A low-firing melilite ceramic Ba2CuGe207 and compositional modulation on microwave dielectric properties through Mg substitution

A melilite Ba2CuGe2O7 ceramic was characterized by low sintering temperature and moderate microwave dielectric properties.Sintered at 960℃,the Ba2CuGe2O7 ceramic had a high relative density 97%,a low relative permittivity(εr)9.43,a quality factor(Q×f)of 20,000 GHz,and a temperature coefficient of resonance frequency(τf)-76 ppm/℃.To get a deep understanding of the relationship between composition,structure,and dielectric performances,magnesium substitution for copper in Ba2CuGe2O7 was conducted.Influences of magnesium doping on the sintering behavior,crystal structure,and microwave dielectric properties were studied.Mg doping in Ba2CuGe2O7 caused negligible changes in the macroscopic crystal structure,grain morphology,and size distribution,while induced visible variation in the local structure as revealed by Raman analysis.Microwave dielectric properties exhibit a remarkable dependence on composition.On increasing the magnesium content,the relative permittivity featured a continuous decrease,while both the quality factor and the temperature coefficient of resonance frequency increased monotonously.Such variations in dielectric performances were clarified in terms of the polarizability,packing fraction,and band valence theory.

Sol-gel approach to low-temperature synthesis of single-phase metastable La_(2)Ga_(3)O_(7.5) melilite with enhanced grain-boundary oxide ionic conductivity via a kinetically favorable mechanism

Starting with the stoichiometric and highly homogeneous gel-precursor,single-phase metastable melilite La_(2)Ga_(3)O_(7.5),as the end-member of solid solution La_(1+x)Sr_(1−x)Ga_(3)O_(7+x/2)(0≤x≤1),has been synthesized by solid-state reaction at 700℃ for 2 h via a kinetically favorable mechanism and characterized by X-ray diffraction(XRD),Raman,X-ray photoelectron spectroscopy(XPS),field emission scanning electron microscopy(FESEM),transmission electron microscopy(TEM),AC impedance spectroscopy,etc.It has been revealed that the as-synthesized melilite La_(2)Ga_(3)O_(7.5) shows an orthorhombic symmetry with crystal cell parameters a=11.4690(1)A,b=11.2825(4)A,and c=10.3735(4)A,while has more Raman active modes than LaSrGa_(3)O_(7) with a tetragonal structure,which was also synthesized under the same conditions for comparison,but tends to slowly decompose into perovskite LaGaO_(3) and Ga2O_(3) when annealed at 700℃ for over 20 h driven by its meta-stability.Moreover,the metastable La2Ga3O7.5 shows a higher XPS binding energy for the excess oxide ions in the crystal structure than those at normal lattice sites.Its intrinsic grain oxide ion conductivity can reach as high as 0.04 and 0.51 mS·cm^(-1) at 550 and 700℃,respectively,characterized by a simple Arrhenius relationship ln(σT)-1/T with invariable activation energy,E_(a)=1.22 eV,over the temperature range from 300 to 700℃,along with an apparent grain boundary conductivity that is about double that from the grains thanks to the clean grain boundaries.This paper provides a new strategic approach to the synthesis of complex oxides that may be of high performance but are difficultly achieved by the conventional ceramic method at high temperatures.

Effects of Y_(2)O_(3) and transition-metal nitrates on phase,microstructures and PL properties of N-containing Ce_(2)Si_(2.5)Al_(0.5)O_(3.5)N_(3.5) melilite

N-containing Ce_(2)Si_(2.5)Al_(0.5)O_(3.5)N_(3.5)(CeSiAlON) melilite was synthesized at 1550 and 1600℃ for 5 h from CeO_(2),Si,Al,and Al_(2)O_(3) in nitrogen by using Y_(2)O_(3) and transition-metal nitrates(Co(NO_(3))_(2)·6 H_(2) O and Ni(NO_(3))_(2)·6 H_(2)O) as additives.The effects of Y_(2)O_(3) and transition-metal nitrates on the phase,microstructures and photoluminescence properties of CeSiAlON melilite were studied.The incorporation of Y_(2)O_(3) can promote the reaction of raw materials to a low degree,and results in a unit cell shrinkage of CeSiAlON due to the smaller radius of Y atom than that of Ce atom.The transition-metal nitrates can accelerate the reaction clearly and facilitate the formation of CeSiAlON fibers.The photoluminescence(PL) properties of CeSiAlON melilite presents a board violet emission band because of the 5 d-4 f transitions of Ce^(3+),and the additives can enhance the PL emission intensities of specimen significantly.