The feldspar-based microwave dielectric ceramic with low relative permittivity(εr)and excellent mechanical properties has attracted much attention in the fifth-generation wireless communication technology.In this wor...The feldspar-based microwave dielectric ceramic with low relative permittivity(εr)and excellent mechanical properties has attracted much attention in the fifth-generation wireless communication technology.In this work,a series of microwave dielectric ceramic SrAl_(2-x)Ga_(x)Si_(2)O_(8)(0.1≤x≤2.0)was synthesized using the traditional solid-state method.X-ray diffraction pattern indicates that Ga^(3+)can be dissolved into Al^(3+),forming a solid solution.Meanwhile,substitution of Ga^(3+)for Al^(3+)can promote the space group transition from I2/c(0.1≤x≤1.4)to P21/a(1.6≤x≤2.0)with coefficient of thermal expansion(CTE)increasing from 2.9×10^(-6)℃^(-1) to 5.2×10^(-6)℃^(-1).During this substitution,the phase transition can significantly improve the structural symmetry to enhance the dielectric properties and mechanical properties.Rietveld refinement results indicate that Ga^(3+)averagely occupied four Al^(3+)compositions to form solid solution.All ceramics have a dense microstructure and high relative density above 95%.An ultralower of 5.8 was obtained at x=1.6 composition with high quality factor(Q´f)of 50700 GHz and negative temperature coefficients of resonant frequency(tf)of approximately−35×10^(-6)℃^(-1).The densification temperature can be reduced to 940℃by adding 4%(in mass)LiF,resulting in good chemical compatibility with Ag electrode.Meanwhile,negativetf can be tuned to near-zero(+3.7×10^(-6)℃^(-1))by adding CaTiO_(3) ceramic.展开更多
ZnAl_(2)O_(4) and ZnAl_(2)O_(4)-based ceramics have attracted much attention from researchers due to their good microwave dielectric,thermal and mechanical properties.In this work,the influence of 5%(in mass)CuO-TiO_(...ZnAl_(2)O_(4) and ZnAl_(2)O_(4)-based ceramics have attracted much attention from researchers due to their good microwave dielectric,thermal and mechanical properties.In this work,the influence of 5%(in mass)CuO-TiO_(2)-Nb_(2)O_(5)(CTN)ternary composite oxide additives with different composition ratios on sintering behavior and properties of ZnAl_(2)O_(4) microwave dielectric ceramics was investigated.When the molar fraction ranges of Cu,Ti and Nb elements in 5%CTN additives are 0.625-0.875,0-0.250 and 0.125-0.625,respectively,sintering temperature of ZnAl_(2)O_(4) ceramics can be reduced from above 1400℃to below 1000℃.The sintering additives CN(Cu:Nb=1:1,molar ratio)and CTN(Cu:Ti:Nb=4:1:3,molar ratio)can reduce sintering temperature of ZnAl_(2)O_(4) ceramics to 975 and 1000℃,respectively,while maintaining good dielectric properties(dielectric constantε_(r)=11.36,quality factor Q׃=8245 GHz andε_(r)=9.52,Q׃=22249 GHz)and flexural strengths(200 and 161 MPa),which are expected to be applied in preparation of low temperature co-fired ceramic(LTCC)materials with copper electrodes.Low-temperature sintering of the ZnAl_(2)O_(4)+CTN system is characterized as activated sintering.Nanometer-level amorphous interfacial films containing Cu,Ti,and Nb elements are observed at the grain boundaries,which may provide fast diffusion pathways for mass transportation during the sintering process.Valence changes of Ti and Cu ions,along with changes of oxygen vacancies,are confirmed,which provides a potential mechanism for reduced sintering temperature of ZnAl_(2)O_(4) ceramics.In addition,a series of reactions occurring at the grain boundaries can activate these boundaries and further promote the sintering densification process.These results suggest a promising way to design a novel LTCC material with excellent properties based on the low temperature sintering of ceramics with the sintering aid of CuO-TiO_(2)-Nb_(2)O_(5) composite oxide.展开更多
基金National Natural Science Foundation of China (52302140)Major Scientific and Technological Innovation Project of Wenzhou (ZG2023040, ZG2023042)Joint Funds of the National Natural Science Foundation of China Key Program (U21B2068)。
文摘The feldspar-based microwave dielectric ceramic with low relative permittivity(εr)and excellent mechanical properties has attracted much attention in the fifth-generation wireless communication technology.In this work,a series of microwave dielectric ceramic SrAl_(2-x)Ga_(x)Si_(2)O_(8)(0.1≤x≤2.0)was synthesized using the traditional solid-state method.X-ray diffraction pattern indicates that Ga^(3+)can be dissolved into Al^(3+),forming a solid solution.Meanwhile,substitution of Ga^(3+)for Al^(3+)can promote the space group transition from I2/c(0.1≤x≤1.4)to P21/a(1.6≤x≤2.0)with coefficient of thermal expansion(CTE)increasing from 2.9×10^(-6)℃^(-1) to 5.2×10^(-6)℃^(-1).During this substitution,the phase transition can significantly improve the structural symmetry to enhance the dielectric properties and mechanical properties.Rietveld refinement results indicate that Ga^(3+)averagely occupied four Al^(3+)compositions to form solid solution.All ceramics have a dense microstructure and high relative density above 95%.An ultralower of 5.8 was obtained at x=1.6 composition with high quality factor(Q´f)of 50700 GHz and negative temperature coefficients of resonant frequency(tf)of approximately−35×10^(-6)℃^(-1).The densification temperature can be reduced to 940℃by adding 4%(in mass)LiF,resulting in good chemical compatibility with Ag electrode.Meanwhile,negativetf can be tuned to near-zero(+3.7×10^(-6)℃^(-1))by adding CaTiO_(3) ceramic.
基金National Natural Science Foundation of China (U24A2052)Shanghai Eastern Talent Plan。
文摘ZnAl_(2)O_(4) and ZnAl_(2)O_(4)-based ceramics have attracted much attention from researchers due to their good microwave dielectric,thermal and mechanical properties.In this work,the influence of 5%(in mass)CuO-TiO_(2)-Nb_(2)O_(5)(CTN)ternary composite oxide additives with different composition ratios on sintering behavior and properties of ZnAl_(2)O_(4) microwave dielectric ceramics was investigated.When the molar fraction ranges of Cu,Ti and Nb elements in 5%CTN additives are 0.625-0.875,0-0.250 and 0.125-0.625,respectively,sintering temperature of ZnAl_(2)O_(4) ceramics can be reduced from above 1400℃to below 1000℃.The sintering additives CN(Cu:Nb=1:1,molar ratio)and CTN(Cu:Ti:Nb=4:1:3,molar ratio)can reduce sintering temperature of ZnAl_(2)O_(4) ceramics to 975 and 1000℃,respectively,while maintaining good dielectric properties(dielectric constantε_(r)=11.36,quality factor Q׃=8245 GHz andε_(r)=9.52,Q׃=22249 GHz)and flexural strengths(200 and 161 MPa),which are expected to be applied in preparation of low temperature co-fired ceramic(LTCC)materials with copper electrodes.Low-temperature sintering of the ZnAl_(2)O_(4)+CTN system is characterized as activated sintering.Nanometer-level amorphous interfacial films containing Cu,Ti,and Nb elements are observed at the grain boundaries,which may provide fast diffusion pathways for mass transportation during the sintering process.Valence changes of Ti and Cu ions,along with changes of oxygen vacancies,are confirmed,which provides a potential mechanism for reduced sintering temperature of ZnAl_(2)O_(4) ceramics.In addition,a series of reactions occurring at the grain boundaries can activate these boundaries and further promote the sintering densification process.These results suggest a promising way to design a novel LTCC material with excellent properties based on the low temperature sintering of ceramics with the sintering aid of CuO-TiO_(2)-Nb_(2)O_(5) composite oxide.
