复合钙钛矿型Ba[(Co_(1-x)Mg_x)_(1/3)Nb_(2/3)]O_3基微波陶瓷的结构与性能
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摘要
采用传统固相法制备复合钙钛矿型Ba[(Co_(1-x)Mg_x)_(1/3)Nb_(2/3)]O_3(0.0≤x≤0.4)微波陶瓷。通过介电性能测试,结合X射线衍射仪、拉曼光谱、透射电镜等表征手段,系统研究Mg掺杂对Ba(Co_(1/3)Nb_(2/3))O_3微波陶瓷的B位1:2有序度与性能的影响。结果表明,Mg掺杂能显著提高Ba(Co_(1/3)Nb_(2/3))O_3陶瓷的B位1:2有序度,进而提高材料的品质因子。1 420℃下烧结的掺杂量x=0.2的陶瓷有序度最高,在1 300℃退火24 h后,其B位1:2有序度进一步提高,并且第二相得以消除,获得与传统Ta基复合钙钛矿微波陶瓷相当的微波性能:介电常数ε_r=30.94,品质因子Q·f=63 161 GHz,谐振频率温度系数τ_f=4.1 ppm/℃。
Ba[(Co_(1-x)Mg_x)_(1/3)Nb_(2/3)]O_3(0.0≤x≤0.4) microwave ceramics were prepared by the conventional solid reaction method. The relationship between the B site 1:2 ordering and microwave dielectric properties of Mg-doped Ba(Co_(1/3)Nb_(2/3))O_3 microwave ceramics were clarified using dielectric performance test XRD, Raman and TEM. The results show that the Q·f of Mg-doped Ba(Co_(1/3)Nb_(2/3))O_3 ceramics is increased because the B site 1:2 ordering degree is enhanced. The highest ordering degree of the ceramics doped with x=0.2 is obtained at 1 420 ℃. After annealing at 1 300 ℃ for 24 h, the ordering degree of 1:2 in B site is further improved, and the second phase is eliminated. Microwave properties with ε_r=30.94, Q·f=63 161 GHz, τ_f =4.1 ppm/℃ comparable to those of conventional Ta based composites perovskite microwave ceramics are obtained.
Ba[(Co_(1-x)Mg_x)_(1/3)Nb_(2/3)]O_3(0.0≤x≤0.4) microwave ceramics were prepared by the conventional solid reaction method. The relationship between the B site 1:2 ordering and microwave dielectric properties of Mg-doped Ba(Co_(1/3)Nb_(2/3))O_3 microwave ceramics were clarified using dielectric performance test XRD, Raman and TEM. The results show that the Q·f of Mg-doped Ba(Co_(1/3)Nb_(2/3))O_3 ceramics is increased because the B site 1:2 ordering degree is enhanced. The highest ordering degree of the ceramics doped with x=0.2 is obtained at 1 420 ℃. After annealing at 1 300 ℃ for 24 h, the ordering degree of 1:2 in B site is further improved, and the second phase is eliminated. Microwave properties with ε_r=30.94, Q·f=63 161 GHz, τ_f =4.1 ppm/℃ comparable to those of conventional Ta based composites perovskite microwave ceramics are obtained.
引文
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[33]KIM B K,HAMAGUCHI H O,KIM I T,et al.Probing of 1:2ordering in Ba(Ni1/3Nb2/3)O3 and Ba(Ni1/3Nb2/3)O3 ceramics by XRD and Raman Spectroscopy[J].Journal of the American Ceramic Society,1995,78(11):3117-3120.
[34]CHEN M Y,CHIA C T,LIN I N,et al.Microwave properties of Ba(Mg1/3Ta2/3)O3,Ba(Mg1/3Nb2/3)O3 and Ba(Co1/3Nb2/3)O3ceramics revealed by Raman scattering[J].Journal of the European Ceramic Society,2006,26(10/11):1965-1968.
[35]DIAO C L,WANG C H,LUO N N,et al.First-principle calculation and assignment for vibrational spectra of Ba(Mg1/3Nb2/3)O3 microwave dielectric ceramic[J].Journal of Applied Physics,2014,115(11):1-12.
[36]MOREIRA R L,MATINAGA F M,DIAS A.Ramanspectroscopic evaluation of the long-range order in Ba(B1/3′B2/3″)O3 ceramics[J].Applied Physics Letters,2001,78(4):428-430.
[37]KIM Y W,PARK J H,PARK J G.Local cationic ordering behaviour in Ba(Mg1/3Nb2/3)O3 ceramics[J].Journal of European Ceramics Society,2004,24(6):1830-1834.
[2]SUN T L,MAO M M,CHEN X M.Effects of annealing atmospheres on microwave dielectric properties of Ba[(Mg1-xCox)1/3Nb2/3]O3 ceramics[J].Materials Research Bulletin,2015,68(2015):142-149.
[3]HIGUCHI Y,TAMURA H.Recent progress on the dielectric properties of dielectric resonator materials with their applications from microwave to optical frequencies[J].Journal of the European Ceramic Society,2003,23(14):2683-2688.
[4]SEBASTIAN M T,UBIC R,JANTUNEN H.Low-loss dielectric ceramic materials and their properties[J].International Materials Reviews,2015,60(7):392-412.
[5]HUGHES H,IDDLES D M,REANEY I M.Niobate-based microwave dielectrics suitable for third generation mobile phone base stations[J].Applied Physics Letters,2001,79(18):2952-2954.
[6]LIU S,TAYLOR R,PETROVIC N S,et al.Experimental and theoretical investigation of the structural,chemical,electronic,and high frequency dielectric properties of barium cadmium tantalate–based ceramics[J].Journal of Applied Physics,2005,97(1):1-8.
[7]DAVIES P K,TONG J.Effect of ordering-induced domain boundaries on low-loss BZT-Ba Zr O3 perovskite microwave dielectrics[J].Journal of the American Ceramic Society,1997,80(7):1727-1740.
[8]KIM I T,KIM Y H,CHUNG S J.Order-disorder transition and microwave dielectric properties of Ba(Ni1/3Nb2/3)O3 ceramics[J].Japanese Journal of Applied Physics,1995,34(8R):4096-4103.
[9]DONG H,SHI F.Effects of Synthesis temperatures on crystal structures and lattice vibration modes of(Ba0.3Sr0.7)[(Zn1–xMgx)1/3Nb2/3]O3 solid solutions[J].Metallurgical and Materials Transactions A,2012,43(13):5128-5139.
[10]KIM I T,KIM Y H.Ordering and microwave dielectric properties of Ba(Ni1/3Nb2/3)O3 ceramics[J].Journal of Materials Research,1996,12(2):518-525.
[11]WANG Z F,HUANG B Y,WANG L X,et al.Low loss(Ba1-xSrx)(Co1/3Nb2/3)O3 solid solution:phase evolution,microstructure and microwave dielectric properties[J].Journal of Materials Science:Material Electron,2015,26:4273-4279.
[12]GALASSO F,PYLE J.Ordering in compounds of the A(B′0.33-Ta0.67)O3 type[J].Inorganic Chemistry,1963,2(3):482-484.
[13]DIAS A,CIMINELLI V S T,MATINAGA F M,et al.Raman scattering and X-ray diffraction investigations on hydrothermal barium magnesium niobate ceramics[J].Journal of the European Ceramic Society,2001,21(15):2739-2744.
[14]REANEY I M.Microwave dielectric ceramics for resonators and filters in mobiles phone networks[J].Journal of the American Ceramic Society,2006,89(7):2063-2072.
[15]ZHANG S,DEVONPORT A,NEWMAN N,et al.Main source of microwave loss in transition-metal-doped Ba(Zn1/3Ta2/3)O3and Ba(Zn1/3Nb2/3)O3 at cryogenic temperatures[J].Journal of the American Ceramic Society,2015,98(4):1188-1194.
[16]LIU H X,TIAN Z Q,WANG H,et al.New microwave dielectric ceramics with near-zeroτf in the Ba(Mg1/3Nb2/3)O3-Ba(Ni1/3Nb2/3)O3 system[J].Journal of Materials Science,2004,39(13):4319-4320.
[17]SCOTT R I,THOMAS M,HAMPSON C.Development of low cost,high performance Ba(Zn1/3Nb2/3)O3 based materials for microwave resonator applications[J].Journal of the European Ceramic Society,2003,23(14):2467-2471.
[18]KIM M H,JEONG Y H,NAHM S,et al.Effect of B2O3 and Cu O additives on the sintering temperature and microwave dielectric properties of Ba(Zn1/3Nb2/3)O3 ceramics[J].Journal of the European Ceramic Society,2006,26(10/11):2139-2142.
[19]AHN C W,NAHM S,LIM Y S,et al.Microstructure and microwave dielectric properties of Ba(Co1/3Nb2/3)O3 ceramics[J].Japanese Journal of Applied Physics,2002,41(8):5277-5280.
[20]DAVIES P K,TONG J.Effect of ordering-induced domain boundaries on low-loss BZT-Ba Zr O3 perovskite microwave dielectrics[J].Journal of the American Ceramic Society,1997,80(7):1727-1740.
[21]ENDO K,FUJIMOTO K,MURAKAWA K.Dielectric properties of ceramics in Ba(Co1/3Nb2/3)O3–Ba(Zn1/3Nb2/3)O3solid solution[J].Journal of the American Ceramic Society,1987,70(9):215-218.
[22]MOLODETSKY I,DAVIES P K.Effect of Ba(Y1/2Nb1/2)O3 and Ba Zr O3 on the cation order and properties of Ba(Co1/3Nb2/3)O3microwave ceramics[J].Journal of the European Ceramic Society,2001,21(15):2587-2591.
[23]AZOUGH F,LEACH C,FREER R.Effect of nonstoichiometry on the structure and microwave dielectric properties of Ba(Co1/3Nb2/3)O3 ceramics[J].Journal of the European Ceramic Society,2006,26(14):2877-2884.
[24]SURENDRAN K P,MOHANAN P,JACOB M V.The effect of dopants on the microwave dielectric properties of Ba(Mg0.333Ta0.67)O3[J].Journal of Applied Physics,2005,98(9):1-9.
[25]KIM E S,YOON K H.Effect of nickel on microwave dielectric properties of Ba(Mg1/3Ta2/3)O3[J].Journal of Materials Science,1994,29(3):830-834.
[26]YOU C C,HUANG C L,WEI C C,et al.Improved high-Q dielectric resonator sintered at low firing temperature[J].Japanese Journal of Applied Physics,1995,34:1911-1915.
[27]HAKKI B W,COLEMAN P D.A dielectric resonator method of measuring inductive capacities in the millimeter range[J].IRE Transactions on Microwave Theory and Techniques,2002,8(4):402-410.
[28]COURTNEY W E.Analysis and evaluation of a method of measuring the complex permittivity and permeability microwave insulators[J].IEEE Transactions on Mocrowave Theory and Techniques,1970,18(8):476-485.
[29]SHANNON R D.Revised effective ionic radii and systematic studies of interatomie distances in halides and chaleogenides[J].Acta Crystallographica,1976,32(SEP1):751-767.
[30]WU H,DAVIES P K.Influence of non-stoichiometry on the structure and properties of Ba(Zn1/3Nb2/3)O3 microwave dielectrics_I.Substitution of Ba3W2O9[J].Journal of the American Ceramic Society,2006,89(7):2239-2249.
[31]JACOBSO A J,COLLINS B M,FENDE B E F.A powder neutron and X-ray diffraction determination of the structure of Ba3Ta2Zn O9:An investigation of perovskite phases in the system Ba-Ta-Zn-O and the preparation of Ba2Ta Cd O5.5 and Ba2Ce In O5.5[J].Acta Crystallographica Section B:Structural Crystallography and Crystal Chemistry,1976,32(4):1083-1087.
[32]WU H,DAVIES P K.Influence of non-stoichiometry on the structure and properties of Ba(Zn1/3Nb2/3)O3 microwave dielectrics_II.compositional variations in Pure BZN[J].Journal of the American Ceramic Society,2006,89(7):2050-2063.
[33]KIM B K,HAMAGUCHI H O,KIM I T,et al.Probing of 1:2ordering in Ba(Ni1/3Nb2/3)O3 and Ba(Ni1/3Nb2/3)O3 ceramics by XRD and Raman Spectroscopy[J].Journal of the American Ceramic Society,1995,78(11):3117-3120.
[34]CHEN M Y,CHIA C T,LIN I N,et al.Microwave properties of Ba(Mg1/3Ta2/3)O3,Ba(Mg1/3Nb2/3)O3 and Ba(Co1/3Nb2/3)O3ceramics revealed by Raman scattering[J].Journal of the European Ceramic Society,2006,26(10/11):1965-1968.
[35]DIAO C L,WANG C H,LUO N N,et al.First-principle calculation and assignment for vibrational spectra of Ba(Mg1/3Nb2/3)O3 microwave dielectric ceramic[J].Journal of Applied Physics,2014,115(11):1-12.
[36]MOREIRA R L,MATINAGA F M,DIAS A.Ramanspectroscopic evaluation of the long-range order in Ba(B1/3′B2/3″)O3 ceramics[J].Applied Physics Letters,2001,78(4):428-430.
[37]KIM Y W,PARK J H,PARK J G.Local cationic ordering behaviour in Ba(Mg1/3Nb2/3)O3 ceramics[J].Journal of European Ceramics Society,2004,24(6):1830-1834.