Microwave dielectric properties of La3Ti2TaO11 ceramics with perovskite-like layered structure

The first characterization of the microwave dielectric properties of the La₃Ti₂TaO₁₁ ceramics is presented. An ordinarily sintered ceramic at 1560 °C exhibits good microwave dielectric properties with ?_r = 46, Q × f = 7500 GHz and τ_f = ?47 ppm/°C. An alternative approach to tailor the temperature coefficient of resonate frequency of La₃Ti₂TaO₁₁ ceramics is also presented. Textured La₃Ti₂TaO₁₁ ceramics were fabricated using spark plasma sintering (SPS). By controlling the sintering temperature, orientation degree increased together with the steadily increase in ?_r and Q × f. A noteworthy change in τ_f from ?43.1 ppm/°C to ?13.6 ppm/°C with increasing orientation degree was observed. These results suggest that grain-orientation control was an effective way to tailor the microwave dielectric properties of La₃Ti₂TaO₁₁ ceramics.     

Effects of sintering parameters and Nd doping on the microwave dielectric properties of Y2O3 ceramics

Y₂O₃ ceramics with good dielectric properties were prepared via co-precipitation reaction and subsequent sintering in a muffle furnace. The effects of Nd doping and sintering temperature on microwave dielectric properties were studied. With the increase in sintering temperature, the density, quality factor (Q×f), and dielectric constant (ε_r) values of pure Y₂O₃ ceramics increased to the maximum and then gradually decreased. The Y₂O₃ ceramics sintered at 1500 °C for 4 h showed optimal dielectric properties: ε_r=10.76, Q×f=82, 188 GHz, and τ_f=−54.4 ppm/°C. With the addition of Nd dopant, the Q×f values, ε_r, and τ_f of the Nd: Y₂O₃ ceramics apparently increased, but excessive amount degraded the quality factor. The Y₂O₃ ceramics with 2 at% Nd₂O₃ sintered at 1460 °C displayed good microwave dielectric properties: ε_r=10.4, Q×f=94, 149 GHz and τ_f=−46.2 ppm/°C.     

Structure and properties of low temperature sintered ZnTa2O6 microwave dielectric ceramics

ZnTa₂O₆ microwave dielectric ceramics have been prepared using ZnTa₂O₆ nano-powders synthesized by sol–gel processing in this study. The crystal structure and microstructure of the ZnTa₂O₆ powders and ceramics were characterized by XRD and SEM techniques. ZnTa₂O₆ ceramics can be densified at a lower sintering temperature of 1200 °C. Microwave dielectric properties show that both of Q × f and ?_r values are lower than those of ceramics prepared by solid state route, and the τ_f values do not show different from that of solid state route. ZnTa₂O₆ ceramics sintered at 1200 °C exhibit good microwave dielectric properties: Q × f = 50,600 GHz, ?_r = 35.12 and τ_f = 9.69 ppm/°C.     

Sintering behavior and microwave dielectric properties of Ca1-xBixW1-xVxO4 ceramics

Structure, sintering behavior and microwave dielectric properties of ceramics have been investigated by x-ray powder diffraction (XRD) and scanning electron microscopy (SEM) in this paper. The microwave dielectric properties of the ceramics were studied with a network analyzer at the frequency of about 6–11 GHz. The sintering temperature and microwave dielectric properties could be successfully tuned in a wide window simultaneously by adjusting the A–O bond characteristics. The sintering temperature of CaWO₄ was successfully reduced from 1100 °C to about 950 °C by BiVO₄ addition. Approximately 95%–96% theoretical density could be obtained after sintering at 950 °C for 2 h. All samples exhibit single Scheelite structure (I4₁/a) phase. The dielectric constant increased, whereas the Q×f value decreased, with the increase of x. The τ_f value changed from negative to positive with the increases of x. Combined excellent microwave dielectric properties with ε_r=22. 1, Q×f=16,730 GHz and τ_f=2.39 ppm/°C could be obtained after sintered at the 950 °C for 2 h for x=0.3 compositions.     

Effects of LiF addition on sintering behavior and microwave dielectric properties of (Mg0.95Zn0.05)2(Ti0.8Sn0.2)O4 ceramics

The effects of LiF addition on the sinterability and microwave dielectric properties of (Mg_0.95Zn_0.05)₂(Ti_0.8Sn_0.2)O₄ (MZTS) ceramics were investigated. A small amount of LiF addition can effectively lower the sintering temperature of MZTS from 1325 °C to 1150 °C due to the liquid phase effect and induce no apparent degradation of the microwave dielectric properties. With increasing LiF content, the apparent density and dielectric constant decreased gradually, the quality factor increased firstly and then decreased. In particular, MZTS–3.0 wt% LiF ceramics sintered at 1150 °C for 5 h exhibited good microwave dielectric properties of ?_r = 13.05, Q · f = 119,310 GHz (at 10 GHz) and τ_f = ?59.2 ppm/°C.     

Low-temperature synthesis and microwave dielectric properties of trirutile-structure MgTa2O6 ceramics by aqueous sol–gel process

Trirutile-structure MgTa₂O₆ ceramics were prepared by aqueous sol–gel method and microwave dielectric properties were investigated. Highly reactive nanosized MgTa₂O₆ powders were successfully synthesized at 500 °C in oxygen atmosphere with particle sizes of 20–40 nm. The evolution of phase formation was detected by DTA–TG and XRD. Sintering characteristic and microwave dielectric properties of MgTa₂O₆ ceramics were studied at different temperatures ranging from 1100 to 1300 °C. With the increase of sintering temperature, density, ?_r and Q · f values increased and saturated at 1200 °C with excellent microwave properties of ?_r ～ 30.1, Q · f ～ 57,300 GHz and τ_f ～ 29 ppm/°C. The sintering temperature of MgTa₂O₆ ceramics was significantly reduced by aqueous sol–gel process compared to conventional solid-state method.     

Influence of sintering temperature on dielectric properties and crystal structure of corundum-structured Mg4Ta2O9 ceramics at microwave frequencies

Microwave dielectric properties of corundum-structured Mg₄Ta₂O₉ ceramics were investigated as a function of sintering temperatures by an aqueous sol–gel process. Crystal structure and microstructure were examined by X-ray diffraction (XRD) technique and field emission scanning electron microscopy (FE-SEM). Sintering characteristics and microwave dielectric properties of Mg₄Ta₂O₉ ceramics were studied as a function of sintering temperature from 1250 °C to 1450 °C. With increasing sintering temperature, the density, ε_r and Qf values increased, saturating at 1300 °C with excellent microwave properties of ε_r=11.9, Qf=195,000 GHz and τ_f=?47 ppm/°C. Evaluation of dielectric properties of Mg₄Ta₂O₉ ceramics were also analyzed by means of first principle calculation method and ionic polarizability theory.     

Low-dielectric-constant LiAlO2 ceramics combined with LBSCA glass for LTCC applications

This study used Li₂O–B₂O₃–SiO₂–CaO–Al₂O₃ (LBSCA) glass to reduce the sintering temperature of LiAlO₂ ceramics and to realise the low dielectric constants (ɛ_r<5) of low-temperature co-fired ceramic (LTCC) materials. LBSCA glass remarkably enhanced the densification of LiAlO₂ ceramics. X-ray diffraction patterns indicated that only the γ-LiAlO₂ phase occurred within the doping range of 1 wt% to 3.5 wt%. Scanning electron microscopy images showed dense and uniform grains in samples with 3.0 wt% LBSCA glass. These samples also exhibited low dielectric constants and low dielectric loss when sintered at 900 °C and 950 °C (i.e., ɛ_r=4.48, Qf=35,540 GHz and τ_f=−53 ppm/°C at 900 °C; ɛ_r=4.50, Qf=38,979 GHz and τ_f=−55 ppm/°C at 950 °C, respectively). The material prepared was chemically compatible with silver and showed potential in applications of high-frequency LTCC microwave substrates.     

Synthesis and microwave dielectric properties of pseudobrookite-type structure Mg5Nb4O15 ceramics by aqueous sol–gel technique

Pseudobrookite-type Mg₅Nb₄O₁₅ ceramics were prepared by aqueous sol–gel process and microwave dielectric properties were investigated. Highly reactive nanosized Mg₅Nb₄O₁₅ powders were successfully synthesized at 600 °C in oxygen atmosphere with particle sizes of 20–40 nm firstly and then phase evolution was detected by DTA-TG and XRD. Sintering characteristics and microwave dielectric properties of Mg₅Nb₄O₁₅ ceramics were studied at different temperatures ranging from 1200 °C to 1400 °C. With the increase of sintering temperature, density, ?_r and Q·f values increased, and then saturated at 1300 °C. Excellent microwave properties of ?_r ～11.3, Q·f ～43,300 GHz and τ_f ～?58 ppm/°C, were obtained finally. The sintering temperature of Mg₅Nb₄O₁₅ ceramics was significantly reduced by aqueous sol–gel process compared to conventional solid-state methods.     

Microwave dielectric properties of BaO–4.3TiO2–0.5ZnO ceramics with BaCu(B2O5)

Effect of BaCu(B₂O₅) (BCB) addition on microwave dielectric properties and sintering behaviors of BaO–4.3TiO₂–0.5ZnO system (BTZ) ceramics were investigated to develop middle-k dielectric composition with low sintering temperatures. When a small amount of BCB was added to BTZ system, the sintering temperature can be lowered from 1100 °C to 900 °C due to the formation of BCB liquid phase. The system added with 7 wt% BCB was sintered at 900 °C for 2 h and ?_r of 31, Q × f of 18,200 GHz and τ_f of 3.8 ppm/°C were obtained. The suitability of BTZ ceramics for tape casting and cofiring with Ag electrodes was investigated, and no evidence of chemical reaction between Ag and ceramics was observed. The dielectric properties of the stacked multilayer plate without any electrodes were also measured. The result shows that the as-prepared BTZ ceramics are suitable for low-temperature co-fired ceramics applications.     

Effects of microwave sintering on the properties of 0.87(Mg0.7Zn0.3)TiO3–0.13(Ca0.61La0.26)TiO3 ceramics

0.87(Mg_0.7Zn_0.3)TiO₃–0.13(Ca_0.61La_0.26)TiO₃ (referred to as 87MZCLT) ceramics were prepared by microwave sintering and conventional sintering. The experimental results demonstrated that the sintering cycle of 87MZCLT ceramics was greatly shortened and the impurity phase (Mg_0.7Zn_0.3)Ti₂O₅ was eliminated by microwave sintering. Moreover, the 87MZCLT ceramics prepared by microwave sintering show more uniform, fine-grained microstructure as well as much less Zn evaporation. As a result, the quality factor was increased by 40% compared with conventional sintering. All samples were sintered at 1275 °C for 20 min with heating and cooling rate of 15 °C/min and gave excellent microwave dielectric properties: ?_r = 26.21, Q × f = 120,000 GHz, τ_f = ?3 ppm/°C.     

Sintering behavior and microwave dielectric properties of 0.67CaTiO3–0.33LaAlO3 ceramics modified by B2O3–Li2O–Al2O3 and CeO2

A low temperature sintering method was used to avoid the relatively high sintering temperatures typically required to prepare 0.67CaTiO₃–0.33LaAlO₃ (CTLA) ceramics. Additionally, CeO₂ was introduced into the CTLA ceramics as an oxygen-storage material to improve their microwave dielectric properties. 0.67CaTiO₃–0.33LaAlO₃ ceramics co-doped with B₂O₃–Li₂O–Al₂O₃ and CeO₂ were prepared by a conventional two-step solid-state reaction process. The sintering behavior, crystal structure, surface morphology, and microwave dielectric proprieties of the prepared ceramic samples were studied, and the reaction mechanism of CeO₂ was elucidated. CTLA+0.05 wt% BLA+3 wt% CeO₂ ceramics sintered at 1360 °C for 4 h exhibited the optimal microwave dielectric properties: dielectric constant (ε_r)=45.02, quality factor (Q×f)=43102 GHz, and temperature coefficient of resonant frequency (τ_f)=2.1 ppm/°C. The successful preparation of high-performance microwave dielectric ceramics provides a direction for the future development and commercialization of CTLA ceramics.     

Low temperature firing of BiSbO4 microwave dielectric ceramic with B2O3–CuO addition

The influence of B₂O₃–CuO addition on the sintering behavior, phase composition, microstructure and microwave dielectric properties of BiSbO₄ ceramic have been investigated. The BiSbO₄ ceramics can be well densified to approach above 95% theoretical density in the sintering temperature range from 840 to 960 °C as the addition amount of B₂O₃–CuO increases from 0.6 to 1.2 wt.%. Sintered ceramic samples were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The microwave permittivity ?_r saturated at 19–20 and Qf values varied between 33,000 and 46,000 GHz while temperature coefficient of resonant frequency shifting between ?70 and ?60 ppm/°C at sintering temperature around 930 °C. Lowering sintering temperature of BiSbO₄ ceramics makes it possible for application in low temperature co-fired ceramic technology.     

Characterization and dielectric behavior of willemite and TiO2-doped willemite ceramics at millimeter-wave frequency

Willemite ceramics (Zn₂SiO₄) have been successfully prepared in the temperature range from 1280 to 1340 °C. It is found that willemite ceramics possess excellent millimeter-wave dielectric properties: a dielectric constant ɛ_r value of 6.6, a quality factor Q × f value of 219,000 GHz and a temperature coefficient of resonant frequency τ_f value of −61 ppm/°C. By adding TiO₂ with large positive τ_f value (450 ppm/°C), near zero τ_f value can be achieved in a wide sintering temperature range. With 11 wt% of TiO₂, an ɛ_r value of 9.3, a Q × f value of 113,000 GHz, and a τ_f value of 1.0 ppm/°C are obtained at 1250 °C. The relationships between microstructure and properties are also studied. Our results show that willemite with appropriate TiO₂ is an ideal temperature stable, low ɛ_r and high Q × f dielectric for millimeter-wave application.     

Synthesis,characterization, and dielectric properties of low loss LaBO3 ceramics

The preparation, sintering behaviour, and dielectric properties of low loss LaBO₃ ceramics have been investigated. Single-phase LaBO₃ powder was synthesized by the conventional solid-state ceramics route and dense ceramics (relative density >96%) with uniform microstructure (grain size ～30 μm) were obtained by sintering at 1300 °C in air. The electrical conductivity of LaBO₃ follows the Arrhenius law and the related activation energies for electrical conduction of bulk and grain boundary are 0.62 eV and 0.90 eV, respectively. The LaBO₃ ceramics sintered at 1300 °C exhibit excellent microwave dielectric properties with a relative permittivity, ?_r ～ 11.8, a quality factor, Q × f₀ value ～76,869 GHz (at ～15 GHz), and a negative temperature coefficient of resonant frequency τ_f ～ ?52 ppm/°C.     

Low-temperature sintered MgWO4–CaTiO3 ceramics with near-zero temperature coefficient of resonant frequency

The phases, microstructure, composition analysis and microwave dielectric properties of (1 ? x)MgWO₄–xCaTiO₃ ceramics with Li₂CO₃–4H₃BO₃ additions prepared by solid-state reaction method have been investigated by using X-ray diffraction, scanning electron microscopy, energy-dispersive spectroscopy and advantest network analyzer. The τ_f of (1 ? x)MgWO₄–xCaTiO₃ were dependent on phase constitutions. The microwave dielectric properties of 0.91MgWO₄–0.09CaTiO₃ ceramics with Li₂CO₃–4H₃BO₃ were characterized, the results indicated that the ?_r and Q × f were associated with the sintering temperature and amount of Li₂CO₃–4H₃BO₃. The sintering temperature of ceramics was reduced to 950 °C from 1150 °C and τ_f was modified to 0 ppm/°C with good Q × f. Addition of 5.0 wt% Li₂CO₃–4H₃BO₃ in 0.91MgWO₄–0.09 CaTiO₃ ceramics sintered at 950 °C showed excellent dielectric properties of ?_r = 15.5, Q × f = 20,780 GHz (f = 7.1 GHz) and τ_f ～ 0 ppm/°C. The material has a chemical compatibility with silver, making it a very promising candidate materials for LTCC applications.     

Microwave dielectric properties of LiNb3O8 ceramics with TiO2 additions

The microwave dielectric properties of LiNb₃O₈ ceramics were investigated as a function of the sintering temperature and the amount of TiO₂ additive. LiNb₃O₈ ceramics, which were calcined at 750 °C and sintered at 1075 °C for 2 h, showed a dielectric constant (ɛ_r) of 34, a quality factor (Q × f₀) of 58,000 GHz and a temperature coefficient of resonance frequency (τ_f) of −96 ppm/°C, respectively. The density of the samples influenced the properties of these properties. As the TiO₂ content increased in the LiNb₃O₈–TiO₂ system, ɛ_r and τ_f of the material were increased due to the mixing effect of TiO₂ phase, which has higher dielectric constant and larger positive τ_f. The 0.65LiNb₃O₈–0.35TiO₂ ceramics showed a dielectric constant ɛ_r of 46.2, a quality factor (Q × f₀) of 5800 GHz and a temperature coefficient of resonance frequency τ_f of near to 0 ppm/°C.     

Microwave dielectric properties of YAG ceramics prepared by sintering pyrolysised nano-sized powders

YAG ceramics with good dielectric properties were prepared via a modified pyrolysis method, with yttrium nitrate as the yttrium source and combined aluminium sulphate and aluminium nitrate as aluminium sources, and subsequent sintering in a muffle furnace. The effects of the different aluminium sources on the powder characteristic and the impact of sintering temperature, sintering aids (TEOS) and additive (TiO₂) on the dielectric properties of the ceramics were studied. The results show that well-dispersed pure YAG nano-powders can be obtained after calcination at 1000 °C with an aluminium sulphate and aluminium nitrate molar ratio of 1.5:2. The relative density, permittivity (ε_r) and quality factor (Q×f) of the YAG ceramics increase with sintering temperature and TEOS addition. TiO₂ can greatly promote τ_f to near-zero but decreases Q×f. The relative density, ε_r, Q×f and τ_f of the YAG–1 wt% TEOS–1 wt% TiO₂ ceramic obtained at 1520 °C are 97.6%, 9.9, 71, 738 GHz and −30 ppm/°C, respectively.     

Two novel ultralow temperature firing microwave dielectric ceramics LiMVO6 (M = Mo,W) and their chemical compatibility with metal electrodes

Low temperature cofired ceramics technology (LTCC) has been widely studied and used in wireless communication because of their outstanding capability for device miniaturization and integration. However, many commercial microwave dielectric materials have high sintering temperatures that pose challenge for cofiring with inner electrodes. Herein, two brannerite vanadate LiMVO₆ (M = Mo, W) ceramics with intrinsically low sintering temperatures were prepared. Dense and stable LiMVO₆ (M = Mo, W) ceramics could obtained at 640 °C for LiMoVO₆ and 700 °C for LiWVO₆. Favorable microwave dielectric properties were also obtained with ε_r = 13.3, Q × f = 12,460 GHz, and τ_f = +101.0 ppm/°C for LiMoVO₆ and ε_r = 11.5, Q × f = 13,260 GHz, and τ_f = +163.8 ppm/°C for LiWVO₆. Moreover, the relationship between crystal structure and microwave dielectric properties was studied by means of packing fraction, bond valence, and octahedral distortion. Their chemical compatibility with the metal electrodes were confirmed.     

Microwave dielectric properties and low-temperature sintering of Ba3Ti4Nb4O21 ceramics with B2O3 and CuO additions

The low sintering temperature and the good dielectric properties such as high dielectric constant (ɛ_r), high quality factor (Q × f) and small temperature coefficient of resonant frequency (τ_f) are required for the application of chip passive components in the wireless communication technologies. In the present study, the sintering behaviors and dielectric properties of Ba₃Ti₄Nb₄O₂₁ ceramics were investigated as a function of B₂O₃–CuO content. Ba₃Ti₄Nb₄O₂₁ ceramics with B₂O₃ or CuO addition could be sintered above 1100 °C. However, the additions of both B₂O₃ and CuO successfully reduced the sintering temperature of Ba₃Ti₄Nb₄O₂₁ ceramics from 1350 to 900 °C without detriment to the microwave dielectric properties. From the X-ray diffraction (XRD) studies, the sintering behaviors and the microwave dielectric properties of low-fired Ba₃Ti₄Nb₄O₂₁ ceramics were examined and discussed in the formation of the secondary phases. The Ba₃Ti₄Nb₄O₂₁ sample with 1 wt% B₂O₃ and 3 wt% CuO addition, sintered at 900 °C for 2 h, had the good dielectric properties: ɛ_r = 65, Q × f = 16,000 GHz and τ_f = 101 ppm/°C.