Characterization of phase transitions on PbZrxTi(1-x)O3 nanocrystal ceramic materials synthesized using the molten salt method
DOI:
https://doi.org/10.11113/mjfas.v15n6.1413Keywords:
Molten Salt Method, Morphotropic Phase Boundary (MPB)Abstract
One of the piezoelectric materials is PbZrxTi(1-x)O3 (Lead Zirconate Titanate, namely PZT) which has the highest piezoelectric properties and is widely applied today. To improve the performance of materials, it is important to enhance the quality of materials, especially in the synthesis process. In this study, molten salt method was employed to synthesis PZT by using salt solution (NaCl and KCl) in accommodating the reaction of raw materials (Pb, ZrO2, and TiO2). The synthesized particles of PZT nanocrystal ceramics have been successfully carried out at the sintering temperature of 875 ℃ for 4 hours. The separations of NaCl and KCl salt to obtain PZT products have been carried out by washing repeatedly with hot water at about 100 ℃. PbZrxTi(1-x)O3 samples with variations of x = 0.30, 0.42, 0.52, 0.58, and 0.70 mol were characterized using X-Ray Diffractometer and followed by analyzing crystal structures using highscore software through refinement process. One of the X-ray diffraction profiles at the angle (2q) between 42.5 and 47o has indicated the phase transition from one peak (representing the rhombohedral crystal system with the plane (202)) to the two peaks (tetragonal with plane (002) and (200)). Regarding this phase transition, the morphotropic phase boundary (MPB) region (rhombohedral and tetragonal phase boundary region) has been successfully obtained at the composition x = 0.52 mol which was identical to the PbZr0.52Ti0.48O3 compound. The largest particle size of crystallites for each rhombohedral and tetragonal phase is approximately equal to 906.117 Å obtained at the composition x = 0.52 mol. The content of the rhombohedral phase decreases, while the content of the tetragonal phase increases if the value of x increases.
References
S. Zhang, R. Xia, T. R. Shrout, "Lead-free piezoelectric ceramics vs. PZT?," J. Electroceram., vol. 19, no. 4, pp. 251 - 257, 2007.
K. Nagata, J. Thongrueng, “Effect of temperature, humidity and load on degradation of multilayer ceramic actuator,” J. Korean Phys. Soc., vol. 32, pp. S1278–S1281, 1998.
L. Medvecky, M. Kmecová, K. Saksl, “Study of Pb (Zr0.53Ti0.47) O3 solid solution formation by interaction of Perovskite phases,” J. Eur. Ceram. Soc., vol. 27, no. 4, pp. 2031–2037, 2007.
C. A. Randall, N. Kim, J.-P. Kucera, W. Cao, T. R. Shrout, “Intrinsic and extrinsic size effects in fine-grained morphotropic-phase-boundary lead zirconate titanate ceramics,” J. Am. Chem. Soc., vol. 81, no. 3, pp. 677–688, 1998.
S. Ahda, S. Misfadhila, T. Y. S. P. Putra, P. Parikin, “Molten salt synthesis and structural characterization of BaTiO3 nanocrystal ceramics,” IOP Conf. Ser. Mater. Sci. Eng., vol. 176, 2017.
J. T. Zeng, K. W. Kwok, H. L. W. Chan, “KxNa1 − xNbO3 powder synthesized by molten-salt process,” Mater. Lett., vol. 61, no. 2, pp. 409–411, 2007.
Y. Haibo, Y. Lin, F. Wang, H. Luo, “Chemical synthesis of K0.5Na0.5NbO3 ceramics and their electrical properties,” Mater. Manuf. Process., vol. 23, no. 5, pp. 489–493, 2008.
N. Sharma, A. Gaur, U. Gaur, “Multiferroic behavior of nanocrystalline BaTiO3 sintered at different temperatures,” Ceram. Int., vol. 40, no. 10 Part B, pp. 16441–16448, 2014.
F. Zhang, L. Han, S. Bai, T. Sun, T. Karaki, M. Adachi, “Hydrothermal synthesis of (K,Na)NbO3 particles’,” Jpn. J. Appl. Phys., vol. 47, no. 9, pp. 7685–7688, 2008.
H. K. Yoon, Y. S. Cho, D. H. Kang, “Molten salt synthesis of lead based relaxors,” J. Mater. Sci., vol. 33, no. 12, pp. 2977–2984, 1998.
J. Joseph, T. Vimala, V. Sivasubramanian, V. Murthy, “Structural investigations on Pb (ZrxT1− x) O3 solid solutions using the X-ray Rietveld method,” J. Mater. Sci., vol. 35, no. 6, pp. 1571–1575, 2000.
H. Yokota, N. Zhang, A. E. Taylor, P. A. Thomas, A. M. Glazer, “Crystal structure of the rhombohedral phase of PbZr 1 − x Ti x O 3 ceramics at room temperature,” Phys. Rev. B, vol. 80, pp. 104109, 2009.
A. Chauhan, P. Chauhan, "Powder XRD technique and its applications in science and technology," J Anal Bioanal Tech vol. 5, no. 5, 2014.
O. Namsar, A. Watcharapasorn, S. Jiansirisomboon, “Fabrication and characterization of PZT/nano-sized Si3N4 ceramics,” J. Microsc. Soc. Thail., vol. 23, no 1, pp. 103–106, 2009.
C. T. Kniess, J. C. de Lima, P. B. Prates, The quantification of crystalline phases in materials: Applications of Rietveld method, sintering - Methods and products, Volodymyr Shatokha (Ed.), IntechOpen. 2012.
N. Sahu, S. Panigrahi, “Mathematical aspects of Rietveld refinement and crystal structure studies on PbTiO3 ceramics,” vol. 34, no. 7, pp. 1495–1500, 2011.
A. S. Karapuzha, N. K. James, H. Khanbareh, S. van der Zwaag, W. A. Groen, “Structure, dielectric and piezoelectric properties of donor doped PZT ceramics across the phase diagram,” J. Ferroelectr., vol. 504, no. 1, pp. 160–171, 2016.
Y. T. Prabhu, K. V. Rao, V. S. S. Kumar, B. S. Kumari, “X-ray analysis by Williamson-Hall and size-strain plot methods of ZnO nanoparticles with fuel variation,” World J. Nano Sci. Eng., vol. 04, no. 1, pp. 21–28, 2014.
C. Suryanarayana, M. G. Norton, X-ray diffraction: A practical approach. New York: Springer, 1998.
E. Sukirman, Y. Sarwanto, “X-rays diffraction study on the iron nanopartcles prepared by two step milling method,” J. Sains Mater. Indones., vol. 15, no. 2, p. 67, 2014.
