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1.
《Ceramics International》2020,46(8):11474-11483
High permittivity Ba4(Pr1-xSmx)28/3Ti18-yAl4y/3O54(0.4≤x ≤ 0.7, 0≤y ≤ 1.5) ceramics were synthesized using a standard solid-state method. The effects of Sm3+ substitution into the A-site and Sm3+/Al3+ cosubstitution into the A/B-sites on the microstructure, crystal structure, Raman spectra, infrared reflectivity (IR) spectra and dielectric characteristics were investigated in a Ba4Pr28/3Ti18O54 solid solution. In the ceramic samples of Ba4(Pr1-xSmx)28/3Ti18O54(0.4≤x ≤ 0.7), Sm3+ partial substitution for Pr3+ could improve the quality factor (Qf) value and reduce the TCF value. Nevertheless, the quality factor (Qf~10,000GHz) needed further improvement and the TCF values (+12.3~+35.4 ppm/°C) were still too large. Therefore, Al3+ was introduced for further optimization of the TCF values and Qf values of the Ba4(Pr1-xSmx)28/3Ti18O54 ceramics. Sm/Al cosubstitution led to a good combination of high εr (εr ≥ 70), high Qf (Qf ≥ 12,000 GHz), and near-zero TCF (−10 < TCF < +10 ppm/°C) in a wide range (0.4≤x ≤ 0.7). Infrared reflectivity (IR) spectra indicated that A-TiO6 vibration modes gave the primary contribution rather than Ti–O bending and stretching modes. The decrease in the degree of B-site cations order could be confirmed by Raman spectra. XPS results demonstrated that the improvement of quality factor (Qf) value was strongly related to the suppression of Ti3+. Excellent dielectric properties were achieved in Ba4(Pr1-xSmx)28/3Ti18-yAl4y/3O54 microwave ceramics with x = 0.5 and y = 1.25: εr = 72.5, Qf = 13,900GHz, TCF = +1.3 ppm/°C.  相似文献   

2.
High dielectric constant Ba4M28/3Ti18O54 (M = La, Pr, Nd, and Sm) ceramics were synthesized via standard solid-state reaction route. All the samples possessed single-phase orthorhombic tungsten-bronze structure, and the unit cell volumes decreased monotonously when rare-earth ion changed from La to Sm. With the decreasing radius of rare-earth ions, the dielectric constant (εr) gradually decreased, which was correlated with the decrease of total ionic polarizability and blue shift of Raman vibration modes. The increase of the quality factor (Q × f) was associated with the increase of packing fraction and the decrease of FWHM of Raman vibration modes (Ag and B1g). The temperature coefficient of resonant frequency (TCF) shifted in the negative direction, which was highly related to the decrease of the TiO6 octahedral tilt angle. Infrared reflection (IR) spectroscopy analysis indicated that the infrared vibration modes between TiO6 octahedron and A-site cation (M3+ and Ba2+) at low frequency dominated microwave dielectric polarization in the Ba4M28/3Ti18O54 ceramics.  相似文献   

3.
《Ceramics International》2021,47(20):28487-28492
In this work, the microwave dielectric properties of Ba4(Nd1-yBiy)28/3Ti18-x(Al1/2Ta1/2)xO54(0≤x≤2, 0.05≤y≤0.2) ceramics co-substituted by A/B-site were studied. Firstly, (Al1/2Ta1/2)4+ was used for substitution at B-site. At 0≤x≤1.5, the above mentioned ceramic was found to exist in single-phase tungsten bronze structure, but at x = 2.0, the secondary phase appeared. Although the dielectric constant decreased by doping the (Al1/2Ta1/2)4+, but the quality factor was observed to improve by 40% and the temperature coefficient of resonant frequency decreased by 75%. Based on the above results, Bi3+ was introduced to Ba4Nd28/3Ti17(Al1/2Ta1/2)O54. The introduction of Bi3+ reduced the sintering temperature, greatly improved the dielectric constant, and ultimately decreased the temperature coefficient of resonant frequency, but it led to deterioration of quality factor. At last, with appropriate site-substitution content control (x = 1.0,y = 0.15), excellent comprehensive properties (εr = 89.0, Q × f = 5844 GHz @ 5.89 GHz,TCF = +8.7 ppm/°C) were obtained for the samples sintered at 1325 °C for 4 h.  相似文献   

4.
Ba4(Sm0.15Nd0.85)9.33Ti18-zAl3z/4O54 (BSNT-zAl, 0.0 ≤ z ≤ 2.5) ceramics were prepared via a solid-state reaction, and the effects of Al doping on the microwave dielectric properties and defect behavior of the title compound were studied. X-ray diffraction (XRD) analysis and scanning electron microscopy (SEM) photographs suggested that Al ions successfully entered the lattice to form tungsten-bronze-like solid solutions. With a small amount of Al substitution, the relative dielectric constant (εr), and the temperature coefficient of resonant frequency (τf) values decreased, whereas the quality factor (Q × f) substantially increased by approximately 50%. The defect-related extrinsic dielectric loss was clarified via the thermally stimulated depolarization current (TSDC) technique. With Al doping, the TSDC relaxation of across-grain-boundary oxygen vacancies () vanished, whereas that of defect dipoles () appeared at relatively low temperatures. Therefore, in the BSNT-zAl ceramics, oxygen vacancies were more inclined to interconnect with to form defect dipoles. This could reduce the activity of and account for the notable improvement in the Q × f values. In particular, the excellent characteristics of εr = 67.33, Q × f = 16 530 GHz, and τf = +0.87 ppm/°C were achieved in the specimens with z = 1.5 sintered at 1350°C for 4 hours.  相似文献   

5.
主要研究了不同Sm掺杂浓度对Ba4La19.33Ti18O54陶瓷的微波介电性能和微观结构的影响。首先利用常规固相反应技术制备了Sm含量y分别为0.0,0.1,0.3,0.5和0.7的五种Ba4(La1-ySmy)9.33Ti18O54陶瓷样品;室温下在0.3~3.0GHz频率范围内,利用网格分析仪测量了这些样品的介电常数和介电损耗因子;结果表明随着Sm掺杂含量的增大,样品介电损耗明显减小,而介电常数只有微小减少。当Sm掺杂含量y=0.5时,样品的介电性能最好。此外,还利用X射线衍射仪和扫描电子显微镜研究了样品的微观结构及随微波介电性能的变化。  相似文献   

6.
Microwave and terahertz communications are increasingly significant, however, the lack of material information in terahertz band limits their development. Moreover, few lightweight materials with a high relative dielectric constant () are found suited for satellite communication and wearable devices. In this study, we developed lightweight porous Ba4[(Sm0.1Nd0.9)0.9Bi0.1]28/3Ti18O54 (BSNBT) ceramics exhibiting a total porosity ranging from 6.3% to 26.5% (bulk density ranging from 5.47 to 4.29 g/cm3) and relatively high ranging from 85.6 to 56.8, which were obtained by sacrificial template method using polymethyl methacrylate spheres (PMMAs) of varying average particle sizes, from 9 to 34 μm, as sacrificial materials. A high refractive index ranging between 7.5 and 8.9 and a low absorption coefficient of approximately 17 cm−1 at 0.3 THz were obtained for the porous ceramics with different total porosities derived from PMMAs with average particle sizes of 9 and 19 μm. Furthermore, effective medium and Mie scattering theories were applied to understand the effects of porous structure on the dielectric properties in microwave and terahertz frequency ranges, respectively, owing to the different wavelengths in the BSNBT matrix. The results of this study suggest that introducing a porous structure can effectively exploit lightweight microwave dielectric ceramic materials and provide valuable information on their terahertz response mechanism.  相似文献   

7.
《Ceramics International》2020,46(5):6079-6084
A novel low-loss and temperature stable NiSnTa2O8 ceramic with trirutile structure was prepared using traditional solid-state method. The structure-performance relationships were investigated by Rietveld refinement, chemical bond theory and far-infrared spectrum. The results show that the relative densities play a dominant role in the change of dielectric constant. Theoretical dielectric constant calculated via bond theory, Clausius-Mossotti equation and fitted result of far-infrared spectrum are close to experimental value. Ta–O bonds with greatest bond ionicity and bond energy have the primary contributions to dielectric polarizabilities and dielectric loss. The optimal microwave dielectric performances of NiSnTa2O8 ceramics were obtained: εr ∼21.04, Q×f ∼31328 GHz and τf = −2.63 ppm/°C at 1425 °C.  相似文献   

8.
Ba2MGa11O20 (M = Bi, La; called BBG and BLG, respectively) ceramics with monoclinic space group I2/m were prepared through a solid-state reaction method. BBG ceramic sintered at 1150 °C for 6 h has the best microwave dielectric properties with low εr = 10.68, Q × f = 41,756 GHz, and negative τf = ?61.3 ppm/°C. BLG ceramic sintered at 1440 °C for 6 h exhibits εr = 13.94, Q × f = 45,592 GHz, and near-zero τf = ?16.3 ppm/°C. The large deviation between εr and εth was ascribed to the “rattling” effect of the cations and the existence of lone pair ions of Bi3+. The difference in Q × f of the two ceramics was discussed in terms of packing fraction, and the τf of BLG was closer to zero than that of BBG due to the smaller τε value. Their intrinsic dielectric properties were analyzed through far-infrared reflectivity spectroscopy.  相似文献   

9.
《Ceramics International》2022,48(16):23044-23050
Nd[(Mg1-xZnx)1/2Ti1/2]O3 perovskite ceramics (x = 0, 0.2, 0.4, 0.6, 0.8) are prepared by the solid-state reaction method. The effects of Zn2+ substitution on the structure, microstructure, especially the B-site 1:1 cation ordering and microwave dielectric properties have been investigated. Sintered Nd[(Mg1-xZnx)1/2Ti1/2]O3 ceramics all adopt dense microstructure, along with increased dimensional uniformity as Zn2+ substitution. All the ceramics are confirmed to have B-site 1:1 ordered monoclinic perovskite structure with P21/n space group. Atomic mass difference of B-site elements might be an important factor affecting the B-site 1:1 cation ordering. HRSTEM observation suggest that the doped Zn2+ cations have roughly entered the Mg2+ sites to promote 1:1 cation ordering. The degree of the 1:1 cation ordering can be negatively reflected by the full width at half maximum (FWHM) of F2g(B) mode at 372 cm?1 in Raman spectra. With Zn2+ doping, the degree of the 1:1 cation ordering first increases then decreases, and reaches its maximum at x = 0.6. Meanwhile the best combination of microwave dielectric properties is obtained, as εr = 31.4, Q × f = 74,000 GHz, τf = ?44 ppm/°C. It is found that the long-range ordering not only decreases the dielectric loss but also affects the dielectric constant, providing a theoretical foundation to understand further the correlation between ionic configuration and microwave dielectric properties.  相似文献   

10.
《Ceramics International》2022,48(9):12118-12125
In this study, (Cu1/3Nb2/3)4+ complex cation and BaO–ZnO–B2O3 glass frit were adopted to solve the high sintering temperature and poor temperature stability of Ba3Nb4Ti4O21 ceramics. It is shown that pure Ba3Nb4Ti4O21 phase was formed when Ti site was partially replaced by (Cu1/3Nb2/3)4+ cation. The increasing number of dopants decreases the dielectric polarizability, correspondingly, the dielectric constant and temperature coefficient of the resonance frequency values are reduced consistently. The variation of the Q × f value is determined by internal ionic packing fraction and external sintering densification. The (Cu1/3Nb2/3)4+ cation effectively decreases the suitable sintering temperature from 1200 to 1050 °C while greatly improving the temperature stability. BaO–ZnO–B2O3 glass was used to further improve the low-temperature sintering characteristics of Ba3Nb4Ti4O21 ceramics. It is proven that the addition of glass frits effectively decreases the temperature to 925 °C with combinational excellent microwave dielectric properties: εr ~55.6, Q × f ~5700 GHz, τf ~3 ppm/°C, making the Ba3Nb4Ti4O21 ceramics promising in the applications of low-temperature cofired ceramic technology.  相似文献   

11.
《Ceramics International》2022,48(14):20446-20455
Ba4(Nd1-xSmx)28/3(Ti0,95Zr0,05)18O54 ceramics with (x = 0; 0.2; 0.4; 0.8 and 1) were synthesized by solid method at 1250 °C for 10 h. The effects of Nd/Sm ratio on the structure and dielectric behavior were studied by changing the value of x. The study of Ba/RE order with (RE = Nd and Sm) in the solid solution Ba4(Nd1-xSmx)28/3(Ti0,95Zr0,05)18O54 was realized by X-ray diffraction. The crystal structure of these phases belongs to the tungsten bronze type, which is constructed on the basis of the (3x3) Ti/ZrO6 octahedron more than (2x2) (orthorhombic symmetry, space group Pnma, a ≈22.3 Å, b ≈ 7.67 Å, c ≈ 12.1 Å). A structural model has been established, corresponding to an order within the structure. The model of formula [Ba4]A2[Ba2-a(Nd1-xSmx)1.33+bc]A1'[(Nd1-xSmx)8-dd]A1(Ti0.95Zr0.05)18O54, corresponds to a model associated to infinite perovskite rows parallels to the Oy axis, constructed on the basis of the octahedron (3x3) Ti/ZrO6. Scanning electron microscopy (SEM) has showed that Ba4(Nd1-xSmx)28/3(Ti0,95Zr0,05)18O54 ceramics have a typical columnar grain, which indicates that the phase structure of tungsten bronze exists in the x range and all samples show a dense microstructure. The average grain size ranges from 1.179 to 0.912 μm. The dielectric properties were studied by complex impedance spectroscopy in the temperature range from 30 °C to 800 °C where an anomaly was observed in a few compositions characterized by a maximum of the dielectric permittivity that shifts with increasing frequency at higher temperatures. The presence of a strong dispersion over a wide range of temperatures, is probably related to cationic disorder within the Ba4(Nd1-xSmx)28/3(Ti0,95Zr0,05)18O54 structure.  相似文献   

12.
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   

13.
The Li2MgTi1-x(Mg1/3Nb2/3)xO4 (0?≤x?≤?0.5) ceramics were prepared by the conventional solid-state method. The relationship among phase composition, substitution amount and microwave dielectric properties of the ceramics was symmetrically investigated. All the samples possess the rock salt structure with the space group of Fm-3m. As the x value increases from 0 to 0.5, the dielectric constant linearly decreases from 16.75 to 15.56, which can be explained by the variation of Raman spectra and infrared spectra. The Q·f value shows an upward tendency in the range of 0?≤x?≤?0.3, but it then decreases when x?>?0.3. In addition, the temperature coefficient of resonant frequency (τf) is shifted toward zero with the increasing (Mg1/3Nb2/3)4+ addition. By comparison, the Li2MgTi0.7(Mg1/3Nb2/3)0.3O4 ceramics sintered at 1400?°C can achieve an excellent combination of microwave dielectric properties: εr=?16.19, Q·f =?160,000?GHz and τf =??3.14?ppm/°C.  相似文献   

14.
In the present work, a high quality (Q) Ca1.15Sm0.85Al0.85Ti0.15O4 (CSAT) ceramic was prepared via reaction sintering (RS) method. The phase structure, surface morphology, packing fraction (PF), and valence bond of the ceramic were systematically investigated. By studying the X-ray diffraction (XRD) pattern of the ceramic, it was determined to exhibit a single-phase tetragonal structure with the dimensions of a = b = 3.6943(13)Å and c = 12.0320(23)Å and volume of V = 164.22(10) Å3. The influence of the intrinsic quality loss factor on the Q × f value was investigated by calculating the PF. Simultaneously, the bond valence of the samarium (Sm) sites was evaluated to elucidate the relationship with the temperature coefficient of resonant frequency (τf). The CSAT ceramic was sintered at 1550 °C for 6 h and exhibited exceptional characteristics in terms of the relative dielectric constant (εr) = 17.5, quality factor (Q × f) = 66700 GHz, and τf = ?6.93 ppm/°C. These results highlighted the excellent suitability of the RS method for preparing CSAT ceramics with outstanding microwave dielectric properties.  相似文献   

15.
《Ceramics International》2023,49(4):6077-6085
Solid-phase method was used to synthesize MgMo1-xWxO4 (x = 0–0.15) ceramics. The influences of substitution Mo6+ with W6+ on crystal structure, vibration characteristics and microwave dielectric properties of MgMo1-xWxO4 ceramics were comprehensively studied. X-Ray diffraction illustrated all samples exhibit single-phase monoclinic wolframite structure when x = 0–0.15, in which W6+ replaces Mo6+ sites formed solid solution. W6+ effectively improves sintering properties of the MgMoO4, the average grain size and relative density were increased. Raman characterization reveals that suitable W6+ substitution amount leads to reduction of v1 Ag peaks FWHM and the enhancement of specific v3 Ag peak for Mo/WO4 tetrahedron, which improves the ordered distribution of the crystal structure. The above combined effect results in the increased Q × f value, but has little influence of W6+ substitution on εr and τf for MgMoO4. When x = 0.09, MgMo0.91W0.09O4 ceramic sintered at 1050 °C has optimal microwave dielectric performance: εr = 7.21, Q×f = 90,829 GHz, τf = ?67 ppm/°C.  相似文献   

16.
《Ceramics International》2022,48(16):22789-22798
(1-x)Li2Zn3Ti4O12-xSr3(VO4)2 (0.1 ≤ x ≤ 0.4) microwave dielectric ceramics were fabricated by solid-state sintering technology. The impact of SV addition on the microstructure, dielectric properties, sintering process, and defects behaviour was studied. The formation of SrTiO3 and the glass phase were observed via XRD and TEM, and the latter resulted in a decrease in the sintering temperature. The variations in microwave dielectric properties were consistent with the empirical mixture rules calculated by XRD refinement, and a near-zero τf value was obtained. The Li, Zn and V elements of the glass phase and the liquid phase sintering model were deduced via DSC, TEM and Raman spectroscopy. Then, the defect behaviour, such as oxygen vacancies, Ti3+, and V4+, was investigated by XPS and complex impedance spectroscopy. It was found that the generation and migration of defects occurred much more easily in 0.7LZT-0.3 SV than in LZT, resulting in a higher dielectric loss. Finally, the 0.7Li2Zn3Ti4O12-0.3Sr3(VO4)2 ceramic sintered at 900 °C exhibited excellent microwave dielectric properties of εr = 17.8, Q × f = 41,891 GHz, and τf = ?4.4 ppm/°C and good compatibility with silver electrode, showing a good potential application for LTCC.  相似文献   

17.
The 〈0 0 1〉-textured Ba4Nd9.33Ti18O54 (BNdT) ceramics were fabricated by templated grain growth process. Acicular particles prepared using K2SO4 molten salt were used as template and aligned by tape casting in the equiaxed BNdT powder. Crystalline phases of sintered specimen exhibited {h k 0} and {0 0 1} development in the plane of parallel and perpendicular to the casting direction, respectively. The formation of a slight amount of secondary phase in the template particles and the compositional deviation inhibited the densification and texture development for BNdT. To improve the sinterability, the composition shifted from BNdT to Ba2Ti9O20 (B2T9) rich side slightly in BaONd2O3TiO2 ternary system, which enables to promote a liquid phase during the sintering, was examined as a matrix phase. Resultant ceramics including B2T9-rich matrix phase displayed high density and large dielectric anisotropy. Temperature dependence of dielectric constant showed negative and positive behavior between the direction of parallel and perpendicular to the 〈0 0 1〉-textured BNdT. Near-zero temperature coefficient of resonant frequency (τf) in TE0 1 1 mode was obtained in the textured ceramics with the degree of {0 0 1} orientation of approximately 0.37 on the disk plane. The exceptional temperature behavior of BNdT made it possible to control the τf over the wide range by the combination of dielectric anisotropy.  相似文献   

18.
《Ceramics International》2022,48(8):10713-10720
Ba2Ti9O20 (short for B2T9) ceramics doped with 0.9 mol% MnO2 and y mol% WO3 were prepared by solid-state reaction. The influence of sintering temperature, content of WO3 dopant and the molar ratio x of TiO2: BaCO3 on crystal structure, microstructures as well as microwave dielectric properties of B2T9 ceramics was systematically investigated. The major phase of all samples is B2T9, and the minor phase is BaWO4, respectively. The content of impurity TiO2 alternates with the variation of compositions and sintering temperature, which also leads to different microwave dielectric properties. With the continuous increase of the sintering temperature, the B2T9 phase grains gradually grow larger and transform from rod grains to plate-like grains. The enlargement and flattening of grains also result in the decrease of compactness and deterioration of microwave dielectric properties. It is found that B2T9 ceramics possess better performance when the sintering temperature is 1340°C, which is related to lower TiO2 content, BaWO4, B2T9 grain size, aspect ratio of B2T9 phase and high compactness. When x = 4 and y = 0.2, the relative dielectric constant, quality factor and the temperature coefficient of resonant frequency are 38, 23758 and 7 ppm/°C, respectively.  相似文献   

19.
《Ceramics International》2020,46(9):13225-13232
The densification and microwave dielectric properties of H3BO3 ceramics prepared by dry pressing at room temperature were studied. The results show that pressure is the key factor of densification of H3BO3 ceramics. No second phase appears in all the as-fabricated H3BO3 ceramic samples. A dense H3BO3 ceramic (relative density~97.6%) was obtained by uniaxial compression of 384 MPa for 300s and the optimal microwave dielectric properties are εr = 2.83, Q × f = 59,400 GHz (f = 16 GHz), τf = −91 ppm/°C, which make it as a prospective candidate for microwave and millimeter-wave devices such as substrates for 5G communication technology.  相似文献   

20.
The microwave dielectric properties of low-loss A0.5Ti0.5NbO4 (A = Zn, Co) ceramics prepared by the solid-state route had been investigated. The influence of various sintering conditions on microwave dielectric properties and the structure for A0.5Ti0.5NbO4 (A = Zn, Co) ceramics were discussed systematically. The Zn0.5Ti0.5NbO4 ceramic (hereafter referred to as ZTN) showed the excellent dielectric properties, with ɛr = 37.4, Q × f = 194,000 (GHz), and τf = −58 ppm/°C and Co0.5Ti0.5NbO4 ceramic (hereafter referred to as CTN) had ɛr = 64, Q × f = 65,300 (GHz), and τf = 223.2 ppm/°C as sintered individually at 1100 and 1120 °C for 6 h. The dielectric constant was dependent on the ionic polarizability. The Q × f and τf are related to the packing fraction and oxygen bond valence of the compounds. Considering the extremely low dielectric loss, A0.5Ti0.5NbO4 (A = Zn and Co) ceramics could be good candidates for microwave or millimeter wave device application.  相似文献   

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