Journal of ELECTRONIC MATERIALS, Vol. 45, No.

5, 2016
DOI: 10.1007/s11664-016-4457-x
Ó 2016 The Minerals, Metals & Materials Society

Iron Nanoparticles Fabricated by High-Energy Ball Milling

for Magnetic Hyperthermia

D.K. TUNG ,1,5 D.H. MANH,1 L.T.H. PHONG,1 P.H. NAM,1 D.N.H. NAM,1
N.T.N. ANH,1 H.T.T. NONG,2 M.H. PHAN,3 and N.X. PHUC1,4

1.—Institute of Materials Science, Vietnam Academy of Science and Technology, 18 Hoang Quoc
Viet, Cau Giay, Hanoi, Vietnam. 2.—University of Science and Technology of Hanoi, 18 Hoang
Quoc Viet, Cau Giay, Hanoi, Vietnam. 3.—Department of Physics, University of South Florida,
4202 East Fowler Avenue, Tampa, FL 33620, USA. 4.—Duy Tan University, K7/25 Quang Trung,
Da Nang, Vietnam. 5.—e-mail: dokhanhtung@gmail.com

Iron nanoparticles (FeNPs) have been successfully prepared by high-energy

ball milling in air for various milling times from 1 h to 32 h. Their structure,
particle size, elemental composition, magnetic, and inductive heating prop-
erties were investigated by means of x-ray diffraction (XRD) analysis, field-
emission scanning electron microscopy, energy-dispersive x-ray (EDX) spec-
troscopy, vibrating-sample magnetometry, and magnetic induction heating,
respectively. XRD analysis showed that the average crystallite size decreased
to 11 nm after 10 h of milling, then remained almost unchanged for longer
milling times. Coexistence of iron (Fe) and iron oxide (FeO) phases was de-
tected after 12 h of milling. EDX analysis also confirmed the occurrence of
oxidation, which can be reconciled with the corresponding decrease and in-
crease in saturation magnetization (Ms) with milling time when exposed to
oxygen and when annealed under H2 ambient due to oxygen reduction. The
time-dependent magnetic and inductive heating responses of the FeNPs were
investigated for prospective application in magnetic hyperthermia. The effect
of varying the alternating-current (AC) magnetic field strength on the satu-
ration heating temperature and specific loss power of FeNP-containing fer-
rofluid with concentration of 4 mg/mL was also studied and is discussed.

Key words: Iron nanoparticles, high-energy ball milling, magnetic inductive

heating, specific loss power, magnetic nanoparticles

INTRODUCTION diagnosis and therapy [such as magnetic resonance

imaging (MRI)], magnetic fluid hyperthermia
Nanoscale magnetic materials have been the sub-
(MFH),12–16 targeted drug delivery,17,18 and biologi-
ject of intense research because of their novel mag-
cal labeling.19 Owing to their advantages such as
netic properties relative to bulk counterparts.1,2
simple synthesis, low-cost materials, high magnetic
Magnetic nanoparticles (MNPs) are of great interest
response, and biocompatibility, iron oxide nanopar-
to researchers from a broad range of disciplines,
ticles (IONPs) are one of the most attractive candi-
including magnetic fluids, data storage, catalysis,
dates for use in biomedical applications, and IONPs
and bioapplications.3–7 In particular, MNPs show
have been applied in in vitro diagnostics for nearly
potentially important biological applications,8,9
half a century.12,20 However, further advances in
including magnetic bioseparation, detection of bio-
MNP-based biotechnology represent a challenging
logical entities (cells, proteins, nucleic acids,
task due to the limited magnetic properties of IONPs
enzymes, bacteria, viruses, etc.),10,11 clinical
(e.g., low saturation magnetization and aniso-
tropy21). Increasing the saturation magnetization of
MNPs has led to development of more efficient
(Received October 12, 2015; accepted March 8, 2016;
published online March 25, 2016) multifunctional agents for simultaneous targeted

2644
Iron Nanoparticles Fabricated by High-Energy Ball Milling for Magnetic Hyperthermia 2645

cell delivery, MRI contrast enhancement, and tar-

geted cancer therapy in the form of local hyperther-
mia. Recent work has begun to take advantage of iron
NPs (FeNPs) due to their high saturation magneti-
zation, high Curie temperature, and novel catalytic
properties.12,20 In comparison with conventional
IONPs with diameter of 10 nm (MS = 52 emu/g),
FeNPs possess higher saturation magnetization
(MS = 70 emu/g) and higher coercivity (by 100
orders of magnitude).22 This increased magnetiza-
tion afforded by FeNPs permits more effective gen-
eration of local hyperthermia.22,23
It is generally known that the magnetic proper-
ties of FeNPs and IONPs depend strongly on their
synthesis process, e.g., thermal decomposition,
reduction of iron salts, vapor-phase methods, the
two-step organometallic route, wet chemical pro-
cessing, or mechanical milling.23–27 Therefore,
development of a simple, reliable, and cost-effective
methodology to synthesize NPs of controlled size
and shape still remains a challenging task. Toward
this target, we recently successfully synthesized
high-magnetization, air-stable FeCo NPs by
mechanical alloying [or high-energy ball milling
(HEBM)] in air,28,29 due to the formation of an oxide
layer on the particle surface to prevent further
oxidation. Using the same approach, we report
herein the results of a study on the structural and
magnetic properties of Fe powders prepared by
HEBM in air. Air-stable, high-saturation-magneti-
zation FeNPs were successfully prepared, and their
structural, magnetic, and heating properties sys-
tematically investigated. The results obtained show
that these FeNPs are a promising candidate for use
in biomedical applications, including magnetic
Fig. 1. XRD patterns of samples (a) milled from 1 h to 32 h;
hyperthermia. (b) details of the (002) peak of Fe and (c) the (101) peak of FeO.

EXPERIMENTAL PROCEDURES
FeNPs were fabricated by HEBM from commer-
cial Fe powder with particle size of about 10 lm
(Merck). The milling process was performed in air
using a Fritsch planetary mono mill Pulverisette 6
with ball-to-powder weight ratio of 15:1 and milling
speed of 450 rpm (see Refs. 28 and 29 for more
details). Samples were milled from 1 h to 32 h,
labeled as M1h to M32h, respectively. The as-milled
samples (M10h, M24h, and M32h) were annealed
for 1 h at 600°C under flowing Ar + H2 (5%) to vary
the grain size and reduce the microstrain, disloca-
tion density, and any oxygen contamination. The
resulting samples are named M10h600, M24h600,
and M32h600, respectively.
Structural characterization was performed using
x-ray diffraction (XRD) analysis (Bruker D8
ADVANCE with DAVINCI.DESIGN). The average
crystallite size, dXRD, and internal strain were cal-
culated using commercial X’Pert HighScore Plus
software.28,29 Morphological and crystallite size were
obtained by field-emission scanning electron micro-
scopy (FESEM; Hitachi S-4800). Elemental analysis
was performed by energy-dispersive x-ray (EDX)
spectroscopy on JEOL JSM-6490 equipment. Mag-
netic properties were measured at room temperature
using a homemade vibrating-sample magnetometry
(VSM) system in magnetic fields of up to 12 kOe.28–30
The magnetic inductive heating response of Fe
ferrofluid was measured in the field range from
60 Oe to 90 Oe at fixed frequency of 178 kHz, using a
commercial generator (RDO HFI 5 kW).
RESULTS AND DISCUSSION
Figure 1 presents a series of XRD patterns for the
as-synthesized Fe powders obtained after different
milling times. These results clearly indicate varia-
tion of the phase and crystallite size of Fe after
various milling times. It is evident that the diffrac-
tion peaks related to the body-centered cubic (bcc)
structure of iron at 2h = 45°, 65°, and 85°, corre-
sponding to crystal planes (011), (002), and (112),
were observed and remained nearly unchanged
with milling time. The diffraction pattern gradually
broadened and the peak intensities decreased as the
2646 Tung, Manh, Phong, P.H. Nam, D.N.H. Nam, Anh, Nong, Phan, and Phuc

Table I. Structural and magnetic parameters of iron samples fabricated by high-energy ball milling
Sample D (nm) r (%) Fe (%) FeO (%) Ms (emu/g) Hs (Oe)

M1h 42 0.23 100 – 211 40

M2h 20 0.34 100 – 202 42
M4h 14 0.53 100 – 198 43
M8h 12 0.62 100 – 194 46
M10h 11 0.73 100 – 190 46
M12h 11 0.73 92 8 188 50
M16h 10 0.69 88.8 11.2 181 71
M24h 10 0.68 82.5 17.5 175 87
M32h 10 0.67 76 24 162 137
Italic values indicate the decrease of lattice strain for 10 h of milling.

Fig. 2. FESEM images and EDX patterns of samples (a, b) M10h and (c, d) M32h. Peak of C is due to carbon paste on EDX measurement. An
amount of Cr (0.3%) in M32h sample may come from steel balls and vial.

particle size decreased with increasing milling time
(see Fig. 1b). These observations indicate that both
the crystallite size and microstrain of the powders
were significantly affected by chemical milling due
to the HEBM process.31,32 While no obvious XRD
peaks corresponding to iron oxides were detected for
the products milled for up to 10 h, iron oxide (FeO)
phase appeared with characteristic peaks near 36°,
42°, and 61° for the samples milled for longer
(Fig. 1a and c). The iron oxide phase volume
fraction increased from 8% (M12h) to 24% (M32h)
as the milling time was increased from 12 h to 32 h.
No additional impurity lines were observed with
increasing milling time, indicating that contamina-
tion between samples and vial was negligible. The
average crystallite size, microstrain, and ratio of Fe
to FeO phase for the as-milled samples, as calcu-
lated from XRD peaks according to Ref. 29, are
presented in Table I. The particle size decreased
considerably from 42 nm (1 h) to 20 nm during the
Iron Nanoparticles Fabricated by High-Energy Ball Milling for Magnetic Hyperthermia 2647

first 2 h of milling. As the milling time was further
increased, the decreasing trend in the crystallite
size became less obvious. As shown in Table I, it
took about 6 h to decrease the particle size from
14 nm (M4h) to 11 nm (M10h), after which it
reached a nearly constant value of 10 nm after
16 h of milling, suggesting that the rate of milling is
approximately equal to the rate of agglomeration.31
Similar behavior was observed in the case of the
microstrain [we note a decrease of lattice strain for
10 h of milling (Table I)]. The final grain size of the
Fig. 3. (a) Hysteresis loops for samples M10h and M32h and (b) Ms
and Hs of iron samples with various milling times. The inset shows
the center of hysteresis loop.
powder after 10 h of milling was determined to be
about 11 nm. This drastic decrease in grain size (as
determined from XRD results) corresponds to a
substantial increase of lattice strain from 0.23% to
0.73% for 1 h and 10 h of milling (Table I), respec-
tively, due to plastic deformation, fracture, and cold
welding of powder particles generated by the large
amount of energy introduced by ball milling.33
However, when the microstrain was sufficiently
high, sliding friction occurred to stabilize the
microstrain, and particles tended to agglomerate
and possibly sintered, resulting in larger
particles.34,35
An FESEM micrograph and EDX spectrum for
samples M10h and M32h are shown in Fig. 2, where
the particles are spherical in shape with grain size
of roughly 11 nm. Only the larger particles tend to
agglomerate. EDX analysis showed that the weight
percentage of Fe decreased from 97.6% to 94.1%,
while that of oxygen increased from 2.4% to 5.9%,
for M10h and M32h, respectively. The increasing
proportion of oxygen is related to increased oxida-
tion. These results agree quite well with the XRD
analysis presented in Table I.
Hysteresis loops measured at room temperature
in the presence of external magnetic fields (H) of up
to ±11 kOe are shown in Fig. 3a for samples M10h
and M32h. It should be noted here that 11 kOe was
insufficient to completely saturate the magnetiza-
tion of the samples. This nonsaturation is likely
related to surface spin disorder.36 The disordering
effect is even more prominent in ball-milled
nanoparticle systems relative to chemically synthe-
sized ones.37 The saturation magnetization (Ms) was
then estimated by using the law of approach to
saturation of an assembly of particles,38 as reported
in Ref. 29:
 
M ð H Þ ¼ MS 1  a=H  b=H 2  c=H 3 þ vd H; ð1Þ
where Ms is the saturation magnetization, vd is the
susceptibility in high magnetic fields, and a, b, and c
are considered as free parameters. The Ms values
obtained by fitting the M(H) data using Eq. 1 are

Table II. Saturation magnetization (M*s) of FeNP samples, calculated according to Eq. 1
Sample M1h M10h M24h M32h M10h600 M24h600 M32h600

M*s (emu/g) 215 194 178 165 202 193 195

Table III. Magnetic parameters of selected as-milled and annealed samples

Sample M10h M10h600 M24h M24h600 M32h M32h600

Hc (Oe) 46 47 87 62 137 63
Ms (emu/g) 190 199 175 192 162 192
2648
Fig. 4. Time dependence of saturation magnetization, Ms(t), for iron
samples stored in air at room temperature.
reported in Table II. The open hysteresis loops
reveal that these powders exhibited dominant fer-
romagnetic behavior at room temperature with high
Ms values of 190 emu/g and 162 emu/g and small
values of Hc (coercive field) of 46 Oe and 137 Oe for
samples M10h and M32h, respectively.
The variations in Ms and Hc as a function of
milling time are shown in Fig. 3b and Table I. It is
observed that Hc increased as the particle size
decreased. There are several possible explanations
for the Hc enhancement with milling time, e.g.,
internal stress, contamination, various defects,
particle interactions, etc.38 As the milling time
was increased from 1 h to 32 h, Ms decreased
sharply from 211 emu/g to 162 emu/g. This could
be due to disordering in crystal structure, size
reduction, and surface effects, or the occurrence of
iron oxidation when samples are milled in atmo-
spheric environment.30 Relative to bulk Fe mate-
rial, the decrease in Ms for the Fe nanoparticles is
likely related to the loss of long-range ferromag-
netism and surface spin disorder, as well as the
presence of an additional iron oxide (FeO) phase in
samples ball-milled for long time. Since FeO is
antiferromagnetic, its presence could cause stron-
ger breakage of long-range ferromagnetic order
and greater reduction of the ferromagnetic volume
fraction in smaller iron–iron oxide core–shell
nanoparticles.39 Additionally, exchange interac-
tions between nanoparticles can also cause Ms to
decrease.37
Table III summarizes the values of Ms and Hc for
the annealed samples (compared with as-milled
samples). It can be seen that the Ms values of the
as-milled samples became larger upon annealing.
The lower initial Ms could be caused by traces of
unreacted materials and/or crystalline disorder.40
The Ms values of all the annealed samples were
smaller overall than for their bulk counterparts.41
Oxidation is one possible reason, but this result may
also be caused by surface/interface anisotropy, in
Tung, Manh, Phong, P.H. Nam, D.N.H. Nam, Anh, Nong, Phan, and Phuc
Fig. 5. (a) Heating curves for different AC magnetic fields and (b)
linear dependence of SLP on AC magnetic field (H2) for FeNPs.
comparison with a previous report.38 Meanwhile, Hc
decreased because the microstrain in the samples
declined after annealing. This finding is consistent
with previously published reports.28–30
Figure 4 illustrates the variation of Ms as a
function of time for particle samples (Ms of
190 emu/g, 175 emu/g, and 162 emu/g for M10h,
M24h, and M32h, respectively) kept in atmospheric
environment. It is noted that Ms remained almost
unchanged for the samples kept in atmospheric
environment for up to 30 days. This indicates that
our FeNPs are very stable under ambient condi-
tions, which can be attributed to the formation of a
thin oxide layer on the FeNP surfaces, acting as a
barrier to further oxidation.29
To study the magnetic inductive heating response
of the FeNPs, the single-phase sample (M10h) was
used to form a magnetic liquid (ferrofluid).
Figure 5a shows the change in temperature of a
4 mg/mL M10h sample as a function of measure-
ment time under an AC external magnetic field of
60 Oe, 70 Oe, 80 Oe, and 90 Oe. It can be observed
that, with increasing time, the temperature of the
sample first increased and then reached saturation
after 1500 s. The saturation heating temperatures
(Ts) were observed to be 36.7°C, 45.6°C, 55.1°C, and
63.2°C for AC magnetic field of 60 Oe, 70 Oe, 80 Oe,
Iron Nanoparticles Fabricated by High-Energy Ball Milling for Magnetic Hyperthermia 2649

fluid. The calculated heating values are reported in

Table IV. Saturation heating temperature Ts, Table IV. A linear dependence was obtained
initial slope of heating curve dT/dt, and specific between the SLP values and the square of the field
loss power (SLP) of Fe ferrofluid with amplitude (H2) for the 4 mg/mL M10h sample, as
concentration of 4 mg/mL for different AC shown in Fig. 5b. This is in agreement with the
magnetic fields
previously established relationship describing var-
H (Oe) f (kHz) T(1500 s) dT/dt (°C/s) SLP (W/g) ious types of lossy processes in a substance inter-
acting with a magnetic field.40,47–49
60 178 36.8 0.0095 9.9 To probe their inductive heating ability, we
70 178 45.6 0.0231 24.1 investigated the stability of the SLP and Ts of the
80 178 55.1 0.0356 37.2 Fe ferrofluids, subjected to external magnetic fields
90 178 63.2 0.0763 79.7 at frequency of 178 kHz and amplitude of 80 Oe
after four times of heating within 13 days. The
results are shown in Fig. 6 and Table V, indicating
that the Ts and SLP remained nearly unchanged: Ts
reduced by about 3%, and SLP by <2% after
Table V. TS, dT/dt, and SLP for 4 mg/mL Fe 13 days. This SLP value is also comparable to those
ferrofluid at AC field of 80 Oe with frequency of reported in previous works.22,23,50 These results
178 kHz indicate that our FeNPs (M10h) are a promising
Number of T(1500 s) dT/dt SLP
candidate for use in magnetic hyperthermia.
heating times (°C) (°C/s) (W/g)
CONCLUSIONS
1 55.1 0.0356 37.2
2 55 0.0355 37.1 FeNPs were successfully fabricated by high-en-
3 54.6 0.0352 36.8 ergy ball milling from iron powder in air. We find
4 53.5 0.0349 36.5 that single-phase crystalline structure of Fe was
retained up to 10 h of milling, with average crys-
tallite size of 11 nm. The saturation magnetization
decreased due to grain size refinement and the
presence of iron oxide phase (after 12 h milling),
while the coercivity increased due to the increase of
grain-boundary defects and increase in internal
strain with milling time. The saturation magneti-
zation of the FeNPs remained almost unchanged
when exposed to air for 30 days, due to the forma-
tion of a thin iron oxide (FeO) layer around the
FeNPs. Good inductive heating response of FeNPs
(M10h) was achieved, indicating that these
nanoparticles are promising for use in magnetic
hyperthermia.
ACKNOWLEDGEMENTS
This research is funded by the Vietnam National
Fig. 6. Stability of SLP and Ts over magnetic inductive heating times Foundation for Science and Technology Develop-
for Fe in 13 days. ment (NAFOSTED) under Grant DT-NCCB-
DHUD.2012-G/08. The authors are also grateful to
the National Key Laboratory for Electronic and
and 90 Oe, respectively. This indicates the useful- Devices, Institute of Materials Science, Vietnam
ness of our FeNPs for hyperthermia applications, Academy of Science and Technology; and Rare
since thermoablation (41°C to 45°C) generates Earth Metallurgical Chemistry, East Paris Institute
enough heat to directly destroy tumor cells and of Chemistry and Materials Science.
tissues.42–45 The specific loss power (SLP) for the Fe
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