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Electrical Properties of Low Temperature

Sintered PiezoceramicsTingting Wang

a, Feifei An

a& Jian Yu

a

aFunctional Materials Research Laboratory, Tongji University,

Shanghai, 200092, China

Version of record first published: 01 Dec 2010.

To cite this article: Tingting Wang , Feifei An & Jian Yu (2010): Electrical Properties of LowTemperature Sintered Piezoceramics, Ferroelectrics, 408:1, 98-102

To link to this article: http://dx.doi.org/10.1080/00150193.2010.485540

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Ferroelectrics , 408:98102, 2010

Copyright Taylor & Francis Group, LLCISSN: 0015-0193 print / 1563-5112 online

DOI: 10.1080/00150193.2010.485540

Electrical Properties of Low TemperatureSintered Piezoceramics

TINGTING WANG, FEIFEI AN, AND JIAN YU

Functional Materials Research Laboratory, Tongji University,

Shanghai 200092, China

In general, commercial PZT piezoceramics are sintered at temperature above 1200C.

Here, one low-temperature sintering technology was developed for PZT piezoceram-ics by adding perovskite-type ferroelectrics with low sintering temperature, alterna-tive to adding non-piezoelectric low-melting glass or eutectic oxides. Through solid

state reaction mechanism, very densified piezoceramics of (Pb0.95Sr0.05)(Zr0.53Ti0.47)O3with 0.6PbTiO30.3Bi(Zn0.5Ti0.5)O30.1BiFeO3 as sintering additive were obtained be-low 1050C. The phase of (Pb,Bi,Sr)(Zr,Ti,Zn,Fe)O3 solid solution piezoceramics wasdemonstrated to be single-phased perovskite structure and the measurements of dielec-tric, ferroelectric and piezoelectric properties showed good piezoelectric performanceequivalent to PZT-8.

I. Introduction

Driven by low driving electric force and large output displacements, multilayer-stackedtransducers have been becoming dominant in the market. Till now, high-temperature sin-

tering technology above 1200C with expensive high-melting point W/Mo inner electrode

and low-temperature sintering technology below 950C with Ag inner electrode have been

developed. Owing to high sintering temperature, the former method accompanies with

volatility of lead content, increased energy consumption and high fabrication costs. By us-

ing the additive of non-piezoelectric low-melting point glass or eutectic oxides, which occur

usually at grain boundaries after sintering process to deteriorate transducer performances,

the latter method remains to maximize piezoelectric performances [13].

In this paper, one sintering technology with low-sintering temperature ferroelectric of

0.6PbTiO30.3Bi(Zn0.5Ti0.5)O30.1BiFeO3 (labeled as PT-BZT-BF) as sintering additive

for PZT piezoceramics was developed [4]. The (Pb,Bi,Sr)(Zr,Ti,Zn,Fe)O3 (labeled as PZT-LTF) piezoceramics were prepared using modified conventional solid state reaction method,

their phase structure, microstructure and piezoelectric properties were presented.

II. Experimental Procedure

The perovskite-type PZT-LTF piezoceramic samples were synthesized with conventional

electronic ceramic processing. Firstly, the oxides of PbO, ZrO2, TiO2, SrCO3 and MnO2

Received August 23, 2009; in final form September 23, 2009.Corresponding author. Tel: +86-21-65980544-103; Fax: +86-21-65985179. E-mail: jyu@tongji.edu.cn

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were weighted in accordance with the chemical formula of (Pb0.95Sr0.05)(Zr0.53Ti0.47)O3 +

0.5wt% MnO2 (labeled as PSZT), ground with ethanol and calcined at 800C for 5 h. Then,

the oxides of PbO, TiO2, Bi2O3, ZnO and Fe2O3 were weighted and mixed in accordance

with the formula of PT-BZT-BF. At last, the PZT-LTF ceramics were prepared by mixing

the calcined PSZT powder and 9wt% PT-BZT-BF. The green pellets of 10 mm diameter

were compacted under 250 MPa, and sintered at temperature between 990 and 1050C for

5 h. For electrical characterization, the ceramic pellets were polished, coated with silver

paste and fired at 600C for 10 min. The processing was described in detail elsewhere [4].

The phase structure and microstructure of those sintered ceramics were analyzed

using an X-ray diffractometer (D8, Bruker, Germany) and a scanning electron microscopy

(JSM EMP-800, Japan), respectively. Their dielectric properties were investigated with HP

4194A impedance analyzer under oscillation voltage of 1.0 V. The polarization-electric field

hysteresis loops were measured with ferroelectric materials analyzer (Radiant, Precision

Premier II, USA). For piezoelectric measurements, the samples were poled in a silicone

oil bath at 150C by applying a DC electric field of 3kV/mm for 15 min. The piezoelectric

constant d33 was measured using a quasi-static piezoelectric d33 meter (Model ZJ-3d,Institute of Acoustics, Chinese Academy of Science).

III. Results and Discussion

For the perovskite-type PT-BZT-BF ferroelectrics is in the tetragonal structure with tetrag-

onality of c/a = 1.105 [5] but PSZT is rhombohedral near the morphotropic phase boundary

at room temperature, it is reasonable to expect the solid solution of PSZT and PT-BZT-BF

in the tetragonal phase. For the PZT-LTF pellets sintered at temperature between 990 and

1050C, the characterization of X-ray diffraction indicated that they are well crystallized

in the tetragonal phase. As an illustration, Fig. 1 showed the pattern for the sample sin-

tered at 1050C for 5 h, of which the tetragonal phase is demonstrated by the splitting of

the (001)/(100) and (002)/(200) peaks. Contemporarily, the microstructure of the fracture

surface observed by scanning electron microscopy was presented in the Fig. 2 for the same

Figure 1. XRD pattern of PZT-LTF pellet sintered at 1050C for 5 h.

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Figure 2. SEM microstructure picture of the fracture surface for the same sample as Fig. 1.

sample as in the Fig. 1. It was seen that the very densified pellet was obtained here at lower

sintering temperature more 150C than the conventional PZT ceramic processing.

In the Fig. 3, the dielectric constant and loss as a function of frequency were presented

for the poled PZT-LTF pellets sintered at temperature between 990 and 1050C. The room

temperature dielectric constant at 1kHz increases with increasing sintering temperature,

= 760 and tan = 0.7% was obtained for the sample sintered at 1050C. Moreover, the

measurement of temperature-dependent dielectric constant indicated the ferroelectric- para-

electric Curie temperature Tc = 298C. In comparison with (Pb0.95Sr0.05)(Zr0.53Ti0.47)O3piezoceramics of = 1002 [6], the reduced dielectric constant of the PZT-LTF ceramics

may result from both the effects of the Mn addition, which usually makes PZT become hard,

and the PT-BZT-BF component with low dielectric constant of 170. On the other hand, the

Figure 3. Frequency-dependent dielectric constant and loss of PZT-LTF ceramics sintered at tem-

perature between 990 and 1050C for 5 h.

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Figure 4. Polarization-electric field hysteresis loops recorded at room temperature for the same

samples as Fig. 3.

Curie temperature of the PZT-LTF ceramics is lower than Tc = 360C of the PSZT and

Tc = 700C of PT-BZT-BF components, which is similar to the case of PZT-BiFeO 3 solid

solution [7].

For the samples sintered between 990 and 1050C, ferroelectric properties were mea-

sured and the obtained Polarization-Electric field hysteresis loops were presented in the

Fig. 4. With increasing sintering temperature, the crystallization of PZT-LTF piezoceram-ics was enhanced and a high permanent polarization Pr of 10.8 C/cm2 and coercive field

Ec of 2.11kV/mm was obtained for the sample sintered at 1050C. Similar to ferroelectric

properties, a high piezoelectric coefficient d33 was also observed as 241pC/N for the sample

sintered at 1050C. So far, it can be seen that the piezoelectric performance of PZT-LTF

ceramics is equivalent to that of commercial PZT-8 with = 1000, d33 = 225pC/N, and

Tc = 300C [8].

IV. Conclusions

One novel low-temperature sintering technology for PZT piezoceramics below 1050C

was developed and demonstrated with the perovskite-type PSZT-PT-BZT-BF solid solution

system. For the PZT-LTF piezoceramics sintered at 1050C, a better piezoelectric perfor-

mance with = 760, tan = 0.7%, d33 = 241pC/N, and Tc = 298C was obtained, which

is equivalent to PZT-8, and can be applied for manufacturing multilayer transducers with

Ag/Pd inner electrode.

Acknowledgments

This work was partially supported by NSFC Grant 50875181, FANEDD-200744, Shanghai

Pujiang Program-07pj14087 and NCET-07-0624.

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102/[1864] Tingting Wang et al.

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