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Low-Temperature Sintering of Bi0.5(Na,K)0.5TiO3 for Multilayer Ceramic

Actuators

Article  in  Journal of the American Ceramic Society · March 2015

DOI: 10.1111/jace.13564

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Journal
Low-Temperature Sintering of Bi0.5(Na,K)0.5TiO3 for Multilayer
Ceramic Actuators
Chang Won Ahn,‡ Hee Sung Kim,‡ Won Seok Woo,‡ Sung Sik Won,‡ Hae Jin Seog,‡ Song A Chae,‡
Bong Chan Park,‡ Ki Bong Jang,§ Yun Po Ok,§ Hyon Ho Chong,§ and Ill Won Kim‡,†
‡
Department of Physics and EHSRC, University of Ulsan, Ulsan 680-749, Korea
We investigated the influence of CuO amount (0.5–3.0 mol%),
sintering temperature (900°C–1000°C), and sintering time
(2–6 h) on the low-temperature sintering behavior of CuO-
added Bi0.5(Na0.78K0.22)0.5TiO3 (BNKT22) ceramics. Normal-
ized strain (Smax/Emax), piezoelectric coefficient (d33), and rem-
anent polarization (Pr) of 1.0 mol% CuO-added BNKT22
ceramics sintered at 950°C for 4 h was 280 pm/V, 180 pC/N,
and 28 lC/cm2, respectively. These values are similar to those
of pure BNKT22 ceramics sintered at 1150°C. In addition, we
investigated the performance of multilayer ceramic actuators
made from CuO-added BNKT22 in acoustic sound speaker
devices. A prototype sound speaker device showed similar out-
put sound pressure levels as a Pb(Zr,Ti)O3-based device in the
frequency range 0.66–20 kHz. This result highlights the feasi-
bility of using low-cost multilayer ceramic devices made of
lead-free BNKT-based piezoelectric materials in sound speaker
devices.
I. Introduction
I N the past decade, lead-free piezoelectric ceramics such as
(K,Na)NbO3 (KNN) and Bi0.5Na0.5TiO3 (BNT)-based
materials have been widely studied as replacements for lead-
based materials because of environmental concerns about
Pb-containing materials such as lead zirconate titanate,
which contains more than 60 wt% Pb.1–3
Recently, many studies on lead-free piezoelectric ceramics
have been published.3–5 Among various lead-free piezoelec-
tric materials, BNT-based ceramics are of particular interest
because of their high electric-field-induced strain6–8 and
blocking force,9,10 which play important roles in piezoelectric
actuator applications.
Even though many studies have reported the physical
properties of BNT-based lead-free ceramics, only a few
reports are available about their practical applications.11–13
Multilayer ceramic devices such as multilayer ceramics actua-
tors (MLCAs) and multilayer ceramics capacitors are widely
used in industry.14,15 In this study, we developed a MLCA
using BNT-based materials. When developing a MLCA, the
difference in thermal expansion coefficients and reaction
between the internal electrode and active material should be
considered because the MLCA is cofired with the internal
electrode. Differences in thermal expansion coefficients or
reactions between the internal electrode and active material
can cause significant problems in the MLCA, such as internal
cracks in the active ceramics layers or microdefects between
J. Jones—contributing editor
Manuscript No. 35978. Received November 26, 2014; approved February 18, 2015.
†
Author to whom correspondence should be addressed. e-mail: kimiw@mail.ulsan.ac.kr
1877
J. Am. Ceram. Soc., 98 [6] 1877–1883 (2015)
DOI: 10.1111/jace.13564
© 2015 The American Ceramic Society
§
R&D Center, Samjeon Co. Ltd, Ulsan 689-934, Korea
the active layers and internal electrodes. Therefore, it is
important to find combinations of materials that do not have
these problems.
Ag–Pd internal electrodes are widely used in MLCAs.
However, Bi ions usually react with Pd elements at high
cofiring temperatures above 1100°C.16,17 Bi0.5Na0.5TiO3-
based ceramics should be sintered at temperatures higher
than 1150°C to obtain complete densification. Therefore, if a
MLCA is produced at a high sintering temperature using
BNT-based ceramics as the active layer material and Ag–Pd
as the internal electrode, the actuating performance of the
MLCA may suffer.
Nguyen et al. tried to fabricate MLCAs using BNT-based
ceramics with Ag–Pd (7:3) internal electrodes.18 However,
the Ag–Pd electrodes were not perfectly active at cofiring
temperatures of 1100°C–1140°C, and the electrical properties
of the MLCAs deteriorated compared to those of bulk
ceramics. Low-temperature sintering of ceramics is therefore
important to prevent a decrease in performance of MLCAs
and to produce them at low cost. High sintering tempera-
tures can decrease the stability of piezoelectric properties
because of the formation of interfacial microdefects and
internal electrode loss. Moreover, the ratio of expensive Pd
in Ag–Pd internal electrodes has to be increased. Therefore,
the sintering temperature of BNT-based ceramics needs to be
decreased for practical application of MLCAs.
In this study, we investigated the low-temperature sinter-
ing behavior of CuO-added Bi0.5(Na0.78K0.22)0.5TiO3
(BNKT22) ceramics. In particular, we evaluated the influence
of the amount of CuO (0.5–3.0 mol%), sintering temperature
(900°C–1000°C), and sintering time (2–6 h). In addition, we
evaluated the performance of acoustic sound speaker devices
containing MLCAs made from CuO-added BNKT22.
II. Experimental Procedures
(1) Low-Temperature Sintering of
Bi0.5(Na0.78K0.22)0.5TiO3 Ceramics
Bi0.5(Na0.78K0.22)0.5TiO3 (BNKT22) powder was prepared
using a conventional solid-state reaction method. Bi2O3,
Na2CO3, TiO2, and K2CO3 (99.9% High Purity Chemicals,
Saitama, Japan) were the starting raw materials. Before
weighing, the raw powders were dried in an oven at 80°C for
24 h to remove any moisture. Starting materials were
weighed according to the stoichiometric ratio and then ball-
milled for 24 h in ethanol with zirconia balls. Upon drying
at 80°C, the powders were ground and calcined at 850°C for
2 h in a covered alumina crucible. Powders were ground and
ball-milled again using the same conditions as described for
the initial milling step to prepare fine and uniform particles.
Then, an excess amount of CuO at 0.5, 1.0, 2.0, or 3.0 mol%
was introduced to the calcined pure BNKT22 powder, and
1878 Journal of the American Ceramic Society—Ahn et al.
the mixed powders were ball-milled again for 24 h, then
dried at 100°C for 24 h. The obtained powders were mixed
with an aqueous polyvinyl alcohol solution, and made into
green disks with diameters of 10 mm at a pressure of
100 MPa. After binder burnout at 500°C, the disks were sin-
tered at sintering temperatures ranging from 900°C to
1000°C and sintering times ranging from 2 to 6 h in closed
alumina crucibles.
Purity and formation of the desired phase in sintered
samples were monitored by powder X-ray diffraction
(XRD; X’ Pert-PRO, PANalytical, Almelo, the Nether-
lands) using CuKa1 radiation. For microstructural analysis,
the surface of the as-sintered samples was removed by lap-
ping. Lapped samples were then mirror-polished and ther-
mally etched at 900°C–1000°C for 10 min depending on
their composition. Finally, Field-emission scanning electron
microscopy (FE-SEM; S-4200, Hitachi, Tokyo, Japan) was
used to examine the microstructure of the polished and
thermally etched samples. Sintered disk-type samples were
polished down to a thickness of 1 mm to assess their elec-
Fig. 1. X-ray diffraction patterns of BNKT22 ceramics sintered at
1150°C and BNKT22-CuO 1 mol% ceramics sintered at 900°C,
950°C, and 1000°C for 4 h.
(a)
(c)
Fig. 2. FE-SEM images of (a) pure BNKT22 ceramics sintered at 1150°C and BNKT22:CuO 1.0 mol% ceramics sintered at (b) 1000°C, (c)
950°C, and (d) 900°C for 4 h. All sample surfaces were thermally etched at each sintering temperature for 10 min after polishing.
Vol. 98, No. 6
trical properties. Silver paste was applied through screen
printing of both surfaces of the disks as electrodes. After
applying the silver paste, disks were fired at 700°C for
30 min. Ferroelectric hysteresis loops were measured in sili-
con oil with the aid of a Sawyer–Tower circuit to apply an
electric field with a sinusoidal waveform. Electric-field-
induced strain was measured with a linear variable differen-
tial transducer (Mitutoyo MCH-331 & M401, Kawasaki,
Japan). The piezoelectric charge coefficient d33 was mea-
sured using a piezo d33 meter (ZJ-3A; Institute of Acous-
tics, Chinese Academy of Sciences, Beijing, China).
(2) Fabrication of Multilayer Ceramic Actuators
Slurries for tape-casting were prepared by mixing the cal-
cined powders, solvent, binder, and plasticizer. As inner elec-
trodes, silver-palladium paste (SJAP-12-510X; Sung Jee
Tech. Co., Suwon, Korea) was screen-printed on the sheet.
Ag and Pd contents were 90% and 10%, respectively. CuO
1.0 mol%-added BNKT22 ceramic green sheets were pre-
pared by tape-casting a slurry containing CuO 1.0 mol%-
added BNKT22 powder, ethyl alcohol (94% purity, ethanol;
SK Chemical, Sungnam, Korea), methyl ethyl ketone
(99.5% purity, MEK; Daejung Chemical & Metals Co., Ltd)
as a solvent, polyvinyl butyral (BM-SZ; Sekisui Chemical
Co., Ltd, Tokyo, Japan) as a binder, dibutyl phthalate
(94%; Daejung Chemical & Metals Co., Ltd) as a plasti-
cizer, and BYK-112 (BYK Chemical, Wesel, Germany) as a
dispersant.
The slurry was tape-casted using a doctor blade to a thick-
ness of about 40 lm and then dried at room temperature.
Ag–Pd paste was screen-printed on the ceramic sheet as the
inner electrode. Ceramic sheets with thick film electrodes
were stacked and then pressed at 50°C under 50 MPa pres-
sure for 5 s to enhance adhesion between layers. Each sheet
was laminated and cut to form a green compact. The final
dimensions of the green compact were about
25.0 mm 9 20.0 mm 9 0.25 mm. Six layers of sheets were
laminated and internal electrodes were connected to the
(b)
(d)
June 2015 Bi0.5(Na,K)0.5TiO3 MLCA 1879

(a) (b) (c)

(d) (e) (f)

Fig. 3. EDX mapping results of BNKT22:CuO 1.0 mol% ceramics sintered at 950°C for 4 h: (a) Surface morphology (b) Cu-mapping, (c) Bi-
mapping, (d) Na-mapping, (e) K-mapping, (f) Ti-mapping.

(a) (b)

(c) (d)

Fig. 4. (a) Piezoelectric coefficient (d33) and normalized strain (Smax/Emax), (b) bipolar S–E loops, (c) unipolar S–E loops, and (d) P–E loops of
BNKT22:CuO 1.0 mol% ceramics samples as a function of sintering temperature. Pure BNKT22 sintered at 1150°C was used as the reference
sample.
1880 Journal of the American Ceramic Society—Ahn et al. Vol. 98, No. 6

external electrode to synthesize piezoelectric speakers. A III. Results and Discussion

schematic diagram of the piezoelectric speaker is presented in
fig. 10(b). Before sintering, the binder was burnt out in air
by heating the samples at 500°C for 10 h. Cofiring was car-
ried out in a covered alumina crucible at a temperature of
950°C with a soaking time of 4 h in air.
Sound pressure level (SPL) of the piezoelectric speakers
was measured using an omnidirectional microphone (UMIK-
1; miniDSP Ltd., Hong Kong, China) and multichannel
dynamic signal analyzer (Electroacoustic toolbox; Faber
Acoustical, LLC, UT) with a 30 Vp-p input signal. The dis-
tance between the speaker and microphone was 10 cm. Sam-
ples were prepared to conform to the KS CIEC 60268-5
standard.
X-ray diffraction patterns of BNKT22 and BNKT22:CuO
1 mol% ceramics in the 2h range 20°–80° are shown in
Fig. 1. All samples exhibited a single-phase perovskite struc-
ture. The XRD profiles suggest that no crystalline second
phase is induced with the addition of CuO within the resolu-
tion limit of the apparatus used.
FE-SEM images of pure BNKT22 ceramics sintered at
1150°C are shown in Fig. 2(a). Pure BNKT22 ceramics had
a dense surface morphology with round grains without any
pores. BNKT22:CuO 1.0 mol% ceramics sintered at 1000°C
and 950°C also had a dense surface morphology, but the
number of pores was much greater in the specimen sintered

(a) (b)

(c) (d)

Fig. 5. Piezoelectric coefficient (d33) and normalized strain (Smax/Emax) of CuO-added BNKT22 ceramics as a function of CuO content at
sintering temperatures of (a) 925°C, (b) 950°C, (c) 975°C, and (d) 1000°C. All specimens were sintered for 4 h.

(a) (b)

Fig. 6. Piezoelectric coefficient (d33) and normalized strain (Smax/Emax) of BNKT22:CuO 1.0 mol% ceramics as a function of sintering time at a
sintering temperature of (a) 925°C and (b) 950°C.
June 2015 Bi0.5(Na,K)0.5TiO3 MLCA
Fig. 7. Temperature-dependent dielectric constant and the
corresponding loss factor of BNKT22 and BNKT22:CuO 1.0 mol%
ceramics.
Fig. 8. Temperature stability of the piezoelectric coefficient (d33) of
poled BNKT22 and BNKT22:CuO 1.0 mol% ceramics.
at 900°C than those sintered at the higher sintering tempera-
tures.
Successful incorporation of CuO into the BNKT22 ceram-
ics was demonstrated by energy-dispersive X-ray spectros-
copy (EDX). EDX mapping spectra of each element in
BNKT22:CuO 1.0 mol% ceramics are shown in Fig. 3.
Homogeneous distribution of Cu was observed [Fig. 3(b)]. It
has been reported that added CuO not only forms a liquid
phase, but also diffuses into the lattice by replacing B-site
ions.19 This leads to homogeneous distribution of Cu ions.
In general, the formation of a liquid phase of CuO leads to
low-temperature sintering behavior and the Cu2+ ions that
replace Ti4+ B-site ions in BNT-based perovskite structures
act as acceptors.19
Piezoelectric coefficient (d33) and normalized strains
(Smax/Emax) of pure BNKT22 ceramics sintered at 1150°C,
and BNKT22:CuO 1.0 mol.% ceramics sintered at various
temperatures ranging from 900°C to 1000°C with 25°C steps
are shown in Fig. 4(a). Piezoelectric coefficient (d33) and
normalized strain (Smax/Emax) of pure BNKT22 sintered at
1150°C were 180 and 275 pm/V, respectively. These proper-
ties were maintained with slight deterioration at the lower
sintering temperature of 925°C in 1.0 mol% CuO-added
samples. The d33 and Smax/Emax of BNKT22:CuO 1.0 mol%
sintered at 950°C were 175 pC/N and 270 pm/V, respec-
tively. These values represent a degradation rate of about
3% compared with those of the pure BNKT22 reference
samples.
1881
S–E loops and P–E loops of BNKT22:CuO 1.0 mol%
ceramics samples in the sintering temperature range 950°C–
1000°C showed similar behaviors to pure BNKT22 sintered
at 1150°C, as shown in Figs. 4(b)–(d). However, these prop-
erties deteriorated drastically at the lower sintering tempera-
ture of 900°C due to the low density of the specimen, as
shown in Fig. 2.
Changes in the d33 and Smax/Emax values of CuO-added
BNKT22 ceramics as a function of CuO content at various
sintering temperature are presented in Fig. 5. Values of d33
and Smax/Emax were stable in specimens within the experi-
mental CuO content range sintered at 925°C and 950°C. The
d33 and Smax/Emax values were about 175 pC/N and 270 pm/
V, respectively. However, the specimens sintered at 975°C
and 1000°C showed a drastic decline in d33 and the Smax/
Emax values at a CuO content above 2 mol%. These
decreases in d33 and Smax/Emax values at relatively high sin-
tering temperatures and high CuO content were likely caused
by the hardening effect of acceptor doping due to replace-
ment of Ti4+ B-site ions with Cu2+.19
Figure 6 shows d33 and Smax/Emax of BNKT22:CuO
1.0 mol% ceramics as a function of sintering time at a sinter-
ing temperature of 925°C and 950°C. While samples sintered
at 925°C had low d33 values after the relatively short sinter-
ing time of less than 4 h, as shown in Fig. 6(a), samples sin-
tered at 950°C had stable d33 and Smax/Emax values over
sintering times ranging from 2 to 6 h, as shown in Fig. 6(b).
In conclusion, the appropriate sintering temperature for
CuO-added BNKT22 ceramics is 950°C based on the results
shown in Figs. 5 and 6. And, the 1.0 mol% CuO-added sam-
ples show relatively reliable piezoelectric properties over wide
sintering temperature and time rang compare with other
CuO contents samples. Therefore, the appropriate fabrication
condition of MLCA specimens was decided as 1.0 mol%
CuO contents and sintering temperature of 950°C.
Temperature-dependent dielectric constant and the corre-
sponding loss factor for the poled materials were measured
from room temperature to 500°C. Profiles of the selected
compositions are presented in Fig. 7. Pure BNKT22 ceramics
exhibited two dielectric anomaly peaks at around 120°C and
250°C within the measuring temperature range. The first
inflection, which matched with the peak of dielectric loss, is
often designed as the depolarization temperature (Td) where
the ferroelectricity of the given system significantly decreases,
whereas the latter inflection point, called Tm, is where the
dielectric constant reaches its maximum. BNKT22:CuO
1.0 mol% ceramics exhibited dielectric anomaly peak related
with Td at 150°C which is 30°C higher than that of pure
BNKT22 ceramics. Furthermore, the peak of dielectric loss
of BNKT22:CuO 1.0 mol% ceramics at 150°C–220°C had a
blunt shape. To more clearly observe the depolarization
behavior, we measured the temperature stability of the piezo-
electric coefficient using poled samples after thermal shock.
The temperature stability of piezoelectric properties (d33)
was measured in the temperature range 40°C–250°C with a
step of 10°C after thermal shock at each temperature for
10 min, as shown in Fig. 8. BNKT22 and BNKT22:CuO
1.0 mol% ceramics had similar d33 values of 180 pC/N at
room temperature. In the case of BNKT22 ceramics, the d33
value decreased suddenly after thermal shock at 130°C for
10 min. However, the d33 value of BNKT22:CuO 1.0 mol%
ceramics decreased slightly to 140 pC/N near 150°C. This d33
value was maintained to 200°C. BNKT22:CuO 1.0 mol%
ceramics had a relatively good temperature stability, due to
the hardening effect of doping of Cu2+ ions at Ti4+ sites
and induced ferroelectric ordering from existing Cu00Ti  V O
defect dipoles.19
The high-temperature stability is important for practical
application of MLCAs, because it provides a wide tempera-
ture range for stable performance. Therefore, the addition of
CuO to BNKT-based ceramics not only decreased the sinter-
ing temperature, but also increased the temperature stability
1882 Journal of the American Ceramic Society—Ahn et al. Vol. 98, No. 6

(a) (b)

Fig. 9. (a) Cross-sectional FE-SEM micrograph and (b) magnified micrograph images of the fracture surface of a multilayer ceramic actuator
(MLCA) fabricated using BNKT22:CuO 1.0 mol% powder and Ag–Pd (9:1) internal electrodes. Specimens were cofired at 950°C for 4 h in air.

(a) (b)

(c)

Fig. 10. (a) Sound pressure level (SPL) versus frequency curve of piezoelectric speakers prepared using (1) Pb-based MLCA (0.12 mm
thickness) in a 24 mm 9 30 mm frame, (2) BNKT22:CuO 1.0 mol% MLCA (0.2 mm thickness) in a 24 mm 9 30 mm frame, and (3) BNKT22:
CuO 1.0 mol% MLCA (0.2 mm thickness) in a 60 mm 9 70 mm frame with a PET diaphragm (250 lm thickness). (b) Schematic diagram of
the piezoelectric MLCA consisting of six active layers. (c) Schematic diagram of the piezoelectric speaker consisting of the piezoelectric MLCA
and PET diaphragm.

of the piezoelectric properties of the ceramics. These data
suggested that BNKT22:CuO 1.0 mol% is suitable for use in
lead-free piezoelectric devices. To investigate the practical
applications of this material, we fabricated a prototype
MLCA device.
To examine the thermal stability of the BNKT22:CuO
1.0 mol% and Ag–Pd (9:1) layers, cross-sectional microstruc-
tures of MLCA specimens were observed by FE-SEM.
Cross-sectional microstructures of the fracture surface of a
MLCA specimen cofired at 950°C for 4 h in air are shown
in Fig. 9. Gray areas in Fig. 9(a) correspond to BNKT22:
CuO 1.0 mol% layers and bright lines between them indicate
electrode layers. MLCA specimen shows dense BNKT22:
CuO 1.0 mol% layers with good thickness uniformity and a
thickness of about 35 lm. When producing MLCAs using
general BNT-based materials, even if using an Ag–Pd (7: 3)
internal electrode, serious defects such as vertical cracks in
active layers and local disconnections in internal electrode
can occur because of the requirement for cofiring at a tem-
perature of 1150°C, which is near the melting point of the
electrode.18 However, in this study, no serious defects were
evident. To more clearly observe the interface between
BNKT22:CuO 1.0 mol% and internal electrode layers,
higher magnification micrographs were taken from the same
specimens as shown in Fig. 9(b). The Ag–Pd (9:1) layer had
good thickness uniformity with a thickness of about 2 lm
regardless of cofiring because of the low firing temperature
of 950°C.
We next fabricated a piezoelectric speaker using a bender-
type piezoelectric MLCA with six active layers of BNKT22:
CuO 1.0 mol% and an Ag–Pd (9:1) internal electrode in a
24 mm 9 30 mm metal frame. A lead-based piezoelectric
speaker was prepared for comparison. The SPL of lead-free
piezoelectric speakers at frequencies ranging from 100 and
20 000 Hz was measured, and the results are shown in
Fig. 10(a) along with those obtained using a lead-based pie-
zoelectric speaker that was prepared using a lead-based mate-
rial with a high d33 value of ~500 pC/N. The SPL of the
speaker was calculated using the following equation:20
 
I
SPL ¼ 10 log 10
Iref
where I is the intensity of the sound and Iref is the intensity
of the reference.
The fundamental frequency (f0) of the lead-free piezoelec-
tric speaker prepared with BNKT22:CuO 1.0 mol% ceramics
was 810 Hz and the SPL value at f0 was about 67 dB. This
speaker had a similar average SPL value to that of the lead-
based piezoelectric speaker in the frequency range from 2 to
20 kHz. However, the f0 (810 Hz) of the BNKT22-based
speaker was higher than that of the lead-based speaker
(300 Hz). This difference in f0 was mainly due to the different
thicknesses of the MLCA. Therefore, the weak SPL at low
frequencies of the BNKT22-based speaker can be modified
by changing the sample size and structure of the speaker. In
this work, the BNKT22-based speaker was modified using a
PET diaphragm to improve SPL characteristics at low fre-
quencies, as shown in Fig. 10(c), and the properties of this
speaker are displayed in Fig. 10(a). The f0 of the BNKT22-
based speaker modified with a PET diaphragm was 660 Hz
 June 2015 Bi0.5(Na,K)0.5TiO3 MLCA
and the SPL value at f0 was about 76 dB. Moreover, the
average SPL of this device was comparable with that of the
lead-based speaker in the frequency range between 660 Hz
and 20 kHz, which is part of the audible frequency range.
Therefore, the BNKT22:CuO 1.0 mol% piezoelectric MLCA
speaker is a good candidate for lead-free audible sound
devices. However, the SPL of the BNKT22:CuO 1.0 mol%
piezoelectric MLCA speaker was relatively low at frequencies
below 660 Hz. This low SPL value can be increased by
reducing the thickness of the MLCA.
IV. Conclusions
Low-temperature sintering properties of lead-free BNKT-
based piezoelectric ceramics with CuO as a sintering additive
were investigated. The optimal conditions for low-tempera-
ture sintering were 1.0 mol% CuO-additive, a sintering tem-
perature of 950°C, and a sintering time of 4 h. Samples
prepared under these conditions had similar piezoelectric
properties to those of pure BNKT22 ceramics sintered at
1150°C. Moreover, the addition of CuO to BNKT-based
ceramics not only decreased the sintering temperature, but
also increased the temperature stability of the piezoelectric
properties due to induced ferroelectric ordering from existing
Cu00Ti  V
O defect dipoles.
A piezoelectric MLCA was fabricated using active layers
of BNKT22:CuO 1.0 mol% and a Ag–Pd (9:1) internal
electrode, and then the performance of a loudspeaker
device with this MLCA was investigated. The average SPL
of this device was comparable to that of the lead-based
speaker in the frequency range between 660 Hz and 20
kHz. Therefore, BNKT22:CuO 1.0 mol% piezoelectric
MLCA speakers are good candidates for lead-free audible
sound devices.
Acknowledgments
This work was supported by the development program of the local science
park funded by the ULSAN Metropolitan City and the Ministry of Science,
ICT and Future Planning (MSIP).
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