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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.
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Keywords:
- lead-free piezoelectric ceramics /
- potassium sodium niobate /
- origin /
- high piezoelectric property
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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]).
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.
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 kp TC /℃ 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 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 kp TC/℃ 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 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 nmKNNS-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 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.
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%. 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 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].
K Nb OⅡ OⅠ KN ∂u3/∂η3 0.108 0.166 –0.092 –0.091 ∂u1/∂η5 0.115 0.210 –0.151 –0.024 K Na Nb OⅡ OI,1 OI,2 KNN ∂u3/∂η3 0.103 0.542 0.125 –0.158 –0.125 –0.135 ∂u1/∂η5 0.094 0.828 0.194 –0.235 –0.061 –0.309 -
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