CN107314353A - A kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device and preparation method thereof - Google Patents

A kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device and preparation method thereof Download PDF

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CN107314353A
CN107314353A CN201710533656.3A CN201710533656A CN107314353A CN 107314353 A CN107314353 A CN 107314353A CN 201710533656 A CN201710533656 A CN 201710533656A CN 107314353 A CN107314353 A CN 107314353A
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graphene
layer
metal
heat dissipation
thermal conductivity
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CN107314353B (en
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雷达
易汉平
李勇
刘庆龙
孟根其其格
董布和
孙丽娅
焦瑞瑞
刘乐
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ORDOS CITY OF CHINESE REDBUD INNOVATION INSTITUTE
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ORDOS CITY OF CHINESE REDBUD INNOVATION INSTITUTE
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    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21LIGHTING
    • F21VFUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
    • F21V29/00Protecting lighting devices from thermal damage; Cooling or heating arrangements specially adapted for lighting devices or systems
    • F21V29/50Cooling arrangements
    • F21V29/70Cooling arrangements characterised by passive heat-dissipating elements, e.g. heat-sinks
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25DPROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
    • C25D15/00Electrolytic or electrophoretic production of coatings containing embedded materials, e.g. particles, whiskers, wires
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21LIGHTING
    • F21VFUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
    • F21V29/00Protecting lighting devices from thermal damage; Cooling or heating arrangements specially adapted for lighting devices or systems
    • F21V29/85Protecting lighting devices from thermal damage; Cooling or heating arrangements specially adapted for lighting devices or systems characterised by the material
    • FMECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F21LIGHTING
    • F21YINDEXING SCHEME ASSOCIATED WITH SUBCLASSES F21K, F21L, F21S and F21V, RELATING TO THE FORM OR THE KIND OF THE LIGHT SOURCES OR OF THE COLOUR OF THE LIGHT EMITTED
    • F21Y2115/00Light-generating elements of semiconductor light sources
    • F21Y2115/10Light-emitting diodes [LED]

Abstract

The invention discloses a kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device and preparation method thereof, belong to technical field of heat dissipation.The radiator includes:The graphene film layer and weld part of metal-based layer, uniform deposition on the metal-based layer surface;Its preparation method is as follows:Graphene powder, additive are added in ethanol solution, dispersed graphene dispersing solution is obtained with ultrasonic wave is scattered;Using uniform thickness bullion piece, after being surface-treated with dust technology, deionized water, absolute ethyl alcohol and ultrasonic wave, as negative electrode;Negative electrode and anode are immersed in graphene dispersing solution together and carry out electrophoretic deposition;Then metal-based layer is closely rolled into after multilayer cylindrical from one end, the other end is welded on the outside of cylinder after annealing, to the graphene metal composite multi-layer heat dissipation device that round pie is cut into perpendicular to the cylinder axial direction.Radiator heat-dissipation efficiency high, the technique of the present invention are simple, energy-conserving and environment-protective, cost are low, and radiating efficiency is high.

Description

A kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device and preparation method thereof
Technical field
The invention belongs to technical field of heat dissipation, more particularly to a kind of high thermal conductivity graphene metal composite multi-layer heat dissipation Device and preparation method thereof.
Background technology
Graphene is a kind of ultralight, ultra-thin, superpower and extra specific surface area quasi- two-dimensional material, surface density about 0.77mg/ m2, the thickness about 0.34nm of single-layer graphene, the toughness of graphene is fabulous, and modulus of elasticity is 1.0TPa, and microstrength is reachable 30GPa, is more than 100 times of traditional steel, theoretical specific surface area is 2630m2/ g, and with very high conduction, thermal conductivity Can, such as resistivity is 2 × 10-6Ω .cm, electron mobility is up to 2 × 105cm2/ V.S, horizontal thermal conductivity is about 5 at room temperature ×103W/m.K.Meanwhile, graphene has high heat endurance, chemical stability and excellent permeability resistance and wear resistence Energy.Therefore, before graphene has been owned by being widely applied in each field such as mechanics, electronics, optics, calorifics and new energy Scape, has especially attracted the extensive concern of people in terms of the synthesis of LED heat sink materials.LED is the new type light source of 21 century, tool Efficient height, long lifespan, the advantage that conventional light source such as cracky can not compare therewith.And LED radiating is bad can cause it Power supply is damaged, light decay is accelerated, reduced lifetime the problems such as, therefore, improve during radiating efficiency is the weight of LED illumination System performance boost Weight.The radiator of traditional LED lamp is all made of copper or aluminum material, and its structure is single, and heat dispersion is nor very It is good.
It is reported that appropriate in metal material add graphene, it can effectively improve its heat dispersion.Current graphite The synthetic method of alkene/metal composite heat radiation material mainly has three kinds:1st, graphene coated thermal dispersant coatings on metallic matrix;2nd, metal Powder method;3rd, refining method etc. altogether is melted.But it is due to the characteristics of graphene is easy reunites, appearance in composite is prepared above-mentioned The problems such as graphene dispersion is uneven and tends to inconsistent, so as to cause to reduce the radiating effect of graphene composite material.In addition, Often using organic coating come be bonded between graphene and metal base surface in first method, and general organic coating Thermal conductivity factor it is all very low, be unfavorable for the raising of heat dispersion.Latter two method is to improve the common method of metal combination property, But technique is more complicated, energy consumption is big, and is also possible to the phenomenons such as generation oxidation or interfacial reaction when high temperature burns and refined and causes material The reduction of performance.
The content of the invention
Present invention aims at for the problems of in the prior art, proposing a kind of high thermal conductivity graphene gold Belong to composite multi-layer radiator and preparation method thereof, method technique of the invention is simple, energy-conserving and environment-protective;The heat spreader structures of the present invention The low simultaneous, good heat dissipation effect of novel, cost, it is adaptable to LED radiating.
To achieve the above object, the present invention is adopted the following technical scheme that:
A kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device, it is characterised in that including:Metal-based layer, graphite Alkene film layer and weld part;Wherein, the graphene film layer uniform deposition forms graphene metal on metal-based layer surface Composite bed, graphene metal composite layer be closely rolled into round pie and formed metal-based layer and graphene film layer alternate it is folded Plus spiral multilayer composite construction, shape is welded in outermost graphene metal composite layer edge and multi-layer compound structure outer surface Into weld part.
The metal-based layer is any one sheet metal or aluminium in strip copper sheet in uniform thickness, aluminium flake, silver strip, platinum Alloy sheet, the metal-based layer thickness is the arbitrary value in the range of 0.05~1mm;The graphene film layer is by uniform electrophoresis The individual layer or few layer graphene lamella being deposited on the metal-based layer surface are constituted, and the graphene film uniformly lies low described On metal-based layer, and mutually combined closely between the metal-based layer or the graphene film.
A kind of preparation method of above-mentioned high thermal conductivity graphene metal composite multi-layer heat dissipation device, it is characterised in that:Including Following steps:
The first step:The graphene that 0.01~0.025mg/ml of concentration is configured to ethanol solution and graphene powder is mixed Liquid is closed, then, metal salt is added in the mixed liquor so that the concentration of metal salt reaches 0.3~1mg/ml, then with ultrasound Wavelength-division dissipates 3~5h, obtains dispersed graphene electrophoresis liquid;
Second step:Take the uniform thickness bullion piece that a thickness is 0.05~1mm as metal-based layer, be 5 in concentration Immersion removes its oxide on surface for 3 minutes in~10% dust technology, then is put into anhydrous second after repeatedly being rinsed with deionized water Ultrasound 5 minutes in alcoholic solution, after taking-up is dried, are used as negative electrode;
3rd step:Using the graphite flake suitable with the cathode size as anode, by the cathode surface and the sun Pole surface is provided parallel to, and the negative electrode and the anode spacing are maintained at 1~2cm, then, the negative electrode and described Anode is immersed in the graphene electrophoresis liquid obtained in the first step together, and electrophoresis is carried out under 80~160V DC voltage 1~6min is deposited, obtaining the uniform fold on the metal-based layer has the product of the graphene film layer;
4th step:The product obtained in the 3rd step is closely rolled into multilayer from one end as rotating shaft with steel nail to justify Another end margin of the product, then, the cylinder outer surface formation is fixed on method of laser welding and welded by cylinder body shape Socket part, obtains sample;
5th step:The sample obtained in 4th step is handled with 200~300 DEG C of annealing temperature in a nitrogen atmosphere 1~3h, after cooling, cuts into round pie structure, so as to obtain high thermal conductivity to perpendicular to the cylinder axial direction Graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention, it is characterised in that: The graphene is the individual layer or few layer graphene piece grown by CVD, and piece footpath is 5~50 microns.
According to the preparation method of the high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention, it is characterised in that: The metal salt is any one or a few combination among magnesium nitrate, aluminum nitrate, copper nitrate, silver nitrate.
The technique effect of the present invention
Technique according to the invention scheme, using the teaching of the invention it is possible to provide a kind of radiating efficiency height, simple technique, energy-conserving and environment-protective, cost are low Radiator and preparation method thereof.The radiator, can efficiently solve the trend of graphene in the composite it is inconsistent and The problems such as skewness, so as to increase substantially the coefficient of heat transfer of conventional metals heat abstractor.Radiator of the present invention Axial thermal conductivity coefficient be much larger than common metal radiator thermal conductivity factor, using the invention offer radiator, Neng Gouxun LED chip temperature is reduced fastly, radiating efficiency is improved, so as to extend the service life of LED lamp.
Brief description of the drawings
Fig. 1 is the structural representation for representing high thermal conductivity graphene metal composite multi-layer heat dissipation device provided by the present invention Figure.
Fig. 2 is the strabismus for representing high thermal conductivity graphene metal composite multi-layer heat dissipation device cross section provided by the present invention Figure.
Fig. 3 is the graphene film layer table of high thermal conductivity graphene metal composite multi-layer heat dissipation device provided by the present invention The scanning electron microscope diagram in face.
In figure:1-metal-based layer, 2-graphene film layer, 3-weld part.
Embodiment
Structure of high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention and preparation method thereof is entered below Row is described in detail.
First, the structure referring to the drawings to the high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention is carried out in detail Describe in detail bright.
The structure of high thermal conductivity graphene metal composite multi-layer heat dissipation device provided by the present invention is as shown in figure 1, this hair Bright high thermal conductivity graphene metal composite multi-layer heat dissipation device, including metal-based layer 1, graphene film layer 2 and weld part 3.The metal-based layer 1 is the alloy uniform thickness formed by any one metal or several metals among aluminium, copper, silver, platinum Strip sheet metal, its thickness is 0.05~1mm.Uniform deposition has one layer of graphene thin on the strip sheet metal surface Film layer 2, its thickness is equal with the thickness of individual layer or few layer graphene.The weld part 3 be in the high thermal conductivity graphene/ The outside of metal composite multi-layer heat dissipation device.
Fig. 2 is the oblique view of high thermal conductivity graphene metal composite multi-layer heat dissipation device cross section provided by the present invention. As can be seen that the high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention is to be sunk by the metal-based layer 1 with uniform Graphene film layer 2 of the product on the surface of metal-based layer 1 is closely rolled into round pie together and constituted, in radiating Inside device, the metal level 1 is alternateed with graphene film layer 2 and is superimposed, and forms a kind of spiral multilayer composite construction.
The graphene film layer 2 of the present invention is in the metal-based layer using electrophoretic deposition by above-mentioned graphene film Film formed by electro-deposition on 1 surface.
Fig. 3 is the graphene film for representing high thermal conductivity graphene metal composite multi-layer heat dissipation device provided by the present invention The surface topography scanning electron microscope diagram of layer 2.As shown in figure 3, the graphene film described in graphene film layer 2 is almost It is all parallel with substrate (metal-based layer 1), and equably lie low on the substrate surface, with the substrate or mutually it Between connect to obtain closed seamless.Show, high thermal conductivity graphene metal composite multi-layer heat dissipation device of the invention not only solves stone The trend problem of black alkene in the composite, and the contact area between graphene and basic unit is also increased, therefore, it is possible to big Amplitude improves the heat conductivility of radiator.
In addition, according to the high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention, its thickness can be according to reality Border situation is arbitrarily selected, i.e., can cut arbitrary dimension according to actual needs.The radius of the round pie radiator be with it is described Metal layer thickness, graphene film thickness degree are relevant with volume layer number, and arbitrary dimension can also be prepared according to actual needs.
High thermal conductivity graphene metal composite multi-layer heat dissipation device in order to further appreciate that the present invention and preparation method thereof, By the following examples, high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention and preparation method thereof is carried out detailed Describe in detail bright.
Embodiment 1:
The high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present invention, including metal-based layer 1, graphene film layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 1mm strip form aluminium flake.It is uniform on the strip form aluminium flake surface Deposition has one layer of graphene film layer 2, and its thickness is equal with the thickness of individual layer or few layer graphene.At the weld part 3 In the outside of the high thermal conductivity graphene aluminium composite multi-layer radiator.The high thermal conductivity graphene aluminium of the present invention is compound more Layer radiator is together with the graphene film layer 2 on the strip form aluminium flake surface of the strip form aluminium flake and uniform deposition Closely it is rolled into round pie and constitutes, inside radiator, the strip form aluminium flake is alternateed with graphene film layer 2 Superposition, forms a kind of spiral multilayer composite construction.The graphene film layer 2 of the present embodiment, being will using electrophoretic deposition Above-mentioned graphene film film formed by electro-deposition on the strip form aluminium flake surface.It is described in graphene film layer 2 Graphene film is nearly all parallel with substrate (strip form aluminium flake), and equably lies low on the substrate surface, with the substrate Or closed seamless is connected to obtain each other.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present embodiment, it includes following step Suddenly:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, it is the mixed of 0.015mg/ml to form concentration Liquid is closed, metal salt is added in the mixed liquor so that metal salt concentrations reach 0.3mg/ml, then, mixed liquor is used super Sound wave separating apparatus ultrasonic disperse 4h, obtains dispersed graphene electrophoresis liquid;Second step:In the super of the graphene mixed liquor In sound dispersion process, the bar shaped aluminium flake that a thickness is 1mm is taken, it as metal-based layer, is soaked in 5% dust technology Its oxide on surface is removed within 3 minutes, and is put into ultrasound 5 minutes in ethanol solution after repeatedly being rinsed with deionized water, It is standby as negative electrode after taking-up is dried;3rd step:Using the graphite flake of size suitable with the negative electrode as anode, by institute State cathode surface and the anode surface is provided parallel to, and the negative electrode is maintained at 1cm with the anode spacing, then, The negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step in the straight of 80V together Flow and electrophoretic deposition 6min is carried out under voltage, obtaining the uniform fold on the bar shaped aluminium flake has the production of the graphene film layer Thing;4th step:The product obtained by 4th step is closely rolled into multilayer circle with steel nail as rotating shaft from one end After cylinder shape, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In a nitrogen atmosphere with 200 DEG C annealing temperature processing 3h, after cooling, sample is cut into round pie structure to axial direction, led so as to obtain the height Hot property graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present embodiment, its used institute It is the individual layer or few layer graphene piece grown by CVD to state graphene, and piece footpath is about 30 microns.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present embodiment, its used institute It is aluminum nitrate to state metal salt.
Embodiment 2:
The high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present embodiment, including metal-based layer 1, graphene film Layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 0.05mm strip aluminum alloy sheet.In the strip aluminium alloy Uniform deposition has one layer of graphene film layer 2 on piece surface, and its thickness is equal with the thickness of individual layer or few layer graphene.Institute State the outside that weld part 3 is in the high thermal conductivity graphene aluminium composite multi-layer radiator.The high thermal conductivity stone of the present invention Black alkene aluminium alloy compound multi-layer heat dissipation device is on the strip aluminum alloy sheet surface by the strip aluminum alloy sheet and uniform deposition On graphene film layer 2 be closely rolled into round pie together and constitute, inside radiator, the strip aluminium alloy Piece is alternateed with graphene film layer 2 and is superimposed, and forms a kind of spiral multilayer composite construction.The graphite of the present embodiment Alkene film layer 2 be using electrophoretic deposition by above-mentioned graphene film on the strip aluminum alloy sheet surface formed by electro-deposition Film.Graphene film is nearly all parallel with substrate (strip aluminum alloy sheet) described in graphene film layer 2, and uniformly Horizon is lain on the substrate surface, with the substrate or being connected to obtain closed seamless each other.
According to the preparation method of the high thermal conductivity graphene aluminium alloy compound multi-layer heat dissipation device of the present embodiment, it include with Lower step:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, concentration is formed for 0.025mg/ml Mixed liquor, add metal salt in the mixed liquor so that metal salt concentrations reach 1mg/ml, then, and mixed liquor is used Ultrasonic wave separating apparatus ultrasonic disperse 4h, obtains dispersed graphene electrophoresis liquid;Second step:In the graphene mixed liquor During ultrasonic disperse, the bar shaped aluminium flake that a thickness is 0.05mm is taken, it as metal-based layer, in 10% dust technology Middle immersion removes its oxide on surface for 3 minutes, and is put into ultrasound 5 in ethanol solution after repeatedly being rinsed with deionized water Minute, it is standby as negative electrode after taking-up is dried;3rd step:Using the graphite flake of size suitable with the negative electrode as anode, The cathode surface and the anode surface are provided parallel to, and the negative electrode is maintained at 1cm with the anode spacing, so Afterwards, the negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step in 100V together DC voltage under carry out electrophoretic deposition 4min, obtaining the uniform fold on the bar shaped aluminium flake has graphene film layer Product;4th step:The product resulting in 4th step is closely rolled into multilayer with steel nail as rotating shaft from one end After cylindrical, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In a nitrogen atmosphere with 300 DEG C of annealing temperature processing 2h, after cooling, round pie structure is cut into by sample to axial direction, so as to obtain described High thermal conductivity graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene aluminium alloy compound multi-layer heat dissipation device of the present embodiment, it is used The graphene be the individual layer that is grown by CVD or few layer graphene piece, piece footpath is about 50 microns.
According to the preparation method of the high thermal conductivity graphene aluminium alloy compound multi-layer heat dissipation device of the present embodiment, it is used The metal salt be magnesium nitrate.
Embodiment 3:
The high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present embodiment, including metal-based layer 1, graphene film Layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 0.1mm strip copper sheet.On the strip copper sheet surface Uniform deposition has one layer of graphene film layer 2, and its thickness is equal with the thickness of individual layer or few layer graphene.The weld part 3 are in the outside of the high thermal conductivity graphene copper composite multi-layer radiator.The high thermal conductivity graphene copper of the present embodiment Composite multi-layer radiator is by the strip copper sheet and the graphene film of the uniform deposition on the strip copper sheet surface Layer 2 is closely rolled into round pie together and constituted, inside radiator, the strip copper sheet and graphene film layer 2 Superposition is alternateed, a kind of spiral multilayer composite construction is formed.The graphene film layer 2 of the present embodiment is heavy using electrophoresis Area method film formed by electro-deposition on the strip copper sheet surface by above-mentioned graphene film.In graphene film layer 2 Described in graphene film it is nearly all parallel with substrate (strip copper sheet), and equably lie low on the substrate surface, with institute State substrate or connect to obtain closed seamless each other.
According to the preparation method of the high thermal conductivity graphene copper composite multi-layer radiator of the present embodiment, it includes following step Suddenly:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, the mixing that concentration is 0.02mg/ml is formed Liquid, metal salt is added in the mixed liquor so that metal salt concentrations reach 0.6mg/ml, then, by mixed liquor ultrasound Ripple separating apparatus ultrasonic disperse 5h, obtains dispersed graphene electrophoresis liquid;Second step:In the ultrasound of the graphene mixed liquor In dispersion process, the bar shaped copper sheet that a thickness is 0.1mm is taken, it as metal-based layer, is soaked in 8% dust technology Its oxide on surface is removed within 3 minutes, and is put into ultrasound 5 minutes in ethanol solution after repeatedly being rinsed with deionized water, It is standby as negative electrode after taking-up is dried;3rd step:Using the graphite flake of size suitable with the negative electrode as anode, by institute State cathode surface and the anode surface is provided parallel to, and the negative electrode is maintained at 1.5cm with the anode spacing, so Afterwards, the negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step in 120V together DC voltage under carry out electrophoretic deposition 3min, obtaining the uniform fold on the bar shaped copper sheet has graphene film layer Product;4th step:The product resulting in 4th step is closely rolled into multilayer with steel nail as rotating shaft from one end After cylindrical, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In a nitrogen atmosphere with 300 DEG C of annealing temperature processing 1h, after cooling, round pie structure is cut into by sample to axial direction, so as to obtain described High thermal conductivity graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene copper composite multi-layer radiator of the present embodiment, its used institute It is the individual layer or few layer graphene piece grown by CVD to state graphene, and piece footpath is about 20 microns.
According to the preparation method of the high thermal conductivity graphene copper composite multi-layer radiator of the present embodiment, its used institute It is copper nitrate to state metal salt.
Embodiment 4:
The high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present embodiment, including metal-based layer 1, graphene film Layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 0.5mm strip silver strip.On the strip silver strip surface Uniform deposition has one layer of graphene film layer 2, and its thickness is equal with the thickness of individual layer or few layer graphene.The weld part 3 outsides in the silver-colored composite multi-layer radiator of the high thermal conductivity graphene.High thermal conductivity graphene/the silver of the present embodiment Composite multi-layer radiator is by the strip silver strip and the graphene film of the uniform deposition on the strip silver strip surface Layer 2 is closely rolled into round pie together and constituted, inside radiator, the strip silver strip and graphene film layer 2 Superposition is alternateed, a kind of spiral multilayer composite construction is formed.The graphene film layer 2 of the present embodiment is heavy using electrophoresis Area method film formed by electro-deposition on the strip silver strip surface by above-mentioned graphene film.In graphene film layer 2 Described in graphene film it is nearly all parallel with substrate (strip silver strip), and equably lie low on the substrate surface, with institute State substrate or connect to obtain closed seamless each other.
According to the preparation method of the silver-colored composite multi-layer radiator of the high thermal conductivity graphene of the present embodiment, it includes following step Suddenly:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, the mixing that concentration is 0.01mg/ml is formed Liquid, metal salt is added in the mixed liquor so that metal salt concentrations reach 0.3mg/ml, then, by mixed liquor ultrasound Ripple separating apparatus ultrasonic disperse 3h, obtains dispersed graphene electrophoresis liquid;Second step:In the ultrasound of the graphene mixed liquor In dispersion process, the bar shaped silver strip that a thickness is 0.5mm is taken, it as metal-based layer, is soaked in 5% dust technology Its oxide on surface is removed within 3 minutes, and is put into ultrasound 5 minutes in ethanol solution after repeatedly being rinsed with deionized water, It is standby as negative electrode after taking-up is dried;3rd step:Using the graphite flake of size suitable with the negative electrode as anode, by institute State cathode surface and the anode surface is provided parallel to, and the negative electrode is maintained at 2cm with the anode spacing, then, The negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step 160V's together Electrophoretic deposition 6min is carried out under DC voltage, obtaining the uniform fold on the bar shaped silver strip has the production of the graphene film layer Thing;4th step:The product obtained by 4th step is closely rolled into multilayer circle with steel nail as rotating shaft from one end After cylinder shape, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In a nitrogen atmosphere with 250 DEG C annealing temperature processing 2h, after cooling, sample is cut into round pie structure to axial direction, led so as to obtain the height Hot property graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the silver-colored composite multi-layer radiator of the high thermal conductivity graphene of the present invention, it is used described Graphene is the individual layer or few layer graphene piece grown by CVD, and piece footpath is about 10 microns.
According to the preparation method of the silver-colored composite multi-layer radiator of the high thermal conductivity graphene of the present embodiment, its used institute It is silver nitrate to state metal salt.
Embodiment 5:
The high thermal conductivity graphene platinum composite multi-layer radiator of the present embodiment, including metal-based layer 1, graphene film Layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 0.2mm strip platinum piece.On the strip silver strip surface Upper uniform deposition has one layer of graphene film layer 2, and its thickness is equal with the thickness of individual layer or few layer graphene.The welding Portion 3 is in the outside of the high thermal conductivity graphene platinum composite multi-layer radiator.The high thermal conductivity graphite of the present embodiment Alkene platinum composite multi-layer radiator is as described in the strip platinum piece and uniform deposition on the strip platinum piece surface Graphene film layer 2 is closely rolled into round pie together and constituted, inside radiator, the strip platinum piece and the stone Black alkene film layer 2 alternates superposition, forms a kind of spiral multilayer composite construction.The graphene film layer 2 of the present embodiment Be using electrophoretic deposition by above-mentioned graphene film the film formed by electro-deposition on the strip platinum piece surface.Described Graphene film is nearly all parallel with substrate (strip platinum piece) described in graphene film layer 2, and equably lies low described On substrate surface, with the substrate or being connected to obtain closed seamless each other.
According to the preparation method of the high thermal conductivity graphene platinum composite multi-layer radiator of the present embodiment, it includes following Step:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, it is 0.015mg/ml's to form concentration Mixed liquor, metal salt is added in the mixed liquor so that metal salt concentrations reach 0.3mg/ml, then, and mixed liquor is used Ultrasonic wave separating apparatus ultrasonic disperse 4h, obtains dispersed graphene electrophoresis liquid;Second step:In the graphene mixed liquor During ultrasonic disperse, the bar shaped platinum piece that a thickness is 0.5mm is taken, it as metal-based layer, in 10% dilute nitre Immersion removes its oxide on surface for 3 minutes in acid, then is put into ultrasound 5 in ethanol solution after repeatedly being rinsed with deionized water Minute, it is standby as negative electrode after taking-up is dried;3rd step:Using the graphite flake of size suitable with the negative electrode as anode, The cathode surface and the anode surface are provided parallel to, and the negative electrode is maintained at 2cm with the anode spacing, so Afterwards, the negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step in 150V together DC voltage under carry out electrophoretic deposition 6min, obtaining the uniform fold on the bar shaped platinum piece has graphene film layer Product;4th step:The product resulting in 4th step is closely rolled into steel nail as rotating shaft from one end many After layer cylindrical, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In 300 DEG C of temperature 3h is made annealing treatment, after cooling, sample round pie structure is cut into axial direction, so as to obtain the high thermal conductivity stone Black alkene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene platinum composite multi-layer radiator of the present invention, its used institute It is the individual layer or few layer graphene piece grown by CVD to state graphene, and piece footpath is about 5 microns.
According to the preparation method of the high thermal conductivity graphene platinum composite multi-layer radiator of the present embodiment, used in it The metal salt is magnesium nitrate.
Embodiment 6:
The high thermal conductivity graphene metal composite multi-layer heat dissipation device of the present embodiment, including metal-based layer 1, graphene film Layer 2 and weld part 3.The metal-based layer 1 is made up of thickness for 0.1mm strip form aluminium flake.On the strip form aluminium flake surface Uniform deposition has one layer of graphene film layer 2, and its thickness is equal with the thickness of individual layer or few layer graphene.The weld part 3 are in the outside of the high thermal conductivity graphene aluminium composite multi-layer radiator.The high thermal conductivity graphene/aluminum of the present invention is answered It is the graphene film layer 2 by the strip form aluminium flake and uniform deposition on the strip form aluminium flake surface to close multi-layer heat dissipation device Closely it is rolled into round pie together and constitutes, inside radiator, the strip form aluminium flake and graphene film layer 2 is mutual Alternately it is superimposed, forms a kind of spiral multilayer composite construction.The graphene film layer 2 of the present embodiment is to utilize electrophoretic deposition By above-mentioned graphene film on the strip form aluminium flake surface film formed by electro-deposition.The institute in graphene film layer 2 State graphene film nearly all parallel with substrate (strip form aluminium flake), and equably lie low on the substrate surface, with the lining Bottom connects to obtain closed seamless each other.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present invention, it includes following step Suddenly:The first step:The ethanol solution of one glass of sufficient amount is taken, graphene powder is added, it is the mixed of 0.025mg/ml to form concentration Liquid is closed, metal salt is added in the mixed liquor so that metal salt concentrations reach 0.8mg/ml, then, mixed liquor is used super Sound wave separating apparatus ultrasonic disperse 4h, obtains dispersed graphene electrophoresis liquid;Second step:In the super of the graphene mixed liquor In sound dispersion process, the bar shaped aluminium flake that a thickness is 0.1mm is taken, it as metal-based layer, is soaked in 5% dust technology Bubble removes its oxide on surface for 3 minutes, and is put into 5 points of ultrasound in ethanol solution after repeatedly being rinsed with deionized water Clock, it is standby as negative electrode after taking-up is dried;3rd step:, will using the graphite flake of size suitable with the negative electrode as anode The cathode surface and the anode surface are provided parallel to, and the negative electrode is maintained at 1cm with the anode spacing, so Afterwards, the negative electrode and the anode are immersed in the graphene electrophoresis liquid obtained in the first step in 120V together DC voltage under carry out electrophoretic deposition 1min, obtaining the uniform fold on the bar shaped aluminium flake has graphene film layer Product;4th step:The product resulting in 4th step is closely rolled into multilayer with steel nail as rotating shaft from one end After cylindrical, the other end is fixed on method of laser welding on the outside of the cylinder;5th step:In a nitrogen atmosphere with 200 DEG C of annealing temperature processing 3h, after cooling, round pie structure is cut into by sample to axial direction, so as to obtain described High thermal conductivity graphene metal composite multi-layer heat dissipation device.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present embodiment, its used institute It is the individual layer or few layer graphene piece grown by CVD to state graphene, and piece footpath is about 40 microns.
According to the preparation method of the high thermal conductivity graphene aluminium composite multi-layer radiator of the present embodiment, its used institute It is aluminum nitrate to state metal salt.
The basic characteristics of several high thermal conductivity graphene metal composite multi-layer heat dissipation devices are described in the embodiment above And preparation method, and it should be understood by those skilled in the art that, the present invention is not limited to the above embodiments, above-described embodiment and The design feature and principle that simply illustrate the present invention described in specification, are not departing from the premise of spirit and scope of the invention Under, various changes and modifications of the present invention are possible, and these changes and improvements all fall within the protetion scope of the claimed invention.This hair Bright claimed scope is by appended claims and its equivalent thereof.

Claims (6)

1. a kind of high thermal conductivity graphene metal composite multi-layer heat dissipation device, it is characterised in that including:Metal-based layer, graphene Film layer and weld part;Wherein, the graphene film layer uniform deposition forms graphene metal on metal-based layer surface and answered Close layer, graphene metal composite layer is closely rolled into round pie and forms metal-based layer and graphene film layer and alternate and be superimposed Spiral multilayer composite construction, outermost graphene metal composite layer edge welds to be formed with multi-layer compound structure outer surface Weld part.
2. graphene metal composite multi-layer heat dissipation device as claimed in claim 1, it is characterised in that the metal-based layer is that thickness is equal Even strip copper sheet, aluminium flake, silver strip, any one sheet metal or aluminum alloy sheet in platinum, the metal-based layer thickness is Arbitrary value in the range of 0.05~1mm.
3. graphene metal composite multi-layer heat dissipation device as claimed in claim 1 or 2, it is characterised in that the graphene film layer It is to be made up of individual layer of the uniform electrophoretic deposition on the metal-based layer surface or few layer graphene lamella, the graphene film is equal It is even to lie low on the metal-based layer, and mutually combined closely between the metal-based layer or the graphene film.
4. a kind of preparation method of high thermal conductivity graphene metal composite multi-layer heat dissipation device as claimed in claim 1, it is special Levy and be:Comprise the following steps:
The first step:The graphene that concentration is 0.01~0.025mg/ml is configured to ethanol solution and graphene powder to mix Liquid, then, metal salt is added in the mixed liquor so that the concentration of metal salt reaches 0.3~1mg/ml, then uses ultrasonic wave Scattered 3~5h, obtains dispersed graphene electrophoresis liquid;
Second step:The uniform thickness bullion piece that a thickness is 0.05~1mm is taken as metal-based layer, 5~10% it is dilute Immersion removes its oxide on surface for 3 minutes in nitric acid, then is put into ethanol solution after repeatedly being rinsed with deionized water and surpasses Sound 5 minutes, after taking-up is dried, is used as negative electrode;
3rd step:Using the graphite flake suitable with the cathode size as anode, by the cathode surface and the anode table Face is provided parallel to, and the negative electrode is maintained at 1~2cm with the anode spacing, then, the negative electrode and the anode It is immersed in together in the graphene electrophoresis liquid obtained in the first step, electrophoretic deposition is carried out under 80~160V DC voltage 1~6min, obtaining the uniform fold on the metal-based layer has the product of the graphene film layer;
4th step:The product obtained in the 3rd step is closely rolled into multilayer cylinder from one end as rotating shaft with steel nail Another end margin of the product, then, the cylinder outer surface formation weld part is fixed on method of laser welding by shape, Obtain sample;
5th step:By the sample obtained in the 4th step in a nitrogen atmosphere with 200~300 DEG C of annealing temperature processing 1~ 3h, after cooling, round pie structure is cut into perpendicular to the cylinder axial direction, so as to obtain high thermal conductivity graphite Alkene metal composite multi-layer heat dissipation device.
5. the preparation method of high thermal conductivity graphene metal composite multi-layer heat dissipation device according to claim 4, its feature It is:The graphene is the individual layer or few layer graphene piece grown by CVD, and piece footpath is 5~50 microns.
6. the preparation method of high thermal conductivity graphene metal composite multi-layer heat dissipation device according to claim 4, its feature It is:The metal salt is any one or a few combination among magnesium nitrate, aluminum nitrate, copper nitrate, silver nitrate.
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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108790368A (en) * 2018-08-30 2018-11-13 兰州交通大学 A kind of preparation method of bullet train IGBT encapsulation graphene/metallic composite
CN113028322A (en) * 2021-03-19 2021-06-25 鄂尔多斯市紫荆创新研究院 LED street lamp
CN115033088A (en) * 2022-06-28 2022-09-09 北京石墨烯技术研究院有限公司 Graphene metal high-thermal-conductivity server radiator and preparation method thereof

Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102538552A (en) * 2010-12-28 2012-07-04 常州碳元科技发展有限公司 Bundle membrane material highly radiating structure and manufacturing method thereof
CN102564200A (en) * 2010-12-31 2012-07-11 上海杰远环保科技有限公司 Roller type high-heat-radiation structure and manufacturing method thereof
CN103123830A (en) * 2013-03-14 2013-05-29 南京科孚纳米技术有限公司 Method for preparing graphene wire and cable
CN103456581A (en) * 2013-09-10 2013-12-18 中国科学院深圳先进技术研究院 Carbon nanometer tube field emitting cathode and manufacturing method thereof
CN104217907A (en) * 2014-09-12 2014-12-17 中国科学院深圳先进技术研究院 Preparation method for graphene field emitting cathode, and graphene field emitting cathode
WO2015142635A1 (en) * 2014-03-18 2015-09-24 Ut-Battelle, Llc Graphene reinforced materials and methods of manufacture
CN106626556A (en) * 2016-12-28 2017-05-10 镇江博昊科技有限公司 Copper-based graphene composite film coil
CN106756869A (en) * 2016-12-09 2017-05-31 中国科学院上海微***与信息技术研究所 A kind of method that Graphene is grown without adhesion metal Mi Dui

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102538552A (en) * 2010-12-28 2012-07-04 常州碳元科技发展有限公司 Bundle membrane material highly radiating structure and manufacturing method thereof
CN102564200A (en) * 2010-12-31 2012-07-11 上海杰远环保科技有限公司 Roller type high-heat-radiation structure and manufacturing method thereof
CN103123830A (en) * 2013-03-14 2013-05-29 南京科孚纳米技术有限公司 Method for preparing graphene wire and cable
CN103456581A (en) * 2013-09-10 2013-12-18 中国科学院深圳先进技术研究院 Carbon nanometer tube field emitting cathode and manufacturing method thereof
WO2015142635A1 (en) * 2014-03-18 2015-09-24 Ut-Battelle, Llc Graphene reinforced materials and methods of manufacture
CN104217907A (en) * 2014-09-12 2014-12-17 中国科学院深圳先进技术研究院 Preparation method for graphene field emitting cathode, and graphene field emitting cathode
CN106756869A (en) * 2016-12-09 2017-05-31 中国科学院上海微***与信息技术研究所 A kind of method that Graphene is grown without adhesion metal Mi Dui
CN106626556A (en) * 2016-12-28 2017-05-10 镇江博昊科技有限公司 Copper-based graphene composite film coil

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108790368A (en) * 2018-08-30 2018-11-13 兰州交通大学 A kind of preparation method of bullet train IGBT encapsulation graphene/metallic composite
CN113028322A (en) * 2021-03-19 2021-06-25 鄂尔多斯市紫荆创新研究院 LED street lamp
CN115033088A (en) * 2022-06-28 2022-09-09 北京石墨烯技术研究院有限公司 Graphene metal high-thermal-conductivity server radiator and preparation method thereof

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