A位Sm掺杂对0.93Na0.5Bi0.5TiO3-0.07BaTiO3陶瓷微结构及电学性能的影响

doi:10.15541/jim20170343

摘要/Abstract

摘要：

采用固相反应烧结方法制备了Sm掺杂的[(Na_0.5Bi_0.5)_0.93Ba_0.07]_1-_xSm_xTiO₃(BNBST)无铅介电储能陶瓷, 系统研究了Sm掺杂含量对BNBST陶瓷的相结构、微观结构、铁电、介电、储能和交、直流电导的影响。研究结果表明: 制备的陶瓷样品具有单一的钙钛矿结构, Sm掺杂固溶于(Na_0.5Bi_0.5)_0.93Ba_0.07TiO₃基材的晶格A位; 晶粒生长被Sm掺杂抑制, 平均晶粒尺寸在2 μm内, 且均匀致密; Sm掺杂显著降低了剩余极化和矫顽场, 表现出双电滞回线特性, 但饱和极化也略有降低; 储能密度和效率随Sm掺杂量增加先增大后减小, 在x=0.02和电场为70 kV/cm时获得最大储能密度0.70 J/cm³, 其效率为40%; BNBST陶瓷具有明显的弛豫铁电体特征, 其介电常数峰T_m随掺杂量增加而降低且平坦化; BNBST陶瓷的绝缘性有较强的温度依赖性, 300℃以下具有良好的绝缘性。

关键词: BNT-BT, Sm掺杂, 储能, 铁电

Abstract:

Sm doped [(Na_0.5Bi_0.5)_0.93Ba_0.07]_1-_xSm_xTiO₃ (BNBST) lead-free dielectric energy storage ceramics were prepared by solid-phase reaction sintering method. Effects of the Sm doping content on phase structure, microstructure, ferroelectric, dielectric, energy storage properties and d.c., and a.c. conductance of BNBST ceramics were systematically investigated. Results indicate that the as-fabricated BNBST ceramics exhibit single-phase perovskite structure, and Sm dopants get into the A-site lattice of (Na_0.5Bi_0.5)_0.93Ba_0.07TiO₃ matrix. Dense and uniform grains are obtained by grain growth inhibition of Sm dopants with average grain size within 2 μm. The remanent polarization and coercivity of BNBST ceramics sharply decrease after introducing Sm dopants, and the double hysteresis loops are observed with a little decrease of saturation polarization. The energy storage density and efficiency increase firstly and then decrease with increasing Sm doping content, the energy storage density reaches a maximum value of 0.70 J/cm³ at x=0.02 and 70 kV/cm electric field, with corresponding efficiency of 40%. The BNBST ceramics show an obvious relaxation ferroelectric characteristic and its dielectric constant peaks of T_m decrease and planarize with increasing Sm doping content. The electric insulativity of BNBST ceramics has strong temperature dependence, and the excellent electric insulativity can be kept when ambient temperature is below 300℃.

Key words: BNT-BT, Sm doping, energy storage, ferroelectric

中图分类号:

TQ174

窦闰镨, 卢晓鹏, 杨玲, 王华, 周昌荣, 许积文. A位Sm掺杂对0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃陶瓷微结构及电学性能的影响[J]. 无机材料学报, 2018, 33(5): 528-534.

DOU Run-Pu, LU Xiao-Peng, YANG Ling, WANG Hua, ZHOU Chang-Rong, XU Ji-Wen. Influence of A-site Sm Doping on Structural and Electrical Property of 0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃ Lead Free Ceramics[J]. Journal of Inorganic Materials, 2018, 33(5): 528-534.

图/表 10

图1 不同Sm掺杂量的BNBST陶瓷在(a) 20°-80°和(b) 46°-47°范围的XRD图谱

Fig. 1 XRD patterns ranging from (a) 20°-80° and (b) 46°- 47° of BNBST ceramics doped with different amounts of Sm

图2 不同Sm掺杂量时BNBST陶瓷的表面SEM照片

Fig. 2 Surface morphologies of BNBST ceramics doped with different amounts of Sm(a) x=0.01; (b) x=0.02; (c) x=0.03; (d) x=0.04

图3 不同Sm掺杂量时BNBST陶瓷的平均晶粒尺寸

Fig. 3 Average grain size of BNBST ceramics doped with different amounts of Sm

图4 不同Sm掺杂量时BNBST陶瓷的电滞回线

Fig. 4 Hysteresis loops of BNBST ceramics doped with different amounts of Sm

图5 不同Sm掺杂量时BNBST陶瓷的储能密度和效率

Fig. 5 Energy storage density and efficiency of BNBST ceramics doped with different amounts of Sm

图6 BNBST陶瓷(x=0.02)不同场强下的电滞回线

Fig. 6 Hysteresis loops of BNBST ceramic (x=0.02) tested at different external electric fields

图7 1、10和100 kHz下不同Sm掺杂量时BNBST陶瓷的介电温谱

Fig. 7 Temperature dependence of dielectric constant and loss of BNBST ceramics doped with different amounts of Sm at 1 kHz、10 kHz and 100 kHz(a) x=0.01; (b) x=0.02; (c) x=0.03; (d) x=0.04

图8 不同Sm掺杂量时BNBST陶瓷的ln(1/ɛ-1/ɛm)与ln(T-Tm)关系曲线

Fig. 8 Plots of ln(1/ε-1/εm) versus ln(T-Tm) of BNBST ceramics doped with different amounts of Sm

图9 BNBST(x=0.02)陶瓷的交流电阻与频率对数的关系, 内插图为直流lgI-lgU曲线

Fig. 9 Resistance of BNBST as a function of frequency, and with inset showing lgI-lgU curve tested by direct current mode

图10 BNBST(x=0.02)陶瓷在100~550℃时的交流阻抗谱

Fig. 10 Cole-Cole plots of BNBST ceramic (x=0.02) measured from 100℃ to 550℃

参考文献 33

[1]	HUANG JIA-JIA, ZHANG YONG, CHEN JI-CHUN.A overview on deliectric materials with high energy storge density. Materials Review, 2009, 23(s1): 307-312.
[2]	LIN FU-CHANG, LI JIN, YAO ZONG-GAN.Choice of capacitors used in electromagnetic launcher.Acta Armamentarii, 2003, 24(3): 416-418.
[3]	ZHANG N, FENG Y, XU Z.Effects of lanthanum modification on electrical and dielectric properties of Pb(Zr0.70,Ti0.30)O3 ceramics.Materials Letters, 2011, 65(11): 1611-1614.
[4]	BIKYASHEV EA, RYUSH IO, RESHETNIKOVA EA.Structures of Pb1-xLax[Zr0.9Mg(0.1+x)/3Nb(0.2-x)/3]O3 solid solutions, electrostriction and energy storage characteristics of a new antiferroelectric phase with disturbed translational symmetry. Ceramics International, 2017, 43(1): 1429-1436.
[5]	CHEN X, LIU Z, XU C,et al. Temperature-dependent dielectric and energy-storage properties of Pb(Zr,Sn,Ti)O3 antiferroelectric bulk ceramics. AIP Advances, 2016, 6(5): 593.
[6]	JIANG S, ZHANG L, ZHANG G,et al. Effect of Zr:Sn ratio in the lead lanthanum zirconate stannate titanate anti-ferroelectric ceramics on energy storage properties. Ceramics International, 2013, 39(5): 5571-5575.
[7]	CHEN ZHI-WU.Development of Bi0.5Na0.5TiO3-BaTiO3 and Bi0.5Na0.5TiO3-Bi0.5K0.5TiO3-based lead-free piezoelectric ceramics.Materials Review, 2006, 20(1): 14-18.
[8]	YANG ZUPEI, LIU BING, WEI LINGLING,et al. Structure and electrical properties of (1-x)Bi0.5Na0.5TiO3-xBi0.5K0.5TiO3 ceramics near morphotropic phase boundary. Materials Research Bulletin, 2008, 43(1): 81-89.
[9]	WOOK JO, JOHN E DANIELS, JACOB L JONES,et al. Evolving morphotropic phase boundary in lead-free Bi1/2Na1/2TiO3- BaTiO3 piezoceramics. Journal of Applied Physics, 2011, 109(1): 014110-1-014110-7.
[10]	SHI J, FAN H, LIU X,et al. Bi deficiencies induced high permittivity in lead-free BNBT-BST high-temperature dielectrics. Journal of Alloys & Compounds, 2015, 627: 463-467.
[11]	HAMZA L, BRAHIM L, MOKHTAR BL,et al. XRD, Raman and electrical studies on the (1-x)(Na0.5Bi0.5)TiO3-xBaTiO3 lead free ceramics. Journal of Alloys and Compounds, 2015, 618: 643-648.
[12]	LIU G, FAN H, DONG G,et al. Enhanced energy storage and dielectric properties of Bi0.487Na0.427K0.06Ba0.026TiO3-xCeO2, anti- ferroelectric ceramics. Journal of Alloys & Compounds, 2016, 664: 632-638.
[13]	CHAOUCHI A, KENNOUR S, DASTORG S,et al. Characterization of Sol-Gel synthesised lead-free (1-x)Na0.5Bi0.5TiO3-xBaTiO3- based ceramics. Journal of Alloys and Compounds, 2011, 509(37): 9138-9143.
[14]	BAI WANGFENG, CHEN DAQIN, ZHENG PENG,et al. Low electric field-driven giant strain response in <001> textured BNT-based lead-free piezoelectric materials. Journal of Materials Science, 2017, 52(6): 3169-3178.
[15]	ADITYA CHAUHAN, SATYANARAYAN PATEL, RAHUL VAISH,et al. Anti-ferroelectric ceramics for high energy density capacitors. Materials, 2015, 8(12): 8009-8031.
[16]	THANABOONSOMBUT A, VANEESORN N.Effect of attrition milling on the piezoelectric properties of Bi0.5Na0.5TiO3-based ceramics. Journal of Electroceramics, 2008, 21(1-4): 414-417.
[17]	LI Q, WANG J, MA L,et al. Large electrocaloric effect in (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ferroelectric ceramics by La2O3 addition. Materials Research Bulletin, 2016, 74: 57-61.
[18]	XU JIWEN, LU XIAOPENG, YANG LING,et al. Enhanced electrical energy storage properties in La-doped (Bi0.5Na0.5)0.93Ba0.07TiO3 lead-free ceramics by addition of La2O3 and La(NO3)3. Journal of Materials Science, 2017, 52(17): 10062-10072.
[19]	FU P, XU Z, CHU R,et al. Effect of Dy2O3 on the structure and electrical properties of (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free piezoelectric ceramics. Journal of Alloys and Compounds, 2010, 508(2): 546-553.
[20]	SHI J, YANG W.Piezoelectric and dielectric properties of CeO2-doped (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics.Journal of Alloys and Compounds, 2009, 472(1): 267-270.
[21]	WANG TING, DU HUI-LING, SHI XIANG.Piezoelectric properties and dielectric relaxation of La3+-doped Na0.5Bi0.5TiO3 based lead-free ceramics.Journal of the Chinese Ceramic Society, 2009, 37(6): 916-921.
[22]	FU P, XU Z, CHU R,et al. Piezoelectric, ferroelectric and dielectric properties of La2O3-doped (Bi0.5Na0.5)0.94Ba0.06TiO3 lead-free ceramics. Materials & Design, 2010, 31(2): 796-801.
[23]	GUO YUCHEN, FAN HUIQING, SHI JING.Origin of the large strain response in tenary SrTi0.8Zr0.2O3 modified Bi0.5Na0.5TiO3- Bi0.5K0.5TiO3 lead-free piezoceramics.Journal of Materials Science, 2015, 50(1): 403-411.
[24]	MONEIM ZANNEN, ABDELILAH LAHMAR, HAMADIKHEMAKHEM,et al. Energy storage property in lead free Gd doped Na1/2Bi1/2TiO3 ceramics. Solid State Communications, 2016, 245: 1-4.
[25]	CHANDRASEKHAR M, SONIA, KUMAR P.Synthesis and characterizations of NaNbO3 modified BNT-BT-BKT ceramics for energy storage applications.Physica B Condensed Matter, 2016, 497: 59-66.
[26]	MA C, TAN X, DUL'KIN E,et al. Domain structure-dielectric property relationship in lead-free (1-x)(Bi1/2Na1/2)TiO3-xBaTiO3 ceramics. Journal of Applied Physics, 2010, 108(10): 797.
[27]	XU Q, LI T, HAO H,et al. Enhanced energy storage properties of NaNbO3 modified Bi0.5Na0.5TiO3 based ceramics. Journal of the European Ceramic Society, 2015, 35(2): 545-553.
[28]	CEN Z, ZHOU C, ZHOU Q,et al. The effect of composite (Li0.5Nd0.5)2+ ions substitution on microstructure, dielectric behavior and electrical properties of 0.95Bi0.5Na0.5TiO3-0.05BaTiO3 ceramics. Ceramics International, 2014, 40(7): 10431-10439.
[29]	GUO Y, FAN H, LONG C,et al. Electromechanical and electrical properties of Bi0.5Na0.5 Ti1-xMnxO3-δ, ceramics with high remnant polarization. Journal of Alloys & Compounds, 2014, 610:189-195.
[30]	KHEMAKHEM L, KABADOU A, MAALEJ A,et al. New relaxor ceramic with composition BaTi1-x(Zn1/3Nb2/3)xO3. Journal of Alloys and Compounds, 2008, 452(2): 451-455.
[31]	UCHINO K, NOMURA S.Critical exponents of the dielectric constants in diffused-phase-transition crystals.Ferroelectrics, 1982, 44(1): 55-61.
[32]	ACHARYA S K, AHN B G, CHANG U J,et al. Effect of Rb doping on ferroelectric and piezoelectric properties of Bi0.5Na0.5TiO3- BaTiO3 thin films. Journal of Alloys & Compounds, 2014, 603(8): 248-254.
[33]	CHEN F, LIU Q X, TANG X G,et al. Diffuse phase transition and high-temperature dielectric relaxation study on (Bi0.5Na0.5)1-xBaxTiO3 ceramics. Physica B: Condensed Matter, 2016, 496: 20-25.

A位Sm掺杂对0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃陶瓷微结构及电学性能的影响

Influence of A-site Sm Doping on Structural and Electrical Property of 0.93Na_0.5Bi_0.5TiO₃-0.07BaTiO₃ Lead Free Ceramics

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