Journal of Alloys and Compounds 694 (2017) 55e60

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Journal of Alloys and Compounds

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

A ductile high entropy alloy with attractive magnetic properties

Panpan Li, Anding Wang, C.T. Liu*
Center for Advanced Structural Materials, Department of Mechanical and Biomedical Engineering, College of Science and Engineering, City University of
Hong Kong, Hong Kong

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

Article history: FeCoNiMn0.25Al0.25 high entropy alloy was investigated thoroughly in this paper from crystal structure to
Received 30 June 2016 magnetic and mechanical properties. We found that this alloy formed simple face centered cubic
Received in revised form structure which was very stable to deformation and heat treatment. Moreover, this alloy showed high
24 August 2016
saturated magnetization, low coercivity, high Curie temperature as well as good tensile ductility. This
Accepted 19 September 2016
Available online 5 October 2016
high entropy alloy shows soft magnetic properties much better than most high entropy alloys reported
previously. This study suggests that the FeCoNiMn0.25Al0.25 high entropy alloy has the potential for use as
soft magnets in the future.
Keywords:
High entropy alloys
© 2016 Elsevier B.V. All rights reserved.
Mechanical properties
Magnetic properties

1. Introduction
Alloy design has been a hot topic for metallurgists and material
scientists for a long time. From ancient to very recently, alloy design
are all based on only one or two principle elements without
exception, while other elements in small amounts are usually
added to enhance some specific properties of certain alloys. As is
well known, steels are based on element iron, while chromium is
used to enhance their corrosion resistance properties. Superalloy
Ni3Al are based on elements nickel and aluminum, while boron is
added to enhance the mechanical properties. Until the year of 2004,
high entropy alloys (HEAs) with at least five principle elements
with each element's concentration between 5 at% to 35 at%, which
are not limited to one or two principle elements any more, have
attracted intensive attentions by their extraordinary characteristics
due to the increased mixing entropy, inciting a fascinating new area
in metallurgy [1e6]. Due to their characteristics such as high en-
tropy effect, sluggish diffusion and significant lattice distortion,
they are reported to be good candidates as structural materials as
they have high strength and hardness, excellent corrosion and wear
resistance, as well as great fatigue resistance [1e6]. Usually, simple
solid solution structures such as body centered cubic or face
centered cubic are formed in high entropy alloys instead of ordered
crystalline intermetallic phases due to the high entropy effect.
* Corresponding author.
E-mail address: chainliu@cityu.edu.hk (C.T. Liu).
Moreover, some high entropy alloys are even reported to have
stable structures at high temperatures without precipitation
[7e10].
Until now, many studies are focused on the microstructures
and mechanical properties of HEAs, while few reports are avail-
able for functional properties (magnetization, magneto caloric
effect, electric resistance, etc.) of HEAs. As is well known, soft
magnetic materials play a fundamental role in many of the elec-
trical systems such as electrical power generation and trans-
mission, electric motors, magnetic shielding, electromagnets, etc.
However, each kind of commercial soft magnets has its short-
comings, such as brittleness and low magnetization of soft fer-
rites, complex and time-consuming producing process of silicon
steels; annealing brittleness and limited size of metallic glass;
stress-sensitivity and low electrical resistivity of Fe-Ni alloys.
Recently, some investigations have shown relatively high satu-
rated magnetization in FeCoNiAlSi HEAs [11] and FeCoNiCrAl
HEAs [12], which open up new applications of FeCoNi-based HEAs
as novel soft magnets. However, studies on the magnetic prop-
erties of HEAs are still limited and more progress on this research
is needed. For example, compared with most soft magnets, the
saturation magnetization of 64 emu/g and coercivity of 4100 A/m
found in FeCoNiCrAl HEAs are not good enough [12]. Many work
needs to be done in order to improve the magnetic properties of
HEAs.
In this report, a new high entropy alloy FeCoNiMn0.25Al0.25 is
studied thoroughly from structures to magnetic, electrical and

http://dx.doi.org/10.1016/j.jallcom.2016.09.186
0925-8388/© 2016 Elsevier B.V. All rights reserved.
56 P. Li et al. / Journal of Alloys and Compounds 694 (2017) 55e60

mechanical properties. High saturated magnetization (>100 emu/

g), low coercivity (<1000 A/m) and high Curie temperature
(~800
C) are found, indicating its potential application as soft
magnet. Meanwhile, good structure stability and tensile ductility
of this alloy indicate its excellent mechanical properties for in-
dustrial use. This study gives a new sight of investigating the
fascinating high entropy alloys and offers a new application area of
HEAs.

2. Experiments

FeCoNiMn0.25Al0.25 alloys were fabricated by vacuum arc

melting in a water-cooled Cu crucible using high purity raw ele-
ments. The Fe, Co, Ni, Al raw elements are ingots with the purity of
99.9%, while the Mn raw element is in small pieces with the purity
of 99.7%. All the starting materials are polished and prepared well
for use. 2 at% more of Mn was added to balance its evaporation
during the melting process. The ingots were re-melted five times to
Fig. 1. X-ray diffraction spectrum and morphology (insets) of as-cast, cold-rolled and
ensure homogeneity. Then they were suction casted into a annealed FeCoNiMn0.25Al0.25 alloys.
3 mm  12 mm  80 mm copper mold (as-cast samples). The plates
were cold rolled of 70% thickness reduction (cold rolled samples)
followed by heat treatment at 900
C for 1 h to obtain full recrys-
FeCoNiMn0.25Al0.25 alloys. It is clearly shown that for these
tallization then quenched in water (annealed samples). The com-
samples, simple FCC structures were formed. It is hard to un-
positions of the three different states are identified by EDS, as
derstand why this alloy shows no any indication of line broad-
shown in Table 1. It is clear that the actual compositions are quite
ening after cold work. From the dashed line in this figure, it is
near the nominal one, indicating there is no obvious composition
also observed that the diffraction peaks have no obvious shift,
change during the process.
suggesting the lattice parameters of this alloy are very stable to
The ingots were sectioned, polished and etched with nitric
variations of stress and temperature. This feature is very different
acid and alcohol solutions for observation and photographed by
from some traditional soft magnets. For example, stresses can
Leica optical microscope. A Rigaku Smartlab X-ray diffractometer
cause significant decrease of magnetization of FeeNi alloys [13]
was utilized for identifying of the crystal structure, using Cu Ka
while the annealing at 900
C can induce structural variation in
radiation. Magnetization hysteresis loops of the samples were
Fe-based metallic glasses as soft magnets [14]. For the annealed
measured in a Lakeshore vibrating sample magnetometer (VSM)
sample, a superlattice peak symbolized by “D” was found in the
up to 2.0 T applied field. Differential scanning calorimetry
XRD spectrum, indicating that a minor ordered phase might be
(Netzsch DSC 204) and thermomagnetic measurements in the
formed. This ordered phase was suggested as a B2 structure
heating/cooling speed of 20 K/min were taken to search for the
phase, as reported previously [15e17]. Inset images in Fig. 1
phase transformation and Curie transition. The electric resistance
reveal the morphology evolution of FeCoNiMn0.25Al0.25 alloys.
is measured by a four-probe method. Hardness measurements of
Typical dendrite and secondary dendrite structure can be
the alloys were conducted using a Vickers hardness tester at a
observed from the as-cast sample, with the secondary dendrite
load of 1.5 N for a loading time of 20 s. Several indentations were
arm spacing less than 10 mm. Stretched grains along the rolling
performed and averaged for each specimen. Tensile samples with
direction are observed in the cold rolled sample. From the
a cross-section of 3.2  1.4 mm and a gauge length of 12.5 mm
morphology of the annealed sample, it can be found that a full
were cut by electro-discharge machining, and polished carefully
crystallization occurred after heat treatment at 900
C for 1 h.
on each side with SiC paper through 2000 grit. Tensile tests were
The crystal size after annealing is about 20e30 mm.
conducted on an MTS tensile testing machine at a strain rate of
To further identify the thermal stability of the as-cast, cold-
103 s1 at room temperature and tensile properties were
rolled and annealed FeCoNiMn0.25Al0.25 alloy, DSC measurement
determined from the stress-strain curves. Fracture surfaces were
was taken and the corresponding curves were shown in Fig. 2(a).
examined by JEOL JSM-5600 scanning electron microscope
No obvious changes were observed up to 1000
C, indicating no
(SEM).
phase transformation occurred until 1000
C. We have already
known from Fig. 1 that annealing as-cast FeCoNiMn0.25Al0.25 alloy at
3. Results and discussion
900
C can induce the formation of a minor B2 phase. However,
from Fig. 2 (a), the DSC curve shows no detection of the phase,
Fig. 1 shows the X-ray diffraction patterns and related
indicating a very small quantity of this phase. In addition, ther-
morphology images of as-cast, cold rolled and annealed
momagnetic curves from room temperature to 950
C were tested
for the as-cast, cold-rolled and annealed FeCoNiMn0.25Al0.25 alloy.
The Curie temperature is determined to be around 800
C, sug-
Table 1 gesting its potential use in high temperatures. The Curie tempera-
Chemical compositions of as-cast, cold-rolled and annealed FeCoNiMn0.25Al0.25 al- ture has not changed obviously in the three states as the structure
loys by EDS analysis. and composition have not altered apparently. From Figs. 1 and 2, we
Compositions Fe (at.%) Co (at.%) Ni (at.%) Mn (at.%) Al (at.%) can draw a conclusion that the crystal structure of FeCoNiM-
n0.25Al0.25 alloy is quite stable to the variations of stress and
Nominal 28.57 28.57 28.57 7.14 7.14
As-cast 28.98 28.08 27.77 7.25 7.92
temperature.
Cold-rolled 28.94 28.81 27.44 7.18 7.63 Fig. 3 shows the magnetization curves of as-cast, cold-rolled and
Annealed 29.09 28.93 27.38 7.13 7.47 annealed FeCoNiMn0.25Al0.25 alloys at room temperature. All of the
 P. Li et al. / Journal of Alloys and Compounds 694 (2017) 55e60
Fig. 2. DSC curves (a) and thermomagnetic curves (b) of as-cast, cold-rolled and
annealed FeCoNiMn0.25Al0.25 alloys.
Fig. 3. Magnetization curves of as-cast, cold-rolled and annealed FeCoNiMn0.25Al0.25
alloys.
alloys can be very easily magnetized to the saturated state with
coercivity lower than 1000 A/m, suggesting their soft magnetic
properties. The saturated magnetization Ms and coercivity Hc are
57
changed differently by cold rolling and annealing. The values are
summarized in Table 2 and compared with other high entropy al-
loys reported previously in Table 3. The magnetic properties in the
present study are much better than most of the previously reported
values of high entropy alloys. Further discussion is detailed in the
discussion part of Tables 2 and 3.
Fig. 4 shows the room-temperature tensile testing results of as-
cast, cold-rolled and annealed FeCoNiMn0.25Al0.25 samples. It is
easy to understand that the as-cast sample shows the best ductility
and lowest strength, while the cold-rolled sample shows the
highest strength and worst ductility due to work hardening. It is
worth noticing that the annealed FeCoNiMn0.25Al0.25 alloy has a
balanced ductility (47.1% total elongation) and yield strength
(331.4 MPa). The ductility of this alloy is much better than that of
grain oriented silicon steel (elongation-to-failure df ¼ 10e20%), one
of the most popular commercial soft magnets [18]. The mechanical
parameters are also included in Table 2. The balanced performance
of strength and ductility might be considered due to the B2 struc-
ture found in Fig. 1, as B2 phase has been recognized as an effective
way to control strength and ductility in Ni3Al superalloy [19] as well
as in bulk metallic glasses [20].
To further identify the underlying mechanism of the ductility
variation in FeCoNiMn0.25Al0.25 alloys, their fracture surfaces after
tensile tests were carefully examined by SEM, as shown in Fig. 5 (a)
as-cast, (b) cold-rolled and (c) annealed, respectively. As is shown,
dimples with features of typical ductile fracture were observed for
all the three samples. In general, the average diameter or depth of
the dimples for as-cast sample is the largest. And the dimples
become much shallower and finer for cold-rolled sample. The
annealed sample with the moderate ductility shows the medium
sized dimples.
The structure, magnetic, electrical and mechanical properties
of FeCoNiMn0.25Al0.25 alloys are summarized in Table 2. It should
be noted that the FeCoNiMn0.25Al0.25 alloys have several special
properties. Firstly, the as-cast FeCoNiMn0.25Al0.25 alloy forms FCC
simple solid solution. The crystal structure has not changed by
cold rolling and annealing. By annealing, a small quantity of the
ordered B2 phase was detected by XRD. However, this phase
might be very tiny that the saturated magnetization has barely
been effected.
Secondly, the saturated magnetization was slightly increased by
cold rolling and annealing while the coercivity and permeability
were changed significantly. This is due to the magnetization is
primarily determined by composition and crystal structure while
the coercivity is affected by impurity, deformation, grain size, stress
and heat treatment. Therefore, the coercivity increased from 268 A/
m (as-cast) to 625 A/m (cold rolled) as a result of internal stress and
defects induced by cold rolling. Then, the coercivity decreased from
625 A/m (cold rolled) to 230 A/m (annealed) because of the
released internal stress and recrystallization. The coercivity of
annealed sample (230 A/m) is slightly lower than that of as-cast
sample (268 A/m), suggesting the average crystal size of the
annealed sample here is a little larger than that of the as-cast
sample according to the well-known coercivity-crystal size rela-
tionship reported by Herzer [21]. As is well known, the initial
permeability and coercivity behave in a contrary manner [22].
Therefore, the annealed alloy has the largest permeability in this
research.
Thirdly, the high Curie temperature around 800
C has been
observed in the annealed FeCoNiMn0.25Al0.25 alloy, suggesting its
potential applications in high temperature area, such as electric
cars, aeronautics and astronautics [23,24]. For example, in the area
of high temperature aerospace power generation, both mechanical
and magnetic properties are demanded due to the higher speed
and higher operating temperature in these devices [23,24]. Also,
58 P. Li et al. / Journal of Alloys and Compounds 694 (2017) 55e60

Table 2
Crystal structures, saturated magnetization (Ms), coercivity (Hc), permeability (me) at 1 kHz, Curie temperature (Tc), electric resistivity (r), yield strength (s0.2), tensile strength
(sul), elongation-to-failure (df) and hardness of FeCoNiMn0.25Al0.25 alloys.

Alloy state Crystal structure Ms (emu/g) me Hc (A/m) Tc (
C) r (U$m) s0.2 (MPa) sul (MPa) df (%) Hardness (HV)

As-cast FCC 101.0 297.2 268 805 1.0  106 138.1 483.9 58.1 150.6
Cold-rolled FCC 104.1 71.5 625 810 1.1  106 662.7 1029.6 7.9 357.2
Annealed FCC 104.2 479.6 230 812 0.91  106 331.4 651.0 47.9 175.8

Table 3
Comparison of magnetic properties of high entropy alloys. Ms denotes saturated magnetization, Hc for coercivity and Tc for the Curie temperature.

Alloy Structure Ms (emu/g) Hc (A/m) Tc (
C) Reference

a
FeCoNiAl0.2Si0.2 FCC 95e131 315e1508 [11,26,27]
FeCoNiCrCuAl BCC þ FCC 38e46 3582 25 [28e30]
FeCoNiCrPd1-2 FCC 33e34 167e230 [29]
FeCoNiCrAl BCC 64 4100 [12]
FeCoNiCrAl1.25 BCC 43.05a 1416 165 [31]
FeCoNiCrAl2 BCC 13e18 157 [29]
FeCoNiMn0.25Al0.25 FCC 101 268 ~800 Current study
a
For the convenience of comparison, the magnetic units are unified. The Ms of FeCoNiAl0.2Si0.2 alloy is reported as 0.838e1.151 T by reference 11 and 26. According to the
magnetic unit conversion table, 1 T ¼ 104/4p emu/cm3 and 1 emu/cm3 ÷r (g/cm3) ¼ 1/r emu/g. normally the alloy density r is between 6.5 g/cm3 to 7.5 g/cm3. Here, we use
r ¼ 7, so 0.838e1.151 T ¼ 667e916 emu/cm3 ¼ 95e131 emu/g. The magnetization of FeCoNiCrAl1.25 is also calculated according to the above equation.

magnetic properties than soft ferrites and comparable properties

Fig. 4. Tensile curve of as-cast, cold-rolled and annealed FeCoNiMn0.25Al0.25 samples.
with FeeNi alloys. Besides, our alloy has several advantages
including stable structure, high Curie temperature and good
ductility. Moreover, many soft magnetic properties (coercivity,
permeability) can be further optimized by controlling the grain size
or alloying minor elements [21].
Soft magnetic materials have been developed for decades. As is
well known, electric steels have been most widely used as the core
material for transformers and motors as they have the highest Ms
with relatively low price. However, the complex production process
and giant energy consumption make electric steels less appealing.
A new energy paradigm with increased concern for energy effi-
ciency in the total energy life cycle has accelerated research into
new materials such as amorphous and nanocrystalline soft mag-
netic materials. There is a persistent demand for core material
which has an even higher energy efficiency. We do see the potential
of this high entropy alloy as the process is simple and their struc-
tures are stable. High entropy alloys deserve much more attention
in the area of soft magnets.

the electrical resistivity is an important parameter related to the

4. Conclusion
energy loss and the eddy current effect in the application of soft
magnets. The electrical resistivity of this alloy is larger than those of
In this paper, the high entropy alloy FeCoNiMn0.25Al0.25 was
FeCoNi(AlSi)x x ¼ 0e0.5 high entropy alloys reported previously
prepared by casting, cold rolling and recrystallization annealing.
[11] and comparable to that of Fe-based metallic glass as soft
Structural, thermal, magnetic, electrical and mechanical properties
magnets [25]. Also, the electric resistance is not sensitive to the
of the alloys were investigated and compared. Structural and
metallurgical variations.
thermal analyses indicate the crystal structure is barely affected by
Finally, the high strength and good ductility observed in this
variations of the stress and temperature. Magnetic tests reveal the
alloy indicate that this material is easy to process and can meet
alloys possess a high magnetization, high Curie temperature and
many mechanical requirements in industry. Usually, hardness is
low coercivity. Mechanical tests demonstrate the alloys have a good
increased by work hardening, which is the reason why the cold
ductility. The good combination of mechanical and magnetic
rolled sample has the highest hardness.
properties makes the FeCoNiMn0.25Al0.25 alloy potentially to be a
Table 3 compared the soft magnetic properties of previously re-
new soft magnetic material. Major conclusions of this paper can be
ported research on HEAs with current study. It can be cleared seen
drawn as follows:
that compared to most high entropy alloys showing soft magnetic
properties, our samples have the lowest Hc, highest Ms and Tc. With
(1) The as-cast FeCoNiMn0.25Al0.25 high entropy alloy forms a
a stable structure and much better soft magnetic properties, our
simple FCC solid solution structure, which is quite stable to
FeCoNiMn0.25Al0.25 alloys show a great prospect as soft magnets.
deformation and temperature. By annealing, a small quantity
Fig. 6 compares the saturated magnetization (Ms) and coercivity
of the ordered B2 phase was detected by XRD.
(Hc) of different soft magnets. The FeCoNiMn0.25Al0.25 alloy
(2) The annealed FeCoNiMn0.25Al0.25 high entropy alloy shows
(marked by a pentagram) reported in this paper presents better
the highest Ms, lowest Hc, high Tc and electrical resistivity,
 P. Li et al. / Journal of Alloys and Compounds 694 (2017) 55e60
Fig. 5. Fractographic SEM images of as-cast (a), cold-rolled (b) and annealed (c)
FeCoNiMn0.25Al0.25 samples.
indicating its applications as soft magnets. Furthermore, this
alloy exhibits excellent stability and reliability at high
temperatures.
(3) The annealed FeCoNiMn0.25Al0.25 high entropy alloy also
show good ductility, advocating it can be easily deformed
and meet many deformation requirements in industry.
It is very likely that we can get much better soft magnetic
properties as well as mechanical properties by controlling the grain
size and the composition of the high entropy alloys. With the
possibility of improving magnetic and mechanical properties
59
Fig. 6. The saturated magnetization and coercivity of FeCoNiMn0.25Al0.25 alloy (marked
by pentagram) compared with other commercialized soft magnets [22].
significantly, further in-depth research in this area is expected in
the future.
Acknowledgments
This research was supported by funding from the Research
Grant Council (RGC), the Hong Kong Government through the
General Research Fund (GRF) with the account number of CityU
11209314.
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