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1.
《Ceramics International》2020,46(14):22221-22229
The (La0.3Pr0.7)1-xCaxCrO3 (x = 0, 0.1, 0.3 and 0.5) ceramics have been synthesized by a sol-gel method. The compounds crystalize in orthorhombic structure with space group Pnma at room temperature. The magnetic measurements confirm that the materials form canted antiferromagnetic (AFM) ordering from 254.1, 231.2, 118.5, 49.3 K for the samples of x = 0, 0.1, 0.3 and 0.5, accompanied by a spin reorientation transition at 191.4, 145.1, 55.8, 38.9 K because of the Pr3+-Cr3+ interaction. Meanwhile, a positive exchange bias effect is observed due to the antiparallel coupling between the Pr3+ and the canted AFM structure of Cr3+. The Néel temperature, compensation temperature as well as the coupling strength of Pr3+-Cr3+ monotonously decrease with the increase of Ca2+ concentration. For the samples of x = 0.1 and 0.3, there exists a field induced Pr3+-Pr3+ AFM ordering. By means of dielectric measurements, large permittivity at room temperature and dielectric relaxation are observed in all the samples. The permittivity is decreased and dielectric relaxation moves to low temperature range with the increase of Ca2+ concentration. A relaxor-like ferroelectric transition is observed in the measuring temperature range in Ca2+ doped samples.  相似文献   

2.
A/B site co-substituted (Ca1?0.3xLa0.2x)[(Mg1/3Ta2/3)1?xTix]O3 ceramics (0.1  x  0.5) were prepared by solid state reaction and the structures, microstructures and dielectric properties were investigated. B site 1:2 cation ordering and oxygen octahedra tilting lead to monoclinic symmetry with space group P21/c for x = 0.1. For x above 0.1, the ordering was destroyed and the crystal structure became orthorhombic with space group Pbnm. The B site 1:2 cation ordering tended to be destroyed to form 1:1 ordering by the A site La3+ substitution. The dielectric constant increased linearly with increasing content of Ti4+ as the increasing second Jahn–Teller distortion enhanced the B site cation rattling. The temperature coefficient of resonant frequency and Qf values showed abnormal variations, which were refined to be caused by the increasing A site cation vacancy and diffused distribution of small size ordering domains respectively. Good combination of microwave dielectric properties was obtained at x = 0.5, where ?r = 48, Qf = 21,000 GHz and τf = 2.2 ppm/°C.  相似文献   

3.
《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   

4.
《Ceramics International》2020,46(10):16185-16195
(1–x)NdGaO3-xBi0.5Na0.5TiO3 [(1–x)NdGaO3-xBNT, 0.05 ≤ x ≤ 0.7)] ceramic systems were fabricated using a conventional solid-state reaction, and their phase structures, microstructures, and microwave dielectric characteristics were systematically investigated. The XRD patterns results showed an orthorhombic perovskite structure as the main phase with a Pbnm space group at x = 0.05. In a range of x = 0.1–0.3, the main Nd3Ga5O12 cubic structure phases (Ia-3d space group) had been formed due to the increase in the cation vacancies resulting from the Na and Bi ion volatilization at the higher densification sintering temperatures (1400–1450 °C). As (Na0.5Bi0.5)2+ ions increased and the sintering temperatures decreased, the orthorhombic perovskite-type Pnma space group solid solutions (the main phases) were detected at x = 0.4 and 0.5, accompanied with a certain amount of second phase Bi2O3 in the samples at x = 0.6 and 0.7. The results of Raman spectroscopy analysis, EDS data analysis, and surface morphologies observations were basically in keeping well with the XRD analysis results, wherein the Raman-active modes also implied that the crystal structure of the main phase actually had a tendency to change the perovskite structure when x = 0.3. The εr value increased gradually as the x value increased from 0.05 to 0.5 because of the increase in the ionic polarizability, and increased slowly at x = 0.6, then decreased slightly as the x value further increased to 0.7 due to the formation of the second phase. The Q × f values of the (1-x)NdGaO3-xBNT (x = 0.05–0.7) ceramic systems were strongly influenced by the densification, lattice defects, and phase composition and content. The τf values could be well predicted by replacing Na, Bi and Ti ions with suitable substitutions for these ceramic systems. As a result, the new temperature-stable ceramics with optimal dielectric properties of εr ~43.1, Q × f ~6700 GHz (at 5.85 GHz), and τf ~ −24.5 ppm/°C and εr ~ 44.5, Q × f ~ 5600 GHz (6.12 GHz), and τf ~ +2.4 ppm/°C were obtained in the (1-x)NdGaO3-xBNT composite series at x = 0.5 and x = 0.6 sintered at 1320 °C and 1250 °C for 4 h, respectively.  相似文献   

5.
The structure evolution, sintering behavior and microwave dielectric properties of La(2−x)/3Nax(Mg1/2W1/2)O3 (x = 0–0.5) were investigated in this paper. The X-ray diffraction (XRD) results show that all samples exhibit single phase, and the structure changed from orthorhombic when 0  x < 0.3 to monoclinic phase when 0.3  x  0.5. The size and ordering degree of A/B-site domains decrease with the increase in x value. The sintering temperature of the Na-doped samples increased compared to the pure La2/3(Mg1/2W1/2)O3 (LMW) due to the estimated decrease in the concentration of A-site vacancies. The addition of Na+ ion does not affect the dielectric permittivity greatly. The Q × f value decreases with the increase in x value, although the estimated concentration of A-site vacancies decreases with increasing x, which may be ascribed to the decrease of A/B-site ordering and domain size with the increase in x. The temperature coefficient of resonant frequency changed from negative values into positive values with the increase in x value.  相似文献   

6.
《Ceramics International》2020,46(10):16416-16421
The magnetic, ferroelectric, and photocatalytic properties of (1-x)BiFeO3-xBaTiO3 (0.0 ≤ x ≤ 0.4) powders synthesized by sol-gel method have been investigated. X-ray diffractometry confirms that the phase of the samples changed from rhombohedral to cubic with the increase in BaTiO3 content. The grain size decreases and the particle shape becomes homogeneous with the introduction of BaTiO3. BaTiO3 substitution enhances the multiferroic properties of the ceramics and the maximum remnant magnetization (0.261 emu/g) and remnant polarization (20 μC/cm2) have acquired in 0.8BiFeO3-0.2BaTiO3 and 0.7BiFeO3-0.3BaTiO3, respectively. The absorbance in ultraviolet and visible light regions is improved obviously for powder with x = 0.3. The energy band gap of the samples decreases from 2.06 eV to 1.57 eV with the introduction of BaTiO3, indicating that the excitation rate of photogenerated electron-hole pairs is improved. The highest methylene blue degradation efficiency of ~62% within 3 h under the visible light is achieved in the 0.7BiFeO3-0.3BaTiO3 which can be attributed to its suitable energy band gap and large remnant polarization.  相似文献   

7.
《Ceramics International》2022,48(11):15282-15292
The Mo-based glass-free spinel-type structure of the (Na1-xKx)2MoO4 (x = 0.0, 0.1, and 0.2) ceramic series was prepared using the traditional solid-state method at the low sintering temperature (<650 °C). The microwave dielectric properties of the (Na1-xKx)2MoO4 series were determined in terms of phase compositions, crystal structure (via XRD), and microstructure analysis (via FE-SEM and EDS). The results revealed that the double-phase (cubic and orthorhombic) formation plays a significant role in the entire (Na1-xKx)2MoO4 series. It exhibits excellent dielectric properties: dielectric constant εr = 4 (1 GHz)/3.77 (15 GHz), tangent loss tan δ = 8.3 × 10?2 (1 GHz)/7 × 10?3 (15 GHz; Q × f = 2143 GHz), temperature coefficient of frequency (TCF) τf = ?6.45 ppm/°C, and room temperature thermal conductivity (κ) = 1.76 W/(m.K) for x = 0.1 at a sintering temperature of 575 °C. These make the (Na1-xKx)2MoO4 ceramic series a potential candidate for low-temperature co-fired ceramic (LTCC) substrate applications (as used in antennas) for high-speed data communications.  相似文献   

8.
In this paper, the crystal structure, vacancy defect, local electron density and magnetic properties of Gd1-xCaxCrO3 (0 ≤ x ≤ 0.3) polycrystalline samples were investigated systematically. The crystal structural analyses show that all the samples are orthorhombic phase and a structural distortion happens around x = 0.3. Due to the formation of Cr4+ ions, both the lattice constant and the Cr–O bond length decrease. The results of positron annihilation spectrum reveals that the vacancy defect concentration increases and the local electron structure changes with the introduction of Ca2+ ions. The field-cooled (FC) and zero-field cooled (ZFC) curves of Gd1-xCaxCrO3 samples measured under H = 100 Oe exhibits negative magnetization characteristics due to the interaction between Gd3+ and Cr3+ ions, and the magnetism can be affected by the structural distortion.  相似文献   

9.
《Ceramics International》2020,46(5):6270-6275
The present study investigated thermo-mechanical behaviour of A-site deficient perovskites Li3xLa1/3-xTaO3 (LLTaO) and Li3xLa1/3-xNbO3 (LLNbO) with x = 0.00 to 0.06 as a function of temperature by means of thermo-mechanical analysis. LLTaO for all compositions exhibits an orthorhombic-tetragonal phase transition around 200 K, above which it has a tetragonal phase. As the temperature increases from 200 K to 400 K, the linear expansion coefficient shows a slight decrease for all the compositions, followed by a constant value of ~3 × 10−6 K−1 above 400 K regardless of x. On the other hand, LLNbO has an orthorhombic phase for x ≤ 0.02 and the tetragonal for x ≥ 0.04 at room temperature. The linear expansion coefficient of LLNbO with x ≤ 0.02 shows a peak around 470 K, which can be attributed to an orthorhombic-tetragonal phase transition. In addition, the expansion coefficient of LLNbO with x ≥ 0.02 significantly increases as the temperature rises from 200 K to 400 K, followed by a plateau and a relatively abrupt decrease after reaching a temperature above 600 K. Additional ionic conductivity measurement of LLNbO suggested that the inconstant expansion behaviour could be attributed to the lithium-ion motion.  相似文献   

10.
Tungsten bronze ceramics of composition Sr2Ag0.2Na0.8Nb5-xTaxO15 were synthesized by solid state methods to investigate the impact of Ta replacement on the structure and energy-storage properties (ESP). The study on the relationship between structure and electric properties revealed three main conclusions: (1) as the Ta5+ concentration increased, the crystal structure transformed from an orthorhombic Im2a phase to a tetragonal paraelectric P4bm phase; (2) a high recoverable energy storage density (1.44 J/cm3) and a moderate efficiency (82%) under low-electric fields was obtained in x = 0.3 sample; (3) both dielectric properties (?9.6 to 232.7 °C) and ESP (30–150 °C) exhibit an excellent thermal stability for x = 0.3 sample. In addition, a high current density (863.69 A/cm2) and a large powder density (70.21 MW/cm3) were achieved simultaneously. The current system could be a promising candidate in temperature-stable dielectric capacitors under low-fields and over a broad temperature range.  相似文献   

11.
Lead-free (Bi0.5Na0.5)1-xSrxBi4Ti4O15 ceramics (x = 0–0.9) are fabricated by solid state reaction process. XRD analysis shows the symmetry divergence from tetragonal to orthorhombic phase accompanied by morphotropic phase boundary with increasing strontium content. Raman spectra confirm the incorporation of strontium into (Bi2.5Na0.5Ti4O13)2- layers. SEM graphs exhibit the typical plate-like morphology with regular variation of grain size and crystallization as strontium increases. Multistage ferroelectric transition is observed with x = 0.2–0.4. Piezoelectric performance measurements present the well thermal stability at x = 0.4. The dielectric properties display a shifting of Curie temperature towards low temperature with increasing strontium ions. It can be due to the crystal lattice distortion by larger radius of strontium and the increasing tolerance factor. ac conductivity and impedance measurements suggest that electron hopping mainly contributes to the low temperature region. Ionization conductivity by oxygen vacancy migration including first-ionization and double-ionization plays the dominating role in the middle and high temperature region. The controllable properties indicate the potential applications for electric devices of (Bi0.5Na0.5)1-xSrxBi4Ti4O15 ceramic.  相似文献   

12.
In this paper, a simple, reproducible and cost-effective solid-state reaction sintering process is developed to fabricate (K0.5Na0.5)NbO3-xBaNi0.5Nb0.5O3-δ (KNN-xBNN) ceramics with a narrow bandgap and room-temperature ferromagnetism. Here, we report a systematic investigation of the influence of the BaNi0.5Nb0.5O3-δ (BNN) concentration on the properties of KNN-xBNN ceramics. All ceramics form orthorhombic perovskite structures with a space group Amm2 and a weak peak at the wavelength of 550 cm?1 that is characteristic of the pillow shoulder of the orthorhombic phase. KNN-xBNN ceramics with x between 0.02 and 0.08 have a narrow bandgap of about 2.5 eV—much smaller than the 3.5 eV of its parent (K0.5Na0.5)NbO3 (KNN) ceramic—which is attributed to Ni2+-oxygen vacancy combinations (Ni2+-VO) raising the valence electron energy level of the KNN ceramic. Furthermore, doping BNN into KNN ceramics can significantly convert the magnetism from diamagnetism to ferromagnetism and the component of x = 0.08 achieves both maximum saturation magnetisation intensity (14 memu/g) and minimum coercive magnetic field (80 Oe). Our findings provide a systematic insight into the bandgap tunability and ferromagnetism induction at room temperature in lead-free perovskite KNN-xBNN ceramics, as well as demonstrate their potential applications in perovskite solar cells and multiferroic devices.  相似文献   

13.
《Ceramics International》2016,42(5):5830-5841
The effect of CuO addition on magnetic and electrical properties of Sr2Bi4Ti5O18 (SBT) lead-free bismuth layered structure ferroelectric ceramics have been studied and reported. Interestingly, the prepared samples exhibit multiferroic behavior with the coexistence of magnetic and ferroelectric phase transition temperature. Magnetic phase transition with Neel׳s temperature (TN) of 657 K is observed at 0.75 mol% of CuO added SBT ceramics, which is higher than the well known multiferroic BiFeO3 (643 K) and the ferroelectric phase transition with Curie temperature (TC) of 587 K is observed at 1 mol% of CuO added SBT ceramics, which is relatively higher than the reported pure SBT ceramics (558 K). Further, the electrical properties such as dielectric, ferroelectric, piezoelectric, leakage current density characteristics and optical properties were investigated as a function of x (x=0, 0.25, 0.5, 0.75 and 1 mol%). Presence of strong magnetic super-exchange interactions in CuO and the creation of oxygen vacancies play a vital role in the enhancement of magnetic and electrical properties of CuO doped SBT ceramics. Moreover, the present results indicate that, small amount (0.25 mol%) of CuO addition in SBT ceramics enhances the electrical properties significantly and vice versa, large amount (0.75 mol%) of CuO addition enhances the magnetic properties. Thus, the presence of magneto-electric coupling effect was observed in CuO doped Sr2Bi4Ti5O18 ferroelectric ceramics.  相似文献   

14.
Domain structure of several poled (K0.50Na0.50)1?xLixNbO3 ceramics (with chemical compositions of x = 0.03, 0.065, and 0.08, respectively) was investigated by means of observing the domain patterns with an acid‐etching technique. Among the three ceramics, the one with x = 0.03 is of orthorhombic phase and the other two are of tetragonal phase at room temperature. It was found that these ceramics possess distinctly different features of domain patterns and show a large difference in the time‐aging stability of piezoelectric properties. For the ceramic with x = 0.03, domain patterns consist of simply one single set or a few sets of parallel stripes inside the polycrystalline grains. In contrast, for those with x = 0.065 or 0.08, herringbone‐type patterns and a large number of watermarks are additionally observed. Furthermore, the ceramic with x = 0.03 was confirmed to have a much better time‐aging stability of piezoelectric properties than the other two. The results indicate that domain structure is more stable in orthorhombic phase than in tetragonal phase.  相似文献   

15.
Multiferroic materials have attracted much interest in the last decade due to both the intriguing fundamental science and the potential applications in spintronics and magnetoelectric data storage devices. In this work, we have investigated and discussed the evolution of the magnetic properties of the multiferroic (1-x)Pb(Fe2/3 W1/3)O3-xBiFeO3 solid solution ((1-x)PFW-xBFO, x = 0, 0.025, 0.05, 0.075, 0.1 and 0.15). The magnetic phase diagram is established based on the magnetic measurement results, which reveals six magnetically ordered states on the PFW-rich side of the solid solution. The origins of the complex evolution of magnetic order in the PFW-BFO solid solution are discussed from the point view of the variations in both the –Fe–O–Fe– and –Fe–O–W–O–Fe– superexchange routes, which are intimately related to the ratio of magnetic Fe3+ ion concentration on the B-site and the changes in the local structural order/disorder and chemical homogeneities. Combining the magnetic phase diagram with the relaxor characteristic phase diagram of the (1-x)PFW-xBFO system, a striking feature is found that the ergodic relaxor (ER) state and the weakly ferromagnetic phase coexist in the composition range of 0.025 ≤ x ≤ 0.1 between the freezing temperature Tf and the Burns temperature TB.  相似文献   

16.
In order to stabilize the perovskite structure and improve the storage energy density (U) of Pb(Tm1/2Nb1/2)O3 (PTmN) based materials, Pb(Mg1/3Nb2/3)O3 (PMN) was introduced into PTmN to form binary (1-x)PTmN-xPMN solid solution ceramics. The XRD patterns show that all the compositions belong to orthorhombic phase with space group Pbnm. The Curie temperature (TC) gradually decreases while the dielectric constant (ε') increases for (1-x)PTmN-xPMN with increasing PMN content. The ε' of each composition above TC obeys the Curie-Weiss law. The appearance double hysteresis loop confirms the antiferroelectric nature of (1-x)PTmN-xPMN (x = 0.02–0.18) ceramics. With the increase of PMN concentration, the maximum polarization slowly increases from 8.58 μC/cm2 to 29.5 μC/cm2 while the threshold electric field (EA-F) gradually declines from 290 kV/cm to 120 kV/cm. The maximum of U (3.12 J/cm3) is obtained in 0.92PTmN-0.08PMN ceramic with moderate EA-F = 220 kV/cm, which makes (1-x)PTmN-xPMN ceramics safe in practical application.  相似文献   

17.
Experimental research of the crystal structure, polarization properties, and reverse nonlinearity of ceramic solid solutions of the (1-x) (Na0·5K0.5)NbO3-xPb(Ti0·5Zr0.5)O3 (KNN-PZT) quasi-binary system with 0.0 = x ≤ 1.0 in a wide range of external influences (temperatures, strength of dc/ac fields) has been done. Based on the X-ray structural data, an x-T diagram of the system has been constructed, and correlations of the behavior of the macroproperties of solid solutions with the features of their phase states with the temperature change have been established. It has been concluded that it is advisable to use the proposed compositions when designing microelectronic devices operating in various extreme conditions.  相似文献   

18.
The microwave dielectric properties of Sr(Ga0.5Nb0.5)1?xTixO3 (x = 0, 0.1, 0.2 and 0.3) ceramics have been investigated together with their microstructures. Single‐phase solid solutions are achieved in this series of ceramics. The ordering features are comprehensively analyzed by transmission electron microscopy and Raman spectroscopy. Local 1:1 ordering in B‐site leads to a double‐cubic structure with space group , while Ti substitution disrupts this 1:1 ordering between Ga and Nb, and the metastable ordering between Ti and (Ga + Nb) is speculated to form due to their large size difference. The dielectric constant and temperature coefficient of resonant frequency increase nonlinearly as x increases, while the Qf value decreases gradually. The variation trend of Qf value is mainly attributed to the intrinsic loss because of the increasing vibrational anharmonicity by Ti substitution. The ordering transition from short coherence, long‐range ordering to short‐range ordering with increasing Ti content has an agreeable and weak effect on the Qf value. The best combination of microwave dielectric properties is achieved for the composition of x = 0.3: εr = 46.6, Qf = 42 200 GHz and τf = 5.0 ppm/°C.  相似文献   

19.
《Ceramics International》2022,48(14):19954-19962
Lead-free (1-x)(K0.5Na0.5)(Nb0.96Sb0.04)O3-x(Bi0.5Na0.5)(Zr0.8Ti0.2)O3 ceramics (abbreviated as (1-x)KNNS-xBNZT, x = 0, 0.01, 0.02, 0.03, 0.035 and 0.04) were synthesized by the solid-state method, and the dependence of phase evolution, microstructure, oxygen vacancy defect and electrical properties on compositions were carefully investigated. All ceramics had a pure perovskite structure and a dense microstructure. The phase transition temperatures (TR-O and TO-T) of the ceramics were adjusted by adding BNZT, and the rhombohedral-tetragonal (R-T) phase coexistence boundary was successfully constructed at room temperature when x = 0.03, the excellent piezoelectric performance (d33 ~ 323 pC/N, kp ~ 0.372) and high Curie temperature (TC ~ 276 °C) have been achieved at this time. The grain size of the ceramics showed a strong difference on x content, and the maximum relative density value of 95.42% was obtained. The domain structure characterized by PFM confirmed that the ceramics possess small-sized nano-domains and complex domains at x = 0.03, which are the origin of enhanced piezoelectric properties. Moreover, the oxygen vacancy defect that can pin the domain walls was increased with the addition of (Bi0.5Na0.5)(Zr0.8Ti0.2)O3. As a result, the doping with BNZT can significantly affect the phase structure and electrical properties of the ceramics, indicating that the (1-x)KNNS-xBNZT ceramics system with a R-T phase boundary is a promising lead-free piezoelectric material.  相似文献   

20.
Bismuth sodium zirconate titanate (Bi0.5Na0.5)Zr1?xTixO3 with (x=0, 0.1, 0.2, 0.3, 0.4, 0.5 and 0.6) ceramics was fabricated by a conventional sintering technique at 850–1000 °C for 2 h. From X-ray diffraction study, three regions of different phases were observed in the ceramic system; i.e., orthorhombic phase region (0≤x≤0.2), mixed-phase region (0.3≤x≤0.4), and rhombohedral phase region (0.5≤x≤0.6). It was observed that the phase evolution from orthorhombic to rhombohedral symmetry resulted in a noticeable increase of the dielectric properties. The results from the high- and low-field dielectric responses indicated that the dielectric properties of both BNZ and BNZT ceramics were dominantly attributed to the reversible contribution. It was also noticed that grain size showed only partial influence on the increase of low-field dielectric constant in Ti-rich BNZT ceramic.  相似文献   

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