Effect of the Oxidizing Atmosphere on the Microstructure and Dielectric Properties of CaCu3Ti4O12 Ceramics

doi:10.15541/jim20150184

Abstract

Abstract:

CaCu₃Ti₄O₁₂ ceramics were synthesized by using the solid-state reaction method, and the roles of heat-treatment in the oxidizing atmosphere on the microstructure and dielectric properties were investigated in this work. It is indicated that after heat-treatment in the oxidizing atmosphere, the dielectric constant is decreased slightly and the dielectric loss tangent is effectively suppressed to 0.03-0.04. In the temperature range of 183-273 K, the dielectric loss is composed of conductance loss and two relaxation loss peaks. It is worth noting that the conductance loss at low frequency is reduced obviously. The result impedance spectra analysis reveals that the grain boundary resistance of CaCu₃Ti₄O₁₂ ceramics is boosted from 1.8×10⁴ Ω to 8.6×10⁴ Ω at 393 K. Furthermore, the results from volt-ampere characteristics (J-E) exhibit that the breakdown field and nonlinear coefficient of CaCu₃Ti₄O₁₂ ceramics are increased from 226 V/mm and 3.52 to 397 V/mm and 4.51, respectively. The barrier height is also increased from 0.56 eV to 0.63 eV.

Key words: CaCu3Ti4O12 ceramics, oxidizing atmosphere, dielectric properties

CLC Number:

TM283

ZHAO Xue-Tong, REN Lu-Lu, LIAO Rui-Jin, LI Jian-Ying, WANG Fei-Peng. Effect of the Oxidizing Atmosphere on the Microstructure and Dielectric Properties of CaCu₃Ti₄O₁₂ Ceramics[J]. Journal of Inorganic Materials, 2015, 30(12): 1303-1309.

Figures/Tables 8

Fig. 1 XRD patterns of CCTO-A(a) and CCTO-B(b) ceramics

Fig. 2 SEM images of CCTO-A (a) and CCTO-B(b) ceramics

Fig. 3 Dielectric frequency spectra of CCTO-A and CCTO-B samples measured at room temperature

Fig. 4 Dielectric frequency spectra of CCTO samples measured in 183-273 K and the calculation of the activation energy for the relaxation peaks. The fitting results of dielectric loss at 273 K in the inset of (a) and (c). (a, b) CCTO-A; (c, d) CCTO-B

Fig. 5 Complex impedance plane measured at 393 K for CCTO-A and CCTO-B samples. Inset is expanded curves of the high-frequency data

Fig. 6 Complex impedance plane measured in 348-473 K for CCTO-A (a) and CCTO-B (b), and the variation of the conductivity for the samples (c) with increasing temperature

Fig. 7 J-E curves measured at room temperature for CCTO-A and CCTO-B samples

Fig. 8 lnJ versus E1/2 plot for CCTO-A (a) and CCTO-B (b) in the temperature of 308-368 K. Calculation of barrier height is shown in the inset (E=0)

References 25

[1]	SUBRAMANIAN M A, LI D, DUAN N, et al.High dielectric constant in ACu3Ti4O12 and ACu3Ti3FeO12 phases.J. Solid State Chem., 2000, 151(2): 323-325.
[2]	HOMES C C, VOGT T, SHAPIRO S M, et al.Optical response of high-dielectric-constant perovskite-related oxide.Science, 2001, 293(5530): 673-676.
[3]	LIU Y, WITHERS R L, WEI X Y. Structurally frustrated relaxor ferroelectric behavior in CaCu3Ti4O12. Phys. Rev. B, 2005, 72(13): 134104-1-4.
[4]	HE L, NEATON J B, COHEN M H, et al. First-principles study of the structure and lattice dielectric response of CaCu3Ti4O12. Phys. Rev. B, 2002, 65(21): 214112-1-11.
[5]	COHEN M H, NEATON J B, HE L, et al.Extrinsic models for the dielectric response of CaCu3Ti4O12.J. Appl. Phys., 2003, 94(5): 3299-3306.
[6]	SINCLAIR D C, ADAMS T B, MORRISON F D.CaCu3Ti4O12: one-step internal barrier layer capacitor.Appl. Phys. Lett., 2002, 80(12): 2153-2155.
[7]	HAO W T, ZHANG J L, TAN Y Q, et al.Origin of giant dielectric permittivity in CaCu3Ti4O12 ceramics.J. Inorg. Mater., 2011, 26(10): 1058-1062.
[8]	BÄRNER K, LUO X J, SONG X P, et al. Correlation between the trap state spectra and dielectric behavior of CaCu3Ti4O12.J. Mater. Res., 2011, 26(1): 36-44.
[9]	LUO X J, YANG C P, SONG X P, et al.Dielectric and impedance performances of giant dielectric constant oxide CaCu3Ti4O12. Acta Phys. Sin., 2012, 59(5): 3516-3522.
[10]	LI J Y, ZHAO X T, GU F, et al. Defects and dc electrical degradation in CaCu3Ti4O12 ceramics: Role of oxygen vacancy migration. Appl. Phys. Lett., 2012, 100(22): 202905-1-4.
[11]	ZHAO X T, LI J Y, LI H, et al. Intrinsic and extrinsic defect relaxation behavior of ZnO ceramics. J. Appl. Phys., 2012, 111(12): 124106-1-8.
[12]	ZHAO X T, LIAO R J, LIANG N C, et al. Role of defects in determining the electrical properties of ZnO ceramics. J. Appl. Phys., 2014, 116(1): 014103-1-10.
[13]	ZANG G Z, ZHANG J L, ZHENG P J.Grain boundary effect on the dielectric properties of CaCu3Ti4O12 ceramics.J. Phys. D: Appl. Phys., 2005, 38(11): 1824-1827.
[14]	FANG T T, MEI L T, HO H F.Effects of Cu stoichiometry on the micro structures, barrier-layer structures, electrical conduction, dielectric responses, and stability of CaCu3Ti4O12.Acta Mater., 2006, 54(10): 2867-2875.
[15]	VANGCHANGYIA S, SWATSITANG E, THONGBAI P, et al.Very low loss tangent and high dielectric permittivity in pure- CaCu3Ti4O12 ceramics prepared by a modified Sol-Gel process. J. Am. Ceram. Soc., 2012, 95(5): 1497-1500.
[16]	YU R, XUE H, CAO Z L, CHEN L, et al.Effect of oxygen sintering atmosphere on the electrical behavior of CCTO ceramics.J. Eur. Ceram. Soc., 2012, 32(6): 1245-1249.
[17]	陈季丹, 刘子玉. 电介质物理学. 北京: 机械工业出版社, 1982: 155-160.
[18]	ADAMS T B, SINCLAIR D C, WEST A R. Characterization of grain boundary impedances in fine- and coarse-grained CaCu3Ti4O12 ceramics. Phys. Rev. B, 2006, 73(9): 094124-1-9.
[19]	ZHANG J L, ZHENG P, WANG C L, et al. Dielectric dispersion of CaCu3Ti4O12 ceramics at high temperatures. Appl. Phys. Lett., 2005, 87(14): 142901-1-3.
[20]	SINCLAIR D C, WEST A R.Impedance and modulus spectroscopy of semiconducting BaTiO3 showing positive temperature- coefficient of resistance.J. Appl. Phys., 1989, 66(8): 3850-3856.
[21]	DENG G C, LI G R, DING A L, et al. Evidence for oxygen vacancy inducing spontaneous normal-relaxor transition in complex perovskite ferroelectrics. Appl. Phys. Lett., 2005, 87(19): 192905-1-3.
[22]	WHANGBO M H, SUBRAMANIAN M A.Structural model of planar defects in CaCu3Ti4O12 exhibiting a giant dielectric constant.Chem. Mater., 2006, 18(14): 3257-3260.
[23]	张美蓉. ZnO压敏陶瓷老化机理的研究. 西安: 西安交通大学博士学位论文, 1991.
[24]	YANG Z, ZHANG Y, ZHANG K, et al.Effect of grain-boundary behavior on the dc electric conduction in Rb-doped CaCu3Ti4O12,J. Mater. Sci.: Mater. Electron., 2013, 24: 1063-1067.
[25]	成鹏飞. 稀土氧化物对ZnO-Bi2O3系压敏陶瓷晶界结构和电气性能的影响. 西安: 西安交通大学博士学位论文, 2008.

Effect of the Oxidizing Atmosphere on the Microstructure and Dielectric Properties of CaCu₃Ti₄O₁₂ Ceramics

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