IntroductionLead zirconate titanate (PZT) ceramics have been widely studied due to their very high electromechanical coupling coefficient. As a result, they have been employed in many applications such as hydrophones, ignitors, fine movement controllers, etc. [1,2]. Earlier studies revealed that the PZT properties are affected by their microstructures which partly depend on size and homogeneity of the starting powders [3,4,5]. Generally, conventional methods using ball milling of the constituent oxides have had difficulty in controlling the powder size, particle size distribution, and homogeneity of the PZT powders [6]. However, fine homogeneous PZT particles can be obtained via chemical processes [7,8,9,10]. Ceramics produced from these powders often yield encouraging piezoelectric and dielectric properties. The PZT ceramics produced via chemical processes usually require a very high purity (> 99.9 %) and high cost chemicals, which are not appropriate for large scale production. The spray-drying technique is of particular interest because quality powders may be produced in large quantity. Lal et al. and Uematsu et al. revealed that fine and very homogeneous particles of strontium-doped PZT and silicon nitride (Si 2 N 4 ), respectively, could be produced via this technique [11,12]. Both of them used the reagent grade of high cost chemicals as starting materials. However, the problem arises that the powders produced via the spray-drying technique in which the starting chemical was of reasonably lower purity (<99.9 wt%) often yielded unexpected secondary phase particles. In this work, attempts have been made to develop a modified chemical method via the spray-drying technique followed by a calcining process using low purity grade (< 99 wt %) and comparatively low priced chemicals to produce PZT powders, which have comparable properties with those produced via the previously described processes. The pH of the mixed nitrate solution of the constituents was carefully controlled and the spray drying process was carried out. The characteristics of the spray-dried PZT powders were investigated. The piezoelectricity, dielectricity, and densities of the corresponding ceramics were also studied.
ExperimentalThe low-priced chemicals used in this work are solutions of lead nitrate (Pb(NO 3 ) 2 , 99 % by weight), zirconyl nitrate hydrate (ZrO(NO 3 ) 2 .6H 2 O, ~27 % of Zr by weight), and tetraisopropyl orthotitanate (C 12 H 28 O 4 Ti, ~99 % by weight). The molar ratio of these solutions were kept at 1:0.52:0.48 which corresponds to the crystal phase of Pb(Zr 0.52 Ti 0.48 )O 3 . By following the work done by Tunkasiri, the aqueous solutions of Pb(NO 3 ) 2 and (ZrO(NO 3 ) 2 .6H 2 O were mixed first [7]. Then a mixture of C 12 H 28 O 4 Ti solution and a strong nitric acid (HNO 3 , pH ~ 1) was gradually added to the solution. In order to stabilize the metals in the solution, hydrogen peroxide (H 2 O 2 ) was added. An aqueous ammonium solution was then slowly added to control the pH of the mixture solution. In order to obtain manga...