Research progress of high piezoelectric activity of potassium sodium niobate based lead-free ceramics

Xing Jie; Tan Zhi; Zheng Ting; Wu Jia-Gang; Xiao Ding-Quan; Zhu Jian-Guo

doi:10.7498/aps.69.20200288

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:

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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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]}

Figure 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]}.

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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])

Figure 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]).

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图 3 KNN基无铅压电陶瓷d₃₃与T_C对比图^[12,15-47]

Figure 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

Figure 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]

Figure 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

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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

DownLoad: CSV

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

DownLoad: CSV

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%.

DownLoad: CSV

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

DownLoad: CSV

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

DownLoad: CSV

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Vol. 69, Issue 12 - 2020-06-20

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