硅酸盐学报

Pb（Sc_1/2Nb_1/2）O₃-Pb（Mg_1/3Nb_2/3）O₃-PbTiO₃织构陶瓷的电学性能和热稳定性

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陈怡菲 ¹ , 惠增哲 ¹ , 郭菲菲 ¹ , 龙伟 ¹ , 周宏桥 ¹ , 高建金 ² , 董文强 ³

硅酸盐学报 | 研究论文 2024,52(12): 3789-3798

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硅酸盐学报 |研究论文 2024 , 52 (12) : 3789 -3798

Pb（Sc_1/2Nb_1/2）O₃-Pb（Mg_1/3Nb_2/3）O₃-PbTiO₃织构陶瓷的电学性能和热稳定性

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陈怡菲¹, 惠增哲¹, 郭菲菲¹, 龙伟¹, 周宏桥¹, 高建金², 董文强³

作者信息

^1．西安工业大学材料与化工学院，西安 710021

^2．长安大学电子与控制工程学院，西安 710064

^3．西安工业大学机电工程学院，西安 710021

通讯作者:

惠增哲（1965—），男，博士，教授。

郭菲菲（1985—），女，博士，副教授。

作者简介:

陈怡菲（1994—），女，博士研究生。

Electrical Properties and Thermal Stability of Pb(Sc_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃ Textured Ceramics

Yifei CHEN¹, Zengzhe HUI¹, Feifei GUO¹, Wei LONG¹, Hongqiao ZHOU¹, Jianjin GAO², Wenqiang DONG³

Affiliations

^1.School of Materials and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China

^2.School of Electronics and Control Engineering, Chang'an University, Xi'an 710064, China

^3.School of Mechanical and Electrical Engineering, Xi'an Technological University, Xi'an 710021, China

Corresponding Author:

HUI Zengzhe (1965-), male, Ph.D., Professor; E-mail: zzhxi@xatu.edu.cn;

GUO Feifei (1985-), female, Ph.D., Associate Professor. guofeifei19850106@163.com

CHEN Yifei (1994-), female, Doctoral candidate. E-mail: C18729048581@163.com

出版时间: 2024-12-20 doi: 10.14062/j.issn.0454-5648.20240437

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摘要

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采用BaTiO₃（BT）片状微晶制备了［001］取向的0.29PSN-0.39PMN-0.32PT（0.29Pb（Sc_1/2Nb_1/2）O₃-0.39Pb（Mg_1/3Nb_2/3）O₃-0.32PbTiO₃）织构陶瓷。制备了不同模板含量的织构陶瓷，并在织构度、微观结构以及压电、铁电和介电性能方面进行了比较。在PSN-PMN-PT织构陶瓷中，在3%（体积分数）BaTiO₃模板下实现了高达98.6%的［001］织构度，并且获得了高的压电性能（d₃₃= 816 pC/N，d₃₃^* = 1 080 pm/V）和高Curie温度（T_c = 185 ℃），这远远优于随机取向的陶瓷。此外，与具有相近压电常数的铅基陶瓷相比，织构化PSN-PMN-PT陶瓷表现出显著改善的热稳定性。高质量的织构化三元陶瓷在新一代高性能、宽温度范围的机电器件中具有广阔的应用前景。

关键词

织构陶瓷 / 铌钪酸铅-铌镁酸铅-钛酸铅 / 压电性能 / 热稳定性

Abstract

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Introduction

As a core element of the sensor, the piezoelectric constant and dielectric constant of piezoelectric materials determine the sensitivity of the sensor. Piezoelectric materials with a high performance and a high stability are urgently needed. The electrical properties of perovskite ferroelectrics are closely related to the crystal orientation. Growing single crystals is thus an effective way to improve the electrical properties of perovskite ferroelectrics. However, the practical application of single crystals is limited due to their relatively high cost, low trigonal-rhombohedral phase transition temperature, and insufficient composition uniformity in inconsistent melting. To solve the above-mentioned single crystal application problems, the template grain growth (TGG) method for preparing textured ceramics is considered as one of the most promising methods.

In this paper, a PSN-PMN-PT ternary solid solution piezoelectric material was prepared, and the [001] oriented growth of ceramics by TGG method was analyzed. In addition, the influence of template content on the phase structure, micromorphology, electrical properties and temperature stability of textured ceramics was also discussed.

Methods

Oxide raw materials were mixed in stoichiometric ratios and pre-sintered at 750 ℃ for 2 h to form a pure perovskite structure. The [001] oriented BaTiO₃(BT) microcrystals were added as templates into a uniform slurry with 0.29Pb(Sc_1/2Nb_1/2)O₃-0.39Pb(Mg_1/3Nb_2/3)O₃-0.32PbTiO₃ matrix powder, solvent, dispersant, plasticizer, and binder, and then ground in a ball mill. The BT templates with x of 0, 1%, 2%, 3%, and 4% were added into the slurry. Afterwards, the slurry was cast via controlling the height of the scraper and the speed of the substrate. The dried raw embryo tapes were cut, stacked, and kept at 550 ℃ for 2 h to remove organics. Finally, the samples were sintered at 1 270 ℃ for 9 h.

The phase structure of the random and textured ceramics was determined by X-ray diffraction. The microstructure of the ceramics was characterized by scanning electron microscopy. To measure the electrical properties, the samples were coated with a silver paste and sintered at 550 ℃ for 40 min to form electrodes and then polarized in silicone oil at 25 kV/cm for 15 min. The piezoelectric coefficient d₃₃ was measured using a model ZJ-6A quasi-static d₃₃ tester. The temperature dependence of the dielectric constant ε_r and dielectric loss tan δ was determined by a model E4980A LCR meter. The polarization electric field (P-E) curve and the strain electric field (S-E) curve were analyzed by a model TF Analyzer 2000E ferroelectric test system. For the determination of temperature stability, the samples were annealed at high temperatures for 30 min and then tested for d₃₃ at room temperature.

Results and discussion

From the XRD analysis, BaTiO₃ as a template can effectively improve the [001] orientation of PSN-PMN-PT ceramics and achieve a high degree of [001] preferred orientation growth. The F₀₀₁ of all the textured ceramics is 97%-99%, among which the F₀₀₁ of 3%(volume fraction) BT-PSN-PMN-PT textured ceramics is 98.6%. From the scanning of the textured ceramics, the template exists stably and is well arranged in the matrix ceramics, which is a fundamental reason why the textured ceramics have a high texture degree. The piezoelectric constant of 3% BT textured PSN-PMN-PT ceramics (816 pC/N) is greater than that of random PSN-PMN-PT ceramics (402 pC/N). Based on the analysis of the dielectric loss at room temperature, the dielectric loss of the textured ceramics reduces to 0.008, which is lower than that of randomly oriented ceramics and most soft piezoelectric ceramics (i.e., >0.020). The high d₃₃, S_positive, S_total, and d₃₃^* of textured ceramics are all related to the "4R" domain engineering state. Only a transition from tetragonal to cubic phase occurs in the textured ceramics, indicating that the textured ceramics have a good temperature stability. The results of annealed piezoelectric constant test show that the d₃₃ change of 3% BT-PSN-PMN-PT ceramics at 30-160 ℃ is only 12%, further proving a good temperature stability of textured ceramics.

Conclusions

The [001] oriented texture PSN-PMN-PT ceramic with a texture degree F₀₀₁ of 98.6% was synthesized by the TGG method, obtaining the high piezoelectric properties (i.e., d₃₃ = 816 pC/N, d₃₃^* = 1 080 pm/V) and high Curie temperature (i.e., T_C = 185 ℃). This enhanced piezoelectric response was attributed to the grain orientation characteristics. Furthermore, the 3% BT-PSN-PMN-PT texture ceramic exhibited an improved temperature stability, compared with previously reported lead-based ceramics with the similar piezoelectric constants. These results showed that the textured PSN-PMN-PT ceramics had high piezoelectric properties and good temperature stability, having the application prospects of textured ceramics in electromechanical devices.

Key words

texture ceramics / Pb(Sc_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃-Ferroelectric / piezoelectric properties / thermal stability

引用本文

陈怡菲, 惠增哲, 郭菲菲, 龙伟, 周宏桥, 高建金, 董文强. Pb（Sc_1/2Nb_1/2）O₃-Pb（Mg_1/3Nb_2/3）O₃-PbTiO₃织构陶瓷的电学性能和热稳定性. 硅酸盐学报, 2024 , 52 (12) : 3789 -3798 . DOI: 10.14062/j.issn.0454-5648.20240437

Yifei CHEN, Zengzhe HUI, Feifei GUO, Wei LONG, Hongqiao ZHOU, Jianjin GAO, Wenqiang DONG. Electrical Properties and Thermal Stability of Pb(Sc_1/2Nb_1/2)O₃-Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃ Textured Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (12) : 3789 -3798 . DOI: 10.14062/j.issn.0454-5648.20240437

基金

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国家自然科学基金(11704249)

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2024年第52卷第12期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240437

接收时间：2024-07-01
首发时间：2026-10-22
出版时间：2024-12-20

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收稿日期：2024-07-01
修回日期：2024-08-14

基金

国家自然科学基金(11704249)

作者信息

^1．西安工业大学材料与化工学院，西安 710021

^2．长安大学电子与控制工程学院，西安 710064

^3．西安工业大学机电工程学院，西安 710021

通讯作者:

惠增哲（1965—），男，博士，教授。

郭菲菲（1985—），女，博士，副教授。

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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