硅酸盐学报

BCZT无铅压电陶瓷的水热法制备及其性能

单位：1. 常州大学材料科学与工程学院江苏省光伏科学与工程协同创新中心江苏常州 213164 2. 上海师范大学光电材料与器件重点实验室上海师范大学物理系上海 200234 3. 中国科学院无机功能材料与器件重点实验室上海 201800

分类号：TM282

出版年,卷(期):页码：2017,45(9):1280-1287

DOI：10.14062/j.issn.0454-5648.2017.09.08

摘要：

通过水热反应法低温烧结制备Ba0.85Ca0.15Zr0.1Ti0.9O3(BCZT)无铅压电陶瓷，研究了烧结温度和时间对BCZT陶瓷的晶体结构和电学性能的影响。与固相反应法相比，由于水热法制备的BCZT前驱体的高活性，可以低温烧结制备BCZT陶瓷，低温烧结制备的BCZT陶瓷呈现纯钙钛矿结构、较为均匀的小晶粒微观形貌(小于10 μm)和更高的致密度。通过水热法制备的BCZT陶瓷呈现优良的电学性能，其介电响应特征接近正常铁电体、又呈现一定的频率色散现象。1 340 ℃烧结18 h制备的BCZT陶瓷的剩余极化强度最大，Pr=6.84 μC/cm2。1 320 ℃烧结18 h制备的BCZT陶瓷压电性能最佳，d33达到最大值213 pC/N。

Ba0.85Ca0.15Zr0.1Ti0.9O3 (BCZT) lead-free piezoelectric ceramics were prepared via a hydrothermal method and low-temperature sintering. The effects of sintering temperature and time on the crystal structure and electrical properties of the BCZT ceramics were investigated. Compared to a solid-state reaction method, the BCZT ceramics can be synthesized at low sintering temperatures due to the higher sintering capability of the BCZT precursor prepared by the hydrothermal method. The low-temperature sintered BCZT ceramics exhibit a pure perovskite structure, rather homogenous microstructural morphology, smaller grain sizes (i.e., <10 μm), and higher relative density. The BCZT ceramics prepared via the hydrothermal method exhibit excellent electrical properties, in which their dielectric response behavior approaches normal ferroelectrics, and presents a slight dielectric frequency dispersion as well. The BCZT ceramic sintered at 1 340 ℃ for 18 h presents the maximum remnant polarization (i.e., Pr=6.84 μC/cm2). The BCZT ceramic sintered at 1 320 ℃ for 18 h exhibits the maximum piezoelectric constant (i.e., 213 pC/N).

基金项目：

国家自然科学基金(51577015)；江苏省产学研合作前瞻性联合研究项目(BY2015027-220)；江苏高校优势学科建设工程资助。

作者简介：

卢晓羽(1992—)，女，硕士研究生。

参考文献：

[1]GUO R, CROSS L E, PARK S E, et al. Origin of the high piezoelectric response in PbZr1–xTixO3[J]. Phys Rev Lett, 2000, 84(23): 5423–5426.

[2]CHEN L, LIANG R, WANG G, et al. Poling induced dielectric anomalies in a PZT ceramic[J]. Ceram Int, 2013, 39(8): 8941–8940.4.

[3]LIU C L, PAN S S, CHEN Z H, et al. Phase diagram of ternary Pb(Mg1/3Nb2/3)O3–PbZrO3–PbTiO3 ferroelectric ceramics prepared via a B-site oxide mixing route[J]. Ferroelectrics, 2015, 482(1): 11–21.

[4]RÖDEL J, JO W, SEIFERT K T P, et al. Perspective on the development of lead-free piezoceramics[J]. J Am Ceram Soc, 2009, 92(6): 1153–1177.

[5]LI Y, MOON K S, WONG C P. Electronics without lead[J]. Science, 2005, 308(5727): 1419–1420.

[6]WADA S, TAKEDA K, TSURUMI T, et al. Preparation of [110] grain oriented barium titanate ceramics by templated grain growth method and their piezoelectric properties[J]. Jpn J Appl Phys, 2007, 46(46): 372–376.

[7]SHEN Z J, BING L N, PENG H Y, et al. Influence of Ge and Si doping on the microstructure and dielectric properties of barium titanate ceramics[J]. Appl Mech Mater, 2013, 464: 44–49.

[8]郭朋彦, 张瑞朱, 郭雯鹏, 等. W、Zr共同掺杂对铌酸钾钠基无铅压电陶瓷的影响[J]. 硅酸盐学报, 2016, 44(9): 1265–1269.

GUO Pengyan, ZHANG Ruizhu, GUO Wenpeng, et al. J Chin Ceram Soc, 2016, 44(9): 1265–1269.

[9]ZHAO Y J, YUAN X Y, ZHAO Y Z, et al. Improved piezoelectricity and luminescence behavior in Er2O3 doped (K, Na)NbO3 ceramics[J]. Mater Lett, 2016, 162: 226–229.

[10]ZUO R Z, FANG X S, YE C. Phase structures and electrical properties of new lead-free (Na0.5K0.5)NbO3–(Bi0.5Na0.5)TiO3 ceramics[J]. Appl Phys Lett, 2007, 90(9): 092900.4

[11]MURYA D, ZHOU Y, WANG Y J, et al. Giant strain with ultra-low hysteresis and high temperature stability in grain oriented lead-free K0.5Bi0.5TiO3–BaTiO3–Na0.5Bi0.5TiO3 piezoelectric materials[J]. Sci Rep, 2015, 5: 8595.

[12]LIU W F, REN X B. Large piezoelectric effect in Pb-free ceramics[J]. Phys Rev Lett, 2009, 103(25): 257602.

[13]JIANG X P, LI L, CHEN C, et al. Effects of Mn-doping on the properties of (Ba0.92Ca0.08)(Ti0.95Zr0.05)O3 lead-free ceramics[J]. J Alloy Compd, 2013, 574(3): 88–91.

[14]ACOSTA M, NOVAK N, JO W, et al. Relationship between electromechanical properties and phase diagram in the Ba(Zr0.2Ti0.8)O3–x(Ba0.7Ca0.3)TiO3 lead-free piezoceramic[J]. Acta Mater, 2014, 80: 48–55.

[15]LIU X, CHEN Z H, FANG B J, et al. Enhancing piezoelectric properties of BCZT ceramics by Sr and Sn co-doping[J]. J Alloy Compd, 2015, 640: 128–133.

[16]FANG B J, WANG W W, DING J N, et al. Preparation and electrical properties of pseudoternary BaTiO3–CaTiO3–BaZrO3 lead free piezoelectric ceramics[J]. Adv Appl Ceram, 2013, 112(5): 257–262.

[17]SU S, ZUO R Z, LU S B, et al. Poling dependence and stability of piezoelectric properties of Ba(Zr0.2Ti0.8)O3–(Ba0.7Ca0.3)TiO3 ceramics with huge piezoelectric coefficients[J]. Curr Appl Phys, 2011, 11(3): S120–S123.

[18]CUI Y, LIU X, JIANG M, et al. Lead-free (Ba0.85Ca0.15)(Ti0.9Zr0.1)O3–CeO2 ceramics with high piezoelectric coefficient obtained by low-temperature sintering Ceram Int, 2012, 24(38): 4761–4760.4.

[19]SHANNON R D. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides[J]. Acta Cryst, 1976, A32: 751–767.

[20]TANG X G, WANG X X, CHEW K H, et al. Relaxor behavior of (Ba, Sr)(Zr, Ti)O3 ferroelectric ceramics[J]. Solid State Comm, 2005, 136(2): 89–93.

[21]LIU X, WU D, CHEN Z, et al. Ferroelectric, dielectric and pyroelectric properties of Sr and Sn co-doped BCZT lead free ceramics[J]. Adv Appl Ceram, 2015, 114(8): 436–441.

[22]XU Q, ZHANG X F, HUANG Y H, et al. Effect of sintering temperature on structure and nonlinear dielectric properties of Ba0.6Sr0.4TiO3 ceramics prepared by the citrate method[J]. J Phys Chem Solid, 2010, 71(11): 1550–1556.

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