CN113929487B - Piezoelectric ceramic composite material and preparation method and application thereof - Google Patents

Piezoelectric ceramic composite material and preparation method and application thereof Download PDF

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CN113929487B
CN113929487B CN202110342855.2A CN202110342855A CN113929487B CN 113929487 B CN113929487 B CN 113929487B CN 202110342855 A CN202110342855 A CN 202110342855A CN 113929487 B CN113929487 B CN 113929487B
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piezoelectric ceramic
reaction
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metal
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CN113929487A (en
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董戈
奥利加
巴维尔
马卡洛夫
沙赫诺夫
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Nanjing Nayan Enterprise Management Partnership LP
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    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B37/00Joining burned ceramic articles with other burned ceramic articles or other articles by heating
    • C04B37/02Joining burned ceramic articles with other burned ceramic articles or other articles by heating with metallic articles
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    • H10SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10NELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N30/00Piezoelectric or electrostrictive devices
    • H10N30/01Manufacture or treatment
    • H10N30/07Forming of piezoelectric or electrostrictive parts or bodies on an electrical element or another base
    • H10N30/072Forming of piezoelectric or electrostrictive parts or bodies on an electrical element or another base by laminating or bonding of piezoelectric or electrostrictive bodies
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2237/00Aspects relating to ceramic laminates or to joining of ceramic articles with other articles by heating
    • C04B2237/02Aspects relating to interlayers, e.g. used to join ceramic articles with other articles by heating
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    • C04B2237/125Metallic interlayers based on noble metals, e.g. silver

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Abstract

The invention relates to the technical field of piezoelectricity, in particular to a piezoelectric ceramic composite material and a preparation method and application thereof. The method comprises the following steps: (1) Disposing a connecting body between the piezoelectric ceramic and the material body, wherein the connecting body comprises a reaction foil, and a first adhesive and a first fusible link material coated on an upper surface of the reaction foil in this order, and a second adhesive and a second fusible link material coated on a lower surface of the reaction foil in this order; (2) Applying pressure to bring the piezoelectric ceramic, the connecting body and the material body into contact; (3) Igniting the reaction foil to carry out self-propagating reaction, so that the connecting body is melted and a welding layer is formed; wherein, before step (2), the piezoelectric ceramic is pretreated. The method provided by the invention utilizes the heat released by the self-propagating reaction of the reaction foil, and improves the firmness between the piezoelectric ceramic and the material body on the premise of not needing auxiliary flux and ensuring the functional characteristics of the piezoelectric ceramic.

Description

Piezoelectric ceramic composite material and preparation method and application thereof
Technical Field
The invention relates to the technical field of piezoelectricity, in particular to a piezoelectric ceramic composite material and a preparation method and application thereof.
Background
Piezoelectric ceramics are widely applied to the industrial production of various components, assemblies and equipment, such as: generators, sensors (sensing elements), actuators (piezoelectric drivers), transducers, and combined systems. Within piezoceramic materials there are again several types, each with different physical characteristics which in turn determine the characteristics of the elements made with them (in particular the connections of the piezoceramic material) and of the device as a whole.
Currently, there are various methods of welding piezoceramic materials to obtain structural components of the device: soldering and conductive adhesive soldering. However, none of the above methods can ensure that the sensitive piezoelectric element is not damaged when connecting such piezoelectric elements.
RU2041776 discloses a method of ceramic to metal soldering in which solder is melted for soldering of materials, the liquid state of the solder being achieved by heating (e.g. soldering iron) at high temperature for a relatively long time. This in turn leads to heating of the connected material and to a damage of the crystal structure of the piezoceramic component and thus to a loss of its electrophysical properties (depolarization of the piezoceramic material). In the actual soldering process, it is not desirable to heat the surfaces to be soldered, cooling the soldering area in the step of solder heating, which significantly increases the soldering time of the material.
Furthermore, the strength of the material weld and the quality of the final product (performance of the piezoelectric ceramic product) depend on the material amount of the solder: insufficient solder can reduce the welding strength, and sufficient solder is the guarantee of product quality. The bonding strength of the material also depends on the magnitude of its clamping force during welding: a smaller clamping force reduces the soldering strength, while an excessive clamping force increases the risk of cracking, relative movement of the soldered parts and solder leakage. With conventional soldering, it is difficult to accurately measure the amount of solder, and it is meaningless to change the magnitude of the clamping force in the case where the amount of solder is not appropriate.
In addition to the above-mentioned drawbacks, additional operations such as pre-cleaning of the soldering surface, which is caused by the reaction of silver on the surface of the piezoelectric ceramic with sulfur in the air, and post-cleaning of the used flux are required, which greatly increases the soldering time of the material.
Disclosure of Invention
The invention aims to solve the problems that in the prior art, the piezoelectric ceramic and metal connection has long welding time, low firmness and damages the functional characteristics of the piezoelectric ceramic, and an auxiliary welding flux is needed to increase the firmness of a piezoelectric material and metal, and provides a piezoelectric ceramic composite material and a preparation method and application thereof. The composite material ensures the functional characteristics of the piezoelectric ceramics and improves the firmness between the piezoelectric ceramics and the material body; meanwhile, the method is rapid and reliable, and is convenient for industrial application.
In order to achieve the above object, a first aspect of the present invention provides a method for preparing a piezoelectric ceramic composite material, the method comprising the steps of:
(1) Disposing a connecting body between the piezoelectric ceramic and the material body, wherein the connecting body comprises a reaction foil, and a first adhesive and a first fusible link material sequentially coated on an upper surface of the reaction foil, and a second adhesive and a second fusible link material sequentially coated on a lower surface of the reaction foil;
(2) Applying pressure to bring the piezoelectric ceramic, the connecting body and the material body into contact;
(3) Igniting the reaction foil to carry out self-propagating reaction, so that the connecting body is melted and a welding layer is formed;
wherein, before the step (2), the piezoelectric ceramics are pretreated.
The invention provides a piezoelectric ceramic composite material prepared by the method provided by the first aspect.
In a third aspect, the present invention provides a piezoelectric ceramic composite material provided in the second aspect, for use in electronic and optical devices.
According to the technical scheme, the reaction foil is used in the preparation process of the piezoelectric ceramic composite material, and particularly, the heat released by the self-propagating reaction of the reaction foil is utilized, the components and the thicknesses of the reaction foil, the adhesive and the fusible connecting material in the connecting body are limited, and pressure is applied to melt the connecting body and form the welding layer, so that the piezoelectric ceramic and the material body are welded, and the firmness between the piezoelectric ceramic and the material body is improved on the premise that auxiliary welding flux is not needed and the functional characteristics of the piezoelectric ceramic are guaranteed.
Drawings
FIG. 1 is a schematic diagram of the present invention for preparing a piezoelectric ceramic composite;
FIG. 2 is a schematic structural view of a linker provided by the present invention;
FIG. 3 is a TEM image of reaction foil O1 provided in preparation example 1, wherein the light phase is Al and the dark phase is Ni; a is a TEM image before magnetron deposition and b is a TEM image after magnetron deposition.
Description of the reference numerals
1. Connected body 2, piezoelectric ceramic 3, and material body
4. Reactive foil 5, first adhesive 6, second adhesive
7. First fusible link material 8, second fusible link material
Detailed Description
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For numerical ranges, each range between its endpoints and individual point values, and each individual point value can be combined with each other to give one or more new numerical ranges, and such numerical ranges should be construed as specifically disclosed herein.
The invention provides a preparation method of a piezoelectric ceramic composite material, which comprises the following steps:
(1) Disposing a connecting body between the piezoelectric ceramic and the material body, wherein the connecting body comprises a reaction foil, and a first adhesive and a first fusible link material coated on an upper surface of the reaction foil in this order, and a second adhesive and a second fusible link material coated on a lower surface of the reaction foil in this order;
(2) Applying pressure to bring the piezoelectric ceramic, the connecting body and the material body into contact;
(3) Igniting the reaction foil to carry out self-propagating reaction, so that the connecting body is melted and a welding layer is formed;
wherein, before the step (2), the piezoelectric ceramics are pretreated.
The inventor of the invention finds in research that: the thickness and the chemical composition of the reaction foil determine that the reaction foil contains a large amount of stored energy, so that the reaction foil is used as a welding heat source between the piezoelectric ceramic and the fusible connecting material, the thickness and the chemical composition of the reaction foil are limited, and the connector containing the adhesive and the fusible connecting material can be quickly melted by utilizing the heat released by the self-propagating reaction of the reaction foil, so that the piezoelectric ceramic is prevented from being overheated; meanwhile, the combination with the applied pressure improves the connection strength of the piezoelectric ceramics and the material body under the condition of not damaging the piezoelectric ceramics.
Specifically, as shown in fig. 1-2, the connected body 1 is disposed between a piezoelectric ceramic 2 and a material body 3, the connected body 1 includes a reaction foil 4, an upper surface of the reaction foil 4 is coated with a first adhesive 5 and a first fusible link material 7 in this order, and a lower surface of the reaction foil 4 is coated with a second adhesive 6 and a second fusible link material 8 in this order; applying pressure to make the piezoelectric ceramics 2, the connecting body 1 and the material body 3 contact; the self-propagating reaction that ignites the reactive foil 4 melts the interconnect 1 and forms a solder layer. That is, the present invention improves the connectivity between the piezoelectric ceramic and the material body without damaging the piezoelectric ceramic by using the reactive foil as a heat source for melt-bonding the piezoelectric ceramic and the material body and applying pressure.
In the present invention, the thickness of the reactive foil, the thickness of the adhesive (i.e., the thickness of the first adhesive and the thickness of the second adhesive), and the thickness of the fusible link material (i.e., the thickness of the first fusible link material and the thickness of the second fusible link material) can be measured by scanning electron microscope image calibration, step surface contact method, ellipsometer noncontact method, without specific indications.
In the present invention, the thickness of the reactive foil depends on the composition of the reactive foil and the thickness of the fusible link material, and preferably the thickness of the reactive foil is 10-100 μm, preferably 20-80 μm.
Further preferably, the reactive foil comprises metal layers and optionally non-metal layers arranged alternately one on top of the other and having a thickness of 2-20 nm.
Preferably, the total number of layers of the metallic layer and the optional non-metallic layer is 1000-8000 layers, preferably 2000-6000 layers. In the present invention, the number of layers of the metal layer and the optional non-metal layer depends on the metal type of the metal layer, the non-metal type of the optional non-metal layer, the thickness of the reactive foil, the thickness of the adhesive, and the thickness of the fusible link material.
According to the present invention, preferably, the metal layer is a layer formed of at least one element of nickel, aluminum, copper, niobium, cobalt, titanium, molybdenum, and tantalum.
According to the present invention, preferably, the non-metal layer is a layer formed of at least one element of carbon, silicon, and boron.
In one embodiment, the reactive foil comprises metal layers which are alternately stacked, namely metal layers A with the thickness of 2-20nm and metal layers A 'with the thickness of 2-20nm, wherein the atomic molar ratio of the metal A to the metal A' is 0.5-2:1, preferably 1: for example, the reactive foil may be Ni-Al, cu-Al, co-Al, ti-Al, but the present invention is not limited thereto.
In another embodiment, the reactive foil comprises metal layers and non-metal layers which are alternately stacked, namely, the metal layers A with the thickness of 2-20nm and the non-metal layers A 'with the thickness of 2-20nm are alternately stacked, wherein the atomic molar ratio of the metal A to the non-metal A' is 0.5-2:1, preferably 1:1. for example: nb-C, ti-Si, mo-2Si, mo-B, ti-C, 2Ta-C, the present invention is not limited thereto.
In the present invention, there is a wide range of options for the method of manufacturing the reactive foil, preferably the reactive foil is manufactured by cold rolling, magnetron sputtering, electron beam physical vapor deposition.
In a preferred embodiment, the reactive foil comprises metal layers a and a 'alternately stacked, wherein the atomic molar ratio of metal a to metal a' is 0.5 to 2:1, alternately stacking two metal foils according to the sequence of a layer of metal A and a layer of metal A', then rolling the metal foils into a cylinder shape, taking out a sample from a clamp after rolling for a plurality of times, dividing the sample and re-stacking the sample until the thickness of the sample is one half of the initial value.
In another preferred embodiment, the reactive foil comprises metal layers a and non-metal layers a 'alternately stacked, wherein the sputtered atomic ratio of metal a and non-metal a' is 0.5-2:1, the deposition thickness ratio is 1:0.5-2, the pressure of the cavity is less than 10mTorr, the atmosphere of the cavity is high-purity argon, the sum of the thicknesses of the single-layer metal layer A and the single-layer non-metal layer A' after deposition is 2-20nm, the thickness of the reaction foil is 10-100 mu m, the silicon substrate deposited with the metal layer and the non-metal layer is immersed in an acetone solution, the photoresist is melted, and the silicon substrate is separated from the reaction foil to obtain the reaction foil.
In the invention, the first adhesive and the second adhesive are respectively coated on the upper surface and the lower surface of the reaction foil, so that strong adhesive force between the fusible connecting material and the reaction foil can be ensured, the fusible connecting material is prevented from being stripped from the reaction foil, and the connectivity of the welding layer is improved.
Preferably, the first and second binders are the same or different; further preferably, the first binder and the second binder are each independently selected from at least one of a silver-based material, a gold-based material, and a copper-based material. The preferable conditions are adopted, so that the coating and welding process has good adhesion, and the welding firmness is improved.
In the present invention, the metal-based material refers to a metal-containing material, and may be a pure metal or a metal-containing alloy. For example, the silver-based material may be elemental silver having a purity of 100%, or may be an alloy containing silver.
Preferably, the thicknesses of the layers formed by the first adhesive and the second adhesive are the same or different; further preferably, the thickness of the layer formed by each of the first adhesive and the second adhesive is the same; more preferably, the thickness of the layer formed by each of the first and second adhesives is 20 to 150nm, preferably 30 to 120nm.
In the present invention, the first fusible link material may be a material that is preferably capable of good connection with the circuit board without affecting the performance of the circuit board. The second soluble joining material may be a material that preferably bonds well to the body of material without affecting the properties of the body of material. Preferably, the first and second fusible link materials are the same or different; further preferably, the first and second fusible link materials are each independently selected from tin-based materials and/or bismuth-based materials; wherein, the tin-bismuth-based material refers to a material containing metallic tin and metallic bismuth, and the tin-indium-based material refers to a mixture containing metallic tin and metallic indium.
Preferably, the thickness of the layer formed by each of the first and second fusible link materials is the same or different; further preferably, the thickness of the layer formed by each of the first and second fusible link materials is the same; more preferably, the layer formed by each of the first and second fusible link materials has a thickness of 1 to 20 μm, preferably 2 to 15 μm.
In the present invention, the first fusible link material and the second fusible link material are each independently coated on the upper surface and the lower surface of the reaction foil by an electroplating method, an electroless deposition method, or a spraying method.
In order to improve the connectivity among the piezoelectric ceramics, the connecting body and the connecting body, it is preferable that the applied pressure is 0.5 to 2.5kg/cm 2 Preferably 0.7 to 2.2kg/cm 2 . In the present invention, the contact time is not limited.
According to the invention, the melting time is preferably between 1 and 60ms, preferably between 5 and 30ms. Wherein the time for melting is from activation of the reactive foil to self-propagating reaction until the connecting body melts.
In the invention, in order to ignite the self-propagating reaction of the reaction foil, the ignition mode is selected from thermal ignition, laser ignition, combustion ignition and voltage ignition, wherein the laser ignition refers to the contact of laser on the reaction foil, the wavelength of the laser is 0.3-10 μm, and the power is 1-100W/min; voltage ignition means that a spark generated by a direct current voltage of 6-12V passes through a small part of the metal foil; hot spots are then defined as brief heating of the tips of the reaction foils using a heat source of 350-600 c.
Preferably, the conditions of the self-propagating reaction include: the temperature of the reaction front is 1000-2000 ℃, the speed of the reaction front is 5-30m/s, and the reaction release energy is 500-1500J/g. With the preferred conditions, the body of material containing the adhesive and fusible link material can be melted and formed into a solder layer quickly, avoiding excessive heating of the piezoelectric ceramic.
In some embodiments of the present invention, it is preferable that the piezoelectric ceramic is pretreated before the step (2); further preferably, the pre-treatment comprises: and carrying out heat treatment and/or coating treatment on the surface to be contacted of the piezoelectric ceramic.
In a preferred embodiment, the conditions of the heat treatment include: the temperature of the heat treatment is not higher than the curie temperature of the piezoelectric ceramic and the connecting body and not higher than the melting point temperature of the reaction foil. The optimal conditions are adopted, so that the welding time is reduced, and the loss of the crystal structure and the physical properties of the piezoelectric ceramic caused by excessive heating is avoided.
In another preferred embodiment, the coating process comprises: and forming a metal coating with the thickness of 50-100nm on the surface to be contacted of the piezoelectric ceramic. The optimal conditions are adopted, so that the welding strength of the piezoelectric ceramics and the material body is improved.
According to the invention, preferably, the melting temperature of the metal coating is lower than the temperature of the leading edge of the reactive foil; further preferably, the metal in the metal coating is selected from at least one of silver, copper and chromium, preferably silver and/or chromium.
In the present invention, there is a wide selection range for the kind of the piezoelectric ceramics, and preferably, the piezoelectric ceramics is selected from a disc-shaped piezoelectric ceramics and/or a column-shaped piezoelectric ceramics, wherein the disc-shaped piezoelectric ceramics has a thickness of 0.1 to 1mm and a diameter of 1 to 10mm, and the column-shaped piezoelectric ceramics has a height of 1 to 20mm and a diameter of 5 to 30mm, but the present invention is not limited thereto.
In the present invention, there is a wide selection range of the material body, preferably, the material body is selected from metal and/or nonmetal, wherein the metal is selected from metal simple substance and/or alloy, wherein the metal simple substance can be selected from copper, gold, nickel, aluminum, etc., and the alloy can be selected from type 1 superconductor, type 2 superconductor, kovar alloy, etc.; the non-metal is selected from ceramics, piezoelectric ceramics, sapphire, amorphous, etc.
The invention provides a piezoelectric ceramic composite material prepared by the method provided by the first aspect.
According to the invention, preferably, the composite material comprises: the piezoelectric ceramic comprises piezoelectric ceramic, a material body and a welding layer arranged between the piezoelectric ceramic and the material body.
In the present invention, the solder layer is formed by fusing the interconnect as described above. The composition of the solder layer formed can include all of the chemical elements of the interconnect. The formed welding layer having such a composition can improve the effect of improving the welding strength between the piezoelectric ceramic and the material body.
In some preferred embodiments of the present invention, in order to improve the weld firmness of the piezoelectric ceramic and the material body, it is preferable that the parameters of the weld layer satisfy: the tensile strength is 20-80MPa, the elastic modulus is 1-20GPa, the shear strength is 20-70MPa, the shear modulus is 1-10GPa, the Poisson ratio is 0.1-0.5 mu, the dielectric loss tangent is 0.001-0.01%, the resonance frequency is 10-50kHz, and the resonance gap is 0.1-1kHz; the parameters of the weld layer were measured using a model FM-250 WPM Masch2168 tensile tester.
Compared with the existing piezoelectric ceramics, the piezoelectric ceramic composite material provided by the invention has the advantages that the piezoelectric ceramics and the fusible connecting material are connected, so that the firmness of the piezoelectric ceramics and the fusible connecting material is improved under the condition of not damaging the piezoelectric ceramics.
A third aspect of the present invention provides a use of the piezoelectric ceramic composite material provided in the first and third aspects in electronic and optical devices.
The present invention will be described in detail below by way of examples.
The thickness of the reactive foil, the thickness of the adhesive and the thickness of the fusible link material were measured by scanning electron microscopy;
parameters of the weld layer (tensile strength, elastic modulus, shear strength, shear modulus, poisson's ratio, dielectric loss tangent, resonance frequency, resonance gap) were measured using an FM-250 model WPM Masch2168 tensile tester;
the performance parameters of the piezoelectric ceramic composite material are measured by monitoring an electromechanical vibration system.
The properties of the reactive foils obtained in preparation examples 1 to 10 and the specific parameters of the interconnect are shown in Table 1.
Preparation example 1
(1)Preparation of the reaction foil: coating a layer of photoresist on the surface of a silicon substrate, and then alternately depositing a nickel layer and an aluminum layer on the surface of the photoresist, wherein the purities of the nickel layer and the aluminum layer are respectively 99.99% and 99.99%, and the sputtering atomic ratio is 1:1, deposition thickness ratio of 1:1, the pressure of a cavity is less than 10mTorr, the atmosphere of the cavity is high-purity argon, the sum of the thicknesses of a single nickel layer and a single aluminum layer after deposition is 7-20nm, the thickness of a reaction foil is 28-80 mu m, a silicon substrate deposited with the nickel layer and the aluminum layer is immersed in an acetone solution, photoresist is melted, and the silicon substrate is separated from the reaction foil to obtain a reaction foil O1;
wherein, the TEM image of the reaction foil O1 is shown in FIG. 3, wherein the light phase is Al and the dark phase is Ni; fig. 3 (a) is a TEM image before magnetron deposition, and fig. 3 (b) is a TEM image after magnetron deposition.
(2)Preparation of the linker: sequentially coating silver-based materials on the upper surface and the lower surface of the reaction foil, wherein the thicknesses of the first adhesive layer and the second adhesive layer are both 80nm; and then respectively coating tin-based fusible connecting materials on the first adhesive layer and the second adhesive layer by adopting an electroplating method, wherein the thicknesses of the first fusible connecting material layer and the second fusible connecting material layer are both 10 mu m, and obtaining the connector P1.
Preparation examples 2 to 10
Linker P2-10 was obtained according to the procedure of preparation example 1, except that the specific parameters of the linker were different.
TABLE 1
Figure BDA0003000041950000101
Note: * Thickness range of the layer formed of the adhesive, thickness range of the layer formed of the fusible link material.
TABLE 1
Figure BDA0003000041950000111
Note: * A thickness range of the layer formed of the adhesive, a thickness range of the layer formed of the fusible link material.
TABLE 1
Figure BDA0003000041950000112
The characteristics of the solder layers in the piezoelectric ceramic composites obtained in examples 1 to 10 are shown in Table 2.
Example 1
(1) The connecting body P1 was disposed between a piezoelectric ceramic (available from Morgan matrix Ltd and russian Avrora-Elma corporation, usa) and a material body (copper plate);
(2) Applying pressure to make the piezoelectric ceramic, the connecting body P1 and the material body contact;
(3) Before contact, carrying out heat treatment and coating treatment on the surface to be contacted of the piezoelectric ceramic, wherein the heat treatment temperature is not higher than the Curie temperature of the piezoelectric ceramic and the melting temperature of the reaction foil, and the coating treatment forms a silver coating with the thickness of 60nm on the surface to be contacted of the piezoelectric ceramic;
(4) And igniting the self-propagating reaction of the reaction foil by laser to melt the connector P1 and form a welding layer Q1, so as to obtain the piezoelectric ceramic composite material S1.
Examples 2 to 10
A piezoelectric ceramic composite material S2 to S10 comprising the solder layers Q2 to Q10 was obtained by following the procedure of example 1 except that the kind of the connected body, the applied pressure, the temperature of the heat treatment and the thickness of the metal coating were changed;
wherein the types of the connecting bodies are respectively replaced by P2-P10.
TABLE 2
Figure BDA0003000041950000121
Figure BDA0003000041950000131
As can be seen from the data in Table 2, the method provided by the invention can reliably weld the piezoceramic material in extremely short time (1-2 ms) without losing the functional characteristics of the material (the measured parameters of the electromechanical oscillation system conform to the standards of GOST 12370-80, GOST R57438-2017 and GOST R8.945-2018).
Test example
The welding layers Q1 to Q10 of the piezoelectric ceramic composite materials (S1 to S10) obtained in examples 1 to 10 were fusion-welded at temperatures higher than the melting point temperatures of the respective fusible connecting materials, respectively, to obtain a piezoelectric ceramic and a material body after being fusion-welded, wherein the piezoelectric ceramic after being fusion-welded did not lose its functional characteristics and could be reused.
Therefore, the piezoelectric ceramic composite material obtained by the method provided by the invention effectively improves the connectivity of the fusible connecting material and the piezoelectric ceramic on the premise of not destroying the functional characteristics of the piezoelectric ceramic, and can be subjected to unsoldering under the condition of not destroying the piezoelectric ceramic.
The preferred embodiments of the present invention have been described above in detail, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, many simple modifications can be made to the technical solution of the invention, including combinations of various technical features in any other suitable way, and these simple modifications and combinations should also be regarded as the disclosure of the invention, and all fall within the scope of the invention.

Claims (23)

1. A preparation method of a piezoelectric ceramic composite material is characterized by comprising the following steps:
(1) Disposing a connecting body between the piezoelectric ceramic and the material body, wherein the connecting body comprises a reaction foil, and a first adhesive and a first fusible link material sequentially coated on an upper surface of the reaction foil, and a second adhesive and a second fusible link material sequentially coated on a lower surface of the reaction foil;
(2) Applying pressure to bring the piezoelectric ceramic, the connecting body and the material body into contact;
(3) Igniting the reaction foil to carry out self-propagating reaction, so that the connecting body is melted and a welding layer is formed;
wherein, before step (2), the piezoelectric ceramic is pretreated;
wherein the thickness of the reaction foil is 10-100 μm;
the reaction foil comprises metal layers and non-metal layers which are alternately stacked, and the sum of the thicknesses of the single-layer metal layers and the single-layer non-metal layers is 2-20nm;
the total number of the metal layers and the nonmetal layers is 1000-8000;
the metal layer is a layer formed of at least one element of nickel, aluminum, copper, niobium, cobalt, titanium, molybdenum, and tantalum;
the non-metal layer is a layer formed of at least one element of carbon, silicon, and boron;
wherein the thickness of the layer formed by the first adhesive and the second adhesive is 20-150nm;
wherein the thickness of each layer formed of the first and second fusible link materials is 1-20 μm;
the conditions of the self-propagating reaction include: the temperature of the reaction front is 1000-2000 ℃, the speed of the reaction front is 5-30m/s, and the reaction release energy is 500-1500J/g.
2. The method according to claim 1, wherein the reaction foil is 20-80 μm thick.
3. The method of claim 1, wherein the total number of metal and non-metal layers is 2000-6000 layers.
4. The method of claim 1, wherein the first and second binders are the same or different, each of the first and second binders being independently selected from at least one of a silver-based material, a gold-based material, and a copper-based material.
5. The method of claim 1, wherein the first and second adhesives each form a layer having the same or different thickness.
6. The method according to claim 5, wherein the first adhesive and the second adhesive each form a layer having a thickness of 30-120nm.
7. The method of any of claims 1-6, wherein the first and second fusible link materials are the same or different, each being independently selected from a tin-based material and/or a bismuth-based material.
8. The method according to claim 1, wherein the thickness of the layer formed by each of the first and second fusible link materials is the same or different.
9. The method according to claim 8, wherein the layer of each of the first and second fusible link materials is 2-15 μm thick.
10. The method of claim 1, wherein the applied pressure is 0.5-2.5kg/cm 2
11. The method of claim 10, whereinThe applied pressure is 0.7-2.2kg/cm 2
12. The method of claim 1, wherein the time of melting is 1-60ms.
13. The method of claim 12, wherein the time of melting is 5-30ms.
14. The method according to any one of claims 1-6, wherein the ignition means is selected from thermal ignition, laser ignition, combustion ignition, voltage ignition.
15. The method of any of claims 1-6, wherein the pre-processing comprises: and carrying out heat treatment and/or coating treatment on the surface to be contacted of the piezoelectric ceramic.
16. The method of claim 15, wherein the conditions of the heat treatment comprise: the temperature of the heat treatment is not higher than the Curie temperature of the piezoelectric ceramic and not higher than the melting point temperature of the reaction foil.
17. The method of claim 15, wherein the coating process comprises: and forming a metal coating with the thickness of 50-100nm on the surface to be contacted of the piezoelectric ceramic.
18. The method of claim 17, wherein the melting temperature of the metal coating is lower than the leading edge temperature of the reactive foil.
19. The method of claim 17, wherein the metal in the metal coating is selected from at least one of silver, copper, and chromium.
20. A piezoelectric ceramic composite material produced by the method according to any one of claims 1 to 19.
21. The composite material of claim 20, wherein the composite material comprises: the piezoelectric ceramic comprises piezoelectric ceramic and a material body, and a welding layer arranged between the piezoelectric ceramic and the material body.
22. The composite of claim 21, wherein the parameters of the weld layer satisfy: the tensile strength is 20-80MPa, the elastic modulus is 1-20GPa, the shear strength is 20-70MPa, the shear modulus is 1-10GPa, the Poisson ratio is 0.1-0.5 mu, the dielectric loss tangent is 0.001-0.01%, the resonance frequency is 10-50kHz, and the resonance gap is 0.1-1kHz.
23. Use of a piezoelectric ceramic composite material according to any one of claims 21 to 22 in electronic and optical devices.
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EP1648652A4 (en) * 2003-07-23 2008-01-09 Univ Johns Hopkins Method of joining using reactive multilayer foils with enhanced control of molten joining materials
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