Relaxor lead-based textured ceramic material with low texturing temperature and high electrical properties, and preparation method and application thereof

Abstract

Relaxation lead-based textured ceramic material with low texture temperature and high electrical performance, preparation method and application thereof relates to relaxation lead-based textured ceramic material and preparation method and application thereof. The problem of high texture temperature of low Zr content ceramic, orientation grain presenting core-shell structure, high Zr content ceramic being difficult to be textured with high quality, leading to high voltage electrical performance and low texture temperature of ceramic being unable to be acquired simultaneously is solved. Chemical formula (1-x-y) Pb (A, Nb) O3-x Pb Zr O3-y Pb Ti O3 is prepared at 850 DEG C-1095 DEG C, the texture Zr content can reach more than 50%, along [001] c The orientation degree is greater than 96%, the grain misplacement degree is less than 0.20, there is no core-shell structure, the Curie temperature is greater than or equal to 200 DEG C, the quasi-static piezoelectric coefficient is greater than 1000 pC / N, and the electromechanical coupling coefficient is greater than 0.85. The method comprises the following steps: preparing a mother body fine powder, preparing a ceramic green body by flow casting and stacking and pressing, and preparing a textured ceramic. The method is used in a multilayer piezoelectric device.

Description

Technical Field

[0001] This invention relates to relaxable lead-based textured ceramic materials, their preparation methods, and applications. Background Technology

[0002] Zirconium-containing relaxor lead-based ferroelectric materials are in high demand in important fields such as medical ultrasound diagnostics, industrial non-destructive testing, deep-sea communications, precision drive control, and energy harvesting due to their outstanding electromechanical conversion properties. Relaxor lead-based ceramics are core materials for many piezoelectric devices, and enhancing their electrical properties is of great significance for promoting the upgrading of related devices and systems. While the piezoelectric properties of ceramics can be improved through methods such as introducing solid solution components, ion substitution, doping modification, and liquid-phase preparation, the piezoelectric properties are often improved at the cost of lowering the Curie temperature due to the symmetric relationship between piezoelectric properties and Curie temperature. This leads to a deterioration in the temperature stability of the material and a shortening of its practical operating temperature range.

[0003] Crystalline texture can leverage the anisotropic properties of grains, potentially significantly improving piezoelectric properties while maintaining the Curie temperature of ceramic materials. For low-zirconium content relaxor lead-based ceramics (1-xy)Pb(A,B)O3-xPbZrO3-yPbTiO3 (x≤0.35, all ternary coefficients are non-zero), related texture studies have been reported. However, the reported high-texture quality ceramics have high sintering temperatures, typically up to 1200℃. This means that expensive, high-temperature-resistant Pd or Pt electrodes are required when preparing multilayer structures, increasing production costs and limiting the expansion of their production and application. Furthermore, in low-zirconium content relaxor lead-based textured ceramics, the template is usually stably present within the textured grains; in other words, these ceramics typically have a core-shell structure. This structure exhibits residual stress near the core-shell interface, which has a clamping effect on polarization reversal, reducing the effective improvement in piezoelectric properties. For the high-zirconium-content relaxor lead-based ceramic (1-xy)Pb(A,B)O3-xPbZrO3-yPbTiO3 (x > 0.35, all coefficients of the ternary composition are not zero) system, it is difficult to prepare ceramics with high texture quality using conventional texturing techniques, which limits the improvement of the electrical properties of this type of system. Specifically, before ceramic texturing, this type of powder will undergo a severe solid-state reaction with the microcrystalline template, causing the template to be unable to complete the task of guiding the directional growth of grains. Therefore, exploring high-quality texturing and low-temperature sintering of Zr-containing relaxor lead-based ferroelectric ceramics, while eliminating the core-shell structure of its textured grains, can not only achieve a significant improvement in electrical properties while maintaining a high Curie temperature, but also significantly broaden the application range of this type of material in devices, and help promote the upgrading of piezoelectric devices and related instrument systems, which has important scientific significance and engineering application value. Summary of the Invention

[0004] The present invention aims to solve the problems of high texture temperature in low Zr content ceramics, the failure of template dissolution during the texture process leading to a core-shell structure of oriented grains, the difficulty in texturering high Zr content ceramics resulting in limited improvement in electrical properties, and the inability to simultaneously achieve high voltage performance and low texture temperature. The invention provides relaxor lead-based textured ceramic materials with low texture temperature and high electrical performance, as well as their preparation methods and applications.

[0005] Relaxor lead-based textured ceramic materials with low texture temperature and high electrical properties have the general chemical formula (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3, where A is one or a combination of Mg, Zn, Sc and In, 0.15≤x≤0.55, 0.15≤y≤0.55, and 0.10≤1-xy≤0.50;

[0006] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is prepared by combining liquid-phase assisted texturing technology and passivation template texturing technology using fine parent powder or reactive parent powder, template, and growth aid; the template is a sheet-like Ba(Zr) m Ti 1-m O3 microcrystals, 0≤m≤0.1, the volume of the template is a% of the volume of the parent fine powder or the reaction parent fine powder, 0.5≤a≤8.0; the growth aid is one or a mixture of several of PbO, Li-containing growth aid, CuO, Bi2O3, Sm2O3 and Eu2O3, the Li-containing growth aid is Li2CO3 or Li2O, the mass of the growth aid is b% of the mass of the parent fine powder or the reaction parent fine powder, 0.1≤b≤3.0;

[0007] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is prepared under low sintering temperatures of 850℃ to 1095℃, and the Zr content of the texture can be as high as 50% or more.

[001] c The orientation degree is higher than 96%, the grain misalignment r measured by the March-Dollase method is less than 0.20, the elemental distribution in the grain is uniform, there is no core-shell structure, and the Curie temperature T is [missing information]. c ≥200℃, quasi-static piezoelectric coefficient d 33 Above 1000pC / N, the electromechanical coupling coefficient k 33 Higher than 0.85.

[0008] A method for preparing relaxor lead-based textured ceramic materials with low texture temperature and high electrical properties is carried out according to the following steps:

[0009] I. Preparation of fine powder from the parent compound:

[0010] ①Synthesize the A-containing niobate precursor powder by the solid-phase method; the A-containing niobate precursor powder is one or several of MgNb2O6, ZnNb2O6, ScNbO4, and InNbO4. The A-containing niobate precursor powder is a pure phase and fine crystal with a particle size less than 200 nm;

[0011] ②Prepare the matrix fine powder or reactive matrix fine powder according to different values of x:

[0012] When 0.15 ≤ x ≤ 0.35, weigh the Pb source powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder according to the stoichiometric ratio of the chemical formula (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3. Use absolute ethanol as the medium for ball milling and drying, and then pre-burn for 1 h to 6 h under the condition of a temperature of 600 °C to 900 °C, and finally perform secondary ball milling and drying to obtain the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder; the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder is a pure perovskite phase and fine crystal with a particle size less than 300 nm, where 0.15 ≤ y ≤ 0.55 and 0.10 ≤ 1 - x - y ≤ 0.50; the Pb source powder is PbO, Pb3O4, or basic lead carbonate;

[0013] When 0.35 < x ≤ 0.55, weigh the Pb source powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder according to the stoichiometric ratio of the chemical formula (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3. Use absolute ethanol as the medium for ball milling and drying, and then pre-burn for 1 h to 6 h under the condition of a temperature of 600 °C to 9,00 °C, and finally perform secondary ball milling and drying to obtain the (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reactive matrix fine powder; the (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reactive matrix fine powder is a pure perovskite phase and fine crystal with a particle size less than 300 nm, where 0.15 ≤ y ≤ 0.55 and 0.10 ≤ 1 - x - y ≤ 0.50; weigh the Pb source powder and ZrO2 powder according to the stoichiometric ratio of PbZrO3, use absolute ethanol as the medium for ball milling and drying, and then pre-burn for 1 h to 6 h under the condition of a temperature of 600 °C to 900 °C, and finally perform secondary ball milling and drying to obtain the PbZrO3 reactive matrix fine powder. The PbZrO3 reactive matrix fine powder is a pure phase and fine crystal with a particle size less than 200 nm; the Pb source powder is PbO, Pb3O4, or basic lead carbonate;

[0014] II. Tape casting, laminating, and pressing to prepare a ceramic green body:

[0015] ①Prepare the tape-casting slurry according to different values of x:

[0016] When 0.15 ≤ x ≤ 0.35, mix (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder, flaky Ba(Zr m Ti 1-m )O3 microcrystals, growth aids, solvents, dispersants, binders and plasticizers, and then evacuate bubbles under vacuum to obtain (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 tape-casting slurry containing template seeds; the volume of the flaky Ba(Zr m Ti 1-m )O3 microcrystals is a% of the volume of the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder, where 0.5 ≤ a ≤ 8.0 and 0 ≤ m ≤ 0.1; the growth aids are one or a mixture of several of PbO, Li-containing growth aids, CuO, Bi2O3, Sm2O3 and Eu2O3, and the mass of the growth aids is b% of the mass of the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder, 0.1 ≤ b ≤ 3.0, and the Li-containing growth aid is Li2CO3 or Li2O;

[0017] When 0.35 < x ≤ 0.55, mix (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder, flaky Ba(Zr m Ti 1-m )O3 microcrystals, growth aids, solvents, dispersants, binders and plasticizers, and then evacuate bubbles under vacuum to obtain (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction tape-casting slurry containing template seeds; mix PbZrO3 reaction matrix fine powder, solvents, dispersants, binders and plasticizers, and then evacuate bubbles under vacuum to obtain PbZrO3 reaction tape-casting slurry without template seeds; the flaky Ba(Zr m Ti 1-m)The volume of the O3 microcrystals is a% of the total volume of the (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 reaction matrix fine powder and the PbZrO3 reaction matrix fine powder, where 0.5 ≤ a ≤ 8.0 and 0 ≤ m ≤ 0.1; the growth aid is one or a mixture of several of PbO, Li-containing growth aids, CuO, Bi2O3, Sm2O3, and Eu2O3, the Li-containing growth aid is Li2CO3 or Li2O, and the mass of the growth aid is b% of the total mass of the (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 reaction matrix fine powder and the PbZrO3 reaction matrix fine powder, 0.1 ≤ b ≤ 3.0;

[0018] ② Tape casting:

[0019] Under the condition of a speed of 0.5 cm / s to 15 cm / s, tape-cast the (1-x-y)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 tape-casting slurry containing the template seed crystal on a tape casting machine, and then dry and cut it to obtain a (1-x-y)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 film sheet containing the template seed crystal;

[0020] Or under the condition of a speed of 0.5 cm / s to 15 cm / s, respectively tape-cast the reaction tape-casting slurry of (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 containing the template seed crystal and the PbZrO3 reaction tape-casting slurry without the template seed crystal on a tape casting machine, and then dry and cut them to obtain a (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 reaction film sheet containing the template seed crystal and a PbZrO3 reaction film sheet without the template seed crystal;

[0021] ③ Stacking according to different values of x:

[0022] When 0.15 ≤ x ≤ 0.35, stack the (1-x-y)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 film sheets containing the template seed crystal to obtain a stacked sample;

[0023] When 0.35 < x ≤ 0.55, stack the (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 reaction film sheets containing the template seed crystal and the PbZrO3 reaction film sheets without the template seed crystal alternately according to the stoichiometric ratio of the chemical formula (1-x-y)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 to obtain a stacked sample;

[0024] ④ Pressurization:

[0025] The stacked samples were hot-pressed and hot-water homogenized to obtain ceramic green bodies;

[0026] III. Preparation of Textured Ceramics:

[0027] ① Debinding and cold isostatic pressing:

[0028] Under conditions of 500℃~700℃, the ceramic green body is debonded for 1h~6h, and then cold isostatically pressed for 1min~10min under a pressure of 150MPa~250MPa to obtain the ceramic green body.

[0029] ②Sintering:

[0030] Textured ceramics are obtained by sintering the ceramic green body for 5 min to 600 min at a low sintering temperature of 850℃ to 1095℃.

[0031] ③Polarization:

[0032] The two surfaces of the textured ceramic perpendicular to the texture direction are polished, cleaned, and dried, and then polarized to obtain a relaxor lead-based textured ceramic material with low texture temperature and high electrical properties.

[0033] Applications: Relaxor lead-based textured ceramic materials with low texture temperature and high electrical properties are used in multilayer piezoelectric devices with high performance, wide temperature range, high power, and high electric field drive. These multilayer piezoelectric devices include high-end ultrasonic transducers, high-end piezoelectric actuators, high-end piezoelectric sensors, and high-end energy harvesters.

[0034] Principle: This invention prepares Zr-containing relaxant lead-based textured ceramic materials with low texture temperature and high electrical performance based on a synergistic strategy of liquid-phase assisted texturing and passivation template texturing. These materials can be applied in next-generation high-performance, wide-temperature-range, high-power, high-electric-field driven multilayer piezoelectric devices. Specifically: ① For a low zirconium content (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 (0.15≤x≤0.35) composition, on the one hand, the added liquid-phase additive accelerates the mass transfer process between the textured grains and the parent material, increasing the growth rate of the textured grains. This significantly improves the textured grain growth rate while lowering the ceramic texture temperature.

[001] cDegree of orientation, the improvement of texture quality effectively enhances the piezoelectric properties of the ceramics. On the other hand, by introducing a suitable liquid-phase additive and combining process regulation, the template seed crystals induce the oriented growth of the matrix while an ion diffusion reaction occurs at the texture mass transfer interface. At the end of the texture process, the template completely dissolves in the texture grains, and the obtained texture grains have a uniform element distribution, without the core-shell structure caused by traditional texture techniques, eliminating the clamping effect of the template in the core-shell structure on the polarization reversal of the texture grains, and further promoting the effective improvement of piezoelectric properties. With the joint contribution of these two aspects, a Zr-containing relaxor lead-based textured ceramic material with a low texture temperature and high electrical properties is obtained. ② For the composition with a high zirconium content (1-x-y)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 (0.35 < x ≤ 0.55), the present invention adopts a multi-layer structure design that can passivate the template, enabling the template seed crystals to first grow along

[001] in the matrix with a low zirconium content (1-x-y)Pb(A,Nb)O3-0.35PbZrO3-yPbTiO3 c to induce the oriented growth of grains, avoiding the destruction of the template at high Zr contents. When the template grows into large, sufficiently stable textured grains, it then guides the matrix with a high Zr content to grow along

[001] c directionally, broadening the textureable Zr content x to more than 50%. At the same time, the present invention combines the liquid-phase assisted texture technique and process regulation, reducing the ceramic texture temperature and enabling the dissolution of the template. With the above synergistic effects, a significantly improved piezoelectric property and a low texture temperature are obtained.

[0035] Advantages of the present invention:

[0036] The present invention solves the problems that the current low-Zr content ceramics have a high texture temperature, and the template does not dissolve during the texture process, resulting in a core-shell structure in the oriented grains, and the high-Zr content ceramics are difficult to texture, leading to the inability to significantly improve the electrical properties, and the problem that high piezoelectric properties and low texture temperature cannot be obtained simultaneously. Based on the synergistic strategy of liquid-phase assisted texture and template passivation texture, the developed lead-based textured ceramic materials can be prepared at low temperatures (850 °C to 1095 °C), the textureable Zr content x can reach more than 50% (0.15 ≤ x ≤ 0.55), and the textured ceramics prepared under such low temperatures have an orientation degree higher than 96% along

[001] c , a grain misorientation degree r lower than 0.20, a uniform element distribution in the texture grains, no grain core-shell structure caused by traditional texture techniques, a Curie temperature T c ≥ 200 °C, a quasi-static piezoelectric coefficient d 33 higher than 1,000 pC / N, and an electromechanical coupling coefficient k 33The piezoelectric value is above 0.85. This material simultaneously exhibits high piezoelectric properties, a wide operating temperature range, and a low texture temperature, significantly outperforming current reports on this type of piezoelectric ceramic material. Furthermore, the preparation process of this invention is simple and efficient, significantly reducing environmental pollution and production costs. This invention provides a design and fabrication approach for developing Zr-containing lead-based textured ceramics with low sintering temperatures and high piezoelectric properties. It also provides novel high-performance piezoelectric materials for developing next-generation high-end multilayer piezoelectric devices such as high-performance ultrasonic transducers, piezoelectric actuators, piezoelectric sensors, and energy harvesters, and is expected to help promote the upgrading of related piezoelectric devices and instrument systems. Attached Figure Description

[0037] Figure 1 The XRD pattern of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1;

[0038] Figure 2 The EBSD inverse pole figure of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1;

[0039] Figure 3 Backscattered SEM image of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1;

[0040] Figure 4 The electrical properties of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1 are shown in the figure.

[0041] Figure 5 The XRD pattern of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 2;

[0042] Figure 6 The electrical properties diagram shows the relaxed lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 2. Detailed Implementation

[0043] The technical solution of the present invention is not limited to the specific embodiments listed below, but also includes any combination of the specific embodiments.

[0044] Specific Implementation Method 1: This implementation method features a relaxor lead-based textured ceramic material with low texture temperature and high electrical performance. Its general chemical formula is (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3, where A is one or a combination of several of Mg, Zn, Sc and In, 0.15≤x≤0.55, 0.15≤y≤0.55, and 0.10≤1-xy≤0.50;

[0045] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is prepared by combining liquid-phase assisted texturing technology and passivation template texturing technology using fine parent powder or reactive parent powder, template, and growth aid; the template is a sheet-like Ba(Zr) m Ti 1-m O3 microcrystals, 0≤m≤0.1, the volume of the template is a% of the volume of the parent fine powder or the reaction parent fine powder, 0.5≤a≤8.0; the growth aid is one or a mixture of several of PbO, Li-containing growth aid, CuO, Bi2O3, Sm2O3 and Eu2O3, the Li-containing growth aid is Li2CO3 or Li2O, the mass of the growth aid is b% of the mass of the parent fine powder or the reaction parent fine powder, 0.1≤b≤3.0;

[0046] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is prepared under low sintering temperatures of 850℃ to 1095℃, and the Zr content of the texture can be as high as 50% or more.

[001] c The orientation degree is higher than 96%, the grain misalignment r measured by the March-Dollase method is less than 0.20, the elemental distribution in the grain is uniform, there is no core-shell structure, and the Curie temperature T is [missing information]. c ≥200℃, quasi-static piezoelectric coefficient d 33 Above 1000pC / N, the electromechanical coupling coefficient k 33 Higher than 0.85.

[0047] The beneficial effects of this specific implementation method are:

[0048] This specific embodiment solves the problems of high texturing temperature for low-Zr-content ceramics, the inability of the template to dissolve during texturing resulting in a core-shell structure for oriented grains, the difficulty in texturing high-Zr-content ceramics leading to limited improvement in electrical properties, and the inability to simultaneously achieve high voltage performance and low texturing temperature. Based on a synergistic strategy of liquid-phase assisted texturing and template passivation texturing, the developed lead-based textured ceramic material can be prepared at low temperatures (850℃~1095℃), with a texturing Zr content x reaching over 50% (0.15≤x≤0.55), and the textured ceramic prepared under these low-temperature conditions along

[001] c Orientation degree higher than 96%, grain misalignment r less than 0.20, uniform element distribution within the textured grains, absence of core-shell structure caused by traditional texturing techniques, Curie temperature T c ≥200℃, quasi-static piezoelectric coefficient d 33 Above 1000pC / N, the electromechanical coupling coefficient k 33Higher than 0.85. This material simultaneously has high piezoelectric performance, a wide operating temperature range, and a low texture temperature, significantly superior to the reported levels of current research on this type of piezoelectric ceramic material. In addition, the preparation process of this specific embodiment is simple and efficient, which can significantly reduce environmental pollution and lower production costs. This specific embodiment provides a design and preparation idea for developing Zr-containing lead-based textured ceramics with low sintering temperature and high piezoelectric performance, and provides new high-performance piezoelectric materials for developing a new generation of high-end multilayer piezoelectric devices such as high-performance ultrasonic transducers, piezoelectric drivers, piezoelectric sensors, and energy harvesters, etc., and is expected to assist in promoting the upgrading of related piezoelectric devices and instrument systems.

[0049] Specific Embodiment Ⅱ: The difference between this embodiment and Specific Embodiment Ⅰ is that: A is Mg, Zn, Sc or In. Others are the same as Specific Embodiment Ⅰ.

[0050] Specific Embodiment Ⅲ: The difference between this embodiment and one of Specific Embodiment Ⅰ or Ⅱ is that: 0 < m ≤ 0.1. Others are the same as Specific Embodiment Ⅰ or Ⅱ.

[0051] Specific Embodiment Ⅳ: A preparation method of a relaxor lead-based textured ceramic material with low texture temperature and high electrical properties, which is completed according to the following steps:

[0052] Ⅰ. Preparation of matrix fine powder:

[0053] ① Synthesize A-niobate precursor powder by solid-phase method; the A-niobate precursor powder is one or several of MgNb2O6, ZnNb2O6, ScNbO4 and InNbO4, and the A-niobate precursor powder is a pure phase and fine crystal with a particle size less than 200 nm;

[0054] ② Prepare matrix fine powder or reactive matrix fine powder respectively according to different values of x:

[0055] When 0.15 ≤ x ≤ 0.35, weigh Pb source powder, A-niobate precursor powder, ZrO2 powder and TiO2 powder according to the stoichiometric ratio of the chemical general formula (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3, ball mill with absolute ethanol as the medium and dry, then pre-burn for 1 h - 6 h at a temperature of 600 °C - 900 °C, and finally ball mill twice and dry to obtain (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder; the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 matrix fine powder is a pure perovskite phase and fine crystal with a particle size less than 300 nm, where 0.15 ≤ y ≤ 0.55, and 0.10 ≤ 1 - x - y ≤ 0.50; the Pb source powder is PbO, Pb3O4 or basic lead carbonate;

[0056] When 0.35 < x ≤ 0.55, weigh the Pb source powder, A-niobate-containing precursor powder, ZrO2 powder and TiO2 powder according to the stoichiometric ratio of the chemical formula (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3, ball-mill them with absolute ethanol as the medium and then dry them. Then, pre-calcine them for 1 h to 6 h under the condition of a temperature of 600°C to 900°C, and finally ball-mill them twice and dry them to obtain the fine powder of the (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix; the fine powder of the (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix is a pure perovskite phase and fine crystal with a particle size less than 300 nm, where 0.15 ≤ y ≤ 0.55 and 0.10 ≤ 1 - x - y ≤ 0.50; weigh the Pb source powder and ZrO2 powder according to the stoichiometric ratio of PbZrO3, ball-mill them with absolute ethanol as the medium and then dry them. Then, pre-calcine them for 1 h to 6 h under the condition of a temperature of 600°C to 900°C, and finally ball-mill them twice and dry them to obtain the fine powder of the PbZrO3 reaction matrix. The fine powder of the PbZrO3 reaction matrix is a pure phase and fine crystal with a particle size less than 200 nm; the Pb source powder is PbO, Pb3O4 or basic lead carbonate;

[0057] II. Preparing a ceramic green body by tape casting and laminating and pressing:

[0058] ① Prepare tape-casting slurries according to different values of x:

[0059] When 0.15 ≤ x ≤ 0.35, mix the fine powder of (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3, flaky Ba(Zr<00,000,32>Ti<00,000,33>)O3 microcrystals, growth aids, solvents, dispersants, binders and plasticizers, and then evacuate the bubbles under vacuum to obtain the tape-casting slurry of (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 containing template seeds; the volume of the flaky Ba(Zr<00,​​​

[0060] When 0.35 < x ≤ 0.55, (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder, flaky Ba(Zr m Ti 1-m )O3 microcrystals, growth aids, solvents, dispersants, binders and plasticizers are mixed, and then vacuum degassed to obtain a reaction tape-casting slurry of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 containing template seeds; PbZrO3 reaction matrix fine powder, solvents, dispersants, binders and plasticizers are mixed, and then vacuum degassed to obtain a PbZrO3 reaction tape-casting slurry without template seeds; the volume of the flaky Ba(Zr m Ti 1-m )O3 microcrystals is a% of the total volume of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder and PbZrO3 reaction matrix fine powder, where 0.5 ≤ a ≤ 8.0, 0 ≤ m ≤ 0.1; the growth aids are one or a mixture of several of PbO, Li-containing growth aids, CuO, Bi2O3, Sm2O3 and Eu2O3, the Li-containing growth aid is Li2CO3 or Li2O, and the mass of the growth aid is b% of the total mass of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder and PbZrO3 reaction matrix fine powder, 0.1 ≤ b ≤ 3.0;

[0061] ② Tape-casting:

[0062] Under the condition of a speed of 0.5 cm / s to 15 cm / s, the (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 tape-casting slurry containing template seeds is tape-cast on a tape-casting machine, and then dried and cut to obtain a (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 film sheet containing template seeds;

[0063] Or under the condition of a speed of 0.5 cm / s to 15 cm / s, the reaction tape-casting slurry of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 containing template seeds and the PbZrO3 reaction tape-casting slurry without template seeds are respectively tape-cast on a tape-casting machine, and then dried and cut to obtain a (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction film sheet containing template seeds and a PbZrO3 reaction film sheet without template seeds;

[0064] ③ Stacking according to different values of x:

[0065] When 0.15 ≤ x ≤ 0.35, laminate (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 film pieces containing template seeds to obtain a stacked sample;

[0066] When 0.35 < x ≤ 0.55, stack (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction film pieces containing template seeds and PbZrO3 reaction film pieces without template seeds alternately according to the stoichiometric ratio of the chemical general formula (1 - x - y)Pb(A,Nb)O3 - xPbZrO3 - yPbTiO3 to obtain a stacked sample;

[0067] ④ Pressurization:

[0068] Subject the stacked sample to hot pressing and hot water isostatic pressing to obtain a green ceramic body;

[0069] III. Preparation of textured ceramics:

[0070] ① Debinding and cold isostatic pressing:

[0071] Debind the green ceramic body for 1 h - 6 h at a temperature of 500 °C - 700 °C, and then perform cold isostatic pressing for 1 min - 10 min under a pressure of 150 MPa - 250 MPa to obtain a ceramic preform;

[0072] ② Sintering:

[0073] Sinter the ceramic preform for 5 min - 600 min at a low sintering temperature of 850 °C - 1095 °C to obtain textured ceramics;

[0074] ③ Poling:

[0075] Grind, clean, and dry the two surfaces of the textured ceramics perpendicular to the texture direction, and then perform electrode poling and poling to obtain a relaxor - based textured ceramic material with a low texture temperature and high electrical properties.

[0076] Specific Embodiment 5: The difference between this embodiment and Specific Embodiment 4 is that in step ①②, ball milling is performed for 24 h - 96 h with absolute ethanol as the medium. Others are the same as Specific Embodiment 4.

[0077] Specific Embodiment 6: The difference between this embodiment and one of Specific Embodiments 4 or 5 is that the secondary ball milling time described in step ①② is 12 h - 72 h. Others are the same as Specific Embodiment 4 or 5.

[0078] Specific Implementation Method Seven: This implementation method differs from Specific Implementation Methods Four to Six in that: the solvent mentioned in step two ① is a mixed solution of xylene and ethanol; the dispersant mentioned in step two ① is melted herring oil; the binder mentioned in step two ① is polyvinyl butyral; and the plasticizer mentioned in step two ① is a mixture of polyalkylene glycol and butyl benzyl phthalate. Everything else is the same as in Specific Implementation Methods Four to Six.

[0079] Specific Implementation Method Eight: This implementation method differs from Specific Implementation Methods Four to Seven in that: the hot pressing described in step two, fourth, is specifically carried out under conditions of 10MPa to 50MPa pressure and 60℃ to 95℃ for 5 to 30 minutes; the hot water uniform pressing described in step two, fourth, is specifically carried out under conditions of 20MPa to 50MPa pressure and 70℃ to 95℃ for 20 to 60 minutes. Everything else is the same as in Specific Implementation Methods Four to Seven.

[0080] Specific Implementation Method Nine: This implementation method differs from Specific Implementation Methods Four to Eight in that: the polarization described in step three ③ specifically involves applying silver paste to the polished surface and then burning the electrode at a temperature of 450℃ to 650℃ for 30 to 90 minutes; the polarization described in step three ③ is specifically performed under a DC or AC electric field of 10kV / cm to 60kV / cm. Everything else is the same as in Specific Implementation Methods Four to Eight.

[0081] Specific Implementation Method 10: This implementation method utilizes a relaxor lead-based textured ceramic material with low texture temperature and high electrical performance. It is applied to multilayer piezoelectric devices with high performance, wide temperature range, high power, and high electric field drive. The multilayer piezoelectric devices include high-end ultrasonic transducers, high-end piezoelectric actuators, high-end piezoelectric sensors, and high-end energy harvesters.

[0082] The beneficial effects of the present invention are verified by the following embodiments:

[0083] Example 1:

[0084] A method for preparing relaxor lead-based textured ceramic materials with low texture temperature and high electrical properties is carried out according to the following steps:

[0085] I. Preparation of fine powder from the parent compound:

[0086] ① A-containing niobate precursor powder is synthesized by solid-state method; the A-containing niobate precursor powder is MgNb2O6, and the A-containing niobate precursor powder is pure phase and fine crystal with a particle size of less than 200nm;

[0087] ②Preparation of fine powder from the parent compound:

[0088] According to the chemical formula 0.42Pb(Mg) 1 / 3 Nb2 / 3 The stoichiometric ratio of Pb-0.25PbZrO3-0.33PbTiO3 was determined by weighing Pb source powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder. The powder was ball-milled and dried using anhydrous ethanol as the medium, then pre-calcined at 700℃ for 1 hour, and finally ball-milled and dried again to obtain 0.42Pb(MgO)O3. 1 / 3 Nb 2 / 3 O3-0.25PbZrO3-0.33PbTiO3 matrix fine powder; the aforementioned 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The fine powder of the parent material, O3-0.25PbZrO3-0.33PbTiO3, is a pure perovskite phase with fine crystals and a particle size of less than 300nm; the Pb source powder is PbO.

[0089] II. Preparation of ceramic green bodies by tape casting and pressure bonding:

[0090] ①Preparation of casting slurry:

[0091] 0.42Pb(Mg) 1 / 3 Nb 2 / 3 O3-0.25PbZrO3-0.33PbTiO3 parent fine powder, flake-like Ba(Zr) m Ti 1-m O3 microcrystals, growth aids, solvents, dispersants, binders, and plasticizers were mixed, and then vacuum-bubbled to obtain 0.42Pb(Mg) containing template seed crystals. 1 / 3 Nb 2 / 3 Ba(ZrO3)-0.25PbZrO3-0.33PbTiO3 casting slurry; the flake-shaped Ba(ZrO3) m Ti 1-m The volume of O3 microcrystals is 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The growth aid is a% of the volume of the fine powder of parent material O3-0.25PbZrO3-0.33PbTiO3, where a = 5 and m = 0; the growth aid is a mixture of Li2CO3 and PbO, and the mass of Li2CO3 is 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The fine powder of the parent compound is 0.2% of the mass of O3-0.25PbZrO3-0.33PbTiO3, and the mass of PbO is 0.42Pb(Mg) 1 / 3 Nb 2 / 3 )O3-0.25PbZrO3-0.33PbTiO3 parent fine powder 1% of the mass;

[0092] ②Casting:

[0093] At a speed of 1.5 cm / s, 0.42Pb(Mg)2 containing template seed crystals was processed on a casting machine. 1 / 3 Nb 2 / 3 The O3-0.25PbZrO3-0.33PbTiO3 casting slurry was cast, then dried and cut to obtain 0.42Pb(MgO) containing template seed crystals. 1 / 3Nb 2 / 3 O3-0.25PbZrO3-0.33PbTiO3 film;

[0094] ③Layering:

[0095] 0.42Pb(Mg) containing template seed crystals 1 / 3 Nb 2 / 3 The O3-0.25PbZrO3-0.33PbTiO3 films were stacked to obtain the stacked sample;

[0096] ④ Pressurization:

[0097] The stacked samples were hot-pressed and hot-water homogenized to obtain ceramic green bodies;

[0098] III. Preparation of Textured Ceramics:

[0099] ① Debinding and cold isostatic pressing:

[0100] The ceramic green body was debonded at 600℃ for 2 hours, and then cold isostatically pressed at 200MPa for 2 minutes to obtain the ceramic green body.

[0101] ②Sintering:

[0102] The ceramic blank was sintered for 360 min at a low sintering temperature of 1075℃ to obtain textured ceramic.

[0103] ③Polarization:

[0104] The two surfaces of the textured ceramic perpendicular to the texture direction are polished, cleaned, and dried, and then polarized to obtain a relaxor lead-based textured ceramic material with low texture temperature and high electrical properties.

[0105] The A-containing niobate precursor powder mentioned in step 1① is prepared according to the following steps: MgO and Nb2O5 are weighed according to the stoichiometric ratio of MgNb2O6, and then kept at 900℃ for 2 hours to obtain MgNb2O6.

[0106] In step 1②, ball milling was performed for 36 hours using anhydrous ethanol as the medium.

[0107] The secondary ball milling time mentioned in step 1② is 48 hours.

[0108] The solvent mentioned in step 2① is a mixed solution of xylene and ethanol, and the mass ratio of xylene to ethanol is 1:1; the dispersant mentioned in step 2① is molten herring oil; the binder mentioned in step 2① is polyvinyl butyral; the plasticizer mentioned in step 2① is a mixture of polyalkylene glycol and butyl benzyl phthalate, and the mass ratio of polyalkylene glycol to butyl benzyl phthalate is 1:1; the 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of fine powder of O3-0.25PbZrO3-0.33PbTiO3 matrix to solvent is 1:0.45; the 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of fine powder of O3-0.25PbZrO3-0.33PbTiO3 matrix to dispersant is 1:0.016; the 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of fine powder of O3-0.25PbZrO3-0.33PbTiO3 matrix to binder is 1:0.038; the 0.42Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of fine powder of O3-0.25PbZrO3-0.33PbTiO3 matrix to plasticizer is 1:0.04.

[0109] The hot pressing mentioned in step 2④ specifically refers to hot pressing for 10 minutes under a pressure of 20MPa and a temperature of 70℃; the hot water uniform pressing mentioned in step 2④ specifically refers to hot water uniform pressing for 30 minutes under a pressure of 20MPa and a temperature of 75℃.

[0110] The polarization described in step 3③ specifically involves applying silver paste to the polished surface and then burning the electrode at a temperature of 550℃ for 60 minutes; the polarization described in step 3③ specifically involves performing the polarization under a DC electric field of 30kV / cm.

[0111] The relaxor lead-based textured ceramic material prepared above, exhibiting low texture temperature and high electrical properties, has the chemical formula 0.42Pb(Mg) 1 / 3 Nb 2 / 3 O3-0.25PbZrO3-0.33PbTiO3;

[0112] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties was prepared at a low-temperature sintering temperature of 1075℃, and the Zr content of the texture was 25%, i.e., x = 0.25, along

[001] c The orientation degree is 99%, the grain misalignment degree r = 0.15 measured by the March-Dollase method, the elemental distribution in the grain is uniform, there is no core-shell structure, and the Curie temperature T is [missing information]. c=203℃, quasi-static piezoelectric coefficient d 33 The electromechanical coupling coefficient is 1250 pC / N. 33 It is 0.92.

[0113] Figure 1 The image shows the XRD pattern of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1. As can be seen from the image, the textured ceramic exhibits a pure perovskite phase structure at a sintering temperature of 1075℃, and almost only the (001) peak is detected, indicating that the ceramic grains are arranged along

[001] . c High orientation, its orientation degree Lotgering factor F 001 Up to 99%.

[0114] Figure 2 This is the EBSD inverse pole figure of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1. The ceramic grains are along

[001] . c It has a high degree of orientation, with few misplaced and micro-misplaced grains. The grain misplacement degree r = 0.15 was measured using the March-Dollase method.

[0115] Figure 3 This is a backscattered SEM image of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1. The textured grains have a uniform composition and no core-shell structure is observed.

[0116] Figure 4 The image shows the electrical properties of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 1. The piezoelectric coefficient d of this material is shown. 33 The electromechanical coupling coefficient is 1250 pC / N. 33 It is 0.92.

[0117] Example 2:

[0118] A method for preparing relaxor lead-based textured ceramic materials with low texture temperature and high electrical properties is carried out according to the following steps:

[0119] I. Preparation of fine powder from the parent compound:

[0120] ① A-containing niobate precursor powder is synthesized by solid-state method; the A-containing niobate precursor powder is MgNb2O6, and the A-containing niobate precursor powder is pure phase and fine crystal with a particle size of less than 200nm;

[0121] ②Preparation of fine powder of reaction precursor:

[0122] According to the chemical formula 0.275Pb(Mg) 1 / 3 Nb 2 / 3The stoichiometric ratio of Pb-based powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder was determined by weighing Pb source powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder. The powder was ball-milled and dried using anhydrous ethanol as the medium, then pre-calcined at 725℃ for 2 hours, and finally ball-milled and dried again to obtain 0.275Pb(MgO)2. 1 / 3 Nb 2 / 3 O3-0.35PbZrO3-0.365PbTiO3 reaction matrix fine powder; the 0.275Pb(Mg) 1 / 3 Nb 2 / 3 The PbZrO3-0.35PbZrO3-0.365PbTiO3 reaction matrix fine powder is a pure perovskite phase with fine crystals and a particle size of less than 300 nm. Pb source powder and ZrO2 powder are weighed according to the stoichiometric ratio of PbZrO3, ball-milled and dried using anhydrous ethanol as the medium, then pre-calcined at 800℃ for 3 hours, and finally ball-milled and dried again to obtain the PbZrO3 reaction matrix fine powder. The PbZrO3 reaction matrix fine powder is a pure phase with fine crystals and a particle size of less than 200 nm. The Pb source powder is PbO.

[0123] II. Preparation of ceramic green bodies by tape casting and pressure bonding:

[0124] ①Preparation of casting slurry:

[0125] 0.275Pb(Mg) 1 / 3 Nb 2 / 3 O3-0.35PbZrO3-0.365PbTiO3 reaction parent material fine powder, flake Ba(Zr) m Ti 1-m O3 microcrystals, growth aids, solvents, dispersants, binders, and plasticizers were mixed, and then vacuum-bubbled to obtain 0.275Pb(Mg) containing template seed crystals. 1 / 3 Nb 2 / 3 A reactive casting slurry of PbZrO3-0.35PbZrO3-0.365PbTiO3 was prepared by mixing fine powder of PbZrO3 reactive matrix, solvent, dispersant, binder and plasticizer, followed by vacuum degassing to obtain a PbZrO3 reactive casting slurry without template seed crystals; the sheet-like Ba(ZrO3)3... m Ti 1-m The volume of O3 microcrystals is 0.275Pb(Mg) 1 / 3 Nb 2 / 3 The growth aid is a% of the total volume of the fine powder of PbTiO3-0.35PbZrO3-0.365PbTiO3 reaction matrix and the fine powder of PbZrO3 reaction matrix, where a = 3 and m = 0.1; the growth aid is a mixture of Li2CO3 and CuO, and the mass of Li2CO3 is 0.275Pb(Mg) 1 / 3Nb 2 / 3 The total mass of the fine powder of reactant parent material (0.08%) is 0.35PbZrO3-0.365PbTiO3 and the fine powder of reactant parent material (0.275Pb(Mg)O), and the mass of CuO is 0.275Pb(Mg)O. 1 / 3 Nb 2 / 3 The total mass of the fine powder of the reaction parent material of O3-0.35PbZrO3-0.365PbTiO3 and the fine powder of the reaction parent material of PbZrO3 is 0.4%.

[0126] ②Casting:

[0127] At a speed of 2 cm / s, 0.275Pb(Mg) oxide sheets containing template seed crystals were processed on a casting machine. 1 / 3 Nb 2 / 3 The reaction casting slurry of O3-0.35PbZrO3-0.365PbTiO3 and the reaction casting slurry of PbZrO3 without template seed crystals were cast, then dried and cut to obtain 0.275Pb(MgO) containing template seed crystals. 1 / 3 Nb 2 / 3 PbZrO3-0.35PbZrO3-0.365PbTiO3 reactive films and PbZrO3 reactive films without template seed crystals;

[0128] ③Layering:

[0129] According to the general chemical formula 0.275Pb(Mg) 1 / 3 Nb 2 / 3 The stoichiometric ratio of O3-0.36PbZrO3-0.365PbTiO3 will be used to prepare 0.275Pb(Mg) containing template seed crystals. 1 / 3 Nb 2 / 3 The O3-0.35PbZrO3-0.365PbTiO3 reactive film and the PbZrO3 reactive film without template seed crystal were alternately stacked to obtain the stacked sample;

[0130] ④ Pressurization:

[0131] The stacked samples were hot-pressed and hot-water homogenized to obtain ceramic green bodies;

[0132] III. Preparation of Textured Ceramics:

[0133] ① Debinding and cold isostatic pressing:

[0134] The ceramic green body was debonded at 600℃ for 2 hours, and then cold isostatically pressed at 200MPa for 3 minutes to obtain the ceramic green body.

[0135] ②Sintering:

[0136] The ceramic green body was sintered for 600 min at a low sintering temperature of 1075℃ to obtain textured ceramic.

[0137] ③Polarization:

[0138] The two surfaces of the textured ceramic perpendicular to the texture direction are polished, cleaned, and dried, and then polarized to obtain a relaxor lead-based textured ceramic material with low texture temperature and high electrical properties.

[0139] The preparation method of the A-containing niobate precursor powder described in step 1① is the same as that in Example 1, and MgNb2O6 is obtained.

[0140] In step 1②, ball milling was performed for 36 hours using anhydrous ethanol as the medium.

[0141] The secondary ball milling time mentioned in step 1② is 48 hours.

[0142] Step 2① contains 0.275Pb(Mg) template seed crystals. 1 / 3 Nb 2 / 3 The solvent, dispersant, binder, and plasticizer are the same in the reaction casting slurry of PbZrO3-0.35PbZrO3-0.365PbTiO3 and the reaction casting slurry of PbZrO3 without template seed crystals; the solvent mentioned in step 2① is a mixed solution of xylene and ethanol, and the mass ratio of xylene to ethanol is 1:1; the dispersant mentioned in step 2① is molten herring oil; the binder mentioned in step 2① is polyvinyl butyral; the plasticizer mentioned in step 2① is a mixture of polyalkylene glycol and butyl benzyl phthalate, and the mass ratio of polyalkylene glycol to butyl benzyl phthalate is 1:1; the 0.275Pb(MgO) containing template seed crystals... 1 / 3 Nb 2 / 3 In the reactive casting slurry of O3-0.35PbZrO3-0.365PbTiO3: the 0.275Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of the parent fine powder to the solvent in the reaction of O3-0.35PbZrO3-0.365PbTiO3 is 1:1.05. The 0.275Pb(Mg) 1 / 3 Nb 2 / 3 The mass ratio of the fine powder of the reaction matrix (0.35PbZrO3-0.365PbTiO3) to the dispersant is 1:0.01. The 0.275Pb(MgO) 1 / 3 Nb 2 / 3 The mass ratio of the reactant fine powder (0.35PbZrO3-0.365PbTiO3) to the binder is 1:0.04. The 0.275Pb(MgO) 1 / 3 Nb 2 / 3The mass ratio of PbZrO3-0.35PbZrO3-0.365PbTiO3 reaction matrix powder to plasticizer is 1:0.05; in the PbZrO3 reaction casting slurry without template seed crystals: the mass ratio of PbZrO3 reaction matrix powder to solvent is 1:1.05, the mass ratio of PbZrO3 reaction matrix powder to dispersant is 1:0.01, the mass ratio of PbZrO3 reaction matrix powder to binder is 1:0.04, and the mass ratio of the total mass of PbZrO3 reaction matrix powder to plasticizer is 1:0.05.

[0143] The hot pressing mentioned in step 2④ specifically refers to hot pressing for 10 minutes under a pressure of 20MPa and a temperature of 75℃; the hot water uniform pressing mentioned in step 2④ specifically refers to hot water uniform pressing for 30 minutes under a pressure of 20MPa and a temperature of 75℃.

[0144] The polarization described in step 3③ specifically involves applying silver paste to the polished surface and then burning the electrode at a temperature of 550℃ for 60 minutes; the polarization described in step 3③ specifically involves performing the polarization under a DC electric field of 30kV / cm.

[0145] The relaxor lead-based textured ceramic material prepared above, exhibiting low texture temperature and high electrical properties, has the chemical formula 0.275Pb(Mg) 1 / 3 Nb 2 / 3 O3-0.36PbZrO3-0.365PbTiO3;

[0146] The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties was prepared at a low-temperature sintering temperature of 1075℃, and the Zr content of the texture was 36%, i.e., x = 0.36, along

[001] c The orientation degree is 98%, the grain misalignment degree r = 0.19 measured by the March-Dollase method, the elemental distribution in the grain is uniform, there is no core-shell structure, and the Curie temperature T is [missing information]. c =260℃, quasi-static piezoelectric coefficient d 33 The electromechanical coupling coefficient is 1040 pC / N. 33 It is 0.89.

[0147] Figure 5 The image shows the XRD pattern of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 2. As can be seen from the image, this textured ceramic exhibits

[001] ... c The high texture, its orientation degree Lotgering factor F 001 Up to 98%.

[0148] Figure 6This is an electrical property diagram of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties prepared in Example 2. The piezoelectric coefficient d of this material is shown. 33 The electromechanical coupling coefficient is 1040 pC / N. 33 It is 0.89.

Claims

1. A relaxor lead-based textured ceramic material with low texture temperature and high electrical properties, characterized in that... Its general chemical formula is (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3, where A is one or a combination of several of Mg, Zn, Sc and In, 0.15≤x≤0.55, 0.15≤y≤0.55, and 0.10≤1-xy≤0.50; The relaxor-based textured ceramic material with low texturing temperature and high electrical properties is prepared by combining the liquid-phase assisted texturing technique and the passivated template texturing technique using matrix fine powder or reactive matrix fine powder, template, and growth aids; the template is flaky Ba(Zr m Ti 1-m )O3 microcrystals, 0 ≤ m ≤ 0.1, and the volume of the template is a % of the volume of the matrix fine powder or reactive matrix fine powder, 3.0 ≤ a ≤ 5.0; when 0.15 ≤ x ≤ 0.35, the growth aid is a mixture of Li2CO3 and PbO, and the mass of the growth aid is b % of the mass of the matrix fine powder, 0.1 ≤ b ≤ 1.2; when 0.35 < x ≤ 0.55, the growth aid is a mixture of Li2CO3 and CuO, and the mass of the growth aid is b % of the mass of the reactive matrix fine powder, 0.1 ≤ b ≤ 0.48; The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is prepared under low sintering temperature conditions of 850℃~1095℃, and the Zr content of the texture can be as high as 50% or more. [001] c Orientation degree ≥ 98%, grain misalignment degree measured using the March-Dollase method r Below 0.20, the elements in the grains are uniformly distributed, with no core-shell structure, and the Curie temperature is [missing information]. T c ≥200 ℃, quasi-static piezoelectric coefficient d 33 Above 1000 pC / N, electromechanical coupling coefficient k 33 Higher than 0.85; The preparation method of the above-mentioned relaxor lead-based textured ceramic material with low texture temperature and high electrical properties is carried out according to the following steps: I. Preparation of fine powder from the parent compound: ① A-containing niobate precursor powder is synthesized by solid-state method; the A-containing niobate precursor powder is one or more of MgNb2O6, ZnNb2O6, ScNbO4 and InNbO4, and the A-containing niobate precursor powder is pure phase and fine crystal with a particle size of less than 200 nm. ② Prepare the parent fine powder or reaction parent fine powder according to different values ​​of x: When 0.15 ≤ x ≤ 0.35, Pb source powder, A-containing niobate precursor powder, ZrO2 powder, and TiO2 powder are weighed according to the stoichiometric ratio of the general chemical formula (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3. The powder is then ball-milled and dried using anhydrous ethanol as the medium. After pre-calcination at 600 ℃~900 ℃ for 1 h~6 h, it is finally ball-milled and dried again to obtain (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 parent fine powder. The (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 parent fine powder is a pure perovskite phase with fine crystals and a particle size less than 300 μm. nm, where 0.15≤y≤0.55, and 0.10≤1-xy≤0.50; the Pb source powder is PbO, Pb3O4 or basic lead carbonate; When 0.35 < x ≤ 0.55, weigh the Pb source powder, A niobate precursor powder containing A, ZrO₂ powder and TiO₂ powder according to the stoichiometric ratio of the chemical formula (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃, ball-mill with absolute ethanol as the medium and dry, then pre-sinter at a temperature of 600 °C to 900 °C for 1 h to 6 h, and finally ball-mill twice and dry to obtain the fine powder of the (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃ reaction matrix; the (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃ reaction matrix fine powder is of pure perovskite phase and fine crystal, with a particle size less than 300 nm, where 0.15 ≤ y ≤ 0.55, and 0.10 ≤ 1 - x - y ≤ 0.50; weigh the Pb source powder and ZrO₂ powder according to the stoichiometric ratio of PbZrO₃, ball-mill with absolute ethanol as the medium and dry, then pre-sinter at a temperature of 600 °C to 900 °C for 1 h to 6 h, and finally ball-mill twice and dry to obtain the PbZrO₃ reaction matrix fine powder, the PbZrO₃ reaction matrix fine powder is of pure phase and fine crystal, with a particle size less than 200 nm; the Pb source powder is PbO, Pb₃O₄ or basic lead carbonate; II. Preparation of ceramic green body by tape casting and laminating pressing: ① Prepare tape-casting slurries according to different values of x: When 0.15≤x≤0.35, the fine powder of (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 parent material and the flake-shaped Ba(Zr)O3 are used. m Ti 1-m (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 casting slurry containing template seed crystals was obtained by mixing O3 microcrystals, growth aids, solvents, dispersants, binders, and plasticizers, followed by vacuum degassing. m Ti 1-m The volume of the O3 microcrystals is a% of the volume of the (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 parent fine powder, where 3.0≤a≤5.0; the growth aid is a mixture of Li2CO3 and PbO, and the mass of the growth aid is b% of the mass of the (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 parent fine powder, where 0.1≤b≤1.2; When 0.35 < x ≤ 0.55, (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder, flaky Ba(Zr m Ti 1-m )O3 microcrystals, growth aids, solvents, dispersants, binders and plasticizers are mixed, and then vacuum degassed to obtain a reaction casting slurry of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 containing template seeds; PbZrO3 reaction matrix fine powder, solvent, dispersant, binder and plasticizer are mixed, and then vacuum degassed to obtain a PbZrO3 reaction casting slurry without template seeds; the volume of the flaky Ba(Zr m Ti 1-m )O3 microcrystals is a% of the total volume of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder and PbZrO3 reaction matrix fine powder, where 3.0 ≤ a ≤ 5.0; the growth aids are a mixture of Li2CO3 and CuO, and the mass of the growth aids is b% of the total mass of (1 - x - y)Pb(A,Nb)O3 - 0.35PbZrO3 - yPbTiO3 reaction matrix fine powder and PbZrO3 reaction matrix fine powder, 0.1 ≤ b ≤ 0.48; ② Tape casting: Under conditions of speeds of 1.5 cm / s to 2 cm / s, a (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 casting slurry containing template seed crystals was cast on a casting machine, then dried and cut to obtain (1-xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 castings containing template seed crystals. - xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 film; Or under the condition of a speed of 1.5 cm / s to 2 cm / s, tape-cast the reaction tape-casting slurry of (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃ containing template seeds and the PbZrO₃ reaction tape-casting slurry without template seeds on a tape-casting machine respectively, then dry and cut to obtain the reaction film of (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃ containing template seeds and the PbZrO₃ reaction film without template seeds; ③ Laminating according to different values of x: When 0.15≤x≤0.35, the (1) containing template seed crystals will be... - xy)Pb(A,Nb)O3-xPbZrO3-yPbTiO3 film stacks were used to obtain the stacked sample; When 0.35 < x ≤ ⅚, stack the reaction film of (1 - x - y)Pb(A,Nb)O₃ - 0.35PbZrO₃ - yPbTiO₃ containing template seeds and the PbZrO₃ reaction film without template seeds alternately according to the stoichiometric ratio of the chemical formula (1 - x - y)Pb(A,Nb)O₃ - xPbZrO₃ - yPbTiO₃ to obtain the stacked sample; ④ Pressing: Hot-press the stacked sample for 10 min and hot-water isostatic press for 30 min to obtain the ceramic green body; III. Preparation of textured ceramics: ① Debinding and cold isostatic pressing: Debind the ceramic green body at a temperature of 500 °C to 700 °C for 1 h to 6 h, then cold isostatic press at a pressure of 150 MPa to 250 MPa for 1 min to 10 min to obtain the ceramic green compact; ② Sintering: Under low sintering temperatures of 850 ℃ to 1095 ℃, ceramic blanks are sintered for 5 min to 600 min to obtain textured ceramics. ③Polarization: The two surfaces of the textured ceramic perpendicular to the texture direction are polished, cleaned and dried, and then polarized and polarized to obtain a relaxor lead-based textured ceramic material with low texture temperature and high electrical properties. The polarization specifically involves applying silver paste to the polished surface and then burning the electrode at a temperature of 450 ℃ to 650 ℃ for 30 min to 90 min; the polarization is specifically carried out under a DC electric field of 30 kV / cm.

2. The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties according to claim 1, characterized in that... In step 1②, ball milling was performed using anhydrous ethanol as the medium for 24 h to 96 h.

3. The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties according to claim 1, characterized in that... The secondary ball milling time mentioned in step 1② is 12 h to 72 h.

4. The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties according to claim 1, characterized in that... The solvent mentioned in step 2① is a mixed solution of xylene and ethanol; the dispersant mentioned in step 2① is melted herring oil; the binder mentioned in step 2① is polyvinyl butyral; and the plasticizer mentioned in step 2① is a mixture of polyalkylene glycol and butyl benzyl phthalate.

5. The relaxor lead-based textured ceramic material with low texture temperature and high electrical properties according to claim 1, characterized in that... The hot pressing mentioned in step 2④ specifically refers to hot pressing for 10 min under a pressure of 10 MPa~50 MPa and a temperature of 60 ℃~95 ℃; the hot water uniform pressing mentioned in step 2④ specifically refers to hot water uniform pressing for 30 min under a pressure of 20 MPa~50 MPa and a temperature of 70 ℃~95 ℃.

6. The application of the relaxor lead-based textured ceramic material with low texture temperature and high electrical properties as described in claim 1, characterized in that... It is applied in multilayer piezoelectric devices with high performance, wide temperature range, high power, and high electric field drive, including high-end ultrasonic transducers, high-end piezoelectric actuators, high-end piezoelectric sensors, and high-end energy harvesters.

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