ZrO_2掺杂对Ba(Mg_(1/3)Ta_(2/3))O_3陶瓷结构及介电性能的影响
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摘要
采用固相烧结法制备Ba(Mg_(1/3)Ta_(2/3))O_3+x%ZrO_2(BMZT)微波介质陶瓷,研究了ZrO_2掺杂对Ba(Mg_(1/3)Ta_(2/3))O_3(BMT)微波介质陶瓷结构和介电性能的影响。结果表明:陶瓷体系中存在2种相,主晶相Ba(Mg_(1/3)Ta_(2/3))O_3和附加相Ba_(0.5)TaO_3。随着x的增大,陶瓷体系的相结构由六方结构逐渐向立方结构转变,同时有序相由1:2有序结构逐渐向1:1有序结构转变。添加适量的ZrO_2可以促进液相烧结,当x=8时,陶瓷致密化烧结温度由纯相时的1 650℃以上降至1 450℃,表观密度ρ=7.568 g/cm~3,相对理论密度达到99.1%,BMZT体系拥有良好的微波介电性能:相对介电常数ε_r=25.5,品质因数与谐振频率的乘积Qf=137 600 GHz(8GHz),谐振频率温度系数τ_f=0.3×10~(-6)/℃。
Ba(Mg_(1/3)Ta_(2/3))O_3(BMT) ceramic with ZrO_2(BMZT) was prepared by a solid-state reaction technique.The structure and microwave dielectric properties were investigated.The results show that there are two phases in the ceramic,i.e.,main crystalline phase of Ba(Mg_(1/3)Ta_(2/3))O_3 and secondary phase of Ba_(0.5)TaO_3.The crystal structure is transformed from a hexagonal structure to a cubic structure and the ordered phase is transformed from the 1:2 ordered structure to the 1:1 ordered structure when x value increases.It is indicated that the liquid phase sintering can be improved when an appropriate amount of ZrO_2 is added.Compared to pure BMT ceramic,when x = 8,the BMZT ceramic shows a lower sintering temperature,its apparent density ρ is 7.568 g/cm~3,its relative theoretical density is 99.1%and BMZT possesses superior microwave dielectric properties(i.e.,relative dielectric constant ε_r of 25.5.the quality factor plus resonant frequency Qf of 137 600 GHz(8 GHz),and the temperature coefficient of resonant frequency value τ_f of 0.3 × 10~(-6)/℃).
Ba(Mg_(1/3)Ta_(2/3))O_3(BMT) ceramic with ZrO_2(BMZT) was prepared by a solid-state reaction technique.The structure and microwave dielectric properties were investigated.The results show that there are two phases in the ceramic,i.e.,main crystalline phase of Ba(Mg_(1/3)Ta_(2/3))O_3 and secondary phase of Ba_(0.5)TaO_3.The crystal structure is transformed from a hexagonal structure to a cubic structure and the ordered phase is transformed from the 1:2 ordered structure to the 1:1 ordered structure when x value increases.It is indicated that the liquid phase sintering can be improved when an appropriate amount of ZrO_2 is added.Compared to pure BMT ceramic,when x = 8,the BMZT ceramic shows a lower sintering temperature,its apparent density ρ is 7.568 g/cm~3,its relative theoretical density is 99.1%and BMZT possesses superior microwave dielectric properties(i.e.,relative dielectric constant ε_r of 25.5.the quality factor plus resonant frequency Qf of 137 600 GHz(8 GHz),and the temperature coefficient of resonant frequency value τ_f of 0.3 × 10~(-6)/℃).
引文
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[19]SURENDRAN K P,SEBASTIAN M T,et al.The effect of dopants on the microwave dielectric properties of Ba(Mg_(0.33)Ta_(0.67))O_3 ceramics[J].J Appl Phys,2005,98(9):1-9.
[20]DESU S B,O'BRYAN H M.Microwave loss quality of BZT ceramics[J].J Am Ceram Soc,1985,68(10):546-551.
[21]陈黎,吴孟强,肖勇,等.Ca-B-Si掺杂对Ba(Zn_(1/3)Ta_(2/3))O_3陶瓷介电性能的影响[J].硅酸盐学报,2011,39(11):1787-1791.CHEN Li,WU Mengqiang,XIAO Yong,et al.J Chin Ceram Soc,2011,39(11):1787-1791.
[22]TANG B,FANG Z X,LI Y X,ZHANG X,ZHANG S R.Microwave dielectric properties of Ba(Co_(0.56)Y_(0.04)Zn_(0.35)_(1/3)Nb_(2/3+x)O_3(x=-0.004~0.008)ceramics[J].J Mater Sci:Mater Electron,2015,26(9):6585-6591.
[23]COLLA E L,REANEY I M,SETTER N.Effect of structural changes in complex perovskites on the temperature coefficient of the relative permittivity[J].J Appl Phys,1993,74(5):3414-3425.
[2]SHI F,DONG H L.Correlation of phonon characteristics and crystal structures of Ba[Zn_(1/3)(Nb_(1-x)Ta_x)_(2/3)]O_3 solid solutions[J].J Appl Phys,2012,111(1):014111-014115.
[3]HUGHES H,IDDLES D M,REANEY I M.Niobate-based microwave dielectrics suitable for third generation mobile phone base stations[J].Appl Phys Lett,2001,79(18):2952-2954.
[4]YANG J I,NAHM S,CHOI C H,LEE H J,PARK H M.Microstructure and microwave dielectric properties of Ba(Zn_(1/3)Ta_(2/3))O_3 ceramics with ZrO_2 addition[J].J Am Ceram Soc,2002,85(1):165-168.
[5]SUN T L,CHEN X M.Raman spectra analysis for Ba[(Mg_(1-x)Ni_x)_(1/3)Nb_(2/3)]O_3 microwave dielectric ceramics[J].AIP Adv,2015,5(1):3-26.
[6]ICHINOSE N,SHIMADA T.Effect of grain size and secondary phase on microwave dielectric properties of Ba(Mg_(1/3)Ta_(2/3))O_3 and Ba([Mg,Zn]_(1/3)Ta_(2/3))O_3 systems[J].J Eur Ceram Soc,2006,26(10/11):1755-1759.
[7]KUZHICHALIL P,SURENDRAN,MAILADIL T,et al.Effect of nonstoichiometry on the structure and microwave dielectric properties ofBa(Mg_(0.33)Ta_(0.67))O_3[J].Chem Mater,2004,17(1):142-151.
[8]WANG C H,JING X P,et al.XRD and Raman studies on the ordering/disordering of Ba(Mg_(1/3)Ta_(2/3))O_3[J].J Am Ceram Soc,2009,92(7):1547-1551.
[9]NING P F,LI L X,et al.Raman scattering,electronic structure and microwave dielectric properties of Ba([Mg_(1-x)Zn_x]_(1/3)Ta_(2/3))O_3ceramics[J].Ceram Int,2012,38(2):1391-1398.
[10]KIM B J,KIM M H,NAHM S,et al.Effect of B_2O_3 on the microstructure and microwave dielectric properties of Ba(Mg_(1/3)Ta_(2/3))O_3 ceramics[J].J Eur Ceram Soc,2007,27(2/3):1065-1069.
[11]MATSUMOTO K,HIUGA T,TAKADA K,et al.Ba(Mg_(1/3)Ta_(2/3))O_3ceramics with ultra-low loss at microwave frequencies[C].IEEE Trans Ultrason Ferroelectr Frequency Control,1986,33(6):118-121.
[12]CHEN X M,SUZUKI Y.Sinterability improvement of Ba(Mg_(1/3)Ta_(2/3))O_3 dielectric ceramics[J].J Mater Electronics,1994,5(6):244-247.
[13]TIEN L C,CHOU C C,TSAI D S.Microstructure of Ba(Mg_(1/3)Ta_(2/3))O_3-BaSnO_3 microwave dielectrics[J].Ceram Int,2000,26(1):57-62.
[14]SEBASTIAN M T,SURENDRAN K P.Tailoring the microwave dielectric properties of Ba(Mg_(1/3)Ta_(2/3))O_3 ceramics[J].J Eur Ceram Soc,2006,26(10/11):1791-1799.
[15]SHIMADA T.Far-infrared reflection and microwave properties of Ba([Mg_(1-x)Zn_x]_(1/3),Ta_(2/3))O_3 ceramics[J].J Eur Ceram Soc,2004,24(6):1799-1803.
[16]SINY I G,TAO R,KATIYAR R S,GUO R,BHALLA A S.Raman spectroscopy of Mg-Ta order-disorder in Ba(Mg_(1/3)Ta_(2/3))O_3[J].J Phys Chem Solids,1998,59(2):181-195.
[17]KIM Y W,PARK J H,PARK J G.Local cationic ordering behavior in Ba(Mg_(1/3)Nb_(2/3))O_3 ceramic[J].J Eur Ceram Soc,2004,24(6):1775-1779.
[18]董云飞,李杨珍,袁亮亮,等.Ba_(1-3x/2)La_x(Mg_(1/3)Ta_(2/3))O_3陶瓷的微波介电性能(Eng)[J].硅酸盐学报,2008,36(6):739-747.DONG Yunfei,LI Yangzhen,YUAN Liangliang,et al.J Chin Ceram Soc,2008,36(6):739-747.
[19]SURENDRAN K P,SEBASTIAN M T,et al.The effect of dopants on the microwave dielectric properties of Ba(Mg_(0.33)Ta_(0.67))O_3 ceramics[J].J Appl Phys,2005,98(9):1-9.
[20]DESU S B,O'BRYAN H M.Microwave loss quality of BZT ceramics[J].J Am Ceram Soc,1985,68(10):546-551.
[21]陈黎,吴孟强,肖勇,等.Ca-B-Si掺杂对Ba(Zn_(1/3)Ta_(2/3))O_3陶瓷介电性能的影响[J].硅酸盐学报,2011,39(11):1787-1791.CHEN Li,WU Mengqiang,XIAO Yong,et al.J Chin Ceram Soc,2011,39(11):1787-1791.
[22]TANG B,FANG Z X,LI Y X,ZHANG X,ZHANG S R.Microwave dielectric properties of Ba(Co_(0.56)Y_(0.04)Zn_(0.35)_(1/3)Nb_(2/3+x)O_3(x=-0.004~0.008)ceramics[J].J Mater Sci:Mater Electron,2015,26(9):6585-6591.
[23]COLLA E L,REANEY I M,SETTER N.Effect of structural changes in complex perovskites on the temperature coefficient of the relative permittivity[J].J Appl Phys,1993,74(5):3414-3425.