CN113981336B - Aluminum alloy composite heat dissipation material containing carbide/graphene sandwich structure for LED lamp and preparation method thereof - Google Patents

Aluminum alloy composite heat dissipation material containing carbide/graphene sandwich structure for LED lamp and preparation method thereof Download PDF

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CN113981336B
CN113981336B CN202111165005.6A CN202111165005A CN113981336B CN 113981336 B CN113981336 B CN 113981336B CN 202111165005 A CN202111165005 A CN 202111165005A CN 113981336 B CN113981336 B CN 113981336B
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graphene
carbide
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黄军同
徐建勇
王志怀
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Shenzhen Lianyu Photoelectric Co ltd
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Abstract

The invention discloses an aluminum alloy composite heat dissipation material containing a carbide/graphene sandwich structure for an LED lamp and a preparation method thereof, wherein the heat dissipation material is formed by compounding nano graphene sheets obtained by stripping, a carbide nanosheet sandwich structure obtained by reaction, carbon nanotubes obtained by reaction, carbide nanofibers, nano metal Ni particles obtained by decomposition and reduction and aluminum alloy; firstly, stirring and mixing a nitrate ethanol solution, resin and expanded graphite, adding the mixture into a three-roll grinding machine, peeling to obtain a nano graphene sheet/resin mixture, adding nano simple substance powder into the mixture, mechanically stirring, carrying out heat treatment, adding the mixture after the heat treatment into a smelted aluminum alloy melt, uniformly stirring and mixing, and pouring the mixture into a mold. The composite heat dissipation material prepared by the invention has the advantages of compact structure, neat surface and high heat conduction and heat dissipation efficiency, effectively improves the heat dissipation efficiency of the LED lamp, and prolongs the service life of the LED lamp.

Description

Aluminum alloy composite heat dissipation material containing carbide/graphene sandwich structure for LED lamp and preparation method thereof
Technical Field
The invention relates to the field of LED lamp heat dissipation materials, in particular to an aluminum alloy composite heat dissipation material containing a carbide/graphene sandwich structure for an LED lamp and a preparation method thereof.
Background
The LED is one of semiconductor diodes, can convert electric energy into light energy, has small volume, can be prepared into lamps in various shapes, and is suitable for a variable environment. The price of the LED is becoming more civilized, and more people tend to use the LED due to the power saving characteristic of the LED. At present, the LED is the most popular light source, but there are many defects in practical use, and because the LED has high heat-generating efficiency, the working performance of the LED is reduced, and the service life of the LED is greatly affected, so that the problem that the improvement of the heat dissipation of the LED is urgently needed to be solved is solved.
The LED heat dissipation substrate is used as one of media for leading out LED heat energy, the heat generated by the LED is mainly transferred to the radiator through the heat dissipation substrate, and the radiator exchanges heat with the external environment through heat convection and heat radiation. The main functions of the heat dissipation substrate are electrical connection, physical support and heat dissipation, and are key links in the heat dissipation process of the LED. The improvement of the heat conducting performance of the heat dissipation substrate has important significance in reducing the temperature of the LED, improving the working efficiency of the LED and prolonging the service life of the LED.
At present, the most common LED heat dissipation substrate material is copper and aluminum alloy, the aluminum alloy is easy to process and low in cost, the most heat dissipation material is applied, and the copper has higher heat conductivity coefficient, so that the instant heat absorption capacity of the LED heat dissipation substrate material is better than that of the aluminum alloy, but the heat dissipation speed is slower than that of the aluminum alloy. Therefore, the heat dissipation substrate, whether pure copper, pure aluminum or aluminum alloy, has a fatal defect: because only one material is used, although the basic heat dissipation capability can easily meet the requirement of slight heat dissipation, the requirements of balanced heat conduction and effective heat dissipation cannot be well met, and therefore the field with higher heat dissipation requirements is difficult to meet.
Nowadays, many novel additives for aluminum-based materials are presented in the form of novel carbon nanomaterials (e.g., carbon nanotubes and graphene), and when incorporated into aluminum alloy substrates, they can improve physical and mechanical properties of the aluminum alloy substrates, and can add many new functions, such as self-lubricating surfaces and enhanced heat dissipation.
Carbon nanotubes have high thermal conductivity and are a promising material for heat dissipation applications including semiconductor devices. Graphene is a single atomic layer of graphite and is of great interest because of its unique electrical conductivity, chemical inertness, excellent optical, thermal and mechanical properties. The heat transfer of graphene is an active research field, has strong heat conduction capability, and the heat conduction coefficient of graphene is 5300W/(m.K), and attracts people's attention due to the potential of heat management application. The excellent properties of graphene are likely to be useful in the fields of thermal conduction, electronics, supercapacitors, sensors and corrosion protection. In recent years, aluminum alloys have been replaced by advanced materials such as graphene/aluminum alloy-based composites, mainly because the graphene/aluminum alloy-based composites have excellent physical and mechanical properties. Therefore, the graphene/aluminum alloy based composite material has a wide application in the automobile industry and the aerospace field.
At present, the graphene size of graphene/aluminum alloy-based composite materials is mostly nano-scale, such as graphene nanosheets, graphene nanoplates, graphene nanoplatelets and the like. Due to the fact that the density of graphene is small, the weight of graphene is light, the graphene is easy to suspend on the surface of the aluminum alloy when the graphene is smelted by a traditional batching method, and the graphene is difficult to dissolve in an aluminum matrix. And the dispersion is poor due to easy agglomeration of graphene caused by van der waals force and high surface area and surface energy among the graphene nanosheets, and the agglomerated graphene can block the dissipation of heat, so that the heat dissipation performance of the composite material is reduced. Although researchers have conducted extensive research on improving the performance of graphene/aluminum alloy based composites in recent years, and have made corresponding progress, the required performance of the composites has been improved, but the graphene/aluminum alloy based composites still have challenges and need to be explored in the future.
In addition, in the conventional technology, in order to improve various properties of the aluminum alloy matrix, including heat dissipation performance, some common ceramic powder and fibers can be added. Therefore, how to effectively prepare the graphene/aluminum alloy base composite material and improve the poor dispersibility of the graphene so that the graphene can be effectively and uniformly dispersed in the aluminum alloy base is the key for obtaining the graphene/aluminum alloy base composite material with high heat dissipation and low cost.
Disclosure of Invention
The invention aims to solve the technical problems in the prior art and provides an aluminum alloy composite heat dissipation material containing a carbide/graphene sandwich structure for an LED lamp and a preparation method thereof.
In order to achieve the purpose, the technical scheme provided by the invention is as follows: an aluminum alloy composite heat dissipation material containing a carbide/graphene sandwich structure for an LED lamp and a preparation method thereof comprise the following steps:
(1) Firstly, 0.51-5 wt% of nickel nitrate nonahydrate is added into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 85.0-94.9 wt% of resin, stirring and mixing for 4-25 min, and then pouring 5.1-10.0 wt% of expanded graphite into the resin, stirring for 10-30 min to obtain a mixture A;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B;
(3) Adding elemental nano powder into the nano graphene sheet/resin mixture B obtained in the step (2) by stripping, wherein the mass ratio of the mixture B to the elemental nano powder is (0.85-1.5): 1, mechanically stirring for 20-40 min to obtain a mixture C, wherein the elementary substance nano powder can be one or more of silicon powder, boron powder, titanium powder, tungsten powder, zirconium powder and the like, the content of a single substance in the elementary substance nano powder is more than or equal to 99.5%, and the particle size is less than or equal to 100nm;
(4) Placing the mixture C obtained in the step (3) in a tubular furnace with air atmosphere for heat treatment, and heating the mixture C from room temperature at 2-3 ℃ for min -1 The temperature rising rate is 100 ℃, and the temperature is kept for 0.5 to 1 hour; then at 1-2 ℃ for min -1 The temperature rising rate is up to 200 ℃, and the temperature is kept for 2 to 4 hours; then introducing argon at 4-8 ℃ for min -1 The temperature is raised to 1000 ℃ at the temperature raising rate, the temperature is kept for 1 to 3 hours, and then the temperature is raised to 3 to 5 ℃ for min -1 The temperature is raised to 1300-1450 ℃ at the temperature raising rate, and the temperature is kept for 0.5-6 h; then naturally cooling to room temperature to obtain a reaction mixture D;
(5) Smelting aluminum alloy at 660-700 ℃ for 3-6 h, then crushing the reaction mixture D obtained in the step (4), adding the crushed mixture into an aluminum alloy melt, adding a deslagging agent, pressing the mixture into the liquid level, repeatedly moving up and down, degassing, slagging off, and fully stirring to obtain a mixed melt E;
(6) And pouring the mixed melt E into a mold, and finally, pouring and molding to obtain the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure.
Preferably, the carbon content of the expanded graphite raw material in the step (1) is more than or equal to 96%, and the particle size is 1.0-5.0 mm; the resin is linear thermoplastic epoxy resin or thermoplastic phenolic resin liquid.
Preferably, the three-roll speed ratio of the three-roll mill in the step (2) is that the feed roll N3, the center roll N2, the discharge roll N1 are 1.
Preferably, the mass ratio of the mixture D and the aluminum alloy in the step (5) is 0.1 to 1:5 to 50 percent, the slag removing agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount of the slag removing agent is 0.5 to 2.2 percent of the total mass of the aluminum alloy in the furnace.
The invention also discloses an aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp, which is characterized in that the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure is prepared by preparing nano graphene sheets from expanded graphite through three-roller grinding and stripping, reacting to obtain a carbide nanosheet sandwich structure, reacting to obtain carbon nanotubes, carbide nanofibers, decomposing and reducing to obtain nano metal Ni particles and compounding with aluminum alloy.
The invention has the beneficial effects that:
1. the invention adopts a three-roller grinding machine grinding stripping technology to overcome the van der Waals force between graphite layers by the shearing force generated by three-roller differential speed and the acting force formed by high-viscosity resin and the surface of the expanded graphite, thereby stripping the expanded graphite with the thickness of millimeter level to prepare a large amount of nano graphene sheets, wherein the thickness of the graphene sheets is from single layer, several layers, dozens of layers to dozens of layers. The graphene is uniformly dispersed in the resin in situ, and has a better dispersion effect than a traditional additional mode.
2. The method adopts the nickel nitrate nonahydrate catalyst, dissolves the nickel nitrate nonahydrate catalyst in ethanol to prepare the nickel nitrate ethanol solution, the nickel nitrate ethanol solution is easy to be uniformly mixed with resin (epoxy resin or phenolic resin), and the resin is easy to be catalyzed to form the carbon nano tube in the subsequent heat treatment process at 1000 ℃, so that the method has better dispersibility than the externally added carbon nano tube and saves the cost.
3. The nano graphene sheets obtained by three-roller grinding and stripping react with the elemental powder at different times of continuously heating to 1300-1450 ℃ and preserving heat to form a sandwich structure of carbide nanosheets and graphene, the sandwich structure has higher specific gravity than pure graphene, the elemental powder reacts with resin to form carbide nanofibers, and the carbide nano material formed by in-situ reaction has better dispersion effect than that additionally arranged in the traditional mode. In addition, the thickness of the carbide formed on the surface of the graphene can be regulated and controlled due to different heat preservation times.
4. The nickel nitrate nonahydrate forms a large amount of metal nickel particles less than 100nm after decomposition and reduction in the heat treatment process of the technical scheme, and the ethanol solution of the transition metal nitrate is used instead of the nano metal particles, so that the agglomeration of directly used metal is avoided, a good dispersion effect is achieved, the catalytic efficiency of the catalyst is greatly improved, and the nano metal Ni can also be used as an alloy component of aluminum. Meanwhile, the ethanol solution of the transition metal nitrate is used as a catalyst, but not an aqueous solution, because the aqueous solution is not mutually soluble with the epoxy resin or the phenolic resin, the aqueous solution cannot be well dispersed.
5. The density of the mixture of the nano graphene sheets finally obtained and the carbide nano sheets obtained by reaction, the carbon nano tubes obtained by reaction, the carbide nano fibers, the nano metal Ni particles obtained by decomposition and reduction and the like can be higher than that of the conventional pure graphene, and the mixture can be better dispersed in aluminum alloy in the smelting process of the aluminum alloy, so that the prepared aluminum alloy composite material containing the carbide/graphene sandwich structure has high heat conductivity coefficient, the heat conductivity of the composite material is improved, and the heat conductivity, the heat dissipation performance and the comprehensive strength of the obtained aluminum alloy-based composite heat dissipation material are better.
The aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp, which is finally prepared by the invention, has the advantages of compact structure, neat surface and high heat conduction efficiency, is particularly suitable for heat dissipation of the LED lamp, effectively improves the heat dissipation efficiency of the LED lamp, and prolongs the service life of the LED lamp.
Drawings
The accompanying drawings, which are included to provide a further understanding of the invention and are incorporated in and constitute a part of this specification, illustrate embodiments of the invention and together with the description serve to explain the invention and not to limit the invention.
FIG. 1 is a schematic diagram of a three-roll grinder for peeling expanded graphite in resin to obtain nano-graphene according to the present invention;
FIG. 2 is a schematic diagram of a sandwich two-dimensional structure of SiC and graphene;
FIG. 3 is an SEM image of exfoliated nanographitic plates, siC nanowires in mixture D prepared according to the invention;
FIG. 4 shows SiC nanofibers in mixture D prepared according to the present invention;
fig. 5 is graphene-based SiC nanoplates in mixture D prepared in the present invention;
fig. 6 is a TEM image of graphene, carbon nanotubes and nanometal Ni particles in mixture D prepared according to the present invention;
fig. 7 is EDS surface scan distribution under HAADF of nano-metallic Ni particles in mixture D prepared by the present invention.
Detailed Description
The following detailed description of the embodiments of the present invention will be provided with reference to the accompanying drawings and examples, so that how to implement the embodiments of the present invention by using technical means to solve the technical problems and achieve the technical effects can be fully understood and implemented.
Referring to fig. 1 to 7, in a preferred embodiment of the present invention, an aluminum alloy composite heat dissipation material for an LED lamp includes a carbide/graphene sandwich structure and a preparation method thereof, wherein the aluminum alloy composite heat dissipation material includes: the method comprises the following steps:
(1) Firstly, 0.51-5 wt% of nickel nitrate nonahydrate is added into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 85.0-94.9 wt% of resin, stirring and mixing for 4-25 min, and then pouring 5.1-10.0 wt% of expanded graphite into the resin, stirring for 10-30 min to obtain a mixture A;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B;
(3) Adding simple substance nano powder into the nano graphene sheet/resin mixture B obtained in the step (2) by stripping, wherein the mass ratio of the mixture B to the simple substance nano powder is 0.85-1.5: 1, mechanically stirring for 20-40 min to obtain a mixture C, wherein the elementary substance nano powder can be one or more of silicon powder, boron powder, titanium powder, tungsten powder, zirconium powder and the like, the content of a single substance in the elementary substance nano powder is more than or equal to 99.5%, and the particle size is less than or equal to 100nm;
(4) Placing the mixture C obtained in the step (3) in a tubular furnace with an air atmosphere for heat treatment at the room temperature of 2-3 ℃ for min -1 The temperature rising rate is 100 ℃, and the temperature is kept for 0.5 to 1 hour; then at 1-2 ℃ for min -1 The temperature rising rate is up to 200 ℃, and the temperature is kept for 2 to 4 hours; then introducing argon at 4-8 ℃ min -1 The temperature is raised to 1000 ℃ at the temperature raising rate, the temperature is kept for 1 to 3 hours, and then the temperature is raised to 3 to 5 ℃ for min -1 The temperature is raised to 1300-1450 ℃ at the temperature raising rate, and the temperature is kept for 0.5-6 h; then naturally cooling to room temperature to obtain a reaction mixture D;
(5) Smelting aluminum alloy at 660-700 ℃ for 3-6 h, then crushing the reaction mixture D obtained in the step (4), adding the crushed mixture into an aluminum alloy melt, adding a deslagging agent, pressing the mixture into the liquid level, repeatedly moving up and down, degassing, slagging off, and fully stirring to obtain a mixed melt E;
(6) And pouring the mixed melt E into a mold, and finally, pouring and molding to obtain the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure.
The method adopts the nickel nitrate nonahydrate catalyst, dissolves the nickel nitrate nonahydrate catalyst in ethanol to prepare the nickel nitrate ethanol solution, the nickel nitrate ethanol solution is easy to be uniformly mixed with resin (epoxy resin or phenolic resin), and the resin is easy to be catalyzed to form the carbon nano tube in the subsequent heat treatment process at 1000 ℃, so that the method has better dispersibility than the externally added carbon nano tube and saves the cost. The nickel nitrate nonahydrate forms a large amount of metal nickel particles less than 100nm after decomposition and reduction in the heat treatment process of the technical scheme, and the ethanol solution of the transition metal nitrate is used instead of the nano metal particles, so that the agglomeration of directly used metal is avoided, a good dispersion effect is achieved, the catalytic efficiency of the catalyst is greatly improved, and the nano metal Ni can also be used as an alloy component of aluminum. Meanwhile, the ethanol solution of the transition metal nitrate is used as a catalyst, but not an aqueous solution, because the aqueous solution is not mutually soluble with the epoxy resin or the phenolic resin, the aqueous solution cannot be well dispersed.
The grinding and stripping technology of the three-roll grinder is adopted in the invention, the van der Waals force between graphite layers is overcome by the shearing force generated by the three-roll differential speed and the acting force formed by the high-viscosity resin and the surface of the expanded graphite, so that the expanded graphite with the thickness of millimeter level is stripped to prepare a large number of nano graphene sheets, and the thickness of the graphene sheets is from single layer, several layers, dozens of layers to dozens of layers. The graphene is uniformly dispersed in the resin in situ, and has a better dispersion effect than the traditional additional mode; the nano graphene sheets obtained by three-roller grinding and stripping react with Si powder at different times of continuously heating to 1300-1450 ℃ and preserving heat to form a sandwich structure of SiC nano sheets and graphene, the sandwich structure has higher specific gravity than pure graphene, meanwhile, siC nano fibers are formed by the reaction of Si powder and resin, and the SiC nano materials formed by in-situ reaction have better dispersion effect than those additionally arranged in the traditional mode. In addition, the heat preservation time is different, and the thickness of SiC formed on the surface of the graphene can be regulated and controlled.
The density of the mixture of the nano graphene sheets finally obtained and the carbide nano sheets obtained by reaction, the carbon nano tubes obtained by reaction, the carbide nano fibers, the nano metal Ni particles obtained by decomposition and reduction and the like can be higher than that of the conventional pure graphene, and the mixture can be better dispersed in aluminum alloy in the smelting process of the aluminum alloy, so that the prepared aluminum alloy composite material containing the carbide/graphene sandwich structure has high heat conductivity coefficient, the heat conductivity of the composite material is improved, and the heat conductivity, the heat dissipation performance and the comprehensive strength of the obtained aluminum alloy-based composite heat dissipation material are better.
The aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp, which is finally prepared by the invention, has the advantages of compact structure, clean surface and high heat conduction efficiency, is especially suitable for heat dissipation of the LED lamp, effectively improves the heat dissipation efficiency of the LED lamp, and prolongs the service life of the LED lamp.
As an embodiment of the invention, it may also have the following additional technical features:
in the embodiment, the carbon content of the expanded graphite raw material in the step (1) is more than or equal to 96%, and the particle size is 1.0-5.0 mm; the resin is linear thermoplastic epoxy resin or thermoplastic phenolic resin liquid.
In this embodiment, the three-roll speed ratio of the three-roll mill in the step (2) is that the feed roll N3, the center roll N2, the discharge roll N1, 1.
In this embodiment, the mass ratio of the mixture D and the aluminum alloy in the step (5) is 0.1 to 1:5 to 50 percent, the slag removing agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount of the slag removing agent is 0.5 to 2.2 percent of the total mass of the aluminum alloy in the furnace.
The invention also discloses an aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp, which is characterized by being formed by preparing a nano graphene sheet from expanded graphite through three-roller grinding and stripping, reacting to obtain a carbide nanosheet sandwich structure, reacting to obtain a carbon nanotube, a carbide nanofiber, decomposing and reducing to obtain nano metal Ni particles and compounding with aluminum alloy.
In order to better understand the technical solution of the present invention, the following will clearly and completely describe the technical solution in connection with the examples of the present invention, which are not limited to the present invention.
Example 1
(1) Firstly, adding 0.51wt% of nickel nitrate nonahydrate into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 90.0wt% of thermoplastic epoxy resin, stirring and mixing for 15min, and then pouring 9.49wt% of expanded graphite into the mixture, and stirring for 12min to obtain a mixture A; the carbon content of the expanded graphite raw material is more than or equal to 96 percent, and the granularity is 5.0mm;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B; the three-roll speed ratio of the three-roll grinder is that a feed roll N3, a center roll N2, a discharge roll N1 is 1;
(3) Adding nano silicon powder into the nano graphene sheet/resin mixture B obtained by stripping, wherein the mass ratio of the mixture B to the nano silicon powder is 0.9;
(4) The mixture C was heat-treated in a tube furnace in an air atmosphere at 2 ℃ C. Min from room temperature -1 The temperature rising rate is 100 ℃, and the temperature is kept for 0.5h; then at 2 ℃ min -1 The temperature rising rate is up to 200 ℃, and the temperature is kept for 2 hours; then argon is introduced at 4 ℃ for min -1 The temperature rise rate of (2) is increased to 1000 ℃, the temperature is kept for 1h, and then the temperature is increased by 3 ℃ min -1 The temperature is raised to 1300 ℃ at the temperature raising rate, and the temperature is kept for 1h; then naturally cooling to room temperature to obtain a reaction mixture D;
(5) Smelting aluminum alloy at 670 ℃ for 3h, adding the crushed reaction mixture D into an aluminum alloy melt, adding a deslagging agent, pressing into a liquid level, repeatedly moving up and down, degassing, removing slag, and fully stirring to obtain a mixed melt E, wherein the mass ratio of the mixture D to the aluminum alloy is 0.1:10, namely 1:100, the deslagging agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount is 0.5wt% of the total mass of the aluminum alloy in the furnace;
(6) And pouring the mixed melt E into a mold, and finally, pouring and molding to obtain the silicon carbide/graphene-containing sandwich-structured aluminum alloy composite heat dissipation material.
Example 2
(1) Firstly, adding 2wt% of nickel nitrate nonahydrate into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 92.5wt% of thermoplastic phenolic resin, stirring and mixing for 10min, and then pouring 5.5wt% of expanded graphite into the mixture, and stirring for 20min to obtain a mixture A; the carbon content of the expanded graphite raw material is more than or equal to 96 percent, and the particle size is 2.0mm;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B; the three-roller speed ratio of the three-roller grinding machine is that a feed roller N3, a center roller N2, a discharge roller N1 is 1;
(3) Adding nano tungsten powder into the nano graphene sheet/resin mixture B obtained by stripping, wherein the mass ratio of the mixture B to the nano tungsten powder is 1.0, and mechanically stirring for 35min to obtain a mixture C, wherein the content of W in the nano tungsten powder is more than or equal to 99.5%, and the particle size is less than or equal to 100nm;
(4) The mixture C was heat-treated in a tube furnace in an air atmosphere at 3 ℃ C. Min from room temperature -1 The temperature rising rate is 100 ℃, and the temperature is kept for 0.8h; then at 2 ℃ min -1 The temperature rising rate is up to 200 ℃, and the temperature is preserved for 3 hours; then argon is introduced at 6 ℃ for min -1 The temperature is raised to 1000 ℃ at the temperature raising rate, the temperature is kept for 2 hours, and then the temperature is raised to 4 ℃ for min -1 The temperature is raised to 1350 ℃ at the temperature raising rate, and the temperature is kept for 2 hours; then naturally cooling to room temperature to obtain a reaction mixture D;
(5) Smelting an aluminum alloy at 680 ℃, wherein the smelting time is 4 hours, then adding a crushed reaction mixture D into an aluminum alloy melt, adding a deslagging agent, pressing into a liquid surface, repeatedly moving up and down, degassing, removing slag, and fully stirring to obtain a mixed melt E, wherein the mass ratio of the mixture D to the aluminum alloy is 0.1:20, namely 1:200, the deslagging agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount is 2wt.% of the total mass of the aluminum alloy in the furnace;
(6) And pouring the mixed melt E into a mold, and finally performing casting molding to obtain the tungsten carbide/graphene sandwich structure-containing aluminum alloy composite heat dissipation material.
Example 3
(1) Firstly, adding 5wt% of nickel nitrate nonahydrate into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 87.5wt% of thermoplastic phenolic resin, stirring and mixing for 10min, and then pouring 7.5wt% of expanded graphite into the mixture, and stirring for 20min to obtain a mixture A; the carbon content of the expanded graphite raw material is more than or equal to 96 percent, and the particle size is 2.0mm;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B; the three-roll speed ratio of the three-roll grinder is that a feed roll N3, a center roll N2, a discharge roll N1 is 1;
(3) Adding nano boron powder into the nano graphene sheet/resin mixture B obtained by stripping, wherein the mass ratio of the mixture B to the nano boron powder is 1.5;
(4) The mixture C was heat-treated in a tube furnace in an air atmosphere at 2 ℃ C. Min from room temperature -1 The temperature rising rate is 100 ℃, and the temperature is kept for 1h; then at 2 ℃ min -1 The temperature rising rate is up to 200 ℃, and the temperature is kept for 4 hours; then argon is introduced at 8 ℃ for min -1 The temperature is raised to 1000 ℃ at the temperature raising rate, the temperature is kept for 2 hours, and then the temperature is raised to 5 ℃ for min -1 The temperature is raised to 1400 ℃ at the temperature raising rate, and the temperature is kept for 3 hours; then naturally cooling to room temperature to obtain a reaction mixture D;
(5) Smelting an aluminum alloy at the temperature of 700 ℃, wherein the smelting time is 5 hours, then adding a crushed reaction mixture D into an aluminum alloy melt, adding a deslagging agent, pressing into a liquid surface, repeatedly moving up and down back and forth, degassing, removing slag, and fully stirring to obtain a mixed melt E, wherein the mass ratio of the mixture D to the aluminum alloy is 0.1:40, namely 1:400, the slag removing agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount of the slag removing agent is 2.2wt% of the total mass of the aluminum alloy in the furnace;
(6) And pouring the mixed melt E into a mold, and finally performing casting molding to obtain the boron carbide/graphene sandwich structure-containing aluminum alloy composite heat dissipation material.
The above additional technical features can be freely combined and used in superposition by those skilled in the art without conflict.
The above description is only a preferred embodiment of the present invention, and the technical solutions that achieve the objects of the present invention by basically the same means are within the protection scope of the present invention.

Claims (5)

1. A preparation method of an aluminum alloy composite heat dissipation material containing carbide/graphene sandwich structure for an LED lamp is characterized by comprising the following steps: the method comprises the following steps:
(1) Firstly, 0.51-5 wt% of nickel nitrate nonahydrate is added into ethanol until the nickel nitrate nonahydrate is completely dissolved; adding the prepared nitrate ethanol solution into 85.0-94.9 wt% of resin, stirring and mixing for 4-25 min, and then pouring 5.1-10.0 wt% of expanded graphite into the resin, stirring for 10-30 min to obtain a mixture A;
(2) Stripping the mixture A in the step (1) through a three-roll grinder, and circularly stripping for 12-20 times to obtain a nano graphene sheet/resin mixture B;
(3) Adding simple substance nano powder into the nano graphene sheet/resin mixture B obtained in the step (2) by stripping, wherein the mass ratio of the mixture B to the simple substance nano powder is 0.85-1.5: 1, mechanically stirring for 20-40 min to obtain a mixture C, wherein the elementary substance nano powder is one or more of silicon powder, boron powder, titanium powder, tungsten powder and zirconium powder, the content of a single substance in the elementary substance nano powder is more than or equal to 99.5%, and the particle size is less than or equal to 100nm;
(4) Placing the mixture C obtained in the step (3) in a tubular furnace with an air atmosphere for heat treatment at the room temperature of 2-3 ℃ for min -1 The temperature rising rate is 100 ℃, and the temperature is kept for 0.5 to 1 hour; then at 1-2 ℃ for min -1 The temperature rising rate is up to 200 ℃, and the temperature is kept for 2 to 4 hours; then introducing argon at 4-8 ℃ for min -1 The temperature is raised to 1000 ℃ at the heating rate, the temperature is kept for 1 to 3 hours, and then the temperature is raised to 3 to 5 ℃ min -1 The temperature is raised to 1300-1450 ℃ at the temperature raising rate, and the temperature is kept for 0.5-6 h; then naturally cooling to room temperatureObtaining a reaction mixture D;
(5) Smelting aluminum alloy at 660-700 ℃ for 3-6 h, then crushing the reaction mixture D obtained in the step (4), adding the crushed mixture D into an aluminum alloy melt, adding a deslagging agent, pressing the mixture into the liquid level, repeatedly moving up and down back and forth, degassing, slagging off, and fully stirring to obtain a mixed melt E;
(6) And pouring the mixed melt E into a mold, and finally, pouring and molding to obtain the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure.
2. The preparation method of the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp according to claim 1 is characterized in that: the carbon content of the expanded graphite raw material in the step (1) is more than or equal to 96 percent, and the particle size is 1.0-5.0 mm; the resin is linear thermoplastic epoxy resin or thermoplastic phenolic resin liquid.
3. The preparation method of the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp according to claim 1, wherein the preparation method comprises the following steps: the three-roll speed ratio of the three-roll grinder in the step (2) is that a feed roll N3, a central roll N2, a discharge roll N1 is 1.
4. The preparation method of the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp according to claim 1, wherein the preparation method comprises the following steps: the mass ratio of the mixture D to the aluminum alloy in the step (5) is 0.1-1: 5 to 50 percent, the slag removing agent is mixed powder of potassium chloride, anhydrous sodium sulphate and industrial salt, and the addition amount of the slag removing agent is 0.5 to 2.2 percent of the total mass of the aluminum alloy in the furnace.
5. The aluminum alloy composite heat dissipation material prepared by the preparation method of the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure for the LED lamp according to claim 1 is characterized in that: the aluminum alloy composite heat dissipation material containing the carbide/graphene sandwich structure is formed by preparing a nano graphene sheet from expanded graphite through three-roller grinding and stripping, reacting to obtain a carbide nanosheet sandwich structure, reacting to obtain a carbon nanotube, a carbide nanofiber, and decomposing and reducing to obtain nano metal Ni particles and aluminum alloy.
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RU2011154031A (en) * 2009-06-03 2013-07-20 Виланд-Верке Аг METHOD FOR PRODUCING COMPOSITE MATERIAL WITH METAL MATRIX
CN110240466A (en) * 2019-07-13 2019-09-17 南昌航空大学 A kind of low-carbon Ultra-low carbon carbon containing refractory and preparation method thereof combined containing the micro-nano graphite flake phenolic resin of two dimension removed in situ
CN110330320A (en) * 2019-07-13 2019-10-15 南昌航空大学 A kind of aluminium silicon carbide carbon refractory of low-carbon Ultra-low carbon and preparation method thereof

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RU2011154031A (en) * 2009-06-03 2013-07-20 Виланд-Верке Аг METHOD FOR PRODUCING COMPOSITE MATERIAL WITH METAL MATRIX
CN110240466A (en) * 2019-07-13 2019-09-17 南昌航空大学 A kind of low-carbon Ultra-low carbon carbon containing refractory and preparation method thereof combined containing the micro-nano graphite flake phenolic resin of two dimension removed in situ
CN110330320A (en) * 2019-07-13 2019-10-15 南昌航空大学 A kind of aluminium silicon carbide carbon refractory of low-carbon Ultra-low carbon and preparation method thereof

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