CN113149714A - Aluminum diamond composite material with aluminum silicon carbide layer coated on surface and preparation method and application thereof - Google Patents

Aluminum diamond composite material with aluminum silicon carbide layer coated on surface and preparation method and application thereof Download PDF

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CN113149714A
CN113149714A CN202110421812.3A CN202110421812A CN113149714A CN 113149714 A CN113149714 A CN 113149714A CN 202110421812 A CN202110421812 A CN 202110421812A CN 113149714 A CN113149714 A CN 113149714A
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aluminum
silicon carbide
diamond
carbide layer
particles
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熊德赣
陈柯
杨盛良
陈迎龙
肖浩
蒋文评
傅志
袁惠程
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Hunan Harvest Technology Development Co ltd
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    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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    • C04B41/00After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
    • C04B41/80After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
    • C04B41/81Coating or impregnation
    • C04B41/85Coating or impregnation with inorganic materials
    • C04B41/88Metals
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    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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    • C04B35/515Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
    • C04B35/56Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
    • C04B35/565Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
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    • 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
    • C04B35/00Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • 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
    • C04B41/00After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
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    • 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
    • C04B41/00After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
    • C04B41/45Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
    • C04B41/50Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
    • C04B41/51Metallising, e.g. infiltration of sintered ceramic preforms with molten metal
    • C04B41/515Other specific metals
    • C04B41/5155Aluminium

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Abstract

The invention discloses an aluminum diamond composite material with an aluminum silicon carbide layer coated on the surface, a preparation method and application thereof, wherein the preparation method comprises the following steps: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises an aluminum matrix and surface-modified diamond particles; the surface aluminum silicon carbide layer comprises an aluminum matrix and silicon carbide particles, the volume fraction of the silicon carbide particles is 60-75%, and the aluminum matrix in the surface aluminum silicon carbide layer and the aluminum matrix in the aluminum diamond core material are in a continuous distribution phase. According to the aluminum diamond composite material with the surface coated with the aluminum silicon carbide, the aluminum silicon carbide layer on the surface can prevent diamond particles in the aluminum diamond core material from being exposed, so that the machining difficulty and the surface roughness of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer are reduced. The surface aluminum silicon carbide layer has high thermal conductivity and expansion coefficient, is matched with the aluminum diamond core material, and has lower interface stress between the aluminum silicon carbide layer and the aluminum diamond core material, thereby meeting the use in the aerospace field with high temperature cycle requirement.

Description

Aluminum diamond composite material with aluminum silicon carbide layer coated on surface and preparation method and application thereof
Technical Field
The invention relates to the field of electronic packaging materials for electronic information industry, in particular to an aluminum diamond composite material with an aluminum silicon carbide layer coated on the surface. In addition, the invention also relates to a preparation method and application of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer.
Background
With the great application of chips such as high-power third-generation semiconductor gallium nitride and the like and the gradual row installation of high-energy laser weapons, the heat dissipation requirement on packaging materials is increasingly strict. The existing packaging materials such as copper/molybdenum/copper, aluminum silicon carbide and the like have limited heat dissipation capability and are difficult to meet the packaging requirements of high-power electronic devices, and the development of a new generation of high-thermal-conductivity packaging material becomes a problem to be solved urgently in the development and application of high-power devices.
Diamond is the best material for heat conduction in nature, the heat conductivity can reach 2200W/(m.K) at the maximum under normal temperature, and the thermal expansion coefficient is 8.6 multiplied by 10-7And the/K meets the use requirements of high thermal conductivity and low expansion coefficient of the electronic packaging material. Aluminum and its alloys are one of the most important engineering materials in the industrial field, and have excellent thermal and electrical conductivity. The diamond and the aluminum matrix are combined together, so that the diamond-aluminum composite material not only has higher thermal conductivity, but also meets the requirements of low expansion and light weight of electronic packaging devices, and is a novel electronic packaging material with high competitiveness. Therefore, the aluminum diamond composite material is becoming a research hotspot of a new generation of packaging materials.
After more than ten years of research and development, the preparation method of the aluminum diamond composite material is mature day by day, the powder metallurgy method, the discharge plasma sintering method, the pressure infiltration method and the like are mainly shown, and the main performance indexes of the prepared aluminum diamond composite material reach the advanced level.
The patent CN202010087108.4 infiltration preparation process of diamond-metal composite material and diamond-metal composite material propose to limit the floating of diamond particles in copper liquid during infiltration process by using wire mesh method, which can form thin metal layers on upper and lower surfaces, but the side surface is not easy to obtain thin metal layers, and is especially not suitable for aluminum diamond and copper diamond shaped pieces and complex pieces.
Patent CN201910868939.2 discloses a ceramic membrane modified diamond/aluminum composite material and its pressureless infiltration preparation process, which comprises the following steps: plating a ceramic film on the surface of the diamond powder, wherein the thickness of the film is 30-300 nm; and placing an aluminum alloy ingot on the diamond powder prefabricated body, and heating in a nitrogen atmosphere with the pressure of 0.08-0.15 MPa to obtain the diamond/aluminum composite material. The surface of the aluminum diamond material has no metal layer, and diamond particles are exposed outside.
The patent CN201910412310.7 invention proposes that diamond particles with the particle size of more than 400 mu m and a mixture of diamond particles with double particle sizes are used as a reinforcing phase to increase the volume fraction of diamond, and a composite material is prepared by using an air pressure infiltration method, so that the diamond/aluminum composite material with ultrahigh thermal conductivity and low density is obtained. The surface of the aluminum diamond material is not covered by other materials, and the diamond particles are easy to expose outside.
Patent CN201711045332.1 first prepares a near net shape mold; then coating the surface of diamond powder; then carrying out assembly air pressure leaching; finally, demoulding to obtain the diamond/aluminum composite material. The surface of the aluminum diamond material is not covered by other materials, and the diamond particles are easy to be exposed outside.
In the preparation process of the aluminum diamond parts prepared at present in China, diamond particles are easy to expose, and the exposure of the diamond particles causes the following two problems:
(1) the surface roughness of the aluminum diamond part is higher, and the performance of the composite material is influenced when the aluminum diamond part is connected with a semiconductor chip or a ceramic substrate. In order to reduce the surface roughness, a metal layer is usually plated with nickel, gold or sprayed on the surface of the aluminum-diamond composite material, and then the metal layer is polished. Although the surface roughness of the aluminum diamond composite material can be greatly reduced by the process, the process is complex and the coating is thick. Because the difference of the thermal expansion coefficients of the diamond particles and the thick metal coating is large, the coating bulges and falls off due to the interface stress easily generated in the application process, and the coating can not meet the application in the fields of aerospace and the like with high temperature cycle requirements.
(2) Because diamond is the most difficult material to process, when diamond particles are exposed, in order to ensure the dimensional accuracy and the flatness of products, only grinding technology or laser etching technology can be adopted for processing, which leads to low processing efficiency and high product cost. Especially when the product drawing has a threaded hole or a step hole, the laser etching process is difficult to complete.
Disclosure of Invention
The invention provides an aluminum diamond composite material with an aluminum silicon carbide layer coated on the surface, and a preparation method and application thereof, and aims to solve the technical problem that diamond particles are easy to be exposed in the preparation process of the currently prepared aluminum diamond parts in China, and the application range of an aluminum diamond product is limited.
The technical scheme adopted by the invention is as follows:
an aluminum-diamond composite having a surface coated with an aluminum-silicon carbide layer, comprising: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises an aluminum matrix and surface-modified diamond particles; the surface aluminum silicon carbide layer comprises an aluminum matrix and silicon carbide particles, and the volume fraction of the silicon carbide particles is 60-75%.
Further, the aluminum matrix in the surface aluminum silicon carbide layer and the aluminum matrix in the aluminum diamond core material are in a continuous distribution phase.
Furthermore, the thickness of the surface aluminum silicon carbide layer is 0.03 mm-0.20 mm.
According to another aspect of the present invention, there is also provided a method for preparing a copper-diamond composite material with a metal layer coated on a surface thereof, comprising the steps of:
preparing a silicon carbide prefabricated part: forming silicon carbide particles to prepare a silicon carbide prefabricated part blank, and heating and sintering the silicon carbide prefabricated part blank in a vacuum or protective atmosphere to obtain a silicon carbide prefabricated part with the porosity of 25-40%;
machining a silicon carbide prefabricated part: machining the silicon carbide prefabricated part by adopting a numerical control milling process to form the silicon carbide prefabricated part for coating the diamond particles with the modified surfaces;
loading of surface modified diamond particles: carrying out surface modification treatment on the diamond particles to obtain surface-modified diamond particles, and filling the surface-modified diamond particles into the machined silicon carbide prefabricated part to form a composite blank;
and (3) aluminizing: and placing the composite blank and the aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing and heating to melt the aluminum matrix into aluminum liquid and pouring the aluminum liquid onto the composite blank, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace to increase the pressure in the furnace, so that the aluminum liquid is infiltrated into pores of the silicon carbide prefabricated part and the surface-modified diamond particles in the composite blank under the action of gas pressure, and cooling to obtain the aluminum-diamond composite material with the surface coated with the aluminum-silicon carbide layer.
Further, in the step of preparing the silicon carbide preform, the silicon carbide particles have a particle diameter of 45 to 125 μm.
Further, the molding treatment of the silicon carbide particles adopts one of a dry method molding method, an injection molding method and a gel injection molding method; the temperature of the heating sintering is 800-1000 ℃, and the time is 1-5 h.
Further, in the step of loading the surface-modified diamond particles, the surface-modified diamond particles have a particle diameter of 80 to 450 μm.
Further, the step of aluminizing specifically includes: placing the composite blank in a graphite mold, placing the graphite mold with the composite blank and an aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing, heating the double chambers, controlling the temperature of a lower treatment chamber provided with the graphite mold to be 570-680 ℃, controlling the temperature of an upper treatment chamber provided with the aluminum matrix to be 680-800 ℃, pouring aluminum liquid formed by the aluminum matrix onto the composite blank of the graphite mold, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to be 1-10 MPa, keeping constant temperature and constant pressure for 5-30 min, so that the aluminum liquid is infiltrated into pores of a silicon carbide prefabricated part and pores of surface-modified diamond particles in the composite blank under the action of gas pressure, cooling and taking out.
Further, in the step of aluminizing, the aluminum substrate is one of pure aluminum, 3003 aluminum alloy, 6061 aluminum alloy, 6063 aluminum alloy, ZL102 aluminum alloy, and ZL101A aluminum alloy.
Further, in the step of aluminizing, a precision machining treatment is also included after cooling.
The invention has the following beneficial effects:
the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer comprises an aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material, wherein the surface aluminum silicon carbide layer can prevent diamond particles in the aluminum diamond core material from being exposed, so that the machining difficulty in preparing parts is reduced, and the surface roughness of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer is also reduced. Meanwhile, the surface aluminum silicon carbide layer has higher thermal conductivity, and the expansion coefficient is matched with the aluminum diamond layer, so that the interface stress between the aluminum diamond core material and the surface aluminum silicon carbide layer is lower, and the aluminum diamond composite material with the nickel-plated surface and the aluminum silicon carbide layer coated on the surface can be brazed with Kovar and other expansion alloys, titanium alloy, copper and the like by adopting silver-based brazing, so that the high-temperature-cycle-requirement aerospace field can be met. Moreover, the aluminum diamond core material enables the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer to have the excellent characteristics of high heat conduction, low expansion coefficient and light weight. And compare single aluminium carborundum combined material, the aluminium diamond core makes the aluminium diamond combined material of surface coating aluminium carborundum layer have higher heat conduction, and compare in the copper diamond combined material of surface coating copper, the coefficient of expansion of surface aluminium carborundum layer and aluminium diamond core is more similar, interfacial stress is littleer in the use, and easily processing on the surface aluminium carborundum layer, the aluminium diamond combined material of surface coating aluminium carborundum layer has simultaneously significantly reduced the quantity and the energy consumption of diamond, and the production cost is reduced.
In addition to the objects, features and advantages described above, other objects, features and advantages of the present invention are also provided. The present invention will be described in further detail below with reference to the accompanying drawings.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this application, illustrate embodiments of the invention and, together with the description, serve to explain the invention and not to limit the invention. In the drawings:
FIG. 1 is a schematic structural view of an aluminum diamond composite material having a surface coated with an aluminum silicon carbide layer prepared in accordance with preferred embodiment 1 of the present invention;
FIG. 2 is a cross-sectional view A-A of preferred embodiment 1 of the present invention, 1, a silicon carbide preform box, 2, a silicon carbide preform cover, 3, diamond particles;
FIG. 3 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 2 of the present invention;
FIG. 4 is a sectional view taken along line B-B of the preferred embodiment 2 of the present invention;
FIG. 5 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 3 of the present invention;
FIG. 6 is a structural view of the preferred embodiment 3 of the present invention;
FIG. 7 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 4 of the present invention; and
fig. 8 is a C-C sectional view of the preferred embodiment 4 of the present invention.
Detailed Description
It should be noted that the embodiments and features of the embodiments in the present application may be combined with each other without conflict. The present invention will be described in detail below with reference to the embodiments with reference to the attached drawings.
FIG. 1 is a schematic structural view of an aluminum diamond composite material having a surface coated with an aluminum silicon carbide layer prepared in accordance with preferred embodiment 1 of the present invention; FIG. 2 is a sectional view A-A of the preferred embodiment 1 of the present invention; FIG. 3 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 2 of the present invention; FIG. 4 is a sectional view taken along line B-B of the preferred embodiment 2 of the present invention; FIG. 5 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 3 of the present invention; FIG. 6 is a structural view of the preferred embodiment 3 of the present invention; FIG. 7 is a front view showing the structure of an aluminum diamond component part having a surface aluminum silicon carbide layer prepared according to preferred embodiment 4 of the present invention; fig. 8 is a C-C sectional view of the preferred embodiment 4 of the present invention.
The aluminum diamond composite material with the aluminum silicon carbide layer coated on the surface comprises: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises an aluminum matrix and surface-modified diamond particles; the surface aluminum silicon carbide layer comprises an aluminum matrix and silicon carbide particles, and the volume fraction of the silicon carbide particles is 60-75%.
The aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer comprises an aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material, wherein the surface aluminum silicon carbide layer can prevent diamond particles in the aluminum diamond core material from being exposed, so that the machining difficulty in preparing parts is reduced, and the surface roughness of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer is reduced. Meanwhile, the surface aluminum silicon carbide layer has higher thermal conductivity, and the expansion coefficient is matched with the aluminum diamond layer, so that the interface stress between the aluminum diamond core material and the surface aluminum silicon carbide layer is lower, and the aluminum diamond composite material with the nickel-plated surface and the aluminum silicon carbide layer coated on the surface can be brazed with Kovar and other expansion alloys, titanium alloy, copper and the like by adopting silver-based brazing, so that the high-temperature-cycle-requirement aerospace field can be met. Moreover, the aluminum diamond core material enables the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer to have the excellent characteristics of high heat conduction, low expansion coefficient and light weight. And compare single aluminium carborundum combined material, the aluminium diamond core makes the aluminium diamond combined material of surface coating aluminium carborundum layer have higher heat conduction, and compare in the copper diamond combined material of surface coating copper, the coefficient of expansion of surface aluminium carborundum layer and aluminium diamond core is more similar, interfacial stress is littleer in the use, and easily processing on the surface aluminium carborundum layer, the aluminium diamond combined material of surface coating aluminium carborundum layer has simultaneously significantly reduced the quantity of diamond, and the energy consumption, and the production cost is reduced.
The volume fraction of the silicon carbide particles is 60-75%, and when the volume fraction of the silicon carbide particles is less than 60%, the difference between the expansion coefficient of the surface aluminum silicon carbide and the expansion coefficient of the core aluminum diamond is large, so that the stress at the interface between the surface aluminum silicon carbide and the core aluminum diamond is increased, and the reliability of parts in the aerospace field is reduced. When the volume fraction of the silicon carbide particles is more than 75%, the processing characteristics of the aluminum silicon carbide material are deteriorated, and the wear of the processing tool is remarkably increased.
In this embodiment, the aluminum matrix in the aluminum silicon carbide layer on the surface and the aluminum matrix in the aluminum diamond core material are in a continuous distribution phase. The aluminum matrix in the surface aluminum silicon carbide layer and the aluminum matrix in the aluminum diamond core material are in a continuous distribution phase, and in the preparation process of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer, the aluminum matrix in the surface aluminum silicon carbide layer and the aluminum matrix in the aluminum diamond core material are synchronously formed to form the continuous distribution phase, so that the high air tightness and the high bonding strength of the interface between the aluminum silicon carbide layer and the aluminum diamond core material are ensured.
In this embodiment, the thickness of the aluminum silicon carbide layer on the surface is 0.03mm to 0.20 mm. Preferably, the thickness of the surface aluminum silicon carbide layer is 0.05 mm-0.10 mm. The thermal conductivity of the aluminum silicon carbide ranges from 180W/(m.K) to 200W/(m.K), the thermal conductivity of the aluminum diamond is larger than 450W/(m.K), the thinner the surface aluminum silicon carbide layer is to improve the thermal conductivity of the aluminum diamond part with the surface coated with the aluminum silicon carbide layer, but from the viewpoint of production process control, the qualification rate of the part is obviously reduced after the surface aluminum silicon carbide layer is less than 0.03 mm. The surface aluminum silicon carbide layer is coated outside the aluminum diamond core material, so that the surface aluminum silicon carbide layer can be processed by adopting a conventional machining method, the production efficiency is high, and the size precision is high.
According to another aspect of the present invention, there is also provided a method for preparing a copper-diamond composite material with a metal layer coated on a surface thereof, comprising the steps of:
preparing a silicon carbide prefabricated part: forming silicon carbide particles to prepare a silicon carbide prefabricated part blank, and heating and sintering the silicon carbide prefabricated part blank in a vacuum or protective atmosphere to obtain a silicon carbide prefabricated part with the porosity of 25-40%;
machining a silicon carbide prefabricated part: machining the silicon carbide prefabricated part by adopting a numerical control milling process to form the silicon carbide prefabricated part for coating the diamond particles with the modified surfaces;
loading of surface modified diamond particles: carrying out surface modification treatment on the diamond particles to obtain surface-modified diamond particles, and filling the surface-modified diamond particles into the machined silicon carbide prefabricated part to form a composite blank;
and (3) aluminizing: and placing the composite blank and the aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing and heating to melt the aluminum matrix into aluminum liquid and pouring the aluminum liquid onto the composite blank, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace to increase the pressure in the furnace, so that the aluminum liquid is infiltrated into pores of the silicon carbide prefabricated part and the surface-modified diamond particles in the composite blank under the action of gas pressure, and cooling to obtain the aluminum-diamond composite material with the surface coated with the aluminum-silicon carbide layer.
The preparation method of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer comprises the steps of firstly preparing a preformed porous silicon carbide prefabricated part and processing the prefabricated part into a structure capable of embedding the diamond particles with the surface modified, secondly filling the diamond particles with the surface modified into the silicon carbide prefabricated part, then preparing the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer by adopting a vacuum pressure infiltration process, and further adopting a precision machining technology to obtain required parts according to requirements. The preparation method is simple, efficient and low in cost, and the prepared aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer is high in thermal conductivity and low in thermal expansion coefficient. In the process of aluminizing, aluminizing the composite blank, allowing molten aluminum to enter the composite blank through gaps of the composite blank, fully contacting the molten aluminum with the surface-modified diamond particles, and cooling to form an aluminum diamond core material; the aluminum liquid fully contacts with the silicon carbide prefabricated part, a surface aluminum silicon carbide layer is formed after cooling, the expansion coefficient of the surface aluminum silicon carbide layer is good in matching performance with the aluminum diamond core material, the bonding strength with the aluminum diamond layer is higher, and the aluminum silicon carbide prefabricated part can be used in the fields of aerospace and the like with high temperature cycle requirements.
Machining the silicon carbide prefabricated part: the silicon carbide preform is machined using a numerically controlled milling process to produce a silicon carbide preform having a cavity, such as a rectangular or cylindrical body, containing the surface-modified diamond particles. And filling the diamond particles with the modified surfaces into the cavity of the silicon carbide prefabricated part after machining, and covering a silicon carbide prefabricated part cover plate to form a composite blank.
In this embodiment, the step of aluminizing specifically includes: placing the composite blank in a graphite mold, placing the graphite mold with the composite blank and an aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing, heating the double chambers, controlling the temperature of a lower treatment chamber provided with the graphite mold to be 570-680 ℃, controlling the temperature of an upper treatment chamber provided with the aluminum matrix to be 680-800 ℃, pouring aluminum liquid formed by the aluminum matrix onto the composite blank of the graphite mold, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to be 1-10 MPa, keeping constant temperature and constant pressure for 5-30 min, so that the aluminum liquid is infiltrated into pores of a silicon carbide prefabricated part and pores of surface-modified diamond particles in the composite blank under the action of gas pressure, cooling and taking out. According to the method for impregnating the aluminum matrix, the aluminum liquid is impregnated into the inner gap and the surface of the composite blank to form the surface aluminum silicon carbide layer and the aluminum diamond layer, and the aluminum liquid simultaneously impregnates the silicon carbide prefabricated part and the diamond pores with the modified surface to form a continuous distribution phase, so that the high air tightness and the high bonding strength of the interface of the aluminum silicon carbide layer and the aluminum diamond core material are ensured.
In this example, in the step of preparing the silicon carbide preform, the particle diameter of the silicon carbide particles is 45 μm to 125 μm. Under the same other conditions, the interface between the aluminum matrix and the aluminum silicon carbide particles is reduced with the increase of the silicon carbide particle size, so that the thermal conductivity of the aluminum silicon carbide is gradually improved, but the bending strength of the aluminum silicon carbide is gradually reduced, and the two performance indexes of the thermal conductivity and the bending strength are combined, so that the particle size of the silicon carbide particles is preferably 45-125 μm. Therefore, the aluminum silicon carbide has higher thermal conductivity, and the formed surface aluminum silicon carbide layer can be processed by adopting a conventional mechanical method, so that the problem that the existing aluminum diamond composite material is difficult to process is solved.
In this embodiment, the molding treatment of the silicon carbide particles is performed by one of a dry molding method, an injection molding method, and a gel injection molding method. The temperature of the heating sintering is 800-1000 ℃, and the time is 1-5 h. Forming the silicon carbide particles into a silicon carbide prefabricated part blank by a dry method mould pressing method, an injection molding method and a gel injection molding method; and sintering at 800-1000 ℃ for 1-5 h to obtain the silicon carbide prefabricated part with the porosity of 25-40%, so that the aluminum liquid enters the pores of the silicon carbide prefabricated part through the gaps in the aluminum matrix infiltration process.
In this example, in the step of loading the surface-modified diamond particles, the particle diameter of the surface-modified diamond particles was 80 μm to 450 μm. In the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer, under the same other conditions, the interface between the aluminum matrix and the diamond particles is reduced along with the increase of the particle size of the diamond particles, so that the thermal conductivity of the aluminum diamond is gradually improved, but the bending strength of the aluminum diamond is gradually reduced, and two performance indexes of the thermal conductivity and the bending strength are combined, so that the particle size of the diamond particles with the modified surface is preferably 80-450 μm.
In the embodiment, the surface modification treatment process of the diamond particles adopts a magnetron sputtering method, when the magnetron sputtering method is adopted, metal powder is firstly magnetron sputtered on the surfaces of the diamond particles, and the thickness of a metal layer formed by the metal powder is 100 nm-300 nm; then the mixture is put under the conditions of vacuum degree of 8Pa to 12Pa, temperature of 1150 ℃ to 1350 ℃ and time of 2h to 4h for reaction to obtain the diamond particles with modified surfaces. Or, the diamond particles are subjected to a surface modification treatment process by adopting a high-temperature reaction method. When a high-temperature reaction method is adopted, the diamond particles and the metal powder are mixed and react under the conditions that the vacuum degree is 0.4 Pa-0.6 Pa, the temperature is 1000-1200 ℃ and the time is 1.5-2.5 h, so that the diamond particles with modified surfaces are obtained. The metal powder is one of tungsten powder, molybdenum powder and iridium powder.
In this example, in the step of impregnating with aluminum, the aluminum matrix is one of pure aluminum, 3003 aluminum alloy, 6061 aluminum alloy, 6063 aluminum alloy, ZL101A aluminum alloy, and ZL102 aluminum alloy.
In this embodiment, the step of impregnating with aluminum further includes precision machining after cooling. The outer layer of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer is the surface aluminum silicon carbide layer, so that precise machining can be realized, and the aluminum diamond composite material part with the surface coated with the aluminum silicon carbide layer is obtained.
According to another aspect of the invention, the application of the aluminum diamond composite material with the surface coated with the aluminum silicon carbide layer obtained by the preparation method in aerospace parts is further provided. The aluminum diamond composite material with the aluminum silicon carbide layer coated on the surface has the advantages of high thermal conductivity, low thermal expansion coefficient and the like, is high in bending strength, and can be used in the fields of aerospace and the like with high temperature cycle requirements.
Examples
Example 1
An aluminum diamond composite material having a surface coated with an aluminum silicon carbide layer, comprising: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises pure aluminum and surface modified diamond particles; the surface aluminum silicon carbide layer is pure aluminum and silicon carbide particles, and the volume fraction of the silicon carbide particles is 65%.
As shown in fig. 1 and 2, the method for preparing the aluminum diamond composite material with the aluminum silicon carbide layer coated on the surface comprises the following steps:
preparing a silicon carbide prefabricated part: the mixed granulation silicon carbide powder with the grain size of 45 microns and the grain size of 100 microns is molded into a frame with the grain size of 40mm multiplied by 2mm under the pressure of 150MPa to prepare a silicon carbide prefabricated part blank, and the silicon carbide prefabricated part with the porosity of 25 percent is obtained by sintering at the constant temperature of 800 ℃ for 1h under the vacuum condition;
machining a silicon carbide prefabricated part: processing the silicon carbide prefabricated part by adopting a numerical control milling process to obtain a silicon carbide prefabricated part box body with a cavity inside and a silicon carbide prefabricated part cover plate for containing surface-modified diamond particles;
loading of surface modified diamond particles: carrying out surface modification treatment on diamond particles, uniformly mixing 2000 g of tungsten powder with the Fischer-Tropsch particle size of 3 microns and 300 g of diamond particles with the particle size of 80 microns, then placing the mixture in a vacuum furnace with the vacuum degree of 0.5Pa and the temperature of 1100 ℃ for keeping the temperature for 2 hours, reacting the tungsten powder with the diamond particles to obtain surface-modified diamond particles, filling the surface-modified diamond particles into a machined silicon carbide prefabricated part box body, and covering a silicon carbide prefabricated part cover plate to form a composite blank;
and (3) aluminizing: placing the composite blank in a graphite mould, placing the graphite mould with the composite blank and pure aluminum in a double-chamber vacuum air pressure infiltration furnace, firstly vacuumizing, heating the two chambers, controlling the temperature of the lower treatment chamber with the graphite mold to be 680 ℃, controlling the temperature of the upper treatment chamber with pure aluminum to be 800 ℃, pouring the molten pure aluminum on the composite blank of the graphite mold, stopping vacuumizing, introducing argon into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to 5MPa, keeping constant temperature and pressure for 5min, so that the aluminum liquid is impregnated into the silicon carbide prefabricated part and the surface modified diamond particle pores in the composite blank under the action of gas pressure, the silicon carbide prefabricated part and the surface modified diamond particle pores are taken out after being cooled, and (3) obtaining the surface aluminum silicon carbide layer with the thickness of 0.05mm coated on all the surfaces through precision machining, and obtaining the aluminum diamond composite material with the surface aluminum silicon carbide layer coated on the surface of 35mm multiplied by 1.0 mm.
Example 2
An aluminum diamond component having a surface aluminum silicon carbide layer comprising: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises 6063 aluminum alloy and surface-modified diamond particles; the surface aluminum silicon carbide layer comprises 6063 aluminum alloy and silicon carbide particles, and the volume fraction of the silicon carbide particles is 70%.
As shown in fig. 3 and 4, the method for manufacturing an aluminum diamond component having an aluminum silicon carbide layer on the surface thereof includes the steps of:
preparing a silicon carbide prefabricated part: gel casting silicon carbide particles with the particle size of 45 mu m into a frame with the size of 23mm multiplied by 6mm, preparing a silicon carbide prefabricated part blank, and sintering at the constant temperature of 1000 ℃ for 1h under the vacuum condition to obtain a silicon carbide prefabricated part with the porosity of 40%;
machining a silicon carbide prefabricated part: processing the silicon carbide prefabricated part blank by adopting a numerical control milling process to form a silicon carbide prefabricated part box body with a cavity inside and a silicon carbide prefabricated part cover plate for containing surface-modified diamond particles;
loading of surface modified diamond particles: carrying out surface modification treatment on diamond particles, carrying out magnetron sputtering on 5000 g of 150 mu m diamond micro powder to obtain a molybdenum layer with the thickness of 180nm, then placing the molybdenum layer and the diamond particles in a vacuum furnace with the vacuum degree of 10Pa and the temperature of 1150 ℃ for constant temperature for 2h, reacting the molybdenum layer and the diamond particles to obtain surface-modified diamond particles, filling the surface-modified diamond particles into a machined silicon carbide prefabricated part box body, and covering a silicon carbide prefabricated part cover plate to form a composite blank;
and (3) aluminizing: placing the composite blank in a graphite mould, placing the graphite mould with the composite blank and 6063 aluminum alloy in a double-chamber vacuum air pressure infiltration furnace, firstly vacuumizing, heating the two chambers, controlling the temperature of a lower treatment chamber provided with a graphite mold to be 640 ℃, controlling the temperature of a treatment chamber provided with 6063 aluminum alloy to be 760 ℃, pouring the 6063 aluminum alloy molten aluminum on the composite blank of the graphite mold, stopping vacuumizing, introducing argon into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to 10MPa, keeping constant temperature and pressure for 15min, so that the aluminum liquid is impregnated into the silicon carbide prefabricated part and the pores of the surface modified diamond particles in the composite blank under the action of gas pressure, the silicon carbide prefabricated part and the pores of the surface modified diamond particles are taken out after cooling, and obtaining a surface aluminum silicon carbide layer with the thickness of 0.2mm and covered on all surfaces through precision machining, and obtaining the aluminum diamond part with the surface coated with the aluminum silicon carbide and the thickness of 20mm multiplied by 4.0 mm.
Example 3
An aluminum diamond component having a surface aluminum silicon carbide layer comprising: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises ZL101A aluminum alloy and surface modified diamond; the surface aluminum silicon carbide layer comprises ZL101A aluminum alloy and silicon carbide particles, and the volume fraction of the silicon carbide particles is 72%.
As shown in fig. 5 and 6, the method for manufacturing an aluminum diamond component having an aluminum silicon carbide layer on the surface thereof includes the steps of:
preparing a silicon carbide prefabricated part: silicon carbide particles with the particle size of 70 mu m are injected and molded into a frame with the diameter of 12.5mm multiplied by 45mm to prepare a silicon carbide prefabricated part blank, and the silicon carbide prefabricated part blank is sintered at the constant temperature of 850 ℃ for 3h under the vacuum condition to obtain a silicon carbide prefabricated part blank with the porosity of 35 percent;
machining a silicon carbide prefabricated part: processing the silicon carbide prefabricated part blank by adopting a numerical control milling process to form a cylinder and a cover plate with a cavity inside, wherein the cylinder and the cover plate are used for containing surface-modified diamond particles;
loading of surface modified diamond particles: carrying out surface modification treatment on diamond particles, carrying out magnetron sputtering on 2500 g of 450 mu m diamond micro powder to form an iridium layer with the thickness of 150nm, then placing the iridium layer and the diamond particles in a vacuum furnace with the vacuum degree of 10Pa and the temperature of 1150 ℃ for constant temperature for 2h, reacting the iridium layer and the diamond particles to obtain surface-modified diamond particles, filling the surface-modified diamond particles into a machined cylinder, and covering a cover plate to form a composite blank;
and (3) aluminizing: placing the composite blank in a graphite mold, placing the graphite mold with the composite blank and ZL101A in a double-chamber vacuum air pressure infiltration furnace, vacuumizing, heating double chambers, controlling the temperature of a lower treatment chamber provided with the graphite mold to be 580 ℃, controlling the temperature of an upper treatment chamber provided with ZL101A to be 680 ℃, pouring ZL101A into molten aluminum, pouring the molten aluminum onto the composite blank of the graphite mold, stopping vacuumizing, introducing argon into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to be 2MPa, keeping constant temperature and constant pressure for 10min, so that the molten aluminum is infiltrated into the silicon carbide prefabricated part and the surface-modified diamond in the composite blank under the action of gas pressure, cooling and taking out. And (3) obtaining the surface aluminum silicon carbide layer with the thickness of 0.10mm coated on all the surfaces through precision turning, and obtaining the aluminum diamond part with the surface coated with the aluminum silicon carbide layer of the step cylinder.
Example 4
An aluminum diamond component having a surface aluminum silicon carbide layer comprising: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material; the aluminum diamond core material comprises 6063 aluminum alloy and surface-modified diamond particles; the surface aluminum silicon carbide layer comprises 6063 aluminum alloy and silicon carbide particles, and the volume fraction of the silicon carbide particles is 64%.
As shown in fig. 7 and 8, the method for manufacturing an aluminum diamond component having an aluminum silicon carbide layer on the surface thereof includes the steps of:
preparing a silicon carbide prefabricated part: pressing and molding the granulated silicon carbide particles with the particle sizes of 50 microns and 125 microns into a frame with the particle sizes of 11mm multiplied by 17.8mm multiplied by 3.0mm to prepare a silicon carbide prefabricated part blank, and sintering the silicon carbide prefabricated part blank at the constant temperature of 850 ℃ for 3 hours under the vacuum condition to obtain the silicon carbide prefabricated part with the porosity of 30 percent;
machining a silicon carbide prefabricated part: processing the silicon carbide prefabricated part by adopting a numerical control milling process to form a silicon carbide prefabricated part box body with a cavity inside and a silicon carbide prefabricated part cover plate for containing surface-modified diamond particles;
loading of surface modified diamond particles: carrying out surface modification treatment on diamond particles, carrying out magnetron sputtering on 5000 g of 300-micron diamond micro powder to form a tungsten layer with the thickness of 300nm, then placing the tungsten layer in a vacuum furnace with the vacuum degree of 10Pa and the temperature of 1350 ℃ for constant temperature for 2h, reacting the tungsten layer with the diamond particles to obtain surface-modified diamond particles, and filling the surface-modified diamond particles with the thickness of 200 microns into a machined tungsten framework to form a composite blank;
and (3) aluminizing: placing the composite blank in a graphite mold, placing the graphite mold with the composite blank and 6063 aluminum alloy in a double-chamber vacuum air pressure infiltration furnace, vacuumizing, heating double chambers, controlling the temperature of a lower treatment chamber provided with the graphite mold to be 690 ℃, controlling the temperature of an upper treatment chamber provided with the 6063 aluminum alloy to be 750 ℃, pouring 6063 aluminum alloy into aluminum liquid, pouring the aluminum liquid onto the composite blank of the graphite mold, stopping vacuumizing, introducing argon into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to 1MPa, keeping constant temperature and constant pressure for 30min, so that the aluminum liquid is infiltrated into the silicon carbide prefabricated part and the surface modified diamond in the composite blank under the action of gas pressure, and taking out after cooling. And (3) obtaining tungsten-copper layers with the thickness of 0.15mm and covered on all surfaces through precise numerical control milling, and obtaining the aluminum diamond parts with the surfaces covered with the aluminum silicon carbide layers with the thickness of 10mm multiplied by 15mm multiplied by 2.0 mm.
The aluminum diamond composite materials with the surface coated with the aluminum silicon carbide layer prepared in examples 1, 2, 3 and 4 were tested for thermal conductivity, bending strength and expansion coefficient.
The thermal conductivity of the aluminum-diamond composite material of example 1 was 463W/(m.K), and the average linear expansion coefficient in the range of 25 ℃ to 125 ℃ was 7.2X 10-6/° c, the bending strength is 316 MPa.
The thermal conductivity of the aluminum-diamond composite material of example 2 was 568W/(m.K), and the average linear expansion coefficient in the range of 25 ℃ to 125 ℃ was 7.6X 10-6/° c, the bending strength is 292 MPa.
The aluminum-diamond composite material of example 3 had a thermal conductivity of 651W/(m.K) and an average linear expansion coefficient of 6.8X 10 in the range of 25 ℃ to 125 ℃-6/° c, the bending strength is 227 MPa.
The thermal conductivity of the aluminum-diamond composite material of example 4 was 606W/(m.K), and the average linear expansion coefficient in the range of 25 ℃ to 125 ℃ was 7.0X 10-6/° c, the bending strength was 244 MPa.
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, and various modifications and changes will occur to those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (10)

1. An aluminum diamond composite material with an aluminum silicon carbide layer coated on the surface is characterized in that,
the method comprises the following steps: the aluminum diamond core material and the surface aluminum silicon carbide layer coated outside the aluminum diamond core material;
the aluminum diamond core material comprises an aluminum matrix and surface-modified diamond particles;
the surface aluminum silicon carbide layer comprises an aluminum matrix and silicon carbide particles, and the volume fraction of the silicon carbide particles is 60-75%.
2. The aluminum-diamond composite material surface-coated with an aluminum silicon carbide layer according to claim 1,
the aluminum matrix in the surface aluminum silicon carbide layer and the aluminum matrix in the aluminum diamond core material are in a continuous distribution phase.
3. The aluminum-diamond composite material surface-coated with an aluminum silicon carbide layer according to claim 1,
the thickness of the surface aluminum silicon carbide layer is 0.03 mm-0.20 mm.
4. A preparation method of an aluminum diamond composite material with an aluminum silicon carbide layer coated on the surface is characterized by comprising the following steps:
preparing a silicon carbide prefabricated part: forming silicon carbide particles to prepare a silicon carbide prefabricated part blank, and heating and sintering the silicon carbide prefabricated part blank in a vacuum or protective atmosphere to obtain a silicon carbide prefabricated part with the porosity of 25-40%;
machining a silicon carbide prefabricated part: machining the silicon carbide prefabricated part by adopting a numerical control milling process to form the silicon carbide prefabricated part for coating the diamond particles with the modified surfaces;
loading of surface modified diamond particles: carrying out surface modification treatment on the diamond particles to obtain surface-modified diamond particles, and filling the surface-modified diamond particles into the machined silicon carbide prefabricated part to form a composite blank;
and (3) aluminizing: and placing the composite blank and the aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing and heating to melt the aluminum matrix into aluminum liquid and pouring the aluminum liquid onto the composite blank, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace to increase the pressure in the furnace, so that the aluminum liquid is infiltrated into pores of the silicon carbide prefabricated part and the surface-modified diamond particles in the composite blank under the action of gas pressure, and cooling to obtain the aluminum-diamond composite material with the surface coated with the aluminum-silicon carbide layer.
5. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 4,
in the step of preparing the silicon carbide preform, the silicon carbide particles have a particle size of 45 to 125 μm.
6. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 5,
the molding treatment of the silicon carbide particles adopts one of a dry method molding method, an injection molding method and a gel injection molding method;
the temperature of the heating sintering is 800-1000 ℃, and the time is 1-5 h.
7. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 4,
in the step of loading the surface-modified diamond particles, the surface-modified diamond particles have a particle size of 80 to 450 μm.
8. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 4,
the step of aluminizing specifically comprises: placing the composite blank in a graphite mold, placing the graphite mold with the composite blank and an aluminum matrix in a double-chamber vacuum air pressure infiltration furnace, vacuumizing, heating the double chambers, controlling the temperature of a lower treatment chamber provided with the graphite mold to be 570-680 ℃, controlling the temperature of an upper treatment chamber provided with the aluminum matrix to be 680-800 ℃, pouring aluminum liquid formed by the aluminum matrix onto the composite blank of the graphite mold, stopping vacuumizing, introducing protective gas into the double-chamber vacuum air pressure infiltration furnace, increasing the pressure in the furnace to be 1-10 MPa, keeping constant temperature and constant pressure for 5-30 min, so that the aluminum liquid is infiltrated into pores of a silicon carbide prefabricated part and pores of surface-modified diamond particles in the composite blank under the action of gas pressure, cooling and taking out.
9. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 4,
in the step of impregnating aluminum, the aluminum matrix is one of pure aluminum, 3003 aluminum alloy, 6061 aluminum alloy, 6063 aluminum alloy, ZL102 aluminum alloy, and ZL101A aluminum alloy.
10. The method for producing an aluminum-diamond composite material having a surface coated with an aluminum silicon carbide layer according to claim 4,
in the step of impregnating aluminum, a precision machining treatment is also included after cooling.
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