Studies on new systems of BNT-based lead-free piezoelectric ceramics

Several new systems of Bi_0.5Na_0.5TiO₃-based lead-free piezoelectric ceramics were proposed based on the design of the multiple complex in the A-site of ABO₃ compounds. These ceramics were prepared by conventional ceramic techniques. The comparison of the piezo- and ferroelectric properties of these ceramics with those of the best properties of the Bi_0.5Na_0.5TiO₃-based lead-free piezoelectric ceramics published recently shows that these ceramics of the new systems have better ferroelectric and piezoelectric performance, and better temperature characteristic of the properties. Among these materials, Bi_0.5(Na_1?x?y K _x Li _y )_0.5TiO₃ possesses higher piezoelectric constant (d ₃₃?=?230.8 pC/N), higher electromechanical couple factor (k _p?=?0.41), larger remanent polarization (P _r?=?40 μC/cm²) and a better P–E hysteresis loop below 200 °C. Practical devices such as ceramic middle frequency filters and buzzers have been made by using these lead-free piezoelectric ceramics.     

Effects of co-doped CaO/MnO on the piezoelectric/dielectric properties and phase transition of lead-Free (Bi0.5Na0.5)0.94Ba0.06TiO3 piezoelectric ceramics

The piezoelectric properties of (1?x)(Bi_0.5Na_0.5)TiO₃-xBaTiO₃ ceramics were reported and their piezoelectric properties reach extreme values near the MPB (about x?=?0.06). The X-ray analysis of (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ ceramics for all compositions exhibited a pure perovskite structure without any secondary phase. Within a certain ratio of contents, the co-doped ceramics enhanced piezoelectric coefficient (d ₃₃ ), lowered the dielectric loss, and increased the sintered density. The temperature dependence of relative dielectric permittivity (K ₃₃ ^T ) reveals that the solid solutions experience two phase transitions, ferroelectric to anti-ferroelectric and anti-ferroelectric to relaxor ferroelectric, which can be proven by P-E hysteresis loops at different temperatures. In addition, the specimen containing 0.04/0.01 wt.% CaO/MnO showed that the coercive field E _c was a minimum value of 26.7 kV/cm, while the remnant polarization P _r was a maximum value of 38.7 μC/cm², corresponding to the enhancement of piezoelectric constant d₃₃ of 179 pC/N, electromechanical coupling factor k _p of 37.3%, and relative dielectric permittivity K ₃₃ ^T of 1137. (Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃ ceramics co-doped with CaO/MnO were considered to be a new and promising candidate for lead-free piezoelectric ceramics owing to their excellent piezoelectric/dielectric properties, which are superior to an un-doped BNBT system.     

Ferroelectric and piezoelectric properties of (Bi1/2K1/2)TiO3 ceramics fabricated by hot-pressing method

Bismuth potassium titanate, (Bi_1/2K_1/2)TiO₃ (BKT), ceramics were prepared by the hot-pressing (HP) method without dopant and with dopants of Bi₂O₃, La₂O₃ and MnCO₃. The relative density of BKT ceramics hot-pressed at 1,060 and 1,080 °C (hereafter abbreviated to BKT-HP1060°C and BKT-HP1080°C) and x mass% Bi₂O₃, La₂O₃ and MnCO₃ doped BKT ceramics hot-pressed at 1,060 °C (hereafter abbreviated as BKTBix; x?=?0.1–0.6, BKTLax; x?=?0.1–0.6 and BKTMnx; x?=?0.1–0.3) were all higher than 97%. In this study, the ferroelectric properties of BKT ceramics were successfully obtained, and the remanent polarization P _r and coercive field E _c of BKT-HP1080°C were 22.2 μC/cm² and 52.5 kV/cm, respectively. A small amount of La tends to increase P _r, and the P _r of BKTLa0.1 was 19.2 μC/cm². The piezoelectricities were improved to optimize poling conditions, and the electromechanical coupling factor k ₃₃ and piezoelectric constant d ₃₃ of BKT-HP1080°C were 0.34 and 82.8 pC/N, respectively.     

Microstructure and electrical properties of the rare-earth doped 0.94Na0.5Bi0.5TiO3-0.06BaTiO3 piezoelectric ceramics

Phase structure, microstructure, piezoelectric and dielectric properties of the 0.4 wt% Ce doped 0.94Bi_0.5Na_0.5TiO₃-0.06BaTiO₃ (Ce-BNT6BT) ceramics sintered at different temperatures have been investigated. The powder X-ray diffraction patterns showed that all of the Ce-BNT6BT ceramics exhibited a single perovskite structure with the co-existence of the rhombohedral and tetragonal phase. The morphologies of inside and outside of the bulk indicated that the different sintering temperatures did not cause the second phase on the inside of bulk. However, the TiO₂ existed on the outside of the bulk due to the Bi₂O₃ and Na₂O volatilizing at higher temperature. The ceramics sintered at 1,200 °C showed a relatively large remnant polarization (P _r) of about 34.2 μC/cm², and a coercive field (E _c) of about 22.6 kV/cm at room temperature. The permittivity ? _r of the ceramics increased with the increasing of sintering temperature in antiferroelectric region, the depolarization temperature (T _d) increased below 1,160 °C then decreased at higher sintering temperature. The resistivity (ρ) of the Ce-BNT6BT ceramics increased linearly as the sintering temperature increased below 1,180 °C, but reduced as the sintering temperature increased further. A maximum value of the ρ was 3.125?×?10¹⁰ ohm m for the Ce-BNT6BT ceramics sintered at 1,180 °C at room temperature.     

Investigation on the design and synthesis of new systems of BNT-based lead-free piezoelectric ceramics

Three primary differences between BNT- and PZT-based ceramics were analyzed from the composition and the active component of the materials. Based on the analysis the authors’ group developed the new idea of the design of the multiple complex in the A-site ions of BNT compounds. (Bi_0.5Na_0.5)²⁺, Bi³⁺ and Na⁺ in the ABO₃ structure are defined as A-site, A₁-site and A₂-site ions, respectively, and A, A₁ and A₂-site ions can be simultaneously or singly substituted partially by alkaline-earth metal ions, metal ions with +3 valence and metal ions with +1 valence, respectively. Under this consideration, Several new systems of Bi_0.5Na_0.5TiO₃ (abbreviated as BNT)-based lead-free piezoelectric ceramics were proposed. These ceramics can be prepared by conventional ceramic techniques and have excellent piezoelectric performance. Among these materials, Bi_0.5(Na_1−x−y K _x Li _y )_0.5TiO₃ possesses higher piezoelectric constant (d ₃₃ = 230 pC/N), higher electromechanical couple factor (k _p = 0.40), larger remanent polarization (P _r = 38.9 μC/cm²) and a better P-E hysteresis loop until about 200^∘C. This work was supported by the projects of NSFC (50410179), (50572066), and (59972020), and NAMMC (2001-AA325060).     

Structure and electrical properties of (Na0.5Bi0.5)1−x Ba x TiO3 ceramics made by a citrate method

(Na_0.5Bi_0.5)_1?x Ba _x TiO₃ (x?=?0–0.12) powders were synthesized by a citrate method, and the structure and electrical properties of the resulting ceramics were investigated. A gradual change of crystal structure with the increase of BaTiO₃ concentration was detected together with a significant evolution in grain size and shape. A rhombohedral-tetragonal morphotropic phase boundary (MPB) near x?=?0.06 at room temperature was ascertained for the ceramics. The dielectric constant (? _r) and dissipation factor (tanδ) attain maximum values at x?=?0.08 and x?=?0.06, respectively. The specimen of x?=?0.06 provides the maximum piezoelectric constant (d ₃₃?=?180 pC/N) and electromechanical coupling factor (k _p?=?0.28), accompanied by a large remanent polarization of P _r?=?37.1 μC/cm² and a low coercive field of E _c ?=?42.7 kV/cm.     

Phase transition,microstructure and properties of (Na<Subscript>0.5</Subscript>Bi<Subscript>0.5</Subscript>)<Subscript>1-x</Subscript>Ba<Subscript>x</Subscript>TiO<Subscript>3</Subscript> lead-free piezoelectric ceramics

In this article, (Na_0.5Bi_0.5)_1-xBa_xTiO₃ lead-free piezoelectric ceramics were prepared by solid-state reaction. The influence of Ba contents on phase structures, compositional distribution and electrical properties of (Na_0.5Bi_0.5)_1-xBa_xTiO₃ ceramics were systematically investigated to further understand the nature of phase transition. It was found that the phase structure of (Na_0.5Bi_0.5)_1-xBa_xTiO₃ transforms from rhombohedral to tetragonal symmetry at x = 0.06 ~ 0.07 and Ba²⁺ segregation forms the coexistence of Ba-rich tetragonal and Ba-deficient rhombohedral phases close to MPB. The electrical properties of prepared samples regularly changed with Ba content, which is closely related to the distribution of rhombohedral and tetragonal phases. The prepared sample near MPB exhibited the largest dielectric constant and the excellent piezoelectric properties (the maximal measuring field reached 78 kV/cm and the piezoelectric constant d ₃₃ = 151pC/N).     

Pyroelectric, dielectric, and piezoelectric properties of MnO2-doped (Na0.82 K0.18)0.5Bi0.5TiO3 lead-free ceramics

MnO₂ doped (Na_0.82 K_0.18)_0.5Bi_0.5TiO₃ lead-free piezoelectric ceramics were prepared by conventional solid-state reaction process and the effect of MnO₂ addition on the pyroelectric, piezoelectric and dielectric properties were studied. The experiment results showed that the pyroelectric, piezoelectric, and dielectric properties strongly depended on MnO₂ addition in the (Na_0.82 K_0.18)_0.5Bi_0.5TiO₃ ceramics. Excellent electrical properties were obtained in (Na_0.82 K_0.18)_0.5Bi_0.5TiO₃ with 0.8?mol% MnO₂. The large dielectric loss of pure BNT ceramics was significantly reduced, the piezoelectric constant was improved, and it also showed excellent pyroelectric properties when compared with other lead free ceramics, with pyroelectric coefficient p?=?17?×?10^?4?C/m²K and figure of merit F _d ?=?6.56?×?10^?5?Pa^?0.5. With these outstanding pyroelectric properties, the 0.8?mol% MnO₂ doped (Na_0.82 K_0.18)_0.5Bi_0.5TiO₃ ceramic can be a promising material for pyroelectric sensor applications in future.     

Preparation,characterisation, and electrical properties of (K0.5Na0.5)NbO3 lead-free piezoelectric ceramics

Na_0.5?K_0.5NbO₃ (KNN) ceramics were sintered at different temperatures (970 °C, 1000 °C, 1030 °C, 1060 °C, and 1090 °C) for 3 h by a pressureless sintering method. The powders had been synthesised by sol–gel method, using citric acid as a coordination agent and ethylene glycol as an esterifying agent. The effects of temperature on the phase, microstructure, dielectric, ferroelectric, and piezoelectric properties of the as-prepared ceramics were analysed. The results revealed that all of the ceramics had a pure perovskite phase with orthorhombic symmetry. The piezoelectric constant (d ₃₃), the relative dielectric constant (ε _r), the planar electromechanical coupling coefficient (K _p), and the remnant polarization (P _r) initially increased and then decreased with increasing of temperature in such KNN ceramics. The volatilization of sodium and potassium increased with increasing sintering temperature. Over the range of temperatures studied, those ceramics sintered at 1060 °C had the following optimal properties: (ρ?=?3.97 g/cm³, d ₃₃?=?119 pC/N, ε _r?=?362.46, tan δ?=?0.05, K _p?=?0.23, P _r?=?11.97 μC/cm², E _c?=?10.35 kV/cm, and T _c?=?408 °C).     

Effect of BiAlO3 concentration on the dielectric and piezoelectric properties of lead-free (Bi0.5Na0.5)0.94Ba0.06TiO3 piezoelectric ceramics

In this paper, lead-free (1-x)(Bi_0.5Na_0.5)_0.94Ba_0.06TiO₃-xBiAlO₃ (BNBT-BA, x?=?0, 0.010, 0.015, 0.020, 0.025, and 0.030) piezoelectric ceramics were synthesized using a conventional solid-state reaction method. The effect of BiAlO₃ concentration on dielectric, ferroelectric and piezoelectric properties were investigated. The ferroelectric and piezoelectric properties of BNBT ceramics are significantly influenced by the presence of BA. In the composition range studied, X-ray diffraction revealed a perovskite phase with the coexistence of rhombohedral and tetragonal phases. The temperature dependence of dielectric properties showed that the depolarization temperature (T _d) shifted towards lower temperatures and that the degree of diffuseness of the phase transition around T _d and T _m became more obvious with increasing BiAlO₃ content. The remanent polarization increased with increasing BA, and reached a maximum value of 30 μC/cm² at x?=?0.020. As a result, at x?=?0.020, the piezoelectric constant (d ₃₃) and the electromechanical coupling factor (k _p) of the ceramics attained maximum values of 188 pC/N and 34.4 %, respectively. These results indicate that BNBT-BA ceramics is a promising candidate for lead-free piezoelectric materials.     

Dielectric,ferroelectric and bipolar electric field induced strain properties of MPB composition of NBT-xKNN system

(1-x) (Na_0.5Bi_0.5TiO₃)-xK_0.5Na_0.5NbO₃/NBT-xKNN [x?=?0.07, 0.06, 0.05] ferroelectric ceramics were prepared by solid state synthesis route (SSSR). The effects of KNN contents on the microstructure, dielectric, piezoelectric and ferroelectric properties of the NBT-xKNN system were investigated in detail. For single perovskite phase formation, the calcination temperature was optimized at 800 °C for 6 h. From the XRD study, the morphotropic phase boundary (MPB) was confirmed for x?=?0.07 composition. For better densification, the sintering temperature was optimized for 1150 °C for 4 h. SEM micrographs illustrate the closely packed and non-uniform distribution of grains. Diffusive type of behaviour was observed in all the ceramics. Polarization (P) vs. electric field (E) study confirmed the ferroelectric nature of the NBT-xKNN ceramics. The bipolar field-induced strain measurement for all the ceramic samples showed butterfly-shaped loops indicating their piezoelectric nature. Among all the different compositions in MPB region, high dielectric constant (ε_r) of?~?3011, high remnant polarization (P _r ) of 17.88μC/cm² and high strain % of 0.41, were obtained in NBT-xKNN system with x?=?0.07 confirming the existence of MPB at this composition.     

Lead-free K<Subscript>0.5</Subscript>Na<Subscript>0.5</Subscript>NbO<Subscript>3</Subscript>–Bi<Subscript>0.5</Subscript>Li<Subscript>0.5</Subscript>ZrO<Subscript>3</Subscript>–BiAlO<Subscript>3</Subscript> ternary ceramics: Structure and piezoelectric properties

Lead-free perovskite (0.995–x)(K_0.5Na_0.5)NbO₃–x(Bi_0.5Li_0.5)ZrO₃–0.005BiAlO₃ ternary piezoelectric ceramics were projected and prepared by a conventional solid-state method. A research was conducted on the effects of (Bi_0.5Li_0.5)ZrO₃ content on the structure and piezoelectric properties of the ceramics. By combining the X-ray diffraction patterns with the temperature dependence of dielectric properties, a rhombohedral–orthorhombic–tetragonal phase coexistence was identified for the ceramics with 0.02 ≤ x ≤ 0.025, and a rhombohedral–tetragonal phase boundary was determined in the composition x = 0.03. Upon further increasing the (Bi_0.5Li_0.5)ZrO₃ content, the rhombohedral–tetragonal phase boundary transformed to a single rhombohedral structure with x ≥ 0.035. An obviously improved piezoelectric activity was obtained for the ceramics with compositions in and around the rhombohedral–tetragonal phase boundary, among which the composition x = 0.025 exhibited the maximum values of piezoelectric constant d ₃₃, and planar and thickness electromechanical coupling coefficients (k _p and k _t), of 252 pC/N, 0.366, and 0.466, respectively. In addition, the ceramic with x = 0.025 was found to possess a relatively high Curie temperature of 368 °C, suggesting it may have a prospect for applications at elevated ambient temperatures.     

Lead-free NKN-5LT piezoelectric materials for multilayer ceramic actuator

As a candidate for lead-free piezoelectric materials, Li₂O excess 0.95(Na_0.5K_0.5)NbO₃–0.05LiTaO₃ (NKN-5LT) ceramics were developed by conventional sintering process. Sintering temperature was lowered by adding Li₂O as a sintering aid. Abnormal grain growth in NKN-5LT ceramics was observed with varying Li₂O content. In the 1 mol% Li₂O excess NKN-5LT samples sintered at 1000°C for 4 h in air, electromechanical coupling factor and piezoelectric constant of NKN-5LT ceramics were found to reach the highest values of 0.37 and 250 pC/N, respectively. Lead-free piezoelectric ceramic, Li₂O excess NKN-5LT, multilayer ceramic actuators (MLCA) were fabricated. 10?×?10?×?1 mm³ size MLCAs were fabricated by conventional tape casting method. The displacement of Li₂O excess NKN-5LT MLCA with 3 mm thickness was ~1 μm at 150 V.     

Lead-free Na0.5K0.5NbO3 piezoelectric ceramics fabricated by spark plasma sintering: Annealing effect on electrical properties

Niobate ceramics such as NaNbO₃ and KNbO₃ have been studied as promising Pb-free piezoelectric ceramics, but their sintering densification is fairly difficult. In the present study, highly dense Na_0.5K_0.5NbO₃ ceramics with submicron grains were prepared using SPS, whose density was raised to 4.47 g/cm³ (>99% of the theoretical density) at 920 °C. Reasonably good ferroelectric and piezoelectric properties were obtained in the SPSed Na_0.5K_0.5NbO₃ ceramics after annealing in air. The effect of annealing time on the electrical properties was investigated to determine optimal processing condition. The piezoelectric parameter (d ₃₃) of the Na_0.5K_0.5NbO₃ ceramics annealed properly reached 148 pC/N.     

The effect of Bi4Ti3O12 particles addition in lead-free Bi0.5(Na0.75K0.25)0.5TiO3 ceramics

We studied the effect of Bi₄Ti₃O₁₂ (BiT) platelet addition in Bi_0.5(Na_0.75K_0.25)_0.5TiO₃ (BNKT) ceramics by preparing two kinds of BNKT ceramics. One type of BNKT ceramic was fabricated by a conventional solid state reaction method (normal sample), while the other by addition of 15 wt% BiT platelets to BNKT powders (BiT-added sample). In the case of BiT-added BNKT ceramics, plate like grains were formed by the reaction of BiT platelets with Na₂CO₃, K₂CO₃, and TiO₂ during the sintering process. The grain size of BiT-added BNKT ceramics was 10 times larger than that of normal BNKT ceramic. The piezoelectric strain and d₃₃ values of BiT-added BNKT ceramics were 0.135% and 225 pm/V, respectively. These values were 35% higher than those of normal BNKT ceramics. The piezoelectric properties of BiT-added BNKT ceramics were enhanced by the higher domain activity due to a decrease in domain density at larger grain sizes.     

Dielectric,ferroelectric, and piezoelectric properties of lead-free Ba0.95Ca0.05Ti1-xZrxO3 ceramics

Abstract

Ba_0.95Ca_0.05Ti_1-xZr_xO₃ (BCTZO) ceramics were prepared by a solid state reaction method. The samples were characterized by X-ray diffraction (XRD), Scanning electron microscopy (SEM) and X-ray absorption near edge structure (XANES). The ceramics exhibit a pure perovskite structure. The average grain size gradually decreases with increasing Zr concentration. XANES results indicate that the intensities of pre-edge peaks dropped with increasing Zr concentration. The BCTZO ceramic of x?=?0.05 has the optimum electrical properties with the maximum dielectric constant (ε'_m), remanent polarization (2P_r), coercive electric field (2E_c) and piezoelectric charge constant (d₃₃) of 7,244, 12.54 (μC/cm²), 5.29 (kV/cm) and 288 (pC/N), respectively.     

Dielectric and pyroelectric properties of Li2CO3 doped 0.2Pb(Mg1/3Nb2/3)O3–0.5Pb(Zr0.48Ti0.52)O3–0.3Pb(Fe1/3Nb2/3)O3 ceramics

Relaxor ferroelectric compositions of 0.2Pb(Mg_1/3Nb_2/3)O₃–0.5Pb(Zr_0.48Ti_0.52)O₃–0.3Pb(Fe_1/3Nb_2/3)O₃ (0.2PMN–0.5PZT–0.3PFN) ceramics were doped with different concentrations of Li₂CO₃ and were prepared by a columbite precursor process. Their structural, dielectric and pyroelectric properties were studied. A phase analysis was performed using the X-ray diffraction patterns from 2θ?=?44° to 46°, over which the tetragonal phase displays two peaks, (002)_T and (200)_T, while the rhombohedral phase displays one peak, (200)_R. A well saturated P–E hysteresis loop was obtained for the 0.2PMN–0.5PZT–0.3PFN ceramic doped with 0.2 wt.% Li₂CO₃, and the values for the remnant polarization (P _r) and coercive field (E _c) were 30 μC/cm² and 5.4 kV/cm, respectively. A maximum value of the pyroelectric coefficient, 518 μC/m²K, was obtained for the 0.2PMN–0.5PZT–0.3PFN ceramic doped with 0.3 wt.% Li₂CO₃ at the maximum temperature (T _max) due to the decrease of the binding energy for the polarization charge which in formed at the surface.     

High piezoelectric properties of (Ba,Ca)TiO3-0.04LiF ceramics sintered at a low temperature

Lead-free piezoelectric ceramics are strongly needed to replace the lead-based piezoelectric ceramics with increasing environmental concerns. Barium titanate (BaTiO₃) systems are one of the most promising candidates due to excellent electrical properties. However, the sintering temperature for traditionally sintered BaTiO₃ ceramics are about 1300°C, which restricts the applications of BaTiO₃ ceramics. It is necessary to develop high piezoelectric properties of BaTiO₃ based ceramics which are able to sinter at low temperature. The (Ba_0.94Ca_x)Ti_0.94O_δ-0.04LiF (x?=?0.00?~?0.05 mol) ceramics were synthesized by a conventional sintering method at 1050°C. All the samples show high relative densities over 90%. X-Ray Diffraction pattern indicated that the crystallographic structure of the samples (x?=?0.00 and 0.01 mol) are orthorhombic phase and changes to pseudocubic one with increasing Ca content to x?=?0.03 mol. Two-phases with orthorhombic and pseudocubic symmetries coexisted at x?=?0.02 mol, which contributes the excellent properties, in which the piezoelectric constant d ₃₃?=?361 pC/N, the planar electromechanical coupling coefficient k_p?=?41.2%, the Curie temperature Tc?=?70°C, the temperature of phase transition T _O-PC?=?34°C near the room temperature, the relative permittivity ε _r?=?4028 and the remanent polarization P _r?=?9.39 μC/cm².     

Piezoelectric and ferroelectric properties of new Pb9Ce2Ti12O36 and lead-free Ba2NdTi2Nb3O15 ceramics

In this paper, measurements of the nonlinear ferroelectric, piezoelectric and dielectric properties of Pb₉Ce₂Ti₁₂O₃₆ (Pb₉CTO) and Ba₂NdTi₂Nb₃O₁₅ (BNTN) ferroelectric ceramics are presented. Hysteresis P(E) loops were measured as a function of applied electric field, frequency and temperature. The coercive field (E _c) and remnant polarization (P _r) displayed temperature and frequency dependence. Lead-free BNTN ceramics exhibited a coercive field E _c?>?2.4 kV mm^?1 and a piezoelectric coefficient d ₃₃?=?2 pC N^?1. The hysteresis loop was pinched above 110°C and a linear response was observed at 155°C, typical of a paraelectric material. Pb₉CTO was shown to be ferroelectric with coercive field E _c?=?1.2 kV mm^?1 and a d ₃₃?=?65 pC N^?1. The frequency dependences of the impedance of the Pb₉CTO discs were analyzed.     

Effect of attrition milling on the piezoelectric properties of Bi0.5Na0.5TiO3-based ceramics

Bismith sodium titanate (BNT)-based powders were prepared by conventionally mixed-oxide method using Bi₂O₃, Na₂CO₃ and TiO₂. The La₂O₃ was added as the modifier to the BNT composition for easily poling and reducing an abnormal dielectric loss at high temperatures. In this study, the investigated compositions were Bi_0.5Na_0.5TiO₃ and Bi_0.5Na_0.485La_0.005TiO₃. The powders were calcined at 900 °C for 2 h by slow heating rate at 100 °C/h. The calcined BNT-based powders were then attrition-milled for 3 h with a high speed at 350 rpm. After drying, the fine powders were uniaxially pressed and then cold-isostatically pressed (CIP) at 240 MPa for 10 min. All pressed pellets were sintered at 1000–1100 °C for 2 h in air atmosphere. The microstructure of sintered pellets was investigated by SEM. Results of dielectric and piezoelectric property measurement were also reported.