Journal of Alloys and Compounds 821 (2020) 153533

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Journal of Alloys and Compounds

journal homepage: http://www.elsevier.com/locate/jalcom

Preparation and investigation of epoxy/Li0.5AlxFe2.5-xO4

nanocomposites for electronic packaging applications
S.T. Assar a, *, H.F. Abosheiasha a, Diaa-Eldin A. Mansour b, M.A. Darwish c
a
Engineering Physics and Mathematics Department, Faculty of Engineering, Tanta University, Tanta, 31511, Egypt
b
Electrical Power and Machines Engineering Department, Faculty of Engineering, Tanta University, Tanta, 31511, Egypt
c
Physics Department, Faculty of Science, Tanta University, Tanta, 31527, Egypt

a r t i c l e i n f o a b s t r a c t

Article history: In recent years, there has been a growing demand for polymer-based multifunctional materials for
Received 1 October 2019 electronic packaging applications. For this purpose, epoxy/Li0.5AlxFe2.5-xO4 (95:5 wt%) nanocomposite
Received in revised form samples have been prepared, where (x ¼ 0, 0.15, 0.25, 0.35, and 0.45). The interface region between the
13 December 2019
epoxy and the inserted nanoferrite fillers plays a significant role in the interpretation of the properties of
Accepted 23 December 2019
Available online 24 December 2019
the nanocomposite samples according to the dual interface nanolayer model. The magnetic properties
(Ms, Mr, Hc) of the composite samples extracted from the M-H hysteresis loops, change with increasing
Al3þ ions content following the same trend as their corresponding pure ferrites counterparts, but with
Keywords:
Ferrites
lower values as expected. Whereas, the dielectric properties (sʹac, εʹ, and tand) almost increase. The
Epoxy dielectric strength and energy density are evaluated for the nanocomposite samples by using sphere to
Nanocomposites plane electrode configuration. The results of εʹ, tand, dielectric strength, energy density and the good
Magnetization magnetic properties of the composite samples, indicate that they are promising candidates for electronic
Dielectric behavior packaging applications as well as can serve as a typical EMI suppressor.
Impedance spectroscopy © 2019 Elsevier B.V. All rights reserved.

1. Introduction Therefore, they are used in several applications including electronic

In the last decade, there is a great interest to develop advanced
functional materials for different applications. Among different
functional materials, polymer-based nanocomposites are prom-
ising for many industrial applications due to their low cost and
comprehensive ability to combine the advantages of both polymer
and nanofiller components [1,2]. For example, the incorporation of
inorganic nanoparticles within specific polymers proved unex-
pected enhancements in the properties of the resultant nano-
composites, even at small weight fractions. These enhancements
were reflected positively on thermal properties such as thermal
conductivity [3], mechanical properties such as tensile strength and
flexural strength [4,5], optical properties such as refractive index
[6], and dielectric properties such as breakdown strength and
partial discharge [7]. Also, polymer nanocomposites can achieve
multiple enhancements in the properties mentioned above [8e10].
* Corresponding author.
E-mail addresses: s_talat@f-eng.tanta.edu.eg, sohatalaat73@gmail.com, soha_
talaat@yahoo.com (S.T. Assar), hatem_fouad@f-eng.tanta.edu.eg, hatemfouad72@
gmail.com (H.F. Abosheiasha).
packaging, optical shielding, electromagnetic radiation shielding,
energy storage, and dielectric industry. Among the different poly-
mer materials, epoxy resin is widely used as a promising polymer
due to its excellent properties, including thermal stability, little
shrinkage, high strength, and toughness. Accordingly, epoxy resin
has found large industrial applications such as adhesives, anti-
corrosion coatings, tissue substitutes, electronics, aerospace, and
so on. However, epoxy is still lacking some fundamental properties,
making it limited in its functionality. In order to overcome the
drawbacks of epoxy and introduce some new functionalities to it,
many researchers have focused on synthesizing the epoxy loaded
by different nanofillers such as carbon nanomaterials [11], metals
[12], metal oxides [13], nanoferrites [14], and nano-clay [15].
With focusing on the field of electronic packaging, epoxy com-
posites have been successfully applied for this field. The desired
dielectric characteristics for electronic packaging applications can
be summarized in high dielectric strength, low dielectric loss, and
low permittivity if it is intended for adhesive applications or as
interlayer dielectrics, and high permittivity if it is intended to
achieve a high capacitance for embedded passive applications. S.
Singha and M. Joy Thomas [16] had studied the dielectric properties

https://doi.org/10.1016/j.jallcom.2019.153533
0925-8388/© 2019 Elsevier B.V. All rights reserved.
2 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533
of Al2O3/epoxy nanocomposite for electronic packaging applica-
tions. They had found a reduction in permittivity and dielectric loss
for the epoxy that was filled by 0.1% of Al2O3 nanoparticles over a
wide frequency range, making it promising for electronic packaging
applications. However, in the same research, a decrement in
dielectric strength occurred for all the considered range of nano-
filler loading.
In fact, another type of inorganic metal oxide is ferrite. What
distinguishes ferrite more than other materials, in that it can be
considered as a functional material in itself as it has interesting
magnetic, dielectric, optical and chemical properties [17,18]. This
prompted many researchers to study intensively ferrite-based
epoxy nanocomposite [19,20]. According to our knowledge, no re-
ports have been found yet in the literature about the investigation
of the physical properties of epoxy/LieAl ferrite (EPX/LAF) nano-
composites. Therefore, the aim of the present work is to adding
different compositions of Al substituted Li-ferrite (Li0.5AlxFe2.5-xO4
(x: 0.0, 0.15, 0.25, 0.35, and 0.45)) into epoxy matrix with constant
loading (5 wt%) to improve their structural, thermal, magnetic, and
dielectric properties, where it is expected that they may be prom-
ising candidates for important practical applications such as elec-
tronic packaging.
2. Experimental
2.1. Samples preparation
2.1.1. Preparation of the ferrite nanoparticles
Nanoparticles of Li0.5AlxFe2.5-xO4 with x ¼ (0.0, 0.15, 0.25, 0.35,
and 0.45) have been prepared by using the citrate precursor
method. The preparation process was detailed in the previous
publication [21]. The characterization of nanoparticles has been
verified for the structure by using X-ray diffraction (XRD), Fourier
transform infrared spectroscopy (FTIR). Also, it has been verified for
morphology by using particle size analysis (PSA) and Transmission
Electron Microscopy (TEM).
2.1.2. Preparation of the epoxy sample
The pure epoxy (EPX) sample has been prepared as follows:
Firstly, the resin viscosity has been reduced through mixing 1 g of
diglycidyl ether of bisphenol A (DGEBA) with a proper amount of
tetrahydrofurane (THF). Secondly, 0.43 g of Triethylenetetramine
has been added to the mixture and stirred thoroughly before
dropping them into a glass dish. The dish has been treated by
dichloro di-methylsilane to avoid the adhesion of the mixture to
the glass surface. Finally, the mixture has been heated under vac-
uum at 60  C for 24 h, then at 110  C for 1 h.
2.1.3. Preparation of the composite samples
Each sample of the epoxy/Li0.5AlxFe2.5-xO4 (EPX/LAF) nano-
composite has been prepared by the following steps where the
weight ratios of epoxy to nanoferrite compositions is 95: 5 wt%. At
first, 0.05 g of the prepared nanoferrite composition and 0.66 g of
epoxy resin (DGEBA) has been mixed and dispersed in 5 ml of (THF)
by using mechanical stirring for 15 min followed by ultrasonication
for 1 h. Secondly, 0.29 g of Triethylenetetramine has been added to
the resultant mixture and mixed vigorously by hand for a 10 min,
then poured into the treated glass dish. This mixture has been
degassed at 40  C for 2 h to remove moisture and trapped air
bubbles formed during hardener mixing. Finally, the glass dish with
the material has been left for curing inside an evacuated oven by
exposing it to the same heat treatment mentioned above.
2.2. Characterization
The scanning electron microscope SEM (JEOL 5200-LV) has been
used to depict the micrograph images of the nanocomposite sam-
ples to investigate their morphological surface.
FTIR spectroscopy is a chemical analysis technique, which de-
tects the vibration characteristics (stretch, contract, bend, etc.) of
various chemical functional groups. In this study, the surface
chemistry of the EPX/LAF nanocomposites has been characterized
over a wave number ranging between 200 cm1 and 4000 cm1 by
a Bruker FTIR TENSOR 27.
Generally, the thermogravimetric analyzer (TGA) can be used to
characterize any material that exhibits a weight change due to
decomposition, oxidation, or dehydration. The TGA (PerkinElmer
STA 6000) has been used to characterize the mass change as a
function of temperature for the pure EPX and the selected EPX/LAF
(x ¼ 0.25) nanocomposite. To do that, about 20 mg of each sample
was put in the TGA sample pan and then was heated in an air at-
mosphere from room temperature to the desired temperature (up
to 450  C) at a rate of 10  C/min.
2.3. Magnetic and electrical measurements
The magnetic behavior of EPX/LAF nanocomposites has been
determined at room-temperature by using Lake Shore-7400
vibrating sample magnetometer (VSM), while the dielectric mea-
surements of their disk-shaped samples with a diameter of 15 mm
and thickness around 1 mm, have been executed by using Imped-
ance analyzer (Hioki 3570 LCR meter) at room temperature. The
details of this setup had been discussed elsewhere [22].
The AC breakdown voltage has been measured at 50 Hz by using
a 100 kV high voltage transformer. The configuration of the copper
electrodes was sphere to plane electrode. The sphere electrode has
a diameter of 2 cm, and the plane electrode has a thickness of 2 mm
and a diameter of 10 cm. The electrodes have been immersed into
an insulating oil as specified in ASTM D149-09 standard in order to
force the breakdown through the sample rather than along its
surface.
3. Results and discussion
3.1. Structural properties
The SEM micrograph of the EPX/LAF nanocomposite samples
from (x ¼ 0 to x ¼ 0.45) is shown from Fig. 1(a) to Fig. 1(e),
respectively. The images exhibit the morphological aspects of the
samples. It can be observed that spherical particles of the nano-
ferrites are embedded and encapsulated inside the epoxy matrix
indicating a good interfacial adhesion between these particles and
the epoxy resin. It is clear that most of the filler nanoferrite particles
are dispersed in the epoxy matrix, but some particles show an
agglomeration where they behave as tiny magnets have a perma-
nent magnetic moment proportional to their volume and tend to
aggregate to each other.
The interface region between epoxy and the inserted nano-
particles plays a significant role in interpreting the properties of the
nanocomposite. It is worth mentioning that, G. Tsagarapoulos et al.
[23], had suggested the dual interface nanolayer model (DINM) in
order to explain polymer nanocomposite interfacial behaviors.
They had reported that the inserted nanoparticles in the polymer
matrix covered by two nanolayers due to the interactions between
polymer chains and nanoparticles themselves. The first nanolayer is
the closest to the nanoparticle surface and linked tightly to it
confining the polymer chains in this region. The second polymer
nanolayer surrounds the first one with a slightly larger thickness. It
 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533 3

Fig. 1. The SEM micrograph of the EPX/LAF nanocomposites of (a) x ¼ 0.00, (b) x ¼ 0.15, (c) x ¼ 0.25, (d) x ¼ 0.35, and (e) x ¼ 0.45.

is characterized by loosely tied polymer chains. By using FTIR
spectroscopy, the chemical changes in the bulk of the nano-
composite can be identified indicating if there is a chemical reac-
tion between epoxy and nanoparticles or not. The FTIR spectra of
the unfilled epoxy and EPX/LAF composites are shown in Fig. 2. It
can be observed clearly from the FTIR spectra that insertion of LieAl
ferrite nanoparticles into the epoxy matrix does not lead to the
formation of new bonds. However, according to DINM, a specific
interaction is expected at the first interfacial nanolayer between the
nanoparticle surface and the epoxy chains. The type of bonding at
the interface region is shown in Fig. 3, where, Fig. 3(a) represents
the base epoxy resin while, Fig. 3(b) represents the hydrogen
bonding between OH groups on the nanoparticle surface and
epoxide groups in epoxy resin after mixing. The existence of the OH
group in the nanocomposite samples can be revealed from the
stretching vibrations around 3418 cm1, and 3063 cm1 as shown
from Fig. 2. Whereas, in the previous work [21], the existence of the
OH groups on the nanoferrite particles (fillers) have been shown
through the vibrations at the peaks around 3400 cm1. In the
previous work [16] it had been reported that OH groups could exist
in two forms on the nanoparticles. The first form represents the free
OH groups attached to the surface of nanoparticle, while the second
form is originated from OH groups attached to absorbed water
molecules on the surface. Most likely both forms exist. The
4 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533
Fig. 2. The FTIR spectra of the EPX and EPX/LAF nanocomposites.
multitude of free OH groups on the surfaces of the nanoparticles
results in the high density of hydrogen-bonded epoxy chains at the
region just close to the surfaces of the nanoparticles. This interprets
the formation of strongly bonded and tightly bound first nanolayer
of epoxy chains at the interface region according to the DINM.
By comparing the transmission peaks of the prepared nano-
composites together with the literature [24e27], the formation of
the desired samples has been confirmed. The absorption bands
around 2927 cm1 and 2868 cm1 correspond to an asymmetrical
CeH stretch of eCH3 group and eCH2 group, respectively, while the
bands around 3063 cm1 correspond to CeH stretch in aromatic.
Also, the bands around 828 cm1 correspond to eCH out of plane
deformation in aromatic. The absorption bands which are observed
around 1247 cm1, and 1182 cm1 are related to asymmetrical ar-
omatic, and asymmetrical aliphatic CeO stretch, respectively. These
absorption bands confirm the attachment of diethylene glycol
Fig. 3. The type of bonding at the interface region where, (a) the base epoxy resin, and (b) the hydrogen bonding between OH groups on the nanoparticle surface and epoxide.
around the particle surfaces. While the vibration bands around
1035 cm1 are related to CeN amino hardener, moreover, the C]C
stretching vibrations in aromatic are depicted around 1608 cm1,
1582 cm1, 1509 cm1 and 1453 cm1. In addition to that, it can be
seen clearly all the characteristic absorption bands assigned to
LieAl ferrites, which have been observed before in the FTIR spectra
of the corresponding pure nanoferrites particles. They have been
discussed in details [21], particularly, the absorption bands n1 and
n2 which are shown at about 586 cm1 and 397 cm1, respectively.
As it is known, the primary absorption band n1 is assigned to the
intrinsic stretching vibrations of Fe3þ-O2- in the tetrahedral sites,
whereas, n2 is attributed to the stretching vibrations of Fe3þ-O2- in
the octahedral sites.
The impact of the ferrite nanoparticles on the thermal stability
of the ferrite/epoxy nanocomposites has been investigated through
thermogravimetric analysis (TGA) as depicted in Fig. 4. The TG
curve EPX/LAF nanocomposite sample of x ¼ 0.25 was presented in
comparison of the neat epoxy at a heating rate of 10  C/min. The
results indicate that there is an early weight loss slightly higher
than 10% extending from ambient room temperature till around
300  C. Such weight loss step occurs due to two separate processes:
the first one is attributed to the decomposition of the unreacted
epoxy or other impurity traces apart from the cured resin [28]. The
second process is due to the evaporation of strongly bound adsor-
bed water molecules existed on the surface of the nanoparticles as
mentioned above. At higher temperatures reach to 380  C, the TGA
curves of the two examined samples reveal a single-steep weight
loss with an approximation decrease of 80%. This rapid mass loss
was anticipated due to the chain scission and resin decomposition,
resulting in fragmentation of the resin into low molecular weight
products [29]. Concerning the EPX and EPX/LAF (x ¼ 0.25) nano-
composite sample, the obtained net weight losses curve reveals
that after the addition of amounts of this ferrite nanoparticles to the
epoxy matrix, the decomposition temperature shifted toward
lower temperatures. This may be due to the existence of some
agglomerated particles which have permanent magnetic moment
 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533 5

Table 1
The magnetic parameters of the hysteresis curves for the EPX/LAF nanocomposites.

Al content Ms Hc Mr Sq Ls

x (emu/cm2) (G) (emu/cm2) (Mr/Ms) (erg/cm2)

0.00 0.37 135.4 0.11 0.30 169.6

0.15 0.29 146.5 0.07 0.24 133.0
0.25 0.29 144.5 0.07 0.24 128.7
0.35 0.23 138.9 0.06 0.26 98.8
0.45 0.23 141.8 0.05 0.23 95.6

Fig. 4. The TGA curves of the EPX and EPX/LAF (x ¼ 0.25) nanocomposite.
as mentioned above, where, it is known from the literature [30]
that, the rightward shift of TG curve of epoxy/nanoparticles com-
posite shows improved thermal stability. This may be due to the
improved dispersion of nanoparticles in epoxy matrix, while the
occurrence of leftward shift of TG curve depicts decreased thermal
stability due to the aggregation of nanoparticles which affect the
degree of their dispersion in the epoxy matrix.
3.2. Magnetic properties
The M-H curves of VSM results of the composite samples are
shown in Fig. 5, while the values of the saturation magnetization
Ms, remnant magnetization Mr coercivity Hc, squareness ratio Sq,
and total area under curve Ls (magnetic losses) are shown in Table 1.
It can be seen that the M-H curves of the composite samples show
S-shaped form with small coercive force as well as the corre-
sponding pure ferrite samples counterparts [21] where the
magnetization for various samples exhibit linear changes at lower
fields and is kept constant at higher fields. The smaller coercive
force for these samples makes them capable of being magnetized
and demagnetized easily, along with having low magnetic loss Ls.
This sort of properties indicates that these samples can be classified
as soft magnetic materials which are typical for low loss and
inductor applications [31] as well as electromagnetic interference
(EMI) suppression applications [32], where, it had been reported
that the low value of Hc (few hundred oersteds) is one of the
necessary conditions of EM materials which can serve as EMI
suppressor [20].
From the results of the previous work [21], it had been shown
that Ms and Mr as well as mexp decrease with increasing Al3þ ions
content. This is attributed to the effect of many factors such as the
decrease of the particle sizes and the measured densities of the
samples which accompanied with high specific surface area, be-
sides the effect of the cation distribution. Thus, it is expected that
Ms and Mr of the nanocomposite samples exhibit the same
behavior. According to the following equation [14]:
Ms ¼ f ms (1)
Where Ms is related to the volume fraction of the magnetic particles
f and the saturation magnetic moment of a single particle ms. As
the volume fractions of the filler particles are constant (5 wt%), and
ms decreases as mexp of the pure ferrite fillers decreases. So, it is
logical that Ms and Mr of the nanocomposite samples decrease with
the increment of Al3þ ions content. Also, they are lower than the
corresponding values of the pure ferrite samples counterparts as
expected. That is because a small mass fraction of the magnetic
nanoparticles is impeded in the nonmagnetic epoxy polymer ma-
trix, which increases the probability of dead layer existence of
disordered spins and non-collinearity of magnetic moments in the
first nanolayers closest to the magnetic nanoparticles surfaces at
the interface region between the magnetic nanoparticles and the
epoxy chains. From Table 1, it can be noticed that Ms and Mr, (in
emu/cm2) decreases significantly with high increasing of Al3þ
content. It is also clear that the Hc of the composite samples
changes in the same trend as the corresponding pure ferrite
counterparts, but with lower values where, the sample of x ¼ 0.15
has the greatest Hc value. It is known from literature that Hc, Ms and
K1 are related by the following relation [32]:

Hc ¼ 0.96K1/Ms (2)

As it is discussed before [21], the first increase of the Hc is

Fig. 5. The hysteresis loops of the EPX/LAF nanocomposites.
attributed to the prominent effect of Ms, which decreases by
increasing Alþ3 ions content. Then the reduction of Hc despite the
decrease of Ms results from the dominant effect of the decrease of
the anisotropy constant K1 as a consequence of the reduction of
Fe3þ ions contribution by the addition of nonmagnetic Al3þ ions.
Nevertheless, regarding the lower values of Hc of the composite
samples compared to their pure ferrite counterparts, this can be
explained as follows: It is known from the literature [33] that the
resultant anisotropy of magnetic materials arises from a combina-
tion of magneto-crystalline anisotropy, surface anisotropy, and
inter-particle interactions. When the fillers of ferrite nanoparticles
6 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533

are inserted in the epoxy matrix, on the one hand, this leads the
inter-particle distances increase, which weakens inter-particle in-
teractions. On the other hand, the interaction between the polymer
chains and the magnetic nanoparticles contributes in decreasing
their surface anisotropy, accordingly the resultant anisotropy de-
creases, causing the decrease of Hc of the composite ferrite samples
more than their pure ferrite counterparts.
The values of Sq of the composite samples show almost the same
behavior of their pure ferrite counterparts, but with lower values,
where they decrease with the increment of the Al3þ ions. This is
attributed to the decrease of their Mr and the dependence of Sq on
the resultant anisotropy, which in turn decreases as mentioned
above. The loss of magnetic energy in the form of heat is a serious
problem facing the magnetic materials used in the high-frequency
band. The magnetic losses Ls of the nanocomposite samples can be
depicted from the area under M-H curve. From Table 1, the Ls of the
nanocomposite samples have the same trend of their pure ferrites
counterparts but show very lower values than them. This is
ascribed to that the values of Hc and Ms of the composite samples
are lower than their pure ferrite counterparts.

Fig. 7. The variation of ε’ versus frequency for the EPX and EPX/LAF nanocomposites.
3.3. Dielectric properties

The frequency dependence of ac conductivity s’ac, dielectric

permittivity ε’, dielectric losses ε’’ , and dielectric loss factor tan d for
the neat EPX and EPX loaded with 5 wt% of LAF are shown in Figs. 6-
9, respectively. For all the samples, the values of s’ac show almost
constant values approach to zero at low frequencies then increase
obviously at high frequencies. In contrast, ε’ , ε’’ , and tan d decrease
rapidly at low frequencies, while at high frequencies they become
approximately frequency independent. Generally, the dielectric
response of polymer-based composites depends on three distinct
dielectric relaxation processes. The first process is interfacial po-
larization (IP) known as Maxwell-Wagner-Sillars (MWS) effect
[34e36]. It is recorded at lower frequencies and regarded as slower
process having longer relaxation time occurs in heterogeneous
systems. The second relaxation process is called a-relaxation. It is
recorded at intermediate frequency range having shorter relaxation
time compared to IP. It arises through the simultaneous segmental
motion of large parts of the macromolecular chains resulting from
the glass to rubber transition of the amorphous polymer matrix.
The third process is b-relaxation which is the standard dipolar

Fig. 8. The variation of ε’’ versus frequency for the EPX and EPX/LAF nanocomposites.

effect mode (IDE). It is a relatively weak mechanism occurs at high

frequencies and arises due to the reorientation of polar side groups
of the main polymer chains [37]. From the above dielectric results,
which are taken at room temperature, and depending on the cor-
relation between the polarization process and conduction mecha-
nism, the predominant relaxation process in these nanocomposite
samples is IP (MWS effect) which describes the s’ac in the hetero-
geneous structure materials. It is well known that [38], in low
frequencies range, surface, interfacial space charge, and orientation
polarizations play a prevalent role among different polarization
processes in determining the dielectric properties of heterogeneous
materials such as ferrites and epoxy. In nanoferrite particles, sur-
face polarization shows a finite contribution, where it exhibits an
initial high value that falling-off rapidly as it cannot follow the high
frequencies of the applied electric field. This is evidenced by the
high ε’ , ε’’ , and tan d values which drop promptly with increasing
frequency. In the present case, the dielectric relaxation of the
composite samples arises from the epoxy and filler of AleLi
Fig. 6. The frequency dependence of s’ac for the EPX and EPX/LAF nanocomposites.
 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533
Fig. 9. The variation of tan d versus frequency for the EPX and EPX/LAF
nanocomposites.
nanoferrites contributions. In the case of epoxy, the dielectric
constant is determined by the total number of oriental dipoles and
their ability to orient under the effect of an applied electric field
[39]. Usually, the molecular groups which are attached perpen-
dicular to the longitudinal polymer chain effect in the dielectric
relaxation mechanisms. At lower frequencies of the applied electric
field, all the free dipolar functional groups in the epoxy chain can
orient themselves resulting in higher values of ε’ , consequently, ε’’ ,
and tan d at those lower frequencies. As the frequency increases,
although the s’ac of the heavier dipolar groups increases, they find it
difficult to orient themselves at the same direction of the alter-
nating field, so the contributions of these dipolar groups to the
polarization cease causing a continuous decreasing of the ε’ , ε’’ , and
tan d of the matrix system at those frequencies [15]. In the case of
ferrites, according to their heterogeneous structure, the charge
carriers accumulate at the interfacial areas between grain and grain
boundary systems. When charge carriers reach the grain bound-
aries through the electron hopping between (Fe3þ 4 Fe2þ), they
will accumulate due to the high resistivity of the grain boundaries
producing IP. So, at lower frequencies the resistive grain boundaries
are more effective while, at higher frequencies the conductive
ferrite grains are more effective causing an increase of s’ac with
increasing frequency. At lower frequencies, the electron hopping
between (Fe3þ 4 Fe2þ) can follow the orientation of the applied
field causing the high value of ε’ , and thus the values of ε’’ , and tan d
are also high. Then, at higher frequencies, the dielectric dispersion
arises from the inability of the hopping charge carriers to follow the
alternation of the applied field. The decreasing effect for both epoxy
matrix and filler ferrite in their ε’, ε’’ , and tan d results in a subse-
quent decrease in these characteristics for the composite samples
when the frequency of the applied field increases. It can be
concluded that the values of effective permittivity and dielectric
losses in EPX/LAF nanocomposites are governed by IP at the epoxy-
nanoparticle interfaces.
From Fig. 6, it can be seen that s’ac value of the composite
samples is higher than the unfilled EPX sample except for the
sample of x ¼ 0.15. Moreover, although the volume fraction of the
nanoferrite fillers is constant in all the nanocomposite samples
(5 wt %), the value of the s’ac almost increases by increasing Al3þ
ions in the LAF (fillers). These results are contrary to what is
7
expected. As per the suggested cation distribution of these nano-
ferrite samples [21], the higher substitution of Al3þ ions in B-sites
decreases the content of Fe3þ ions which causes decreasing the
electron hopping (Fe3þ 4 Fe2þ) consequently, decreases the s’ac .
These interesting results can be ascribed to the effect of two factors:
the first one is the value of specific surface area of the ferrite
nanoparticles interfaced to the EPX segments. The second one is the
nature of bonding at the interface region. In the previous work [21],
it was found that the average particle sizes decrease as the Al3þ ions
increase, and subsequently the overall specific surface area in-
creases. This will lead to an increase in the contacting areas be-
tween the EPX segments and the ferrite nanoparticles,
consequently increases the interactions at the interface regions.
Actually, Zhang et al. [40] had reported that there is an increase in
the electrical conductivity of the interface region due to the for-
mation of hydrogen bonds at this region with a subsequent
improvement in the mobility of charge carriers. Accordingly, the
obtained conductivity results for the investigated nanocomposites
confirm the formation of hydrogen bonding at the first nanolayer of
the interface region as per the DINM. Also, the second nanolayer of
the interface region is electrically conductive. The loose nature of
the EPX material will allow the existence of high mobility free
charge carriers due to impurities [16]. Therefore, it can be predicted
that the electrical conductivity in the interface region of the EPX-
nanocomposite is higher as compared to the unfilled EPX where
there are no interactions between epoxy segments and nano-
particles. Regarding the composite sample of x ¼ 0.15, which
exhibited a lower s’ac value than the unfilled EPX on the contrary to
the other samples, it can be explained as follows. The high content
of defects may be presented in the second nanolayers of the loose
EPX in this composite sample leads to the formation of charge
trapping sites causing high probabilities of charge trapping and
charge neutralizations [16]. That is besides that the nano AleLi
ferrite filler (x ¼ 0.15) in this composite sample has a relatively
small specific surface area which means the existence of small
interacting regions between epoxy and nanofillers.
Furthermore, it is clear that ε’’ (see Fig. 8) and tan d (see Fig. 9)
have the same trend of s’ac regarding the effect of Al3þ ions content.
This is logically expected, science dielectric losses ε’’ of a material is
directly proportional to its s’ac as shown in the following relation
[41]:
s’ac
ε’’ ¼ (3)
uε o
Also, tan d of a material is directly related to the dielectric losses
ε’’ as follows [41]:
ε’’
tan d ¼ (4)
ε’
where it represents the ratio between the dissipation energy dur-
ing the polarization process to the stored energy arises from the
dielectric polarization. Although, the composite sample of
(x ¼ 0.45) has the highest dielectric losses ε’’ , it exhibits a reduction
in its tan d than the other samples. This is due to the stored energy
in this composite sample is higher than the dissipation energy
during the polarization process. From Fig. 7 it can be noticed that ε’
of the composite samples shows almost the same trend of s’ac
variation with increasing Al3þ ions content where the maximum
value is obtained in the sample of x ¼ 0.45 and the minimum one in
that of x ¼ 0.15. This confirms the strong correlation between po-
larization and conduction process in heterogeneous materials such
as the present composite samples.
From the above results, at the frequency of 5 MHz, the ε’ of the
8 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533

unfilled EPX is 8.31, then it decreases until reach 3.19 for the
composite sample of x ¼ 0.15, then it increases again to reach
17.52 at x ¼ 0.45. It is worth mentioning that, Santanu Singha and
M. Joy Thomas [16] had found that at frequency of 1 GHz, ε’ of the
unfilled EPX was 3.45 and decreased to reach only 3.10 for the
sample of 0.1% Al2O3 filled nanocomposite. As for tand in the pre-
sent work, the composite samples of x ¼ 0.0 and 0.15 have values
around 0.5 then, tand decreases to reach around 0.30 for the sam-
ples from x ¼ 0.25 to 0.45 which is regarded closer to the value of
the EPX sample (0.23). It can be said that the nanocomposite
samples can be designed with enhancements in some properties
with a compromise on other properties depending on the re-
quirements of the application. The lower values of ε’ and tand in the
nanocomposite samples, especially the sample of x ¼ 0.15, making
them promising candidates for electronic packaging applications
particularly that requires lower values of permittivity and tand.
Electric modulus formalism is regarded as a powerful tool and
provides an insight into the relaxation processes of the material
characterized by the smallest capacitance. Also, it can be used to
suppress the unwanted effects of extrinsic relaxation, electrode
polarization, adsorbed impurities, etc.. The complex electric
modulus M*(u) is obtained as follows [41]:

1
M * ð uÞ ¼ ¼ M’ ðuÞ þ iM’’ ðuÞ (5)
ε* ðuÞ

where ε*(u) is the complex permittivity. So, the real part M ’ (u) and
the imaginary part M’’ (u) of the electrical modulus can be repre-
sented in the following forms [42]:

ε ’ ð uÞ
M ’ ðuÞ ¼ 2 2
(6)
ε ’ ð uÞ þ ε’’ ðuÞ

ε’’ ðuÞ
M ’’ ðuÞ ¼ (7)
’2
ε ðuÞ þ ε’’ ðuÞ
2

Fig. 10 (a) illustrates the M ’ values of the composite samples. In

the low-frequency region below 1 kHz, they are almost constant
and approach zero; then they start increasing at the middle fre-
quencies, after that reach maximum at high frequencies, which
confirm suppressing the electrode polarization. The high values of
M ’ at high frequencies are attributed to the low values of ε’ and
diminishing the polarization when the dipoles fail to follow the fast
changes in the applied electric field. The values of M ’ almost
decrease with increasing Al3þ ions indicating the enhanced het-
erogeneity of the composite samples except for the sample of
x ¼ 0.15 as mentioned above. Moreover, in the Mʺ curves shown in
Fig. 10 (b), a relaxation peak is observed which depends on the
conduction process, and it was not evident from the ε’’ curves. In
these composite samples, the peaks of Mʺ curves correspond to the
prominent MWS relaxation and represent the transition point from
long-range to short-range mobility with increasing the frequency
[12]. The relaxation time constant tM’’ of the samples which is
max
determined at the relaxation peak of Mʺ is shown in Table 2. The
increase of Al3þ ions in the filler ferrite nanoparticles decreases the
Mʺ peaks values and shifts them to higher frequencies except for
the sample of x ¼ 0.15. This is attributed to the increase in the ac
conductivity which arises from the mobility increase of the charge
carriers of the fillers and the dipolar parts of the epoxy macro-
molecules causing a diminish in their relaxation times. The Cole-
Cole (Mʹ-Mʺ) plots of the composite nanosamples are shown in
Fig. 11. It can be noticed that all the semicircles start from the origin,
indicating that there is no blocking charge layer at the interface
with electrodes [12]. This means that the electrode polarization can
Fig. 10. The variation of (a) M ’ and (b) M ’’ versus frequency for the EPX and EPX/LAF
nanocomposites.
be neglected. The (Mʹ-Mʺ) formalism of each sample shows three
semicircles, two completely overlapping semicircles appear as one
arc and suggest a presence of different relaxation processes arise
from effective grain boundary (at low frequencies) and effective
grain (at relatively high frequencies) contributions which have
comparable capacitance values; and another suppressed semicircle
revealing the presence of intermediate dipolar relaxation effect (at
very high frequencies) [42]. As the centers of the semicircles lay
below the x-axis, this indicates the non-Debye type of relaxation of
these composite samples. The asymmetry of the arcs particularly in
the low-frequency region (where hump is observed) manifests the
dominance of MWS relaxation. The variation in radius of the
semicircles is attributed to the difference of the capacitance and
heterogeneity in each sample which has a constant content (wt. 5%)
of a different composition of the nanoferrite fillers.
In this work, the impedance spectroscopy effective method (IS)
has been used to reveal the correlation between the dielectric
properties of the composite samples and their interior structure.
The frequency dependence of the real Z ’ (resistive part) and
imaginary Z ’’ (reactive part) of the complex impedance of the
nanocomposite samples is shown in Fig. 12(a) and Fig. 12(b),
respectively. It can be observed that as the frequency increases, the
values of Z ’ of the nanocomposite samples show as expected the
 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533 9

Table 2
The electrical parameters of the EG and EGB for the EPX and EPX/LAF nanocomposites.

Al Content, x Reg Ceg teg Regb Cegb tegb tZ 00 tM00

max max

EPX/LAF(x) (MU) (pF) -4

(x10 s) (MU) (pF) -4
(x10 s) (x10 s) -4
(x10-4s)

0 0.70 44.8 1.97 1.15 28.0 2.02 2.29 1.00

0.15 0.88 17.7 0.98 1.80 10.3 1.16 1.05 0.50
0.25 0.34 36.2 0.78 0.40 32.6 0.82 0.90 0.50
0.35 0.25 66.5 1.03 0.31 58.9 1.14 1.39 0.02
0.45 0.03 93.3 0.19 - - - 0.46 0.004
EPX 2.80 21.0 3.69 5.65 12.1 4.28 3.33 2.22

Fig. 11. The Cole-Cole (Mʹ-Mʺ) plots for the EPX and EPX/LAF nanocomposites.

reverse trend of the ac conductivity where they have high constant

values up to 1 kHz, then decreases significantly up to 100 kHz, after
that show a slight decrease approaches to zero. In the case of Z ’’ ,
their values increase until they reach maximum Z ’’max then they
decrease again. This can be explained depending on two competed
factors affect the imaginary impedance of the samples (where, Z ’’ is
almost inversely proportional to the frequency and capacitance of a
dielectric material). At the low-frequency region, when the polar-
ization has pronounced effect, diminishing the capacitance of the
samples has the dominant effect causing the increment of Z ’’ . Then,
Z ’’ reaches a maximum value Z ’’max at the relaxation frequency,
when the natural frequency of the dipoles coincides with the fre-
quency of the applied field and the capacitance of the samples
reaches minimum value. The relaxation time tZ ’’ of the samples
determined at Z ’’max is shown in Table 2. At high frequencies, the
max

capacitance of the samples has weak effect where, their interfacial

polarization ceases and cannot follow the orientations of the
applied electric field, so, Z ’’ decreases again by increasing the fre-
quency. It is worth mentioning that the variation of the Z ’ and the
Z ’’max values of the composite samples with different Al3þ ions in the
LAF (fillers) shows the reverse trend of the variation of the ac
conductivity and dielectric constant as expected.
The Nyquist plots (Zʹ-Zʺ) of the nanocomposite samples are
shown in Fig. 13. All the samples exhibit two overlapping incom-
plete semicircles with centers lay below the x-axis, indicating the
non-Debye type of relaxation process. The relative position of the
semicircles depends upon their electrical parameters. They repre-
sent the conduction of poor conducting regions at low frequencies
and well conducting regions at high frequencies which can be
Fig. 12. The variation of (a) Z ’ and (b) Z ’’ versus frequency for the EPX and EPX/LAF
nanocomposites.
regarded as effective grains’ boundaries (EGB) and effective grains
(EG), respectively. The variation of the semicircle diameters in-
dicates the variation of the internal resistance of the EGB and EG of
the composite samples. From the obtained results, the overall
response of the composite samples can be approximately modelled
by two parallel ReC equivalent circuits in series. The different
electrical parameters: resistance R, capacitance C, and relaxation
time constant t of the EGB (Regb, Cegb, and tegb) and EG (Reg, Ceg, and
teg) have been extracted from the analysis of (Zʹ-Zʺ) plots and their
values are listed in Table 2.
10 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533

This can be interpreted depending on the fact that the modulus plot
picks out the phenomenon of the smallest capacitance (i.e. the
highly conductive part), while the impedance plot highlights the
relaxation dynamics of the largest resistance [44].
It is worthily mentioned that, Sinclair and West [45] had re-
ported that if the peaks of Mʺ and Zʺ versus f will occur at the same
frequency, then the relaxation process is long-range, and if they will
occur at different frequencies, then the process is localized.
Consequently, from the foregoing results, i.e. the broadening of the
peaks of Mʺ and Zʺ versus f and their occurrence at different fre-
quencies (as manifested from the difference of their relaxation time
constants tM’’ and tZ ’’ ), so, it can be concluded that, in these
max max
nanocomposite samples, the relaxation processes are localized and
of a non-Debye type.

3.4. Breakdown voltage and energy storage

The breakdown voltage has been measured for the different

samples using the sphere to plane electrode configuration. For the
sake of comparison of dielectric strength among the different
Fig. 13. The Cole-Cole (Zʹ-Zʺ) plots for the EPX and EPX/LAF nanocomposites. samples, the electrode configuration has been simulated in COM-
SOL Multiphysics, and the electric field distribution has been drawn
for the measured breakdown voltage using finite element method
For all the composite samples, as it is expected, it can be noticed
(FEM). Fig. 14 shows the electric field distribution for the neat EPX
that the resistance Reg is lower than Regb. In contrast, the capaci-
sample. The highest electric field at the sphere electrode tip has
tance Ceg is higher than Cegb where the disordered arrangement of
been obtained and compared for all the samples. The thickness of
the atoms near the grain boundary region causes an electron
all samples is different. Since the electric field is dependent on the
scattering increment. Also, the relaxation time constant of the teg is
sample thickness, the results have been normalized to 1 mm
shorter than tegb, where, the longer relaxation time is accompanied
thickness using the inverse power low relationships described in
by, the higher resistance. As the Al3þ ions content of the ferrite
Ref. [46] for EPX and EPX/LAF nanocomposites. The results are
fillers increasing, the variation of both Reg and Regb explains the
depicted in Fig. 15. The electric field strength for the neat EPX
variation of the ac conductivity of the composite samples.
sample is 7.2 kV/mm. After adding the nanoferrite fillers, the
Furthermore, the variation of both Ceg, and Cegb is in good agree-
electric field strength values decrease below that of the neat EPX
ment with the variation of the dielectric constant of the samples.
sample with increasing Al3þ ions content up to the composite
For example, it is found that the resistance (i.e. Reg and Regb) of the
sample of x ¼ 0.15, then increase again where the composite
nanocomposite samples is lower than the neat epoxy sample,
sample of x ¼ 0.35 almost has the same value of that of the neat EPX
while, their capacitance (i.e. Ceg, and Cegb) is higher than it, except
sample. Further increase of Al3þ ions contents up to x ¼ 0.45 results
for the sample of x ¼ 0.15. Also, the sample of x ¼ 0.45 has the
in a dramatic increase in electric field strength which is attained
lowest resistivity (i.e. Reg and Regb) and the highest capacitance (i.e.
18.4 kV/mm. These results can be explained as follows: For the
Ceg, and Cegb) as manifested in the previous results. Accordingly, it
measurement of electric field strength, the level of applied voltage
can be said that the values of the electrical components of the
is much higher than that applied for dielectric measurements.
nanocomposites equivalent circuits reflect a visible image for the
Therefore, the mobility of charge carriers for EPX/LAF nano-
material and interpret the dielectric properties of them.
composite samples of x ¼ 0 and x ¼ 0.15 will be extremely
By looking carefully in Figs. 11 and 13, it can be noticed the two
improved causing a decrement in dielectric strength compared to
different shapes of the Nyquist plots of (Mʹ-Mʺ) and (Zʹ-Zʺ).
the neat EPX. When Al3þ ions content increases, the crystallite size
Generally, it is known from literature [43] that, the (Mʹ-Mʺ)
decreases [21], resulting in a significant increase in the interface
modulus formalism is more effective than (Zʹ-Zʺ) impedance
region between the nanoparticles and polymer matrix. Accordingly,
formalism for its ability to separate minutely the different relaxa-
the breakdown mechanism becomes dominated by the role of
tion processes like a relaxation due to grain and grain boundary as
interface region. The first nanolayer of DINM weakens the propa-
well as other relaxation effects, as it has been observed in the
gation of the discharge channel through it, while the second
present nanocomposite samples. Furthermore, the relaxation of the
nanolayer of DINM acts as a rigid structure around the surface of
electric field in the materials is also denoted by the electric
the nanoparticles [47] causing a complete energy loss of discharge
modulus since the electric displacement remains constant [44].
channel making it follows a zigzag path [48]. This results in an

Fig. 14. Electric field distribution for neat epoxy sample for sphere to plane electrode.
 S.T. Assar et al. / Journal of Alloys and Compounds 821 (2020) 153533
Fig. 15. Electric field strength for the EPX and EPX/LAF nanocomposites.
elongation of the channel and improvement in breakdown
strength. Moreover, the significant increase in permittivity after
increasing the Al3þ ions content causes discharges to be concen-
trated on a strong nanoparticles region rather than weak polymer
matrix.
The increase in dielectric strength is reflected positively on the
energy density of EPX/LAF nanocomposites. The energy density
results are depicted in Fig. 16 as a function of electric field up to the
maximum electric field strength for each sample. The energy
density of the neat EPX sample is the lowest one, where the
decrement in the electric field strength for the composite samples
of x ¼ 0 and x ¼ 0.15 is compensated by the increase in permittivity.
The energy density increases slightly with increasing the content of
Al3þ ions. However, for the composite sample of x ¼ 0.45, an
extreme increase in energy density has occurred, where at this
content both permittivity and dielectric strength increase signifi-
cantly. The energy density that can be obtained in this sample is
2.8 J/cm3.
4. Conclusions
In this work, constant loading (5 wt%) of different compositions
of AleLi ferrites have been dispersed in the epoxy matrix. The
structural, magnetic, and dielectric properties of those nano-
composites have been studied. The FTIR spectra have confirmed the
formation of the investigated nanocomposite samples. The
Fig. 16. Energy density against electric field for the EPX and EPX/LAF nanocomposites.
11
stretching vibrations around 3418 cm1 and 3063 cm1 reveal the
existence of the OH group on the surfaces of the nanoparticles,
causing the high density of hydrogen-bonded epoxy chains at the
region just close to the surfaces of the nanoparticles.
The S-shaped M-H curves of the composite samples with small
Hc and Ls, classify them as typical soft magnetic materials which
may be used in low loss and inductor applications as well as EMI
suppression applications. It is worth mentioning too that despite
the constant value of AleLi ferrites loading, the Ms, Mr, Hc, Sq, and Ls
of the composite samples almost decrease with increasing Al3þ ions
following the same trend of the pure ferrites counterparts but with
lower values. This finding is mainly attributed to the increment of
the nonmagnetic Al3þ ions at the expense of the magnetic Fe3þ ions
in the ferrite fillers.
The frequency dependence behavior of the s’ac , εʹ, and εʹʹ with
the addition of Al3þ ions content has been discussed depending on
the dual interface nanolayer model (DINM). From the dielectric
results taken at room temperature, and depending on the correla-
tion between the polarization process and conduction mechanism,
the predominant relaxation process in these samples is suggested
to be the interfacial polarization (IP) known as Maxwell-Wagner-
Sillars (MWS) effect. The overall electrical response of the com-
posite samples has been represented by two parallel ReC equiva-
lent circuits in series where their electrical parameters have been
extracted from the analysis of (Zʹ-Zʺ) plots. Finally, it can be
concluded that the lower values of the εʹ and tand, the good
breakdown strength and energy density, and the good magnetic
properties of the present nanocomposite samples; all these factors
indicate that these samples are promising candidates for electronic
packaging applications and also can serve as EMI suppressors.
Author contributions
S.T. Assar: Conceptualization, Investigation, Writing - original
draft, Writing - review and editing. H.F.Abosheiasha: Investigation,
Project administration, Funding acquisition. Diaa-Eldin A. Mansour:
Investigation, Writing - original draft. M.A. Darwish: Methodology,
Investigation, Validation.
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.
Acknowledgement
This work is financially supported by the Project (code No. TU-5-
15-3) which is funded by Research Fund at Tanta University, Egypt.
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