Ba1-xMgxAl2Si2O8晶体结构与微波介电性能的研究

doi:10.15541/jim20160272

摘要/Abstract

摘要：

采用固相烧结法, 按化学计量比Ba_1-_xMg_xAl₂Si₂O₈(x=0, 0.05, 0.1, 0.15, 0.3, 0.5)制备样品, 考察不同MgO含量对BaO-Al₂O₃-SiO₂系介电材料晶体结构及微波介电性能的影响。结果表明, MgO可以降低烧结温度, 促进六方相转变为单斜相, 当添加量x≥0.15时, 相转变可以达到100%。当x≤0.15时, 适量的MgO可以有效地促进单斜钡长石晶粒的长大。在0.05≤x≤0.1范围内, 随着MgO含量的增加, 单斜钡长石衍射峰增强, 晶粒尺寸增大, 密度、介电常数与τ_f均随MgO含量的增加而增大。在x=0.1, 烧结温度为1400℃时, 可获得综合性能相对较好的单斜钡长石, 其介电性能ε_r=6.44, Q×f=16461 GHz, τ_f= -30.6×10^-6K^-1。

关键词: MgO, 钡长石, 单斜相, 晶体结构, 微波介电性能

Abstract:

Barium feldspar BaO-Al₂O₃-SiO₂ system materials have been studied extensively for application in microwave devices, microwave substrate and packaging in recent years, due to their remarkable dielectric properties. The hexacelsian-celsian transition, relationship between dielectric properties, and structure of BaO-Al₂O₃-SiO₂ system has attracted widely academic interest. Ba_1-_xMg_xAl₂Si₂O₈ (x=0, 0.05, 0.1, 0.15, 0.3, 0.5) ceramics were prepared by solid state sintering processing. The crystal structure and microwave dielectric properties of BaO-Al₂O₃-SiO₂ with different MgO contents were studied. The results show that MgO doping reduces sintering temperature and greatly promotes the transition from hexacelisian to celsian at x≥0.15, while the transition reachs 100%. MgO doping effectively increases grain size at x≤0.15. The diffraction peak of celsian is enhanced and the grain size gets larger. Moreover, the density, dielectric constant andτ_f of Ba_1-_xMg_xAl₂Si₂O₈ ceramics increases with the increase of MgO content in the range of 0.05≤x≤0.1. In addition, the resonant frequency temperature coefficient is negative. The Ba_0.9Mg_0.1Al₂Si₂O₈ sintered at 1400℃ exhibits a high Q×f value of 16461 GHz, ε_r=6.44 and τ_f= -30.6×10^-6K^-1 at x=0.1. The dielectric constant of Ba_1-_xMg_xAl₂Si₂O₈ ceramics is related with its Mg²⁺ polarizability and its structure. The effect of electronegativity, the size of ions and the crystal structure on Q×f value of Ba_1-_xMg_xAl₂Si₂O₈ ceramics are also discussed.

Key words: magnesium oxide, feldspar, celsian, crystal structure, microwave dielectric properties

中图分类号:

TQ174

张瑶, 丁士华, 刘杨琼, 段绍英, 肖鹏, 韩林材. Ba_1-_xMg_xAl₂Si₂O₈晶体结构与微波介电性能的研究[J]. 无机材料学报, 2017, 32(1): 91-95.

ZHANG Yao, DING Shi-Hua, LIU Yang-Qiong, DUAN Shao-Ying, XIAO Peng, HAN Lin-Cai. Crystal Structure and Microwave Dielectric Property of Ba_1-_xMg_xAl₂Si₂O₈[J]. Journal of Inorganic Materials, 2017, 32(1): 91-95.

图/表 8

图1 Ba1-xMgxAl2Si2O8样品密度与烧结温度的关系曲线

Fig. 1 Relationship between density and sintering temperature of the Ba1-xMgxAl2Si2O8

表1 Ba1-xMgxAl2Si2O8随MgO含量变化的烧结情况

Table 1 Sintering conditions of the samples Ba1-xMgxAl2Si2O8 with different MgO amounts

Ba_1-_xMg_x Al₂Si₂O₈	Sintering temperature/℃		Main crystalline phase
x=0	1400	2.8929	Hexacelsian
x=0.05	1400	2.9129	Celsian
x=0.1	1400	2.9889	Celsian
x=0.15	1375	2.9556	Celsian
x=0.3	1375	2.9385	Celsian
x=0.5	1350	2.6964	Celsian

图2 Ba1-xMgxAl2Si2O8 样品的XRD图谱

Fig. 2 XRD patterns of the Ba1-xMgxAl2Si2O8 samples

表2 主晶相的晶格常数与晶胞体积

Table 2 Lattice constant and unit cell volume of the Ba1-xMgxAl2Si2O8 samples with different MgO amounts

Ba_1-_xMg_xAl₂Si₂O₈	a/nm	b/nm	c/nm	V/nm³
x=0 (Hexacelsian)	0.530506	0.530506	0.779730	0.19004
x=0.05(Celsian)	0.864706	1.304903	0.722291	0.74016
x=0.1 (Celsian)	0.865584	1.306700	0.721656	0.73998
x=0.15(Celsian)	0.861000	1.302623	0.718374	0.73038
x=0.3 (Celsian)	0.863250	1.305660	0.720369	0.73588
x=0. 5(Celsian)	0.866638	1.305692	0.722445	0.73898

图3 Ba1-xMgxAl2Si2O8样品的SEM照片

Fig. 3 SEM images of the samples with different MgO amounts(a) x=0; (b) x=0.05; (c) x=0.1; (d) x=0.15; (e) x=0.3; (f) x=0.5

图4 Ba1-xMgxAl2Si2O8样品的介电常数变化曲线

Fig. 4 Dielectric constant of the samples Ba1-xMgxAl2Si2O8 with different MgO amounts

图5 Ba1-xMgxAl2Si2O8样品的品质因数曲线

Fig. 5 Q×f of the samples Ba1-xMgxAl2Si2O8 with different MgO amounts

图6 Ba1-xMgxAl2Si2O8样品的谐振频率温度系数曲线

Fig. 6 τf of the sample Ba1-xMgxAl2Si2O8 with different MgO amounts

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Ba_1-_xMg_xAl₂Si₂O₈晶体结构与微波介电性能的研究

Crystal Structure and Microwave Dielectric Property of Ba_1-_xMg_xAl₂Si₂O₈

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