Materials Sciences and Applications, 2013, 4, 478-482
http://dx.doi.org/10.4236/msa.2013.48058 Published Online August 2013 (http://www.scirp.org/journal/msa)
Microstructure and Dielectric Properties of PZS-PLZT
Ceramics System
Sakri Adel*, Boutarfaia Ahmed
Laboratory of Applied Chemistry, University of Biskra, Biskra, Algeria.
Received June 5th, 2013; revised July 8th, 2013; accepted July 17th, 2013
Copyright © 2013 Sakri Adel, Boutarfaia Ahmed. This is an open access article distributed under the Creative Commons Attribution
License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
ABSTRACT
Piezoelectric ceramics are an important class of solid-state materials as they exhibit a wide range of applications. This
article investigates the sintering temperature effect on microstructure and dielectric properties of a new ceramics mate-
rial Pb (Zn, Sb) O3-PbLa (Zr, Ti) O3 (PZS-PLZT), which was prepared by a solid mixed-oxide solution method. Scan-
ning electron micrograph (SEM) and X-ray diffraction (XRD) techniques was employed to examine the crystallization
of the ceramics. The results of XRD show that the phase structure of the samples is tetragonal. The lattice parameters
and the density increased with increase of the sintering temperature. The dielectric constant and the dielectric loss of the
investigated samples decreased with increase in the frequency.
Keywords: Ferroelectric; Microstructure; Piezoelectric Ceramics; Dielectric Properties
1. Introduction
The piezoelectric property plays an important role for
electric and electronic materials. The most widely used
piezoelectric materials are based on the PbTiO3-PbZrO3
system (PZT) [1-3]. The application of the PZT compo-
nent is wide, including nonvolatile memory elements,
pyroelectric detectors, piezoelectric transducers, and pho-
toelectric devices [4,5], but the electrical and thermal
properties of PZT ceramics depend to a large extent on
their surface microstructures [6]. Many researchers have
considered modified PZT compositions with suitable
substitution at the A and B sites [7-9] with some dopants
to improve their electrical and mechanical property of
piezoelectric materials in recent years, this dopants can
be classified into two categories: donor dopants which
induce Pb vacancies by changing with a higher valence
ion for Pb2+ or (Ti, Zr)4+ like Sb5+, La3+. And the acceptor
dopants induce O vacancies by changing with a lower
valance ion for Pb2+ or (Ti, Zr)4+ example K+, Fe3+ [10,
11]. So the properties of a PZT samples are very sen-
sitive to additives, composition and synthesis methods.
Whatmore et al. [12] and Chaipanich et al. [13] have
reported that the electric properties of PZT ceramics
could be improved by the doping of Sb2O3. [14]. It was
found that sintering behavior had obvious effects on the
microstructure and piezoelectric properties. With the in-
crease of sintering temperature, the microstructure of the
ceramic samples changed accordingly and the porosity
decreased [15].
There have been several reports on La substituted PZT.
It has been reported that substitution of Pb2+ by La3+ ions
created vacancies in the A site of perovskite ABO3
structured PZT ceramics. The 7% La doped PZT ceram-
ics PLZT (7/60/40) composition is one of the most im-
portant candidates for piezoelectric applications due to its
extremely high piezoelectric and electromechanical cou-
pling coefficients reported in literature [16-18].
In this work, a new ceramics material based PZT is
prepared by a solid mixed-oxide solution method, and we
investigate the structural, dielectrical properties of a
doped PZT ceramic with La, Sb and Zn for different sin-
tered temperature.
2. Experimental
The composition of PZS-PLZT system was 0.3Pb(Zn1/3,
Sb2/3)O3-0.7Pb0.98La0.02(Zr0.48,Ti0.52)O3 were synthesized
from high purity oxide powders PbO (99.90%), ZrO2
(99.90%), TiO2 (99.80%), Sb2O3 (99.90%), ZnO
(99.90%), and La2O3 (99.90%), the samples were pre-
pared by the conventional ceramic procedure. Stoichio-
metric amount of metal for the designated PZS-PLZT
*Corresponding author.

Microstructure and Dielectric Properties of PZS-PLZT Ceramics System 479
composition was mixed for 2 hours as the grinding media
and ethanol as the solvent. After milling for 6 hours, the
resultant slurry was dried in an oven and then the pow-
ders were calcined in a high-temperature furnace at
850˚C for 120 min. Then, the calcined powder was ball-
milled again to ensure a fine particle size for 6 hours.
After drying, the powder was pressed as disks and sin-
tered at two different temperatures 1050˚C and 1200˚C in
a closed aluminum crucible, the atmosphere was en-
riched in PbO vapor using PbZrO3 powder, the density of
the sintered component was measured from its mass and
dimensions. The sintered discs were next mechanically
processed by abrasion, dried and electrified with a silver
paste burned out at 700˚C for 30 min. The polling was
carried out in a silicon oil bath at 100˚C under an electric
field of 3 kV/mm and cooled down to room temperature
still being under the influence of the electric field. They
were aged for 24 h prior to testing. The temperature de-
pendence of dielectric properties was measured at tem-
peratures ranging from room temperature to 650˚C with a
heating using an impedance analyzer. An X-ray diffract
meter BRUKER-AXE, D8 with CuKα radiation (λ =
1.5406 Å). Using the JCPDS database we can identify
the presence of the perovskite structure and phases of the
sintered samples. Surface microstructures of the ceramics
were observed using a scanning electron microscopy
(SEM) (JEOL JSM-6390LV) at room temperature.
3. Results and Discussion
3.1. X-ray Diffraction (XRD)
The XRD patterns of PZS-PLZT ceramics shown in
Figure 1 were identified as a material with perovskite
structure having tetragonal symmetry according to
JCPDS (Joint Committee of Powder Diffraction Stan-
dards) card n 00-046-0504. The tetragonal lattice pa-
rameters were determined from the evolution of the
tetragonal peaks (200) and (002) by using CELREF
software.
The results given in Table 1 revealed that the tetrago-
nal cell parameters are associated with some physical
properties of the sintered samples. The lattice parameters
and the density increased with increase the sintering tem-
perature.
3.2. Scanning Electron Micrograph (SEM)
Figure 2 shows the scanning electron micrograph (SEM)
microstructure of the porous PZS-PLZT prepared sam-
ples sintered at 1050˚C and 1200˚C by (SEM: JEOL
JSM-6390LV). The increase of grain size from ≈1.83 µm
to ≈3.12 µm is observed significantly with the increasing
of sintering temperature from 1050˚C to 1200˚C respec-
tively, and it can clearly be seen that the prepared PZS-
PLZT ceramics is porous and has a not uniform distribu-
tions of grain shape and size.
Figure 1. XRD patterns of PZS-PLZT ceramics sintered at (a) 1050˚C and (b) 1200˚C.
Table 1. Some physical properties of the sintered PZS-PLZT ceramics.
lattice parameters
Sintering temperature (˚C) Thickness [cm] Diameter [cm] specific weight [g/cm3] phase
a [Å] b [Å] c [Å]
1050˚C 0.18 1.20 6.635 T 4.0155 4.0155 4.0517
1200˚C 0.18 1.15 7.598 T 4.0346 4.0346 4.0714

Microstructure and Dielectric Properties of PZS-PLZT Ceramics System 480
Figure 2. SEM micrographs of PZS-PLZT ceramics sintered at (a) 1050˚C; (b) 1200˚C for 2 hours.
Figure 3. Temperature dependence of ɛr for PZS-PLZT
samples sintered at 1050˚C and 1200˚C.
3.3. Dielectric Properties and the Loss Factor
Figure 3 shows the variation of the dielectric constant at
5 kHz with increment of temperature for the two samples
witch sintered at 1050˚C and 1200˚C. Similar to normal
ferroelectrics, the dielectric constant increases gradually
with increasing temperature up to the transition tem-
perature, then it decreases. Here we can note the most
important characteristic of a disordered perovskite struc-
ture. The dielectric constant reaches a maximum value of
19,130 (Tc = 500˚C) for sample sintered at 1050˚C, but
for the sintering temperature 1200˚C, the dielectric
constant continues increasing (out of range temperature
Tc > 650˚C). There, may be that this result is due to the
change in the bulk density and the grain morphology
with the change of sintering temperature [19]. This
constant decreases gradually with increasing frequency
(Figure 4) it reaches a maximum value at small values of
frequency which explained by existence of different
polarization models [20,21]. The dielectric constant of
Figure 4. Frequency dependence of ɛr for PZS-PLZT sam-
ples sintered at 1050˚C and 1200˚C.
Figure 5. Temperature dependence of Tangδ for PZS-PLZT
samples sintered at 1050˚C and 1200˚C.
sample sintered at 1200˚C decreases slowly than of

Microstructure and Dielectric Properties of PZS-PLZT Ceramics System 481
Figure 6. Frequency dependence of Tangδ for PZS-PLZT
samples sintered at 1050˚C and 1200˚C.
1050˚C sintered sample.
Figure 5 shows the variation of the loss factor Tangδ
with temperature. Tangδ increases gradually with in-
creasing temperature. For sintered temperature 1050˚C
the loss factor reaches a maximum value of 0.65 at (Tc =
550˚C), but for the sintering temperature 1200˚C, the
dielectric constant continues increasing (out of range
temperature Tc > 650˚C). This may be caused by the
losses due to the electrical conduction. This factor de-
creases with increasing frequency (Figure 6), which is a
characteristic of ferroelectrics [22,23].
4. Conclusion
PZS-PLZT was successfully prepared by a solid mixed-
oxide solution method; The X-ray diffraction measure-
ments for all 0.3Pb(Zn1/3,Sb2/3)O3-0.7Pb0.98La0.02(Zr0.48,
Ti0.52)O3 sintered samples indicated the presence of te-
tragonal phase and the scanning electron micrograph
shows a porous nature of ceramics and the grain size
increases with increasing the temperature. The influence
of the sintering temperature on the properties of PZS-
PLZT ceramics was studied. The lattice parameters and
the density increased with increase of the sintering tem-
perature. The dielectric constant and the dielectric loss of
the sintered samples decreased with increase in the fre-
quency. The effects of the sintering temperature on the
dielectric properties can be attributed to the change in the
bulk density and the grain morphology with the change
of the sintering temperature.
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