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Journal of Magnetism and Magnetic Materials 324 (2012) 578583

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Journal of Magnetism and Magnetic Materials


journal homepage: www.elsevier.com/locate/jmmm

Low temperature sintering of sub-stoichiometric NiCuZn ferrites:


Shrinkage, microstructure and permeability
n

J. Murbe,
J. Topfer

University of Applied Sciences Jena, Dept. SciTec, Carl-Zeiss-Promenade 2, 07745 Jena, Germany

a r t i c l e i n f o

a b s t r a c t

Article history:
Received 27 April 2011
Received in revised form
23 August 2011
Available online 1 September 2011

We have studied sub-stoichiometric NiCuZn ferrites with iron deciency (i.e., o 50mol% Fe2O3) of
composition Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) with 0 r z r 0.06. The temperature of maximum shrinkage rate is shifted from T 1000 1C for z 0 towards lower temperatures down to T 900 1C for a substoichiometric ferrite with z 0.02. Dense samples are obtained after ring at 900 1C for z 40 only. Substoichiometric compositions (z 40) do not form single-phase spinel ferrites after sintering at 900 1C,
but rather represent mixtures of CuO and a stoichiometric ferrite with slightly modied composition.
The formation of small amounts of CuO at grain boundaries is demonstrated by XRD and SEM. The
permeability is increased from m 80 for stoichiometric ferrites (z 0) to m 660 for z 0.02. The
formation of CuO during sintering of sub-stoichiometric ferrites supports densication and is a
prerequisite for low temperature ring of multilayer inductors. Addition of 1 wt% Bi2O3 as liquid phase
sintering aid is required to provide sufcient densication of the stoichiometric ferrite (z 0) at 900 1C.
Addition of 0.37 wt% Bi2O3 to a sub-stoichiometric ferrite (z 0.02) results in dense samples after ring
at 900 1C; however, the microstructure formation is dominated by heterogeneous grain growth.
& 2011 Elsevier B.V. All rights reserved.

Keywords:
Soft ferrite
Low temperature sintering
Permeability
Sub-stoichiometry

1. Introduction
NiCuZn ferrites are standard materials for multilayer inductors
because of their low sintering temperature and good performance
up to MHz frequencies [13]. The temperature for co-ring the
multilayer component is restricted to about 900 1C because of the
melting point of silver used as metallization material. Consequently,
the choice of a proper ferrite composition and optimum processing
route is crucial for the fabrication of devices. The positive effect of Cu
on lowering the sintering temperature of NiZn ferrites has been
known for years [4]. However, papers reporting on correlations
among NiCuZn ferrite composition, sintering behavior and magnetic properties are scarce [59]. Moreover, a common feature of
typical low-ring ferrite compositions seems to be a small deciency of iron oxide, i.e. less than 50mol% Fe2O3 is used in the
starting mixture of oxides. Such compositions are referred to as substoichiometric here. Their composition typically translates into a
spinel formula with less than two Fe per formula unit, e.g.
Ni0.20Cu0.20Zn0.62Fe1.98O3.99, compared to stoichiometric ferrites
with 50mol% Fe2O3 and two Fe per formula unit MeFe2O4. The
effect of sub-stoichiometry through iron deciency has been investigated earlier. It was shown that sub-stoichiometry enhances
densication [9,10]. Precipitation of Cu at grain boundaries of a

Corresponding author. Tel.: 49 3641 205479; fax.: 49 3641 205451.

E-mail address: joerg.toepfer@fh-jena.de (J. Topfer).

0304-8853/$ - see front matter & 2011 Elsevier B.V. All rights reserved.
doi:10.1016/j.jmmm.2011.08.040

sub-stoichiometric NiCuZn ferrite was observed by TEM [11].


Additionally, bismuth oxide has frequently been suggested as
sintering additive to improve densication of the ferrites [1214].
The addition of o1 wt% of Bi2O3 has been shown to be effective for
preparing NiCuZn ferrites with m 900 [15,16].
In this contribution, we report a systematic study of the shrinkage
and permeability behaviors of sub-stoichiometric, iron-decient
NiCuZn ferrites. Moreover, the effect of Bi2O3 addition to stoichiometric and sub-stoichiometric NiCuZn ferrites on the microstructure formation and permeability was investigated.

2. Experimental
Ferrite powders of composition Ni0.20Cu0.20Zn0.60 zFe2 zO4 (z/2)
with 0rzr0.06 were prepared by the standard ceramic route.
a-Fe2O3 (TKS Germany, HP grade) with a specic surface S4.3 m2/g;
NiO (Inco, Black Nickel Oxide, Grade F) with S 70 m2/g; CuO.
(Merck, Germany) with S4.6 m2/g and ZnO (Harzsiegel Heubach,
Germany, standard grade) with S4.5 m2/g were used as starting
materials. The oxides were wet mixed for 12 h in a polyethylene
container. After drying the powder was calcined at 750 1C for 2 h and
subsequently milled in a planetary ball mill using zirconia grinding
media. Bi2O3 was added during ne-milling. The powders were
compacted using polyvinyl-alcohol as a binder to give pellets for
sintering studies or toroids for permeability measurements.

J. M
urbe, J. T
opfer / Journal of Magnetism and Magnetic Materials 324 (2012) 578583

579

The phase formation of the materials was evaluated by XRD


(Siemens D5000). The particle size of the powders was measured
using a laser diffraction system (Malvern Mastersizer 2000). The
specic surface S of the powders was measured by nitrogen
adsorption (BET, Nova 2000, Quantachrome Instruments); a mean
particle size dBET was estimated using the relation dBET 6/rS
(with density r; assuming spherical particles). Shrinkage measurements were made with a Netsch DIL402 dilatometer on
cylindrical compacts during heating to 10001200 1C at 4 K/min
heating rate. The bulk density of sintered samples was determined from the dimensions and the weight. The microstructure of
the samples was studied with a scanning electron microscope
(SEM, Zeiss DSM940A). The permeability of the sintered toroids
was measured using an impedance analyzer in the frequency
range 11000 kHz. For frequencies up to 2 GHz, permeability
measurements were performed using an Agilent E4991A impedance/materials analyzer.

3. Results and discussion


Single-phase ferrite powders were obtained after calcinations
at 750 1C (XRD results not shown here). After ne-milling an
aggregate size of d50 0.6 mm was measured by laser diffraction.
The specic surface of the ferrite powders S 12 m2/g corresponds to a mean particle diameter of dBET 100 nm. Dilatometric
shrinkage measurements performed on pellets made of nemilled powders demonstrate that the sub-stoichiometry z in
Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) with 0 rzr0.06 signicantly
affects the shrinkage and shrinkage rate (Fig. 1). Stoichiometric
Ni0.2Cu0.2Zn0.6Fe2O4 (z0) has its maximum shrinkage rate at
1000 1C. Shrinkage is shifted towards lower temperatures with
increasing sub-stoichiometry in the range 0 rzr0.02. For example, in Ni0.20Cu0.20Zn0.62Fe1.98O3.99 (z 0.02) maximum shrinkage
appears at 900 1C. On the other hand, for z4 0.02, the temperature of maximum shrinkage rate is not decreased further anymore
(Fig. 1). The observed differences in the shrinkage of stoichiometric and sub-stoichiometric NiCuZn ferrites are also reected
in the densication behavior. The density of pellets after sintering
at 900 1C for 2 h is shown in Fig. 2. The measured variation of
density vs. z clearly demonstrates that the stoichiometric ferrite
(z0) experiences limited densication only (83%). With increasing z the densication is largely enhanced and reaches almost
theoretical density for z 0.02. The reason for this will be
discussed below.
The phase composition of the ferrites Ni0.20Cu0.20Zn0.60 zFe2 z
O4 (z/2) with 0rzr0.06 (sintered at 900 1C) was investigated with
X-ray diffraction. For z0 a single phase ferrite with spinel-type
structure was found (Fig. 3). This is in agreement with earlier
studies on ferrite formation in the series Ni1 x yCuyZnxFe2O4 with
0.4rxr0.6 and 0ryr0.25 [9]. It clearly demonstrates that the
selected composition Ni0.20Cu0.20Zn0.60Fe2O4 (z0) is within the
ferrite phase eld of Cu-substituted NiZn ferrites. In contrast, the
XRD pattern of the sample with z0.06 shows an additional peak at
2y 38.71, which was identied as (1 1 0) reection of tenorite CuO.
This peak was observed in all sub-stoichiometric samples with
z40.02; for smaller z the concentration of CuO is below the XRD
detection limit. This nding is in contrast to earlier reports on substoichiometric iron-decient ferrites. For ferrites with very large substoichiometry, e.g. (Ni0.76Zn0.24)O(Fe2O3)0.575, Ling et al. [17] observed
a mixture of a halite phase (Ni/Zn)O coexisting with a ferrite. Very
recently, NiCuZn ferrites with iron deciency between 47 and 50
mol% Fe2O3 (sintered between 1040 and 1200 1C) were reported to
contain a ZnO secondary phase [18]. However, our XRD results
suggest that CuO coexists with the ferrite after sintering at 900 1C.

Fig. 1. Shrinkage (a) and shrinkage rate (b) of Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2)
with 0r zr 0.06.

Fig. 2. Density vs. z of Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) with 0r z r0.06 sintered
at 900 1C for 2 h.

Nominally sub-stoichiometric ferrite compositions are represented by




2z
3z
Cu2y3z Ni22x2y Zn2x 2z Fe2 O4
CuO
Cuy Ni1xy Znx z Fe2z O4z=2 2z
2z
2z
2
2
1

580

J. M
urbe, J. T
opfer / Journal of Magnetism and Magnetic Materials 324 (2012) 578583

Fig. 3. XRD patterns of ferrites sintered at 900 1C for 2 h with z 0 and 0.06.

Fig. 4. Lattice parameters of Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) ferrites with


0r zr 0.06 sintered at 900 1C for 2 h; inset: SEM micrographs of ferrites sintered
at 900 1C with z 0 (left) and z 0.06 (right).

Sub-stoichiometry caused by iron deciency in the nominal ferrite


composition leads to the formation of a Cu-poor stoichiometric ferrite
and CuO as the second phase. The synthesized ferrite series reported
here corresponds to compositions with y0.20 and x0.60 in Eq. (1).
For small iron deciency, e.g. z 0.02, this results in the formation of a
spinel Ni0.202Cu0.172Zn0.626Fe2O4 and 0.03 CuO (not detectable by
XRD). For z0.06 the ferrite Ni0.206Cu0.113Zn0.680Fe2O4 coexists with
0.09 CuO. A slight increase of the lattice parameter a0 of the spinel
ferrite as a function of the sub-stoichiometry z is observed (Fig. 4),
conrming a small change in the ferrite composition with z. This is
consistent with the fact that an increase of a0 has been observed in
NiZn ferrites with increasing Zn content [19]. The decomposition of
nominally sub-stoichiometric ferrites into a mixture of a stoichiometric spinel and CuO during sintering is also reected in the ceramic
microstructure (inset of Fig. 4). For z0 a homogeneous microstructure consisting of ferrite grains only is found. The presence of an
additional phase between the ferrite grains (identied as Cu-rich
phase by EDX) is demonstrated for a sub-stoichiometric sample with
z0.06. This grain boundary phase obviously enhances densication
as shown in Fig. 2. The exact composition of this Cu-rich phase as a
function of temperature and whether or not it acts as a liquid phase
sintering aid during ring at 900 1C are not known yet. However, after
cooling to room temperature, the segregated grain boundary phase

consists of copper oxide, as shown by XRD for large z, and represented


by Eq. (1).
The permeability of Ni0.20Cu0.20Zn0.60 zFe2 zO4 (z/2) (0rzr0.06)
sintered at 900 1C is shown as a function of frequency in Fig. 5. The
frequency dispersion of permeability shows that the absolute values
of the real part of the permeability m0 at 1 MHz increases up to
z0.02 and decrease with larger iron deciency z. The variation of m
at 1 MHz vs. z (Fig. 8b) has a maximum at z0.02. This behavior is
caused by (i) the increase of density for 0rzr0.02; the reduced
porosity in the sample with z 0.02 enhances domain wall mobility
and permeability; (ii) for z40.02 the amount of segregated, nonmagnetic CuO at grain boundaries and triple points tends to reduce
the permeability and (iii) the increase of Zn-concentration with
increasing z in the ferrite matrix (to 0.60 z) as expressed in Eq. (1)
leads to a reduction of the saturation magnetization Ms and permeability. It was shown early that in ferromagnetic spinels, e.g. NiZn
ferrites Ni1 xZnxFe2O4, Zn-concentrations exceeding a critical value of
0.5rxr0.6 tend to reduce Ms because of changes in the cation
distribution and resulting magnetic moments [19]. In addition, the
magneto-crystalline anisotropy also impacts the resulting permeability. This results in a complex interplay between microstructure and
intrinsic magnetic parameters. In the ferrite series studied here,
the reduction of permeability for zZ0.02 might be interpreted by
microstructure effects (i) and (ii) in combination with reduced
magnetization and anisotropy.
The real part of permeability m0 starts to decay between 2 and
5 MHz for 0.02 rzr0.06, whereas for z r0.02 the reduction of
permeability begins at above 10 MHz. Simultaneously, the imaginary part of permeability m00 peaks at the resonance frequency
(not shown here), where m0 is reduced to 50% of its low frequency
value. This is the expected behavior because according to Snoeks
law the shift of the resonance frequency toward higher frequencies is accompanied by a decrease of the absolute values of
permeability. The variation of permeability vs. temperature is
shown in Fig. 6. The Curie temperature is reduced from Tc 112 1C
for z 0.02 to Tc 70 1C for z 0.06. This might be interpreted by
the shift of ferrite composition with z according to Eq. (1); the
ferrite tends to become more Zn-rich and Cu-poor with increasing
z. The Curie temperatures of NiZn ferrites were shown to
decrease with increasing Zn-concentrations [20].
Because of the limited densication of the stoichiometric
ferrite (z0), Bi2O3 was added as a liquid-phase sintering aid

Fig. 5. Permeability vs. frequency for Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) with
0r zr 0.06, inset: permeability at 1 MHz vs. z.

J. M
urbe, J. T
opfer / Journal of Magnetism and Magnetic Materials 324 (2012) 578583

Fig. 6. Permeability vs. temperature for Ni0.20Cu0.20Zn0.60 zFe2  zO4  (z/2) ferrites.

581

identical Bi2O3 concentrations (Fig. 7b). The shrinkage rate displays a change from a broad peak for Bi2O3-free samples to a
series of sharp rate peaks for samples containing bismuth oxide,
which is interpreted as signature of the dominance of liquid phase
sintering in the latter case. For stoichiometric Ni0.20Cu0.20Zn0.60Fe2O4 (z0) the shrinkage rate peak is shifted subsequently down
to lower temperatures and reaches 900 1C for a sample with
addition of 1 wt% Bi2O3 (Fig. 7a). For the sub-stoichiometric ferrite
with z 0.02 signicantly lower Bi2O3 concentrations are sufcient to shift the maximum shrinkage rate to 900 1C (Fig. 7b). This
effect is supported by the fact that the temperature of the
maximum shrinkage rate of the sub-stoichiometric ferrite with
z0.02 appears at lower temperatures compared to z 0 already
for samples without Bi2O3 additive. Closer inspection of the
shrinkage rates of stoichiometric ferrites (z 0) reveals that the
maximum shrinkage rate peak is shifted from 990 to 900 1C for
0.375 and 1 wt% Bi2O3, respectively (Fig. 7a). A second, smaller
peak is also systematically shifted from 1055 1C to 965 1C for
0.375 and 1 wt% Bi2O3, respectively. In the case of sub-stoichiometric samples (z 0.02) a similar shift of the two shrinkage rate
peaks is found (Fig. 7b); however, an additional third peak at
around 840 1C signals the formation of a liquid phase and
subsequent rearrangement of particles. Liquid phase sintering
might be triggered by the formation of an eutectic in the system
Bi2O3CuONiOZnOFe2O3. Formation of eutectics at as low as
740 and 770 1C has been reported in the pseudo-binary ZnO
Bi2O3 and CuOBi2O3 systems, respectively [21,22]. Since this
shrinkage rate peak at 840 1C does not occur in the shrinkage rate
curves of stoichiometric ferrites with Bi2O3 additive (Fig. 7a),
melting of Bi2O3 (825 1C) is an unlikely reason for the appearance
of this peak in the case of sub-stoichiometric ferrites (Fig. 7b).
This observation suggests that the process of liquid phase formation includes CuO, which appears as an impurity phase during
ring of sub-stoichiometric ferrites. However, the observed series
of several shrinkage rate peaks is a signature of the underlying
liquid phase sintering, i.e. liquid formation, rearrangement and
solution-precipitation processes.
The density of powder compacts sintered at 900 1C for 2 h as a
function of the Bi2O3 additive concentration is shown in Fig. 8.
Stoichiometric ferrites exhibit little densication only; samples with
addition of 0.5 wt% Bi2O3 show a low density of about 4.3 g/cm3

Fig. 7. Shrinkage rate vs. temperature of compacts of Ni0.20Cu0.20Zn0.60Fe2.00O4.00


(a) and Ni0.20Cu0.20Zn0.62Fe1.98O3.99 (b) with additions of 0, 0.37, 0.5 and 1 wt%
Bi2O3.

(0.375, 0.5 and 1 wt%). The variation of the shrinkage rate as a


function of the additive concentration is shown in Fig. 7a and
compared to that of sub-stoichiometric ferrite with z0.02 and

Fig. 8. Density of Ni0.20Cu0.20Zn0.60Fe2.00O4.00 (z 0) and Ni0.20Cu0.20Zn0.62Fe1.98O3.99 (z 0.02) sintered for 2 h at 900 1C as a function of bismuth oxide
concentration.

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J. M
urbe, J. T
opfer / Journal of Magnetism and Magnetic Materials 324 (2012) 578583

(83%). A signicant increase in density to r 5.13 g/cm3 (99%) is


found at an additive concentration of 1 wt%. A different densication
behavior is observed for sub-stoichiometric ferrites. The density after
sintering at 900 1C of the sub-stoichiometric ferrite with z0.02 is
much larger even without addition of Bi2O3 (r 5.0 g/cm3 (96%)). The
density moderately increases through the addition of sintering aid
and a maximum density of 5.15 g/cm3 (99%) is obtained for 0.75 wt%
Bi2O3 addition [15]. These two different densication characteristics
signal that the Bi2O3 additive seems to have a different effect in the
case of stoichiometric and sub-stoichiometric NiCuZn ferrites.
The permeability of the stoichiometric ferrite Ni0.20Cu0.20
Zn0.60Fe2.00O4.00 (z 0) sintered at 900 1C with Bi2O3 additions as
a function of frequency is shown in Fig. 9. Small additive
concentrations (e.g. 0.5 wt%) result in low permeability due to
insufcient densication. These samples exhibit signicant porosity, which is detrimental with respect to domain wall movement and permeability. An increase of the Bi2O3 concentration
(1 wt%) leads to dense samples and improved permeability of
m 230 at 1 MHz. However, sub-stoichiometric ferrites with
z0.02 exhibit larger permeability. This is demonstrated for a

sample with 1% Bi2O3 additive concentration in Fig. 9; m 420 is


observed at 1 MHz. It was shown that the permeability of NiCu
Zn ferrites varies with additive concentration [15]. Samples with
low Bi2O3 concentrations exhibit a ne-grained microstructure
(grain size around 2 mm) and a permeability of m 400600.
Samples with intermediate Bi2O3 concentration (0.30.5%) show
heterogeneous microstructures formed through exaggerates grain
growth with large permeability of m 900. For larger additive
concentrations the ferrites are coarse-grained (grain size 10
20 mm) with m 400600 [15]. The microstructures of
Ni0.20Cu0.20Zn0.60Fe2.00O4.00 (z 0) and Ni0.20Cu0.20Zn0.62Fe1.98O3.99
(z 0.02) with additions of 1 wt% Bi2O3 are compared in Fig. 10.
For z 0 (Fig. 10a) the sintering additive has induced signicant
grain growth with a grain size of about 68 mm. Sintering additive
can be recognized as a thin lm between some of the grains. In
the sample with z0.02 and 1% Bi2O3 (Fig. 10b) discontinuous
grain growth has led to a fraction of large grains (about 10
20 mm) in a matrix of grains of 510 mm in size. Solidied additive
is found between the grains and in triple points. In addition, CuO
is segregated between some grains. The formation of large ferrite
grains is thought to be the main reason for the enhanced
permeability in sub-stoichiometric NiCuZn ferrite. It was
demonstrated that the permeability of NiCuZn ferrites scales
with grain size [23].

4. Conclusions
The sintering behavior and permeability of sub-stoichiometric Ni
CuZn ferrites of the iron-decient series Ni0.20Cu0.20Zn0.60 zFe2 z
O4 (z/2) (0rzr0.06) was investigated. It is shown that, compared to
stoichiometric ferrites (z0), sub-stoichiometric ferrites exhibit specic shrinkage behavior, microstructure and permeability:

Fig. 9. Permeability vs. frequency for Ni0.20Cu0.20Zn0.60Fe2O4


Ni0.20Cu0.20Zn0.62Fe1.98O3.99 (z 0.02) with additions of Bi2O3 (wt%).

(z 0)

and

1) With increasing sub-stoichiometry z the temperature of the


maximum shrinkage rate is shifted from T 1000 1C for z0
towards To900 1C for a sub-stoichiometric composition with
z Z0.02. After ring at 900 1C dense samples are obtained for
sub-stoichiometric ferrites (z40) only.
2) Nominally sub-stoichiometric ferrites decompose at 900 1C
into a stoichiometric ferrite and copper oxide. The appearance
of CuO seems to enhance the shrinkage signicantly.

Fig. 10. SEM micrographs of ferrites with z 0 (a) and z 0.02 (b) sintered for 2 h at 900 1C with addition of 1 wt% Bi2O3.

J. M
urbe, J. T
opfer / Journal of Magnetism and Magnetic Materials 324 (2012) 578583

3) Addition of Bi2O3 as a liquid phase sintering aid leads to an


additional shrinkage enhancement; however, the effect is
more pronounced for sub-stoichiometric ferrites. This is due
to the formation of low-melting eutectics.
4) Regular grain growth is observed in stoichiometric ferrites. The
addition of 1 wt% Bi2O3 to a sub-stoichiometric ferrite with
z0.02 results in a dense and inhomogeneous microstructure.
The permeability is increased from m 230 for stoichiometric
ferrites (z0) to m 430 for a sample with z 0.02. The
formation of CuO during sintering of sub-stoichiometric ferrites supports densication and is a prerequisite for low
temperature ring of multilayer inductors.

Acknowledgment

This work was supported by the Bundesministerium fur


Bildung und Forschung (Germany) via the research project NIKOL
(FKZ 03X45003F). The authors thank Dr. S. Barth (IKTS, Germany)
for helpful discussion.
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