Parjansri et al.
Modifying the Electrical Properties of Ba0ꢀ85Ca0ꢀ15Zr0ꢀ1Ti0ꢀ9O Ceramics by the Nanocrystals-Induced Method
3
develop a single crystal growth under controlled tempera-
ture conditions, observing good electrical properties. Li
et al. reported the perovskite phase formation and electri-
thickness and diameter about 2.0 mm and 10 mm, respec-
tively; afterwards, we sintered them at 1450 C for 4 h.
7
–9
ꢀ
We investigated the phase formation and microstructure
of the samples by X-ray diffraction (XRD) (XRD 6000,
Shimadzu) and scanning electron microscopy (SEM). For
electrical properties characterization, we polished the sin-
tered ceramics, and we coated both faces with silver as
electrodes. We investigated the dielectric properties of the
sintered ceramics as a function of frequency and tempera-
ture by using an automated dielectric measurement system
(E4980A Precision LCR meter). The coated samples had
an applied electric field of 1–2 kV/mm for measuring fer-
roelectric properties by using a Sawyer Tower circuit. We
poled the specimens by applying a DC field of 3 kV/mm
cal properties of Pb(Zn1/3Ta2/3ꢁO ceramic, prepared using
3
PbTiO3 as seeds, finding that a pure perovskite phase
could be formed at low calcination temperatures, while
obtaining a high dielectric constant (ꢂ ) and low dielec-
r
8
tric loss (tan ꢃ) for the seed-added sample. Ye et al. have
9
reported the template grain growth method, studying the
effect of BaTiO (BT) template on the electrical properties
3
of Ba0ꢀ85Ca0ꢀ15Zr0ꢀ10Ti0ꢀ90O . Preparing the BT-template by
3
the molten-salt method and using a calcination tempera-
ꢀ
ture of 1100 C, these researchers found that the textured
BCZT ceramics (templates-added sample) showed a piezo-
electric coefficient of d33 ∼470 pC/N, an electromechani-
cal coefficient of k ∼ 40%, and a Curie temperature (T )
ꢀ
for 30 min in a silicone oil bath at 28 C. After 24 h,
we measured the piezoelectric charge coefficient (d ) by
p
C
33
higher than the sample without BT templates. The above
literature suggests that the seed-induced method and tem-
plate grain growth can enhance the electrical properties of
piezoelectric ceramics using a low calcination temperature.
In the present work, we prepared and characterized
Ba0ꢀ85Ca0ꢀ15Zr Ti O ceramics using the seed-induce
using a S5865 d33 meter (KCF Technologies). Moreover,
we calculated the piezoelectric voltage coefficient (g ) and
3
3
the electromechanical coupling coefficients (k ), plotted as
t
a function of the CT seed content
0ꢀ1
0ꢀ9
3
3
. RESULTS AND DISCUSSION
method. We used CaTiO (CT) prepared by the molten-
3
From the introduction section, many researchers have
carried out studies on developing lead-free piezoelectric
ceramics to replace the PZT-based ceramics in piezoelec-
tric applications.
salt method as seeds, because it exhibits different struc-
tures depending on the transition temperature and shows
1
0
an orthorhombic phase at room temperature. However,
we obtained the perovskite structure of CT powder from
a preparation by a mixed oxide method using a high cal-
Delivered by Ingenta to: Florida State University, College of Medicine
Ba Ca Zr Ti O ceramic represents one of
0
ꢀ85
0ꢀ15
0ꢀ1 0ꢀ9
3
IP: 185.46.86.229 On: Sun, 04 Dec 2016 19:16:33
ꢀ
11
the materials of interest, displaying the highest
cination temperature of about 1350 CC .o p yTr hi gu hs t, : wA em ue sr ei cd an Scientific Publishers
d
value. However, some electrical properties (e.g., ꢂ ,
3
3
r
nano-size particles of CT powder prepared by the molten
salt method as seed for producing the pure perovskite
phase, controlling the grain orientation and crystal orien-
tation direction and improving the electrical properties for
the BCZT ceramics.
tan ꢃ, and T ) still cannot compare with PZT-based
C
ceramics. Also, we obtained the highest d33 value at the
highest calcination temperature, using very long dwelling
times. The modification of crystal structure by controlling
the grain orientation serves as a well-known method to
enhance the properties and performance of piezoelectric
materials. In this research, we used the seed-induced
method. We successfully obtained BCZT ceramics, pre-
pared using the CT seed-induced method. We investigated
the phase structure, microstructure, and the electrical
properties. We synthesized the CT seed powder by the
molten-salt method. The phase formation of the CT seed
presented that we obtained pure perovskite with a small
particle size of about ∼300 nm, by using heating temper-
2
. EXPERIMENTAL DETAILS
We synthesized the Ba0ꢀ85Ca0ꢀ15Zr Ti O ceramic sam-
0ꢀ1
0ꢀ9
3
ples using the seed-induced method. We prepared the seed
via the molten salt method, using CaCO and TiO oxides
3
2
as starting materials. We mixed the starting powder by
ball-milling for 24 h, mixed with KCl–NaCl salt (1:1) for
ꢀ
3
0 min, then heated at 900 C for 2 h. Then, we washed
them with hot deionized water several times until finding
no trace of anion. After that, we mixed the CT seed with
the starting material of the BCZT system, prepared by the
mixed oxide method. We mixed stoichiometric amounts
of BaCO (99%, Sigma–Aldrich), CaCO (98.5–100.5%,
ꢀ
atures of 900 C for 2 h. We indexed the pure perovskite
phase of the CT seed in reference to the orthorhombic
structure of CaTiO (JCPDS No. 01-086-1393), confirmed
3
from XRD patterns, as shown in Figure 1. Inset (a)
in Figure 1 shows the microstructure of the CT seed
powder. We mixed the CT seed obtained with the metal
oxides of BCZT systems by the mixed oxide method.
The results showed that the non-seed sample and CT
seed-added sample possessed a pure perovskite phase,
as displayed in Figure 2. For the expanded graph of
3
3
Sigma–Aldrich), ZrO (99%, Sigma–Aldrich), TiO (99–
2
2
1
05.5%, Sigma–Aldrich), Nb O (99%, Sigma–Aldrich),
2 5
and CT seeds. We varied the CT seed content from 0.0 to
1
0.0 mol% (x = 0.0, 0.04, 0.08, and 0.10). We ball-milled
the mixed powder for 24 h using ethanol as a solvent with
zirconia grinding media, then dried in an oven at 120 C.
We calcined all ceramic powders at 1250 C for 2 h.
ꢀ
ꢀ
ꢀ
XRD patterns around 2ꢄ of 44–46 , the non-seed sample
Then, we pressed the calcined powder into a disk shape of
and seed-added samples showed a broad peak and sharp
J. Nanosci. Nanotechnol. 16, 12956–12961, 2016
12957