A Novel Low‐Firing and Low Loss Microwave Dielectric Ceramic Li2Mg2W2O9 with Corundum Structure

The crystal structure and microwave dielectric properties of a novel low‐firing compound Li₂Mg₂W₂O₉ were investigated in this study. The phase purity and crystal structure were investigated using X‐ray diffraction analyses and Rietveld refinement. The best microwave dielectric properties of the ceramic with a low permittivity (ε_r) ~11.5, a quality factor (Q × f) ~31 900 GHz (at 10.76 GHz) and a temperature coefficient of the resonant frequency (τ_f) ~ ?66.0 ppm/°C were obtained at the optimum sintering temperature (920°C). CaTiO₃ was added into the Li₂Mg₂W₂O₉ ceramic to obtain a near zero τ_f, and 0.93Li₂Mg₂W₂O₉–0.07CaTiO₃ ceramic exhibited improved microwave dielectric properties with a near‐zero τ_f ~ ?1.3 ppm/°C, a ε_r ~21.6, a high Q_u × f value ~20 657 GHz. The low sintering temperature and favorable microwave dielectric properties make it a promising candidate for LTCC applications.     

Low‐Temperature Sintering Microwave Characteristics of B2O3‐doped CaLa4Ti4O15 Dielectric Ceramics

Preparation and microwave dielectric properties of B₂O₃‐doped CaLa₄Ti₄O₁₅ ceramics have been investigated. X‐ray diffraction data show that CaLa₄Ti₄O₁₅ ceramic has a trigonal structure coupled with a second phase of CaLa₄Ti₅O₁₇. The CaLa₄Ti₄O₁₅ ceramic with addition of 0.5 wt% B₂O₃, sintered at 1220°C for 4 h, exhibits microwave dielectric properties with a dielectric constant of 45.8, Q × f value of 24,000 GHz, and temperature coefficient of resonant frequency (τ_f) of ?19 ppm/^°C. B₂O₃‐doped CaLa₄Ti₄O₁₅ ceramics, which have better sintering behavior (decrease in sintering temperature ~ 330°C) and dielectric properties than pure CaLa₄Ti₄O₁₅ ceramics, are candidates for applications in microwave devices.     

Low‐Fire Processing of Microwave BNBT‐Based High‐k Dielectric with Li2O–ZnO–B2O3 Glass

The effects of Li₂O–ZnO–B₂O₃ (LZB) glass addition on densification and dielectric properties of Ba₄(Nd_0.85Bi_0.15)_9.33Ti₁₈O₅₄ (BNBT) have been investigated. At a given ratio of ZnO/B₂O₃, the glass softening point decreases, but the thermal expansion coefficient and dielectric constant increase with increasing Li₂O content in the LZB glass. With 10 vol% LZB glass, the densification temperature reduces greatly from 1300°C for pure BNBT to 875°C–900°C for BNBT + LZB dielectric, and the densification enhancement becomes more significant with increasing Li₂O content in the LZB glass. The above result is attributed to a chemical reaction taking place at the interface of LZB/BNBT during firing, which becomes less extensive with increasing Li₂O content in the LZB glass. Therefore, more residual LZB glass, which acts as a densification promoter to BNBT, is left with increasing Li₂O content. For the LZB glass with a Li₂O content in the range 10–30 mol%, the resulting 90 vol% BNBT + 10 vol% LZB microwave dielectric has a dielectric constant of 55–70, product (Q × f_r) of quality factor (Q) and resonant frequency (f_r) of 1000–3000 GHz at 5–5.79 GHz, and a temperature coefficient of resonant frequency (τ_f) of 10–60 ppm/°C in the temperature range between 25°C and 80°C.     

Novel Temperature Stable Li2MnO3 Dielectric Ceramics with High Q for LTCC Applications

Novel microwave dielectric ceramics in the Li₂MnO₃ system with high Q prepared through a conventional solid‐state route had been investigated. All the specimens exhibited single phase ceramics sintered in the temperature range 1140°C–1230°C. The microwave dielectric properties of Li₂MnO₃ ceramics were strongly correlated with sintering temperature and density. The best microwave dielectric properties of ε_r = 13.6, Q × f = 97 000 (GHz), and τ_f = ?5.2 ppm/°C could be obtained as sintered at 1200°C for 4 h. BaCu(B₂O₅) (BCB) could effectively lower the sintering temperature from 1200°C to 930°C and slightly induced degradation of the microwave dielectric properties. The Li₂MnO₃ ceramics doped with 2 wt% BaCu(B₂O₅) had excellent dielectric properties of ε_r = 11.9, Q × f = 80 600 (GHz), and τ_f = 0 ppm/°C. With low sintering temperature and good dielectric properties, the BCB added Li₂MnO₃ ceramics are suitable candidates for LTCC applications in wireless communication system.     

Low‐temperature sintering and thermal stability of Li2GeO3‐based microwave dielectric ceramics with low permittivity

A low‐permittivity dielectric ceramic Li₂GeO₃ was prepared by the solid‐state reaction route. Single‐phase Li₂GeO₃ crystallized in an orthorhombic structure. Dense ceramics with high relative density and homogeneous microstructure were obtained as sintered at 1000‐1100°C. The optimum microwave dielectric properties were achieved in the sample sintered at 1080°C with a high relative density ~ 96%, a relative permittivity ε_r ~ 6.36, a quality factor Q × f ~ 29 000 GHz (at 14.5 GHz), and a temperature coefficient of resonance frequency τ_f ~ ?72 ppm/^°C. The sintering temperature of Li₂GeO₃ was successfully lowered via the appropriate addition of B₂O₃. Only 2 wt.% B₂O₃ addition contributed to a 21.2% decrease in sintering temperature to 850°C without deteriorating the dielectric properties. The temperature dependence of the resonance frequency was successfully suppressed by the addition of TiO₂ to form Li₂TiO₃ with a positive τ_f value. These results demonstrate potential applications of Li₂GeO₃ in low‐temperature cofiring ceramics technology.     

Low‐Temperature Sinterable (1−x)Ba3(VO4)2–xLiMg0.9Zn0.1PO4 Microwave Dielectric Ceramics

The novel low‐temperature sinterable (1 ? x)Ba₃(VO₄)₂–xLiMg_0.9Zn_0.1PO₄ microwave dielectric ceramics were prepared by cofiring the mixtures of pure‐phase Ba₃(VO₄)₂ and LiMg_0.9Zn_0.1PO₄. The phase structure and grain morphology of the ceramics were evaluated using X‐ray diffraction, Raman spectra, and scanning electron microscopy. The results indicated that Ba₃(VO₄)₂ and LiMg_0.9Zn_0.1PO₄ phases can well coexist in the sintered body. Nevertheless, a small amount of LiZnPO₄ and some vanadate phases with low melting points were observed, which not only can influence the microwave dielectric properties of the ceramic but also can obviously improve the densification behavior at a relatively low sintering temperature. The near‐zero temperature coefficients of the resonant frequency (τ_f) could be achieved by adjusting the relative content of the two phases owing to their opposite τ_f values and simultaneously a desirable quality factor Q × f value can be maintained. No chemical reaction between the matrix ceramic phase and Ag took place after sintering at 800°C for 4 h. The ceramics with 45 vol% LiMg_0.9Zn_0.1PO₄ can be well sintered at only 800°C and exhibit excellent microwave dielectric properties of ε_r ~ 10, Q × f ~ 64 500 GHz, and τ_f ~ ?2.1 ppm/°C, thus showing a great potential as a low‐permittivity low‐temperature cofired microwave dielectric material.     

Liquid‐phase sintering,microstructural evolution,and microwave dielectric properties of Li2Mg3SnO6–LiF ceramics

The liquid‐phase sintering behavior and microstructural evolution of x wt% LiF aided Li₂Mg₃SnO₆ ceramics (x = 1‐7) were investigated for the purpose to prepare dense phase‐pure ceramic samples. The grain and pore morphology, density variation, and phase structures were especially correlated with the subsequent microwave dielectric properties. The experimental results demonstrate a typical liquid‐phase sintering in LiF–Li₂Mg₃SnO₆ ceramics, in which LiF proves to be an effective sintering aid for the Li₂Mg₃SnO₆ ceramic and obviously reduces its optimum sintering temperature from ~1200°C to ~850°C. The actual sample density and microstructure (grain and pores) strongly depended on both the amount of LiF additive and the sintering temperature. Higher sintering temperature tended to cause the formation of closed pores in Li₂Mg₃SnO₆‐x wt% LiF ceramics owing to the increase in the migration ability of grain boundary. An obvious transition of fracture modes from transgranular to intergranular ones was observed approximately at x = 4. A single‐phase dense Li₂Mg₃SnO₆ ceramic could be obtained in the temperature range of 875°C‐1100°C, beyond which the secondary phase Li₄MgSn₂O₇ (<850°C) and Mg₂SnO₄ (>1100°C) appeared. Excellent microwave dielectric properties of Q × f = 230 000‐330 000 GHz, ε_r = ~10.5 and τ_f = ~?40 ppm/°C were obtained for Li₂Mg₃SnO₆ ceramics with x = 2‐5 as sintered at ~1150°C. For LTCC applications, a desirable Q × f value of ~133 000 GHz could be achieved in samples with x = 3‐4 as sintered at 875°C.     

Microwave Dielectric Properties of Novel Glass‐Free Low‐Firing Li2CeO3 Ceramics

Novel glass–free low temperature firing microwave dielectric ceramics Li₂CeO₃ with high Q prepared through a conventional solid‐state reaction method had been investigated. All the specimens in this paper have sintering temperature lower than 750°C. XRD studies revealed single cubic phase. The microwave dielectric properties were correlated with the sintering conditions. At 720°C/4 h, Li₂CeO₃ ceramics possessed the excellent microwave dielectric properties of ε_r = 15.8, Q × f = 143 700 (GHz), and τ_f  = ?123 ppm/°C. Li₂CeO₃ ceramics could be excellent candidates for glass‐free low‐temperature co‐fired ceramics substrates.     

Microwave Dielectric Properties of a Low‐Firing Ba2BiV3O11 Ceramic

A low‐firing microwave dielectric ceramic Ba₂BiV₃O₁₁ was prepared via solid‐state reaction method. Ba₂BiV₃O₁₁ ceramic could be well sintered at 840°C–880°C, with a ε_r ~14.2, a high Q × f value ~68 700 GHz (at 8.7 GHz), and a negative temperature coefficient of ?81 ppm/°C. τ_f of Ba₂BiV₃O₁₁ was tuned to be near zero by formation of a composite with TiO₂. 0.7Ba₂BiV₃O₁₁–0.3TiO₂ ceramic sintered at 910°C showed improved properties with ε_r = 15.7, Q × f = 53 200 GHz, and τ_f  = ?2 ppm/°C.     

Low‐Temperature Sintering and Microwave Dielectric Properties of CaMoO4‐Based Temperature Stable LTCC Material

The CaMoO₄–xY₂O₃–xLi₂O ceramics were prepared by the solid‐state reaction method. The sintering behavior, phase evolution, microstructure, and microwave dielectric properties were investigated. CaMoO₄ solid solution was obtained when x = 0.030, and two‐phase system including tetragonal CaMoO₄ phase and cubic Y₂O₃ phase formed when 0.066 ≤ x ≤ 1.417. A temperature stable CaMoO₄‐based microwave dielectric ceramic with ultralow sintering temperature (775°C) was obtained in the CaMoO₄–xY₂O₃–xLi₂O system when x = 0.306, which showed good microwave dielectric properties with a low permittivity of 9.5, a high Q_f value of 63 240 GHz, and a near‐zero temperature coefficient of resonant frequency of +7.2 ppm/°C.     

Cold sintering co-firing of (Ca,Bi)(Mo,V)O4–PTFE composites in a single step

Because of large differences in the processing temperature windows between ceramics and polymers, the single-step co-sintering of microwave dielectric ceramic–polymer substrates remains challenging. In this work, a dense (Ca_0.65Bi_0.35)(Mo_0.65V_0.35)O₄ (CBMVO) ceramic was first prepared through cold sintering at 150°C, under a uniaxial pressure of 300 MPa for 60 min with Li₂MoO₄ (LMO) as a transient low-temperature solvent. Cold-sintered CBMVO–5 wt% LMO ceramic shows excellent microwave dielectric properties: ε_r ∼ 11.4, Q × f ∼ 7070 GHz, τ_f ∼ −7.4 ppm/°C. Moreover, the optimized cold sintering process enabled the preparation of a layered co-sintered (2–2 type) CBMVO–polytetrafluoroethylene composite, which maintained excellent microwave dielectric properties and showed a good heterogeneous interface bonding. The proposed cold sintering co-firing of ceramic–polymer composites in a single step shows great potential for application in the seamless integration between ceramics and polymer substrates.     

Silver Co‐Firable Li2ZnTi3O8 Microwave Dielectric Ceramics with LZB Glass Additive and TiO2 Dopant

New dielectric ceramics are prepared by the conventional solid‐state ceramic route. Effects of LZB glass on sintering, phase purity, microstructure, and dielectric properties of Li₂ZnTi₃O₈ ceramics have been investigated. Adding LZB lowers sintering temperature from 1050°C to 875°C, and does not induce much degradation of dielectric properties. The 1.0 wt% LZB glass‐added ceramic has better properties of ε_r = 23.9, Q × f = 31,608 GHz, τ_f = ?14.3 ppm/°C. Additions of TiO₂ markedly improve microwave properties. Typically, the Li₂ZnTi₃O₈ + 1 wt%LZB + 3.5 wt%TiO₂ sintered at 900°C shows ε_r = 26.1, Q × f = 45,168 GHz, τ_f = ?4.1 ppm/°C. Compatibility with Ag electrode indicates that this material may be applied to LTCC devices.     

Low‐firing and temperature stable microwave dielectric ceramics: Ba2LnV3O11 (Ln = Nd,Sm)

Low‐firing and temperature stable microwave dielectric ceramics of Ba₂LnV₃O₁₁ (Ln = Nd, Sm) were prepared by solid‐state reaction. X‐ray diffraction (XRD) and scanning electron microscopy (SEM) were used to investigate the phase purity, crystal structure, sintering behavior, and microstructure. The XRD patterns indicated that Ba₂LnV₃O₁₁ (Ln = Nd, Sm) ceramics belong to monoclinic crystal system with P2₁/c space group in the whole sintering temperature range (800°C ‐900°C). Both ceramics could be well densified at 880°C for 4 hours with relative densities higher than 96%. The Ba₂LnV₃O₁₁ (Ln = Nd, Sm) samples sintered at 880°C for 4 hours exhibited excellent microwave dielectric properties: ε_r = 12.05, Q × f = 23 010 GHz, τ_f = ?7.7 ppm/°C, and ε_r = 12.19, Q × f = 27 120 GHz, τ_f = ?16.2 ppm/°C, respectively. Besides, Ba₂LnV₃O₁₁ (Ln = Nd, Sm) ceramics could be well co‐fired with the silver electrode at 880°C.     

Effects of ZnO and B2O3 on the Microstructure and Microwave Dielectric Properties of 5Li2O‐1Nb2O5‐5TiO2 Ceramics

The effects of ZnO and B₂O₃ addition on the sintering behavior, microstructure, and the microwave dielectric properties of 5Li₂O‐1Nb₂O₅‐5TiO₂ (LNT) ceramics have been investigated. With addition of low‐level doping of ZnO and B₂O₃, the sintering temperature of the LNT ceramics can be lowered down to near 920°C due to the liquid phase effect. The Li₂TiO₃ss and the “M‐phase” are the two main phases, whereas other phase could be observed when co‐doping with ZnO and B₂O₃ in the ceramics. And the amount of the other phase increases with the ZnO content increasing. The addition of ZnO does not induce much degradation in the microwave dielectric properties but lowers the τ_f value to near zero. Typically, the good microwave dielectric properties of ε_r = 36.4, Q × f = 8835 GHz, τ_f = 4.4 ppm/°C could be obtained for the 1 wt% B₂O₃ and 4 wt% ZnO co‐doped sample sintered at 920°C, which is promising for application of the multilayer microwave devices using Ag as internal electrode.     

Preparation and Microwave Dielectric Properties of Ultra‐low Temperature Sintering Ceramics in K2O–MoO3 Binary System

A series of microwave dielectric ceramics in the compositions of K₂Mo₂O₇, K₂Mo₃O₁₀, and K₂Mo₄O₁₃ in K₂O–MoO₃ binary system with ultra low sintering temperatures were prepared using the solid‐state reaction method. Their synthesis, phase composition, compatibility with metal electrodes, microstructures, and microwave dielectric properties were investigated. The K₂Mo₂O₇ ceramic sintered at 460°C with a triclinic structure has a relative permittivity of 7.5, a Q × f value of 22 000 GHz, and a τ_f value of ?63 ppm/°C. The X‐ray diffraction patterns indicate that K₂Mo₂O₇ does not react with Ag and Al electrodes at the co‐fired temperatures. The K₂Mo₃O₁₀ ceramic can be sintered well at 520°C with a relative permittivity of 5.6, a Q × f value of 35 830 GHz, and a τ_f value of ?92 ppm/°C. It has compatibility with Ag electrode. The K₂Mo₄O₁₃ ceramic sintered at 540°C possesses good microwave dielectric properties with a relative permittivity of 6.8, a Q × f value of 39 290 GHz and a τ_f value of ?67 ppm/°C and it is compatible with Al electrode. For K₂Mo₂O₇ and K₂Mo₄O₁₃, it is found that the grain sizes and the number of grain boundaries play an important role in the dielectric loss. From this study, it can be seen that the three ceramics in K₂O–MoO₃ system have good microwave dielectric properties, ultra‐low sintering temperatures, non‐toxic, and low‐cost characteristics. So they can be potentially applied to ultra‐LTCC devices.     

Microwave Dielectric Properties of Ultralow‐Temperature Cofirable Ba3V4O13 Ceramics

Ultralow‐temperature sinterable Ba₃V₄O₁₃ ceramics have been prepared through solid‐state ceramic route. Structural properties of the ceramic material are studied using powder X‐ray diffraction. Ba₃V₄O₁₃ ceramic has monoclinic structure and the existence of [V₄O₁₃]^6? polyhedra is confirmed through Laser Raman studies. The sample sintered at 600°C for 1 h shows dense microstructure with microwave dielectric properties of ε_r = 9.6, Q × f = 56 100 GHz, and τ_f = ?42 ppm/°C. The ceramics under study show good chemical compatibility with aluminum during cofiring.     

Low-fire processing and microwave dielectric properties of LB glass-doped Ba3.75Nd9.5Ti17.5(Cr0.5Nb0.5)0.5O54 ceramic

The effects of LB glass on the sintering behavior, structure, and dielectric properties for the Ba_3.75Nd_9.5Ti_17.5(Cr_0.5Nb_0.5)_0.5O₅₄ (BNTCN) ceramic were investigated. The results showed that the LB glass, as an effective sintering aid, successfully lowered the sintering temperature of BNTCN ceramic by formation of the liquid phase. Furthermore, the change of the structure and decrease in grain size had influences on the electrical conductivity, thermal stability, and microwave dielectric properties for the BNTCN ceramics doped LB glass. Finally, the excellent microwave dielectric properties with ε_r = 73.4, Q × f = 5277 GHz, and τ_f = +7.1 ppm/°C were obtained for samples sintered at 950°C when x = 5, indicating the BNTCN ceramic doped with 5 wt% LB glass is a promoting LTCC material.     

A Novel Magnetodielectric Solid Solution Ceramic 0.4LiFe5O8–0.6Li2MgTi3O8 with Excellent Microwave Dielectric Properties

In this study, a novel spinel solid solution ceramic of 0.4LiFe₅O₈–0.6Li₂MgTi₃O₈ (0.4LFO–0.6LMT) has been developed and investigated. It is found that the 40 mol% LiFe₅O₈ and 60 mol% Li₂MgTi₃O₈ are fully soluble in each other and a disordered spinel phase is formed. The ceramic sample sintered at 1050°C/2 h exhibits both good magnetic and dielectric properties in the frequency range 1–10 MHz, with a permeability between 29.9~14.1 and magnetic loss tangent between 0.12~0.67, permittivity between 16.92~16.94 and dielectric loss tangent between 5.9 × 10^?3–2.3 × 10^?2. The sample also has good microwave dielectric properties with a relative permittivity of 16.1, a high quality factor (Q × f) ~28 500 GHz (at 7.8 GHz). Furthermore, 3 wt% H₃BO₃–CuO (BCu) addition can effectively lower the sintering temperature to 925°C and does not degrade the magnetodielectric properties. The chemical compatibility with silver electrode indicates that this kind of ceramics is a good candidate for the low‐temperature cofired ceramic (LTCC) application.     

Improvement of microwave dielectric properties of the LiNb0.6Ti0.5O3 M-phase by doping with (Co1/3Nb2/3)4+

Structural evolution and microwave dielectric properties of LiNb_0.6(Ti_1-x[Co_1/3Nb_2/3]_x)_0.5O₃ (.05≤x≤.2) ceramics have been studied in this paper. Although the doped compositions maintain the M-phase solid solutions, compositional fluctuation due to nonuniform dispersion of minor dopants could be observed as x < .05, and trace amount of Li₂TiO₃-based solid solution (Li₂TiO₃ss) secondary phase presents in the x > .05 compositions. The microwave dielectric properties could be remarkably improved by the doping of (Co_1/2Nb_1/2)⁴⁺ in comparison to the undoped counterpart. Optimized microwave dielectric properties with Q × f = ∼6500 GHz, ε_r = ∼74 and τ_f = +8.2 ppm/°C could be obtained at x = .10 after sintering at 1050°C/2 h. The sintering temperature could be further reduced to 900°C/2 h by adding .2 wt% B₂O₃ without affecting significantly its microwave dielectric properties: ε_r = 73, Q × f = 6000 GHz, τ_f = +8.5 ppm/°C. The LiNb_0.6(Ti_1-x[Co_1/3Nb_2/3]_x)_0.5O₃ ceramics obtained in this case exhibit large dielectric permittivity coupled with much improved Q × f values, near zero τ_f, and low sintering temperature simultaneously, which makes it a promising high-k microwave dielectric material for low temperature cofired ceramic applications.     

Facile Synthesis of “Quench‐Free Glass” and Ceramic‐Glass Composite for LTCC Applications

The 10 mol% ZnO–2 mol% B₂O₃–8 mol% P₂O₅–80 mol% TeO₂ (ZBPT) glass was prepared by quenching as well as slowly cooling the melt. The ZBPT glass prepared by both methods show similar microwave dielectric properties. ZBPT glass has an ε_r of 22.5 (at 7 GHz), Q_u × f of 1500 GHz, and τ_f of ?100 ppm/°C. The ceramic‐glass composites of Sr₂ZnTeO₆ (SZT) and ZBPT is prepared through two convenient methods: (a) conventional way of co‐firing the ceramic with ZBPT glass powder and (b) a nonconventional facile route by co‐firing the ceramic with precursor oxide mixture of ZBPT glass at 950°C. In the former route, SZT + 5 wt% ZBPT composite sintered at 950°C showed moderately good microwave dielectric properties (ε_r = 13.4, Q_u × f = 4500 GHz and τ_f = ?52 ppm/°C). Although the SZT + 5 wt% ZBPT composite prepared through the nonconventional method also showed similar microwave dielectric properties (ε_r = 13.8, Q_u × f = 5300 GHz and τ_f = ?50 ppm/°C), the synthesis procedure is much simplified in the latter case. The composites are found to be chemically compatible with Ag. The composite containing 5 wt% ZBPT prepared through conventional and nonconventional ways shows linear coefficients of thermal expansion of 7.0 ppm/°C and 7.1 ppm/°C, respectively. Both the composites have a room‐temperature thermal conductivity of 2.1 Wm^?1 K^?1.