Sintering Behavior and Microwave Dielectric Properties of BBSZL Glass-doped ZnTiO₃ Ceramics for LTCC Applications

Abstract

A novel low temperature co-fired ceramic (LTCC) material was fabricated by zinc titanate (ZnTiO₃) ceramics doped with B₂O₃-BaO-SiO₂-ZnO-Li₂O (BBSZL) glass. The influences of BBSZL glass on wetting behavior, sintering activation energy, phase composition, microstructure and microwave dielectric properties were investigated. The experimental results show that the sintering temperature of ZnTiO₃ ceramics can be reduced from 1 100 to 925 °C, meanwhile the sintering activation energy is decreased from 465.32 to 390.54 kJ·mol^-1 by BBSZL glass aid, respectively. Moreover, BBSZL glass can inhibit the high Q×f ZnTiO₃ phase decompose into the low Q×f value Zn₂TiO₄ phase, which is propitious to obtain high Q×f value LTCC material. The ZnTiO₃-BBSZL composite sintered at 925 °C displays the excellent microwave dielectric properties with ε_r of 21.8, Q×f value of 42000 GHz, and τ_f of -75 ppm·°C^-1.

Keywords

ZnTiO₃ ceramics / BBSZL glass / sintering behavior / dielectric properties

References

[1] Sebastian MT, Jantunen H. Low Loss Dielectric Materials for LTCC Applications: A Review[J]. Int. Mat. Rev., 2008, 53: 57-90.

[2] Yang WR, Huang PZ, Huang CL. Microwave Dielectric Properties of low–loss (Zn1−xCox)3Nb2O8 ceramics for LTCC applications[J]. J. Alloy. Compd., 2015, 620: 18-23.

[3] Lee YC, Chang CS, Huang YL. Microwave Dielectric Properties and microstructures of Nb2O5–Zn0.95Mg0.05TiO3+0.25TiO2Ceramics with Bi2O3 addition[J]. J. Eur. Ceram. Soc., 2010, 30: 963-970.

[4] Liu XC, Zuo CG. Effect of Copper Vanadate Sintering Aid on the Microstructure and Dielectric Properties of (Zn, Mg)TiO3Ceramics[J]. J. Mater. Sci–Mater. EI., 2016, 27: 5 462.

[5] Yamaguchi O, Morimi M, Kawabata H. J. Am. Ceram. Soc., 2010, 70: For-ation and Transformation of ZnTiO3[J].

[6] Sugiura M, Ikeda K. Studies on the Dielectrics of the TiO2–ZnO System[ J]. J. Ceram. Soc. Jpn., 1947, 55: 62-66.

[7] Chang YS, Chang YH, Chen IG. Synthesis and Characterization of Zinc Titanate Doped with Magnesium[J]. Solid. State. Commun., 2003, 128: 203-208.

[8] Kim HT, Kim Y, Valant M. Titanium Incorporation in Zn2TiO4Spinel Ceramics[J]. J. Am. Ceram. Soc., 2010, 84: 1 081-1 086.

[9] Yuan Y, Zhang S, Zhou X. Low–temperature Sintering and Microwave Dielectric Properties of (Zn0.65Mg0.35)TiO3–CaTiO3 Ceramics with H3BO3 Addition[J]. J. Ceram–Silikaty., 2009, 53: 5-8.

[10] Liu X, Zuo C. Molten Salt Synthesis of (Zn,Mg)TiO3, Micro/Nano Crystals with Pure Hexagonal Ilmenite Structure[J]. J. Mater. Sci–Mater. El., 2016, 27: 8 319-8 324.

[11] Wu SP, Luo JH, Cao SX. Microwave Dielectric Properties of B2O3–doped ZnTiO3Ceramics Made with Sol–gel Technique[J]. J. Alloy. Compd., 2010, 502: 147-152.

[12] Li B, Zhou X, Zhang S. Low–temperature Sintered (Zn0.65Mg0.35)TiO3Microwave Ceramics Doped with CuV2O6[J]. J. Mater. Sci–Mater. El., 2009, 20: 1 123-1 128.

[13] Lee YC, Lee WH, Shao FT. Microwave Dielectric Properties of Zn0.95Mg0.05TiO3+0.25TiO2 Ceramics with 3ZnO–B2O3 Addition[J]. Jpn. J. Appl. Phys., 2004, 43: 7 596-7 599.

[14] Wang YR, Wang SF, Lin YM. Low Temperature Sintering of (Zn1−x Mgx)TiO3 Microwave Dielectrics[J]. Ceram. Int., 2005, 31: 905-909.

[15] Ding Z, Su H, Tang X. Low–temperature Sintering Characteristic and Microwave Dielectric Properties of (Zn0.7Mg0.3)TiO3 Ceramics with LBSCA Glass[J]. Ceram. Int., 2015, 41: 10 133-10 136.

[16] Chao CA. ZnTiO3 Ceramic Sintered at Low Temperature with Glass Phase Addition for LTCC Applications[J]. Mater. Chem. Phys., 2007, 103: 106-111.

[17] Chao CA, Aliouat M, Marinel S. Effects of Additives on the Sintering Temperature and Dielectric Properties of ZnTiO3 Based Ceramic[J]. Ceram. Int., 2007, 33: 245-248.

[18] Zhang QL, Yang H, Zou JL. Sintering and Microwave Dielectric Properties of LTCC–Zinc Titanate Multilayer[J]. Mater. Lett., 2005, 59: 880.

[19] Li B. Dielectric Properties and Microstructure of TiO2 Modified (ZnMg) TiO3 Microwave Ceramics with CaO–B2O3–SiO2[J]. J. Mater. Sci., 2009, 44: 4 993-4 998.

[20] Chai YL, Chang YS, Hsiao YJ. Effects of Borosilicate Glass Addition on the Structure and Dielectric Properties of ZnTiO3 Ceramics[J]. Mater. Res. Bull., 2008, 43: 257-263.

[21] Yu YH, Li HN, Xia M. Research on Low Temperature Sintering of ZnO–TiO2 Ceramics Doped with Li2CO3–B2O3–V2O5[J]. Mater. Review., 2012, 26: 136-139.

[22] Wu SP, Luo JH, Cao SX. Microwave Dielectric Properties of B2O3–doped ZnTiO3 Ceramics Made with Sol–gel Technique[J]. J. Alloy. Compd., 2010, 502: 150-152.

[23] Liu ZC, Zhou DX, Gong SP, Hu YX. Sintering and Phase Transition of 0.25CuO–0.75MoO(3) Doped ZnO–TiO2 Microwave Dielectric Ceramics[ J]. J. Inorg. Mater., 2009, 24: 712-716.

[24] Yue Z, Yan J, Zhao F. Low–temperature Sintering and Microwave Dielectric Properties of ZnTiO3–based LTCC Materials[J]. J. Electroceramic., 2008, 21: 141-144.

[25] Yan J, Yue ZX, Wang J. Effect of ZnO–V2O5 Co–Doping on Phase Stability and Microwave Dielectric Properties of ZnTiO3 Ceramics[J]. Key Eng. Mater., 2007, 336–338: 297-300.

[26] Ren HS, Xie TY, Dang MZ. The Influence of BBZ Glass on Phase Evolution, Sintering Behavior and Dielectric Properties of BaTi4O9 Ceramics[J]. J. Mater. Sci–Mater. El., 2017, 28: 1-8.

[27] Huang CL, Weng MH, Chen HL. Effect of Additives on Microstructure and Microwave Dielectric Properties of (Zr,Sn)TiO4 Ceramic[J]. Mater. Chem. Phys., 2001, 71: 17-22.

[28] Song JB, Song KX, Wei JS, et al. Ionic Occupation, Structures, and Microwave Dielectric Properties of Y3MgAl3SiO12 Garnet–type Ceramics[ J]. J. Am. Ceram. Soc., 2018, 101: 244-251.