Structure, Microstructure, and Dielectric Properties of Bi_0.5(Na_0.78K_0.22)_0.5TiO₃ Lead-Free Ceramic

Abstract:

In this article, the structural, microstructural, and dielectric properties of Lead- free perovskite ceramic Bi_0.5(Na_0.78K_0.22)_0.5TiO₃ [BNKT] have been reported. The material was synthesized through the solid-state reaction method. The compound formed is found to have a hexagonal structure, confirmed by XRD analysis of the sample. The microstructural analysis of the compound revealed the polycrystalline nature of the ceramic having quasi-cubic grain morphology with distinct grain boundaries. From the dielectric study, it was found that the dielectric constant increases with temperature and attained maximum value at temperature T_c = 335° C, after which it decreased. The frequency independence of transition temperature (T_c) suggested the classic ferroelectric behaviour of the compound. The broad dielectric peak around transition temperature confirms the relaxor behaviour of the compound as well as diffused phase transition at T_c. The value of the relative permittivity and loss tangent at ambient temperature for 1kHz frequency is 627 and 0.223 respectively. The synthesized material can be utilized for the fabrication of capacitors and energy storage applications.

• Periodical: Materials Science Forum (Volume 1097)
• Pages: 91-97
• DOI: https://doi.org/10.4028/p-ZT2gQo
• Online since: September 2023
• Authors: Rahul K. Singh, Mrityunjay Kumar, Sumit K. Roy*
• Keywords: Capacitor, Ferroelectric, Hexagonal, Perovskite, Polycrystalline, Quasi-Cubic, Relaxor

References

[1] B. Jaffe, W.R. Cook, H. Jaffe, Piezoelectric Ceramics, Academic, New York, 1971.

[2] Roy, S.K., Singh, S.N., Mukherjee, S.K., & Prasad, K. (2017). Ba0.06(Na1/2Bi1/2)0.94TiO3–Ba(Fe1/2Ta1/2)O3: giant permittivity lead-free ceramics. Journal of Materials Science: Materials in Electronics, 28, 4763-4771.

DOI: 10.1007/s10854-016-6121-x

[3] Roy, S.K., Chaudhuri, S., Kotnala, R. K., Singh, D. K., Singh, B. P., Singh, S. N., ... & Prasad, K. (2016). Dielectric and Raman studies of Ba0. 06(Na1/2Bi1/2)0.94TiO3-NaNbO3 ceramics. Materials Science-Poland, 34(2), 437-445.

DOI: 10.1515/msp-2016-0041

[4] Roy, S. K., Singh, S. N., Mukherjee, S. K., & Prasad, K. (2019). Structure and dielectric studies of (1-x)Ba0.06(Na0.5Bi0.5)0.94TiO3-xBa(Fe0.5Nb0.5)O3 lead-free ceramics. Processing and Application of Ceramics, 13(4), 418-426.

DOI: 10.2298/pac1904418r

[5] Behera, D., & Mukherjee, S. K. (2023). First-principles calculations to investigate structural, optoelectronics, and thermoelectric properties of lead free Cs2GeSnX6 (X= Cl, Br). Materials Science and Engineering: B, 292, 116421.

DOI: 10.1016/j.mseb.2023.116421

[6] Behera, D., & Mukherjee, S. K. (2022). Theoretical Investigation of the Lead-Free K2InBiX6 (X= Cl, Br) Double Perovskite Compounds Using Ab Initio Calculation. JETP Letters, 116(8), 537-546.

DOI: 10.1134/s0021364022601944

[7] G.A. Smolenskii, V.A. Isupov, A.I. Agranovskaya, N.N. Krainik, New ferroelectrics of complex composition IV, Sov. Phys. Solid State 2 (1961) 2651.

[8] G. O. Jones and P. A. Thomas, "Investigation of the structure and phase transitions in the novel A-site substituted distorted perovskite compound Na0.5Bi0.5TiO3," Acta Crystallographica B, vol. 58, p.168–178, 2002.

[9] P. Woodward, "Octahedral tilting in perovskites. I. Geometrical considerations," Acta Crystallographica B, vol. 53, p.32–43, 1997.

[10] R. Dittmer, W. Jo, J. Roedel, et al., Nanoscale insight into lead-free BNT-BT-xKNN, Adv. Funct. Mater. 22 (2012) 4208–4215.

DOI: 10.1002/adfm.201200592

[11] X.Y. Kang, et al., BNT-based multi-layer ceramic actuator with enhanced temperature stability, J. Alloys Compd. 771 (2019) 541–546.

DOI: 10.1016/j.jallcom.2018.08.311

[12] S. Pattipaka, A.R. James, P. Dobbidi, Enhanced dielectric and piezoelectric properties of BNT-KNNG piezoelectric ceramics, J. Alloys Compd. 765 (2019) 1195–1208.

DOI: 10.1016/j.jallcom.2018.06.138

[13] G. A. Smolenskii and A. I. Agranovskaya, "Dielectric polarization of a series of compounds of complex composition," Fizika Tverdogo Tela, vol. 1, p.1562–1572, 1959.

[14] O. N. Razumovskaya, T. B. Kuleshova, and L. M. Rudkovskaya, "Reactions of formation of BiFeO3, K0.5Bi0.5TiO3, and Na0.5Bi0.5TiO3," Neorganicheskie Materialy [Inorganic Materials], vol. 19, p.113–115, 1983.

[15] G. A. Smolensky, V. A. Isupov, A. I. Agranovskaya, and N. N. Krainic, "New ferroelectrics with complex compounds. IV," Fizika Tverdogo Tela, vol. 2, p.2982–2985, 1960.

[16] G. A. Smolenskii and A. I. Agranovskaya, "Dielectric polarization of a series of compounds of complex composition," Fizika Tverdogo Tela, vol. 1, p.1562–1572, 1959.

[17] C. F. Buhrer, "Some properties of bismuth perovskites," The Journal of Chemical Physics, vol. 36, p.798–803, 1962.

DOI: 10.1063/1.1732613

[18] I. P. Pronin, N. N. Parfenova, N. V. Zaitseva, V. A. Isupov, and G. A. Smolenskii, "Phase transitions in solid solutions of sodium bismuth and potassium bismuth titanates," Fizika Tverdogo Tela, vol. 24, p.1060–1062, 1982.

[19] A. Sasaki, T. Chiba, Y. Mamiya, and E. Otsuki, "Dielectric and piezoelectric properties of (Bi0.5Na0.5)TiO3–(Bi0.5K0.5)TiO3 systems," Japanese Journal of Applied Physics, vol. 38, no. 9, p.5564, 1999.

[20] Jones, G. O., Kreisel, J., & Thomas, P. A. (2002). A structural study of the (Na1-xKx)0.5Bi0. 5TiO3 perovskite series as a function of substitution (x) and temperature. Powder diffraction, 17(4), 301-319.

[21] Zidani, J., Zannen, M., Hadouchi, M., Alzahrani, H. A., Birks, E., Khemakhem, H., ... & Lahmar, A. (2023). Structural, electrical, and optical properties of lanthanide-doped Na0· 4K0.1Bi0.5TiO3 ceramics. Physica B: Condensed Matter, 653, 414680.

DOI: 10.1016/j.physb.2023.414680

[22] Simões, A. Z., Cavalcante, L. S., Moura, F., Longo, E., & Varela, J. A. (2011). Structure, ferroelectric/magnetoelectric properties, and leakage current density of (Bi0. 85Nd0. 15)FeO3 thin films. Journal of alloys and compounds, 509(17), 5326-5335.

DOI: 10.1016/j.jallcom.2011.02.030

[23] Parija, B., Rout, S. K., Cavalcante, L. S., Simoes, A. Z., Panigrahi, S., Longo, E., & Batista, N. C. (2012). Structure, microstructure, and dielectric properties of 100-x([Bi. sub. 0.5][Na. sub.0.5])Ti[O. sub.3]-x[SrTi[O.sub.3]] composites. Appl Phys A, 109, 715-723.

DOI: 10.1007/s00339-012-7105-1

[24] Momma, K., & Izumi, F. (2011). VESTA 3 for three-dimensional visualization of crystal, volumetric, and morphology data. Journal of applied crystallography, 44(6), 1272-1276.

DOI: 10.1107/s0021889811038970

[25] Siroha, P., Singh, D., Soni, R., & Gangwar, J. (2018, August). Comparative study on the crystallographic representation of transition metal oxide polymorphs nanomaterials using VESTA software: A case study on Fe2O3 and TiO2. In AIP Conference Proceedings (Vol. 2006, No. 1, p.030038). AIP Publishing LLC.

DOI: 10.1063/1.5051294

[26] Parija, B., Badapanda, T., Rout, S. K., Cavalcante, L. S., Panigrahi, S., Longo, E., ... & Sinha, T. P. (2013). Morphotropic phase boundary and electrical properties of 1− x[Bi0. 5Na0. 5]TiO3–xBa[Zr0. 25Ti0. 75]O3 lead-free piezoelectric ceramics. Ceramics International, 39(5), 4877-4886.

DOI: 10.1016/j.ceramint.2012.11.080

[27] http://en.wikipedia.org/wiki/Cuboctahedron

[28] Zhang, Y., Tian, Y., Zhang, Z., Jia, Y., Zhang, B., Jiang, M., ... & Ren, Z. (2022). Magnetic properties and giant cryogenic magnetocaloric effect in B-site ordered antiferromagnetic Gd2MgTiO6 double perovskite oxide. Acta Materialia, 226, 117669.

DOI: 10.1016/j.actamat.2022.117669

[29] Rayssi, C., Kossi, S.E., Dhahri, J., & Khirouni, K. (2018). Frequency and temperature-dependence of dielectric permittivity and electric modulus studies of the solid solution Ca 0.85 Er0.1Ti1− xCo4x/3O3 (0≤ x≤ 0.1). RSC Advances, 8(31), 17139-17150.

DOI: 10.1039/c8ra00794b

[30] Tran, V.D.N., Ullah, A., Dinh, T.H., & Lee, J. S. (2016). Effect of Ba Substitution on Dielectric and Piezoelectric Properties of Lead-Free Bi1/2(Na0.82K0.18)1/2TiO3 Ceramics. Journal of Nanoscience and Nanotechnology, 16(8), 8025-8029.

DOI: 10.1166/jnn.2016.12752

[31] Srivastava, A., Singh, A.K., Srivastava, O.N., Tewari, H.S., Masood, K.B., & Singh, J. (2020). Magnetic and dielectric properties of La and Ni Co-substituted BiFeO3 nanoceramics. Frontiers in Physics, 8, 282.

DOI: 10.3389/fphy.2020.00282

[32] Barick, B.K., Mishra, K.K., Arora, A.K., Choudhary, R.N.P., & Pradhan, D.K. (2011). Impedance and Raman spectroscopic studies of (Na0. 5Bi0. 5)TiO3. Journal of Physics D: Applied Physics, 44(35), 355402.

DOI: 10.1088/0022-3727/44/35/355402

[33] Arya, B. B., & Choudhary, R. N. P. (2021). Studies of structural and electrical characteristics of multi-substituted (Bi0.5Na0.5)TiO3 ferroelectric ceramics. Journal of Materials Science: Materials in Electronics, 32, 11547-11567.

DOI: 10.1007/s10854-021-05743-7

[34] Li, Y. M., Chen, W., Xu, Q., Zhou, J., Sun, H. J., & Liao, M. S. (2005). Dielectric and Piezoelectric Properties of Na0.5Bi0.5TiO3-K0.5Bi0.5TiO3-NaNbO3 Lead-Free Ceramics. Journal of Electroceramics, 14, 53-58.

DOI: 10.1016/j.ceramint.2020.06.187

[35] Das, R., & Choudhary, R.N.P. (2019). Structure, dielectric and electrical properties of relaxor lead-free double perovskite: Nd2NiMnO6. Processing and Application of Ceramics, 13(1), 1-11.

DOI: 10.2298/pac1901001d

[36] Singh, A., Prasad, K., & Prasad, A. (2015). Effects of Sr2+ doping on the electrical properties of (Bi0. 5Na0. 5)0.94Ba0.06TiO3 ceramics. Processing and Application of Ceramics, 9(1), 33-42.

DOI: 10.2298/pac1501033s

[37] Tahri, T., Hamdaoui, N., Omri, A., Hcini, S., Beji, L., Dhahri, E., & Es-Souni, M. (2016). Study of electrical and dielectric properties of CaMn0.6 Fe0.4O2.8 perovskite. Journal of Materials Science: Materials in Electronics, 27, 10525-10531.

DOI: 10.1007/s10854-016-5143-8