2178
Z. Zhang et al. / Journal of Magnetism and Magnetic Materials 324 (2012) 2177–2182
composites is as follows: First, 1 g of Sr0.8La0.2Fe11.8Co0.2O19 powders
and 5 mL of iron pentacarbonyl [Fe(CO)5] were added into an airproof
reactor and evaporator, respectively. Fe(CO)5 was evaporated at 65 1C,
while Sr0.8La0.2Fe11.8Co0.2O19 powders were heated and maintained at
250 1C. Fe(CO)5 vapor was bowed into the reactor by argon gas at a
rate of 150 mL/min for 3, 9 and 18 min. To obtain a uniform coating,
the reactor was vigorously and continuously stirring mechanically.
Shell-core Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites were obtained after
slow-cooling to room temperature, and the whole experiment was
protected by argon. The weight content of iron in the composites was
determined by comparing the weights of specimens before and after
the experiment. The mass ratios of Sr0.8La0.2Fe11.8Co0.2O19 to Fe were
approximately 9:1, 7:3 and 4:6.
3.2. Crystal structures
Fig. 3 shows the X-ray diffraction (XRD) patterns of Sr0.8La0.2-
Fe11.8Co0.2O19
,
CI, and Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites.
Fig. 3(b) shows peaks at 19.341, 23.221, 30.931, 31.131, 32.611, 34.21,
36.051, 37.801, 41.061, 57.461, and 64.31, which are respectively
attributed to the (102), (006), (110), (008), (107), (201), (203), (205),
(206), (2011), and (220) phases of the Sr0.8La0.2Fe11.8Co0.2O19 particles.
These peaks can be indexed to the pure M-type hexa ferrite structure,
in agreement with JCPDS Card no. 720739. No impurity peaks were
detected, indicating the high purity of the powders. The shell-core-
structured Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites [Fig. 3(c)] had simi-
lar diffraction peaks to Sr0.8La0.2Fe11.8Co0.2O19 and CI, but the intensity
of the peaks decreased. In addition, a peak around 2
observed, indicating that the shell layer was composed of iron.
y¼44.61 was
2.3. The preparation of composites coatings
3.3. Complex permittivity and permeability
The Fe–Sr0.8La0.2Fe11.8Co0.2O19 powders were dispersed into
the epoxide resin via adding solvent and a high energy ultrasonic
treatment for 30 min. Afterwards, hardener was added into the
mixtures, followed by stirring at 1000 rpm for 10 min. Finally, the
composite materials are fabricated on an aluminum substrate
with a standard size (180 mm ꢁ 180 mm ꢁ 3 mm).
Fig. 4 shows the complex permittivity and permeability of pure
Sr0.8La0.2Fe11.8Co0.2O19 and Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites.
Fig. 4(a) and (b) respectively show the real (e0) and imaginary (e00
)
parts of the permittivity of the specimens plotted as a function of
frequency. e0 and e00 represent the energy storage ability and loss
ability, respectively. The e0 and e00 values of the specimens remained
constant with slight fluctuations over the entire frequency range and
increased with increasing weight ratio of Fe. The e0 and e00 of
Sr0.8La0.2Fe11.8Co0.2O19 were almost constant with nearly no differ-
ence throughout the frequency range studied (e0 ¼6, e00 ¼0.5), indicat-
ing poor dielectric loss. When the mass fraction of Fe was increased
by 60%, the e0 values increased from 6 to 12 while the e00 values
increased from 0.5 to 2.3. Dielectric loss commonly results from
electron polarization, iron polarization, and electric dipolar polariza-
tion [16]. The experiments showed that the Fe shell, which forms a
surface layer, greatly increases the conductivity of the samples and
contributes to the enhancement of permittivity. Because of the
metallic properties of the shell, electrons can travel freely and
accumulate on the Fe–Sr0.8La0.2Fe11.8Co0.2O19 interface, forming a
structure similar to a boundary-layer capacitor and generating
interfacial electric dipolar polarization. According to previous
research [17], electron and iron polarization only occur at frequencies
higher than the infrared range. Thus, the enhanced dielectric loss
found in our samples could be attributed to electric dipolar polariza-
tion. Optimizing the weight ratio of Fe would likely cause the
composites to attain the permittivity necessary in microwave absorb-
ing materials.
2.4. Measurement of properties
The phase structure of the powder was identified by X-ray
diffraction (XRD; D/max-IIB, Japan). A VEGA II XMU INCA scan-
ning electron microscope (SEM) was employed for morphological
analysis. EM parameters (i.e., complex permeability and permit-
tivity) were measured using
a vector network analyzer
(HP-8720ES) in the frequency range of 2–18 GHz. The samples
used for EM parameter measurements were prepared by disper-
sing powders into paraffin wax at a mass fraction of 60%, and then
pressing the mixtures into a compact toroidal shape with outer
and inner diameters of 7.0 and 3.0 mm, respectively. The reflec-
tion loss of the prepared absorbers versus the frequency is studied
using an HP 8510B vector network analyzer and standard horn
antennas in an anechoic chamber.
3. Results and discussion
The real (m0) and imaginary (m00) parts of the permeability are
shown in Fig. 5(a) and (b), respectively. An intersecting point at
8.5 GHz was observed on the curve of m0. Higher m0 values were found
for Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites with higher Fe contents
prior to this intersecting point. Inverse changes were detected after
the intersecting point. Meanwhile, the m00 of Fe–Sr0.8La0.2Fe11.8
Co0.2O19 was uniformly smaller than that of pure Sr0.8La0.2Fe11.8-
Co0.2O19 over the range of 2–18 GHz, and decreased with increasing
Fe content. Broad peaks at 3–7 GHz were present in the
Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites. Generally, for ferrite magnetic
materials, the microwave magnetic loss originates mainly from
domain wall resonance and natural ferromagnetic resonance [18].
Domain wall resonance is usually exhibited in the low-frequency
region (o2 GHz). However, resonance due to the spin rotational
component occurs at high-frequency regions. Thus, the resonance
peak observed may be attributed to natural resonance.
3.1. SEM analysis
An SEM image of the Sr0.8La0.2Fe11.8Co0.2O19 particles shows
irregularly shaped platelet-like crystals with smooth surfaces,
as shown in Fig. 1(a). The particles stack on top of each other
due to magnetic attraction between particles and are uni-
formly coated with iron, as illustrated in Fig. 1(b)–(d). The
Fe–Sr0.8La0.2Fe11.8Co0.2O19 micro-structured composites have a
full shell-core structure. When a small amount of Fe(CO)5 vapor
was added, CI particles with average diameters of approximately
0.02–0.1 mm were found in some of the Sr0.8La0.2Fe11.8Co0.2O19
particles [Fig. 1(b)]. Sr0.8La0.2Fe11.8Co0.2O19 particles coated with
CI showed coarse surfaces, as shown in Fig. 1(c). An increase in
the CI content of the Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites
changed the shape of the particles to coralloid, and their arris
disappeared due to increasing thickness of the carbonyl shells.
Fig. 2 (a) and (b) are the surface and section SEM observation,
which show the microstructure of the coating filled with 60%
Fe–Sr0.8La0.2Fe11.8Co0.2O19 composites. It was observed that the
fillers are well dispersed in the EP matrix and no significant
porosity was noticed.
3.4. Microwave absorption properties
The normalized input impedance, Zin, of a metal-backed
microwave absorption layer is derived from the following