新型铁电固溶体铌镥酸铅-铌镁酸铅-钛酸铅的制备与表征

doi:10.15541/jim20130655

无机材料学报 ›› 2014, Vol. 29 ›› Issue (9): 912-916.DOI: 10.15541/jim20130655 CSTR: 32189.14.10.15541/jim20130655

新型铁电固溶体铌镥酸铅-铌镁酸铅-钛酸铅的制备与表征

刘颖^{1, 2}, 赖发春¹, 黄志高¹, 沈东全², 龙西法²

(1. 福建师范大学物理与能源学院, 福州 350117; 2. 中国科学院福建物质结构研究所, 光电材料化学与物理重点实验室, 福州 350002)

收稿日期:2013-12-11 修回日期:2014-02-14 出版日期:2014-09-17 网络出版日期:2014-08-21
作者简介:刘颖(1986–), 男, 助理研究员. E-mail: liuying@fjirsm.ac.cn
基金资助:
国家自然科学基金 (91122020)

Preparation and Characterization of A New Ferroelectric Ternary Solid Solution Pb(Lu_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃

LIU Ying^1,2, LAI Fa-Chun¹, Huang Zhi-Gao¹, SHEN Dong-Quan², LONG Xi-Fa²

(1. College of Physics and Energy, Fujian Normal University, Fuzhou 350117, China; 2. Key Laboratory of Optoelectric Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China)

Received:2013-12-11 Revised:2014-02-14 Published:2014-09-17 Online:2014-08-21
About author:LIU Ying. E-mail: liuying@fjirsm.ac.cn
Supported by:
National Natural Science Foundation of China (91122020)

摘要/Abstract

摘要：

采用二次合成法制备了纯相钙钛矿结构三元(0.7-x)Pb(Lu_1/2Nb_1/2)O₃-0.3Pb(Mg_1/3Nb_2/3)O₃-xPbTiO₃(PLN- PMN-PT) (0.38 ≤ x ≤ 0.46) 压电陶瓷, 研究了准同型相界(MPB)附近组分的介电、压电和铁电性能。XRD分析表明PLN-PMN-PT存在准同型相界, 且准同型相界区域大致为0.40 ≤ x ≤ 0.44。MPB附近组分为0.29PLN-0.3PMN- 0.41PT陶瓷具有较高的居里温度和相变温度, 分别为270℃和135℃, 同时该组分表现出较好的铁电压电性能, 压电系数达到460 pC/N, 矫顽场为14.8 kV/cm, 剩余极化强度P_r为34.6 μC/cm²。PLN-PMN-PT材料在压电领域具有潜在的应用前景。

关键词: 压电陶瓷, 固相法, PLMNT, 压电性能

Abstract:

Ceramics of (0.7-x)Pb(Lu_1/2Nb_1/2)O₃-0.3Pb(Mg_1/3Nb_2/3)O₃-xPbTiO₃(PLN-PMN-PT) (0.38 ≤ x ≤ 0.46) ternary system were synthesized by means of a two-step columbite precursor method which can effectively suppress the pyrochlore phase. A morphotropic phase boundary (MPB) region in the ternary systems was found in the range of 0.40 ≤ x ≤ 0.44 and the electric properties of the compositions near MPB region were investigated. Those compositions within MPB exhibit good comprehensive piezoelectric properties. The ceramic with composition of 0.29PLN- 0.3PMN-0.41PT shows a high Curie temperature of 270℃ and a high rhombohedral-tetragonal phase transition temperature of 135℃, whose piezoelectric coefficient d₃₃, coercive field E_c and remnant polarization P_r are found to be 460 pC/N, 14.8 kV/cm and 34.6 μC/cm², respectively. The large coercive field and high T_c enable it a promising candidate for application in the piezoelectricity field.

Key words: piezoelectric ceramics, solid state reaction, PLMNT, piezoelectric properties

中图分类号:

TQ174

刘颖, 赖发春, 黄志高, 沈东全, 龙西法. 新型铁电固溶体铌镥酸铅-铌镁酸铅-钛酸铅的制备与表征[J]. 无机材料学报, 2014, 29(9): 912-916.

LIU Ying, LAI Fa-Chun, Huang Zhi-Gao, SHEN Dong-Quan, LONG Xi-Fa. Preparation and Characterization of A New Ferroelectric Ternary Solid Solution Pb(Lu_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃[J]. Journal of Inorganic Materials, 2014, 29(9): 912-916.

图/表 8

图1 室温三元PLN-PMN-PT陶瓷相图

Fig. 1 Ternary phase diagram of PLN-PMN-PT at room temperature

表1 (0.7-x)PLN-0.3PMN-xPT陶瓷的烧结工艺

Table 1 Sintering process of (0.7-x)PLN-0.3PMN-xPT ceramics

Composition	Sintering temperature/℃	Sintering time/h
0.32PLN-0.30PMN-0.38PT	1050	3
0.30PLN-0.30PMN-0.40PT	1060	3
0.29PLN-0.30PMN-0.41PT	1070	3
0.28PLN-0.30PMN-0.42PT	1070	3
0.26PLN-0.30PMN-0.44PT	1080	3
0.24PLN-0.30PMN-0.46PT	1100	3

图2 (0.7-x)PLN-0.3PMN-xPT陶瓷XRD图谱

Fig. 2 XRD patterns of (0.7-x)PLN-0.3PMN-xPT ceramics

图3 (0.7-x)PLN-0.3PMN-xPT陶瓷样品的SEM照片

Fig. 3 SEM images of (0.7-x)PLN-0.3PMN-xPT ceramics

图4 0.3PLN-0.30PMN-0.40PT陶瓷的介电温谱

Fig. 4 Variations of dielectric constant of 0.3PLN-0.30PMN- 0.40PT ceramic measured at 10 Hz to 100 kHz

图5 (0.7-x)PLN-0.3PMN-xPT各组分的介电温谱

Fig. 5 Variations of dielectric constant of (0.7-x)PLN-0.3PMN- xPT ceramics with different compositions measured at 1 kHz

图6 室温下(0.7-x)PLN-0.3PMN-xPT陶瓷电滞回线

Fig. 6 Hysteresis loops for the (0.7-x)PLN-0.3PMN-xPT ceramics measured at room temperature

图7 (0.7-x)PLN-0.3PMN-xPT陶瓷的矫顽场EC和压电系数d33随组分x的变化曲线

Fig. 7 Coercive field Ec and piezoelectric coefficient d33 as a function of PT contents for (0.7-x)PLN-0.3PMN-xPT ceramics

参考文献 23

[1]	KUMAR P, PRAKASH C,THAKUR O P, et al. Dielectric, ferroelectric and pyroelectric properties of PMNT ceramics. Physica B, 2006, 371: 313-316.
[2]	DONG M, YE Z G. High-temperature solution growth and characterization of the piezo-/ferroelectric (1-x)Pb(Mg1/3Nb2/3)O3- xPbTiO3 [PMNT] single crystals. Journal of Crystal Growth, 2000, 209(1): 81-90.
[3]	PARK S E, SHROUT T R. Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals. Journal of Applied Physics, 1997, 82(4): 1804-1811.
[4]	SUN D Z, ZHAO M Y, LUO H S, et al. Piezoelectric and dielectric properties of PMNT ceramic materials. Journal of Inorganic Materials, 2000, 15(5): 939-942.
[5]	LEE D H, KIM N K. Crystallographic, dielectric, and diffuseness characteristics of PZN-PT ceramics. Materials Letters, 1998, 34: 299-304.
[6]	WANG X L, HUANG B, YAO X. Effect of excess PbO on phase structures and dielectric properties of PZN-PT ceramics. Ferroelectrics, 1994, 154: 301-306.
[7]	ARI-GUR P, BENGUIGUI L. Direct determination of the coexistence region in the solid sollutions Pb(ZrxTi1-x)O3. J. Phys. D: Appl. Phys., 1975, 8: 1856-1862.
[8]	WERSING W, LUBITZ K, MOHAUPT J. Dielectric, elastic and piezoelectric properties of porous pzt ceramics. Ferroelectrics, 1986, 68: 77-97.
[9]	KELLY J, LEONARD M, TANTIGATE C, et al. Effect of composition on the electromechanical properties of (1-x)Pb(Mg1/3Nb2/3)O3- xPbTiO3 ceramics. J. Am. Ceram. Soc., 1997, 80(4): 957-964.
[10]	YE Z G. High-performance piezoelectric single crystals of complex perovskite solid solutions. Mat. Res. Bull., 2009, 34(4): 277-283.
[11]	NOHEDA B, COX D E, SHIRANE G, et al. Phase diagram of the ferroelectric relaxor (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3. Physical Review B, 2002, 66: 054104-1-10.
[12]	LIM J B, ZHANG S J, SHROUT T R. Relaxor behavior of piezoelectric Pb(Yb1/2Nb1/2)O3-PbTiO3 ceramics sintered at low temperature. J. Electroceram., 2011, 26: 68-73.
[13]	SHEN D Q, LI X Z, WANG Z J, et al. Preparation and characterization of (1-x)Pb(Lu1/2Nb1/2)O3-xPbTiO3 binary ferroelectric ceramics with high curie temperature. Materials Letters, 2012, 84: 1-4.
[14]	HE C, WANG Z J, LI X Z, et al. Synthesis, structure and electric properties of Pb(Yb1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 ternary ceramics. J. Phys. D: Appl. Phys. , 2012, 45: 105305-1-3.
[15]	HE C, WANG Z J, LI X Z, et al. Ferroelectric ternary solid solution of Pb(Mg1/3Nb2/3)O3-PbSnO3-PbTiO3 with morphotropic phase boundary. Ceram. Int., 2013, 39: 853-856.
[16]	STERNBERG A, SHEBANOVS L. BIRKS E, et al. Effects of structure ordering, structure defects and external conditions on properties of complex ferroelectric perovskites. Ferroelectrics, 1998, 217(1): 307-317.
[17]	STEMBERG A, SHEBANOVS L, ANTONOVA M, et al. New high piezoelectric coupling PLuNT binary system ceramics. Nanostructured Materials, 1999, 12: 645-648.
[18]	LEJEUNE M, BOILOT J P. Formaton mechanism and ceramics process of the ferroelectric perovskites: Pb(Mg1/3Nb2/3)O3 and Pb(Fe1/2Nb1/2)O3. Ceram. Int., 1982, 8: 99-103.
[19]	BOUQUIN O, LEJEUNE M, BOILOT J P. Formation of the perovskite phase in the PMN-PT system. J. Am. Ceram. Soc., 1991, 74: 1152-1157.
[20]	JANG S J, UCHINO K, NOMURA S, et al. Electrostrictrive behavior of lead magnesium niobate based ceramic dielectrics. Ferroelectrics, 1980, 27: 31-35.
[21]	JONES S L, NORMAN C J. Dehydration of hydrous zirconia with methanol. J. Am. Ceram. Soc., 1988, 71: 190-191.
[22]	SWARTZ S L, SHROUT T R. Fabricaton of perovskite lead magnesium niobate. Mat. Res. Bull., 1982, 17: 1245-1249.
[23]	CHAPUT F, BOILOT J P, LEJEUNE M, et al. Low temperature route to lead magnesium niobate. J. Am. Ceram. Soc., 1989, 72(8): 1335-1340.

新型铁电固溶体铌镥酸铅-铌镁酸铅-钛酸铅的制备与表征

Preparation and Characterization of A New Ferroelectric Ternary Solid Solution Pb(Lu_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃

RichHTML

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 8

参考文献 23

相关文章 15

编辑推荐

Metrics

本文评价

[1]	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.
[2]	张家维, 陈宁, 程原, 王博, 朱建国, 金城. Bi₄Ti₃O₁₂铋层状压电陶瓷的A/B位掺杂及其电学性能[J]. 无机材料学报, 2025, 40(6): 690-696.
[3]	吴琼, 沈炳林, 张茂华, 姚方周, 邢志鹏, 王轲. 铅基织构压电陶瓷研究进展[J]. 无机材料学报, 2025, 40(6): 563-574.
[4]	周阳阳, 张艳艳, 于子怡, 傅正钱, 许钫钫, 梁瑞虹, 周志勇. 通过Bi³⁺自掺杂增强CaBi₄Ti₄O₁₅基陶瓷压电性能[J]. 无机材料学报, 2025, 40(6): 719-728.
[5]	姜昆, 李乐天, 郑木鹏, 胡永明, 潘勤学, 吴超峰, 王轲. PZT陶瓷的低温烧结研究进展[J]. 无机材料学报, 2025, 40(6): 627-638.
[6]	谌广昌, 段小明, 朱金荣, 龚情, 蔡德龙, 李宇航, 杨东雷, 陈彪, 李新民, 邓旭东, 余瑾, 刘博雅, 何培刚, 贾德昌, 周玉. 直升机特定结构先进陶瓷材料研究进展与应用展望[J]. 无机材料学报, 2025, 40(3): 225-244.
[7]	高天宇, 刘东, 赵思雪, 邓伟, 张波萍, 朱立峰. 温度稳定性优异的K_0.5Na_0.5NbO₃基压电陶瓷及其1-3型换能器[J]. 无机材料学报, 2025, 40(3): 297-304.
[8]	黄建锋, 梁瑞虹, 周志勇. W/Cr共掺杂对CaBi₂Nb₂O₉陶瓷晶体结构及电学性能的影响[J]. 无机材料学报, 2024, 39(8): 887-894.
[9]	彭萍, 谭礼涛. CuO掺杂(Ba,Ca)(Ti,Sn)O₃陶瓷的结构与压电性能[J]. 无机材料学报, 2024, 39(10): 1100-1106.
[10]	邹凯, 张文斌, 关胜, 孙海轶, 彭凯伦, 邹家杰, 李学红, 王成, 冷雨欣, 梁瑞虹, 周志勇. 压电式高温液滴喷射元件研制[J]. 无机材料学报, 2023, 38(8): 987-988.
[11]	孔国强, 冷明哲, 周战荣, 夏池, 沈晓芳. Sb掺杂O3型Na_0.9Ni_0.5Mn_0.3Ti_0.2O₂钠离子电池正极材料[J]. 无机材料学报, 2023, 38(6): 656-662.
[12]	南博, 臧佳栋, 陆文龙, 杨廷旺, 张升伟, 张海波. 增材制造压电陶瓷研究进展[J]. 无机材料学报, 2022, 37(6): 585-595.
[13]	田俊亭, 李晓兵, 丁伟艳, 聂生东, 梁柱. 软模板法制备高频超声换能器用1-3复合压电材料[J]. 无机材料学报, 2022, 37(5): 507-512.
[14]	王新健, 朱逸璇, 张鹏, 杨文龙, 王挺, 郇宇. (Ba_0.85Ca_0.15)(Ti_0.9Zr_0.1-_xSn_x)O₃无铅压电陶瓷的相结构与压电性能[J]. 无机材料学报, 2022, 37(5): 513-519.
[15]	刘凯, 孙策, 史玉升, 胡佳明, 张庆庆, 孙云飞, 章嵩, 涂溶, 闫春泽, 陈张伟, 黄尚宇, 孙华君. 增材制造压电陶瓷的现状与展望[J]. 无机材料学报, 2022, 37(3): 278-288.

新型铁电固溶体铌镥酸铅-铌镁酸铅-钛酸铅的制备与表征

Preparation and Characterization of A New Ferroelectric Ternary Solid Solution Pb(Lu1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3

RichHTML

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 8

参考文献 23

相关文章 15

编辑推荐

Metrics

本文评价

Preparation and Characterization of A New Ferroelectric Ternary Solid Solution Pb(Lu_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃