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1.
《Ceramics International》2022,48(1):199-204
MgNb2-xVx/2O6-1.25x (0.1≤x≤0.6) ceramics with orthorhombic columbite structures were prepared at low-temperature by a solid-phase process. The phase component, microscopic morphology, low-temperature sintering mechanism and microwave dielectric performance of MgNb2-xVx/2O6-1.25x ceramics were comprehensively investigated. Low-temperature sintering densification of dielectric ceramics was achieved via the nonstoichiometric substitution of vanadium (V) at the Nb-site. In contrast to pure MgNb2O6 ceramics, the sintering temperature of MgNb2-xVx/2O6-1.25x (x = 0.2) ceramics was reduced by nearly 300 °C owing to the liquid-phase assisted sintering mechanism. The liquid phase arises from the autogenous low-melting-point phase. Meanwhile, MgNb2-xVx/2O6-1.25x (x = 0.2) samples with nonstoichiometric substitution could achieve a more than 900% improvement in the Q × f value, compared with stoichiometrically MgNb2-xVxO6 (x = 0.1, 0.2) ceramics. Finally, MgNb2-xVx/2O6-1.25x dielectric ceramics possess outstanding microwave dielectric properties: εr = 20.5, Q × f = 91000, and τf = -65 ppm/°C when sintered at 1030 °C for x = 0.2, which provides an alternative material for LTCC technology and an effective approach for low-temperature sintering of Nb-based microwave dielectric ceramics.  相似文献   

2.
Mg(Ti1-xNbx)O3 (x = 0–0.09) ceramics were prepared by the conventional solid-state reaction method. The phase composition, sintering characteristics, microstructure and dielectric properties of Ti4+ replacement by Nb5+ in the formed solid solution Mg(Ti1-xNbx)O3 (x = 0–0.09) ceramics were systematically studied. The structural variations and influence of Nb5+ doping in Mg(Ti1-xNbx)O3 were also systematically investigated by X-ray diffraction and Raman spectroscopy, respectively. X-ray diffraction and its Rietveld refinement results confirmed that Mg(Ti1-xNbx)O3 (x = 0–0.09) ceramics crystallised into an ilmenite-type with R-3 (148) space group. The replacement of the low valence Ti4+ by the high valence Nb5+ can improve the dielectric properties of Mg(Ti1-xNbx)O3 (x = 0–0.09). This paper also studied the different sintering temperatures for Mg(Ti1-xNbx)O3 (x = 0–0.09) ceramics. The obtained results proved that 1350 °C is the best sintering temperature. The permittivity and Q × f initially increased and then decreased mainly due to the effects of porosity caused by the sintering temperature and the doping amount of Nb2O5, respectively. Furthermore, the increased Q × f is correlated to the increase in Ti–O bond strength as confirmed by Raman spectroscopy, and the electrons generated by the oxygen vacancies will be compensated by Nb5+ to a certain extent to suppress Ti4+ to Ti3+, which was confirmed by XPS. The increase in τf from ?47 ppm/°C to ?40.1 ppm/°C is due to the increment in cell polarisability. Another reason for the increased τf is the reduction in the distortion degree of the [TiO6] octahedral, which was also confirmed by Raman spectroscopy. Mg(Ti0.95Nb0.05)O3 ceramics sintered at 1350 °C for 2 h possessed excellent microwave dielectric properties of εr = 18.12, Q × f = 163618 GHz and τf = ?40.1 ppm/°C.  相似文献   

3.
《Ceramics International》2023,49(3):4290-4297
Li(Al1-xLix)SiO4-x (x = 0.005, 0.01, 0.015, and 0.02) ceramics were synthesized via a traditional solid phase reaction method with different sintering temperatures. To determine the positions occupied by Li+ in the lattice, the defect formation energies and total energies of various sites of LiAlSiO4 (LAS) occupied by Li+ were examined, and the energy of LAS systems were calculated using density functional theory of first-principle with the CASTEP module. The results demonstrated that the Al-sites occupied by Li+ had the lowest formation energies and total energy, so Li + should substitute Al3+. The impacts of replacing Al3+ with Li+ on the bulk density, sintering properties, phase composition, microstructure, and microwave dielectric properties of Li(Al1-xLix)SiO4-x (0 = x ≤ 0.02) ceramics were thoroughly studied. With Li+-doping, the sintering temperature decreased from 1300 °C (x = 0) to 1175 °C (x = 0.02), while the Q × f and τf values of LAS ceramics significantly increased. The Li(Al0.99Li0.01)SiO3.99 ceramic was fully sintered at 1250 °C for 10 h to obtain excellent microwave dielectric properties: εr = 3.49, Q × f = 51,358 GHz, and τf = ?51.48 × 10?6 °C?1.  相似文献   

4.
Herein, the influence of Mo6+ substitution on the crystal structure, microstructures, chemical bond characteristics, vibration characteristics and microwave dielectric properties of ZnMoxW1-xO4(x = 0−0.12) ceramics prepared by a solid-state reaction were investigated. The results show that Mo6+ substitution does not produce secondary phase, the densification temperature decreases from 1100 to 925 ℃, and Q × f values increased from 19605 GHz (x = 0) to 61640 GHz (x = 0.06) at 925 ℃, which resulted from the packing fraction, UtW-O and microstructures. Also, the τf values were optimized to −34 ppm/°C due to changes in the degree of structural order and stability of chemical bonds.AfiW-O, molecular polarizability and porosity first led to an increase in permittivity and decrease thereafter. The ZnMo0.06W0.94O4 ceramics sintered at 925℃ exhibited satisfactory properties (εr = 15.10, Q × f = 61,640 GHz, and τf = -34 ppm/°C), providing a potential candidate for microwave devices.  相似文献   

5.
《Ceramics International》2022,48(12):16554-16561
Herein, we report the solid-state synthesis of (KMg)xFe2-xMo3O12 (0 = x ≤ 1.5) ceramics. Phase composition, crystal structure, morphology, phase transition and thermal expansion behavior of the (KMg)xFe2-xMo3O12 ceramics were investigated by XRD, Raman, XPS, HRTEM, EDX, SEM, TMA and high-temperature XRD. Results indicate that (KMg)3+ dual-cations have successfully replaced Fe3+ in Fe2Mo3O12 ceramics and single-phase monoclinic (KMg)xFe2-xMo3O12 ceramics were prepared for 0.25 = x ≤ 1. (KMg)3+ introduction can increase the density of (KMg)xFe2-xMo3O12 ceramics and effectively improve their negative thermal expansion (NTE) performance. In addition, the phase transition temperature (Tc) of Fe2Mo3O12 was reduced from 508.1 °C to room temperature with the increase of (KMg)3+-substitution. Monoclinic KMgFeMo3O12 ceramics was observed to show stronger NTE in a wider temperature range of 30–700 °C for the first time. Its corresponding coefficient of thermal expansion (CTE) is as high as ?17.21 × 10?6 °C?1. The distortion of [FeO6/MgO6] polyhedra in (KMg)xFe2-xMo3O12 caused by (KMg)3+-substitution contributed to the stronger NTE.  相似文献   

6.
《Ceramics International》2020,46(13):21336-21342
Li3Mg2(Nb1-xWx)O6+x/2 (0 ≤ x ≤ 0.08) ceramics were synthesized by the solid-state reaction route. The effects of W6+ substitution on the phase composition, microstructure and microwave dielectric properties of Li3Mg2NbO6 ceramics were investigated systematically. The XRD results showed that all the samples formed a pure solid solution in the whole doping range. The SEM iamges and relative density revealed the dense structure of Li3Mg2(Nb1-xWx)O6+x/2 ceramics. The relationship between the crystal structure and dielectric properties of Li3Mg2(Nb1-xWx)O6+x/2 ceramics was researched through polarizability, average bond valence, and bond energy. The substitution of W6+ for Nb5+ in Li3Mg2(Nb1-xWx)O6+x/2 ceramics significantly promoted the Q × f values. In addition, the increase of W6+ content improved the thermal stability of the Li3Mg2(Nb1-xWx)O6+x/2 ceramics. The Li3Mg2(Nb0.94W0.06)O6.03 ceramics sintered at 1175 °C for 6h possessed excellent properties: εr ~ 15.82, Q × f ~ 124,187 GHz, τf ~ −18.28 ppm/°C.  相似文献   

7.
In this study, Zn2+-substituted Li2MgSiO4 ceramics (Li2(Mg1-xZnx)SiO4, x = 0.00, 0.05, 0.10, 0.15, and 0.20) were synthesized using a traditional solid-state method. A fixed amount of LiF sintering aid (1.5 wt%) was added to the ceramics for decreasing the sintering temperature and adjusting their microwave dielectric properties. X-ray diffraction (XRD) results revealed no secondary phases, and scanning electron microscopy (SEM) data suggest that the Zn2+ ion substitution increased the size and uniformity of the grains, thereby affecting the densification of the prepared ceramics. The maximum bulk density (2.94 g/cm3) was found in a Zn2+ ion-substituted ceramic with x = 0.10 at a relative density of 94.2% (compared with the XRD theoretical density). Excellent microwave dielectric properties (εr = 6.28, Q × f = 50400 GHz, and τf = ?145 ppm/°C) can also be obtained at this zirconium content. We believe that the developed ceramics are promising for use as antenna substrates or transmit/receive modules in low-temperature co-firing ceramic applications.  相似文献   

8.
《Ceramics International》2022,48(12):16677-16684
Calcium bismuth niobate (CaBi2Nb2O9) is a typical bismuth-layer structured piezoelectrics (BLSPs) with a high Curie temperature (TC) of ~943 °C, but it has low piezoelectric coefficient and high-temperature resistivity which severely limits signal acquisition in the high-temperature piezoelectric vibration sensors. Ion-doping modification is regarded as an effective way to enhance electrical properties. In this work, W6+ donor-doping at Nb5+ site in the CaBi2Nb2-xWxO9 (x = 0, 0.020, 0.025, 0.030, 0.035 and 0.040) piezoelectric ceramics with TC of 931 ± 2 °C were fabricated by the conventional solid-state reaction method. The effects of W6+-doping on crystal structure of CaBi2Nb2-xWxO9 as well as microscopic morphology and electrical properties of ceramics were investigated systematically. The tetragonality, isotropy and electrical properties of the ceramics were enhanced with the introduction of W6+ dopant. It was found that x = 0.025 was the optimal W6+-doping ratio that yielded remnant polarization of 8.0 μC/cm2, electrical resistivity of 3.0 × 106 Ω cm at 600 °C, piezoelectric coefficient (d33) of 14.4 pC/N, and good thermal depoling property. Our work has established a feasible approach to tune the structure of CaBi2Nb2O9 to improve piezoelectric properties for potential applications in high-temperature piezoelectric vibration sensors.  相似文献   

9.
The crystal structure, microstructure, and microwave dielectric properties of forsterite‐based (Mg1–xNix)2SiO4 (= 0.02–0.20) ceramics were systematically investigated. All samples present a single forsterite phase of an orthorhombic structure with a space group Pbnm except for a little MgSiO3 secondary phase as x > 0.08. Lattice parameters in all axes decrease linearly with increasing Ni content due to the smaller ionic radius of Ni2+ compared to Mg2+. The substitution of an appropriate amount of Ni2+ could greatly improve the sintering behavior and produce a uniform and closely packed microstructure of the Mg2SiO4 ceramics such that a superior × f value (152 300 GHz) can be achieved as = 0.05. The τf value was found to increase with increasing A‐site ionic bond valences. In addition, various additives were used as sintering aids to lower the sintering temperature from 1500°C to the middle sintering temperature range. Excellent microwave dielectric properties of εr~6.9, × f~99800 GHz and τf~?50 ppm/°C can be obtained for 12 wt% Li2CO3‐V2O5‐doped (Mg0.95Ni0.05)2SiO4 ceramics sintered at 1150°C for 4 h.  相似文献   

10.
《Ceramics International》2020,46(11):19046-19051
In the present work, MgAl2-x(Mg0·5Ti0.5)xO4 (x = 0.02, 0.04, 0.06, 0.08, 0.10) solid solutions were synthesized via the traditional solid-state reaction route. The valence state of Ti ions, crystal structural characteristics, and microwave dielectric properties were discussed. A solid solution with spinel structure was revealed by the Rietveld refinement results. The partial substitution of (Mg0·5Ti0.5)3+ for Al3+ lowered the sintering temperature and improved the Q × f value of MgAl2O4 ceramic. The MgAl2-x(Mg0·5Ti0.5)xO4 solid solutions with x = 0.06 can be well sintered at 1425 °C in an oxygen atmosphere for 8 h and exhibits excellent microwave dielectric properties with εr = 9.1, Q × f = 98,000 GHz, τf = −61.36 ppm/°C. The sintering temperature of MgAl1·94(Mg0·5Ti0.5)0.06O4 microwave dielectric ceramics was approximately 200 °C lower than that of conventional MgAl2O4 ceramics.  相似文献   

11.
《Ceramics International》2021,47(23):33064-33069
In this paper, Mg2Ti1-xAl4/3xO4 ceramics (0.01 ≤ x ≤ 0.09) were synthesized through conventional solid-state ceramic route. The cubic spinel structure, microstructure and microwave properties of Mg2Ti1-xAl4/3xO4 (x = 0.01, 0.03, 0.05, 0.07, 0.09) ceramics were investigated by X-ray diffraction, Raman spectra, infrared spectra. Rietveld refinements confirm that a spinel structure phase with space group Fd-3m is formed. The variation of the permittivity was concerned with the ionic polarizability, and the value of τf was influenced by the bond valence. Both Q × f values and relative density showed an identical trend. Intrinsic properties of Mg2Ti1-xAl4/3xO4 ceramics were analyzed by infrared spectra and Raman spectra. In addition, the Mg2Ti1-xAl4/3xO4 ceramic sintered at 1420 °C for 4 h possessed optimal dielectric properties (εr = 14.65, Q × f = 182347 GHz, τf = −57.7 ppm/°C) when x = 0.09.  相似文献   

12.
《Ceramics International》2022,48(1):837-846
Hierarchical structure Bi2MoxW1-xO6 (x = 0, 0.1, 0.2, 0.3, 0.4 and 0.5) solid solutions with high surface area are prepared by hydrothermal method without employing any surfactant. All the as-prepared products are hierarchical microspheres self-assembled by nanosheets. The piezocatalytic performance of Bi2MoxW1-xO6 solid solutions are investigated by the degradation of RhB under ultrasonic vibration. The experimental results show that the x value of Bi2MoxW1-xO6 has great influence on the piezocatalytic efficiency. Among which, the Bi2Mo0.4W0.6O6 presents a high value of the rate constant k of 0.119 min-1 by degrading 97.5% of RhB dye solution in 30 min. It is about 43.4% higher than that of pure Bi2WO6 sample, for which k is 0.083 min-1. Radical trapping test indicates that holes (h+) are the dominating active species in the degradation process. The improved piezocatalytic performance for Bi2Mo0.4W0.6O6 sample ascribes to the larger piezoelectric potential generated under a strained state, which facilitates the transfer of charge carriers and accelerate the piezocatalytic process. Our work presents a new design strategy of piezocatalysts for remediation of water pollution.  相似文献   

13.
《Ceramics International》2021,47(24):34687-34694
To improve the negative thermal expansion (NTE) performance of ln2W3O12, a novel series of NTE (KMg)xln2-xW3O12 ceramics were fabricated via the solid-state method. The effects of (KMg)3+ substitution on the phase composition, microstructure and thermal expansion property of the ln2W3O12 ceramics were characterized using X-ray diffraction (XRD), Raman spectrometer (Raman), X-ray photoelectron spectrometer (XPS), scanning electron microscopy (SEM), transmission electron microscope (TEM) and thermal mechanical analyzer (TMA). Results indicate that (KMg)3+ can partially replace In3+ in In2W3O12 and form a new phase KxMgxln2-xW3O12 with monoclinic symmetry. For x = 0.5, pure monoclinic (KMg)0.5ln1.5W3O12 ceramics is prepared and shows strong NTE. Its coefficient of thermal expansion is −7.89 × 10−6 °C−1 in 30–700 °C, in addition, no phase transition was observed over the entire testing temperature range. These research results indicate that double cations co-substitution is an effective strategy to improve the NTE property of ln2W3O12 through crystal structure modulation. This strategy could be extended to the performance modulation of other NTE materials.  相似文献   

14.
Al2Mo3O12 is a typical negative thermal expansion (NTE) material, whose thermal expansion behavior depends on its crystal phase. The thermal shock caused by temperature-induced phase transition limits its wide application. The two series of Al2. xScxMo3O12 (0 ≤ x ≤ 1) and Al2Mo3-xWxO12 (0 ≤ x ≤ 2.5) solid solutions with controllable phase transition temperature were synthesized via single cation substitution at the A or B position. The problem of thermal shock caused by the change of temperature is effectively solved in the synthesized Al1.6Sc0.4Mo3O12 and Al2Mo0.5W2.5O12, showing stable NTE performance above room temperature, and the coefficients of thermal expansion of which are ?2.19 × 10?6 °C?1 in 100–550 °C and ?4.25 × 10?6 °C?1 in 85–500 °C, respectively. A-site cation substitution is a more effective way to tune the thermal expansion properties of Al2Mo3O12, which is attributed to the fact that the bond strength of A-O is weaker than that of B–O in the compound.  相似文献   

15.
CaTi1-x (Mg1/2W1/2)xO3 (x = 0, 0.02, 0.04, 0.06, 0.08) dielectric ceramics were synthesized via the traditional solid-state reaction method. Crystal structure and microwave dielectric properties of CaTi1-x (Mg1/2W1/2)xO3 system were systematically investigated based on chemistry bond theory (P–V-L theory) for the first time. The pure perovskite phase was obtained for all doped samples, as confirmed through the XRD and Rietveld refinement results. The lattice characteristics were closely related to the microwave dielectric properties. The bond ionicity, lattice energy, and bond energy affected the dielectric constant, quality factor, and temperature stability of the ceramic material. Through the use of (Mg1/2W1/2)4+ doped on B-site, the CaTi1-x (Mg1/2W1/2)xO3 system can maintain a high dielectric constant (εr > 100) while effectively reducing the τf value from 800 ppm/°C to less than 300 ppm/°C and improving the Q × f value to 9650 GHz (at 3.76 GHz).  相似文献   

16.
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 εr = 9.6, Q × f = 56 100 GHz, and τf = ?42 ppm/°C. The ceramics under study show good chemical compatibility with aluminum during cofiring.  相似文献   

17.
To suppress the impurity phases and porous microstructure caused by lithium volatilization, the Li2Mg3ZrO6 and Zr-deficiency Li2Mg3Zr1-xO6 (x = 0.02, 0.04, 0.06, 0.08, 0.10) ceramics were successfully synthesized via the solid-state method assisted with atmosphere-controlled sintering. The influences of non-stoichiometric on structure characteristics, morphology and microwave dielectric properties of Li2Mg3Zr1-xO6 ceramics were investigated. The XRD and SEM results proved that the Zr-deficiency restrained the formation of impurity phases and remarkably improved the densification of Li2Mg3Zr1-xO6 samples. The variation trend of dielectric constant (εr) was explained by the relative density and theoretical dielectric polarizability. The quality factor (Q × f) was strongly associated with the impurity phases and relative density. Additionally, the temperature coefficient of resonant frequency (τf) showed the same trend as the total bond energy Etotal, indicating the bond energy might play vital roles in thermal stability of Li2Mg3Zr1-xO6 samples. Typically, the Li2Mg3Zr1-xO6 sample obtained at x = 0.06 possessed remarkable dielectric performances: εr = 13.13, Q × f = 116,400 GHz (10.14 GHz) and τf = ?26.30 ppm/°C.  相似文献   

18.
The crystal structure and microwave dielectric properties of Zn3-xCux(BO3)2 (x = 0–0.12) ceramics prepared via a traditional solid-state reaction method were investigated by means of X-ray diffraction (XRD) utilizing the Rietveld refinement, complex chemical bond theory, and Raman spectroscopy. XRD showed that all samples were single phase. The samples maintained a low permittivity, even at higher Cu2+ contents, which is conducive to the shortening of signal delay time, and intimately related to the average bond ionicity and Raman shift. Moreover, proper Cu2+ substitution greatly reduced the dielectric loss associated with the lattice energy. Cu2+ entering the lattice optimized the temperature coefficient of resonance frequency (τf) values and improved the temperature stability of samples by affecting the bond energy. Optimal microwave dielectric properties were: εr = 6.64, Q × f = 160,887 GHz, τf = ?42.76 ppm/°C for Zn2.96Cu0.04(BO3)2 ceramics sintered at 850 °C for 3 h, which exhibited good chemical compatibility with silver and are therefore good candidate materials for Low temperature co-fired ceramic applications.  相似文献   

19.
《Ceramics International》2020,46(6):7259-7267
Co-precipitation was successfully applied to synthesize the Sc3+ doped In2-xScx (WO4)3 (x = 0, 0.3, 0.6, 0.9 and 1.2) compounds. The composition- and temperature-induced structural phase transition and thermal expansion behaviors of Sc3+ doped In2(WO4)3 were investigated. Results indicate that In2-xScx (WO4)3 crystalizes in a monoclinic structure at 300 °C for x ≤ 0.3 and changes into hexagonal structure for x ≥ 0.6. Hexagonal In1.1Sc0.9(WO4)3 displays negative thermal expansion (NTE) with an average linear coefficient of thermal expansion (CTE) of −1.85 × 10−6 °C −1. After sintering at 700 °C and above, a phase transition from hexagonal to orthorhombic phase was observed in In2-xScx (WO4)3 (x ≥ 0.6). Sc3+ doping successfully reduce the temperature-induced phase transition temperature of In2-xScx (WO4)3 ceramics from 250 °C (x = 0) to room temperature (x = 0.9). When x = 0.9 and 1.2, the average linear CTEs of In2-xScx (WO4)3 ceramics are −5.45 × 10−6 °C−1 and -4.43 × 10−6 °C−1 in a wider temperature range of 25–700 °C, respectively.  相似文献   

20.
Spinel Mg(Al1?xGax)2O4 (= 0–1) solid solutions were synthesized via solid‐state method. Replacement of Al3+ by Ga3+ in MgAl2O4 gave rise to the expansion of the lattice, as well as blueshifts of FT‐IR and Raman peaks. The homogeneous solid solutions, high relative densities, large grain sizes, and compact microstructures resulted in excellent microwave dielectric properties for spinel Mg(Al1?xGax)2O4 (= 0.6) ceramics sintered at 1485°C: that is, εr = 8.87, Q × f = 107 000 GHz (at 14.8 GHz), and τf = ?16 ppm/°C. Spinel‐structured Mg(Al1?xGax)2O4 (= 0–1) solid solutions possessed low sintering temperatures, wide temperature regions (~100°C), and small negative τf values. These outstanding performance make Mg(Al, Ga)2O4 a promising candidate material for millimeter‐wave devices.  相似文献   

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