Journal Home > Volume 9 , issue 5

The non-stoichiometric Li3Mg2Sb1-xO6 (0.05 ≤ x ≤ 0.125) compounds have been prepared via the mixed oxide method. The influences of Sb nonstoichiometry on the sintering behavior, microstructure, phase composition along with microwave dielectric performances for Li3Mg2Sb1-xO6 ceramics were studied. Combined with X-ray diffraction (XRD) and Raman spectra, it was confirmed that phase composition could not be affected by the Sb nonstoichiometry and almost pure phase Li3Mg2SbO6 was formed in all compositions. Appropriate Sb-deficiency in Li3Mg2SbO6 not only lowered its sintering temperature but also remarkably improved its Q×f value. In particular, non-stoichiometric Li3Mg2Sb0.9O6 ceramics sintered at 1250 ℃/5 h owned seldom low dielectric constant εr = 10.8, near-zero resonant frequency temperature coefficient τf = -8.0 ppm/℃, and high quality factor Q×f = 86,300 GHz (at 10.4 GHz). This study provides an alternative approach to ameliorate its dielectric performances for Li3Mg2SbO6-based compounds through defect-engineering.


menu
Abstract
Full text
Outline
About this article

Effect of Sb-site nonstoichiometry on the structure and microwave dielectric properties of Li3Mg2Sb1-xO6 ceramics

Show Author's information Cuijin PEIaJingjing TANaYang LIaGuoguang YAOa,b( )Yanmin JIAaZhaoyu RENbPeng LIUcHuaiwu ZHANGd
School of Science, Xi’an University of Posts and Telecommunications, Xi’an 710121, China
School of Physics, Northwest University, Xi’an 710069, China
College of Physics and Information Technology, Shaanxi Normal University, Xi’an 710062, China
State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 610054, China

Abstract

The non-stoichiometric Li3Mg2Sb1-xO6 (0.05 ≤ x ≤ 0.125) compounds have been prepared via the mixed oxide method. The influences of Sb nonstoichiometry on the sintering behavior, microstructure, phase composition along with microwave dielectric performances for Li3Mg2Sb1-xO6 ceramics were studied. Combined with X-ray diffraction (XRD) and Raman spectra, it was confirmed that phase composition could not be affected by the Sb nonstoichiometry and almost pure phase Li3Mg2SbO6 was formed in all compositions. Appropriate Sb-deficiency in Li3Mg2SbO6 not only lowered its sintering temperature but also remarkably improved its Q×f value. In particular, non-stoichiometric Li3Mg2Sb0.9O6 ceramics sintered at 1250 ℃/5 h owned seldom low dielectric constant εr = 10.8, near-zero resonant frequency temperature coefficient τf = -8.0 ppm/℃, and high quality factor Q×f = 86,300 GHz (at 10.4 GHz). This study provides an alternative approach to ameliorate its dielectric performances for Li3Mg2SbO6-based compounds through defect-engineering.

Keywords:

microwave dielectric properties, ceramics, sintering, antimony compounds
Received: 14 January 2020 Revised: 31 May 2020 Accepted: 13 June 2020 Published: 11 September 2020 Issue date: October 2020
References(36)
[1]
X Zhang, B Tang, ZX Fang, et al. Structural evolution and microwave dielectric properties of a novel Li3Mg2-x/3 Nb1-2x/3TixO6 system with a rock salt structure. Inorg Chem Front 2018, 5: 3113-3125.
[2]
YH Zhang, JJ Sun, N Dai, et al. Crystal structure, infrared spectra and microwave dielectric properties of novel extra low-temperature fired Eu2Zr3(MoO4)9 ceramics. J Eur Ceram Soc 2019, 39: 1127-1131.
[3]
IM Reaney, D Iddles. Microwave dielectric ceramics for resonators and filters in mobile phone networks. J Am Ceram Soc 2006, 89: 2063-2072.
[4]
FF Gu, GH Chen, XQ Li, et al. Structural and microwave dielectric properties of the (1−x)Li3NbO4−xCa0.8Sr0.2TiO3 thermally stable ceramics. Mater Chem Phys 2015, 167: 354-359.
[5]
ZY Zou, ZH Chen, XK Lan, et al. Weak ferroelectricity and low-permittivity microwave dielectric properties of Ba2Zn(1+x)Si2O(7+x) ceramics. J Eur Ceram Soc 2017, 37: 3065-3071.
[6]
MZ Dong, ZX Yue, H Zhuang, et al. Microstructure and microwave dielectric properties of TiO2-doped Zn2SiO4 ceramics synthesized through the sol-gel process. J Am Ceram Soc 2008, 91: 3981-3985.
[7]
CL Huang, YW Tseng. Structure, dielectric properties, and applications of CaTiO3-modified Ca4MgNb2TiO12 ceramics at microwave frequency. J Am Ceram Soc 2011, 94: 1824-1828.
[8]
M Castellanos, JA Gard, AR West. Crystal data for a new family of phases, Li3Mg2XO6: X = Nb, Ta, Sb. J Appl Cryst 1982, 15: 116-119.
[9]
GG Yao, CJ Pei, Y Gong, et al. Microwave dielectric properties of temperature stable (1 - x)Li3Mg2SbO6-xBa3(VO4)2 composite ceramics. J Mater Sci: Mater Electron 2018, 29: 9979-9983.
[10]
CJ Pei, CD Hou, Y Li, et al. A low εr and temperature-stable Li3Mg2SbO6 microwave dielectric ceramics. J Alloys Compd 2019, 792: 46-49.
[11]
SY Wang, Q Sun, B Devakumar, et al. Mn4+-activated Li3Mg2SbO6 as an ultrabright fluoride-free red-emitting phosphor for warm white light-emitting diodes. RSC Adv 2019, 9: 3429-3435.
[12]
JS Zhong, X Chen, DQ Chen, et al. A novel rare-earth free red-emitting Li3Mg2SbO6: Mn4+ phosphor-in-glass for warm w-LEDs: Synthesis, structure, and luminescence properties. J Alloys Compd 2019, 773: 413-422.
[13]
P Zhang, SX Wu, M Xiao. Effect of Sb5+ ion substitution for Nb5+ on crystal structure and microwave dielectric properties for Li3Mg2NbO6 ceramics. J Alloys Compd 2018, 766: 498-505.
[14]
WJ Guo, J Zhang, Y Luo, et al. Microwave dielectric properties and thermally stimulated depolarization of Al-doped Ba4(Sm,Nd)9.33Ti18O54 ceramics. J Am Ceram Soc 2019, 102: 5494-5502.
[15]
B Li, JG Zheng, W Li. Enhanced effect of vanadium ions non-stoichiometry on microwave dielectric properties of Ca5Co4V6+xO24 ceramics. Mater Chem Phys 2018, 207: 282-288.
[16]
A Belous, O Ovchar, B Jancar, et al. The effect of non- stoichiometry on the microstructure and microwave dielectric properties of the columbites A2+Nb2O6. J Eur Ceram Soc 2007, 27: 2933-2936.
[17]
JM Li, CG Fan, ZX Cheng, et al. Influence of Zn nonstoichiometry on the phase structure, microstructure and microwave dielectric properties of Nd(Zn0.5Ti0.5)O3 ceramics. J Alloys Compd 2019, 793: 385-392.
[18]
LX Pang, D Zhou, ZX Yue. Temperature independent low firing [Ca0.25(Nd1-xBix)0.5]MoO4 (0.2 ≤ x ≤ 0.8) microwave dielectric ceramics. J Alloys Compd 2019, 781: 385-388.
[19]
WG Pan, MH Cao, JL Qi, et al. Defect structure and dielectric behavior in SrTi1-x(Zn1/3Nb2/3)xO3 ceramics. J Alloys Compd 2019, 784: 1303-1310.
[20]
R Muhammad, A Khesro. Influence of A-site nonstopichiometry on the electrical properties of BT-BMT. J Am Ceram Soc 2017, 100: 1091-1097.
[21]
ES Kim, BS Chun, R Freer, et al. 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 2010, 30: 1731-1736.
[22]
Y Wang, TL Tang, JT Zhang, et al. Preparation and microwave dielectric properties of new low-loss NiZrTa2O8 ceramics. J Alloys Compd 2019, 778: 576-578.
[23]
FD Hardcastle, IE Wachs. Determination of molybdenum- oxygen bond distances and bond orders by Raman spectroscopy. J Raman Spectrosc 1990, 21: 683-691.
[24]
SP Wu, DF Chen, C Jiang, et al. Synthesis of monoclinic CaSnSiO5 ceramics and their microwave dielectric properties. Mater Lett 2013, 91: 239-241.
[25]
JB Song, KX Song, JS Wei, et al. Microstructure characteristics and microwave dielectric properties of calcium apatite ceramics as microwave substrates. J Alloys Compd 2018, 731: 264-270.
[26]
JJ Bian, GX Song, K Yan. Structure and microwave dielectric properties of Ba1+x[(Co0.7Zn0.3)1/3Nb2/3]O3 (-0.015 ≤ x ≤ 0.015). J Eur Ceram Soc 2007, 27: 2817-2821.
[27]
S George, MT Sebastian. Synthesis and microwave dielectric properties of novel temperature stable high Q, Li2ATi3O8 (A = Mg, Zn) ceramics. J Am Ceram Soc 2010, 93: 2164-2166.
[28]
VL Gurevich, AK Tagantsev. Intrinsic dielectric loss in crystals. Adv Phys 1991, 40: 719-767.
[29]
KG Wang, HF Zhou, XB Liu, 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.
[30]
C Kai, CC Li, HC Xiang, et al. Phase formation and microwave dielectric properties of BiMVO5 (M = Ca, Mg) ceramics potential for low temperature co-fired ceramics application. J Am Ceram Soc 2019, 102: 362-371.
[31]
SS Kim, HG Na, YJ Kwon, et al. Synthesis and room-temperature NO2 sensing properties of Sb2O5 nanowires. Met Mater Int 2015, 21: 415-421.
[32]
R Freer, F Azough. Microstructural engineering of microwave dielectric ceramics. J Eur Ceram Soc 2008, 28: 1433-1441.
[33]
RC Pullar, SJ Penn, XR Wang, et al. Dielectric loss caused by oxygen vacancies in titania ceramics. J Eur Ceram Soc 2009, 29: 419-424.
[34]
KP Surendran, MT Sebastian, P Mohanan, et al. Effect of nonstoichiometry on the structure and microwave dielectric properties of Ba(Mg0.33Ta0.67)O3. Chem Mater 2005, 17: 142-151.
[35]
TW Zhang, RZ Zuo. Effect of Li2O-V2O5 addition on the sintering behavior and microwave dielectric properties of Li3(Mg1-xZnx)2NbO6 ceramics. Ceram Int 2014, 40: 15677-15684.
[36]
SB Desu, HM O'Bryan. Microwave loss quality of BaZn13Ta2/3O3 ceramics. J Am Ceram Soc 1985, 68: 546-551.
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 14 January 2020
Revised: 31 May 2020
Accepted: 13 June 2020
Published: 11 September 2020
Issue date: October 2020

Copyright

© The author(s) 2020

Acknowledgements

The authors acknowledge the support from the National Natural Science Foundation of China (Grant No. 51402235), China Postdoctoral Science Foundation (2015M582696), Science and Technology Plan Project of Xi'an Bureau of Science and Technology (GXYD17.19), Education Department of Shaanxi Province (18JK0711), and Innovation Funds of Graduate Programs of Xi'an University of Posts and Telecommunications (CXJJLD2019020).

Rights and permissions

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 Permission requests may be sought directly from editorial office.

Return