(Nd_(0.5)Ta_(0.5))~(4+)复合离子对BNT-BKT陶瓷微结构及电学性能的影响
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摘要
采用固相烧结法制备了(Nd_(0.5)Ta_(0.5))~(4+)复合离子调控的Bi_(0.5)(Na_(0.82)K_(0.18))_(0.5)Ti_(1-x)(Nd_(0.5)Ta_(0.5))_xO_3(BNKT-xNT)无铅陶瓷。研究了(Nd_(0.5)Ta_(0.5))~(4+)复合离子掺杂量对BNKT陶瓷的表面形貌、微观结构,以及铁电、介电、储能、阻抗等电学性能的影响。研究结果表明:(Nd_(0.5)Ta_(0.5))~(4+)复合离子进入了BNKT陶瓷的B位并形成了单一的钙钛矿结构;晶粒分布均匀、致密,晶界清晰;(Nd_(0.5)Ta_(0.5))~(4+)复合离子的引入显著降低了BNKT陶瓷的剩余极化强度、饱和极化强度以及矫顽场,电滞回线变得瘦小、细长,储能效率随之升高,并在x=0.08和60×10~3 V/cm电场下达到了70%;储能密度先减小、后增大、再减小,在x=0.04时达到最大值0.36 J/cm~3;电致应变在x=0.03时最大为0.183%;随着掺杂含量的增加,BNKT-xNT陶瓷从铁电相与弛豫铁电相共存转变为弛豫铁电相,其介电常数峰T_m逐渐降低且平坦化;交流阻抗谱表明BNKT-xNT陶瓷在低温下具有良好的绝缘性。
The(Nd_(0.5)Ta_(0.5))~(4+) complex-ions doped Bi_(0.5)(Na_(0.82) K_(0.18))_(0.5)Ti_(1-x)(Nd_(0.5)Ta_(0.5))_xO_3(BNKT-xNT) lead-free ceramics were prepared by solid-phase reaction method.The effects of the(Nd_(0.5)Ta_(0.5))~(4+) complex-ions content on the morphology,microstructure,ferroelectric,dielectric,energy storage properties and impedance of BNKT-xNT ceramics were investigated.The results indicate that(Nd_(0.5)Ta_(0.5))~(4+) complex-ions enter the B-sites of BNKT matrix and form single-phase perovskite structure.The grains are dense and uniform and the grain boundaries are clear.The introduction of(Nd_(0.5)Ta_(0.5))~(4+) complex-ions lead to significantly decrease of the remnant polarization,maximum polarization and coercive field.The hysteresis loops become slim and the energy storage efficiency was improved.70% of energy storage efficiency was obtained at x=0.08 and 60 kV/cm electric field.The energy storage density decreases at first and then increases,and finally decreases again.The optimal energy storage density is 0.36 J/cm~3 at x=0.04.The optimal strain is 0.183% at x=0.03.The ceramic transforms from the coexistence of ferroelectric and relaxorphase to the ideal relaxtorphase.And the peak of dielectric constant T_m decreases and becomes flat with increasing(Nd_(0.5)Ta_(0.5))~(4+)complex-ions content.The BNKT-xNT ceramics have excellent insulation behavior at low temperature,which is confirmed by impedance spectroscopy.
The(Nd_(0.5)Ta_(0.5))~(4+) complex-ions doped Bi_(0.5)(Na_(0.82) K_(0.18))_(0.5)Ti_(1-x)(Nd_(0.5)Ta_(0.5))_xO_3(BNKT-xNT) lead-free ceramics were prepared by solid-phase reaction method.The effects of the(Nd_(0.5)Ta_(0.5))~(4+) complex-ions content on the morphology,microstructure,ferroelectric,dielectric,energy storage properties and impedance of BNKT-xNT ceramics were investigated.The results indicate that(Nd_(0.5)Ta_(0.5))~(4+) complex-ions enter the B-sites of BNKT matrix and form single-phase perovskite structure.The grains are dense and uniform and the grain boundaries are clear.The introduction of(Nd_(0.5)Ta_(0.5))~(4+) complex-ions lead to significantly decrease of the remnant polarization,maximum polarization and coercive field.The hysteresis loops become slim and the energy storage efficiency was improved.70% of energy storage efficiency was obtained at x=0.08 and 60 kV/cm electric field.The energy storage density decreases at first and then increases,and finally decreases again.The optimal energy storage density is 0.36 J/cm~3 at x=0.04.The optimal strain is 0.183% at x=0.03.The ceramic transforms from the coexistence of ferroelectric and relaxorphase to the ideal relaxtorphase.And the peak of dielectric constant T_m decreases and becomes flat with increasing(Nd_(0.5)Ta_(0.5))~(4+)complex-ions content.The BNKT-xNT ceramics have excellent insulation behavior at low temperature,which is confirmed by impedance spectroscopy.
引文
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[28]Ullah A,Ahn C W,Malik R A,et al.Dielectric and impedance spectroscopy of lead-free 0.99[(Bi0.5Na0.4K0.1)(Ti0.980Nb0.020)O3]-0.01(Ba0.7Sr0.3)TiO3 ceramics [J].Physica B:Condensed Matter,2014,444:27-33.
[29]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 [J].Physica B:Condensed Matter,2016,496:20-25.
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本文系“第十七届全国电介质会议暨第十九届全国电子元件会议及2018国际固态制冷材料和器件研讨会”会议论文。
[2]Zheng T,Wu J G,Xiao D Q,et al.Recent development in lead-free perovskite piezoelectric bulk materials [J].Progress in Materials Science,2018,98(2018):552-624.
[3]Chen N,Yao W J,Liang C,et al.Phase structure,ferroelectric properties,and electric field-induced large strain in lead-free 0.99[(1-x)(B0.5Na0.5)TiO3-x(Bi0.5K0.5)TiO3]-0.01Ta piezoelectric ceramics [J].Ceramics International,2016,42(8):9660-9666.
[4]Yang Z P,Liu B,Wei L L,et al.Structure and electrical properties of (1-x)Bi0.5Na0.5TiO3-xBi0.5K0.5TiO3 ceramics near morphotropic phase boundary [J].Materials Research Bulletin,2008,43(1):81-89.
[5]Zhou C R,Liu X Y,Li W Z,et al.Dielectric and piezoelectric properties of Bi0.5Na0.5TiO3-Bi0.5K0.5TiO3-BiCrO3 lead-free piezoelectric ceramics [J].Journal of Alloys and Compounds,2009,478(1/2):381-385.
[6]Butnoi P,Manotham S,Jaita P,et al.High thermal stability of energy storage density and large strain improvement of lead-free Bi0.5(Na0.40K0.10)TiO3 piezoelectric ceramics doped with La and Zr [J].Journal of the European Ceramic Society,2018,38(11):3822-3832.
[7]Sumang R,Bongkarn T,Kumar N,et al.Investigation of a new lead-free (1-x-y)BNT-xBKT-yBZT piezoelectric ceramics [J].Ceramics International,2017,43:S102-S109.
[8]Sumang R,Cann D P,Kumar N,et al.Large strain in lead-free piezoelectric (1-x-y)Bi0.5Na0.5TiO3-xBi0.5K0.5TiO3-yBi0.5Li0.5TiO3 system near MPB prepared via the combustion technique [J].Ceramics International,2015,41:S127-S135.
[9]Zhou C R,Liu X Y,Li W Z,et al.Structure and piezoelectric properties of Bi0.5Na0.5TiO3-Bi0.5K0.5TiO3-BiFeO3 lead-free piezoelectric ceramics [J].Materials Chemistry and Physics,2009,114(2/3):832-836.
[10]Marwat M A,Xie B,Ashtar M,et al.High remnant polarization,high dielectric constant and impedance performance of Nb/In Co-doped Bi0.49La0.01Na0.49Li0.01TiO3-δ ceramics [J].Ceramics International,2018,44(6):6843-6850.
[11]Ge R F,Zhao Z H,Duan S F,et al.Large electro-strain response of La3+ and Nb5+ co-doped ternary 0.85Bi0.5Na0.5TiO3-0.11Bi0.5K0.5TiO3-0.04BaTiO3 lead-free piezoelectric ceramics [J].Journal of Alloys and Compounds,2017,724:1000-1006.
[12]Zhao Y Y,Xu J,Yang L,et al.High energy storage property and breakdown strength of Bi0.5(Na0.82K0.18)0.5TiO3 ceramics modified by (Al0.5Nb0.5)4+ complex-ion [J].Journal of Alloys and Compounds,2016,666:209-216.
[13]Fan P Y,Zhang Y Y,Xie B,et al.Large electric-field-induced strain in B-site complex-ion (Fe0.5Nb0.5)4+-doped Bi1/2(Na0.82K0.12)1/2TiO3 lead-free piezoceramics [J].Ceramics International,2018,44(3):3211-3217.
[14]Yang Z P,Hou Y T,Liu B,et al.Structure and electrical properties of Nd2O3-doped 0.82Bi0.5Na0.5TiO3-0.18Bi0.5K0.5TiO3 ceramics [J].Ceramics International,2009,35(4):1423-1427.
[15]Han W H,Koh J H.Shrinkage mechanism and enhanced piezoelectric properties of Ta doped 0.94Bi0.5Na0.5TiO3-0.06BaTiO3 lead free ceramics [J].Ceramics International,2018,44(5):5352-5358.
[16]Quyet N V,Bac L H,Odkhuu D,et al.Effect of Li2CO3 addition on the structural,optical,ferroelectric,and electric-field-induced strain of lead-free BNKT-based ceramics [J].Journal of Physics and Chemistry of Solids,2015,85:148-154.
[17]Zhang L,Pu X Y,Chen M,et al.Influence of BaSnO3 additive on the energy storage properties of Na0.5Bi0.5TiO3-based relaxor ferroelectrics [J].Journal of the European Ceramic Society,2018,38(5):2304-2311.
[18]Wang C M,Xu Z J,Cheng R F,et al.Electric field-induced giant strain and piezoelectricity enhancement effect in (Bi1/2Na1/2)0.935+xBa0.065Ti1-x(Pr1/2Nb1/2)O3 lead-free ceramics [J].Ceramics International,2016,42(3):4354-4360.
[19]Yu Z L,Liu Y F,Shen M Y,et al.Enhanced energy storage properties of BiAlO3 modified Bi0.5Na0.5TiO3-Bi0.5K0.5TiO3 lead-free antiferroelectric ceramics [J].Ceramics International,2017,43(10):7653-7659.
[20]Liu X,Li F,Li P,et al.Tuning the ferroelectric-relaxor transition temperature in NBT-based lead-free ceramics by Bi nonstoichiometry [J].Journal of the European Ceramic Society,2017,37(15):4585-4595.
[21]Liu X M,Tan X L.Giant strains in non-textured (Bi1/2Na1/2)TiO3-based lead-free ceramics [J].Advanced Materials,2016,28(3):574-578.
[22]Wang C,Lou X J,Xia T D,et al.The dielectric,strain and energy storage density of BNT-BKHxT1-x piezoelectric ceramics [J].Ceramics International,2017,43(12):9253-9258.
[23]Pal V,Kumar A,Thakur O P,et al.Preparation,microstructure and relaxor ferroelectric characteristics of BLNT-BCT lead-free piezoceramics [J].Journal of Alloys and Compounds,2017,714:725-735.
[24]Guo Y C,Fan H Q,Long C B,et al.Electromechanical and electrical properties of Bi0.5Na0.5Ti1-xMnxO3-δ ceramics with high remnant polarization [J].Journal of Alloys and Compounds,2014,610:189-195.
[25]Obilor U,Pascual-Gonzalez C,Murakami S,et al.Study of the temperature dependence of the giant electric field-induced strain in Nb-doped BNT-BT-BKT piezoceramics [J].Materials Research Bulletin,2018,97:385-392.
[26]Uchino K,Nomura S.Critical exponents of the dielectric constants in diffused-phase-transition crystals [J].Ferroelectrics,2011,44(1):55-61.
[27]Khemakhem L,Kabadou A,Maalej A,et al.New relaxor ceramic with composition BaTi1-x(Zn1/3Nb2/3)xO3 [J].Journal of Alloys and Compounds,2008,452(2):451-455.
[28]Ullah A,Ahn C W,Malik R A,et al.Dielectric and impedance spectroscopy of lead-free 0.99[(Bi0.5Na0.4K0.1)(Ti0.980Nb0.020)O3]-0.01(Ba0.7Sr0.3)TiO3 ceramics [J].Physica B:Condensed Matter,2014,444:27-33.
[29]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 [J].Physica B:Condensed Matter,2016,496:20-25.
[30]Acharya S K,Ahn B G,Jung C U,et al.Effect of Rb doping on ferroelectric and piezoelectric properties of Bi0.5Na0.5TiO3-BaTiO3 thin films [J].Journal of Alloys and Compounds,2014,603:248-254.
本文系“第十七届全国电介质会议暨第十九届全国电子元件会议及2018国际固态制冷材料和器件研讨会”会议论文。