晶粒尺寸对钙钛矿型压电陶瓷压电性能的影响

刘亦轩; 李昭; 汤浩正; 逯景桐; 李敬锋; 龚文; 王轲

doi:10.7498/aps.69.20201079

摘要

压电陶瓷能够通过正/逆压电效应实现电能与机械能之间的相互转化, 在电子信息、通信、传感等领域中具有广阔的应用前景. 压电陶瓷的压电性能对晶粒尺寸极为敏感, 其晶粒尺寸效应的研究受到了广泛关注. 本文对目前应用较多的几类钙钛矿型压电陶瓷, 包括钛酸钡、锆钛酸铅、铌酸钾钠、钛酸铋钠陶瓷的压电性能晶粒尺寸效应的研究与进展进行了综述; 总结了这些体系中晶粒尺寸的调控方法, 晶粒尺寸效应的表现规律, 同时回顾了相关物理模型与理论机制. 本文为系统理解压电性能的晶粒尺寸效应提供了指导, 并对压电陶瓷晶粒尺寸效应的未来研究方向做出了展望.

关键词:

Abstract

Piezoelectric ceramics is a versatile functional material that can realize interconversion between electrical energy and mechanical energy. As the electrical properties of piezoelectric ceramics are extremely sensitive to the grain size variation, the investigation of grain size effect has attracted much attention. In this paper, the recent research progress of the grain size effect on perovskite piezoelectric ceramics, including barium titanate (BT), lead zirconate titanate (PZT), potassium sodium niobate (KNN), and sodium bismuth titanate (BNT), is comprehensively reviewed. We especially focus on topics including feasible ways of fabricating piezoelectric ceramics with the desired grain sizes, the influence of the grain size effect on piezoelectric properties, and the corresponding physical mechanisms. This review would be beneficial to understanding the influence of the grain size effect on piezoelectric properties. The review concludes with the prediction of the further investigation on the grain size effect.

Keywords:

作者及机构信息

1.
清华大学材料学院, 新型陶瓷与精细工艺国家重点实验室, 北京　100084

2.
浙江清华长三角研究院, 先进陶瓷材料与器件研究中心, 嘉兴　314006

通信作者: 龚文, gongwen@tsinghua-zj.edu.cn ; 王轲, wang-ke@tsinghua.edu.cn

基金项目: 国家自然科学基金优秀青年科学基金(批准号: 51822206)、国家自然科学基金(批准号: 51972005)和科学挑战专题(批准号: TZ2018003)资助的课题

Authors and contacts

1.
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

2.
Advanced Ceramic Materials & Devices Research Center, Yangtze Delta Region Institute of Tsinghua University, Jiaxing 314006, China

Corresponding author: Gong Wen, gongwen@tsinghua-zj.edu.cn ; Wang Ke, wang-ke@tsinghua.edu.cn

Funds: Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 51822206), the National Natural Science Foundation of China (Grant No. 51972005), and the Science Challenge Project, China (Grant No. TZ2018003)

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施引文献

图 1 本综述行文结构与主要内容

Fig. 1. Outline of this review.

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图 2 (a) 六种烧结机制的扩散路径; (b) 烧结过程中致密化与晶粒长大示意图, 黑色曲线表示相对密度的变化

Fig. 2. (a) Six possible sintering mechanisms; (b) schematic view of the powder evolution at different stages during sintering; the black curve corresponds to the variation of relative density.

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图 3 BT压电陶瓷的晶粒形貌及晶粒尺寸对压电性能的影响　(a) BT陶瓷中不同尺寸(5 nm—100 μm)晶粒的扫描电子显微镜照片^{[27,30,52,54,63,93-95]}; (b) 典型BT陶瓷中ε与d₃₃^[98]; (c) 双向极化应变曲线; (d) 电滞回线; (e) 单向极化应变曲线随晶粒尺寸的变化^[99]

Fig. 3. The grain size effect on BT ceramics: (a) A wide range of grain size varying from 5 nm to 100 μm can be obtained in BT ceramics^{[27,30,52,54,63,93-95]}; (b) ε and d₃₃^[98]; (c) bipolar strain curve; (d) hysteresis loop; (e) unipolar strain loop measured as a function of grain size^[99].

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图 4 BT陶瓷中(a)畴尺寸、(b)介电常数ε及(c)压电常数d₃₃随晶粒尺寸的变化趋势; (d)高能X射线衍射图谱显示不同晶粒尺寸的BT陶瓷中平均晶面间距及(002)和(200)衍射峰强度在电场激励下的变化^[95]. “nano”, “micro”分别表示纳米级和微米级粒径的BT陶瓷粉体; “MS”, “HP”, “SPS”, “CS”和“TSS”分别表示微波烧结、热压烧结、等离子放电烧结、普通烧结及两步法烧结方法

Fig. 4. (a) Ferroelectric domain size, (b) ε, and (c) d₃₃ of BT ceramics summarized as a function of grain size; (d) extrinsic contribution was found maximized when the grain size of BT ceramic is around 2 μm in a high-energy XRD measurement^[95]. Note: “nano” and “micro” implies that the raw materials are nano-sized and micro-sized BaTiO₃ powders. “MS”, “HP”, “SPS”, “CS”, and “TSS” represents the microwave sintering, hot-pressing, spark plasma sintering, conventional sintering and two-step sintering, respectively.

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图 5 采用不同方法制得的BT陶瓷和带有不同相结构的BT陶瓷中, 晶粒尺寸效应呈现显著的不同　(a) 不同陶瓷粉体粒径和烧结方法制备BT陶瓷中d₃₃随晶粒尺寸的变化趋势^[28]; (b) Ba(Ti_0.96Sn_0.04)O₃ (BTS)和(Ba_0.85Ca_0.15)(Zr_0.1Ti_0.9)O₃ (BCZT)陶瓷中d₃₃与${d}_{33}^{{*}}$随晶粒尺寸的变化趋势^[119,120]

Fig. 5. Grain size effect can be different among BT ceramics with virous phase structure and by different preparation method: (a) Grain size dependence of d₃₃ of BT ceramics prepared by using different sintering method^[28]; (b) d₃₃ and $ {d}_{33}^{{*}} $ of Ba(Ti_0.96Sn_0.04)O₃, (Ba_0.85Ca_0.15)(Zr_0.1Ti_0.9)O₃ ceramics with different average grain sizes^[119,120].

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图 6 (a) 通过控制烧结温度获得晶粒尺寸不同的PZT陶瓷^[141]; (b) d₃₃和d₃₁随烧结温度的变化^[141]; (c) 晶粒尺寸效应的“空间电荷模型”^[132]

Fig. 6. (a) Grain size evolution in PZT ceramics as a function of sintering temperature^[141]; (b) piezoelectric coefficients of PZT ceramics measured as a function of sintering temperature^[141]; (c) illustration of the “space-charge model” ^[132].

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图 7 (a) PZT陶瓷的d₃₃, d₃₁, d_h和P_r与晶粒尺寸的关系^[25]; (b) PZT陶瓷的晶体四方性c/a与晶粒尺寸的关系^[25]; (c) 晶粒尺寸为3.9 μm和10.4 μm的PZT陶瓷的压电力显微镜(PFM)图^[150]; (d) 在细晶粒陶瓷的晶界上观察到比较强烈的局部矫顽场^[150]; (e) 不同晶粒尺寸PZT陶瓷样品经过2000次电循环去老化后测量的电致应变曲线(左), 双极化应变S_bip和P_r与晶粒尺寸的关系(右)^[150]

Fig. 7. (a) d₃₃, d₃₁, d_h, and P_r of PZT ceramics measured as a function of grain size^[25]; (b) c/a ratio measured as a function of grain size^[25]; (c) PFM amplitude images of PZT samples with average grain sizes of 3.9 μm and 10.4 μm^[150]; (d) stronger local coercive voltages can be obtained at the grain boundary in the fine grain^[150]; (e) bipolar strain and P_r of PZT ceramics measured as a function of grain size after de-aging^[150].

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图 8 (a) KNN-x Sr陶瓷中铁电畴尺寸随着晶粒尺寸的变化; 在总体畴壁密度提升的同时, 导电畴壁的数量也大幅增加^[170]; (b) KNN基陶瓷的铁电与压电性能随着晶粒尺寸的变化^[171]

Fig. 8. (a) Variation of domain size as a function of grain size in KNN-x Sr ceramics; an increased amount of conductive domain wall is observed as the grain size decreases^[170]; (b) evolution of ferroelectric and piezoelectric properties as a function of grain size in KNN-based ceramics^[171].

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图 9 (a) KNN陶瓷在高温烧结过程中产生液相导致的异常晶粒长大^[176]; (b) 通过改变烧结气氛可以抑制陶瓷中的异常晶粒长大^[177]; (c) 在KNN基陶瓷预烧粉末中观察到的异常晶粒长大^[178]

Fig. 9. (a) Abnormal grain growth in sintered KNN ceramics caused by the formation of the liquid phase at high temperature^[176]; (b) abnormal grain growth in sintered ceramics can be suppressed by controlling sintering atmosphere^[177]; (c) irregular grain growth observed in calcined KNN-based ceramic powder^[178].

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图 10 (a) 利用闪速烧结方式制备细晶粒BNT基陶瓷^[191]; (b) BNT基陶瓷中晶粒尺寸效应的物理模型^[196]; (c) BNT基陶瓷的压电性能随晶粒尺寸的变化^[197]

Fig. 10. (a) Fine-grained BNT-based ceramics prepared by flash sintering^[191]; (b) a qualitative model of the grain size effect in BNT-based ceramics^[196]; (c) variation of piezoelectric properties of BNT-based ceramics as a function of grain size^[197].

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表 1 不同粉体制备方法与最细粉体粒径

Table 1. Ceramic powders prepared by using different approaches.

分类	制备方法	最细粉体粒径/nm	文献
气相法	气相合成法	～100	[34]
固相法	固相反应合成法	100	[35]
	研磨-离心法	300	[36]
	高能球磨法	16	[37]
液相法	溶胶-凝胶法	38	[38]
	水热法	< 100	[39,40]
	微波水热法	30	[41]
	溶剂热合成法	20	[42]
	醇盐法	5	[43]
	水解法	100	[44]
	微乳液法	< 10	[45,46]
	低温直接合成法	< 10	[47,48]
其他方法	生物法	4	[49]
其他方法	微模板法	6	[50]

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表 2 不同烧结方法与晶粒尺寸

Table 2. Grain size variation among BT, PZT, and KNN ceramics prepared by using different sintering techniques.

烧结方法	晶粒尺寸/μm
烧结方法	BT	PZT	KNN
普通烧结	0.5—100^[51,52]	1—10^[25]	0.5—4^[53]
两步法烧结	0.005—8.6^[27,54]	1.6—6.4^[55]	1.6—3.8^[56,57]
热压烧结	0.3—1.2^[23]	2—5^[58]	~0.31^[57]
热等静压烧结	0.32—47.3^[59,60]	2—4^[61]	~0.34^[62]
微波烧结	~3.4^[63]	~2^[64]	< 1^[65]
等离子放电烧结	0.02—1.2^[52,66,67]	0.3—0.5^[68]	0.2—1^[69-71]
闪速烧结	0.3—0.4^[72]	^#0.168—1.4 (AC)^[73] 0.269—4 (DC)^[74]	^* < 0.5&4^[75]
注: ^#AC指在交流电场下的闪速烧结, DC指在直流电场下的闪速烧结; ^*晶粒尺寸呈现双峰分布.

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