INFLUENCE OF MIXING AND THERMAL PARAMETERS ON THE STRUCTURAL HOMOGENEITY AND DIELECTRIC PERFORMANCE OF NBT CERAMICS
DOI:
https://doi.org/10.11113/jurnalteknologi.v88.24729Keywords:
Sodium Bismuth Titanate (NBT), Solid state reaction method, structural, dielectric propertiesAbstract
Sodium Bismuth Titanate (Na₀.₅Bi₀.₅TiO₃, NBT) is a promising lead-free ferroelectric materials, but the role of processing parameters on its structural and dielectric performance is not well understood. This study investigates the impact of four different mixing methods: no ball milling, mixing and milling, moderate mixing and milling, and short-intensity mixing, on the properties of NBT ceramics synthesized by solid-state reaction and sintered at 1150 °C. The results show that enhanced mixing improves phase purity and structural uniformity. Notably, short-intensity mixing yields ceramics with sharp X-ray diffraction peaks of the rhombohedral R3c phase and high relative densities (73 - 91%). These features are associated with excellent dielectric properties, including high permittivity (2000 - 6000 at 1 kHz, 300 °C) and a stable Curie temperature (320 °C). This study highlights the importance of mixing conditions in optimizing the structure–property relationship of NBT ceramics and offers practical guidelines for processing high-performance lead-free ferroelectric devices.
References
Aissa, M., M. A. Slimani, A. Dhahri, M. Rasheed, Z. Raddaoui, S. E. Kossi, et al. 2022. Multifunctionality of Rare Earth Doped 0.925 Na0.5Bi0.5TiO3–0.075 K0.5Na0.5NbO3 Ferroelectric Ceramics. Journal of Alloys and Compounds. 921: 166188.
Ancy, G. C., L. Venkidu, P. M. P. Dharsini, D. Dayanithi, N. V. Giridharan, and B. Sundarakannan. 2023. Temperature-Dependent Energy Storage Performance of the Ceramics in MPB Region Identified from the (1−(x+y))(Bi0.5Na0.5)TiO3-xBaTiO3-yBaZrO3 Ternary Ceramics. Journal of Materials Science: Materials in Electronics. 34(17): 1373. https://doi.org/10.1007/s10854-023-10799-8.
Azlan, U. A. A., W. Krengvirat, A. F. M. Noor, K. A. Razak, and S. Sreekantan. 2012. Sintering and Characterization of Rare Earth Doped Bismuth Titanate Ceramics Prepared by Soft Combustion Synthesis. In Sintering of Ceramics—New Emerging Techniques. Winchester. InTech.
Benyoussef, M., M. Zannen, C. Bouzidi, K. Taibi, H. Belmabrouk, S. Alaya, and J. Dhahri. 2021. Structural, Dielectric, and Ferroelectric Properties of Na0.5(Bi1-xNdx)0.5TiO3 Ceramics for Energy Storage and Electrocaloric Applications. Ceramics International. 47(18): 26539–51.
Benyoussef, M., M. Zannen, C. Bouzidi, K. Taibi, H. Belmabrouk, S. Alaya, and J. Dhahri. 2018. Dielectric, Ferroelectric, and Energy Storage Properties in Dysprosium Doped Sodium Bismuth Titanate Ceramics. Ceramics International. 44(16): 19451–60. https://doi.org/10.1016/j.ceramint.2018.07.182.
Bi, N., W. G. Wang, X. Y. Li, T. Liu, and G. L. Hao. 2018. The Effect of Dual Substitution of Na and Al on Ionic Conductivity. Results in Physics. 11: 422–26. https://doi.org/10.1016/j.rinp.2018.09.028.
Bikse, L., E. Platacis, M. Antonova, A. Sternberg, and A. Kalvane. 2021. Impact of Thermal Treatment on the Surface of Na0.5Bi0.5TiO3-Based Ceramics. Crystals. 11(10): 1266. https://doi.org/10.3390/cryst11101266.
Cui, C., Y. Wang, B. Li, L. Zhang, H. Du, D. Zhou, et al. 2017. Structure, Dielectric and Relaxor Properties in Lead-Free ST-NBT Ceramics for High Energy Storage Applications. Journal of Alloys and Compounds. 711: 319–26.
Dawson, J. A., H. Chen, and I. Tanaka. 2015. Crystal Structure, Defect Chemistry and Oxygen Ion Transport of the Ferroelectric Perovskite, Na0.5Bi0.5TiO3: Insights from First-Principles Calculations. Journal of Materials Chemistry A. 3(32): 16574–82. https://doi.org/10.1039/C5TA03705K.
Diaz, J. C. C. A., J.-C. M’peko, M. Venet, and P. S. da Silva. 2020. Unveiling the High-Temperature Dielectric Response of Bi0.5Na0.5TiO3. Scientific Reports. 10(1): 19491.
Fancher, C. M., S. Brewer, C. C. Chung, S. Röhrig, T. Rojac, G. Esteves, et al. 2017. The Contribution of 180° Domain Wall Motion to Dielectric Properties Quantified from In Situ X-Ray Diffraction. Acta Materialia. 126: 36–43. https://doi.org/10.1016/j.actamat.2016.12.037.
França, E., P. Romanholo, S. Simões, E. Falcão, A. Franco Jr., and F. Machado. 2021. Enhancing the Electrical Properties of NBT Ceramics by the Addition of Small Amounts of Yb. Journal of Alloys and Compounds. 873: 159845.
Feng, W., B. Luo, S. Bian, E. Tian, Z. Zhang, A. Kursumovic, J. L. MacManus-Driscoll, X. Wang, and L. Li. 2022. Heterostrain-Enabled Ultrahigh Electrostrain in Lead-Free Piezoelectric. Nature Communications. 13(1): 5086.
Goutham, C., S. Raavi, and S. Asthana. 2019. Particle Size Dependent Properties of Na0.5Bi0.5TiO3 Synthesized Using Hydrothermal Technique. https://doi.org/10.1063/1.5093828.
Jayasri, S., P. Elorika, and S. Anwar. 2023. Effect of Sintering Time on Electrical, Ferroelectric, and Piezoelectric Performances of Microwave Synthesized Sodium Bismuth Titanate Ceramics. Materials Science and Engineering B. 298: 116823.
Khan, I. H., M. S. Habib, A. Maqbool, M. A. Rafiq, A. Ali, K. Nur, et al. 2024. Comparative Analysis of Bulk Ceramics and Thick Film Coatings for Optimized Energy Storage Technologies. Scientific Reports. 14(1): 31800.
Kuanar, B., H. Mohanty, B. Dalai, and D. Behera. 2022. Structural and Electrical Properties of Bismuth Sodium Titanate Ceramic. In IOP Conference Series: Materials Science and Engineering. 1258(1): 012007.
Kuanar, B., B. Dalai, D. Behera, and H. S. Mohanty. 2023. Impact of Gd3+ Substitution on the Structural, Morphological, and Electrical Properties of Lead-Free Bi0.5Na0.5TiO3 Ceramics. Journal of Materials Science: Materials in Electronics. 34(6): 506.
Li, Y., H. Chen, Y. Wang, H. Du, J. Shi, X. Liu, et al. 2020. Improved Electric Energy Storage Properties of BT-SBT Lead-Free Ceramics Incorporating A-Site Substitution with Na and Bi Ions and Liquid Sintering Generated by Na0.5Bi0.5TiO3. Journal of Alloys and Compounds. 156708. https://doi.org/10.1016/j.jallcom.2020.156708.
Li, Y., R. Rao, Y. Wang, H. Du, J. Shi, and X. Liu. 2023. Effect of Chemical Inhomogeneity on the Dielectric and Impedance Behaviors of Bismuth Sodium Titanate Based Relaxors. ECS Journal of Solid State Science and Technology. 12(1): 013005.
Li, M., Q. Xu, C. Zhu, W. Luo, Y. Gu, X. Wang, et al. 2021. Investigation of Ga Doping for Non-Stoichiometric Sodium Bismuth Titanate Ceramics. Journal of Materials Science: Materials in Electronics. 32: 16104–12.
Madolappa, S., H. K. Choudhary, N. Punia, A. V. Anupama, and B. Sahoo. 2021. Dielectric Properties of A-Site Mn-Doped Bismuth Sodium Titanate Perovskite: (Bi0.5Na0.5)0.9Mn0.1TiO3. Materials Chemistry and Physics. 270: 124849. https://doi.org/10.1016/j.matchemphys.2021.124849.
Malathi, A. R., G. S. Kumar, and G. Prasad. 2015. Effect of SrTiO3 on Dielectric and Piezoelectric Properties of NBT. Phase Transitions. 88(2): 169–82. https://doi.org/10.1080/01411594.2014.964715.
Mesrar, M., A. Elbasset, N.-S. Echatoui, F. Abdi, and T. Lamcharfi. 2022. Studies of Structural, Dielectric, and Impedance Spectroscopy of KBT-Modified Sodium Bismuth Titanate Lead-Free Ceramics. ACS Omega. 7(42): 37142–63. https://doi.org/10.1021/acsomega.2c03139.
Mesrar, M., T. Lamcharfi, N. S. Echatoui, and F. Abdi. 2022. Effect of Sintering Temperature on the Microstructure and Electrical Properties of Na0.5Bi0.5TiO3 Processed by the Sol–Gel Method. Journal of Sol-Gel Science and Technology. 103 (3): 820–31. https://doi.org/10.1007/s10971-022-05885-y.
Nakonieczny, D. S., F. Kern, L. Dufner, A. Dubiel, M. Antonowicz, and K. Matus. 2021. Effect of Calcination Temperature on the Phase Composition, Morphology, and Thermal Properties of ZrO2 and Al2O3 Modified with APTES (3-Aminopropyltriethoxysilane). Materials. 14(21): 6651.
Niu, X., X. Jian, X. Chen, H. Li, W. Liang, J. Chen, et al. 2023. Superior Energy Storage Properties in Lead-Free Na0.5Bi0.5TiO3-Based Relaxor Ferroelectric Ceramics via Compositional Tailoring and Bandgap Engineering. Scripta Materialia. 230: 115387.
Pal, V., R. Dwivedi, and O. Thakur. 2014. Effect of Neodymium Substitution on Structural and Ferroelectric Properties of BNT Ceramics. Materials Research Bulletin. 51: 189–96.
Pascual, M. N.-L., E. M. Moreno, L. O. Jøsang, M. Merlo, and J. J. Biendicho. 2024. Revealing the Impact of CO2 Exposure During Calcination on the Physicochemical and Electrochemical Properties of LiNi0.8Co0.1Mn0.1O2. Nanoscale. 16(48): 22326–36.
Paterson, A. R., H. Nagata, X. Tan, J. E. Daniels, M. Hinterstein, R. Ranjan, et al. 2018. Relaxor-Ferroelectric Transitions: Sodium Bismuth Titanate Derivatives. MRS Bulletin. 43 (8): 600–606.
Ren, P., Z. Wang, N. Sun, P. Zhao, Y. Liu, Y. Guo, et al. 2021. High Field Electroformation of Sodium Bismuth Titanate and Its Solid Solutions with Barium Titanate. Journal of Materials Chemistry C. 9(9): 3334–42. https://doi.org/10.1039/D0TC05728B.
Rhimi, N., N. Dhahri, M. Khelifi, E. Hlil, and J. Dhahri. 2022. Structural, Morphological, Optical and Dielectric Properties of Sodium Bismuth Titanate Ceramics. Inorganic Chemistry Communications. 146: 110119.
Riess, K., N. H. Khansur, A. Martin, A. Benčan, H. Uršič, and K. G. Webber. 2021. Stress- and Frequency-Dependent Properties of Relaxor-Like Sodium Bismuth Titanate. Physical Review B. 103(9): 094113. https://doi.org/10.1103/PhysRevB.103.094113.
Sahu, R. K., and S. Asthana. 2024. Enhanced Energy Storage Performance, Breakdown Strength, and Thermal Stability in Compositionally Designed Relaxor Eu3+ Substituted Na0.2K0.3Bi0.5TiO3. Journal of Energy Storage. 91: 112020. https://doi.org/10.1016/j.est.2024.112020.
Samantaray, K. S., A. Mishra, D. Rout, A. Srinivas, A. Perumal, and S. Sahoo. 2023. Room Temperature Magneto-Dielectric Coupling in the CaMnO3 Modified NBT Lead-Free Ceramics. Applied Physics A. 129(4): 237. https://doi.org/10.1007/s00339-023-06513-4.
Shrout, T. R., and S. J. Zhang. 2007. Lead-Free Piezoelectric Ceramics: Alternatives for PZT? Journal of Electroceramics. 19(1): 113–26.
Singh, S., A. Kaur, P. Kaur, and L. Singh. 2023. High-Temperature Dielectric Relaxation and Electric Conduction Mechanisms in a LaCoO3-Modified Na0.5Bi0.5TiO3 System. ACS Omega. 8(28): 25623–38.
Steiner, S., J. Heldt, O. Sobol, W. Unger, and T. Frömling. 2021. Influence of Oxygen Vacancies on Core-Shell Formation in Solid Solutions of (Na,Bi)TiO3 and SrTiO3. Journal of the American Ceramic Society. 104(9): 4341–50.
Takiul, I., S. Lee, and H. Hwang. 2024. Sinterability, Microstructural Evolution, and Dielectric Performance of Bismuth Sodium Titanate (Bi0.5Na0.5TiO3) Lead-Free Ferroelectric Ceramics. Archives of Metallurgy and Materials. 33–38.
Viola, G., Y. Tian, C. Yu, Y. Tan, V. Koval, X. Wei, K.-L. Choy, and H. Yan. 2021. Electric Field-Induced Transformations in Bismuth Sodium Titanate-Based Materials. Progress in Materials Science. 122: 100837.
Wang, Z., D. Xue, Y. Zhou, N. Wang, X. Ding, J. Sun, T. Lookman, and D. Xue. 2021. Enhanced Energy-Storage Density by Reversible Domain Switching in Acceptor-Doped Ferroelectrics. Physical Review Applied. 15(3): 034061.
Wu, J., H. Wang, D. Su, G. Liu, B. Zhang, H. Du, et al. 2022. Enhanced Energy-Storage Performances in Sodium Bismuth Titanate-Based Relaxation Ferroelectric Ceramics with Optimized Polarization by Tuning Sintering Temperature. Materials. 15(14): 4981. https://doi.org/10.3390/ma15144981.
Yang, F., M. Wu, Y. Huang, P. Li, W. Zhao, and S. Xu. 2020. From Insulator to Oxide-Ion Conductor by a Synergistic Effect from Defect Chemistry and Microstructure: Acceptor-Doped Bi-Excess Sodium Bismuth Titanate Na0.5Bi0.51TiO3.015. Journal of Materials Chemistry A. 8(47): 25120–30. https://doi.org/10.1039/D0TA10071D.
Zhang, Y., X. Ke, K. Zhao, Z. Zhou, and R. Liang. 2022. Ca2+ Doping Effects on the Structural and Electrical Properties of Na0.5Bi4.5Ti4O15 Piezoceramics. Ceramics International. https://doi.org/10.1016/j.ceramint.2022.06.201.
Zou, K., Y. Dan, H. Xu, Q. Zhang, Y. Lu, H. Huang, and Y. He. 2019. Recent Advances in Lead-Free Dielectric Materials for Energy Storage. Materials Research Bulletin. 113: 190–201.
Downloads
Published
Issue
Section
License
Copyright of articles that appear in Jurnal Teknologi belongs exclusively to Penerbit Universiti Teknologi Malaysia (Penerbit UTM Press). This copyright covers the rights to reproduce the article, including reprints, electronic reproductions, or any other reproductions of similar nature.













