相界工程和畴工程调控(1-x)(0.8PZT-0.2PZN)-xBZT陶瓷的压电性能

doi:10.15541/jim20240463

摘要/Abstract

摘要： Pb(Zr,Ti)O₃-Pb(Zn_1/3Nb_2/3)O₃(PZT-PZN)基陶瓷作为重要的压电材料, 在传感器和执行器等领域具有广泛应用, 优化其压电性能一直是研究热点。本研究旨在通过相界工程和畴工程调控与优化(1-x)[0.8Pb(Zr_0.5Ti_0.5)O₃- 0.2Pb(Zn_1/3Nb_2/3)O₃]-xBi(Zn_0.5Ti_0.5)O₃((1-x)(0.8PZT-0.2PZN)-xBZT)陶瓷的压电性能, 利用不同手段详细表征陶瓷样品的晶相结构和微观形貌。结果显示, 所有样品均具有纯钙钛矿结构, 且加入BZT使晶粒尺寸逐渐增大。研究发现, 加入BZT使陶瓷样品从准同型相界(MPB)向四方相发生变化, 这种相变对于优化压电性能至关重要。通过调控BZT的含量, 精确控制相界位置, 可以优化压电性能。畴结构是影响压电性能的关键因素之一。通过畴工程手段, 优化晶粒尺寸和畴尺寸等, 显著提高了陶瓷样品的压电性能。具体而言, 当x=0.08时, 压电常数d₃₃(320 pC/N)和机电耦合系数k_p(0.44)达到最大。结合实验结果和理论分析, 探讨了相界工程和畴工程对压电性能的影响机制, 研究发现加入BZT不仅促进了晶粒生长, 还优化了畴结构, 使得极化反转过程更加容易进行, 从而提高了压电性能。这些研究成果不仅为高性能压电陶瓷的设计提供了新思路, 还为相关电子器件的研制奠定了理论基础。

关键词: 相界, 0.8PZT-0.2PZN, 畴工程, 压电性能

Abstract:

Pb(Zr,Ti)O₃-Pb(Zn_1/3Nb_2/3)O₃ (PZT-PZN) based ceramics, as important piezoelectric materials, have a wide range of applications in fields such as sensors and actuators, thus the optimization of their piezoelectric properties has been a hot research topic. This study investigated the effects of phase boundary engineering and domain engineering on (1-x)[0.8Pb(Zr_0.5Ti_0.5)O₃-0.2Pb(Zn_1/3Nb_2/3)O₃]-xBi(Zn_0.5Ti_0.5)O₃ ((1-x)(0.8PZT-0.2PZN)- xBZT) ceramic to obtain excellent piezoelectric properties. The crystal phase structure and microstructure of ceramic samples were characterized. The results showed that all samples had a pure perovskite structure, and the addition of BZT gradually increased the grain size. The addition of BZT caused a phase transition in ceramic samples from the morphotropic phase boundary (MPB) towards the tetragonal phase region, which is crucial for optimizing piezoelectric properties. By adjusting content of BZT and precisely controlling position of the phase boundary, the piezoelectric performance can be optimized. Domain structure is one of the key factors affecting piezoelectric performance. By using domain engineering techniques to optimize grain size and domain size, piezoelectric properties of ceramic samples have been significantly improved. Specifically, excellent piezoelectric properties (piezoelectric constant d₃₃=320 pC/N, electromechanical coupling factor k_p=0.44) were obtained simultaneously for x=0.08. Based on experimental results and theoretical analysis, influence mechanisms of phase boundary engineering and domain engineering on piezoelectric properties were explored. The study shows that addition of BZT not only promotes grain growth, but also optimizes the domain structure, enabling the polarization reversal process easier, thereby improving piezoelectric properties. These research results not only provide new ideas for the design of high-performance piezoelectric ceramics, but also lay a theoretical foundation for development of related electronic devices.

Key words: phase boundary, 0.8PZT-0.2PZN, domain engineering, piezoelectric property

中图分类号:

TB34

陈相杰, 李玲, 雷添福, 王佳佳, 汪尧进. 相界工程和畴工程调控(1-x)(0.8PZT-0.2PZN)-xBZT陶瓷的压电性能[J]. 无机材料学报, 2025, 40(6): 729-734.

CHEN Xiangjie, LI Ling, LEI Tianfu, WANG Jiajia, WANG Yaojin. Enhanced Piezoelectric Properties of (1-x)(0.8PZT-0.2PZN)-xBZT Ceramics via Phase Boundary and Domain Engineering[J]. Journal of Inorganic Materials, 2025, 40(6): 729-734.

图/表 7

Fig. 1 XRD patterns of (1-x)(0.8PZT-0.2PZN)-xBZT ceramics

Fig. 2 SEM images (a-h) and average grain sizes (i) of (1-x)(0.8PZT-0.2PZN)-xBZT ceramics

Fig. 3 Microstructure (a) and element mappings (b-f) of (1-x)(0.8PZT-0.2PZN)-xBZT (x=0.08) ceramics

Fig. 4 P-E hysteresis loops (a), J-E curves (b) and variation trends of the remnant polarization Pr and coercive field Ec (c) for (1-x)(0.8PZT-0.2PZN)-xBZT ceramics at room temperature Colorful figures are available on website

Fig. 5 Room temperature out-of-plane height, amplitude, and phase images of (1-x)(0.8PZT-0.2PZN)-xBZT ceramics (a) x=0; (b) x=0.08; (c) x=0.14. Colorful figures are available on website

Fig. 6 Temperature dependence of εr and tanδ of (1-x)(0.8PZT-0.2PZN)-xBZT ceramics (a) x=0; (b) x=0.02; (c) x=0.04; (d) x=0.06; (e) x=0.08; (f) x=0.10; (g) x=0.12; (h) x=0.14. Colorful figures are available on website

Fig. 7 d33 and kp of (1-x)(0.8PZT-0.2PZN)-xBZT ceramics

参考文献 30

[1]	FURUKAWA T, ISHIDA K, FUKADA E. Piezoelectric properties in the composite systems of polymers and PZT ceramics. J. Appl. Phys., 1979, 50(7): 4904.
[2]	WU J, XIAO D, ZHU J. Potassium-sodium niobate lead-free piezoelectric materials: past, present, and future of phase boundaries. Chem. Rev., 2015, 115(7): 2559.
[3]	BENECH P, DUCHAMP J M. Piezoelectric materials and their applications in radio frequency domain and telecommunications. Adv. Appl. Ceram., 2015, 114(4): 220.
[4]	GUO R, CROSS L E, PARK S E, et al. Origin of the high piezoelectric response in PbZr_1-_xTi_xO₃. Phys. Rev. Lett., 2000, 84(23): 5423.
[5]	YAN Y, CHO K H, PRIYA S. Role of secondary phase in high power piezoelectric PMN-PZT ceramics. J. Am. Ceram. Soc., 2011, 94(12): 4138.
[6]	GRINBERG I, SUCHOMEL M R, DAVIES P K, et al. Predicting morphotropic phase boundary locations and transition temperatures in Pb- and Bi-based perovskite solid solutions from crystal chemical data and first-principles calculations. J. Appl. Phys., 2005, 98(9): 094111.
[7]	REMA K P, KUMAR V. Structure-property relationship in Mn-doped (Pb_0.94Sr_0.06)(Zr_0.53Ti_0.47)O₃. J. Am. Ceram. Soc., 2008, 91(1): 164.
[8]	YU X, HOU Y, ZHAO H, et al. Refreshing doping concept in perovskite piezoceramics: composite modulation hidden behind lattice substitution. J. Am. Ceram. Soc., 2020, 103(11): 6378.
[9]	QUANG D A, VUONG L D. Enhanced piezoelectric properties of Fe₂O₃ and Li₂CO₃ co-doped Pb[(Zr_0.48Ti_0.52)_0.8(Zn_1/3Nb_2/3)_0.125(Mn_1/3Nb_2/3)_0.075]O₃ ceramics for ultrasound transducer applications. J. Sci-Adv. Mater. Dev., 2022, 7(2): 100436.
[10]	ZHENG M, HOU Y, ZHU M, et al. Nanodomains in metal/ ferroelectric0-3 type composites: on the origin of the strong piezoelectric effect. Scripta. Mater., 2018, 145: 19.
[11]	YU X, HOU Y, ZHAO H, et al. The role of secondary phase in enhancing transduction coefficient of piezoelectric energy harvesting composites. J. Mater. Chem. C, 2019, 7(12): 3479.
[12]	KIM S W, LEE H C. Development of PZN-PMN-PZT piezoelectric ceramics with high d₃₃ and Q_m values. Materials, 2022, 15(20): 7070.
[13]	LIU Q, SUN Q, MA W, et al. Large-strain 0.7Pb(Zr_xTi_1-_x)O₃- 0.1Pb(Zn_1/3Nb_2/3)O₃-0.2Pb(Ni_1/3Nb_2/3)O₃ piezoelectric ceramics for high-temperature application. J. Eur. Ceram. Soc., 2014, 34(5): 1181.
[14]	XU X, FENG X, ZHOU L, et al. Phase structure and electrical properties of 0.28PIN-0.32PZN-(0.4-x)PT-xPZ piezoelectric ceramics. Crystals, 2023, 13(9): 1362.
[15]	WANG H, ZENG K. Humidity effects on domain structure and polarization switching of Pb(Zn_1/3Nb_2/3)O₃-x%PbTiO₃ (PZN-x%PT) single crystals. Materials, 2021, 14(9): 2447.
[16]	DU J, YANG C, LI Y, et al. Microstructural, dielectric, piezoelectric and ferroelectric properties of xPZN-PZT ternary ceramics. J. Mater. Sci-Mater. El., 2023, 34(9): 780.
[17]	SUCHOMEL M R, FOGG A M, ALLIX M, et al. Bi₂ZnTiO₆: a lead-free closed-shell polar perovskite with a calculated ionic polarization of 150 μC·cm^-2 Chem. Mater., 2006, 18(21): 4987.
[18]	YAN Y, CHO K H, PRIYA S. Identification and effect of secondary phase in MnO₂-doped 0.8Pb(Zr_0.52Ti_0.48)O₃-0.2Pb(Zn_1/3Nb_2/3)O₃ piezoelectric ceramics. J. Am. Ceram. Soc., 2011, 94(11): 3953.
[19]	CAO W W, RANDALL C A. Grain size and domain size relations in bulk ceramic ferroelectric materials. J. Phys. Chem. Solids, 1996, 57(10): 1499.
[20]	LI F, ZHANG S, XU Z, et al. Piezoelectric activity of relaxor- PbTiO₃ based single crystals and polycrystalline ceramics at cryogenic temperatures: intrinsic and extrinsic contributions. Appl. Phys. Lett., 2010, 96(19): 192903.
[21]	LI F, ZHANG S, XU Z, et al. Composition and phase dependence of the intrinsic and extrinsic piezoelectric activity of domain engineered (1-x)Pb(Mg_1/3Nb_2/3)O₃-xPbTiO₃ crystals. J. Appl. Phys., 2010, 108(3): 034106.
[22]	ZHENG L, YI X, ZHANG S, et al. Complete set of material constants of 0.95(Na_0.5Bi_0.5)TiO₃-0.05BaTiO₃ lead-free piezoelectric single crystal and the delineation of extrinsic contributions. Appl. Phys. Lett., 2013, 103(12): 122905.
[23]	LI L, ZHANG J, WANG R X, et al. Thermally-stable large strain in Bi(Mn_0.5Ti_0.5)O₃ modified 0.8Bi_0.5Na_0.5TiO₃-0.2Bi_0.5K_0.5TiO₃ ceramics. J. Eur. Ceram. Soc., 2019, 39(5): 1827.
[24]	LI L, ZHU M, WEI Q, et al. Microstructure and suppressed thermal depolarisation behaviours of lead-free Na_0.5Bi_0.5TiO₃:ZnO ferroelectric composite ceramics. Adv. Appl. Ceram., 2017, 117(3): 133.
[25]	WANG S, LI X, WANG J, et al. Enhanced electromechanical properties in MnCO₃-modified Pb(Ni,Nb)O₃-PbZrO₃-PbTiO₃ ceramics via defect and domain engineering. J. Am. Ceram. Soc., 2022, 106(3): 1970.
[26]	LU X M, HUANG F Z, ZHU J S. Domains in ferroelectrics: formation, structure, mobility and related properties. Acta Phys. Sin., 2020, 69(12): 127704.
[27]	XUE H, ZHENG T, WU J. Understanding the nature of temperature stability in potassium sodium niobate based ceramics from structure evolution under external field. ACS Appl. Mater. Inter., 2020, 12(29): 32925.
[28]	LIU Y X, LI Z, THONG H C, et al. Grain size effect on piezoelectric performance in perovskite-based piezoceramics. Acta Phys. Sin., 2020, 69(21): 217704.
[29]	LI F, ZHANG S, YANG T, et al. The origin of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution crystals. Nat. Commun., 2016, 7: 13807.
[30]	LI F, ZHANG S, DAMJANOVIC D, et al. Local structural heterogeneity and electromechanical responses of ferroelectrics: learning from relaxor ferroelectrics. Adv. Funct. Mater., 2018, 28(37): 1801504.