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IEEE TRANSACTIONS ON MAGNETICS 1

Analysis of Magnetic Losses and Complex Permeability in Novel


Soft Magnetic Composite With Ferrite Nanofibers
L’. Ďáková1, J. Füzer1 , S. Dobák 1 , P. Kollár1 , Y. Osadchuk1, M. Strečková2, M. Fáberová2,
R. Bureš2 , P. Kurek2 , and M. Vojtko2
1 Faculty of Science, Institute of Physics, Pavol Jozef Šafárik University, 041 54 Košice, Slovakia
2 Institute of Materials Research, Slovak Academy of Sciences, 040 01 Košice, Slovakia

This paper investigated the magnetic properties of novel soft magnetic composite (SMC) with ferrite nanofibers. Material consists
of FeSi powder covered by resin and different amounts of Ni0.3 Zn0.7 Fe2 O4 ferrite nanofibers. We prepared SMC with very high
specific electrical resistivity. FeSi/resin (0.49 wt% ferrite) sample exhibits the highest electrical resistivity (6.05 ·m) due to low
interparticle contacts. The image analysis of SEM pictures was used for the evaluation of effective area, in which local eddy currents
are flowing. The FeSi/resin (0.49 wt% ferrite) sample displays the lowest total losses in the measured frequency range due to the
highest specific electrical resistivity and appropriately covered FeSi particles. Loss separation and the analysis of movable magnetic
objects were performed for all studied materials.
Index Terms— Magnetic losses, magnetic properties, powder metallurgy, soft magnetic materials.

I. I NTRODUCTION magnetic permeability at frequencies of interest for possible


SMC applications [6]. Total losses of SMCs with various
S OFT magnetic composites (SMCs) are used in the elec-
trical equipment as transformers, electric motors, sensors,
low-frequency filters, etc. The amount of energy dissipated
ferromagnetic and insulation materials have been studied by
Wu et al. [7], de la Barrière et al. [8], [9], Taghvaei et al. [10],
during the magnetization cycle is one of the important char- Ďáková et al. [11], Lauda et al. [12], Birčáková et al. [13].
acteristics of magnetic materials. Hysteresis loss contribution de la Barrière et al. [8] have experimentally found that total
in SMCs is higher than that in electrical steel laminations, but magnetic losses may depend on the sample cross-sectional area
they can offer low total losses at high frequencies due to low S only in the sufficiently large cores (S > 5 mm×5 mm) of the
eddy currents. SMCs are applied in the frequency range from resistivity of a few 10−4 ·m or lower. This effect is related
several tens of hertz to few tens of kilohertz. These materials to the rising macroscopic eddy current contribution with the
exhibit several advantages including the 3-D isotropic structure sample cross section. In smaller samples of this resistivity,
in the bulk, low total losses at high frequencies, and SMCs eddy current paths are well-confined to the microscopic scale
can be produced in desired shapes and sizes by pressing of individual particles or their clusters and macroscopic term
technology. SMC consists of ferromagnetic powder particles can be disregarded. Bertotti [14] has found that with increasing
surrounded by an electrical insulating layer [1]. Addition of frequency, there is a linear increase of number of active mag-
insulating material is an important part of the manufacturing netic objects (MOs) (i.e., domain walls) in various materials.
process. The task of suitable electrical insulating material is In this paper, FeSi powder was insulated by a mixture of
to improve the electrical resistivity of SMC and to reduce boron phenol–formaldehyde resin and Ni0.3 Zn0.7 Fe2 O4 ferrite
eddy current losses due to negligible interparticle junctions. nanofibers. The bulk samples were prepared by the compaction
The advantages of organic material insulation are the simple under high pressure to form the ring-shaped cores for the
coating process and uniform insulation of particles. These investigation of electrical and magnetic properties. The com-
properties lead to higher electrical resistivity of powder bulk posites exhibit very high electrical resistivity in comparison
core. The main disadvantage of resin is a low thermal sta- with the other SMCs found in [2], [3], and [10]. The image
bility [2]. The inorganic coating material possesses sufficient analysis was applied to SEM photographs of bulk samples to
thermal resistance for removing internal stresses created during find the average area of ferromagnetic clusters and accordingly
the pressing; however, there are brittleness of compacts and calculate the eddy current loss contribution.
peeling of insulation layer leading to the metal-on-metal
contacts. Nowadays, some authors use ferrite as an inorganic II. E XPERIMENT
insulation of powder particles [2]–[5]. Mn–Zn, Ni–Zn, and
The ferromagnetic component of prepared SMC was
Ni ferrites possess appropriate properties such as very high
FeSi powder available by Höganäs Corporation. FeSi
electrical resistivity, low eddy current losses, and superior
powder was coated by 3 wt% phenol–formaldehyde
Manuscript received April 11, 2018; revised July 12, 2018; resin enriched by boron (PFRB). The molar ratio of
accepted August 19, 2018. Corresponding author: S. Dobák (e-mail: phenol/formaldehyde/ammonia/boric acid was set to
samuel.dobak@student.upjs.sk). 1/1.5/0.35/0.1. PFRB resin synthesis was described in [15]
Color versions of one or more of the figures in this paper are available
online at http://ieeexplore.ieee.org. and [16]. The Ni0.2 Zn0.8 Fe2 O4 fibers were made of 7
Digital Object Identifier 10.1109/TMAG.2018.2866814 wt% solution of polyvinyl alcohol with Ni(NO3 )2 ·6H2 O,
0018-9464 © 2018 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission.
See http://www.ieee.org/publications_standards/publications/rights/index.html for more information.
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2 IEEE TRANSACTIONS ON MAGNETICS

TABLE I
P HYSICAL P ROPERTIES OF C OMPOSITES , D ENSITY δ, S PECIFIC E LECTRICAL R ESISTIVITY ρ, C OERCIVITY Hc ,
H YSTERESIS L OSS Wh , AND AVERAGE C LUSTER A REA S

Zn(NO3)2 ·6H2 O, and Fe(NO3 )3 ·9H2 O. The molar ratio of


Ni2+ /Zn2+ /Fe3+ was 0.3/0.7/2. Ferrite was prepared by
a needle-less electrospinning technology by a Nanospider
NS Laboratory (ELMARCO) from polyvinyl alcohol/metal
nitrates solution. Electrospun nanofibers were dried at
90 °C for 15 min and then annealed at 800 °C for 4 h.
Ni0.3 Zn0.7 Fe2 O4 fibers were added to the resin. Prepared
samples consisted of different portions of ferrite nanofibers
in resin. PFRB resin contained 0, 0.24, 0.49, and 1.46 wt%
of Ni0.3 Zn0.7 Fe2 O4 fibers, respectively. Powder with resin
was pressed into the ring and cylinder shapes under the
uniaxial pressure of 600 MPa. The ring dimensions were as
follows: the outer diameter of 24 mm, the inner diameter
of 17 mm, and the height of 2 mm. The cylinders had Fig. 1. SEM image of FeSi/resin sample with bounded cluster areas of FeSi
the dimensions: the diameter of 10 mm and the height particles.
of 2 mm. Green-pressed composites were slowly cured up to
220 °C. The toroidal shape was used for the measurements
of specific electrical resistivity, total magnetic losses, and hysteresis loss and coercivity. Sample FeSi/resin (0.49 wt%
complex permeability. Cylindrical samples were used for ferrite) has the lowest hysteresis loss and coercivity and the
the coercivity measurements. Specific electrical resistivity lowest average area of ferromagnetic clusters due to the best
was measured by a standard four-point method. Real and homogenization of resin in the sample supported by ferrite
imaginary parts of complex permeability were measured by nanofiber reinforcement.
an impedance analyzer (HP4194A) in the frequency range For the calculation of eddy current losses inside the ferro-
from 1 kHz to 40 MHz. Total losses were measured at the magnetic particles, it is necessary to know the area, in which
peak magnetic induction Bmax = 0.1 T. The dc hysteresis the eddy currents flow. The powder clusters may be created
loops were measured by a dc flux meter-based hysteresis in the compression process. For that reason, SEM images
graph. Hysteresis loss was determined as an area of a were subjected to an extensive ImageJ software analysis
quasi-dc hysteresis loop in J/m3 . The ac hysteresis loops were to determine the average area of the cluster related to the
measured by an AMH-1K-S hysteresis graph in the frequency area where the eddy currents flow. After the image analy-
interval from 100 Hz to 1.2 kHz and by a MATS-2010SA sis, the average cluster area was determined, and individ-
permeameter in the frequency range from 1 to 37 kHz. ual ferromagnetic particles and their clusters are shown in
Fig. 1 (red).
III. R ESULTS AND D ISCUSSION In Fig. 2, size and number of clusters are compared for
Density, specific electrical resistivity ρ, coercivity Hc , each sample. It is obvious that the composition of dielectric
hysteresis loss Wh , and average cross-sectional area S of part influences the clustering of FeSi powders. FeSi/resin
the ferromagnetic component of samples are summarized (0.49 wt% ferrite) sample consists of the largest number of
in Table I. The specific electrical resistivity of the composite small clusters [Fig. 2(c)]. It is because of the properly coated
samples is very high in comparison with previously studied particles. This sample shows the highest measured specific
composites (5.5 × 10−5 ·m [17], 1.1 ·m [18], 1.28 × electrical resistivity of the studied composites.
10−6 ·m [19], and 8.53 × 10−6 ·m [20]) and also high in The real part of complex permeability depends on the
comparison with Fe–6.5 wt% Si/MnZn(Fe2O4 )2 powder core density; sample FeSi/resin (1.46 wt% ferrite) achieves the
(2.9 × 10−5 ·m) [21]. Sample FeSi/resin (0.49 wt% ferrite) highest real part of complex permeability (59 at a frequency
exhibits the highest specific electrical resistivity (6.05 ·m) of 1 MHz, Fig. 3). Samples FeSi/resin, FeSi/resin (0.24 wt%
and the lowest cluster cross-sectional area while the sample ferrite), and FeSi/resin (0.49 wt% ferrite) do not attain their
FeSi/resin (1.46 wt% ferrite) the highest density. Hysteresis relaxation frequency in measured frequency range due to
loss and coercivity depend on the structure of the ferro- high specific electrical resistivity. Composite with 1.46 wt%
magnetic component. Impurities in the materials hinder the ferrite in resin has a relaxation frequency at 15.2 MHz
movement of the domain walls and cause the increase of (Fig. 4).
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ĎÁKOVÁ et al.: ANALYSIS OF MAGNETIC LOSSES AND COMPLEX PERMEABILITY IN NOVEL SMC 3

Fig. 2. Number of clusters with their average cross-sectional area. (a) FeSi/resin. (b) FeSi/resin (0.24 wt% ferrite). (c) FeSi/resin (0.49 wt% ferrite). (d)
FeSi/resin (1.46 wt% ferrite).

Fig. 3. Frequency dependencies of the real part of complex permeability.


Fig. 4. Frequency dependencies of the imaginary part of complex perme-
ability.
Total losses were measured at Bmax = 0.1 T with quasi-
static and alternating magnetization in the frequency range by the effective dimension, in which eddy currents flow in
from 100 Hz to 37 kHz. Sample FeSi/resin (0.49 wt% ferrite) the cross section of the sample. In SMC, there are two
has the lowest losses due to the lowest hysteresis loss, low different paths for eddy currents, inside particles and between
coercivity, and high specific electrical resistivity (Fig. 5). particles (due to damaged insulation). Wexc originate in the
The one key property of magnetic materials is energy eddy currents generated by the movement of the domain walls,
dissipated during the magnetization cycle. Total losses can be hence depend on the domain structure.
divided into three components, namely, hysteresis losses Wh , According to [8], the eddy current losses inside the ferro-
eddy current losses Wclass , and excess losses Wexc . The intra were calculated as
magnetic particles Wclass
stress in ferromagnetic particles generated during the pressing  T  2
process leads to the creation of pinning centers which block 1 dB
Wclass =
intra
K (R)S dt (1)
the movement of the domain walls [1]. Wclass are determined ρFeSi 0 dt
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4 IEEE TRANSACTIONS ON MAGNETICS

Bertotti’s statistical approach leads to the conclusion that


the behavior of magnetic domains can be described by the
dynamic term n of the statistically independent MOs, where
each corresponds to a group of neighboring interacting domain
walls. This reduces the loss study to the investigation of the
properties of n as a function of f and B [14]. According
to this theory, excess losses arise from the compensation of
inhomogeneous internal counterfield by an applied magnetic
field. The number n of activated objects is related to the excess
field Hexc [22].
The number of active MOs per area depending on Hexc
was calculated according to [14] and [22] using the following
relations:
n 16 GB2max f
= (3)
S Wexc ρFeSi
Fig. 5. Dependence of total magnetic losses on frequency at Bmax = 0.1 T.
Wexc
Hexc = (4)
TABLE II
4 Bmax
FeSi PARTICLE A SPECT R ATIO R where n is the number of simultaneously activated MOs,
G = 0.1356, Bmax is the maximum magnetic induction, S is
the sample cross-sectional area, f is the frequency, Wexc are
the eddy current losses caused by the movement of domain
walls, ρFeSi is the FeSi specific electrical resistivity, and Hexc
is the excess field acting on a domain wall that is dynamically
where ρFeSi is the specific electrical resistivity of FeSi parti- applied against mesoscopic eddy currents (i.e., eddy currents
cles, K (R) is the function of a FeSi particle aspect ratio R, near the domain walls) [9]. Since the ferrite amount was
R is the width-to-length ratio, and it was determined for each negligible with respect to FeSi particles, the number of active
ferromagnetic cluster separately from the SEM cross-sectional MOs was calculated only within FeSi ferromagnetic particles.
view. R values of FeSi component for each sample are The dependence of the number of activated MOs on the excess
in Table II; S is the area where eddy currents are present; Bmax field is displayed in Fig. 7. MOs in the particles were activated
is the maximum magnetic induction [8]. For the calculation by increasing frequency. Higher value of n 0 corresponds to
inter of the sample,
of eddy current losses in cross-sectional Wclass the lower average cluster size (Table III). The number of
the following relation [8] was used: active MOs in quasi-static magnetization n 0 was determined
from the fit of this dependence for each sample. FeSi/resin
 T  2
1 dB sample exhibits the lowest excess losses at low frequencies
inter
Wclass = K (R)S dt (2)
ρcomposite 0 dt due to the highest number of active MOs in the quasi-static
magnetization.
where ρcomposite is the specific electrical resistivity of com-
posite, K (R) is the function of a sample cross section aspect IV. C ONCLUSION
ratio R.
The aim of our research was to study the properties of
Fig. 6 shows the frequency dependence of total losses
FeSi composites with ferrite nanofibers in PFRB resin. The
and their separation. Sample FeSi/resin (0.49 wt% ferrite)
inter in the measured SEM image analysis was used to determine the average area
shows the lowest eddy current losses Wclass
inter depend of the ferromagnetic component, where local eddy currents
frequency range in the sample cross section. Wclass
flow, to calculate the eddy current losses. The result of the
on the specific electrical resistivity of the whole sample.
image analysis showed that FeSi/resin (0.49 wt% ferrite) has
Different coating qualities of particles are the result of various
the smallest average area due to the best insulated particles.
amounts of ferrites in the resin. Ferromagnetic clusters with
This was reflected in the highest specific electrical resistivity
different average areas for each sample are thus formed during
and the lowest total losses. The optimal amount of ferrite fibers
pressing. FeSi/resin (0.49 wt% ferrite) composite has the
can increase the specific electrical resistivity to the very high
smallest average cluster area and therefore has the lowest eddy
intra [Fig. 6(c)]. W values. SMCs with very high electrical resistivity can find
current losses inside particles Wclass exc are the
intra , W inter , and W from the total application in high-frequency devices from a few hundreds of
result of subtracting Wclass class h
kilohertz to 1 MHz in telecommunication engineering, signal
losses. SEM images showed that the further addition of ferrite
transformers, and high-frequency magnetic cores.
fibers to the same amount of polymer caused desiccation of the
FeSi surface. This fact can be explained by the increase of FeSi
surface with respect to the porous nature of fibers that leads to ACKNOWLEDGMENT
insufficient coverage of FeSi surface by resin, resulted in the This work was supported in part by the Slovak Research
moderate deterioration of electrical and magnetic properties. and Development Agency under Grant APVV-15-0115, in part
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ĎÁKOVÁ et al.: ANALYSIS OF MAGNETIC LOSSES AND COMPLEX PERMEABILITY IN NOVEL SMC 5

Fig. 6. Separation of total losses in the frequency range from 1 to 37 kHz for samples at Bmax = 0.1 T. (a) FeSi/resin. (b) FeSi/resin (0.24 wt% ferrite).
(c) FeSi/resin (0.49 wt% ferrite). (d) FeSi/resin (1.46 wt% ferrite).

Internal Scientific Grant of the Faculty of Science, Pavol Jozef


Šafárik University, Košice, under Grant VVGS-PF-2017-230.
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