Sintering mechanism and microwave dielectric properties of BaTi4O9-BBZ composite for LTCC technology

Sintering mechanism and microwave dielectric properties of BaTi4O9-BBZ composite for LTCC technology
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DOI:
10.1016/j.ceramint.2017.06.178
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发表时间:
2017-10
影响因子:
5.2
通讯作者:
Haishen Ren;T. Xie;Mingzhao Dang;Jiang Shaohu;Hui Lin;L. Luo
Haishen Ren;T. Xie;Mingzhao Dang;Jiang Shaohu;Hui Lin;L. Luo
中科院分区:
材料科学1区
文献类型:
--
作者:
Haishen Ren;T. Xie;Mingzhao Dang;Jiang Shaohu;Hui Lin;L. Luo

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将bati4o9陶瓷与BaO-B2O3-ZnO (BBZ)玻璃混合制备了低温共烧陶瓷(LTCC)材料。通过BaTi4O9-BBZ复合材料的润湿行为、活化能、相演化、微观结构和微波介电性能进一步分析了烧结机理。结果表明:BBZ玻璃可将bati4o9陶瓷的烧结温度从1300℃显著降低到925℃;这是由于三个阶段的部分反应性液体辅助烧结过程,包括玻璃重排和局部晶粒重排,溶液-再沉淀包括玻璃结晶和玻璃与陶瓷之间的反应,以及整体晶粒重排,孔隙闭合和粘性流动。XRD谱图表明,烧结过程中bati4o9与BBZ玻璃的结晶相发生了明显的反应,形成了两个新相BaTi(BO3)2和Ba4Ti13O30。bati4o9陶瓷的活化能为520.9±40.46 kJ/mol,而BaTi4O9-BBZ复合材料的活化能为330.98±47.34 kJ/mol。随着烧结温度的升高,介电常数εr和质量因子Q×f先增大后减小,谐振频率温度系数τf略有减小。在925℃下烧结2 h的BaTi4O9-BBZ复合材料具有优异的微波介电性能,εr= 26.4, Q×f = 27300 GHz, τf= + 0.3 ppm/°C。此外,该材料与银电极良好的化学相容性使其成为LTCC技术的潜在候选材料。
A low temperature co-fired ceramic (LTCC) material was fabricated by mixing BaTi4O9ceramic with BaO-B2O3-ZnO (BBZ) glass. The sintering mechanism was further analyzed through the wetting behavior, activation energy, phase evolution, microstructure and microwave dielectric properties of the BaTi4O9-BBZ composite. The results show that the sintering temperature of the BaTi4O9ceramics can be significantly lowered from 1300 to 925 °C by the BBZ glass. This is due to the three-stage partially reactive liquid assisted sintering process which consists of glass redistribution and local grains rearrangement, solution-reprecipitaion including glass crystallization and reactions between the glass and ceramic, and global grain rearrangement, closure of pores and viscous flow. XRD patterns exhibit that BaTi4O9reacts with the crystallization phase of BBZ glass obviously during sintering to form two new phases BaTi(BO3)2and Ba4Ti13O30. The activation energy of BaTi4O9ceramic is calculated to be 520.9 ± 40.46 kJ/mol, while that of BaTi4O9-BBZ composite is reduced to 330.98 ± 47.34 kJ/mol. With increasing sintering temperature, the dielectric constant (εr) and the quality factor (Q×f) value increases firstly and then decreases, and the temperature coefficient of resonant frequency (τf) value slightly decreases. Typically, the BaTi4O9-BBZ composite sintered at 925 °C for 2 h displays excellent microwave dielectric properties of εr= 26.4, Q×f = 27300 GHz and τf= + 0.3 ppm/°C. In addition, the good chemical compatibility of this material with Ag electrode makes it as a potential candidate for LTCC technology.