Skip to main content

Sintering behaviour and microwave dielectric properties of MgO-2B2O3-xwt%BaCu(B2O5)-ywt%H3BO3 ceramics

Abstract

This study investigates the bulk density, sintering behaviour, and microwave dielectric properties of the MgO-2B2O3 series ceramics synthesised by solid-state reaction. According to the X-ray diffraction and microstructural analyses, the as-prepared MgO-2B2O3 ceramics possess a single-phase structure with a rod-like morphology. The effects of different quantities of H3BO3 and BaCu(B2O5) (BCB) on the bulk density, sintering behaviour, and microwave dielectric properties of the MgO-2B2O3 ceramics were investigated. Accordingly, the optimal sintering temperature was obtained by adding 30 wt% H3BO3 and 8 wt% BCB. We also reduced the sintering temperature to 825 °C. Furthermore, the addition of 40 wt% H3BO3 and 4 wt% BCB increased the quality factor, permittivity, and temperature coefficient of resonance frequency of MgO-2B2O3 to 44,306 GHz (at 15 GHz), 5.1, and −32 ppm/°C, respectively. These properties make MgO-2B2O3 a viable low-temperature co-fired ceramic with broad applications in microwave dielectrics.

References

  1. [1]

    Sebastian MT, Jantunen H. Low loss dielectric materials for LTCC applications: A review. Int Mater Rev 2008, 53: 57–90.

    CAS  Article  Google Scholar 

  2. [2]

    Zhou HF, Liu XB, Chen XL, et al. ZnLi2/3Ti4/3O4: A new low loss spinel microwave dielectric ceramic. J Eur Ceram Soc 2012, 32: 261–265.

    CAS  Article  Google Scholar 

  3. [3]

    Zhou D, Guo D, Li WB, et al. Novel temperature stable high-εr microwave dielectrics in the Bi2O3-TiO2-V2O5 system. J Mater Chem C 2016, 4: 5357–5362.

    CAS  Article  Google Scholar 

  4. [4]

    Zhou D, Pang LX, Wang DW, et al. Novel water-assisting low firing MoO3 microwave dielectric ceramics. J Eur Ceram Soc 2019, 39: 2374–2378.

    CAS  Article  Google Scholar 

  5. [5]

    Dou G, Zhou DX, Guo M, et al. Low-temperature sintered Zn2SiO4-CaTiO3 ceramics with near-zero temperature coefficient of resonant frequency. J Alloys Compd 2012, 513: 466–473.

    CAS  Article  Google Scholar 

  6. [6]

    Wang KG, Zhou HF, Liu XB, et al. A lithium aluminium borate composite microwave dielectric ceramic with low permittivity, near-zero shrinkage, and low sintering temperature. J Eur Ceram Soc 2019, 39: 1122–1126.

    Article  CAS  Google Scholar 

  7. [7]

    Hughes H, Iddles DM, Reaney IM. Niobate-based microwave dielectrics suitable for third generation mobile phone base stations. Appl Phys Lett 2001, 79: 2952–2954.

    CAS  Article  Google Scholar 

  8. [8]

    Li YX, Li H, Tang B, et al. Microwave dielectric properties of low-fired Li2ZnTi3O8-TiO2 composite ceramics with Li2WO4 addition. J Mater Sci: Mater Electron 2015, 26: 1181–1185.

    CAS  Google Scholar 

  9. [9]

    Hao SZ, Zhou D, Hussain F, et al. Structure, spectral analysis and microwave dielectric properties of novel x(NaBi)0.5MoO4−(1−x)Bi2/3MoO4 (x = 0.2 ∼ 0.8) ceramics with low sintering temperatures. J Eur Ceram Soc 2020, 40: 3569–3576.

    CAS  Article  Google Scholar 

  10. [10]

    Bi JX, Xing CF, Yang CH, et al. Phase composition, microstructure and microwave dielectric properties of rock salt structured Li2ZrO3-MgO ceramics. J Eur Ceram Soc 2018, 38: 3840–3846.

    CAS  Article  Google Scholar 

  11. [11]

    Davis HM, Knight MA. The system magnesium oxide-boric oxide. J Am Ceram Soc 1945, 28: 97–102.

    CAS  Article  Google Scholar 

  12. [12]

    Nishizuka M, Ogawa H, Kan A, et al. Synthesis and microwave dielectric properties of MgO-xmol%B2O3 (x = 33 and 25) ceramics in MgO-B2O3 system. Ferroelectrics 2009, 388: 101–108.

    CAS  Article  Google Scholar 

  13. [13]

    Peng R, Li YX, Su H, et al. Three-phase borate solid solution with low sintering temperature, high-quality factor, and low dielectric constant. J Am Ceram Soc 2021, 104: 3303–3315.

    CAS  Article  Google Scholar 

  14. [14]

    Peng R, Su H, Li YX, et al. Microstructure and microwave dielectric properties of Ni doped zinc borate ceramics for LTCC applications. J Alloys Compd 2021, 868: 159006.

    CAS  Article  Google Scholar 

  15. [15]

    Peng R, Su H, An D, et al. The sintering and dielectric properties modification of Li2MgSiO4 ceramic with Ni2+-ion doping based on calculation and experiment. J Mater Res Technol 2020, 9: 1344–1356.

    CAS  Article  Google Scholar 

  16. [16]

    Fan GC, Zhou HF, Chen XL. Optimized sintering temperature and enhanced microwave dielectric performance of Mg2B2O5 ceramic. J Mater Sci: Mater Electron 2017, 28: 818–822.

    CAS  Google Scholar 

  17. [17]

    Zhou HF, Tan XH, Liu XB, et al. Low permittivity MgO-xB2O3-yBaCu(B2O5) microwave dielectric ceramics for low temperature co-fired ceramics technology. J Mater Sci: Mater Electron 2018, 29: 18486–18492.

    CAS  Google Scholar 

  18. [18]

    Zhou HF, Tan XH, Wang KG, et al. Microstructure and sintering behavior of low temperature cofired Li4/5Mg4/5Ti7/5O4 ceramics containing BaCu(B2O5) and TiO2 and their compatibility with a silver electrode. RSC Adv 2017, 7: 44706–44711.

    CAS  Article  Google Scholar 

  19. [19]

    Guo HH, Zhou D, Du C, et al. Temperature stable Li2Ti0.75(Mg1/3Nb2/3)0.25O3-based microwave dielectric ceramics with low sintering temperature and ultra-low dielectric loss for dielectric resonator antenna applications. J Mater Chem C 2020, 8: 4690–4700.

    CAS  Article  Google Scholar 

  20. [20]

    Iddles DM, Bell AJ, Moulson AJ. Relationships between dopants, microstructure and the microwave dielectric properties of ZrO2-TiO2-SnO2 ceramics. J Mater Sci 1992, 27: 6303–6310.

    CAS  Article  Google Scholar 

  21. [21]

    Wu JM, Huang HL. Microwave properties of zinc, barium and lead borosilicate glasses. J Non-Cryst Solids 1999, 260: 116–124.

    CAS  Article  Google Scholar 

  22. [22]

    Tzou WC, Yang CF, Chen YC, et al. Improvements in the sintering and microwave properties of BiNbO4 microwave ceramics by V2O5 addition. J Eur Ceram Soc 2000, 20: 991–996.

    CAS  Article  Google Scholar 

  23. [23]

    Li EZ, Chen YW, Xiong J, et al. Low-temperature firing and microwave dielectric properties of Ba-Nd-Ti with composite doping Li-B-Si and Ba-Zn-B glasses. J Mater Sci: Mater Electron 2016, 27: 8428–8432.

    CAS  Google Scholar 

  24. [24]

    Kim MH, Lim JB, Kim JC, et al. Synthesis of BaCu(B2O5) ceramics and their effect on the sintering temperature and microwave dielectric properties of Ba(Zn1/3Nb2/3)O3 ceramics. J Am Ceram Soc 2006, 89: 3124–3128.

    CAS  Article  Google Scholar 

  25. [25]

    Huang CL, Weng MH, Lion CT, et al. Low temperature sintering and microwave dielectric properties of Ba2Ti9O20 ceramics using glass additions. Mater Res Bull 2000, 35: 2445–2456.

    CAS  Article  Google Scholar 

  26. [26]

    Zhou HF, Wang H, Zhou D, et al. Effect of ZnO and B2O3 on the sintering temperature and microwave dielectric properties of LiNb0.6Ti0.5O3 ceramics. Mater Chem Phys 2008, 109: 510–514.

    CAS  Article  Google Scholar 

  27. [27]

    Li EZ, Niu N, Wang J, et al. Effect of Li-B-Si glass on the low temperature sintering behaviors and microwave dielectric properties of the Li-modified ss-phase Li2O-Nb2O5-TiO2 ceramics. J Mater Sci: Mater Electron 2015, 26: 3330–3335.

    CAS  Google Scholar 

  28. [28]

    Zhou D, Pang LX, Wang DW, et al. High permittivity and low loss microwave dielectrics suitable for 5G resonators and low temperature co-fired ceramic architecture. J Mater Chem C 2017, 5: 10094–10098.

    CAS  Article  Google Scholar 

  29. [29]

    Pang LX, Zhou D, Qi ZM, et al. Structure-property relationships of low sintering temperature scheelite-structured (1−x)BiVO4−xLaNbO4 microwave dielectric ceramics. J Mater Chem C 2017, 5: 2695–2701.

    CAS  Article  Google Scholar 

  30. [30]

    Lu XY, Fang BJ, Zhang S, et al. Decreasing sintering temperature for BCZT lead-free ceramics prepared via hydrothermal route. Funct Mater Lett 2017, 10: 1750046.

    CAS  Article  Google Scholar 

  31. [31]

    Huang CL, Wang JJ, Huang CY. Sintering behavior and microwave dielectric properties of nano alpha-alumina. Mater Lett 2005, 59: 3746–3749.

    CAS  Article  Google Scholar 

  32. [32]

    Bafrooei HB, Feizpour M, Sayyadi-Shahraki A, et al. High-performance ZnTiNb2O8 microwave dielectric ceramics produced from ZnNb2O6-TiO2 nano powders. J Alloys Compd 2020, 834: 155082.

    CAS  Article  Google Scholar 

  33. [33]

    Liu F, Liu SJ, Cui XJ, et al. Ordered domains and microwave properties of sub-micron structured Ba(Zn1/3Ta2/3)O3 ceramics obtained by spark plasma sintering. Materials 2019, 12: 638.

    CAS  Article  Google Scholar 

  34. [34]

    Bari M, Taheri-Nassaj E. Taghipour-Armaki H. Role of nano- and micron-sized particles of TiO2 additive on microwave dielectric properties of Li2ZnTi3O8-4wt% TiO2 ceramics. J Am Ceram Soc 2013, 96: 3737–3741.

    CAS  Article  Google Scholar 

  35. [35]

    Yoon SH, Choi GK, Kim DW, et al. Mixture behavior and microwave dielectric properties of (1−x)CaWO4−xTiO2. J Eur Ceram Soc 2007, 27: 3087–3091.

    CAS  Article  Google Scholar 

  36. [36]

    Pan HL, Mao YX, Cheng L, et al. New Li3Ni2NbO6 microwave dielectric ceramics with the orthorhombic structure for LTCC applications. J Alloys Compd 2017, 723: 667–674.

    CAS  Article  Google Scholar 

  37. [37]

    Zhang P, Hao MM, Mao XR, et al. A novel low sintering temperature scheelite-structured CaBiVMoO8 microwave dielectric ceramics. J Alloys Compd 2020, 840: 155187.

    CAS  Article  Google Scholar 

  38. [38]

    Lim JB, Nahm S, Kim HT, et al. Effect of B2O3 and CuO on the sintering temperature and microwave dielectric properties of the BaTi4O9 ceramics. J Electroceramics 2006, 17: 393–397.

    CAS  Article  Google Scholar 

  39. [39]

    Navias L, Green FL. Dielectric properties of glasses at ultra-high frequencies and their relation to composition. J Am Ceram Soc 1946, 29: 267–276.

    CAS  Article  Google Scholar 

  40. [40]

    Tang B, Guo X, Yu SQ, et al. The shrinking process and microwave dielectric properties of BaCu(B2O5)-added 0.85BaTi4O9-0.15BaZn2Ti4O11 ceramics. Mater Res Bull 2015, 66: 163–168.

    CAS  Article  Google Scholar 

  41. [41]

    Ullah B, Lei W, Cao QS, et al. Structure and microwave dielectric behavior of A-site-doped Sr(1−1.5x)CexTiO3 ceramics system. J Am Ceram Soc 2016, 99: 3286–3292.

    CAS  Article  Google Scholar 

  42. [42]

    Lan XK, Li J, Zou ZY, et al. Lattice structure analysis and optimised microwave dielectric properties of LiAl1−x(Zn0.5Si0.5)xO2 solid solutions. J Eur Ceram Soc 2019, 39: 2360–2364.

    CAS  Article  Google Scholar 

  43. [43]

    Ferreira VM, Baptista JL. Preparation and microwave dielectric properties of pure and doped magnesium titanate ceramics. Mater Res Bull 1994, 29: 1017–1023.

    CAS  Article  Google Scholar 

  44. [44]

    Lei W, Lu WZ, Wang XC, et al. Effects of CaTiO3 on microstructures and properties of (1−x)ZnAl2O4xMg2TiO4 (x=0.21) microwave dielectric ceramics. J Inorg Mater 2009, 24: 957–961.

    CAS  Article  Google Scholar 

  45. [45]

    Zhang P, Zhao YG, Li LX. The correlations among bond ionicity, lattice energy and microwave dielectric properties of (Nd1−xLax)NbO4 ceramics. Phys Chem Chem Phys 2015, 17: 16692–16698.

    CAS  Article  Google Scholar 

  46. [46]

    Zhao YG, Zhang P. High-Q microwave dielectric ceramics using Zn3Nb1.88Ta0.12O8 solid solutions. J Alloys Compd 2016, 662: 455–460.

    CAS  Article  Google Scholar 

  47. [47]

    Zhou DX, Sun F, Hu YX, et al. Low-temperature sintering and microwave dielectric properties of Mg3B2O6-LMZBS composites. J Mater Sci: Mater Electron 2012, 23: 981–989.

    CAS  Google Scholar 

  48. [48]

    Dou G, Guo M, Li YX, et al. The effect of LMBS glass on the microwave dielectric properties of the Mg3B2O6 for LTCC. J Mater Sci: Mater Electron 2015, 26: 4207–1211.

    CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 61761015 and 12064007), the Natural Science Foundation of Guangxi (Nos. 2018GXNSFFA050001, 2017GXNSFDA198027, and 2017GXNSFFA198011), High Level Innovation Team and Outstanding Scholar Program of Guangxi Institutes. References

Author information

Affiliations

Authors

Corresponding author

Correspondence to Huanfu Zhou.

Rights and permissions

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Wang, H., Li, S., Wang, K. et al. Sintering behaviour and microwave dielectric properties of MgO-2B2O3-xwt%BaCu(B2O5)-ywt%H3BO3 ceramics. J Adv Ceram (2021). https://doi.org/10.1007/s40145-021-0503-0

Download citation

Keywords

  • low-temperature co-fired ceramics (LTCC)
  • sintering temperature
  • MgO-2B2O3
  • H3BO3
  • microwave dielectrics
  • temperature coefficient of resonance frequency