三倍金红石型MgTa<sub>2</sub>O<sub>6</sub>微波介质陶瓷的低温烧结及温度稳定性调控

许承智; 杨鸿宇; 杨鸿程; 邢林庄; 王媛; 李智敏; 李恩竹; 赵国瑞

doi:10.1007/s12613-023-2791-6

Volume 31 Issue 8

Aug. 2024

Turn off MathJax

图(10) / 表(6)

数据统计

计量

文章访问数: 974
HTML全文浏览量: 161
PDF下载量: 13
被引次数: 0

文章导航 > 矿物冶金与材料学报（英文） > 2024 > 31(8): 1935-1943

Chengzhi Xu, Hongyu Yang, Hongcheng Yang, Linzhuang Xing, Yuan Wang, Zhimin Li, Enzhu Li, and Guorui Zhao, Low-firing and temperature stability regulation of tri-rutile MgTa₂O₆ microwave dielectric ceramics, Int. J. Miner. Metall. Mater., 31(2024), No. 8, pp. 1935-1943. https://doi.org/10.1007/s12613-023-2791-6

Cite this article as:

Chengzhi Xu, Hongyu Yang, Hongcheng Yang, Linzhuang Xing, Yuan Wang, Zhimin Li, Enzhu Li, and Guorui Zhao, Low-firing and temperature stability regulation of tri-rutile MgTa2O6 microwave dielectric ceramics, Int. J. Miner. Metall. Mater., 31(2024), No. 8, pp. 1935-1943. https://doi.org/10.1007/s12613-023-2791-6

Citation:

PDF( 3836 KB)

引用本文 PDF XML SpringerLink

研究论文

三倍金红石型MgTa₂O₆微波介质陶瓷的低温烧结及温度稳定性调控

1)
西安电子科技大学先进材料与纳米科技学院, 西安 710071, 中国
2)
西安电子科技大学前沿交叉研究院, 西安 710071, 中国
3)
西南石油大学新能源与材料学院, 成都610500, 中国
4)
电子科技大学国家电磁辐射控制材料工程技术研究中心, 多频谱吸波材料与结构教育部重点实验室, 成都610054, 中国
5)
松山湖材料实验室, 东莞 523808, 中国

通讯作者:
杨鸿宇 E-mail: yanghongyu@xidian.edu.cn

李智敏 E-mail: zmli@mail.xidian.edu.cn

文章亮点

(1) 系统地研究了Li₂O–MgO–ZnO–B₂O₃–SiO₂玻璃对MgTa₂O₆陶瓷的低温烧结行为、晶体结构畸变与微波介电性能的影响规律

(2) 协同解决了MgTa₂O₆微波介质陶瓷较高烧结温度与较差温度稳定性的问题

(3) 制备出具有优异微波介电性能的MgTa₂O₆基微波介质陶瓷：ε_r = 26.1, Q×f = 34267 GHz, τ_f = –8.7 × 10^–6 /°C

中文摘要

三倍金红石型MgTa₂O₆微波介质陶瓷常被用于制作介质滤波器与介质谐振器等电子元器件，是5G基站通信领域中的一种重要材料类型。然而，该材料的烧结温度较高且温度稳定型较差，限制了其在高频通信中的进一步应用。为了协同解决MgTa₂O₆微波介质陶瓷较高的烧结温度与较差的温度稳定性的问题，本文采用了一种含有Li₂O–MgO–ZnO–B₂O₃–SiO₂组分的玻璃，利用传统固相烧结工艺研究了玻璃掺杂对MgTa₂O₆陶瓷的低温烧结行为、晶体结构畸变与微波介电性能的影响。研究表明，掺杂2wt%的玻璃不会引入杂质相，体系仍为单一的三倍金红石型MgTa₂O₆物相，说明玻璃掺杂形成了MgTa₂O₆固溶体。当添加2wt%玻璃，在1150°C时可以获得致密性优异且微波介电性能良好的材料体系：ε_r = 26.1, Q×f = 34267 GHz, τ_f = –8.7 × 10^–6 /°C。研究表明，Li₂O–MgO–ZnO–B₂O₃–SiO₂玻璃不仅极大地改善了MgTa₂O₆陶瓷的低温烧结特性，而且在保持高Q×f值的同时仍有效提高了温度稳定性，这进一步发掘了该材料在高频通信中的应用潜力。

关键词:

Research Article

Low-firing and temperature stability regulation of tri-rutile MgTa₂O₆ microwave dielectric ceramics

+ Author Affiliations

1)
School of Advanced Materials and Nanotechnology, Xidian University, Xi’an 710071, China
2)
Academy of Advanced Interdisciplinary Research, Xidian University, Xi’an 710071, China
3)
School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China
4)
National Engineering Research Center of Electromagnetic Radiation Control Materials and Key Laboratory of Multi-Spectral Absorbing Materials and Structures of Ministry of Education, University of Electronic Science and Technology of China, Chengdu 610054, China
5)
Songshan Lake Materials Laboratory A1 Building, University Innovation Park, Dongguan 523808, China

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Corresponding authors:
Hongyu Yang E-mail: yanghongyu@xidian.edu.cn

Zhimin Li E-mail: zmli@mail.xidian.edu.cn
Received: 10 July 2023; Revised: 16 October 2023; Accepted: 17 November 2023; Available online: 21 November 2023

Abstract

Abstract

A glass frit containing Li₂O–MgO–ZnO–B₂O₃–SiO₂ component was used to explore the low-temperature sintering behaviors and microwave dielectric characteristics of tri-rutile MgTa₂O₆ ceramics in this study. The good low-firing effects are presented due to the high matching relevance between Li₂O–MgO–ZnO–B₂O₃–SiO₂ glass and MgTa₂O₆ ceramics. The pure tri-rutile MgTa₂O₆ structure remains unchanged, and high sintering compactness can also be achieved at 1150°C. We found that the Li₂O–MgO–ZnO–B₂O₃–SiO₂ glass not only greatly improves the low-temperature sintering characteristics of MgTa₂O₆ ceramics but also maintains a high (quality factor (Q) × resonance frequency (f)) value while still improving the temperature stability. Typically, great microwave dielectric characteristics when added with 2wt% Li₂O–MgO–ZnO–B₂O₃–SiO₂ glass can be achieved at 1150°C: dielectric constant, ε_r = 26.1; Q × f = 34267 GHz; temperature coefficient of resonance frequency, τ_f = −8.7 × 10⁻⁶ /°C.
- MgTa₂O₆;
- ceramic;
- microwave dielectric characteristics;
- glass

FullText(HTML)

Supplements(0)

References(37)

References

[1]	F.F. Wu, D. Zhou, C. Du, et al., Temperature stable Sm(Nb_{1– x}V_x)O₄ (0.0 ≤ x ≤ 0.9) microwave dielectric ceramics with ultra-low dielectric loss for dielectric resonator antenna applications, J. Mater. Chem. C, 9(2021), No. 31, p. 9962. doi: 10.1039/D1TC02390J
[2]	H.C. Xiang, J. Kilpijärvi, S. Myllymäki, H.T. Yang, L. Fang, and H. Jantunen, Spinel-olivine microwave dielectric ceramics with low sintering temperature and high quality factor for 5GHz Wi-Fi antennas, Appl. Mater. Today, 21(2020), art. No. 100826. doi: 10.1016/j.apmt.2020.100826
[3]	M.T. Sebastian and H. Jantunen, Low loss dielectric materials for LTCC applications: A review, Int. Mater. Rev., 53(2008), No. 2, p. 57. doi: 10.1179/174328008X277524
[4]	F.F. Wu, D. Zhou, C. Du, et al., Design of a sub-6 GHz dielectric resonator antenna with novel temperature-stabilized (Sm_{1– x}Bi_x)NbO₄ (x = 0–0.15) microwave dielectric ceramics, ACS Appl. Mater. Interfaces, 14(2022), No. 5, p. 7030. doi: 10.1021/acsami.1c24307
[5]	H. Yang, S. Zhang, H. Yang, et al., The latest process and challenges of microwave dielectric ceramics based on pseudo phase diagrams, J. Adv. Ceram., 10(2021), No. 5, p. 885. doi: 10.1007/s40145-021-0528-4
[6]	H.J. Lee, K.S. Hong, and I.T. Kim, Crystal structure and microwave dielectric properties of M(Nb_xTa_{1− x})₂O₆ solid solution (M = Mg or Zn), J. Mater. Res., 12(1997), No. 6, p. 1437. doi: 10.1557/JMR.1997.0196
[7]	E.S. Kim and C.J. Jeon, Dependence of microwave dielectric properties on structural characteristics of ilmenite, tri-rutile and wolframite ceramics, J. Adv. Dielectr., 1(2011), No. 1, p. 127. doi: 10.1142/S2010135X11000161
[8]	H.T. Wu, Y.S. Jiang, and Y.L. Yue, Low-temperature synthesis and microwave dielectric properties of trirutile-structure MgTa₂O₆ ceramics by aqueous sol–gel process, Ceram. Int., 38(2012), No. 6, p. 5151. doi: 10.1016/j.ceramint.2012.03.020
[9]	B.J. Fu, Y.C. Zhang, X.L. Su, Y.H. Liu, and M. Hong, Effects of CuO addition on the microstructure and microwave dielectric properties of MgTa₂O₆ ceramics, Key Eng. Mater., 512-515(2012), p. 1222. doi: 10.4028/www.scientific.net/KEM.512-515.1222
[10]	H.Y. Yang, L. Chai, G.C. Liang, et al., Structure, far-infrared spectroscopy, microwave dielectric properties, and improved low-temperature sintering characteristics of tri-rutile Mg_0.5Ti_0.5TaO₄ ceramics, J. Adv. Ceram., 12(2023), No. 2, p. 296. doi: 10.26599/JAC.2023.9220683
[11]	H.Y. Yang, L. Chai, Y.C. Wang, M.J. Xing, Y.W. Chen, and E.Z. Li, Matching correlation study of titanium-based ceramics with glass based on dissolution characteristics, J. Eur. Ceram. Soc., 42(2022), No. 13, p. 5778. doi: 10.1016/j.jeurceramsoc.2022.06.014
[12]	M. Valant, D. Suvorov, R.C. Pullar, K. Sarma, and N.M. Alford, A mechanism for low-temperature sintering, J. Eur. Ceram. Soc., 26(2006), No. 13, p. 2777. doi: 10.1016/j.jeurceramsoc.2005.06.026
[13]	B.H. Toby, EXPGUI, a graphical user interface for GSAS , J. Appl. Crystallogr., 34(2001), No. 2, p. 210.
[14]	A.C. Larson and R.B. Von Dreele, General Structure Analysis System (GSAS ), Los Alamos National Laboratory Report LAUR 86-748, U.S. Department of Energy: Washington, DC, 2004.
[15]	T. Takada, S.F. Wang, S. Yoshikawa, S.J. Jang, and R.E. Newnham, Effect of glass additions on BaO–TiO₂–WO₃ microwave ceramics, ChemInform, 25(1994), No. 7, p. 1909.
[16]	H.Y. Yang, S.R. Zhang, H.C. Yang, X. Zhang, and E.Z. Li, Structural evolution and microwave dielectric properties of xZn_0.5Ti_0.5NbO_{4–(1– x)}Zn_0.15Nb_0.3Ti_0.55O₂ ceramics, Inorg. Chem., 57(2018), No. 14, p. 8264. doi: 10.1021/acs.inorgchem.8b00873
[17]	E.A. Nenasheva, S.S. Redozubov, N.F. Kartenko, and I.M. Gaidamaka, Microwave dielectric properties and structure of ZnO–Nb₂O₅–TiO₂ ceramics, J. Eur. Ceram. Soc., 31(2011), No. 6, p. 1097. doi: 10.1016/j.jeurceramsoc.2010.12.023
[18]	X.C. Fan, X.M. Chen, and X.Q. Liu, Structural dependence of microwave dielectric properties of SrRAlO₄ (R = Sm, Nd, La) ceramics: Crystal structure refinement and infrared reflectivity study, Chem. Mater., 20(2008), No. 12, p. 4092. doi: 10.1021/cm703273z
[19]	R.D. Shannon, Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides, Acta Crystallogr., Sect. A, 32(1976), No. 5, p. 751. doi: 10.1107/S0567739476001551
[20]	Z.Q. Yuan, B. Liu, X.Q. Liu, and X.M. Chen, Structure and microwave dielectric characteristics of Sr(La_{1− x}Sm_x)₂Al₂O₇ ceramics, RSC Adv., 6(2016), No. 98, p. 96229. doi: 10.1039/C6RA20776F
[21]	E.S. Kim, C.J. Jeon, and P.G. Clem, Effects of crystal structure on the microwave dielectric properties of ABO₄ (A = Ni, Mg, Zn and B = Mo, W) ceramics, J. Am. Ceram. Soc., 95(2012), No. 9, p. 2934. doi: 10.1111/j.1551-2916.2012.05274.x
[22]	N.E. Brese and M. O'Keeffe, Bond-valence parameters for solids, Acta Crystallogr., Sect. B, 47(1991), No. 2, p. 192. doi: 10.1107/S0108768190011041
[23]	H.R. Tian, J.J. Zheng, L.T. Liu, et al., Structure characteristics and microwave dielectric properties of Pr₂(Zr_{1– x}Ti_x)₃(MoO₄)₉ solid solution ceramic with a stable temperature coefficient, J. Mater. Sci. Technol., 116(2022), p. 121. doi: 10.1016/j.jmst.2021.10.051
[24]	H.Y. Yang, E.Z. Li, H.C. Yang, H.C. He, and R.S. Zhang, Synthesis of Zn_0.5Ti_0.5NbO₄ microwave dielectric ceramics with Li₂O–B₂O₃–SiO₂ glass for LTCC application, Int. J. Appl. Glass Sci., 9(2018), No. 3, p. 392. doi: 10.1111/ijag.12334
[25]	L.S. Xie, C.W. Zhong, Z.X. Fang, Y. Zhao, B. Tang, and S.R. Zhang, Microwave dielectric properties of Li₂O–xMgO–ZnO–B₂O₃–SiO₂ glass-ceramics (x = 30–50 wt.%), J. Ceram. Soc. Jpn, 126(2018), No. 3, p. 163. doi: 10.2109/jcersj2.17156
[26]	C.F. Tseng, Microwave dielectric properties of low loss microwave dielectric ceramics: A_0.5Ti_0.5NbO₄ (A = Zn, Co), J. Eur. Ceram. Soc., 34(2014), No. 15, p. 3641. doi: 10.1016/j.jeurceramsoc.2014.06.010
[27]	H.Y. Yang, E.Z. Li, Y.F. Yang, Y. Shi, H.C. He, and S.R. Zhang, Co₂O₃ substitution effects on the structure and microwave dielectric properties of low-firing (Zn_0.9Mg_0.1)TiO₃ ceramics, Ceram. Int., 44(2018), No. 5, p. 5010. doi: 10.1016/j.ceramint.2017.12.097
[28]	R.D. Shannon, Dielectric polarizabilities of ions in oxides and fluorides, J. Appl. Phys., 73(1993), No. 1, p. 348. doi: 10.1063/1.353856
[29]	D. Zhou, X.Q. Fan, X.W. Jin, D.W. He, and G.H. Chen, Structures, phase transformations, and dielectric properties of BiTaO₄ ceramics, Inorg. Chem., 55(2016), No. 22, p. 11979. doi: 10.1021/acs.inorgchem.6b02153
[30]	H.Y. Yang, S.R. Zhang, H.C. Yang, Y. Yuan, and E.Z. Li, Intrinsic dielectric properties of columbite ZnNb₂O₆ ceramics studied by P–V–L bond theory and Infrared spectroscopy, J. Am. Ceram. Soc., 102(2019), No. 9, p. 5365. doi: 10.1111/jace.16385
[31]	E.S. Kim, B.S. Chun, R. Freer, and R.J. Cernik, Effects of packing fraction and bond valence on microwave dielectric properties of A²⁺B⁶⁺O₄ (A²⁺: Ca, Pb, Ba; B⁶⁺: Mo, W) ceramics, J. Eur. Ceram. Soc., 30(2010), No. 7, p. 1731. doi: 10.1016/j.jeurceramsoc.2009.12.018
[32]	J. Bao, Y.P. Zhang, H. Kimura, H.T. Wu, and Z.X. Yue, Crystal structure, chemical bond characteristics, infrared reflection spectrum, and microwave dielectric properties of Nd₂(Zr_{1– x}Ti_x )₃(MoO₄)₉ ceramics, J. Adv. Ceram., 12(2023), No. 1, p. 82. doi: 10.26599/JAC.2023.9220668
[33]	H. Tian, X. Zhou, T. Jiang, et al., Bond characteristics and microwave dielectric characteristics of (Mn_1/3Sb_2/3)⁴⁺ doped molybdate based low-temperature sintering ceramics, J. Alloys Compd., 906(2022), art. No. 164333. doi: 10.1016/j.jallcom.2022.164333
[34]	Z.X. Fang, B. Tang, F. Si, and S.R. Zhang, Low temperature sintering of high permittivity Ca–Li–Nd–Ti microwave dielectric ceramics with BaCu(B₂O₅) additives, J. Alloys Compd., 693(2017), p. 843. doi: 10.1016/j.jallcom.2016.09.292
[35]	A.J. Bosman and E.E. Havinga, Temperature dependence of dielectric constants of cubic ionic compounds, Phys. Rev., 129(1963), No. 4, p. 1593. doi: 10.1103/PhysRev.129.1593
[36]	M.Z. Dang, H.X. Lin, X.G. Yao, et al., Effects of B₂O₃ and MgO on the microwave dielectric properties of MgTa₂O₆ ceramics, Ceram. Int., 45(2019), No. 18, p. 24244. doi: 10.1016/j.ceramint.2019.08.135
[37]	C.L. Huang, K.H. Chiang, and C.Y. Huang, Microwave dielectric properties and microstructures of MgTa₂O₆ ceramics with CuO addition, Mater. Chem. Phys., 90(2005), No. 2-3, p. 373. doi: 10.1016/j.matchemphys.2004.10.037

Relative Articles

Cited By

Proportional views

数据统计

姓名
邮箱
手机号码
标题
留言内容
验证码

留言板

数据统计

分享

计量

三倍金红石型MgTa₂O₆微波介质陶瓷的低温烧结及温度稳定性调控

文章亮点

中文摘要

Low-firing and temperature stability regulation of tri-rutile MgTa₂O₆ microwave dielectric ceramics

Abstract

References

数据统计

Catalog

留言板

数据统计

分享

计量

三倍金红石型MgTa2O6微波介质陶瓷的低温烧结及温度稳定性调控

文章亮点

中文摘要

Low-firing and temperature stability regulation of tri-rutile MgTa2O6 microwave dielectric ceramics

Abstract

References

数据统计

Catalog

三倍金红石型MgTa₂O₆微波介质陶瓷的低温烧结及温度稳定性调控

Low-firing and temperature stability regulation of tri-rutile MgTa₂O₆ microwave dielectric ceramics