烧结方式对(K,Na,Li)(Nb,Sb,Ta)O3压电陶瓷的微观结构和物理性能的影响

doi:10.15541/jim20180447

摘要/Abstract

摘要：

(K,Na)NbO₃基陶瓷(KNLNST陶瓷)是一类很有发展潜力的无铅压电材料, 目前对其进行两步烧结相关的研究还很少。本工作分别采用普通烧结(Conventional Sintering, CS)和两步烧结(Two-step Sintering, TSS)制备了(K_0.4425Na_0.52Li_0.0375)(Nb_0.8825Sb_0.08Ta_0.0375)O₃陶瓷, 并进行微观结构与物性的对比研究。TSS可将(K,Na)NbO₃基陶瓷的相对密度ρ°由CS时的95.0%提高至97.0%, 压电系数d₃₃由CS时的363 pC/N增大到387 pC/N。两种烧结方式制备的KNLNST陶瓷的微观组织结构和电畴结构有着很大的差异。KNLNST-CS陶瓷的晶粒尺寸较小而且分布较为均匀, 极化后多数晶粒的电畴图案为简单的平行条纹。KNLNST-TSS陶瓷的晶粒尺寸则大小分布不均匀, 极化后许多大晶粒中呈现带状条纹内部又存在着精细的平行条纹的电畴图案。

关键词: (K,Na)NbO₃基陶瓷, 两步烧结, 压电性能, 相变, 微观组织结构, 电畴结构

Abstract:

(K,Na)NbO₃-based ceramics (KNLNST ceramics) are a very promising type of lead-free piezoelectric materials. However, only limited studies were reported on them prepared by two-step sintering. Here, a comparison study was performed between two kinds of (K_0.4425Na_0.52Li_0.0375)(Nb_0.8825Sb_0.08Ta_0.0375)O₃ ceramics that were prepared by either conventional sintering (CS) or two-step sintering (TSS). It was found that TSS largely increases the relative density ρ° and piezoelectric coefficient d₃₃ from 95.0% and 363 pC/N of CS to 97.0% and 387 pC/N, respectively. KNLNST ceramics prepared by two kinds of sintering methods show significant differences between microstructure and domain structure. The KNLNST-CS ceramic has small grain sizes but distributed uniformly, and their domain patterns in most grains are simply a group or groups of parallel stripes. In contrast, the KNLNST-CS ceramic has a non-uniform grain-size distribution, with many large grains displaying broad bands, and existing fine strips.

Key words: (K,Na)NbO₃-based ceramics, two-step sintering, piezoelectric property, phase transitions, microstructure, domain structure

中图分类号:

TQ174

张晓晨, 王雪梅, 王春雷. 烧结方式对(K,Na,Li)(Nb,Sb,Ta)O₃压电陶瓷的微观结构和物理性能的影响[J]. 无机材料学报, 2019, 34(7): 721-726.

ZHANG Xiao-Chen, WANG Xue-Mei, WANG Chun-Lei. Influences of Sintering Methods on Microstructure and Physical Property of (K,Na,Li)(Nb,Sb,Ta)O₃ Piezoelectric Ceramics[J]. Journal of Inorganic Materials, 2019, 34(7): 721-726.

图/表 6

表1 不同烧结条件下制备的KNLNST陶瓷的物理性能

Table 1 Physical property of KNLNST ceramics prepared under different sintering conditions

Sample	Sintering conditions	ρ/(g?cm^-3)	d₃₃/(pC?N^-1)	k_p
CS	1090 ℃, 5 h	4.40	363	0.48
TSS-1	1130 ℃/1050 ℃, 4 h	4.43	369	0.47
TSS-2	1140 ℃/1050 ℃, 4 h	4.44	370	0.43
TSS-3	1150 ℃/1040 ℃, 4 h	4.36	358	0.44
TSS-4	1150 ℃/1050 ℃, 4 h	4.47	387	0.49
TSS-5	1150 ℃/1060 ℃, 4 h	4.42	378	0.48
TSS-6	1160 ℃/1050 ℃, 4 h	4.35	379	0.46

图1 (a)各种未极化状态的KNLNST陶瓷于室温下的XRD图谱, (b) 2θ为46.0°附近的部分放大谱图。

Fig. 1 (a) Room-temperature XRD patterns of the various unpoled KNN ceramics and (b) enlarged parts in (a)

图2 未极化状态的两种代表性KNLNST陶瓷在升温过程中测试得到的介电温谱, 插图为正交相至四方相的相变的介电温谱峰的部分放大图

Fig. 2 Temperature dependence of dielectric permittivity ε' of two representative unpoled KNLNST ceramics, prepared by conventional sintering and two-step sintering, respectively. Inset is partially enlarged curves of dielectric temperature peak of the phase transition from orthorhombic to tetragonal phase

图3 未极化状态的两种代表性KNLNST陶瓷的电畴图案的典型扫描电镜照片

Fig. 3 Typical SEM images of domain patterns observed in the two unpoled representative KNLNST ceramics (a) KNLNST-CS ceramic; (b) Partially enlarged view of (a); (c) and (d) KNLNST-TSS ceramic, corresponding to different locations of the same specimen

图4 极化处理的KNLNST-CS陶瓷的微观组织结构和电畴图案的典型扫描电镜照片, (b)是(a)的部分放大照片

Fig. 4 (a) Typical SEM image of microstructure and domain pattern of a poled KNLNST-CS ceramic, (b) a partially enlarged image in (a)

图5 极化处理的KNLNST-TSS陶瓷的微观结构和电畴图案的典型扫描电镜照片

Fig. 5 Typical SEM images of microstructure and domain patterns observed in a poled KNLNST-TSS ceramic. (a-c) Correspond to different positions of the same sample; (d) A partial enlarged image in (c)

参考文献 25

[1]	GAO Y, ZHANG J L, ZONG X J , et al. Extremely temperature- stable piezoelectric properties of orthorhombic phase in (K,Na) NbO₃- based ceramics. J. Appl. Phys., 2010, 107(7): 074101-1-5.
[2]	SAITO Y, TAKAO H, TANI T , et al. Lead-free piezoceramics. Nature, 2004,432(4):84-87. DOI
[3]	GUO Y P, KAKIMOTO K, OHSATO H . Phase transitional behavior and piezoelectric properties of (Na_0.5K_0.5)NbO₃-LiNbO₃ ceramics. Appl. Phys. Lett., 2004,85(18):4121-4123. DOI URL
[4]	GUO Y P, KAKIMOTO K, OHSATO H .( Na_0.5K_0.5)NbO₃-LiTaO₃ lead-free piezoelectric ceramics. Mater. Lett., 2005. 59(2/3):241-244. DOI URL
[5]	FU J, ZUO R Z, WANG X H , et al. Polymorphic phase transition and enhanced piezoelectric properties of LiTaO₃-modified (Na_0.52K_0.48)(Nb_0.93Sb_0.07)O₃ lead-free ceramics. J. Phys. D: Appl. Phys., 2009, 42(1): 012006-1-4.
[6]	GAO Y, ZHANG J L, QIN Y L , et al. Remarkably strong piezoelectricity of lead-free (K_0.45Na_0.55)_0.98Li_0.02(Nb_0.77Ta_0.18Sb_0.05)O₃ ceramic. J. Am. Ceram. Soc., 2011,94(9):2968-2973. DOI URL
[7]	ZHANG B Y, WU J G, CHENG X J , et al. Lead-free piezoelectrics based on potassium-sodium niobate with giant d₃₃. ACS Appl. Mater. Interfaces, 2013,5(16):7718-7725. DOI URL
[8]	WANG X P, WU J G, XIAO D Q , et al. Giant piezoelectricity in potassium-sodium niobate lead-free ceramics.[J]. Am. Chem. Soc., 2014,136(7):2905-2910. DOI URL
[9]	ZHENG T, WU J G, CHEN Q , et al. Composition-driven phase boundary and piezoelectricity in potassium-sodium niobate-based ceramics. ACS Appl. Mater. Interfaces, 2015,7(36):20332-20341. DOI URL
[10]	WU B, WU H J, WU J G , et al. Giant piezoelectricity and high Curie temperature in nanostructured alkali niobate lead-free piezoceramics through phase coexistence.[J]. Am. Chem. Soc., 2016,138(47):15459-15464. DOI URL
[11]	XU K, LI J, LÜ X , et al. Superior piezoelectric properties in potassium- sodium niobate lead-free ceramics. Adv. Mater., 2016,28(38):8519-8523. DOI URL
[12]	ZHANG M H, WANG K, DU Y J , et al. High and temperature- insensitive piezoelectric strain in alkali niobate lead-free perovskite.[J]. Am. Chem. Soc., 2017,139(10):3889-3895. DOI URL
[13]	JAEGER E, EGERTON L . Hot pressing of potassium-sodium niobates.[J]. Am. Ceram. Soc., 1962,45(5):209-213. DOI URL
[14]	ZHANG S J, LEE H J, MA C , et al. Sintering effect on microstructure and properties of (K, Na)NbO₃ ceramics. J. Am. Ceram. Soc., 2011,94(11):3659-3665. DOI URL
[15]	LI J F, WANG K, ZHANG B P , et al. Ferroelectric and piezoelectric properties of fine-grained Na_0.5K_0.5NbO₃ lead-free piezoelectric ceramics prepared by spark plasma sintering.[J]. Am. Ceram. Soc., 2006,89(2):706-709. DOI URL
[16]	ERIKSON M, YAN H X, VIOLA G , et al. Ferroelectric domain structures and electrical properties of fine-grained lead-free sodium potassium niobate ceramics.[J]. Am. Ceram. Soc., 2011,94(10):3391-3396. DOI URL
[17]	CHEN I W, WANG H X . Sintering dense nanocrystalline ceramics without final-stage grain growth. Nature, 2000,404(9):168-71. DOI
[18]	WANG X H, CHEN P L, CHEN I W . Two-step sintering of ceramics with constant grain-size.[J]. Am. Ceram. Soc., 2006,89(2):431-437. DOI URL
[19]	WANG X H, DENG X Y, BAI H L , et al. Two-step sintering of ceramics with constant grain-size, II: BaTiO₃ and Ni-Cu-Zn ferrite.[J]. Am. Ceram. Soc., 2006,89(2):438-443. DOI URL
[20]	FANG J, WANG X H, TIAN Z B , et al. Two-step sintering: an approach to broaden the sintering temperature range of alkaline niobate-based lead-free piezoceramics.[J]. Am. Ceram. Soc., 2010,93(11):3552-3555. DOI URL
[21]	PANG X M, QIU J H, ZHU K J , et al. ( K,Na)NbO₃-based lead-free piezoelectric ceramics manufactured by two-step sintering. Ceram. Int., 2012,38(3):2521-2527. DOI URL
[22]	WU J G, WANG Y M . Two-step sintering of new potassium sodium niobate ceramics: a high d₃₃ and wide sintering temperature range. Dalton Trans., 2014,43(34):12836-12841. DOI URL
[23]	ZHANG J L, QIN Y L, GAO Y , et al. Improvement of physical properties for KNN-based ceramics by modified two-step sintering.[J]. Am. Ceram. Soc., 2014,97(3):759-764. DOI URL
[24]	ARLT G, SASKO P . Domain configuration and equilibrium size of domains in BaTiO₃ ceramics.[J]. Appl. Phys., 1980,51(9):4956-496. DOI URL
[25]	JUAREZ R L, PERALTA O N, GARCÍA F G , et al. Ferroelectric domain structure of lead-free potassium-sodium niobate ceramics.[J]. Eur. Ceram. Soc., 2011,31(9):1861-1864. DOI URL

烧结方式对(K,Na,Li)(Nb,Sb,Ta)O₃压电陶瓷的微观结构和物理性能的影响

Influences of Sintering Methods on Microstructure and Physical Property of (K,Na,Li)(Nb,Sb,Ta)O₃ Piezoelectric Ceramics

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