CN113957283A - High-thermal-conductivity composite material with embedded structure and preparation method thereof - Google Patents

High-thermal-conductivity composite material with embedded structure and preparation method thereof Download PDF

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Publication number
CN113957283A
CN113957283A CN202111222448.4A CN202111222448A CN113957283A CN 113957283 A CN113957283 A CN 113957283A CN 202111222448 A CN202111222448 A CN 202111222448A CN 113957283 A CN113957283 A CN 113957283A
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composite material
alloy
porous ceramic
thermal
conductivity
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刘湘宁
张双玉
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Henan Hanyin Photoelectric Technology Co ltd
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    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C1/00Making non-ferrous alloys
    • C22C1/10Alloys containing non-metals
    • C22C1/1036Alloys containing non-metals starting from a melt
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09KMATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/08Materials not undergoing a change of physical state when used
    • C09K5/14Solid materials, e.g. powdery or granular
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C1/00Making non-ferrous alloys
    • C22C1/10Alloys containing non-metals
    • C22C1/1005Pretreatment of the non-metallic additives
    • C22C1/1015Pretreatment of the non-metallic additives by preparing or treating a non-metallic additive preform
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C1/00Making non-ferrous alloys
    • C22C1/10Alloys containing non-metals
    • C22C1/1005Pretreatment of the non-metallic additives
    • C22C1/1015Pretreatment of the non-metallic additives by preparing or treating a non-metallic additive preform
    • C22C1/1021Pretreatment of the non-metallic additives by preparing or treating a non-metallic additive preform the preform being ceramic
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C1/00Making non-ferrous alloys
    • C22C1/10Alloys containing non-metals
    • C22C1/1036Alloys containing non-metals starting from a melt
    • C22C1/1073Infiltration or casting under mechanical pressure, e.g. squeeze casting

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Ceramic Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Thermal Sciences (AREA)
  • Ceramic Products (AREA)
  • Manufacture Of Alloys Or Alloy Compounds (AREA)

Abstract

The invention relates to a high-thermal-conductivity composite material with an embedded structure and a preparation method thereof. The embedded structure high-thermal-conductivity composite material is constructed by an ultrahigh-thermal-conductivity material and a porous ceramic metal composite material; wherein: the ultrahigh heat conduction material is one of a diamond metal composite material, a graphene metal composite material, a carbon nanotube metal composite material, a boron nitride metal composite material and oriented pyrolytic graphite, and the transverse or longitudinal heat conductivity is more than 300W/m.K; the porous ceramic metal composite material is formed by compounding porous ceramic and metal, wherein the porous ceramic is SiC, AlN, BN, Si3N4、Al2O3、TiC、TiB2Or B4One of C; the metal is one of pure copper, copper alloy, pure aluminum, aluminum alloy, pure magnesium or magnesium alloy. Measured byThe trial thermal conductivity range is 200-1500W/m.k, the material preparation cost can be effectively reduced, and the rapid preparation of the high-performance thermal management material is realized.

Description

High-thermal-conductivity composite material with embedded structure and preparation method thereof
Technical Field
The invention belongs to the field of composite materials, and particularly relates to a high-thermal-conductivity composite material with an embedded structure and a preparation method thereof.
Background
At present, the power module is more and more widely applied to the fields of new energy automobiles, smart power grids, rail transit, frequency converters, inverter welding machines, induction heating and the like, but in the actual use process of the existing power module, the heat dissipation problem of the power module is more and more prominent, namely the heat dissipation of the power module plays a key role in the service life and the reliability of the power module, and particularly along with the development of power electronic technology, the requirement on the reliability of the power module in the aspects of structure and circuit is higher.
Metal matrix composites are one of the high performance heat dissipating materials that have been rapidly developed in recent years. By adding various reinforcements into the metal material, the high-performance composite material which has good heat conduction and electric conduction performance, impact resistance, corrosion resistance, fatigue resistance and fracture toughness, high strength, high rigidity, strong wear resistance and low thermal expansion coefficient can be obtained. The development of the metal-based composite material plays a vital role in promoting the high-tech modernization of military and civil fields of all countries in the world.
At present, the latest generation of heat-dissipating metal-based composites include aluminum silicon carbide composites, diamond/copper composites, diamond aluminum composites, and the like. The high volume fraction aluminum silicon carbide composite material can achieve excellent performances of stable size, high heat conduction, high specific stiffness, high specific strength and the like of the composite material by adjusting the content of a designed reinforcement, the components of an aluminum alloy, the proportion of two phases or the heat treatment state of the composite material, thereby meeting the quality requirements of the aerospace field on electronic packaging materials, and being an excellent electronic packaging material and a structural material of precision equipment. At present, many domestic and foreign companies have developed a thermal conductivity value of 170--6The aluminum silicon carbide composite material product of/K is commercialized. But the heat-conducting property still hardly meets the application requirement of the ultrahigh power module. In the aspect of thermal conductivity, the copper-diamond composite material is far superior to other materials, and the excellent heat dissipation property of the packaging device can be ensured. By controlling the volume fraction of diamond, the thermal expansion coefficient of the composite material can be adjusted, so that the composite material can be mixed with Si, GaAs, AlN and Al2O3、Si3N4And matching the equal phases. The thermal conductivity can reach as high as 800W/m.K. The high elastic modulus helps to reduce thermal deformation, thereby improving the sealing performance of the packaged device. Compared with a copper diamond composite material, the aluminum diamond composite material has the advantages of low density and low synthesis temperature, and the heat conductivity of the pure aluminum-diamond composite material is as high as 600W/m.K. Although the metal diamond composite has high heat conductivity, it has a high heat conductivityThe cost is high, the processing difficulty is high, and the application of the composite material is limited. Diamond, carbon nanotubes and highly oriented pyrolytic graphite are known materials with higher thermal conductivity. However, carbon nanotubes and highly oriented pyrolytic graphite are expensive and cannot be used alone as substrate materials.
Therefore, the technical scheme of the invention is provided.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a high-thermal-conductivity composite material with an embedded structure and a preparation method thereof. The high-thermal-conductivity composite material with the embedded structure takes the porous ceramic metal composite material as a carrier, plays a role in supporting, reduces the preparation cost of the material, can realize ultrahigh thermal conductivity by the ultrahigh thermal-conductivity material, and can effectively achieve the purpose of quickly conducting heat. By adopting the structural design and the preparation method, the high-thermal-conductivity composite material with the embedded structure and adjustable thermal conductivity height can be prepared. The thermal conductivity range obtained by testing is 200-1500W/m.k, the preparation cost of the material can be effectively reduced, and the rapid preparation of the high-performance thermal management material is realized.
The scheme of the invention is that the high-thermal-conductivity composite material with the embedded structure is constructed by the ultrahigh-thermal-conductivity material and the porous ceramic metal composite material; wherein:
the ultrahigh heat conduction material is one of a diamond metal composite material, a graphene metal composite material, a carbon nanotube metal composite material, a boron nitride metal composite material and oriented pyrolytic graphite, and the transverse or longitudinal heat conductivity is more than 300W/m.K;
the porous ceramic metal composite material is formed by compounding porous ceramic and metal, wherein the porous ceramic is SiC, AlN, BN, Si3N4、Al2O3、TiC、TiB2Or B4One of C; the metal is one of pure copper, copper alloy, pure aluminum, aluminum alloy, pure magnesium or magnesium alloy.
Preferably, the porosity of the porous ceramic is 30-80%, the average pore size is 0.1-500 μm, and the mass fraction of pure ceramic of the porous ceramic is greater than 95%.
Preferably, the copper alloy is one of brass, cupronickel or bronze; the aluminum alloy is one of aluminum-silicon alloy, aluminum-magnesium-silicon alloy, aluminum-copper alloy, aluminum-magnesium alloy, aluminum-manganese alloy, aluminum-zinc alloy or aluminum-lithium alloy; the magnesium alloy is one of magnesium-manganese alloy, magnesium-lithium alloy, magnesium-rare earth alloy, magnesium-silver alloy or magnesium-thorium alloy.
Preferably, the ultra-high thermal conductivity material is disposed in the porous ceramic metal composite core.
Preferably, the ultrahigh heat conduction material is embedded in the surface of the porous ceramic-metal composite material.
Based on the same technical concept, the invention also provides a preparation method of the high-thermal-conductivity composite material with the embedded structure, which comprises the following steps:
(1) preparing porous ceramics: molding the porous ceramic powder to obtain a blank; sintering and insulating the green body to obtain porous ceramic;
(2) introducing ultrahigh heat conduction material: embedding the ultrahigh heat conduction material into the bicontinuous ceramic to obtain a prefabricated body;
(3) compounding: adopting one of extrusion casting, pressureless infiltration or pressure infiltration; the extrusion casting is as follows: preheating the prefabricated body in an inert atmosphere, then placing the prefabricated body into a composite die, casting a metal solution, and pressurizing and filling; the non-pressure infiltration comprises the following steps: placing the prefabricated body into a composite die, placing a metal solution on the top of the prefabricated body, and impregnating the porous ceramic in an inert atmosphere; the pressure infiltration is as follows: and (3) placing the prefabricated body into a composite die, placing a metal solution at the top of the prefabricated body, vacuumizing, preserving heat, and inflating and pressurizing to ensure that the metal solution is impregnated into the porous ceramic.
Preferably, in the step (1), the sintering temperature is 1000-2500 ℃, and the heat preservation time is more than 10 min.
Preferably, the preheating temperature in the extrusion casting is 300-1000 ℃; the temperature of the composite die is 200-400 ℃; the casting temperature is 500-1450 ℃; the pressurization is 5-200 MPa, the pressurization time is more than 5s, and the pressure maintaining time is more than 5 s.
Preferably, in the pressureless infiltration, the temperature of the infiltration is 700-1400 ℃, and the temperature is kept for 60-120 min in the infiltration process.
Preferably, in the pressure infiltration, the temperature of the infiltration is 900-1400 ℃, the temperature is kept for 60-120 min in the infiltration process, and the pressure of the pressurization is 1-10 Mpa.
In addition, the composite process can also be a method such as differential pressure casting, normal pressure casting, vacuum casting, negative pressure suction casting and the like, so that molten metal enters the mesh holes of the prefabricated body to obtain the high-thermal-conductivity composite material with the embedded structure.
The invention has the beneficial effects that:
the high-thermal-conductivity composite material with the embedded structure is formed by a porous ceramic metal composite material and an ultrahigh-thermal-conductivity material. The porous ceramic metal composite material is used as a carrier, so that the support effect is achieved, the material preparation cost is reduced, the ultrahigh heat conduction material can achieve ultrahigh heat conduction rate, and the purpose of quickly conducting heat can be effectively achieved. By adopting the structural design and the preparation method, the high-thermal-conductivity composite material with the embedded structure and adjustable thermal conductivity height can be prepared. The thermal conductivity range obtained by testing is 200-1500W/m.k, the preparation cost of the material can be effectively reduced, and the rapid preparation of the high-performance thermal management material is realized.
In addition, the composite material with the embedded structure and high thermal conductivity has the characteristics of adjustable size, structure and thermal conductivity, and is favorable for different application environment requirements; compared with the traditional heat management composite material, the composite material with the embedded structure and high heat conductivity combines the functions and the structure, and overcomes the defects that the composite material with the ultrahigh heat conductivity is high in preparation cost, difficult to process, not suitable for being used as a structural material and the like; finally, the composite material with the embedded structure and high thermal conductivity has the advantages of simple preparation process, high efficiency and wide application prospect, and can be applied to the field of heat dissipation requirements of various power devices.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the technical solutions of the present invention will be described in detail below. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be derived by a person skilled in the art from the examples given herein without any inventive step, are within the scope of the present invention.
Example 1
The embodiment provides a preparation method of a high-thermal-conductivity composite material with an embedded structure, which comprises the following steps:
(1) preparing porous ceramics: pressing and molding the porous silicon carbide ceramic powder to obtain a blank; sintering the blank at 1700 ℃ in a nitrogen atmosphere (60% vol) and preserving heat for 1h to obtain porous ceramic;
(2) introducing ultrahigh heat conduction material: embedding the nickel-plated diamond micro powder with the average grain size of 320 meshes into the porous ceramic core to obtain a prefabricated body;
(3) metal smelting: selecting industrial pure aluminum, putting the industrial pure aluminum into a pit furnace for smelting at the temperature of 850 ℃ to obtain aluminum liquid;
(4) extrusion casting: and putting the prefabricated body into a vacuum box type furnace for preheating, wherein the preheating temperature is 800 ℃ under the protection of argon, and simultaneously preheating the composite die to 300 ℃. And (3) putting the preheated preform into a composite die at the temperature of 300 ℃, casting the molten aluminum at the temperature of 850 ℃ into the die, pressurizing to 80MPa within 10s, and maintaining the pressure for 30 s.
(5) Finish machining: and (4) after demolding, machining to the required size to obtain the porous silicon aluminum carbide composite material embedded with the diamond aluminum composite material.
Example 2
The embodiment provides a preparation method of a high-thermal-conductivity composite material with an embedded structure, which is different from the embodiment 1 in that the embedded high-thermal-conductivity material is oriented pyrolytic graphite.
Example 3
The embodiment provides a preparation method of a high-thermal-conductivity composite material with an embedded structure, which is different from the embodiment 1 in that a metal smelting material is magnesium aluminum AZ81, the smelting temperature is 700 ℃, and about 75% of air and about 24.8% of CO are mixed together2About 0.2% SF6Mixed gas is carried outAnd (4) protecting.
Example 4
This example provides a method for preparing a composite material with embedded structure and high thermal conductivity, which is different from example 1 in the selection of squeeze casting metal. The metal for extrusion casting is pure copper, and the smelting temperature is 1380 ℃.
Example 5
The embodiment provides a preparation method of a high-thermal-conductivity composite material with an embedded structure, which comprises the following steps:
(1) preparing porous ceramics: pressing and molding the porous silicon nitride ceramic powder to obtain a blank; sintering the blank at 1800 ℃ in a nitrogen atmosphere (55% vol) and preserving heat for 1h to obtain porous ceramic;
(2) introducing ultrahigh heat conduction material: embedding the titanium-plated diamond micro powder with the average grain size of 240 meshes into the porous ceramic core to obtain a prefabricated body;
(3) pressure infiltration: firstly, placing the preform into a graphite mold, then placing Al-7Si-Mg alloy on the preform, placing the mold into an air pressure infiltration furnace, vacuumizing, preheating at 800 ℃, and preserving heat for 1 h. Inflating and pressurizing at 5MPa for 60s after the temperature is reached; the dwell time was 0.5 h. And cooling and discharging to obtain the high-thermal-conductivity composite material with the embedded structure.
Example 6
The embodiment provides a preparation method of a high-thermal-conductivity composite material with an embedded structure, which comprises the following steps:
(1) preparing porous ceramics: pressing and molding the porous silicon carbide ceramic powder to obtain a blank; sintering the blank at 2000 ℃ in a nitrogen atmosphere (65% vol) and preserving heat for 0.5h to obtain porous ceramic;
(2) introducing ultrahigh heat conduction material; embedding the nickel-plated diamond/Cu composite material with the average grain diameter of 320 meshes on the surface of the porous silicon carbide ceramic material;
(3) pressureless infiltration: firstly, placing a prefabricated body into a graphite mould, then placing a certain amount of Al-12Si-Mg alloy on the prefabricated body, placing the mould into a vacuum furnace, protecting with nitrogen, preheating at 1000 ℃, preserving heat for 1h, and cooling out of the furnace to obtain the required composite material.
The above description is only for the specific embodiments of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art can easily conceive of the changes or substitutions within the technical scope of the present invention, and all the changes or substitutions should be covered within the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the appended claims.

Claims (10)

1. The composite material with the embedded structure and high thermal conductivity is characterized by being constructed by an ultrahigh thermal conductive material and a porous ceramic metal composite material; wherein:
the ultrahigh heat conduction material is one of a diamond metal composite material, a graphene metal composite material, a carbon nanotube metal composite material, a boron nitride metal composite material and oriented pyrolytic graphite, and the transverse or longitudinal heat conductivity is more than 300W/m.K;
the porous ceramic metal composite material is formed by compounding porous ceramic and metal, wherein the porous ceramic is SiC, AlN, BN, Si3N4、Al2O3、TiC、TiB2Or B4One of C; the metal is one of pure copper, copper alloy, pure aluminum, aluminum alloy, pure magnesium or magnesium alloy.
2. The embedded structure high thermal conductivity composite material according to claim 1, wherein the porosity of the porous ceramic is 30 to 80%, the average pore size is 0.1 to 500 μm, and the pure ceramic mass fraction of the porous ceramic is more than 95%.
3. The embedded structural high thermal conductivity composite of claim 1, wherein the copper alloy is one of brass, cupronickel, or bronze; the aluminum alloy is one of aluminum-silicon alloy, aluminum-magnesium-silicon alloy, aluminum-copper alloy, aluminum-magnesium alloy, aluminum-manganese alloy, aluminum-zinc alloy or aluminum-lithium alloy; the magnesium alloy is one of magnesium-manganese alloy, magnesium-lithium alloy, magnesium-rare earth alloy, magnesium-silver alloy or magnesium-thorium alloy.
4. The embedded structural HTC composite of claim 1, wherein the UHT material is disposed in the porous ceramic-metal composite core.
5. The embedded structure HTC composite of claim 1, wherein the UHT material is embedded in the porous ceramic metal composite surface.
6. The method for preparing the high-thermal-conductivity composite material with the embedded structure as claimed in any one of claims 1 to 5, is characterized by comprising the following steps:
(1) preparing porous ceramics: molding the porous ceramic powder to obtain a blank; sintering and insulating the green body to obtain porous ceramic;
(2) introducing ultrahigh heat conduction material: embedding the ultrahigh heat conduction material into the bicontinuous ceramic to obtain a prefabricated body;
(3) compounding: adopting one of extrusion casting, pressureless infiltration or pressure infiltration; the extrusion casting is as follows: preheating the prefabricated body in an inert atmosphere, then placing the prefabricated body into a composite die, casting a metal solution, and pressurizing and filling; the non-pressure infiltration comprises the following steps: placing the prefabricated body into a composite die, placing a metal solution on the top of the prefabricated body, and impregnating the porous ceramic in an inert atmosphere; the pressure infiltration is as follows: and (3) placing the prefabricated body into a composite die, placing a metal solution at the top of the prefabricated body, vacuumizing, preserving heat, and inflating and pressurizing to ensure that the metal solution is impregnated into the porous ceramic.
7. The method for preparing the high-thermal-conductivity composite material with the embedded structure according to claim 6, wherein in the step (1), the sintering temperature is 1000-2500 ℃, and the heat preservation time is more than 10 min.
8. The method for preparing the high-thermal-conductivity composite material with the embedded structure according to claim 6, wherein the preheating temperature in the extrusion casting is 300-1000 ℃; the temperature of the composite die is 200-400 ℃; the casting temperature is 500-1450 ℃; the pressurization is 5-200 MPa, the pressurization time is more than 5s, and the pressure maintaining time is more than 5 s.
9. The preparation method of the high-thermal-conductivity composite material with the embedded structure, according to claim 6, is characterized in that the temperature of infiltration is 700-1400 ℃ in the pressureless infiltration process, and the temperature is kept for 60-120 min in the infiltration process.
10. The preparation method of the high-thermal-conductivity composite material with the embedded structure according to claim 6 is characterized in that in the pressure infiltration, the temperature of the infiltration is 900-1400 ℃, the temperature is kept for 60-120 min in the infiltration process, and the pressure of pressurization is 1-10 MPa.
CN202111222448.4A 2021-10-20 2021-10-20 High-thermal-conductivity composite material with embedded structure and preparation method thereof Pending CN113957283A (en)

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Cited By (1)

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CN116037930A (en) * 2022-12-14 2023-05-02 哈尔滨工业大学 Preparation method of graphene-silicon nitride synergistically-reinforced aluminum-based composite material

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CN111500892A (en) * 2020-06-18 2020-08-07 哈尔滨锦威科技有限公司 Preparation method of large-size flaky diamond/copper composite material with ultrahigh thermal conductivity
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JP2011139000A (en) * 2010-01-04 2011-07-14 Denki Kagaku Kogyo Kk Power module structure and method of manufacturing the same
JP2012117085A (en) * 2010-11-29 2012-06-21 Denki Kagaku Kogyo Kk Aluminum-diamond composite and method for producing the same
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Publication number Priority date Publication date Assignee Title
CN116037930A (en) * 2022-12-14 2023-05-02 哈尔滨工业大学 Preparation method of graphene-silicon nitride synergistically-reinforced aluminum-based composite material
CN116037930B (en) * 2022-12-14 2023-09-08 哈尔滨工业大学 Preparation method of graphene-silicon nitride synergistically-reinforced aluminum-based composite material

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Application publication date: 20220121