Sains Malaysiana 53(2)(2024): 421-432

http://doi.org/10.17576/jsm-2024-5302-15

 

Kesan Penggantian Litium ke atas Struktur, Sifat Fizikal dan Sifat Elektrik terhadap Seramik BCZT

(The Effect of Lithium Substitution on the Structure, Physical, and Electrical Properties of BCZT Ceramic)

 

HAZIQAH FADHLINA1, A. ATIQAH1,*, ZALITA ZAINUDDIN2, NUR SHAKILA OTHMAN2, SOLEHAH ALI2 & NOR AMALINA2

 

1Institute of Microengineering and Nanoelectronics, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia

2School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia

 

Received: 30 July 2023/Accepted: 24 January 2024

 

Abstract

The invention of novel lead-free piezoelectric materials with ABO3 perovskite structure, based on barium calcium zirconate titanate (BCZT) for application in various device especially in sensor application. In this work, BCZT with lithium substitution at the calcium site with composition Ba0.85Ca0.15-xLi2xZr0.1Ti0.9O3 (x = 0.00, 0.03, 0.06, 0.09 and 0.12) were synthesized by using the conventional, solid state reaction method. The influence of different Li content on the structure, microstructure, density, and electrical properties were investigated. The results show that substitution led to the improvement of the physical and electrical properties of the piezoelectric ceramic materials. The physical properties show the largest grain size and the highest value of density, ρ which is 4.158 g/cm3 for x = 0.06. This physical properties led to the highest value of piezoelectric coefficient, d33, remnant polarisation, Pr and saturated polarization, Ps which are 304.6 pC/N, 3.27 µC/cm2, and 5.54 µC/cm2, respectively, while the highest dielectric constant, ɛr was 3994 when x = 0.12.

 

Keywords: BCZT materials; ceramic materials; d33; lead-free piezoelectric material; lithium substitution; piezoelectric coefficient

 

Abstrak

Inovasi bahan piezoelektrik bebas plumbum yang berstruktur perovskit ABO3, berasaskan barium kalsium zirkonat titanat (BCZT) bagi mencipta peranti yang dapat digunakan secara meluas terutamanya dalam aplikasi sensor. Dalam kajian ini, BCZT dengan penggantian litium pada tapak kalsium dengan komposisi bahan Ba0.85Ca0.15-xLi2xZr0.1Ti0.9O3 (x = 0.00, 0.03, 0.06, 0.09 dan 0.12) telah disintesis menggunakan kaedah konvensional, tindak balas keadaan pepejal. Kesan kandungan Li yang berbeza terhadap struktur, mikrostruktur, ketumpatan dan sifat elektik telah dikaji. Hasi kajian menunjukkan penggantian Li membawa kepada peningkatan sifat fizikal dan elektrik bahan seramik piezoelektrik. Sifat fizikal bahan menunjukkan saiz butiran yang paling besar dan nilai ketumpatan, ρ yang paling tinggi iaitu 4.158 g/cm3 apabila x = 0.06. Sifat fizikal ini menyumbang kepada nilai pemalar piezoelektrik, d33, pengutuban baki, Pr dan pengutuban tepu, Ps yang tertinggi dengan nilai masing-masing ialah 304.6 pC/N, 3.27µC/cm2 dan 5.54 µC/cm2 manakala bagi pemalar dielektrik, ɛr nilai paling tinggi diperoleh apabila x = 0.12 iaitu 3994.

 

Kata kunci: Bahan BCZT; bahan piezoelektrik bebas plumbum; bahan seramik; d33; pemalar piezoelektrik; penggantian litium

 

REFERENCES

Awan, M.Q., Ahmad, J., Sun, Q., Hu, W., Berlie, A. & Liu, Y. 2018. Structure, dielectric and ferroelectric properties of lead-free (Ba,Ca)(Ti,Zr)O3-XBiErO3 piezoelectric ceramics. Ceramics International 44(6): 6872-6877. https://doi.org/10.1016/j.ceramint.2018.01.112

Aziguli, H., Zhang, T. & Yu, P. 2020. Effect of additive glycerol on piezoelectric properties of modified sol-gel (Ba0.85Ca0.15)(Ti0.9Zr0.1)O3 ceramics. Materials Science Forum 993 MSF: 791-798. https://doi.org/10.4028/www.scientific.net/MSF.993.791

Bajpai, P.K. & Tamrakar, P. 2017. Structural and dielectric behavior of doped bismuth sodium titanate: Lead free piezoelectric materials. AIP Conference Proceedings 1837(1): 040062. https://doi.org/10.1063/1.4982146

Bansal, P., Kumar, M., Syal, R., Singh, A.K. & Kumar, S. 2021. Magnetoelectric coupling enhancement in lead-free BCTZ–XNZFO composites. Journal of Materials Science: Materials in Electronics 32(13): 17512-17523. https://doi.org/10.1007/s10854-021-06284-9

Benyoussef, M., Zannen, M., Belhadi, J., Monoun, B., Dellis, J-L., El Marssi, M. & Lahmar, A. 2018. Dielectric, ferroelectric, and energy storage properties in dysprosium doped sodium bismuth titanate ceramics. Ceramics International 44(16): 19451-19460. https://doi.org/10.1016/j.ceramint.2018.07.182

Chen, X., Ruan, X., Zhao, K., He, X., Zeng, J., Li, Y., Zheng, L., Hong, C. & Li, G. 2015. Low sintering temperature and high piezoelectric properties of Li-doped (Ba, Ca)(Ti, Zr) O3 lead-free ceramics. Journal of Alloys and Compounds 632: 103-109. https://doi.org/10.1016/j.jallcom.2015.01.088

Chen, X., Zeng, J., Kim, D., Zheng, L., Lou, Q., Hong, C. & Li, G. 2019. Understanding of role of Li in high-performance Pb-free Li-doped (Ba0.85 Ca0.15)(Ti0.9 Zr0.1)O3 piezoceramics from theory and experiments. Materials Chemistry and Physics  https://doi.org/10.1016/j.matchemphys.2019.04.011

Cheng, Y., Xing, J., Wu, C., Wang, T., Xie, L., Liu, Y., Xu, X., Wang, K., Xiao, D. & Zhu, J. 2020. Investigation of high piezoelectric properties of KNNSb-SrxBNZ ceramics. Journal of Alloys and Compounds 815: 152252. https://doi.org/10.1016/j.jallcom.2019.152252

Deng, Y., Wang, J., Zhang, C., Bai, C., Liu, D., Wu, F. & Yang, B. 2020. Structural and electric properties of MnO2 -Doped KNN-LT lead-free piezoelectric ceramics. Crystals 10(8): 705. https://doi.org/10.3390/cryst10080705

Fadhlina, H., Afdzaluddin, A. & Zainuddin, Z. 2022. A review on lithium doped lead-free piezoelectric materials. Materials Today Communications 33: 104835. https://doi.org/10.1016/j.mtcomm.2022.104835

Gao, X., Dong, N., Xia, F., Guo, Q., Hao, H., Liu, H. & Zhang, S. 2020. Impact of phase structure on piezoelectric properties of textured lead-free ceramics. Crystals 10(5): 367. https://doi.org/10.3390/cryst10050367

Gio, P.D. & Phong, N.D. 2015. Effects of LiF on the structure and electrical properties of (Na0.52K0.435Li0.045)Nb0.87Sb0.08Ta0.05O3 lead-free piezoelectric ceramics sintered at low temperatures. Journal of Materials Science and Chemical Engineering 3(11): 13-20. http://dx.doi.org/10.4236/msce.2015.311003

Halim, N.A., Abd. Majid, W.H. & Velayutham, T.S. 2019. Ferroelectric, pyroelectric and piezoelectric properties of CeO2‑doped Na0.5Bi0.5TiO3 ceramics. SN Applied Sciences 1: 582. https://doi.org/10.1007/s42452-019-0593-2

He, X., Han, F., Liu, M., Yuan, Z., Jiang, X., Hu, C., Ren, S., Lei, X. & Liu, L. 2020. High-temperature dielectric and relaxation behavior of tantalum-doped sodium bismuth titanate-barium titanate ceramics. Journal of Electronic Materials 49(11): 6643-6655. https://doi.org/10.1007/s11664-020-08441-y

Hwang, C-C., Chou, C-C., Wang, J-L., Hsieh, T-Y. & Tseng, J-T. 2012. The lithium doping effect on (Na0.5K0.5)NbO3 lead-free piezo-ceramics structure structure stability and ferroelectric characteristics. 217-219: 682-685. https://doi.org/10.4028/www.scientific.net/AMM.217-219.682

Izzuddin, I., Jumali, M.H.H., Zalita, Z., Huwaida, J.N. & Awang, R. 2016. Influence of crystal structural orientation on impedance and piezoelectric properties of KNN ceramic prepared using sol-gel method. Sains Malaysiana 45(8): 1281-1287.

Jain Ruth, D.E., Venkidu, L. & Sundarakannan, B. 2018. Structure-property relation to enhance the piezoelectric free piezoelectric ceramics. Journal of Materials Science: Materials in Electronics 29: 5433-5438. https://doi.org/10.1007/s10854-017-8509-7

Jiang, M., Zhang, J., Rao, G., Li, D., Randall, C.A., Li, T., Peng, B., Li, L., Gu, Z., Liu, X. & Huang, H. 2019. Ultrahigh piezoelectric coefficient of a lead-free K0.5Na0.5NbO3-based single crystal fabricated by a simple seed-free solid-state growth method. Journal of Materials Chemistry C 7: 14845-14854. https://doi.org/10.1039/c9tc05143k

Kaleva, G.M., Politova, E.D., Mosunov, A.V. & Stefanovich, S.Y. 2020. Phase formation, structure, and dielectric properties of modified potassium sodium niobate ceramics. Inorganic Materials 56(10): 1072-1078. https://doi.org/10.1134/S0020168520100076

Kim, J., Ji, J-H., Shin, D-J. & Koh, J-H. 2018. Improved Li and Sb doped lead-free (Na,K)NbO3 piezoelectric ceramics for energy harvesting applications. Ceramics International 44(18):  22219-22224. https://doi.org/10.1016/j.ceramint.2018.08.341

Kornphom, C., Laowanidwatana, A. & Bongkarn, T. 2017. Influence of sintering temperature on properties of BNKLLT–wt% BCTZ binary lead-free piezoelectric ceramic prepared through the solid-state combustion technique. Phase Transitions 90(3): 317-324. https://doi.org/10.1080/01411594.2016.1192169

Kornphom, C., Udeye, T., Thongbai, P. & Bongkarn, T. 2017. Phase structures, PPT region and electrical properties of new lead-free KNLNTS-BCTZ ceramics fabricated via the solid-state combustion technique. Ceramics International 43(Supplement 1): S182-S192. https://doi.org/10.1016/j.ceramint.2017.05.180

Kumar, S., Kurchania, R. & Kumar, A. 2019. Dielectric and impedance spectroscopic study of lithium doped potassium tantalum niobium oxide. Ceramics International 45(14): 17137-17143. https://doi.org/10.1016/j.ceramint.2019.05.267

Li, P., Fu, Z., Wang, F., Huan, Y., Zhou, Z., Zhai, J., Shen, B. & Zhang, S. 2020. High piezoelectricity and stable output in BaHfO3 and (Bi0.5 Na 0.5)ZrO3 modified (K0.5Na0.5)(Nb0.96Sb0.04)O3 textured ceramics. Acta Materialia 199: 542-550. https://doi.org/10.1016/j.actamat.2020.08.058

Ma, J., Wu, J., Wu, B. & Wu, W. 2020. Advances in the modification of the contradictory relationship between piezoelectricity and curie temperature: Simultaneous realization of large piezoelectricity and high curie temperature in potassium sodium niobate-based ferroelectrics. Journal of Materials Chemistry C 8(28): 9506-9510. https://doi.org/10.1039/d0tc01888k

Mawani, H.D., Shastri, N.M., Mangrola, M.H. & Joshi, V.G. 2020. Structural and electrical properties of sodium bismuth titanate prepared by solid state reaction method. AIP Conference Proceedings 2220(1): 140055. https://doi.org/10.1063/5.0002127

Mekonnen, M.A. & Tadesse, M.Z. 2021. Low temperature sintering of (Ba0.85Ca0.15)(Ti0.90Zr0.10)O3 lead-free piezoceramic with the additive of MnO2. Journal of Electroceramics 46: 115-123. https://doi.org/10.1007/s10832-021-00250-x

Ming, B-Q., Wang, J-F. & Zang, G-Z. 2008. Effects of Li substitution and sintering temperature on properties of Bi0.5(Na,K)0.5TiO3 lead-free piezoelectric ceramics. Chinese Physics Letters 25(10): 3776-3778. http://dx.doi.org/10.1088/0256-307X/25/10/070

Mohammad Hafizuddin Haji Jumali, Mohd Riduan Mohd, Ngoi Yung Wee, Muhammad Yahaya & Muhammad Mat Salleh. 2010. Kelakuan pengesanan tekanan bagi seramik natrium bismut titanat. Sains Malaysiana 39(4): 621-626.

Negi, N.S., Kumar, R., Sharma, H., Shah, J. & Kotnala, R.K. 2018. Structural, multiferroic, dielectric and magnetoelectric properties of (1-x)Ba0.85Ca0.15Ti0.90Zr0.10O3-(x)CoFe2O4 lead-free composites. Journal of Magnetism and Magnetic Materials 456: 292-299. https://doi.org/10.1016/j.jmmm.2017.12.095

Nor Huwaida Binti Janil @ Jamil, Mohammad Hafizuddin Bin Hj Jumali, Zalita Binti Zainuddin, Izura Binti Izzuddin & Soodkhet Pojprapai. 2019. Penentuan parameter optimum bagi rawatan pengutuban elektrik ke atas seramik-piezo (BaTiO3) menggunakan sistem buatan sendiri. Sains Malaysiana 48(2): 425-433. https://doi.org/10.17576/jsm-2019-4802-21

Orlik, K., Lorgouilloux, Y., Marchet, P., Thuault, A., Jean, F., Rguiti, M. & Courtois, C. 2020. Influence of microwave sintering on electrical properties of BCTZ lead free piezoelectric ceramics. Journal of the European Ceramic Society 40(4): 1212-1216. https://doi.org/10.1016/j.jeurceramsoc.2019.12.010

Perumal, R.N., Athikesavan, V. & Nair, P. 2018. Influence of lead titanate additive on the structural and electrical properties of Na0.5Bi0.5TiO3-SrTiO3 piezoelectric ceramics. Ceramics International 44(11): 13259-13266. https://doi.org/10.1016/j.ceramint.2018.04.155

Politova, E.D., Strebkov, D.A., Belkova, D.A., Kaleva, G.M., Mosunov, A.V., Sadovskaya, N.V. & Stefanovich, S.Y. 2020. Phase formation and relaxor properties of lead-free perovskite ceramics on the base of sodium-bismuth titanate (Na0.5Bi0.5)(Ti,Mg)O3. Ferroelectrics 560(1): 48-53. https://doi.org/10.1080/00150193.2020.1722882

Reshetnikova, E.A., Lisnevskaya, I.V. & Terekhin, A.I. 2020. Hydrothermal synthesis of sodium bismuth titanate ferroelectrics. Inorganic Materials 56(1): 83-90. https://doi.org/10.1134/S0020168520010136

Sarizal Md Ani, Andanastuti Muchtar, Norhamidi Muhamad, & Jaharah A. Ghani. 2017. Kesan suhu pensinteran terhadap sifat mekanik dan mikrostruktur alumina-zirkonia yang difabrikasi dengan kaedah pengacuan suntikan seramik. Sains Malaysiana 46(10): 1979-1986. https://doi.org/10.17576/jsm-2017-4610-37

Sharma, S., Sharma, H., Thakur, S., Shah, J., Kotnala, R.K. & Negi, N.S. 2021a. Structural, magnetic, magneto-dielectric and magneto-electric properties of (1-x) Ba0.85Ca0.15Ti0.90Zr0.10O3 – (x) CoFe2O4 lead-free multiferroic composites sintered at higher temperature. Journal of Magnetism and Magnetic Materials 538: 168243. https://doi.org/10.1016/j.jmmm.2021.168243

Sharma, S., Thakur, S., Shah, J., Kotnala, R.K. & Negi, N.S. 2021b. Influence of phase dominance on structural, magneto-dielectric, magnetic-electric properties of (Ba0.85Ca0.15Zr0.1Ti0.9)O3-CoFe2O3 composites. Journal of Materials Science: Materials in Electronics 32(5): 6570-6585. https://doi.org/10.1007/s10854-021-05373-z

Shi, S., Hashimoto, H. & Sekino, T. 2021. Enhancing piezoelectric properties of Ba0.88Ca0.12Zr0.12Ti0.88O3 lead-free ceramics by doping Co ions. Ceramics International 47(3): 3272-3278. https://doi.org/10.1016/j.ceramint.2020.09.167

Sun, Y., Yang, H., Guan, S., Cao, Y., Jiang, M. & Liu, X. 2019. Strong piezoelectricity of Li2CO3-Doped BiFeO3–BaTiO3–Bi(Zn0.5Ti0.5)O3 lead-free piezoelectric ceramics with high curie temperature and high temperature stability. Journal of Alloys and Compounds 2019: 153058. https://doi.org/10.1016/j.jallcom.2019.153058

Tan, C.K.I., Yao, K. & Ma, J. 2013. Effects of LiF on the structure and properties of Ba0.85Ca0.15Zr0.1Ti0.9O3 lead-free piezoelectric ceramics. International Journal of Applied Ceramic Technology 10(4): 701-706. https://doi.org/10.1111/j.1744-7402.2012.02771.x

Tian, Y., Wang, Q., Zhang, B., Qin, P., Gong, Y., Ji, X. & Jing, Q. 2020. Temperature-dependent ferroelectric and piezoelectric response of Yb3+ and Tm3+ co-doped Ba0.85Ca0.15Zr0.1Ti0.9O3 lead-free ceramics. Research Square https://doi.org/10.21203/rs.3.rs-53948/v2

Ul, R., Marchet, P., Pham-Thi, M. & Tran-Hue-Huu, L-P. 2019. Improved properties of doped BaTiO3 piezoelectric ceramics. Physica Status Solidi 2019: 1900413. https://doi.org/10.1002/pssa.201900413

Verma, A., Yadav, A.K., Khatun, N., Kumar, S., Jangir, R., Srihari, V., Raghavendra Reddy, V., Liu, S.W., Biring, S. & Sen, S. 2018. Structural, dielectric and ferroelectric studies of thermally stable and efficient energy storage ceramic material (Na0.5-xKxBi0.5-XLax)TiO3. Ceramics International 44(16): 20178-20186. https://doi.org/10.1016/j.ceramint.2018.07.312

Wang, C., Li, Q., Zhang, W., Yan, B., Yadav, A.K., Peng, H. & Fan, H. 2020. [Bi0.5(Na0.4-XLixK0.1)]0.96Sr0.04Ti0.975Ta0.025O3 lead-free relaxor ceramics with the enhanced recoverable energy density. Ceramics International 46(1): 715-721. https://doi.org/10.1016/j.ceramint.2019.09.024

Wang, Q., Lin, J., Zhou, Y., Lin, C., Lin, T. & Wu, X. 2020. Sm-induced multifunctionality and poling effect on luminescence of Sm-doped (Ba0.85Ca0.15)(Ti0.9Zr0.1)O3 piezoceramics. Functional Materials Letters 13(5): 2051023. https://doi.org/10.1142/S1793604720510236

Wang, X., Yue, J. & Liu, J. 2021. Enhanced temperature stability and electrical properties of Bi/Mn Co-doped (Ba,Ca) (Zr,Ti)O3 lead-free ceramics. Ceramics International 47(2): 2525-2530. https://doi.org/10.1016/j.ceramint.2020.09.096

Wongsaenmai, S., Ananta, S. & Yimnirun, R. 2012. Effect of Li addition on phase formation behavior and electrical properties of (K0.5Na0.5)NbO3 lead free ceramics. Ceramics International 38(1): 147-152. https://doi.org/10.1016/j.ceramint.2011.06.049

Wu, Y., Ma, F., Qu, J., Luo, Y., Lv, C., Guo, Q. & Qi, T. 2019. Vertically-aligned lead-free BCTZY nanofibers with enhanced electrical properties for flexible piezoelectric nanogenerators. Applied Surface Science 469: 283-291. https://doi.org/10.1016/j.apsusc.2018.10.229

Wu, Y., Ma, F., Qu, J., Luo, Y., Song, J., Wei, G., Zhang, Y. & Qi, T. 2018. Role of Cu and Y in sintering, phase transition, and electrical properties of BCZT lead-free piezoceramics. Ceramics International 44(13): 15001-15009. https://doi.org/10.1016/j.ceramint.2018.05.129

Xu, J., Lu, Q., Lin, J., Lin, C., Zheng, X., Lin, T. & Wu, X. 2020. Enhanced ferro-/piezoelectric properties of tape-casting-derived Er3+-doped Ba0.85Ca0.15Ti0.9Zr0.1O3 optoelectronic thick films. Journal of Advanced Ceramics 9(6): 693-702. https://doi.org/10.1007/s40145-020-0405-6

Xu, J., Zhou, Y., Li, Z., Lin, C., Zheng, X., Lin, T., Wu, X. & Wang, F. 2021. Microstructural, ferroelectric and photoluminescence properties of Er3+-doped Ba0.85Ca0.15Ti0.9Zr0.1O3 thin films. Materials Chemistry and Physics 262: 124320. https://doi.org/10.1016/j.matchemphys.2021.124320

Yan, X., Zheng, M., Zhu, M. & Hou, Y. 2019. Enhanced electrical resistivity and mechanical properties in BCTZ-based composite ceramic. Journal of Advanced Dielectrics 9(5): 1950036. https://doi.org/10.1142/S2010135X1950036X

Zhai, Y., Du, J., Chen, C., Li, W. & Hao, J. 2020. The photoluminescence and piezoelectric properties of Eu2O3 doped KNN-based ceramics. Journal of Alloys and Compounds 829: 154518. https://doi.org/10.1016/j.jallcom.2020.154518

Zhang, Y., Sun, H.J. & Chen, W. 2016. Li-modified Ba0.99Ca0.01Zr0.02Ti0.98O3lead-free ceramics with highly improved piezoelectricity. Journal of Alloys and Compounds 694: 745-751. https://doi.org/10.1016/j.jallcom.2016.10.061

Zhao, R., Li, Y., Zheng, Z. & Kang, W. 2020. Phase structure regulation and enhanced piezoelectric properties of Li-doped KNN-based ceramics. Materials Chemistry and Physics 245: 122806. https://doi.org/10.1016/j.matchemphys.2020.122806

 

*Corresponding author; email: a.atiqah@ukm.edu.my

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

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