMS
matrix. Moreover, the obtained Co2Z/PDMS films have large perme­
ability although the working frequency more than 1.0 GHz. Fig. 1. Phase structure of the obtained ferrite particles. The XRD pattern
includes Co2Z main phase (asterisk) and BaM second phase (hollow circle).
2. Experimental section

2.1. Materials

Analytically pure raw materials of BaCo3, Co3O4 and Fe2O3 are

provided by Aladdin Reagent Co., Ltd (Shanghai, China). PDMS pre­
cursor and curing agent (10:1, Sylgard 184) are purchased from Dow
Corning (Midland, Michigan, USA).

2.2. Synthesis of ferrite particles

Firstly, the high-performance ferrite particles are synthesized by

solid phase method at ~1250 ◦ C [18]. In detail, according to molar ratio
of 9:2:36, the powders of BaCO3, Co3O4 and Fe2O3 are weighted and
mixed using ball-milling method. Next, these oxide materials are
pre-sintered at 1200 ◦ C for 2.0 h. After that, the powders are granulated
using PVA binder and are pressed into toroidal samples at ~10 MPa.
Finally, the as-obtained ferrites are sintered at 1250 ◦ C for 4 h. Through
grinding and centrifugal treatment, we obtain micron-size ferrite
particles.

2.3. Preparation of xCo2Z/PDMS composite film

The xCo2Z/PDMS composite films, which are consisted of PDMS

matrix and different quantity of micro-sized ferrite particles, are pre­ Fig. 2. Microstructure of the ferrite particles. The hexagonal shapes of Co2Z
phase are destroyed. The BaM ferrite particles (red circles) are observed in the
pared by mechanical mixing method. Firstly, through centrifugation and
FESEM micrograph, scale bar is 20 μm. (For interpretation of the references to
ultrasonic treatment, we have removed most of impurities and abnor­
colour in this figure legend, the reader is referred to the Web version of
mally larger particles. In Table 1, according to mass ratio of 5:0.5:x (x =
this article.)
2, 4, 6, 8, and 10), the PDMS precursor, curing agent and ferrite particles
are weight and blended. These samples are labeled as xCo2Z/PDMS,
using a vibrating sample magnetometer (EZ7, Quantum Design, USA).
respectively. Using vacuum drying oven, the air bubbles on the above
All the tests are carried out under room temperature.
mixtures are removed before the curing. At last, the xCo2Z/PDMS
composite film are obtained when cured at 100 ◦ C.
3. Results and discussions

2.4. Characterization
XRD pattern of the obtained ferrite is obtained by X-ray diffraction
using Cu Kα radiation (SmartLab, Rigaku, Japan). Microstructure of
ferrite particles and xCo2Z/PDMS composite films are observed by field
emission scanning electron microscope (Quanta 250 FEG, FEI, USA).
Frequency-dependent magnetic and dielectric spectra of the composites
are obtained by Impedance Analyzer (E4991B, Agilent, USA). Magne­
tization curves of the xCo2Z/PDMS composite films are investigated by
3.1. Structure and magnetic-dielectric properties of the obtained ferrite
particles
Phase composition of the obtained ferrite particles is shown in Fig. 1.
It can be seen that the ferrite particle exhibits a Co2Z main phase, which
is marked with an asterisk. However, we can observe an unremarkable
difference between the XRD pattern and standard Co2Z ferrite card
(PDF#19-0097). Our analysis indicates that, through comparison with

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Fig. 3. Magnetic and dielectric parameters of the bulk ferrite: frequency-dependent of (a) permeability μ′ and magnetic loss tanδμ and (b) permittivity ε′ and
dielectric loss tanδε. Results indicate that the ferrite possess high magnetic and dielectric properties and low loss at high frequency.

Fig. 4. Fracture surface of the xCo2Z/PDMS composites: FESEM micrograph of samples (a) 2Co2Z/PDMS; (b) 4Co2Z/PDMS; (c) 6Co2Z/PDMS and (d) 8Co2Z/
PDMS. All the samples have dense microstructure. Scale bar of insert is 20 μm.

other similar PDF cards, the impurity peaks (hollow circle) belong to ferrite particles, the morphology characteristic is revealed in Fig. 2. Due
BaM ferrite phase (PDF#39-1433). More importantly, due to anisotropic to grinding and centrifugal treatment, hexagonal shapes of Co2Z phase
of the BaM phase, we notice obvious increase in (0014) and (0018) are destroyed (seeing Fig. S1). A phenomenon is that the morphology of
peaks [8]. To further discuss composition and structure of the magnetic these particles is diverse, which is significantly different from spinel

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Fig. 5. Magnetic and dielectric spectra of the xCo2Z/PDMS composite films: (a) permeability (μ′ ); (b) permittivity (ε′ ); (c) magnetic loss tanδμ and (d) dielectric
loss tanδε. The values of μ′ and ε′ increase obviously with the increase of x. The films possess low loss at wide frequency range.
ferrites [19,20]. Through aborative observation, we can find out BaM
ferrite particle marked by red circles [21,22]. In a word, through anal­
ysis and discussion of phase composition and microstructure, we
demonstrate that the obtained ferrite particles are constituted of Co2Z
main phase and BaM second phase.
Frequency-dependent magnetic and dielectric parameters of the
ferrite are revealed in Fig. 3. In Fig. 3a, the bulk ferrite possesses high
real permeability (μ’ = 10.6) and low magnetic loss (tanδμ = 0.04) at
100 MHz. Moreover, the permeability of ferrite maintains the high value
at 1.0 GHz, which means cut-off frequency of the ferrite more than 1.0
GHz. Fig. 3b shows the changes of dielectric constant (ε′ ) and loss (tanδε)
of the ferrite. Results reveal that the value of ε′ and tanδε are ~14.2 and
~0.035 within a wide frequency range, respectively. However, there is a
small peak when frequency more than 1.0 GHz, which is similar with
previous reports [23,24]. Compared to other spinel ferrite, the obtained
ferrite possess better high-frequency magnetic performance, which
could be a suitable candidate to improving magnetic-dielectric perfor­
mance of polymer materials [25–27].
3.2. Structure of xCo2Z/PDMS composite film
Fracture surface morphologies of xCo2Z/PDMS composite films are
shown in Fig. 4. Zoom in are inserted in right-hand corner. A common
characteristic is that all films possess compact structure due to remove of
air bubble. However, with the increase of the ferrite particle, the frac­
ture surface of the film is getting worse. In Fig. 4d and Fig. S2, cracks
start to appear when mass of ferrite particles more than 8.0. In the
previous literature, Xie et al. demonstrated that proper ferrite filled
PDMS film has good elastic properties [28]. In our experiment, we can
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see that the films (revealed in Fig. 4a and b) keep good microstructure.
In addition, no obvious particle aggregation is observed in the composite
films.
3.3. Magnetic and dielectric spectra of xCo2Z/PDMS composite film
Frequency-dependent magnetic and dielectric spectra of the xCo2Z/
PDMS composite films are revealed in Fig. 5. In Fig. 5a, the permeability
(μ′ ) of the samples gradually increase along with the increase of mass of
ferrite particles. Moreover, improvement of working frequency results in
deterioration of μ’. A reliable explanation is that boundary of ferrite are
replaced by non-magnetic PDMS, which leads to decrease of perme­
ability of bulk ferrite (see Fig. 3a). Fig. 5b shows changes of permittivity
of the composites. Based on effective medium theory (EMT), we can
predict increasing trend of dielectric constant (ε′ ). Results indicate that
the ε′ of composite film not only is nearly twice as much as PDMS film,
but present stable and low dielectric loss value at wide frequency range.
The above results indicate that the obtained ferrite is a good filler to
flexible PDMS matrix for high-frequency application. Loss parameters of
the films, including magnetic and dielectric loss, are displayed in Fig. 5c
and d. For the magnetic loss, it presents a similar trend with Fig. 5a, i.e.,
lower μ′ possess lower magnetic loss. A difference is that the influence of
ferrite particle on magnetic loss is less than permeability. In Fig. 5d, the
effect of ferrite on dielectric loss of the composite is negligible when
frequency lower than 500 MHz. A reason is that the ferrite has low
dielectric loss, as shown in Fig. 3b. Thus, control of dielectric loss is key
for the composite film. Through analysis and discussion, we demonstrate
that the high-frequency loss of the composite films is mainly from
magnetic loss. Compared with PDMS composite films filled by LiZnTi or
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Fig. 6. Hysteresis loops of the xCo2Z/PDMS composite films: (a) x = 2.0; (b) x = 4.0; (c) x = 6.0; (d) x = 8.0; (e) x = 10.0 and (f) value of saturation
magnetization. The films exhibit same loop with the bulk ferrite.

NiCuZn ferrite [19,20], the PDMS film filled by Co2Z ferrite possess composite films.
lower magnetic loss. Thus, enhancing high-frequency magnetic prop­
erties of ferrite is effective method to lower loss of ferrite/PDMS 3.4. Magnetization curves of xCo2Z/PDMS composite film

Fig. 6 shows hysteresis loops of the xCo2Z/PDMS composite films.

Table 2 The films exhibit same loop with the bulk ferrite [7]. Due to
Magnetic and dielectric parameters of xCo2Z/PDMS composites at 800 MHz. non-magnetic characteristic of the PDMS, the magnetization of the films
Sample ε’ μ’ tanδε tanδμ is derived from ferrite material. Fig. 6f shows that magnetization state of
the xCo2Z/PDMS films reached saturation when magnetic field more
2Co2Z/PDMS 4.22 1.25 0.007 0.028
4Co2Z/PDMS 4.54 1.49 0.008 0.058 than ~3500 Oe. In detail, the value of saturation magnetization
6Co2Z/PDMS 4.91 1.74 0.009 0.037 monotonically increases from 11.17 emu/g to 26.03 emu/g.
8Co2Z/PDMS 5.41 2.11 0.010 0.031
10Co2Z/PDMS 5.99 2.34 0.013 0.059

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3.5. Discussions
The rapid development of flexible electronics is attracting widely
interests for next generation electronics, especially wearable electronics.
However, most of flexible materials, such as polymer materials, possess
very low high-frequency magnetic and dielectric properties, such as
permeability and permittivity. Here, we firstly synthesize one type
ferrite at ~1250 ◦ C by solid phase method. In Table 2, through filler of
the ferrite particles, we obviously enhance high-frequency magnetic-
dielectric properties of the PDMS matrix. In detail, the values of ε′ , μ′ ,
tanδε and tanδμ of 4Co2Z/PDMS sample are 4.54, 1.49, 0.008 and 0.058,
respectively. Thus, ferrite particle with optimized magnetic properties is
a promising candidate for flexible electronics.
4. Conclusion
We have investigated the frequency dependence of magnetic and
dielectric spectra in xCo2Z/PDMS composite films obtained by ultra­
sonic stirring and vacuum-pumping process. It is found that the micron-
size magnetic particles dispersed in PDMS matrix have the capability of
improving its permittivity and magnetic properties at high frequency,
which indicating the magnetic ferrite particles could be an alternative
filler of polymer-matrix. Moreover, the 4Co2Z/PDMS composite film
exhibits enhanced performance at 800 MHz (ε’ = 4.54, μ’ = 1.49, tanδε
= 0.008 and tanδμ = 0.058). Thus, these results present in this work
could pave the way for further studies on flexible electronics applied for
high-frequency applications.
Declaration of competing 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.
Acknowledgments
This work was financially supported by Key Research and Develop­
ment Projects of Sichuan Science and Technology Plan (No.
2021YFG0223), Project of Southwest University of Science and Tech­
nology (No. 20zx7101), National Natural Science Foundation of China
of China (No. 61971094), Project of State Key Laboratory of
Environment-friendly Energy Materials, Southwest University of Science
and Technology (No. 18fksy0209).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.ceramint.2021.03.144.
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