摘要
采用固相反应法制备xSiO_2-(1-x)BPO_4微波介质陶瓷,研究了LMZBS玻璃助烧剂对陶瓷物相组成、显微结构、微波介电性能的影响。结果表明:添加LMZBS玻璃可使SiO_2-BPO_4玻璃陶瓷的烧结温度降低至900℃。当LMZBS的添加量为4%(质量分数,下同)时,70SiO_2-30BPO_4(质量分数/%)在900℃烧结2 h时,陶瓷的介电性能最佳(ε_r=4.0、Q×f=22 600 GHz、τ_f=-22×10~(-6)/℃)。同时,烧结过程中玻璃相的存在抑制了体系中硼离子的挥发,改善了陶瓷的显微结构,保证了其与银电极具有良好的共烧性。此外,CaTiO_3的引入能有效调节70SiO_2-30BPO_4陶瓷的τ_f,当CaTiO_3添加量为5%(质量分数)、烧结温度为900℃时,陶瓷具有最佳的介电性能(ε_r=4.4,Q×f=17 800 GHz,τ_f=6×10~(-6)/℃),有望应用于LTCC基板。
xSiO_2-(1-x)BPO_4 microwave dielectric ceramics had been prepared by solid-state reaction. The effects of LMZBS glass sintering aid on the phase composition, microstructure and microwave dielectric properties of ceramics was studied. The results show that the addition of LMZBS glass could lower the sintering temperature of SiO_2-BPO_4 glass ceramics to 900 ℃, and the best dielectric properties of the ceramics(i.e.,ε_r=4.0, Q×f=22 600 GHz, τ_f=-22 ×10~(-6)/℃) are obtained when the mass ratio of silicon and boron-phosphors is 70∶30 and the addition of LMZBS is 4 wt% at 900 ℃ for 2 h. Moreover, the presence of glass phase in the sintering process inhibited boron ions volatilization, which improved the microstructure and ensured excellent co-firing with Ag electrode. In addition, the introduction of CaTiO_3 can effectively adjust the τ_f of 70 SiO_2-30 BPO_4 ceramics. The ceramics possess optimum dielectric properties(ε_r=4.4, Q×f=17 800 GHz, τ_f=6×10~(-6)/℃) when the addition of CaTiO_3 is 5 wt% and sintered at 900 ℃, which is a promised candidate for LTCC application.
引文
1 Tan X H,Zhou H F,Huan G J,et al.Journal of Electronic Materials,2017,46(10),5950.
2 Ohashi M,Ogawa H,Kan A,et al.Journal of the European Ceramic Society,2005,25(12),2877.
3 Lai Y M,Hong C Y,Jin L H,et al.Ceramics International,2017,43,16167.
4 Hu J,Zhang T Y,Li Z,et al.Materials Review,2017,31(S2),107(in Chinese).胡杰,张天宇,李真,等.材料导报,2017,31(专辑30),107.
5 Hu C X,Liu P.Journal of Alloys & Compounds,2013,559(5),129.
6 Xia G B,He L T,Yang D A.Journal of Alloys & Compounds,2012,53(1),70.
7 Li B,Yue Z X,Ji Z,et al.Materials Letters,2002,54(1),25.
8 Chen G H,Liu X Y.Journal of Alloys & Compounds,2007,431(1),282.
9 Zhu H Y,Fu R L,Agathopoulos Simeon,et al.Ceramics International,2018,44,10147.
10 Li B,Yu Z X,Zhou J,et al.Journal of Inorganic Materials,2001,16(5),974(in Chinese).李勃,岳振星,周济,等.无机材料学报,2001,16(5),974.
11 Bian J J,Xie Y R,et al.Journal of the European Ceramic Society,2018,38(7),2747.
12 Baret G,Baret G.Journal of the Electrochemical Society,1991,138(9),2830.
13 Li H K,Zeng B,Yang X F,et al.Inorganic Chemicals Industry,2014,46(1),31(in Chinese).李海昆,曾波,杨学芬,等.无机盐工业,2014,46(1),31.
14 Huang C L,Wang M H.Materials Research Bulletin,2001,36(15),2677.