CN110759718B - Preparation method of arched flaky dielectric material and flexural voltage electric composite material - Google Patents

Preparation method of arched flaky dielectric material and flexural voltage electric composite material Download PDF

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CN110759718B
CN110759718B CN201911175676.3A CN201911175676A CN110759718B CN 110759718 B CN110759718 B CN 110759718B CN 201911175676 A CN201911175676 A CN 201911175676A CN 110759718 B CN110759718 B CN 110759718B
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周万丰
初宝进
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CETC 43 Research Institute
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Abstract

The invention discloses a preparation method of an arched flaky dielectric material and a deflection voltage electric composite material, which comprises the following steps: laminating n layers of ceramic materials to form a laminated body green body and then cutting, wherein n is more than or equal to 2, and the shrinkage rate of at least one layer of ceramic material positioned at the bottom layer in the laminated body green body is smaller or larger than that of the ceramic material positioned above the bottom layer; and sintering the green laminate to form the arched flaky dielectric material. The method has simple process, can greatly reduce the waste of raw materials, is suitable for industrial mass production, and improves the stability between batch preparation.

Description

Preparation method of arched flaky dielectric material and flexural voltage electric composite material
Technical Field
The invention belongs to the field of functional materials, and particularly relates to a preparation method of an arched flaky dielectric material, and also relates to a flexural voltage electric composite material.
Background
The piezoelectric effect comprises a positive voltage effect and an inverse piezoelectric effect, wherein the positive voltage effect is that the material generates electric polarization response when bearing pressure, the inverse piezoelectric effect is that the material generates strain response under an electric field, and the conversion between mechanical energy and electric energy can be realized through the piezoelectric effect. At present, piezoelectric materials are a class of materials with piezoelectric effect, such as lead zirconate titanate ceramics (PZT) and the like, which are widely used for preparing devices such as sensors, drivers, transducers, energy recovery and the like, and have very important application in the fields of civil use and national defense. However, with the rapid development of scientific technology, the service conditions of piezoelectric materials also face more and more challenges, such as high temperature resistant piezoelectric materials used in the aerospace field. Because the piezoelectricity of the traditional piezoelectric material has certain structural limitation and can only exist in a crystal structure without central symmetry, most of the piezoelectric materials widely applied at present are ferroelectric piezoelectric materials with excellent piezoelectric performance, and when the piezoelectric materials are used, the piezoelectric materials are subjected to phase change to generate a central symmetry structure and lose the piezoelectric performance after the use temperature exceeds the Curie temperature of the materials. Therefore, it has been a technical problem in the field of piezoelectric materials to increase the use temperature of piezoelectric materials.
In order to overcome the technical problem of the use temperature of the piezoelectric material, researchers design a piezoelectric composite material which can be used at a high temperature by utilizing an electromechanical coupling effect similar to the piezoelectric effect. This electromechanical coupling effect, which is similar to the piezoelectric effect, is called the flexoelectric effect, which is the polarization response of a material in the presence of a strain gradient (positive flexoelectric effect) or the stress response in the presence of an electric field gradient (inverse flexoelectric effect), and can be described by the formula:
positive flexoelectric effect:
Figure BDA0002289871840000011
inverse flexoelectric effect:
Figure BDA0002289871840000012
in the above formula, PlIs the dielectric polarization in the material; elIs the electric field strength in the material; t is a unit ofijAnd SijStress and strain in the material, respectively; mu.sijklFor the flexoelectric coefficient, the strength of the flexoelectric effect of the material is reflected. The flexoelectric coefficient is a fourth order tensor, and thus there is a non-zero component in all symmetric materials. In many documents, muijklOften reduced to determinant component form muij。
The flexoelectric piezoelectric material converts force or electric signals borne by the material into corresponding gradients through a special structure, and can generate corresponding electric polarization response or stress response due to the flexoelectric effect of the material, so that the conversion from mechanical energy to electric energy or from electric energy to mechanical energy is realized, and an apparent piezoelectric response or an inverse piezoelectric response is formed. The key to the design of such piezoelectric composites is the structure that converts the force or electrical signal experienced by the material into a corresponding gradient and that allows the apparent piezoelectric response of the material to be as large as possible, i.e., the efficiency of the conversion of the flexural piezoelectric response of the material into a piezoelectric response to be as high as possible.
Several flex voltage electrical material designs have been demonstrated to be feasible in experiments. The first is a flexural voltage electric composite material with a pyramid-like structure, and due to the asymmetric structure of the material, the force or voltage applied to the two surfaces of the structure forms stress or electric field gradient in the material, and the material shows apparent piezoelectric performance, but the strain gradient generated by the material is small, the generated apparent piezoelectric response is small, and the preparation process of the piezoelectric composite material is complex; the second is the design of bending type deflection voltage electric composite material, the composite material transmits the force applied on a metal flat plate to a long strip-shaped ceramic sheet through a tungsten wire, the applied force is converted into the bending deformation of the long strip-shaped material, a strain gradient generated due to the bending deformation is generated in the material, the material shows stronger apparent piezoelectric performance, the length of the long strip is far greater than the width and the thickness of the material, and the use range of the material is reduced and the bearing capacity of the material is reduced; the third is a point-ring type flexural piezoelectric composite material, as shown in fig. 1, which is composed of a sheet dielectric material 10 with an electrode 11, an annular support 12 for supporting the edge of the sheet material and a flat plate 13 for supporting the annular support 12, and which can generate a large apparent piezoelectric response and is simple in preparation process; the fourth is a point-surface type piezoelectric bending voltage electric composite material, as shown in fig. 2, the point-surface type structure is similar to a point-ring type structure but has a simpler structure, and the point-surface type piezoelectric bending voltage electric composite material is composed of a sheet-shaped dielectric material 20 with an arch structure and a flat plate 13, the material has a simpler structure, and can also generate larger apparent piezoelectric response, when the traditional point-surface type bending voltage electric composite material is prepared, a common mechanical processing mode can be adopted, but for the dielectric material, particularly the dielectric ceramic material, the processing technology difficulty is large, and the raw material cost is higher; the reduction process is also used to contact the flaky dielectric ceramic with graphite for high-temperature treatment to generate a layer of reduced dielectric material, and an arch structure is generated during rapid quenching.
Disclosure of Invention
In view of the above, the present invention provides a method for preparing an arched sheet-like dielectric material, which adopts a multi-layer laminated sheet-like structure, and solves the technical problems of complex process and poor product stability in batch preparation of the existing point-surface type deflection point piezoelectric composite material, because the materials in the sheet-like structure have different shrinkage rates, the arched structure is directly formed after sintering.
In order to achieve the purpose, the invention adopts the following technical scheme:
a preparation method of an arched sheet dielectric material comprises the following steps:
laminating n layers of ceramic materials to form a laminated body green body and then cutting, wherein n is more than or equal to 2, and the shrinkage rate of at least one layer of ceramic material positioned at the bottom layer in the laminated body green body is smaller or larger than that of the ceramic material positioned above the bottom layer;
and sintering the green laminate to form the arched flaky dielectric material.
Furthermore, the ceramic materials are the same ceramic material, and different amounts of sintering aids, different types of sintering aids, different tape casting systems or ceramic raw materials with different particle sizes are added into the ceramic materials of different layers to adjust the shrinkage of each layer.
Further, the ceramic materials are different ceramic materials, and the ceramic materials with different shrinkage rate systems are adopted or the materials with different shrinkage rates from the green body are printed on one surface of the green body of the laminated body.
Preferably, the material with different shrinkage rate from the blank body is an electrode material or a resistance material.
Further, the cut shape includes a circle or a square.
The present invention also provides a deflection voltage electrical composite comprising:
the arched flaky dielectric material is prepared by the preparation method;
an electrode formed on at least one surface of the arched sheet dielectric material;
and two ends of the arched flaky dielectric material are in point-surface contact with the flat plate.
Further, the electrode comprises a sputtering gold electrode, a sputtering platinum electrode, a silver burning electrode, a sputtering silver electrode, an aluminum electrode or a palladium electrode.
Further, the flat plate includes alumina, cemented carbide, or a natural hard material.
Compared with the prior art, the invention has the following beneficial effects:
the invention is prepared into a multilayer sheet structure during material molding, and the shrinkage rate of at least one layer is different from that of other layers by adjusting the shrinkage rates of different layers, so that the sheet material forms an arch effect due to different deformation caused by different shrinkage rates during co-firing molding. In addition, the height of the arch can be adjusted by the number of layers in the multilayer sheet structure or the difference of the shrinkage rate between the layers, the process is simple, the waste of raw materials can be greatly reduced, and the method is suitable for industrial mass production and improves the stability between batch preparation.
Drawings
FIG. 1 is a schematic diagram of a prior art midpoint-ring type deflection voltage electrical composite;
FIG. 2 is a schematic structural diagram of a point-and-plane piezoelectric bending voltage electric composite material in the prior art;
FIG. 3 is a schematic view of the green laminate of the present invention;
FIG. 4 is a schematic structural view of the green laminate of FIG. 3 sintered into an arched sheet of dielectric material;
FIG. 5 is a schematic structural view of a flexoelectric piezoelectric composite comprising the arched sheet of dielectric material of FIG. 4.
In the figure: 10-sheet dielectric material, 11-electrode, 12-annular support, 13-plate, 20-sheet dielectric material with arch structure, 30-green laminate, 31-arch sheet dielectric material.
Detailed Description
In order that the invention may be more fully understood, reference will now be made to the following description of specific embodiments. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used herein in the description of the invention is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention.
A preparation method of an arched sheet dielectric material comprises the following steps:
laminating n layers of ceramic materials to form a laminated body green body and then cutting, wherein n is more than or equal to 2, and the shrinkage rate of at least one layer of ceramic material positioned at the bottom layer in the laminated body green body is smaller or larger than that of the ceramic material positioned above the bottom layer;
and sintering the laminated body green body to form the arched flaky dielectric material.
Specifically, the present invention is to form an arched sheet-like dielectric material by laminating ceramic materials to form a green laminate, and then forming an arched structure by forming a difference in deformation caused by sintering due to a difference in shrinkage rate, so that the ceramic materials in the green laminate should be regularly arranged to form an arched structure, for example, the green laminate may be divided into a bottom layer region and a top layer region, wherein the bottom layer region or the top layer regionIt may be composed of at least one layer of ceramic material, and the shrinkage rate of the ceramic material in the bottom layer region should be different from that of the ceramic material in the top layer region, i.e. the shrinkage rate of the ceramic material in the bottom layer region should be greater or smaller than that of the ceramic material in the top layer region, so that the ceramic material in the bottom layer region deforms to a different extent during sintering to form a dome shape. The method of the present invention can adjust the doming height of the domed sheet dielectric material by adjusting the number of layers of the green laminate or the differential shrinkage between the different layers. It is understood that the ceramic material is commonly used in the art, such as low temperature co-fired ceramic, alumina powder, BaTiO3The preparation of the dielectric ceramic materials such as ceramics can adopt casting technology, printing technology or other forming technology commonly used in the field, as long as the shrinkage rate in the invention is different, the ceramic materials commonly used in the field can be used for realizing the technical effect in the invention, the lamination of the ceramic materials can adopt warm isostatic pressing after lamination to form a green laminated body, but the method is not limited to the method, the lamination method commonly used in the field can be used in the invention, and the detailed description is omitted. It should be noted that the sintering temperature or curing temperature of the ceramic material forming the green laminate should be close to each other as long as the co-firing or simultaneous forming thereof is achieved.
Furthermore, the ceramic materials are the same ceramic material, and different amounts of sintering aids, different types of sintering aids, different tape casting systems or ceramic raw materials with different particle sizes are added into the ceramic materials of different layers to adjust the shrinkage of each layer. In some embodiments of the invention, the ceramic material of each layer in the green laminate is the same ceramic material. Specifically, the shrinkage difference of the ceramic materials between different layers is mainly adjusted in four ways, one is to add different amounts or different types of sintering aids into the ceramic materials of different layers, and the different amounts or different types of sintering aids have different sintering aid effects on the ceramic, so that the densification degree of the ceramic between different layers during sintering is different, and the shrinkage effects are different, therefore, the different layers can be realized by adding different amounts or different types of sintering aidsThe difference in shrinkage of the ceramic material is understood to mean that the sintering aid used here is a sintering aid conventionally used in the art, such as Ca-La-Bb glass, SiO2GE glass (main components are LiF and BaF), CuO, etc., and those skilled in the art can select a suitable sintering aid according to the different ceramic material systems adopted, and therefore, the invention is not specifically limited herein; in the process of forming ceramic green tapes with different layers by casting, because the formula of the casting system comprises ceramic powder, a binder, a solvent, a dispersant, a plasticizer and other auxiliaries, by adjusting different casting systems, for example, by using different binders, the solid content in the cast green tapes can be different, so that the densification degree of the ceramics between different layers is different during sintering, the generated shrinkage effects are also different, and the shrinkage rates of the ceramic materials of different layers are different, it can be understood that the binder, the solvent, the dispersant, the plasticizer and the like are all the auxiliaries conventionally used in the cast green tapes in the field, and the technical personnel in the field can adjust the auxiliaries as required, so the details are not described herein; the raw porcelain strips of each layer can be prepared by adopting ceramic raw materials with different particle sizes, and the ceramic powder density in each raw porcelain strip casted by adopting the ceramic raw materials with different particle sizes is different, so that the densification degree of ceramics between different layers is different during sintering, and the generated shrinkage effect is also different, therefore, the shrinkage rate can be adjusted by adjusting the particle size of the ceramic raw materials for preparing the raw porcelain strips.
Further, the ceramic materials are different ceramic materials, and ceramic materials with different shrinkage rate systems are adopted or other materials with different shrinkage rates from the green body are printed on the green body of the bottom layer ceramic material. In other embodiments of the invention, the ceramic materials of the layers in the green laminate are different types of ceramic materials. Specifically, firstly, the LTCC green tapes with different shrinkage rate systems, such as directly adopted LTCC green tapes, have different shrinkage rates, and are laminated and sintered, so that the process is simpler than other processes; and secondly, materials with different shrinkage rates from the green body can be printed on the green body of the laminated body, and due to the fact that the green body materials and the surface layer printing materials have different shrinkage behaviors during sintering, the shrinkage effect generated after sintering is different. The printing material is preferably an electrode material or a resistive material, and may be adjusted by a person skilled in the art as needed as long as the shrinkage rate of the printing material is different from that of the blank, and thus, the printing material is not particularly limited herein.
Further, the green laminated body may need to be cut into different shapes after being laminated into the green laminated body, and this may be adjusted as needed, and in some embodiments of the present invention, the cut shape includes a circular shape or a square shape, it is understood that the cut shape is not limited to the above two, and those skilled in the art can adjust the shape as needed, such as a special shape like an oval shape.
The invention also discloses a deflection voltage electric composite material, the specific structure of which is shown in figure 5, comprising:
an arched sheet-like dielectric material 31 prepared as described above;
an electrode 11 formed on at least one surface of the arched sheet-like dielectric material 31; that is, the electrode 11 may be two or one, and fig. 3 shows an embodiment in which the electrode is two.
And a flat plate 13, wherein two ends of the arched sheet-shaped dielectric material 31 are in point-surface contact with the flat plate 13.
The flexoelectric piezoelectric composite material of the present invention is prepared by first laminating ceramic green tapes having different shrinkage rates to form a green laminate 30, which is sintered to form an arched sheet-like dielectric material 31 as shown in fig. 3, and then arching the arched sheet-like dielectric material 31 to a certain height, which generates a strain gradient and a flexoelectric response in the arching height direction when a force is applied to the arched sheet-like dielectric material 31, thereby generating an apparent piezoelectric effect, as shown in fig. 4.
Generally, the electrode 11 may be any conductive electrode in the art as long as it has conductive properties, and in some embodiments of the present invention, the electrode 11 is preferably a sputtered gold electrode, a sputtered platinum electrode, a silver-fired electrode, a sputtered silver electrode, an aluminum electrode, or a palladium electrode, and it is understood that the electrode 11 is selected from the group consisting of, but not limited to, the foregoing electrodes.
Meanwhile, the flat plate has only to have a flat surface and high hardness, and in some embodiments of the present invention, the flat plate 13 is made of alumina, cemented carbide, or a natural hard material. The electrodes and the flat plates are made of piezoelectric composite materials which are conventionally used in the field, and can be adjusted by a person skilled in the art according to the needs, and it is understood that the selection includes but is not limited to the above.
The technical solution of the present invention will be more clearly and completely described below with reference to specific embodiments.
Example 1
The green laminate in this example was laminated with 5 layers of a commercially available LTCC green tape, 4 layers of A6M green tape (shrinkage of 15.5%) manufactured by the U.S. FERRO company and 1 layer of 951 green tape (shrinkage of 12.7%) manufactured by the U.S. Dupont company, and was hot isostatic pressed and cut into a 25 mm-diameter wafer. Sintering at 850 deg.C to obtain arched sheet dielectric material, forming good arched structure with arched height up to 960 μm due to mismatched contraction of A6M green ceramic tape and 951 green ceramic tape, preparing silver electrodes on both sides of the material, and forming point-surface type bending voltage electric composite material on a planar substrate due to low bending electric coefficient of the material33The apparent piezoelectric property of 0.5pC/N is obtained by measurement.
Example 2
The green laminate in this example was laminated with 5 layers of the laminate as it is by using a commercially available LTCC green tape, and 3 layers of A6M green tape (shrinkage of 15.5%) manufactured by FERRO, USA, and 2 layers of 951 green tape (shrinkage of 12.7%) manufactured by Dupont, USA, and the laminate was laminated with 5 layers in total, hot isostatic pressed, and cut into straight sheetsA circular piece with the diameter of 25 mm. Sintering into arched sheet dielectric material at 850 deg.C, forming good arched structure with arched height of 1007 μm due to mismatched contraction of A6M green tape and 951 green tape, preparing silver electrodes on both sides of the material, and forming point-surface type bending voltage electric composite material on a planar substrate due to low bending electric coefficient of the material33The apparent piezoelectric property of 0.5pC/N is obtained by measurement.
Example 3
Al at particle size D50 of about 2.5 microns2O3Adding 50 wt% of Ca-La-Bb glass serving as a sintering aid into the powder, fully ball-milling and uniformly mixing to reduce the sintering temperature of the alumina ceramic to 850 ℃. And adding a binder PVB, a solvent ethanol, butanone, a dispersant triethanolamine and a plasticizer DBP into the mixed powder, casting the mixed powder into a green ceramic tape with uniform thickness, laminating 5 layers in total, hot isostatic pressing the laminated green ceramic tape, and cutting the laminated green ceramic tape into a wafer with the diameter of 25 mm. Printing silver conductor slurry with shrinkage rate not matched with the raw porcelain tape on the whole surface of one surface of a green ceramic wafer, sintering the green ceramic wafer and the silver conductor slurry at 850 ℃ to form an arch-shaped sheet dielectric material, wherein the alumina ceramic green body and the silver conductor slurry are not matched in shrinkage, a good arch structure can be formed, the arch height can reach 1080 mu m, then preparing a silver electrode on the other surface of the ceramic wafer, and placing the silver electrode on a planar substrate to form a point-surface type deflection voltage electric composite material, wherein the deflection electric coefficient of the material is not high, and the point-surface type deflection voltage electric composite material is formed in a ZJ-6A quasi-static state d33The apparent piezoelectric property of 0.6pC/N is obtained by measurement.
Example 4
About 2.5 μm Al at D502O3Adding about 50 wt% of Ca-La-Bb glass as a sintering aid into the powder to reduce the sintering temperature of the alumina ceramic to 850 ℃. And adding a binder PVB, a solvent ethanol, butanone, a dispersant triethanolamine and a plasticizer DBP into the mixed powder, and casting the mixture into a green ceramic tape with uniform thickness. In which 4 layers of green tiles using a casting support using PVB as a binder and 1 layer of green tiles using a casting support using an acrylic resin using PVB as a binder were laminated together in a total of 5 layers and subjected to hot isostatic pressing, and then cut into a wafer having a diameter of 25 mm. After sintering at 850 ℃ the green porcelain is sintered due to the shrinkage between the different layersDifferent, can form a good arch structure, the height of the arch can reach 304 μm, then silver electrodes are prepared on two sides of the arch sheet dielectric material, and the silver electrodes are placed on a plane substrate to form a point-plane type flexural voltage electric composite material, because the flexural electric coefficient of the material is not high, the material is in a ZJ-6A quasi-static state d33The apparent piezoelectric property of 0.6pC/N is obtained by measurement.
Example 5
BaTiO prepared by traditional solid phase synthesis method3Ceramics, according to BaTiO to be prepared3Stoichiometric ratio of ceramics to BaCO3，TiO2(analytically pure, national medicine group) adding alcohol, ball milling for 6-8 hours, drying, and keeping the temperature at 1200 ℃ for 2 hours to prepare BaTiO3A ceramic. Then BaTiO is added3Ceramic ball milling, adding adhesive PVB, solvent ethanol, butanone, dispersant triethanolamine and plasticizer DBP, and casting into a raw ceramic band with uniform thickness. Stacking 4 layers of pure BaTiO3Cast green tiles and 1 layer 0.15 wt% SiO addition2BaTiO as sintering aid3Cast green ceramic sheets, a total of 5 layers were laminated together and hot isostatically pressed, cut into 25mm diameter discs and sintered at 1280 ℃ since 4 layers of pure BaTiO3The shrinkage of the green ceramic chip and 1 layer of green ceramic chip containing sintering aid is not matched, the arch height can reach 483 mu m, then silver electrodes are prepared on two surfaces of the material, the silver electrodes are placed on a plane substrate to form a point-surface type deflection voltage electric composite material, and the point-surface type deflection voltage electric composite material is subjected to quasi-static d in ZJ-6A33The apparent piezoelectric property of 70-110pC/N is measured by the instrument.
Example 6
BaTiO prepared by traditional solid phase synthesis method3Ceramics, according to BaTiO to be prepared3Stoichiometric ratio of ceramic BaCO3，TiO2(analytically pure, national medicine group) is added with alcohol, ball milled for 6 to 8 hours, dried and then is synthesized by heat preservation for 2 hours at 1200 ℃. Then ball milling the synthesized powder, adding a binder PVB, a solvent ethanol and butanone, a dispersant triethanolamine and a plasticizer DBP, and casting into a green ceramic tape with uniform thickness. Stacking 4 layers of pure BaTiO3Cast green tiles and 1 layer BaTiO sintered with 0.5 wt% GE glass (mainly LiF and BaF) as sintering aid3Cast green ceramic sheets, a total of 5, were laminated together and heatedAfter isostatic pressing, cut into 25mm diameter circular sheets, sintered at 1280 ℃ due to 4 layers of pure BaTiO3The shrinkage of the green ceramic chip and 1 layer of green ceramic chip containing sintering aid is not matched, the arch height can reach 205 μm, then silver electrodes are prepared on two surfaces of the material, the silver electrodes are placed on a plane substrate to form a point-surface type deflection voltage electric composite material, and the point-surface type deflection voltage electric composite material is subjected to quasi-static d in ZJ-6A33The apparent piezoelectric property of 50-80pC/N is obtained by measurement.
Example 7
BaTiO prepared by traditional solid phase synthesis method3Ceramics, according to BaTiO to be prepared3Stoichiometric ratio of ceramics to BaCO3，TiO2(analytically pure, national medicine group) is added with alcohol, ball milled for 6 to 8 hours, dried and then is synthesized by heat preservation for 2 hours at 1200 ℃. Then the synthesized powder is divided into two parts, one part is ball milled for 6 hours, and the other part is ball milled for 12 hours. Then adding the same adhesive PVB, solvent ethanol and butanone, dispersant triethanolamine and plasticizer DBP respectively to cast into a green ceramic band with uniform thickness. Stack 4 layers of ball milling for 6 hours BaTiO3Cast green tile and 1-layer ball milled for 12 hours BaTiO3Cast green tiles, 5 in total, were laminated together and hot isostatically pressed and cut into 25mm diameter disks. Sintering at 1280 deg.C, with different ball milling time, different particle size of powder and different sintering property, so that the shrinkage of the green ceramic chip is different, the arch height can reach 185 μm, preparing silver electrodes on two sides of the material, placing on a planar substrate to form point-surface type deflection voltage electric composite material, and sintering at ZJ-6A quasi-static d33The apparent piezoelectric property of 60-100pC/N is measured by the instrument.
Example 8
Ba prepared by conventional solid phase synthesis0.67Sr0.33TiO3Ceramics prepared by mixing BaCO at a certain ratio3，SrCO3，TiO2(analytically pure, national medicine group) is added with alcohol, ball milled for 6 to 8 hours, dried and then is synthesized by heat preservation for 2 hours at 1200 ℃. Then ball milling the synthesized powder, adding a binder PVB, a solvent ethanol and butanone, a dispersant triethanolamine and a plasticizer DBP, and casting into a green ceramic tape with uniform thickness. Stacking 4 layers of pure Ba0.67Sr0.33TiO3Tape-cast green ceramic chipAnd 1 layer of Ba added with 1 wt% of CuO as sintering aid0.67Sr0.33TiO3Cast green tiles, 5 in total, were laminated together and hot isostatically pressed and cut into 25mm diameter disks. Sintering at 1350 deg.C due to 4 layers of pure Ba0.67Sr0.33TiO3The shrinkage of the green ceramic chip is not matched with that of 1 layer of green ceramic chip containing sintering aid, the arch height can reach 209 micrometers, then silver electrodes are prepared on two surfaces of the material, the material is placed on a plane substrate to form a point-surface type deflection voltage electric composite material, and the point-surface type deflection voltage electric composite material is formed in a quasi-static state d of ZJ-6A33The apparent piezoelectric performance of 90-130pC/N is measured by the instrument.
Example 9
Preparation of 0.92Na by conventional solid phase synthesis1/2Bi1/2TiO3-0.08BaTiO3、0.94Na1/2Bi1/2TiO3-0.06BaTiO3A ceramic. Bi is added according to the metering ratio2O3，Na2CO3，BaCO3，TiO2(analytically pure, national drug group) is added with alcohol, ball milled for 6 to 8 hours, dried and then is synthesized by heat preservation for 2 hours at 800-. Then ball milling the synthesized powder, adding a binder PVB, a solvent ethanol and butanone, a dispersant triethanolamine and a plasticizer DBP, and casting into a green ceramic tape with uniform thickness. Stack of 4 layers of pure 0.92Na1/ 2Bi1/2TiO3-0.08BaTiO3Cast green tile and 1 layer of pure 0.94Na1/2Bi1/2TiO3-0.06BaTiO3The green ceramic sheets of (1) were laminated together, hot isostatically pressed, and cut into 25mm diameter disks. Sintering at 1175 deg.C, due to 4 layers of 0.92Na1/2Bi1/ 2TiO3-0.08BaTiO3Green ceramic chip and 1 layer of 0.94Na1/2Bi1/2TiO3-0.06BaTiO3The shrinkage of the green ceramic chip is not matched, the arch height can reach 89 mu m, then silver electrodes are prepared on two surfaces of the material, the material is placed on a plane substrate to form a point-surface type deflection voltage electric composite material, and the point-surface type deflection voltage electric composite material is arranged on a ZJ-6A quasi-static d33The apparent piezoelectric performance of 2-4pC/N is obtained by measurement.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent should be subject to the appended claims.

Claims (8)

1. A preparation method of an arched sheet dielectric material is characterized by comprising the following steps:
laminating n layers of ceramic materials to form a laminated body green body and then cutting, wherein n is more than or equal to 2, the shrinkage rate of at least one layer of ceramic material positioned at the bottom layer in the laminated body green body is smaller or larger than that of the ceramic material positioned at the upper part of the bottom layer, and the ceramic material is prepared by adopting a tape casting process;
and sintering the green laminate to form the arched flaky dielectric material.
2. The method according to claim 1, wherein the ceramic materials are the same ceramic material, and the shrinkage of each layer is adjusted by adding different amounts of sintering aids, adding different kinds of sintering aids, using different casting systems, or using ceramic raw materials of different particle sizes to the ceramic materials of different layers.
3. The method of claim 1, wherein the ceramic materials are different ceramic materials, and the shrinkage of the green laminate is controlled by using ceramic materials having different shrinkage systems or by printing a material having a different shrinkage from that of the green laminate on one side of the green laminate.
4. The method according to claim 3, wherein the material having a different shrinkage rate from the green body is an electrode material or a resistive material.
5. The method of claim 1, wherein the cut shape comprises a circle or a square.
6. A flexural voltage electrical composite material, comprising:
an arched sheet-like dielectric material produced by the production method according to any one of claims 1 to 5;
an electrode formed on at least one surface of the arched sheet dielectric material;
and two ends of the arched flaky dielectric material are in point-surface contact with the flat plate.
7. The flexoelectric piezoelectric composite of claim 6, wherein the electrode comprises a sputtered gold electrode, a sputtered platinum electrode, a silver-fired electrode, a sputtered silver electrode, an aluminum electrode, or a palladium electrode.
8. The flexoelectric piezoelectric composite of claim 6, wherein said plate comprises alumina, cemented carbide or natural hard materials.
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