高于居里温度极化的硬性PZT压电陶瓷的制备及叠层驱动器性能研究

doi:10.15541/jim20240161

无机材料学报 ›› 2024, Vol. 39 ›› Issue (10): 1091-1099.DOI: 10.15541/jim20240161 CSTR: 32189.14.10.15541/jim20240161

高于居里温度极化的硬性PZT压电陶瓷的制备及叠层驱动器性能研究

江强¹^,²(), 施立志¹, 陈政燃¹, 周志勇¹, 梁瑞虹¹()

1.中国科学院上海硅酸盐研究所, 中国科学院无机功能材料与器件重点实验室, 上海 200050
2.中国科学院大学材料科学与光电技术学院, 北京 100049

收稿日期:2024-04-02 修回日期:2024-05-05 出版日期:2024-10-20 网络出版日期:2024-05-16
通讯作者: 梁瑞虹, 研究员. E-mail: liangruihong@mail.sic.ac.cn
作者简介:江强(1997-), 男, 硕士研究生. E-mail: jiangqiang2009@126.com
基金资助:
国家重点研发计划(2022YFF0709702);国家自然科学基金(U2241242)

Preparation and Properties of Hard PZT Piezoelectric Ceramics Poled above Curie Temperature and Multilayer Actuators

JIANG Qiang¹^,²(), SHI Lizhi¹, CHEN Zhengran¹, ZHOU Zhiyong¹, LIANG Ruihong¹()

1. Key Laboratory of Inorganic Functional Materials and Devices of CAS, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2024-04-02 Revised:2024-05-05 Published:2024-10-20 Online:2024-05-16
Contact: LIANG Ruihong, professor. E-mail: liangruihong@mail.sic.ac.cn
About author:JIANG Qiang (1997-), male, Master candidate. E-mail: jiangqiang2009@126.com
Supported by:
National Key R&D Program of China(2022YFF0709702);National Natural Science Foundation of China(U2241242)

摘要/Abstract

摘要：

压电叠层驱动器具有低驱动电压、大位移的特点, 被广泛应用于诸多领域。作为目前压电叠层驱动器中最常使用的材料, 软性锆钛酸铅(PZT)陶瓷较大的介电常数和损耗往往会导致较高的功耗和发热量, 进而影响驱动器的疲劳特性和稳定性。为了制备出低发热量、适用于压电叠层驱动器的压电陶瓷, 本工作选取Mn掺杂(摩尔分数)的Pb(Sb_1/2Nb_1/2)_0.02Zr_0.51Ti_0.47O₃-0.6%MnCO₃(PSN-PZT)硬性压电陶瓷作为基体材料, 通过掺入一定含量的Li₂CO₃烧结助剂来降低陶瓷的烧结温度, 并采用高于居里温度极化工艺进一步提升陶瓷的电学性能。最后采用该材料, 利用流延工艺制备出压电叠层驱动器, 并与相同工艺制备的Pb(Mg_1/3Nb_2/3)_0.25(Ti_0.48Zr_0.52)_0.75O₃(PMN-PZT)驱动器进行比较。结果显示,Li₂CO₃通过引入液相烧结的方式将PSN-PZT陶瓷烧结温度降低至1050 ℃。当Li₂CO₃含量为0.1%(质量分数)时, 高于居里温度极化的PSN-PZT陶瓷电学性能最优, 其压电系数(d₃₃)和2 kV/mm电场下的单极应变分别为388 pC/N和0.13%。在200 Hz下, PSN-PZT驱动器温升比PMN-PZT驱动器低大约20 ℃, 且经过5×10⁶次循环后应变仅降低6%。这表明Li₂CO₃低温烧结的PSN-PZT陶瓷不仅具备不错的压电性能, 而且在发热和疲劳特性方面有较大优势, 在大功率、高频等苛刻工况中有潜在的应用前景。

关键词: 硬性PZT, 低温烧结, 压电叠层驱动器, 温升, 疲劳特性

Abstract:

Piezoelectric multilayer actuators feature large displacement generation at a relatively low driving voltage and are widely used in various fields. As the most commonly used material in multilayer actuators, soft lead zirconate titanate (PZT) ceramics have higher dielectric constant and loss, which often lead to higher power consumption and heat generation that in turn affect fatigue characteristics and stability of piezoelectric multilayer actuators. In this work, Mn-doped (in mole fraction) Pb(Sb_1/2Nb_1/2)_0.02Zr_0.51Ti_0.47O₃-0.6%MnCO₃(PSN-PZT) hard ceramic was selected as base material in order to prepare piezoelectric ceramics that have low heat generation and are suitable for the application of piezoelectric multilayer actuator. Certain amount of Li₂CO₃ was doped as sintering aid for lowering sintering temperature of ceramics, and above-Curie-temperature polarization was utilized to enhance electric properties of ceramics. Eventually, multilayer actuator composed of this material was fabricated via tape-casting process and compared with Pb(Mg_1/3Nb_2/3)_0.25(Ti_0.48Zr_0.52)_0.75O₃ (PMN-PZT) actuator prepared with the same parameters. The results indicated that the sintering temperature of PSN-PZT ceramic was decreased to 1050 ℃ due to Li₂CO₃ sintering aid, which introduced liquid sintering during the sintering process. PSN-PZT ceramics poled above the Curie temperature obtained optimal electric performance with 0.1% (in mass) Li₂CO₃ doping, and the piezoelectric coefficient (d₃₃) and unipolar strain at 2 kV/mm reached 388 pC/N and 0.13%, respectively. The results of temperature rise and strain degradation of both multilayer actuators indicated that the temperature rise of hard PSN-PZT actuator was about 20 ℃ lower than that of PMN-PZT actuator under 200 Hz and the strain decreased by 6% after 5×10⁶ cycles. It indicates that PSN-PZT ceramics with Li₂CO₃ doping for lowering sintering temperature have some advantages in heat generation and fatigue characteristic while having descent piezoelectric properties, which endows it an important potential application in high-power, high-frequency and other demanding working conditions.

Key words: hard PZT, low-temperature sintering, piezoelectric multilayer actuator, temperature rise, fatigue characteristic

中图分类号:

TQ174

江强, 施立志, 陈政燃, 周志勇, 梁瑞虹. 高于居里温度极化的硬性PZT压电陶瓷的制备及叠层驱动器性能研究[J]. 无机材料学报, 2024, 39(10): 1091-1099.

JIANG Qiang, SHI Lizhi, CHEN Zhengran, ZHOU Zhiyong, LIANG Ruihong. Preparation and Properties of Hard PZT Piezoelectric Ceramics Poled above Curie Temperature and Multilayer Actuators[J]. Journal of Inorganic Materials, 2024, 39(10): 1091-1099.

图/表 13

图1 不同烧结温度和Li2CO3含量的PSN-PZT陶瓷样品密度

Fig. 1 Densities of PSN-PZT samples with variation of sintering temperature and Li2CO3 addition

图2 不同Li2CO3含量的PSN-PZT陶瓷样品的XRD图谱

Fig. 2 XRD patterns of PSN-PZT samples with different Li2CO3 additions (a) 2θ=10°-70°; (b) 2θ=43°-47°

图3 不同Li2CO3含量的PSN-PZT陶瓷样品表面形貌及晶粒尺寸分布图

Fig. 3 Surface morphologies and distributions of grain sizes of PSN-PZT samples with different Li2CO3 additions (a) 0.05%; (b) 0.1%; (c) 0.2%; (d) 0.3%; (e) 0.5%. M: Mean particle diameter

图4 PSN-PZT陶瓷样品的性能随烧结温度和Li2CO3含量的变化曲线

Fig. 4 Change of properties of PSN-PZT samples with Li2CO3 addition and sintering temperature (a) Piezoelectric coefficient d33; (b) Unipolar strain at 2 kV/mm

图5 PSN-PZT陶瓷样品机电耦合系数kp、机械品质因子Qm和介电损耗tanδ随Li2CO3含量的变化图

Fig. 5 kp, Qm, and tanδ of PSN-PZT samples with different Li2CO3 additions

图6 常规极化和高于居里温度极化不同Li2CO3含量PSN-PZT陶瓷样品的性能变化图

Fig. 6 Properties of PSN-PZT samples with different Li2CO3 additions under conventional polarization and above-Curie-temperature polarization (a) Piezoelectric coefficient d33; (b) Unipolar strain

图7 常规极化和高于居里温度极化PSN-PZT陶瓷样品铁电畴结构图(a, b)和相位分布图(c)

Fig. 7 Diagrams of domain structures (a, b) of PSN-PZT samples under conventional polarization (a) and above-Curie-temperature polarization (b), and their corresponding distributions of phases (c)

表1 本研究及文献报道的压电陶瓷性能对比

Table 1 Comparison of properties between piezoelectric ceramics in this work and literatures

Sample	Sintering temperature/℃	d₃₃/(pC·N^-1)	k_p	tanδ/%	Strain/%@2 kV/mm	Ref.
PSN-PZT-MnCO₃-Li₂CO₃	1050	388	0.66	0.30	0.13	This Work
PZT	1250	210	0.52	1.2	-	[29]
PZT-Mn	1230	180	0.62	0.80	-	[30]
PMS-PZT	1240	374	0.60	0.41	-	[31]
PZT4	>1200	289	0.70	0.4	0.02	[32]
PZT-PbO-WO₃	~1100	-	0.25	0.35	-	[19]
PZT-ZnO	1150	240	0.50	1.2	-	[33]
PBaSrZT-LiBiO₂-CuO-MnCO₃	900	255	0.58	0.58	-	[34]

图8 硬性PSN-PZT压电叠层驱动器(右)和PMN-PZT压电叠层驱动器(左)照片

Fig. 8 Photographs of the hard PSN-PZT multilayer actuator (right) and the PMN-PZT multilayer actuator (left)

图9 硬性PSN-PZT(a)和PMN-PZT(b)压电叠层驱动器的SEM照片

Fig. 9 SEM images of the hard PSN-PZT actuator (a) and PMN-PZT actuator (b)

表2 硬性PSN-PZT和PMN-PZT驱动器的介电性能

Table 2 Dielectric properties of the hard PSN-PZT and PMN-PZT actuators

Sample	C/μF	tanδ/%
Hard PSN-PZT actuator	0.32	0.45
PMN-PZT actuator	0.71	2.29

图10 150 V驱动电压下硬性PSN-PZT和PMN-PZT压电叠层驱动器在不同频率下的温升

Fig. 10 Temperature rise of the hard PSN-PZT actuator and PMN-PZT actuator under 150 V driving voltage and various frequencies (a) 50 Hz; (b) 100 Hz; (c) 150 Hz; (d) 200 Hz

图11 硬性PSN-PZT和PMN-PZT压电叠层驱动器在150 V驱动电压和200 Hz频率下的应变衰减

Fig. 11 Strain degradation of the hard PSN-PZT actuator and PMN-PZT actuator under 150 V driving voltage and 200 Hz driving frequency

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高于居里温度极化的硬性PZT压电陶瓷的制备及叠层驱动器性能研究

Preparation and Properties of Hard PZT Piezoelectric Ceramics Poled above Curie Temperature and Multilayer Actuators

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