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1.
x ZnO- (100-x) B2O3 (x = 45–64 mol%) glass-ceramics for ULTCC applications were prepared via the solid-state reaction method, and their crystallization behavior, sintering mechanism, microstructure and microwave dielectric properties were investigated. In this work, the zinc boron binary glasses can be formed in the range of 45–73 mol% ZnO content, and the glass with 55 mol% ZnO content has the highest glass-forming ability. The Zn4B6O13 crystal is formed in binary ZnO-B2O3 glass at 640 °C, which is much lower than that in ceramics. The glass-ceramics exhibit large grains with 5 ~ 10 µm consisting of fine and uniform secondary structures. The precipitation of Zn4B6O13 crystal and the refinement secondary structure improves the microwave dielectric properties. The 55 ZnO - 45 B2O3 glass-ceramic sintered at 640 °C for 5 h exhibits the optimum microwave dielectric properties of εr = 6.09, Q×f = 20,389 GHz, τf = 14 ppm/°C, and also high Vickers hardness of 625 kgf/mm2 and good chemical compatibility with Ag or Al electrode, which is a good candidate for ULTCC substrate materials.  相似文献   

2.
《Ceramics International》2019,45(16):19689-19694
Li–Al–B–Si–O (LABS) glass-ceramics with a sintering temperature of 600 °C were studied for ultra-low temperature co-fired ceramics (ULTCC) applications. The crystal phase of LABS glass-ceramics is dendritic β-spodumene. The permittivity and dielectric loss of LABS glass-ceramics are εr = 5.8 and tgδ = 1.3 × 10−3 at 10 MHz, respectively. The coefficient of thermal expansion (CTE) of LABS glass-ceramics is 3.23 ppm/°C, which is close to that of silicon. The dielectric and thermal properties of LABS glass-ceramics are closely correlated to the degree of its crystallization. The permittivity decreases continually while the dielectric loss decreases first and slightly increases with the increasing of crystallization of β-spodumene. The CTE of LABS glass-ceramics decreases as β-spodumene crystallized from LABS glass. The crystallization kinetic and mechanism of LABS glass-ceramics indicate that the β-spodumene crystallizes in a two-dimensional interfacial growth mechanism due to the migration of Li-ions. The diffusion coefficients derived from energy-dispersive X-ray spectroscopy (EDS) results indicated that both Al and Ag electrodes have good compatibilities with ULTCC tapes, which could reduce the cost of multilayer electro-ceramic devices dramatically by using the ULTCC and base metallization.  相似文献   

3.
《Ceramics International》2022,48(14):20053-20061
The composition governs the crystallization ability, the type and content of crystal phases of glass-ceramics. Glass-ceramic joining materials have generated more research interest in recent years. Here, we prepared a novel Li2O–MgO–Al2O3–SiO2 glass-ceramic for the application of joining Si3N4 ceramics. We investigated the influence of the MgO/Al2O3 composition ratio on microstructure and crystallization behaviour. The crystallization kinetics demonstrated that the glasses had excellent crystallization ability and high crystallinity. β-LiAlSi2O6 and Mg2SiO4 were precipitated from the glass-ceramics, and the increase of MgO concentration was conducive to the precipitation of Mg2SiO4. Among the glass-ceramic samples, the thermal expansion coefficient of LMAS2 glass-ceramic was 3.1 × 10?6/°C, which was very close to that of Si3N4 ceramics. The wetting test showed that the final contact angle of the glass droplet on the Si3N4 ceramic surface was 32° and the interface was well bonded.  相似文献   

4.
The dielectric and structural properties of the as-quenched melts of three CaO–B2O3–SiO2 compositions (denoted CBS-1, CBS-2, and CBS-3) were investigated to determine their suitability for use in millimeter-wave applications. The CBS-1 glass-ceramic exhibited the lowest coefficient of thermal expansion (CTE = 3.2 ppm/°C), lowest dielectric constant (εr = 4.04) at 60 GHz, and highest dielectric loss (tan δ = 0.0029) at 60 GHz, which were attributed to the presence of quartz (SiO2) as the major phase. In contrast, as the major phase constituent of the CBS-2 and CBS-3 glass-ceramics was β-CaSiO3, they presented relatively high CTEs (6.6 and 5.9 ppm/°C, respectively), relatively high dielectric constants at 60 GHz (6.29 and 7.61, respectively), and relatively low dielectric losses at 60 GHz (0.0020 and 0.0012, respectively). The CBS-1 glass-ceramic exhibited the highest dielectric loss because of the presence of SiO2 as the major phase constituent as well as lattice scattering induced by the high glassy phase content. The thermal conductivities (κ) of the CBS-1, CBS-2, and CBS-3 glass-ceramics were determined to be 2.43, 1.06, and 0.82 W/mK, respectively. Structural analysis using Raman and Fourier transform infrared spectroscopy revealed an absence of nonbridging oxygen in the CBS-1 glass-ceramic, while the high CaO content (>40 mol%) of the CBS-2 and CBS-3 glass-ceramics triggered the formation of nonbridging oxygen in the tetrahedral silicate units. The increase in CaO content of the glass-ceramics increased the number of nonbridging oxygen atoms, thereby resulting in the relaxation of the structure. Consequently, the CBS-2 and CBS-3 glass-ceramics exhibited low thermal conductivity. All the prepared glass-ceramics presented high electrical resistivities of greater than 5 × 1011 Ω cm. The CBS-1 glass-ceramic displayed the highest breakdown strength of 15.20 kV/mm. Overall, the excellent microwave dielectric properties and thermal properties of the CBS glass-ceramics will facilitate the utilization of these materials in millimeter-wave applications.  相似文献   

5.
《Ceramics International》2015,41(6):7645-7650
Nano-sized ZnTiTa2O8 powders with ixiolite structure, with particle sizes ranging from 10 nm to 30 nm, were synthesized by thermal decomposition at 950 °C. The precursors were obtained by aqueous sol–gel and the compacted and sintered ceramics with nearly full density were obtained through subsequent heat treatment. The microstructure and electrical performance were characterized by field emission scanning electron microscopy, x-ray diffraction, and microwave dielectric measurements. All the samples prepared in the range 950–1150 °C exhibit single ixiolite phase and relative density between ~87% and ~94%. The variation of permittivity and Q·ƒ value agreed with that of the relative density. Pure ZnTiTa2O8 ceramic sintered at 1050 °C for 4 h exhibited good microwave dielectric properties with a permittivity of 35.7, Q·ƒ value of 57,550 GHz, and the temperature coefficient of resonant frequency of about −24.7 ppm/°C. The relatively low sintering temperature and excellent dielectric properties in the microwave range would make these ceramics promising for applications in electronics.  相似文献   

6.
《Ceramics International》2022,48(7):9030-9037
In this study, sol–gel derived CaO–B2O3–SiO2 glass-ceramics with a set B2O3 content of 22.2 mol% and CaO/SiO2 ratios ranging between 0.15 and 0.27 were used for low-temperature cofired ceramic applications in the 5G millimeter-wave bands. X-ray diffraction analysis, scanning electron microscopy, Fourier-transform infrared spectroscopy, and Raman spectroscopy data indicated that, unlike the typical CaO–B2O3–SiO2 glass-ceramics prepared via melting resulted in the presence of calcium silicates, the CaO–B2O3–SiO2 glass-ceramics in this study comprised only an amorphous phase containing different amounts of CaB2O4 crystallites depending on the CaO/SiO2 ratio. Among the formulations evaluated, the 14.5CaO?22.2B2O3?63.3SiO2 glass-ceramic sintered at 950 °C exhibited a dielectric constant of 4.33 and a dielectric loss of 0.0012 at 60 GHz, which conferred its low signal propagation delay and low signal attenuation in applications. In addition, the electrical resistivity, breakdown strength, thermal conductivity, and coefficient of thermal expansion of the 14.5CaO?22.2B2O3?63.3SiO2 glass-ceramic were 1.72 × 1012 Ω cm, 15.49 kV/mm, 1.70 W/mK, and 4.1 ppm/°C, respectively. The 14.5CaO?22.2B2O3?63.3SiO2 glass-ceramic exhibited excellent insulating properties, facilitating its use as substrate material; moreover, its thermal properties matched those of Si and GaAs.  相似文献   

7.
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 (× 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.  相似文献   

8.
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 εr ~ 6.36, a quality factor Q × f ~ 29 000 GHz (at 14.5 GHz), and a temperature coefficient of resonance frequency τf ~ ?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 τf value. These results demonstrate potential applications of Li2GeO3 in low‐temperature cofiring ceramics technology.  相似文献   

9.
This paper reports the results of a study focused on the obtainment of glass-ceramic by using rice husk ash (RHA) as silica precursor. RHA is a by-product generated in biomass plants using rice husk as fuel for kilns or in the rice mills to generate steam for the parboiling process. Worldwide, it is annually produced about 132 Mt of rice husk, which gives rise to a production of 33 Mt/year of RHA. Glass-ceramic tiles were produced by a sinter-crystallization process using a glassy frit formulated in the MgO–Al2O3-SiO2 composition system. The realized glass-ceramics were studied according to ISO rules for sintering and technological properties (water absorption, apparent density, bending strength, Young's modulus, deep abrasion, Mohs hardness). To complete the investigation crystalline phase formation and microstructural characterization of the glass-ceramic materials was carried out using X-ray diffraction (XRD) and scanning electron microscopy (SEM). Finally, chemical durability tests on parent glass and derived glass-ceramics were performed. The results obtained showed that it is possible to use RHA to produce glass-ceramic tiles by a sinter-crystallization process, obtaining nepheline (Na2O*Al2O3*SiO2) as main crystalline phase and forsterite (2MgO*SiO2) at 900 °C. Regarding technological features, the sintered materials showed bending strength values and Mohs hardness higher with respect to commercial glass-ceramics like NeopariesR. Other properties as water absorption (0.5%) allowed to classify these materials into the Group BIa characteristic of high sintered ceramic tiles according to European Standard rule.  相似文献   

10.
《Ceramics International》2022,48(16):23104-23110
Herein, Mg–Al–Si–Ba–O-based glass ceramics were studied as potential candidates to protect Mn–Co–Ni–O-based negative temperature coefficient (NTC) thermistors at high temperatures such as 900 °C. The ceramics were prepared in three glass formulations (1#: 15MgO–15Al2O3-44.7SiO2–25BaO, 2#: 17MgO–17Al2O3–41SiO2–25BaO and 3#: 17MgO–17Al2O3–41SiO2–20BaO–5Y2O3 (in mol%)) and their glass-transition temperatures (Tg) were determined using the differential scanning calorimetry (DSC) method. Scanning electronic microscopy (SEM) and X-ray diffraction (XRD) were used to characterize the parent glasses and glass-ceramic coatings. The sealing effects of the glass ceramics were examined by conducting an insulation test. The glass-ceramic sealing structures were subjected to 1000 thermal shock cycles at temperatures varying from room temperature to 900 °C. Notably, the sealing structure of glass-ceramic coating 1# was compact at a Tg of 760.9 °C. The glass-ceramic coatings effectively maintained the NTC properties of the sensitive ceramics in all three formulations. Interestingly, the glass-ceramic coating 3# containing Y2O3 demonstrated an increase in electrical resistance. Both the NTC thermistors coated with 1# and 2# glass formulations successfully passed 1000 thermal shock cycles without visible failures, and their resistance change ratios were well below the requisite 20%.  相似文献   

11.
To decrease the sintering temperature of MgO‐Y2O3 composites to avoid undesired grain coarsening, high reactive MgO‐Y2O3 nanopowders were synthesized via microwave combustion method. The degree of combustion was enhanced effectively by adding an extra oxidant ammonium nitrate. The as‐synthesized MgO‐Y2O3 nanopowders, ~18 nm in size, showed high specific surface area of 64.55 m2/g and low agglomeration. Relative density of 98% was obtained when sintered at a low sintering temperature of 1350°C. The high reactivity can be attributed to the lower activation energy Q (131.13 kJ/mol), compared with samples without extra oxidant (192.97 kJ/mol).  相似文献   

12.
This study focused on the glass forming, crystallization, and physical properties of ZnO doped MgO-Al2O3-SiO2-B2O3 glass-ceramics. The results show that the glass forming ability enhances first with ZnO increasing from 0 to 0.5 mol%, and then weakens with further addition of ZnO which acted as network modifier. No nucleating agent was used and the crystallization of studied glasses is controlled by a surface crystallization mechanism. The predominant phase in glass-ceramics changed from α-cordierite to spinel/gahnite as ZnO gradually replaced MgO. The phase type did not change; however, the crystallinity and grain size in glass-ceramics increased when the glasses were treated from 1030 °C to 1100 °C. The introduction of ZnO can improve the thermal, mechanical, and dielectric properties of the glass-ceramics. The results reveal a rational mechanism of glass formation, crystal precipitation, and evolution between structure and performance in the xZnO-(20-x)MgO-20Al2O3-57SiO2-3B2O3 (0 ≤ x ≤ 20 mol%) system.  相似文献   

13.
Ceramics in the system MgO–SiO2–TiO2 were prepared by standard mixed oxide route. By adding ZnO–B2O3 to the starting mixtures, the firing temperature of the ceramics could be reduced to 1160 °C. Small additions of MnCO3 and CaTiO3 improve microwave dielectric properties leading to an increase in insulation resistance and a decrease in temperature coefficient of capacitance. By adding Co2O3 grain growth can be inhibited and the dielectric Qf value greatly increased. The resultant ceramic material exhibited low dielectric constant and low dielectric loss: relative permittivity (εr): 20±2; temperature coefficient of capacitance (τc): 0±30 ppm/°C; Qf: 100,000 (at 10 GHz); insulation resistance: 1013 Ω cm:  相似文献   

14.
Bioactivity of ferrimagnetic glass-ceramics is useful as thermo seeds for hyperthermia treatment of cancer. Ferrimagnetic glass-ceramics were prepared from the BaFe12O19(BF)–SiO2–CaO–Na2O–P2O5 system using the incorporation method. The mixture was then further sintered at 800 °C to form the glass-ceramic samples. The structure and microstructure of the samples were characterized by X-ray diffraction, energy dispersive X-ray analysis (EDXA) and scanning electron microscopy. Magnetic hysteresis loops of the glass-ceramic samples were obtained with maximum field of 10 kOe, in order to evaluate the potential of these samples for hyperthermia treatment of cancer. In vitro bioactivity was investigated in simulated body fluid (SBF) for 14 days. The results showed that Na2Ca2Si3O9 and BaFe12O19 were the main phases in the glass-ceramic samples. Apatite was formed on the surface layers of the glass-ceramics, confirming their biocompatibility. It was found that the bioactivity increased with an increase in BF contents.  相似文献   

15.
(Zn0.65Mg0.35)TiO3xCaTiO3-based dielectric ceramics sintered at low temperature thanks to ZnO–B2O3 glass phase addition are investigated. The effects of such additions on the dilatometric curves, the microstructure, the phase composition and the dielectric properties have been carefully examined. It is shown that the sintering temperature is significantly lowered to 930 °C by the addition of 2 wt.% of ZnO–B2O3 glass phase. The temperature coefficient of permittivity (τ?) could be controlled by varying the CaTiO3 content and lead to near zero τ? value. As an optimal composition, (Zn0.65Mg0.35)TiO3 + 7%CaTiO3, co-sinterable with silver electrodes at 930 °C, exhibits at 1 MHz, a relative permittivity of ?r = 21, a temperature coefficient of the permittivity τ? of ?4 ppm/°C and low dielectric losses (tan(δ) < 10?3). These interesting properties make this system promising to manufacture Ag-based electrodes multilayer dielectric devices.  相似文献   

16.
The acceptor-doped rutile TiO2 ceramics, x mol% M2O3-(1-x) mol% TiO2 (M = Al3+, Ga3+, and In3+), were prepared by solid state reaction method. The influence of Ar/H2 annealing on the structural and dielectric properties of the ceramics were systematically investigated. Our results reveal that the dielectric properties of the ceramics can be significantly improved by the Ar/H2 annealing. Ga3+ is found to be the most suitable dopant with the best doping level of 5 mol%. Excellent dielectric properties of colossal and flat dielectric permittivity (~1.2 × 105 (@1 kHz and 25 °C), low dielectric loss (~0.1), and good frequency stability were achieved over the temperature range of -70–150 °C in the Ar/H2-annealed 5 mol% Ga2O3-95 mol% TiO2 ceramic. This approach of acceptor-doping and Ar/H2 annealing leads to two thermally activated relaxations in the sample. The low-temperature relaxation is argued to be a Maxwell-Wagner relaxation caused by frozen electrons, while the high-temperature relaxation is a glass-transition-like relaxation associated with the freezing process of the electrons. This work highlights that engineering low-temperature Maxwell-Wagner relaxation paves a new way other than the frequently used acceptor-donor dual doping to design superior dielectric properties in the TiO2 system.  相似文献   

17.
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 × f value of 22 000 GHz, and a τf 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 × f value of 35 830 GHz, and a τf 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 τf 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.  相似文献   

18.
《Ceramics International》2016,42(4):4978-4983
The supercapacitor based piezoelectric material composite (Na,K)NbO3–CaCu3Ti4O12 (NKN–CCTO) is investigated for possible application in piezoelectric devices. (1−x)NKN–xCCTO (0.015≤x≤0.06) with different sintering conditions is researched for supercapacitor based piezoelectric applications. The 0.94NKN–0.06CCTO composite sintered at 975 °C shows the highest dielectric permittivity of 796. Clear SEM images of (1−x)NKN–xCCTO reveal that these compositions have high density well-crystallized structures. The composition and sintering temperature dependence of dielectric permittivities and piezoelectric coefficients, plotted in three dimensions, show that the 0.985NKN–0.015CCTO composite sintered at 1025 °C has a moderate dielectric permittivity of 405 and a piezoelectric constant of 98 pC/N.  相似文献   

19.
《Ceramics International》2023,49(1):216-225
In order to obtain lithium disilicate glass-ceramics for dental restoration with both high strength and high translucency, lithium disilicate glass-ceramics with different MgO contents were prepared by melt-casting and heat treatment method. The effects of MgO content on the crystallization temperature, microstructure and flexural strength of lithium disilicate glass-ceramics were investigated. The results indicate that Mg2+ exists in the form of [MgO4] in the network of lithium disilicate glass-ceramics when the MgO content is 0.56 mol% (M0.56), which is beneficial to increasing the homogeneity and thermal stability of the glass system, and short rod-like lithium disilicate crystals can be formed after heat treatment at 840°C. Thus, the obtained lithium disilicate glass-ceramics exhibit excellent comprehensive performance, with the flexural strength being 312 ± 23 MPa, and the average transmittance of visible light being 37.3% (d = 1.62 mm). Especially, the glass-ceramic sample shows better translucency than the commercially available products. The research results are of great significance for developing high performance lithium disilicate glass ceramics and promoting its broad application in the field of dental restoration.  相似文献   

20.
《Ceramics International》2022,48(16):23119-23126
The high-strength mica-containing glass-ceramics were prepared from granite wastes by bulk crystallization. The influences of SiO2/Al2O3 molar ratio (S/A = 7.72, 9.62, 12.58, 17.82 and 29.67) on the crystallization behavior, microstructure, mechanical properties and machinability of glass-ceramics were investigated. The results demonstrated that the polymerization degree of the glass network decreased with the S/A ratio increasing, which further caused the decrease in glass transition temperature and crystallization temperatures. The increase in the S/A ratio promoted the precipitation of diopside, hectorite, kalsilite and tainiolite in glass-ceramics when the samples were heated at 750 °C, while inhibiting the precipitation of forsterite. For the glass-ceramics crystallized at 800 and 900 °C, the main crystalline phases transformed from diopside, forsterite, and nepheline to diopside, kalsilite, and tainiolite, with the S/A ratio increasing. As the SiO2 gradually replaced Al2O3, the morphology of crystals changed from lamellar to granular, while the mean size of crystals reduced. The Vickers-Hardness values of glass-ceramics crystallized at 800 and 900 °C ascended with S/A ratio rising, and the values were above 6.30 GPa. The bending strength of most glass-ceramics is stable between 90 and 140 MPa, among which the maximum bending strength is 133.28 ± 14.81 MPa. The fracture toughness of the glass-ceramic crystallized at 800 and 900 °C declined, while that at 700 °C increased with a larger S/A ratio. Glass-ceramics after heat-treated at 900 °C with S/A ratio of 9.62 had the largest fracture toughness of 3.28 ± 0.15 MPa m1/2. In preliminary tests of machinability, glass-ceramic after heat-treated at 900 °C with S/A ratio of 9.62 showed better results.  相似文献   

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