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1.
It is difficult to maintain strong piezoelectric properties over a wide temperature range in (K,Na)NbO3 (KNN)-based ceramics owing to the polymorphic phase boundary (PPB). Here, we propose advantageously utilizing the synergistic effect of crystal orientation and phase structure to address this issue. The 〈0 0 1〉pc textured (1 − x)(K0.48Na0.52)(Nb0.96Sb0.04)O3x(Bi0.5Ag0.5)ZrO3 (KNNS–xBAZ) ceramics with different phase structures were synthesized via the templated grain growth method. A high piezoelectric coefficient (d33) of 505 ± 25 pC/N, an electric field-induced strain of 0.21%, and a superior temperature stability (d33 exhibited a high retention of ≥78% at the temperature up to 200°C; strain maintained within 5.7% change over a temperature range of 30–150°C) were simultaneously achieved in textured KNNS–0.03BAZ ceramics. The flattened Gibbs free energy induced by the R–O–T multiphase coexistence, the strong anisotropy of crystals, and the abundant nanodomains contributed to the enhanced piezoelectric properties. The contribution of the strong anisotropy of crystals in 〈0 0 1〉pc textured ceramics compensates for the deterioration of the piezoelectric properties caused by the phase structure deviation from the PPB with increasing temperature, which benefits the superior temperature stability of the textured KNNS–0.03BAZ ceramics. The previous merits prove that utilizing the synergistic effect of crystal orientation and phase structure is an effective strategy to boost the piezoelectricity and their temperature stability of KNN-based ceramics.  相似文献   

2.
Lead-free 0.955K0.5Na0.5NbO3-0.045Bi0.5Na0.5ZrO3?+?0.6%MnO (KNN-0.045BNZ?+?Mn0.6) ceramics have been prepared by a conventional solid-state sintering method in air. All the samples sintered at different temperatures possess a coexisting phase boundary (CPB) between rhombohedral (R) phase and tetragonal (T) phase. The increase of sintering temperature (Ts) increases the phase fraction of T phase in CPB region. Mn2+, Mn3+ and Mn4+ ions coexist in all the KNN-0.045BNZ?+?Mn0.6 ceramics sintered at 1110?°C to 1190?°C. High sintering temperature can induce a transformation from MnNb'' defects to MnNb' defects. The samples with fine grain show stable octahedral structure. The KNN-0.045BNZ?+?Mn0.6 ceramics with fine grain possess excellent temperature stability of d33* due to the wide phase transition region. The increase of sintering temperature induces the (R-T) phase transition temperature to move to room temperature.  相似文献   

3.
(Bi1/2Na1/2)TiO3-based materials have received much attention due to large electro-strain and high piezoelectric constant (d33), but the tough issue is that the existence of inherent depolarization temperature (Td) limits the temperature stability and application temperature range. Previously, reports about the formation of BNT/oxide (i.e., ZnO, Al2O3) composites thought that Td can be deferred to a higher temperature and then thermal depolarization improves. However, the deferred Td of BNT/oxide composites is limited, accompanied by a low d33. Here, we design the {[Bi0.5(Na0.8K0.2)0.5]1-xPbx}TiO3 ceramics, leading to a big shift of Td from 77 ℃ to 390 ℃. Large d33 (140 pC/N) and high Td (∼263 ℃) can be simultaneously achieved for the sample with Pb=0.05, and Td could be further deferred higher (390 ℃) for Pb=0.20. The off-centre displacement of Pb induced by Pb-O hybridization in the PbO12 polyhedron and ferroelectric order stabilized by the addition of Pb can provide the driving force to strengthen the ferroelectric order, and then promote the thermal stability.  相似文献   

4.
《Ceramics International》2020,46(17):26616-26625
New types of Ce-doped CexBi7-xTi4.5W0.5O21 (BTW-BIT-xCe) Aurivillius intergrowth ceramics with high Curie temperatures were synthesized to improve the piezoelectric performances as well as the conduction behaviour, and these ceramics exhibit great potential for high-temperature lead-free piezoelectric applications. The crystal structure, electrical properties and conduction behaviour of BTW-BIT-xCe samples were analysed thoroughly. The XRD patterns combined with Rietveld refinements of the patterns showed that the crystal structure transformed from orthorhombic structure towards pseudo-tetragonal structure with increasing CeO2 dopant, indicating that a higher symmetry was obtained. The dielectric properties of Ce-doped samples were improved, accompanied by a significant drop in the dielectric loss and a slight decreased Curie temperature (705 °C–683 °C). An enhanced piezoelectric constant d33 of 25.3 pC/N was obtained in BTW-BIT-0.12Ce, which may be attributed to a common decrease in the electrical conductivity and coercive field. Besides, a low electrical conductivity of 2 × 10-6 S/cm at 540 °C was achieved in the same component owing to a decreased concentration of the oxygen vacancies, which was verified by analyses on XPS spectra. The above results indicate that Ce-doped BTW-BIT samples have great development potential for high temperature piezoelectric applications.  相似文献   

5.
It has great research value and application potential to develop K0.5Na0.5NbO3(KNN)-based ceramics with low sintering temperature (Tsinter) and excellent piezoelectric properties. However, it is difficult to achieve the two goals of reducing Tsinter and improving piezoelectric properties together. We provide a new process (NP) to solve this problem. Compared with traditional process (TP), Tsinter of 0.945K0.48Na0.52Nb0.96Ta0.04O3-0.055BaZrO3+6 mol%MnO (KNNT-0.055BZ+6 Mn) sintered by NP is reduced greatly and its piezoelectric strains are improved obviously. Reducing atmosphere is an important part for NP. The reducing atmosphere condition can improve piezoelectric strain by increasing extrinsic contribution of reversible non-180° domains and intrinsic contribution of reversible R(rhombohedral)-M(monoclinic) phase transition. NP ceramics sintered at low Tsinter = 1045 °C (NP1045) possess excellent d*33 (575 pm/V) at the electric field (20 kV/cm). The NP1045 ceramics fatigued after 106 unipolar cycles show excellent fatigue resistance. Its d*33 (575 pm/V) varies less than 10 % from room temperature to 185 °C.  相似文献   

6.
《Ceramics International》2022,48(16):23241-23248
In this work, a two-step solid-state reaction method is used to prepare the 0.55 Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3/xSnO2 (PNN-PZT/xSnO2) ceramics. The influences of SnO2 on the crystalline structure, electromechanical properties, and temperature stability of PNN-PZT ceramics were studied in detail. The results demonstrate that the Sn4+ ions are successfully introduced into the PNN-PZT crystalline lattice and substitute B-site Ni2+ and Zr4+. The x = 0.0025 ceramic with the coexistence of rhombohedral, tetragonal, and pseudocubic phases exhibits the optimized comprehensive properties: the quasi-static piezoelectric constant d33, large-signal d33*, electromechanical coupling coefficients kp and kt, free dielectric constant εr, and mechanical quality factor Qm are 1123 pC/N, 1250 p.m./V, 0.63, 0.54, 9529, and 57, respectively. Meanwhile, the Curie temperature for this composition is 103 °C, almost maintaining the same level as the PNN-PZT matrix. After annealing at 75 °C, the retained d33 of x = 0.0025 ceramic is as high as 975 pC/N, superior to the PNN-PZT matrix (retained d33 ≈ 873 pC/N). Our results provide a promising piezoelectric material for board bandwidth, high sensitivity, and miniaturized medical ultrasonic transducers applications.  相似文献   

7.
《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   

8.
In this work a microstructural qualitative and quantitative study of spatial stress distributions in modified KNN ceramics (K0.44Na0.52Li0.04)1-xCox/2 (Nb0.86Ta0.10Sb0.04)O3, according to the polarization state is shown. X-ray diffraction reflects a perovskite crystalline structure with coexistence of Tetragonal and Orthorhombic phases (T/O). Confocal Raman microscopy shows that these crystalline phases are distributed in randomly micrometric regions through the ceramic volume. Tetragonal regions show higher piezoelectric coefficient and exhibit a higher micro-stress that hardens the ferroelectric response. By the contrary, the occurrence of orthorhombic micro-regions softened the ferroelectric behavior and reduced their piezoelectric coefficients. The ferroelectric response of ceramics is studied, where poling is also shown as a factor that affects the spatial micro-stress distributions. Finally, a model that relates the results obtained by Raman characterization with the ferroelectric properties and stress states is proposed.  相似文献   

9.
Lead-free 0.99(0.96K0.46Na0.54Nb1-xTaxO3-0.04Bi0.5(Na0.82K0.18)0.5ZrO3)-0.01CaZrO3 (0.99(0.96KNNTax-0.04BNZ)-0.01CZ) ceramics were prepared by a solid-state sintering method. Ta2O5 doped in the 0.99(0.96KNNTax-0.04BNZ)-0.01CZ ceramics results in a phase structure transition from the orthorhombic (O)/tetragonal (T) phase to the rhombohedral (R)/T phase. The Ta2O5 dopant induces a decrease in the average grain size from ~1.70 to ~0.69 μm. At = 0.02 and 0.04, the ceramics have a high reverse piezoelectric coefficient (~500 pm/V under 25 kV/cm). The ceramics with x = 0.04 show an optimal level of unipolar strain, reaching 0.17% under 35 kV/cm at room temperature, and their field-induced strain varies <10% in the temperature range from 25 to 135°C. The presence of the O phase in the polymorphic phase boundary (PPB) improves the temperature stability the reverse piezoelectric coefficient (). Obtaining KNN-based ceramics with good piezoelectric properties and weak temperature sensitivity by designing a R/O/T phase boundary and controlling the average grain size to the submicrometer level is highly feasible.  相似文献   

10.
The (Ba0.94Ca0.06)(Ti0.9Sn0.1)O3 (BCTS) ceramics with pure perovskite structure were prepared by conventional solid-state reaction route with the addition of 0–0.8?mol% MnO2. The crystal structure, microstructure, and electric properties were investigated systematically. X-ray diffraction patterns showed that the addition of MnO2 changed the ratio of the coexistence of orthorhombic and tetragonal phases, which had apparent influences on the piezoelectric properties of ceramics. When the addition amount is 0.2?mol%, the average grain size increases from ~41.88–52.24?µm, and, however, the average grain size decreases with further addition > 0.2?mol%. A good combination of properties and performance could be achieved with the addition of 0.4?mol% MnO2. The mechanical quality factor Qm, dielectric loss tanδ, piezoelectric constant d33, and planar electromechanical coefficient kp measured are 216, 0.011, 578?pC/N, and 0.39, respectively. Therefore, results of this study suggest that the BCTS-Mn ceramics synthesized could exhibit a great potential for piezoelectric component applications.  相似文献   

11.
<001> ‐textured 0.99(K0.49Na0.49Li0.02)(Nb0.97‐xSb0.03Tax)O3‐0.01CaZrO3 [abbreviated as 0.99KNLN0.97‐xSTx‐0.01CZ, x = 0.03, 0.07, 0.10, 0.15, 0.20, 0.25] ceramics were prepared by templated grain growth (TGG) method and a two‐step sintering process. Giant longitudinal piezoelectric coefficient d33 (391 pC/N) and piezoelectric strain coefficient d33* (630 pm/V under an AC E‐field of 20 kV/cm) can be obtained in the textured ceramics with x = 0.25. All textured ceramics display superior kp (>54%) and g33 (>23 × 10?3 Vm/N) which are in an order of magnitude with PZT ceramics. The maximum value of kp (~63.3%) obtained in textured ceramics with x = 0.15 is higher than that of famous textured LF4 ceramics. Excellent comprehensive properties suggest that <001> ‐textured 0.99KNLN0.97‐xSTx‐0.01CZ ceramics are promising candidates in the field of lead‐free piezoelectric materials.  相似文献   

12.
[001] textured 0.40BiScO3-0.60PbTiO3-0.125 mol%Nb5+ (BS-60PT-0.125Nb) high-temperature piezoelectric ceramics were synthesized using templated grain growth process. A high texture degree F001 of 99% was obtained using 2 vol% BaTiO3 (BT) templates. The piezoelectric charge constant d33 and the unipolar strain under 40 kV cm−1 at room temperature for the textured ceramics are 646 pC N−1 and 0.36%, respectively, which is over two times as those for untextured ceramics (∼243 pC N−1 and 0.17%). The electrostriction Q33 value of the textured sample remarkably increased from 0.034 m4 C−2 to 0.068 m4 C−2 under 30 kV cm−1, showing a twice higher than untextured. Compared with random ceramics, the improvement piezoelectric response of the textured ceramics is primarily attributed to the increase of the dielectric constant εr and electrostriction coefficient Q33 along [001] orientation, which is originating from the anisotropy of piezoelectricity. The BS-60PT-0.125Nb textured ceramics have large piezoelectric response and ultrahigh electrostriction with high temperature stability (high depolarization temperature Td of ∼360°C and high Curie temperature Tc of 421°C), showing great potential for the piezoelectric applications at high temperatures.  相似文献   

13.
The microstructure of Bi0.5(Na0.70K0.20Li0.10)0.5TiO3 (BNKLT) coatings fabricated by thermal spray method was closely examined by TEM, revealing the coexistence of rhombohedral and tetragonal perovskite main phases, and very minor secondary phases, while all amorphous phase was crystallized after heat treatment. Obtaining coexisting rhombohedral and tetragonal perovskite phases after the thermal spray process involving the melting-recrystallization and heat treatment process resulted in piezoelectric ceramic coating with excellent electrical and electromechanical properties. The effective piezoelectric coefficient d33 of the heat-treated BNKLT coating reached 86?pm/V with substrate clamping, measured over macroscale by laser scanning vibrometer.  相似文献   

14.
Although KNN-based ceramics with high electrical properties are obtained through a variety of strategies, the temperature sensitivity is still one of the key technical bottlenecks hindering practical applications. Here, we use a new strategy, meticulously tailoring phase boundary, to refine the ferroelectric boundary of KNN-based ceramics, leading to high piezoelectricity companied with improving temperature stability. The highest d33 value in this system reaches 501 pC/N with a TC ∼ 240°C, whereas a large strain of ∼0.134% can be kept with 10% lower deterioration until 100°C. The origin of high piezoelectricity is mainly attributed to the well-preserved multiphase coexistence and the appearance of nanodomains, which greatly facilitate the polarization rotation. Instead of the changed intrinsic thermal insensitivity, the precision phase boundary engineering plays an important role in strengthening the temperature stability of electric-induced strain. This work provides a simple and effective method to obtain both high electrical properties and excellent thermal stability in KNN-based ceramics, which is expected to promote the practical applications in the future.  相似文献   

15.
《Ceramics International》2020,46(3):2798-2804
To further improve the properties of KNN-based lead-free ceramics, a new ceramic system, (0.98-x)K0.525Na0.475Nb0.965Sb0.035O3-0.02 BaZr0.5Hf0.5O3-x(Bi0.5Na0.5)ZrO3(KNNS-BZH-xBNZ) was designed, the relevant properties such as piezoelectricity, strain, and temperature stability were analysed in detail. It was found that the R-T phase boundary can be successfully constructed when x=0.030, and this two-phase coexistence shows relatively good comprehensive properties (d33~410 pC/N, TC~255 °C, Suni~0.132%, and d33*~441 pm/V). Meanwhile, its strain property also shows good temperature stability from room temperature to 180 °C (Suni100°C/SuniRT~97.5% and Suni180°C/SuniRT~83.9%), which is comparatively superior to many KNN-based ceramics and some lead-based ceramics. Therefore, KNNS-BZH-xBNZ ceramics may broaden the practical application of lead-free ceramics.  相似文献   

16.
《Ceramics International》2020,46(2):1390-1395
With close attention being paid to environmental issues and more legislation coming into force to limit the application of Pb-based materials, accelerating research on lead-free piezoelectric ceramics has become increasingly requisite and urgent. Herein, we have devised and synthesized (1-x)(K0.5Na0.5)0.98Ag0.02(Nb0.96Sb0.04)O3-x(Bi0.5Na0.5)ZrO3 [abbreviated as (1-x)KNANS-xBNZ, x = 0.01, 0.02, 0.03, 0.035, 0.04, 0.045, 0.05, 0.06] Pb-free ceramics. Phase transition, microstructure, electrical properties, and temperature stability of the ceramics have been comprehensively investigated. The findings illustrate that optimizing BNZ content can give rise to a rhombohedral-tetragonal (R-T) phase boundary when x = 0.04, 0.045, 0.05. The specimens with x = 0.04 show improved piezoelectric properties (d33 ~ 440 pC/N, kp ~ 53%, TC ~ 250 °C, d33* ~ 553 pm/V) and good temperature stability. The overall performance is excellent and indicates that (1-x)KNANS-xBNZ ceramics have great potential for replacing their lead-based counterparts.  相似文献   

17.
W/Cr co-doped Aurivillius-type CaBi2Nb2-x(W2/3Cr1/3)xO9 (CBN) (x?=?0.025, 0.050, 0.075, 0.100, and 0.150) piezoelectric ceramics were prepared by the conventional solid-state reaction method. The crystal structure, microstructure, dielectric properties, piezoelectric properties, and electrical conductivity of these ceramics were systematically investigated. After optimum W/Cr modification, the CBN ceramics showed both high d33 and TC. The ceramic with x?=?0.1 showed a remarkably high d33 value of ~15 pC/N along with a high TC of ~931?°C. Moreover, the ceramic also showed excellent thermal stability evident from the increase in its planar electromechanical coupling factor kp from 8.14% at room temperature to 11.04% at 600?°C. After annealing at 900?°C for 2?h, the ceramic showed a d33 value of 14?pC/N. Furthermore, at 600?°C, the ceramic also showed a relatively high resistivity of 4.9?×?105 Ω?cm and a low tanδ of 9%. The results demonstrated the potential of the W/Cr co-doped CBN ceramics for high-temperature applications. We also elucidated the mechanism for the enhanced electrical properties of the ceramics.  相似文献   

18.
The bismuth layer-structured Na0.5Bi4.5-xPrxTi4O15 (x?=?0, 0.1, 0.2, 0.3, 0.4, and 0.5) (NBT-xPr3+) ceramics were fabricated using the traditional solid reaction process. The effect of different Pr3+ contents on dielectric, ferroelectric and piezoelectric properties of Na0.5Bi4.5Ti4O15 ceramics were investigated. The grain size of Pr3+-doping ceramics was found to be smaller than that of pure one, the maximum dielectric constant and Curie temperature Tc gradually decreased with increasing Pr3+ contents, and the dielectric loss decreased at high temperature by Pr3+-doping. Moreover, the activation energy (Ea), resistivity (Z’), remanent polarization (2Pr) and piezoelectric constant (d33) increased by Pr3+-doping. The NBT-xPr3+ ceramics with x?=?0.3 achieved the optimal properties with the maximum dielectric constant of 1109.18, minimum loss of 0.00822 (250?kHz), Ea of 1.122?eV, Z’ of 7.9?kΩ?cm (725 ºC), d33 of 18 pC/N, 2Pr of 12.04 μC/cm2. The enhancement was due to the addition of Pr3+ which suppressed the decreasing of resistivity at high temperature and made it possible for NBT-xPr3+ ceramics to be poled in perpendicular direction, implying that it is a great improvement for Na0.5Bi4.5Ti4O15 ceramics in electrical properties.  相似文献   

19.
Lead-free (Ba0.85Ca0.15)(Ti1−xZrx)O3 (BCTZ) piezoelectric ceramics were fabricated by normal sintering in air atmosphere. BCTZ ceramics with x = 0.10 possess a coexistence of tetragonal and rhombohedral phases at ∼40 °C. The Curie temperature of BCTZ ceramics decreases with increasing the Zr content. Piezoelectric properties of BCTZ ceramics are dependent on the poling conditions (i.e., the poling temperature and the poling electric field), and the underlying physical mechanism is illuminated by the phase angle. The BCTZ (x = 0.10) ceramic, which locates at the existence of two phases and is poled at E ∼ 4.0 kV/mm and Tp ∼ 40 °C, exhibits an optimum electrical behavior at a room temperature of ∼20 °C: d33 ∼ 423 pC/N, kp ∼ 51.2%, 2Pr ∼ 18.86 μC/cm2, 2Ec ∼ 0.47 kV/mm, ?r ∼ 2892, and tan δ ∼ 1.53%.  相似文献   

20.
Ferroelectric and piezoelectric properties of BaTiO3 and Al-doped BaTiO3 ceramics were investigated. The ferroelectric study demonstrated that, by doping Al3+ ions in the A-site of BaTiO3, the polarization–electric field loop exhibited enhanced remnant polarization (from 12 to 17.5  μC/cm2), saturation and switching. In addition, the piezoelectric constant (d33) increased with Al-doping for both static and dynamic strain values (from 75 to 135 and from 29.2 to 57.9 pC/N, respectively, at a maximum applied electric field of 16 kV/cm). Furthermore, the dielectric constant values increased and both the dielectric loss factor and leakage current decreased, even though the transition temperature shifted to lower temperature (from 121 to 113 °C) for the Al-doped sample. Therefore, the Al-doped BaTiO3 has adjustable piezoelectric and ferroelectric properties.  相似文献   

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