铌酸钾钠基无铅压电陶瓷的高压电活性研究进展

邢洁; 谭智; 郑婷; 吴家刚; 肖定全; 朱建国

doi:10.7498/aps.69.20200288

摘要

以Pb(Zr_1–xTi_x)O₃ (PZT)为代表的铅基压电陶瓷因为具有良好的压电性能和机电耦合性能已被广泛应用于科技、工业、军事以及日常生活中. 但是, PZT基陶瓷中Pb的含量超过了60% (质量比), 在生产、使用及废弃处理过程中都会给人类生态环境造成严重损害. 因此, 发展无铅压电陶瓷已成为世界压电陶瓷研究的热点之一. 铌酸钾钠 (K_0.5Na_0.5)NbO₃ (KNN)无铅压电陶瓷因为具有较为优异的压电性能以及较高的居里温度, 被认为是最可能取代铅基压电陶瓷的材料体系之一. 经过研究者们的努力工作, 改性后的KNN基无铅压电陶瓷压电性能已经接近或超过了某些铅基压电陶瓷的性能. 本文综合介绍了具有高压电活性的KNN基无铅压电陶瓷国内外的研究进展, 重点阐述了高性能铌酸钾钠基无铅压电陶瓷制备工艺及相关理论基础的研究进展, 并就今后铌酸钾钠基无铅压电陶瓷研究发展的方向及前景提出建议.

关键词:

Abstract

Due to excellent piezoelectric properties and electromechanical coupling properties, lead-based piezoelectric ceramics represented by lead zirconate titanate Pb(Zr_xTi_1–x)O₃ (PZT) are widely used in science and technology, industry, military and daily life. However, the content of Pb in PZT-based ceramics exceeds 60% (mass ratio), which will cause serious damage to human ecological environment in the process of their production, use and waste treatment. Therefore, the development of lead-free piezoelectric ceramics has become one of the hot research spots. Potassium sodium niobate (K_0.5Na_0.5)NbO₃ (KNN) lead-free piezoelectric ceramics are considered as one of the most promising material systems to substitute for lead-based piezoelectric ceramics because of their good piezoelectric properties and higher Curie temperature. Through many years of researches, the piezoelectric properties of modified KNN based lead-free piezoelectric ceramics have approached to or even exceeded those of some lead-based piezoelectric ceramics. Combining with our relevant work, we comprehensively review the research progress of high piezoelectric activity of KNN based lead-free piezoelectric ceramics, especially focus on the research progress of high-performance potassium sodium niobate lead-free piezoelectric ceramics, preparation technology and related theoretical mechanisms. The future research direction and prospect of KNN-based lead-free piezoelectric ceramics are also presented.

Keywords:

作者及机构信息

四川大学材料科学与工程学院, 成都　610064

通信作者: 朱建国, nic0400@scu.edu.cn

基金项目: 国家级-国家自然科学基金(51932010)

Authors and contacts

College of Materials Science and Engineering, Sichuan University, Chengdu 610064, China

Corresponding author: Zhu Jian-Guo, nic0400@scu.edu.cn

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施引文献

图 1 (a) KNN基无铅压电陶瓷d₃₃的历史演变图; (b) KNN基无铅压电陶瓷与铅基陶瓷d₃₃对比图^{[11,12,34,37,43,45]}

Fig. 1. (a) Historical evolution in d₃₃ values of KNN-based ceramics as a function of time; (b) comparison of d₃₃ values among KNN-based ceramics and PZT materials^{[11,12,34,37,43,45]}.

下载: 全尺寸图片幻灯片

图 2 (a)正交相(K_0.5Na_0.5NbO₃陶瓷^[56,61]); (b)室温下O-T相界(KNNL-BZ-BNT陶瓷体系^[62], KNNSL-BNZ-BZ-MnO₂陶瓷体系^[63]); (c)室温下R-T/R-O-T相界KNN基陶瓷的畴结构(KNNS-BF-BNZ陶瓷体系^[43], KNNS-BNZ-BZ陶瓷体系^[34])

Fig. 2. Domain structures of KNN-based ceramcis with different phase boundaries at room temperature: (a) Orthorhombic (K_0.5Na_0.5NbO₃ ceramics^[56,61]); (b) O-T phase boundaries (KNNL-BZ-BNT ceramics^[62], KNNSL-BNZ-BZ-MnO₂ ceramics^[63]); (c) R-T/R-O-T phase boundaries (KNNS-BF-BNZ ceramics^[43], KNNS-BNZ-BZ ceramics^[34]).

下载: 全尺寸图片幻灯片

图 3 KNN基无铅压电陶瓷d₃₃与T_C对比图^[12,15-47]

Fig. 3. Comparison of d₃₃ and T_C values of KNN-based ceramics^[12,15-47].

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图 4 根据文献[120]重画的KNbO₃中Nb原子位置在(001)平面的投影示意图

Fig. 4. Projections of real Nb off-center displacements on the (001) plane redrawn from the Ref. [120].

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图 5 B位原子在单四方相与两相共存时沿[$ \overline{1} 01$]方向的能量分布示意图^[125]

Fig. 5. Energy distribution for B-site atom in single tetragonal phase and two-phase coexistence along [$ \overline{1} 01$] direction^[125].

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表 1 室温下具有O-T相界的KNN压电陶瓷性能

Table 1. Properties of KNN ceramics with O-T phase boundary at room temperature.

Material system	d₃₃/pC·N^–1	k_p	T_C/℃
KNLANT^[15]	252	0.454	438
KNLN-BCZT^[16]	180	0.34	425
KNN-KLN^[17]	121	0.39	—
KNLN-AS^[18]	230	0.39	430
KNLN-BNCT^[19]	262	0.36	～400
KNN-BC^[20]	165	0.40	～390
KNN-LS^[21]	280	0.494	364
KNN-BLZ^[22]	265	0.365	364
KNN-BC-BNH^[23]	272	0.47	333

下载: 导出CSV

表 2 室温下具有R-O-T相界的KNN压电陶瓷的性能

Table 2. Properties of KNN ceramics with R-O-T phase boundary at room temperature.

Material system	d₃₃/pC·N^–1	k_p	T_C /℃
KNN-BNZ-BG^[24]	312	0.44	341
KNN-BZ-BNZ^[25]	345	0.50	～260
KNN-NS-BNKZH^[26]	452	0.63	～270
KNNS-BNCZ^[27]	415	0.46	245
KNNTS-BNKZ^[28]	400	0.46	240
KNN-BNZN^[29]	318 ± 10	—	360
KNNS-BKZH^[30]	451	0.52	258
KNNS-BLKZ^[31]	385	—	245
KNNS-SZ-BNH^[32]	470 ± 5	0.51 ± 0.02	244
KNNS-BS-BNZ^[33]	～480	—	～225
KNNS-BNZ-BZ^[34]	610	0.58	241
KNNS-BNKZ-Fe-AS^[12]	650	—	～180

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表 3 室温下具有R-T相界的KNN压电陶瓷的性能

Table 3. Properties of KNN ceramics with R-T phase boundary at room temperature.

Material system	d₃₃ /pC·N^–1	k_p	T_C/℃
KNNS-BNZSn^[35]	465	0.51	240
KNNS-BZH^[36]	410	—	255
KNNS-BNKZ^[37]	490	0.46	227
KNNTS-BNKZ^[38]	460	0.40	～220
KNNS-BNH^[39]	419	0.45	242
KNNS-BKZS^[40]	430	—	243
KNNS-BNLCZ^[41]	485	0.48	227
KNNS-BNKH^[42]	525	—	～210
KNNS-BF-BNZ^[43]	550	—	237
KNNS-CZ-BKHT-MnO₂^[44]	425	0.49	215
KNNS-BZ-BKH^[45]	570 ± 10	—	～190
KNNS-BNZ-BF^[46]	511	0.515	269
KNANS-BNZ^[47]	440	0.50	250

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表 4 KNN基无铅压电陶瓷压电常数与畴结构尺寸

Table 4. Piezoelectric constant of KNN ceramics with domain size.

Material system	d₃₃ or $ {d}_{33}^{*} $	Domain size
KNNS-SZ-BAZ^[52]	487 pC/N	30—65 nm, 65—160 nm, 30—45 nm
KNNS-BZ-BNH^[48]	600 pm/V	10—100 nm
KNNS-BNKH^[42]	525 pC/N	10—30 nm
KNNS-BNKZ-Fe-AS^[12]	(650 ± 20) pC/N	2 nm
KNNS-BNZ-BZ^[34]	610 pC/N	50—70 nm
KNNT-BNKZ-CZ^[51]	482 pm/V	60 nm
KNNS-BZ-BNZ^[65]	300 pC/N	150 nm—1.0 μm
KNNS-CZ-BKH^[66]	550 pC/N	30—230 nm
KNNS-BNH^[67]	512 pC/N	100 nm
KNNS-SZ-BNZ^[68]	450 pC/N	50—200 nm
KNLNTS^[54]	455 pC/N	110—310 nm
KNNS-BNZ-BF^[46]	510 pC/N	< 1 μm
KNN-BNZ-MnO₂-Sb₂O₃^[69]	318 pC/N	< 1 μm
KNN-BI-BNZ^[57]	317 pC/N	～200 nm
KNNdNS-BNZ^[70]	400 pC/N	～ 1 μm

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表 5 同时具有高压电性能和高居里温度的KNN陶瓷体系

Table 5. The KNN-based ceramics with high piezoelectric constant and high Curie temperature.

Material system	d₃₃ /pC·N^–1	T_C/℃
KNN-BNH^[71]	385	315
KNN-BNZ-LF^[72]	345	314
KNN-BNZ-MnO₂^[73]	300	345
KNN-BNZ-BG^[24]	312	341
KNN-BNZ-BA^[74]	355	335
KNN-BAZ^[75]	347	318
KNN-BNZ^[76]	360	329
KNN-BKZ-BZ^[77]	305	～300
KNLNS-BS^[78]	325	358
KNN-BNZS^[79]	350	315
KNN-BS-BNKLZ^[80]	366	335
KNN-BNT-BNZ^[81]	318	326
KNN-BNZ-BI^[57]	317	336

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表 6 温度稳定性高的KNN陶瓷体系的压电常数以及变化量

Table 6. Comparison of piezoelectric constant and variation among KNN-based ceramics.

	d₃₃/pC·N^–1	d₃₃ variation/%	$ {d}_{33}^{*} $/pm·V^–1	$ {d}_{33}^{*} $ variation/%
KNLNT-CZ^[86]	—	—	—	almost unchanged @140 ℃
KNN-BNZ-LF^[72]	345	—	420	8%@100 ℃
KNNT-BNKZ-SZ-MnO₂^[49]	—	—	400	10%@180 ℃
KNNT-BNKZ-CZ-MnO₂^[51]	—	—	482	10%@120 ℃
KNNS-BNZ-SZ^[87]	390	—	—	13%@180 ℃
KNN-BLT-BZ-MnO₂^[88]	—	—	470	8.5%@100 ℃, 21.2%@170 ℃
KNNS-BZ-BNZ^[65]	300	10@100 ℃	—	—
KNNS-(BHo)NHf^[89]	—	—	～386	almost unchanged @140 ℃
KNNT-BNZ-CZ^[90]	—	—	502	10%@135 ℃
KNNS-BNKH^[42]	525	—	460	10%@80 ℃
KNN-BZ-BNH-MnO₂^[91]	300	15@120 ℃	540 ± 10	5%@100 ℃
KNN-BNH-BF-MnO₂^[92]	450	—	—	28%@160 ℃
KNN-BNZ-MnO₂-Sb₂O₃^[69]	318	—	—	9%@170 ℃
KNNS-BZH-BNZ^[36]	410	—	441	2.5%@100 ℃, 16.1%@180 ℃
注: 16.1%@180 ℃表示到180 ℃性能下降16.1%.

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表 7 处于6配位时的离子半径表^[131]

Table 7. The ionic radii in six-fold coordination^[131].

	Nb⁵⁺	Ta⁵⁺	Zr⁴⁺	Hf⁴⁺	Sn⁴⁺	Ti⁴⁺	Sb⁵⁺	Sb³⁺	Ga³⁺
离子半径/Å	0.64	0.64	0.72	0.71	0.69	0.605	0.60	0.76	0.62

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表 8 不同结构下原子内坐标随应变的梯度, 注意O_I位于Bmm2不包含Nb原子的(010)平面, KNN中O_I,1和O_I,2沿a方向分别靠近K和Na原子^[138]

Table 8. Internal atomic coordinate gradients as a function of strains in different structure, noted that O_I is located at the (010) plane without Nb atoms in Bmm2, O_I,1 and O_I,2 are close to K and Na along a axis, respectively^[139].

		K	Nb		O_Ⅱ		O_Ⅰ
KN	∂u₃/∂η₃	0.108	0.166		–0.092		–0.091
KN	∂u₁/∂η₅	0.115	0.210		–0.151		–0.024

		K	Na	Nb	O_Ⅱ	O_I,1	O_I,2
KNN	∂u₃/∂η₃	0.103	0.542	0.125	–0.158	–0.125	–0.135
KNN	∂u₁/∂η₅	0.094	0.828	0.194	–0.235	–0.061	–0.309

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