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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

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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

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
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  • 以Pb(Zr1–xTix)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 (K0.5Na0.5)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.
    Due to excellent piezoelectric properties and electromechanical coupling properties, lead-based piezoelectric ceramics represented by lead zirconate titanate Pb(ZrxTi1–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 (K0.5Na0.5)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.
      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)
      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]

    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].

    图 2  (a)正交相(K0.5Na0.5NbO3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 (K0.5Na0.5NbO3 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]).

    图 3  KNN基无铅压电陶瓷d33TC对比图[12,15-47]

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

    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].

    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].

    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 systemd33/pC·N–1kpTC/℃
    KNLANT[15]2520.454438
    KNLN-BCZT[16]1800.34425
    KNN-KLN[17]1210.39
    KNLN-AS[18]2300.39430
    KNLN-BNCT[19]2620.36~400
    KNN-BC[20]1650.40~390
    KNN-LS[21]2800.494364
    KNN-BLZ[22]2650.365364
    KNN-BC-BNH[23]2720.47333
    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 systemd33/pC·N–1kpTC /℃
    KNN-BNZ-BG[24]3120.44341
    KNN-BZ-BNZ[25]3450.50~260
    KNN-NS-BNKZH[26]4520.63~270
    KNNS-BNCZ[27]4150.46245
    KNNTS-BNKZ[28]4000.46240
    KNN-BNZN[29]318 ± 10360
    KNNS-BKZH[30]4510.52258
    KNNS-BLKZ[31]385245
    KNNS-SZ-BNH[32]470 ± 50.51 ± 0.02244
    KNNS-BS-BNZ[33]~480~225
    KNNS-BNZ-BZ[34]6100.58241
    KNNS-BNKZ-Fe-AS[12]650~180
    下载: 导出CSV

    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 systemd33 /pC·N–1kpTC/℃
    KNNS-BNZSn[35]4650.51240
    KNNS-BZH[36]410255
    KNNS-BNKZ[37]4900.46227
    KNNTS-BNKZ[38]4600.40~220
    KNNS-BNH[39]4190.45242
    KNNS-BKZS[40]430243
    KNNS-BNLCZ[41]4850.48227
    KNNS-BNKH[42]525~210
    KNNS-BF-BNZ[43]550237
    KNNS-CZ-BKHT-MnO2[44]4250.49215
    KNNS-BZ-BKH[45]570 ± 10~190
    KNNS-BNZ-BF[46]5110.515269
    KNANS-BNZ[47]4400.50250
    下载: 导出CSV

    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 systemd33 or $ {d}_{33}^{*} $Domain size
    KNNS-SZ-BAZ[52]487 pC/N30—65 nm,
    65—160 nm,
    30—45 nm
    KNNS-BZ-BNH[48]600 pm/V10—100 nm
    KNNS-BNKH[42]525 pC/N10—30 nm
    KNNS-BNKZ-Fe-AS[12](650 ± 20) pC/N2 nm
    KNNS-BNZ-BZ[34]610 pC/N50—70 nm
    KNNT-BNKZ-CZ[51]482 pm/V60 nm
    KNNS-BZ-BNZ[65]300 pC/N150 nm—1.0 μm
    KNNS-CZ-BKH[66]550 pC/N30—230 nm
    KNNS-BNH[67]512 pC/N100 nm
    KNNS-SZ-BNZ[68]450 pC/N50—200 nm
    KNLNTS[54]455 pC/N110—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
    下载: 导出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 systemd33 /pC·N–1TC/℃
    KNN-BNH[71]385315
    KNN-BNZ-LF[72]345314
    KNN-BNZ-MnO2[73]300345
    KNN-BNZ-BG[24]312341
    KNN-BNZ-BA[74]355335
    KNN-BAZ[75]347318
    KNN-BNZ[76]360329
    KNN-BKZ-BZ[77]305~300
    KNLNS-BS[78]325358
    KNN-BNZS[79]350315
    KNN-BS-BNKLZ[80]366335
    KNN-BNT-BNZ[81]318326
    KNN-BNZ-BI[57]317336
    下载: 导出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–1d33 variation/%$ {d}_{33}^{*} $/pm·V–1$ {d}_{33}^{*} $ variation/%
    KNLNT-CZ[86]almost unchanged @140 ℃
    KNN-BNZ-LF[72]3454208%@100 ℃
    KNNT-BNKZ-SZ-MnO2[49]40010%@180 ℃
    KNNT-BNKZ-CZ-MnO2[51]48210%@120 ℃
    KNNS-BNZ-SZ[87]39013%@180 ℃
    KNN-BLT-BZ-MnO2[88]4708.5%@100 ℃, 21.2%@170 ℃
    KNNS-BZ-BNZ[65]30010@100 ℃
    KNNS-(BHo)NHf[89]~386almost unchanged @140 ℃
    KNNT-BNZ-CZ[90]50210%@135 ℃
    KNNS-BNKH[42]52546010%@80 ℃
    KNN-BZ-BNH-MnO2[91]30015@120 ℃540 ± 105%@100 ℃
    KNN-BNH-BF-MnO2[92]45028%@160 ℃
    KNN-BNZ-MnO2-Sb2O3[69]3189%@170 ℃
    KNNS-BZH-BNZ[36]4104412.5%@100 ℃, 16.1%@180 ℃
    注: 16.1%@180 ℃表示到180 ℃性能下降16.1%.
    下载: 导出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/Å0.640.640.720.710.690.6050.600.760.62
    下载: 导出CSV

    表 8  不同结构下原子内坐标随应变的梯度, 注意OI位于Bmm2不包含Nb原子的(010)平面, KNN中OI,1和OI,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 OI is located at the (010) plane without Nb atoms in Bmm2, OI,1 and OI,2 are close to K and Na along a axis, respectively[139].

    KNbOO
    KNu3/∂η30.1080.166–0.092–0.091
    u1/∂η50.1150.210–0.151–0.024
    KNaNbOOI,1OI,2
    KNNu3/∂η30.1030.5420.125–0.158–0.125–0.135
    u1/∂η50.0940.8280.194–0.235–0.061–0.309
    下载: 导出CSV
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  • 收稿日期:  2020-02-25
  • 修回日期:  2020-03-20
  • 刊出日期:  2020-06-20

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