Piezoelectric properties, densification behavior and microstructural evolution of low temperature sintered PZT ceramics with sintering aids

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Abstract

Pb(Zr0.53Ti0.47)O3 Ceramics can be made densified at as low as 800°C for 2 h by incorporating LiBiO2+CuO as the sintering aids. It exhibits high dielectric constant 1000–1300 and coupling factor 55–60% over a wide temperature range 800–1000°C. The optimal properties were obtained for the ceramics sintered at 880°C for 2 h. The densification behavior was investigated by using nonisothermal techniques. In the densification curve, the three sintering stages were found for Pb(Zr0.53Ti0.47)O3 ceramics with the sintering aids at a certain addition amount. The additives were characterized by TG-DSC. The microstructure development of the ceramics was observed by SEM and compared to that of Pb(Zr0.53Ti0.47)O3 ceramics. XPS was used to analyze the distribution of the additives in sintered ceramics.

Introduction

Pb(Zr,Ti)O3 ceramics (PZT) has been widely applied to various fields because of its excellent piezoelectric properties. But for conventional PZT ceramics, the vaporization of PbO in its composition during sintering is of great significance, which makes it difficult to control microstructure and the electromechanical properties of PZT and also causes the environmental pollution. The low temperature sintering of PZT ceramics can not only solve the problems from the vaporization of PbO, but also reduce the energy consumption and fabrication cost. Thus the study on lowering the sintering temperature of PZT ceramics has aroused more and more attentions from the researchers.

Previous research works have revealed that the sintering temperature of PZT ceramics can be lowered by employing the additives with low melting point.1, 2, 3, 4, 5 In this way, however, it is difficult to keep the piezoelectric properties of the based composition. Therefore, it is generally believed that the employment of a proper additive as a sintering aid is favorable to low temperature sintering of Pb(Zr0.53Ti0.47)O3 ceramics (abbreviated as PZT). In this study, the additives LiBiO2+CuO (abbreviated as LBCu) were employed for facilitating the sintering process of Pb(Zr0.53Ti0.47)O3 ceramics. LBCu were chosen as a sintering aid because of their effects on enhancing the densification of PZT ceramics and improving the piezoelectric properties.6, 7, 8

Section snippets

Experimental

The Pb(Zr0.53Ti0.47)O3 powder was prepared via a conventional mixed-oxide route by using commercially available PbO, TiO2 and ZrO2 of 99.9% purity as starting materials. The calcination was done at 890°C for 2 h. The sintering aid: 1 wt.% LiBiO2+0.06 wt.%CuO was added to calcined PZT powder as a mixture of Li2CO3, Bi2O3 and CuO powders. They are mixed in ethanol for 12 h. Disc specimens were formed at 800 kg/cm2 in a diameter of 22 mm and thickness of 2.5 mm and sintered from 800 to 1000°C for

Results and discussion

Fig. 1 gives the density as a function of sintering temperature for PZT and PZT composition with 1.06 wt.% LiBiO2+CuO added. The initial sintering temperature for the PZT based composite is higher than 1150°C. In contrast to that, the LBCu added PZT powders has attained a high density at 800°C. With a minor addition of LBCu additives, the sintering temperature of PZT powders can be reduced by 350°C.

Fig. 2 shows the SEM micrographs of the surfaces of PZT and LBCu added PZT compositions. An

Conclusion

Low temperature sintering of Pb(Zr0.53Ti0.47)O3 composition has been successfully attempted by using LiBiO2+CuO additives as sintering aids. The densification of LiBiO2+CuO added Pb(Zr0.53Ti0.47)O3 composition occurs at around 600°C through particle rearrangement process due to the formation of a small amount of liquid phase from the melting of the additives. The main densification mechanism at relatively higher temperature is similar to solid-state sintering by volume diffusion. The additives

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    LiBiO2 can melt and form a liquid phase at approximately 700 °C [19]. The combination of CuO and LiBiO2 can further reduce the liquid formation temperature to approximately 600 °C [12,19]. However, the limited literature available on this subject has reported that the sintering temperature of PSbN-PZT piezoceramics can be reduced to approximately 1050 °C [20], which still cannot fully meet the requirement for low temperature (i.e., less than 950 °C) co-fired multilayer piezoactuators.

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