CN105986158A - High-thermal-conductivity diamond-metal composite material and preparation method thereof - Google Patents

High-thermal-conductivity diamond-metal composite material and preparation method thereof Download PDF

Info

Publication number
CN105986158A
CN105986158A CN201510075147.1A CN201510075147A CN105986158A CN 105986158 A CN105986158 A CN 105986158A CN 201510075147 A CN201510075147 A CN 201510075147A CN 105986158 A CN105986158 A CN 105986158A
Authority
CN
China
Prior art keywords
composite
diamond
mixture
metallic matrix
boron
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
CN201510075147.1A
Other languages
Chinese (zh)
Other versions
CN105986158B (en
Inventor
马洪兵
白华
江南
张军安
西村仁
西村一仁
邹煌辉
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Ningbo Jingduan Industrial Technology Co ltd
Ningbo Institute of Material Technology and Engineering of CAS
Original Assignee
Ningbo Jingduan Industrial Technology Co ltd
Ningbo Institute of Material Technology and Engineering of CAS
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Ningbo Jingduan Industrial Technology Co ltd, Ningbo Institute of Material Technology and Engineering of CAS filed Critical Ningbo Jingduan Industrial Technology Co ltd
Priority to CN201510075147.1A priority Critical patent/CN105986158B/en
Publication of CN105986158A publication Critical patent/CN105986158A/en
Application granted granted Critical
Publication of CN105986158B publication Critical patent/CN105986158B/en
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Landscapes

  • Cooling Or The Like Of Semiconductors Or Solid State Devices (AREA)
  • Powder Metallurgy (AREA)

Abstract

The invention relates to a diamond-metal composite material. Specifically, the composite material comprises metal matrices and diamond composites. The diamond composites comprise diamond particles and surface coatings compounded on the surfaces of the diamond particles. The invention further discloses a preparation method and application of the composite material. The preparation method is simple, effective, feasible, and low in cost, and the obtained composite material is excellent in performance and has great market prospects in the fields of electronic packaging and heat sink.

Description

A kind of high heat-conductive diamond-metallic composite and preparation method thereof
Technical field
The present invention relates to diamond composite field, be specifically related to a kind of high heat-conductive diamond-Metals composite Material and preparation method thereof.
Background technology
Along with being increasingly miniaturized and the development of highly integrated high power, high power device running of electronic product The event that middle hot injury causes device normally to work accounts for more than the 60% of whole electronic device loss rate.Cause This has the high heat sink material with electronic device matched coefficients of thermal expansion of heat conductivity and is paid close attention to widely.
With high thermal conductivity coefficient CNT, diamond is for strengthening phase, with the metal such as Al, Cu, Ag as matrix Third generation Heat Conduction Material be just continuously developed, but there is also some problems.For diamond-aluminium composite material For, most researchers excessively focuses on the raising of heat conductivity, ignores composite and prepared Cheng Zhong, facile hydrolysis phase Al4C3Generation cause composite to ultimately result at humid air median surface poor stability The composite of preparation cannot obtain preferably application in practice.Poor for two-phase interface bond strength For diamond-copper (silver-colored) composite, in existing preparation process condition, often introduce carbon in the two interface Compound element (such as B, W, Cr, Ti, Mo, Si etc.) obtains preferable binding ability, but boundary layer one As thermal conductivity relatively low, interfacial layer thickness controls improper to affect obtained matrices of composite material to a certain extent Thermal conductivity, thus cause heat conductivity to decline.
In sum, this area has the compound of high heat conductance and high stability in the urgent need to exploitation is a kind of simultaneously Material.
Summary of the invention
It is an object of the invention to provide a kind of composite with high heat conductance and high stability.
A first aspect of the present invention, it is provided that a kind of diamond-metallic composite, described composite comprises Metallic matrix and the diamond complex compound with described metallic matrix, wherein,
Described diamond complex comprises diamond particles and is compound in the plated surface of described diamond particle surfaces Layer;
Described overlay coating comprises the boron carbide layer being compound in described diamond particle surfaces and is compound in described carbonization The boron layer on boron layer surface.
In another preference, described in be complex as chemical bonds.
In another preference, described metallic matrix is selected from lower group: copper, aluminum, silver or its alloy or its group Close.
In another preference, being shaped as of described metallic matrix: graininess, sheet.
In another preference, the particle diameter of described metallic matrix is 1-400 μm, preferably 10-100 μm, more Goodly for 30-80 μm.
In another preference, the particle diameter of described diamond complex is 80-520 μm.
In another preference, the particle diameter of described diamond complex is 100-500 μm, preferably 150-420 μm, is more preferably 200-400 μm.
In another preference, described diamond complex be shaped as graininess.
In another preference, based on the cumulative volume of described composite, the volume hundred of described diamond complex Proportion by subtraction is 15-85%.
In another preference, based on the cumulative volume of described composite, the volume hundred of described diamond complex Proportion by subtraction is 40%-85%, preferably 45%-85%, is more preferably 50%-80%.
In another preference, described overlay coating thickness is 1-5000nm.
In another preference, described overlay coating thickness is 10-3000nm, preferably 100-2000nm, more Goodly for 100-1000nm, it is most preferably 100-200nm.
In another preference, described overlay coating is evenly coated at described diamond particle surfaces.
In another preference, in described overlay coating, the thickness ratio of described boron carbide layer and described boron layer is 1: 200, preferably 1:100, be more preferably 1:1.
In another preference, the thickness of described boron carbide layer is 1-500nm, preferably 1-50nm, more Goodly for 1-40nm.
In another preference, the thickness of described boron layer is 1-2000nm, preferably 1-500nm, more preferably Ground is 1-80nm.
In another preference, described composite has one or more features selected from lower group:
1) when metallic matrix is aluminum, the thermal conductivity of gained composite >=480W/m k;
2) when metallic matrix is aluminum, the thermal coefficient of expansion≤8.3ppm/K of gained composite;
3) when metallic matrix is copper, the thermal conductivity of gained composite >=528W/m K;
4) when metallic matrix is copper, the thermal coefficient of expansion≤8.8ppm/k of gained composite;
In another preference, without hydrolysis phase in described composite.
A second aspect of the present invention, it is provided that the preparation side of the composite described in a kind of first aspect present invention Method, described method comprises the steps:
A-1) provide a kind of by diamond particles, boron raw material and the homogeneous mixture A of organic solution composition;
A-2) under vacuo, mixture A described in heat treatment, obtain diamond complex;
B-1) a kind of step a-2 is provided) diamond complex of gained and the mixture B of raw metal;
B-2) mixture B described in hot pressed sintering, obtains the composite described in first aspect present invention.
In another preference, described boron raw material is powder, liquid.
In another preference, described boron raw material is selected from lower group: boron powder, boride or a combination thereof.
In another preference, the particle diameter of described boron raw material is 100-50000nm, preferably 100-20000nm; It is more preferably 100-10000nm.
In another preference, the particle diameter of described diamond particles is 100-500 μm, preferably 150-400 μm, It it is more preferably 200-400 μm.
In another preference, described organic solution is selected from lower group: ethanol, polyvinyl alcohol water solution, poly-second two Alcohol-water solution or a combination thereof.
In another preference, based on the gross weight of described mixture A, the content of diamond particles is 80- 99wt%;And/or
The content of boron raw material is 1-15wt%.
In another preference, based on the gross weight of described mixture A, the content of diamond particles is 85- 99wt%, preferably 85-95wt%.
In another preference, based on the gross weight of described mixture A, the content of boron raw material is 1-12wt%, Preferably 1-10wt%.
In another preference, described heat treatment temperature is 1000-1400 DEG C, preferably 1000-1350 DEG C, more Goodly for 1000-1300 DEG C.
In another preference, the heat treatment time in described heat treatment temperature is 30-300min, preferably 30-100min, is more preferably 30-60min.
In another preference, described vacuum≤10-1Pa;Preferably 10-2Pa。
In another preference, described heat treatment is carried out in vacuum carbon tube furnace.
In another preference, described vacuum carbon tube furnace is heated to heat treatment temperature with rate of heat addition 1-40 DEG C/min, Preferably 5-10 DEG C/min, is more preferably 8-10 DEG C/min.
In another preference, the sintering temperature of described mixture B is 600-2000 DEG C, preferably 700-1500 DEG C, more preferably it is 700-1200 DEG C.
In another preference, the sintering time of described mixture B is 30-300min, preferably 60-150min, It is more preferably 60-120min.
In another preference, the pressure of described mixture B hot pressed sintering is 30-150MPa, preferably 40-80MPa。
In another preference, described mould is warmed up to sintering temperature with the rate of heat addition of 5-50 DEG C/min, preferably The rate of heat addition be 5-30 DEG C/min, the more preferably rate of heat addition be 5-25 DEG C/min.
A third aspect of the present invention, it is provided that a kind of goods, described goods comprise described in first aspect present invention Composite or be made up of the composite described in first aspect present invention.
A fourth aspect of the present invention, it is provided that the purposes of the composite described in a kind of first aspect present invention, uses In processing machinery goods, composite, electronic devices and components.
In another preference, described machinework is selected from lower group: cutter, grinding tool, file, emery wheel, saw Sheet, drill bit.
In another preference, described electronic devices and components are selected from lower group: encapsulation base material, fin.
In should be understood that within the scope of the present invention, above-mentioned each technical characteristic of the present invention and below (such as embodiment) Can be combined with each other between each technical characteristic of middle specific descriptions, thus constitute new or preferred technical side Case.As space is limited, the most tired at this state.
Accompanying drawing explanation
Fig. 1 be the SEM figure of the embodiment of the present invention 1 diamond complex 1 and EDS can spectrogram, a) and b) SEM for diamond complex 1 schemes, and c) is that the EDS of diamond complex 1 can spectrogram.
Fig. 2 a) it is the SEM picture of the composite 1 of the embodiment of the present invention 1, Fig. 2 b) it is the embodiment of the present invention 3 The SEM picture of composite 3.
Fig. 3 a) it is the XRD figure sheet of the composite 1 of the embodiment of the present invention 1, Fig. 3 b) it is the embodiment of the present invention 3 The XRD figure sheet of composite 3.
Fig. 4 a) and b) be the SEM picture of composite C1 of comparative example 1 of the present invention, Fig. 4 c) it is the present invention couple The SEM picture of the composite C2 of ratio 2.
Detailed description of the invention
The present inventor is through in-depth study for a long time, it has unexpectedly been found that diamond carries out surface process, After its plated surface boron carbide layer and boron layer, then by itself and metal composite, can prepare have simultaneously high heat conductance, High stability and the composite of low thermal coefficient of expansion.Based on above-mentioned discovery, inventor completes the present invention.
Term
As used herein, term " overlay coating of the present invention ", " overlay coating " or " carbide lamella " are interchangeable Use, refer both to be compound in the boron carbide layer of described diamond particle surfaces and be compound in described boron carbide layer surface The coating that boron layer is formed.
Diamond particles
In the present invention, described diamond particles is not particularly limited.
Typically, the shape of described diamond includes (but being not limited to): powdery, bulk, lamellar or film Shape.
Typically, described diamond is natural or for generating through high temperature, high pressure or chemical gaseous phase deposition.
In the present invention, the particle diameter of described diamond particles is not particularly limited, can be arbitrary dimension Grain.
Specifically, the particle diameter of described diamond particles is preferably 100-500 μm, preferably 150-400 μm, more Goodly for 200-400 μm.
Diamond particles used by the present invention is the substrate for boride layer of the present invention growth, is the most also diffusion The carrier of boron atom.In the present invention, diamond is the indispensable carrier material of boron atoms permeating, Buddha's warrior attendant Stone is due to the feature of its lattice parameter so that boron atom forms uniform boride layer at diamond surface.
Boron raw material
In the present invention, described boron raw material is not particularly limited.
Typically, the shape of described boron raw material includes (but being not limited to): powder, liquid.
Typically, described boron raw material includes (but being not limited to): boron powder, boride or a combination thereof.
Typically, the particle diameter of described boron raw material is 100-50000nm, preferably 100-20000nm;More preferably For 100-10000nm.
Organic solution
In the present invention, described organic solution is not particularly limited, and can select the material that this area is conventional, or Person prepares by conventional method, or is commercially available from market.
Typically, described organic solution includes (but being not limited to): ethanol, polyvinyl alcohol water solution, poly- Glycol water or a combination thereof.
Composite
The invention provides a kind of diamond-metallic composite, described composite comprise metallic matrix and with institute State the diamond complex that metallic matrix is compound, wherein,
Described diamond complex comprises diamond particles and is compound in the plated surface of described diamond particle surfaces Layer;
Described overlay coating comprises the boron carbide layer being compound in described diamond particle surfaces and is compound in described carbonization The boron layer on boron layer surface.
In another preference, described in be complex as chemical bonds.
The metallic matrix of the present invention include field of radiating can metal (including simple metal and alloy), do not have Limit especially.
Typically, described metallic matrix includes (but being not limited to): copper, aluminum, silver or its alloy or A combination thereof.
Typically, the shape of described metallic matrix includes (but being not limited to): graininess, sheet.
Typically, the particle diameter of described metallic matrix is preferably 1-400 μm, preferably 10-100 μm, more preferably For 30-80 μm.
In the present invention, the particle diameter of described diamond complex is not particularly limited, preferably 80-520 μm.
Typically, the particle diameter of described diamond complex is 100-500 μm, preferably 150-420 μm, more Goodly for 200-400 μm.
Typically, the shape of described diamond complex includes (but being not limited to): graininess.
Typically, based on the cumulative volume of described composite, the percent by volume of described diamond complex is 15 -85%.
Specifically, based on the cumulative volume of described composite, the percent by volume of described diamond complex is 40%-85%, preferably 45%-85%, be more preferably 50%-80%.
In the present invention, described overlay coating thickness is 1-5000nm.
Typically, described overlay coating thickness is 10-3000nm, preferably 100-2000nm, is more preferably 100-1000nm, is most preferably 100-200nm.
Should be understood that in the present invention, described overlay coating is evenly coated at described diamond particle surfaces.
In another preference, in described overlay coating, the thickness ratio of described boron carbide layer and described boron layer is 1: 200, preferably 1:100, be more preferably 1:1.
In another preference, the thickness of described boron carbide layer is 1-500nm, preferably 1-50nm, more Goodly for 1-40nm.
In another preference, the thickness of described boron layer is 1-2000nm, preferably 1-500nm, more preferably Ground is 1-80nm.
Should be understood that in the present invention, the thickness of described boron layer and roughness can be by regulation state modulator.
In another preference, described composite has one or more features selected from lower group:
1) when metallic matrix is aluminum, the thermal conductivity of gained composite >=480W/m k;
2) when metallic matrix is aluminum, the thermal coefficient of expansion≤8.3ppm/K of gained composite;
3) when metallic matrix is copper, the thermal conductivity of gained composite >=528W/m K;
4) when metallic matrix is copper, the thermal coefficient of expansion≤8.8ppm/k of gained composite;
In another preference, without hydrolysis phase in described composite.
Preparation method
The invention provides the preparation method of a kind of described composite, described method comprises the steps:
A-1) provide a kind of by diamond particles, boron raw material and the homogeneous mixture A of organic solution composition;
A-2) under vacuo, mixture A described in heat treatment, obtain diamond complex;
B-1) a kind of step a-2 is provided) diamond complex of gained and the mixture B of raw metal;
B-2) mixture B described in hot pressed sintering, obtains the composite described in claim 1.
Specifically, based on the gross weight of described mixture A, the content of diamond particles is 80-99wt%;With / or
The content of boron raw material is 1-15wt%.
Typically, based on the gross weight of described mixture A, the content of diamond particles is 85-99wt%, relatively Goodly for 85-95wt%.
Typically, based on the gross weight of described mixture A, the content of boron raw material is 1-12wt%, preferably 1-10wt%.
In the present invention, described heat treatment time, vacuum, the rate of heat addition are not particularly limited.
In another preference, described heat treatment temperature is 1000-1400 DEG C, preferably 1000-1350 DEG C, more Goodly for 1000-1300 DEG C.
In another preference, the heat treatment time in described heat treatment temperature is 30-300min, preferably 30-100min, is more preferably 30-60min.
In another preference, described vacuum≤10-1Pa;Preferably 10-2Pa。
In another preference, described heat treatment is carried out in vacuum carbon tube furnace.
In another preference, described vacuum carbon tube furnace is heated to heat treatment temperature with rate of heat addition 1-40 DEG C/min, Preferably 5-10 DEG C/min, is more preferably 8-10 DEG C/min.
In another preference, the sintering temperature of described mixture B is 600-2000 DEG C, preferably 700-1500 DEG C, more preferably it is 700-1200 DEG C.
In another preference, the sintering time of described mixture B is not particularly limited, preferably 30-300min, Preferably 60-150min, is more preferably 60-120min.
In another preference, the pressure of described mixture B hot pressed sintering is not particularly limited, and is preferably 30-150MPa, preferably 40-80MPa.
In another preference, described mould is warmed up to sintering temperature with the rate of heat addition of 5-50 DEG C/min, preferably The rate of heat addition be 5-30 DEG C/min, the more preferably rate of heat addition be 5-25 DEG C/min.
Application
Present invention also offers a kind of goods, described goods comprise described composite or by described composite wood Material is constituted.
Present invention also offers the purposes of a kind of described composite, for processing machinery goods, composite, Electronic devices and components.
Typically, described machinework includes (but being not limited to): cutter, grinding tool, file, emery wheel, Saw blade, drill bit.
Typically, described electronic devices and components include (but being not limited to): encapsulation base material, fin.
Compared with prior art, the present invention has a following major advantage:
(1) interfacial shear strength prepared by the present invention is excellent, and good stability, heat conductivility is good.
(2) Thermal expansion coefficient of composites prepared by the present invention is low and controlled;
(3) preparation method of the present invention is simple, and operation is simple, and equipment requirements is simple, low cost, suitable Close industrial production operation;
(4) large-sized composite material can be prepared.
Below in conjunction with specific embodiment, the present invention is expanded on further.Should be understood that these embodiments are merely to illustrate The present invention rather than restriction the scope of the present invention.The experimental technique of unreceipted actual conditions in the following example is logical Often according to normal condition or according to the condition proposed by manufacturer.Unless otherwise indicated, otherwise percentage ratio and number Calculate by weight.Unless stated otherwise, test according to a conventional method the density of composite of the present invention, thermal conductivity, The performances such as thermal coefficient of expansion.
Unless otherwise defined, all specialties used in literary composition are familiar with one skilled in the art with scientific words Same meaning.Additionally, any method similar or impartial to described content and material all can be applicable to the present invention In method.Preferable implementation described in literary composition only presents a demonstration with material and is used.
Embodiment 1
1.1 prepare diamond complex 1
Mean diameter is about the diamond particles of 200 μm respectively, and a small amount of boron powder and concentration are the polyethylene of 5% Alcohol-water solution mix homogeneously, forms mixture.Wherein, calculate by the gross weight of mixture, the quality of B powder Mark is 10%, and the mass fraction of diamond particles is 85%.Mixture is put in vacuum carbon tube furnace, take out Vacuum to vacuum is 10-2Pa, is that 10 DEG C/min is warming up to 1300 DEG C with heating rate, is incubated 60min, so After cool to room temperature with the furnace.The mixture high-temperature process crossed takes out, cross respectively 30 mesh, 60 mesh, 80 mesh, 100 mesh, 150 mesh sieves, remove superfluous boron powder, it is thus achieved that superficial growth has the diamond complex of boride layer 1。
Result
Diamond complex 1 is carried out surface morphology and composition test.
Fig. 1 is SEM figure and the EDS energy spectrogram of diamond complex 1, from figure 1 it appears that carbide Layer is evenly coated at diamond particle surfaces.
1.2 prepare diamond-aluminium composite material 1
To mix homogeneously, after mixing through the diamond complex 1 of aforementioned step process is common with high-purity aluminium powder Powder gross weight calculate, aluminium powder mass fraction is 30%.By mixed powder in high-accuracy mould, Being heated to 700 DEG C with 10 DEG C/min of heating rate to be sintered, temperature retention time is 60min, and pressure is 50MPa; Then cooling to room temperature with the furnace, obtain diamond-aluminium composite material 1, its density is 3.2g/cm3, thermal conductivity is 560W/m K, thermal coefficient of expansion is 8.22ppm/K.
Result
Gained composite 1 is carried out surface morphology and composition test.
Fig. 2 a) it is the SEM picture of composite 1, from Fig. 2 a) it can be seen that diamond complex 1 and gold Belonging to and combine densification between aluminum, this shows that diamond complex 1 and metallic aluminium have high consistency and combine strong Degree.
Fig. 3 a) be the XRD figure sheet of composite 1, from Fig. 3 a) it can be seen that in composite 1 There is not Al4C3Hydrolysis phase, this shows that composite 1 will not hydrolyze in humid air, can stablize Exist.
Embodiment 2
2.1 prepare diamond complex 2
Mean diameter is about the diamond particles of 300 μm respectively, and a small amount of boron powder and concentration are the poly-second two of 5% Alcohol-water solution mix homogeneously, forms mixture.Wherein, calculate by the gross weight of mixture, the quality of B powder Mark is 10%, and the mass fraction of diamond is 80%.Above-mentioned mixture is put in vacuum carbon tube furnace, takes out Vacuum to vacuum is 10-2Pa, is that 10 DEG C/min is warming up to 1250 DEG C with heating rate, is incubated 60min, so After cool to room temperature with the furnace.The mixture high-temperature process crossed takes out, cross respectively 30 mesh, 60 mesh, 80 mesh, 100 mesh, 150 mesh sieves, remove superfluous boron powder, it is thus achieved that superficial growth has the diamond complex of boride layer 2。
2.2 prepare diamond-aluminium composite material 2
The diamond complex 2 step process before this obtained is put in die casting, with the speed of 25 DEG C/min After high-frequency heating makes mould be preheating to 700 degree, the aluminum water after then adding heat fusing pours rapidly die casting into In carry out hot pressing, pressure is 50MPa, then cools to room temperature with the furnace, obtains diamond-aluminium composite material 2. Calculating by the gross weight of material after mixing, the mass fraction of aluminum is 40%.The density of gained composite 2 is 3.01g/cm3, thermal conductivity is 480W/m K, and thermal coefficient of expansion is 8.04ppm/K.
Embodiment 3
3.1 prepare diamond complex 3
Mean diameter is about the diamond particles of 300 μm respectively, and a small amount of boron powder and concentration are the polyethylene of 5% Alcohol-water solution mix homogeneously, forms mixture.Wherein, calculate by the gross weight of mixture, the quality of B powder Mark is 8%, and the mass fraction of diamond particles is 80%.Above-mentioned mixture is put in vacuum carbon tube furnace, Being evacuated to vacuum is 10-2Pa, is that 8 DEG C/min is warming up to 1300 DEG C with heating rate, is incubated 60min, so After cool to room temperature with the furnace.The mixture high-temperature process crossed takes out, cross respectively 30 mesh, 60 mesh, 80 mesh, 100 mesh, 150 mesh sieves, remove superfluous boron powder, it is thus achieved that superficial growth has the diamond complex of boride layer 3。
3.2 prepare diamond-copper composite material 3
To mix homogeneously, after mixing through the diamond complex 3 of aforementioned step process is common with high-purity copper powder Powder gross weight calculate, copper powder mass fraction is 50%.By mixed powder at vacuum hotpressing stove mould Being heated to 1100 DEG C with 8 DEG C/min of heating rate in tool to be sintered, sintering pressure is 45MPa, prepares Buddha's warrior attendant Stone-carbon/carbon-copper composite material 3, its density is 6.22g/cm3, thermal conductivity is 528W/m K, and thermal coefficient of expansion is 8.794 ppm/K。
Result
Fig. 2 b) it is the SEM picture of diamond-copper composite material, in figure, diamond is well combined with copper;Fig. 3 b) For the XRD figure sheet of composite 3, from Fig. 3 b) it can be seen that there are not other in composite 3 and close Metallographic material.
Embodiment 4
4.1 prepare diamond complex 4
Mean diameter is about the diamond particles of 300 μm respectively, and a small amount of boron powder and concentration are the poly-second two of 5% Alcohol-water solution mix homogeneously, forms mixture.Wherein, calculate by the gross weight of mixture, the quality of B powder Mark is 8%, and the mass fraction of diamond is 80%.Above-mentioned mixture is put in vacuum carbon tube furnace, takes out true Sky to vacuum is 10-2Pa, is that 8 DEG C/min is warming up to 1250 DEG C with heating rate, be incubated 60min, then with Stove is cooled to room temperature.Mixture high-temperature process crossed takes out, and crosses 30 mesh, 60 mesh, 80 mesh sieves respectively, goes Except superfluous boron powder, it is thus achieved that superficial growth has the diamond complex 4 of boride layer.
4.2 prepare diamond-copper composite material 4
By diamond complex 4 uniform spreading through aforementioned step process on copper sheet, the most uniformly completing Diamond complex 4 surface place copper sheet one layer.Gains are put into discharge plasma sintering furnace mould In, it being heated to 1000 DEG C with 10 DEG C/min of heating rate and be sintered, temperature retention time is 60min, sintering pressure For 50MPa, then cooling to room temperature with the furnace, obtain diamond-copper composite material 4, its density is 6.258g/cm3, thermal conductivity is 590W/m K, and thermal coefficient of expansion is 8.11ppm/K.
Comparative example 1
Diamond-aluminium composite material C1
Undressed diamond powder body is being sintered under 1.2 identical sintering conditions in embodiment 1 with aluminium powder Process obtains composite C1.
Fig. 4 a) and the SEM figure of b) the composite C1 of to be original diamond powder body with metallic aluminium powder be combined gained Sheet, from Fig. 4 a) and b) can be seen that aluminium powder is optionally attached on diamond surface, cause aluminium powder and Buddha's warrior attendant The bond strength of stone granule is less.Additionally, prepare composite material at high temperature, composite material interface combines Place has facile hydrolysis brittlement phase Al4C3Generation, cause composite C1 in humid air median surface stability Difference.
Comparative example 2
Diamond-copper composite material C2
Undressed diamond powder body is being sintered under 3.2 identical sintering conditions in embodiment 3 with copper powder Process obtains composite C2.
Fig. 4 c) it is original diamond powder body and the copper powder composite C2 that is combined gained, from Fig. 4 c) In can be seen that combine between copper powder and diamond particles poor.This is due to diamond particles and metallic copper circle Almost without wellability between face, causing gained composite C2 binding ability poor, thermal conductivity is relatively low (248W/m·K)。
Compared to comparative example 1 and 2, the diamond after the method for the invention processes sinters institute with metallic matrix The stability of composite, bond strength, thermal conductivity and thermal coefficient of expansion be all significantly improved and Promoting, wherein thermal conductivity rises a height of 528W/m K from 248W/m K, and enhancing rate is up to 113%.
The all documents mentioned in the present invention are incorporated as reference the most in this application, just as each document It is individually recited as with reference to like that.In addition, it is to be understood that after the above-mentioned teachings having read the present invention, The present invention can be made various changes or modifications by those skilled in the art, and these equivalent form of values fall within this Shen equally Please appended claims limited range.

Claims (10)

1. diamond-metallic composite, it is characterised in that described composite comprises metallic matrix and the diamond complex compound with described metallic matrix, wherein,
Described diamond complex comprises diamond particles and is compound in the overlay coating of described diamond particle surfaces;
Described overlay coating comprises the boron carbide layer being compound in described diamond particle surfaces and the boron layer being compound in described boron carbide layer surface.
2. composite as claimed in claim 1, it is characterised in that described metallic matrix is selected from lower group: copper, aluminum, silver or its alloy or a combination thereof.
3. composite as claimed in claim 1, it is characterised in that the particle diameter of described diamond complex is 80-520 μm.
4. composite as claimed in claim 1, it is characterised in that based on the cumulative volume of described composite, the percent by volume of described diamond complex is 15-85%.
5. composite as claimed in claim 1, it is characterised in that described overlay coating thickness is 1-5000nm.
6. composite as claimed in claim 1, it is characterised in that described composite has one or more features selected from lower group:
1) when metallic matrix is aluminum, the thermal conductivity of gained composite >=480W/m k;
2) when metallic matrix is aluminum, the thermal coefficient of expansion≤8.3ppm/K of gained composite;
3) when metallic matrix is copper, the thermal conductivity of gained composite >=528W/m K;
4) when metallic matrix is copper, the thermal coefficient of expansion≤8.8ppm/k of gained composite.
7. the preparation method of the composite described in a claim 1, it is characterised in that described method comprises the steps:
A-1) provide a kind of by diamond particles, boron raw material and the homogeneous mixture A of organic solution composition;
A-2) under vacuo, mixture A described in heat treatment, obtain diamond complex;
B-1) a kind of step a-2 is provided) diamond complex of gained and the mixture B of raw metal;
B-2) mixture B described in hot pressed sintering, obtains the composite described in claim 1.
8. preparation method as claimed in claim 7, it is characterised in that based on the gross weight of described mixture A, the content of diamond particles is 80-99wt%;And/or
The content of boron raw material is 1-15wt%.
9. goods, it is characterised in that described goods comprise the composite described in claim 1 or are made up of the composite described in claim 1.
10. the purposes of the composite described in a claim 1, it is characterised in that for processing machinery goods, composite, electronic devices and components.
CN201510075147.1A 2015-02-12 2015-02-12 A kind of high heat-conductive diamond metallic composite and preparation method thereof Active CN105986158B (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN201510075147.1A CN105986158B (en) 2015-02-12 2015-02-12 A kind of high heat-conductive diamond metallic composite and preparation method thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN201510075147.1A CN105986158B (en) 2015-02-12 2015-02-12 A kind of high heat-conductive diamond metallic composite and preparation method thereof

Publications (2)

Publication Number Publication Date
CN105986158A true CN105986158A (en) 2016-10-05
CN105986158B CN105986158B (en) 2018-03-06

Family

ID=57041142

Family Applications (1)

Application Number Title Priority Date Filing Date
CN201510075147.1A Active CN105986158B (en) 2015-02-12 2015-02-12 A kind of high heat-conductive diamond metallic composite and preparation method thereof

Country Status (1)

Country Link
CN (1) CN105986158B (en)

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107419133A (en) * 2017-05-12 2017-12-01 南通鑫祥锌业有限公司 High-volume fractional diamond zinc composite
CN107649688A (en) * 2017-08-21 2018-02-02 武汉速博酷新材料科技有限公司 A kind of diamond heat-conducting composite of easy processing and its preparation method and application
CN107937783A (en) * 2017-11-17 2018-04-20 湖南大学 Increase the method for binding ability between diamond and metallic matrix
CN108179004A (en) * 2016-12-08 2018-06-19 中国科学院宁波材料技术与工程研究所 A kind of PcBN composite and its preparation and application
CN109371303A (en) * 2018-11-07 2019-02-22 中国科学院宁波材料技术与工程研究所 Heat-conductive composite material and preparation method thereof, radiating piece
CN113210602A (en) * 2021-05-18 2021-08-06 许昌学院 Preparation method of copper-aluminum alloy coated diamond complex
CN115323211A (en) * 2022-08-15 2022-11-11 广东奔朗新材料股份有限公司 Diamond-copper composite material and preparation method thereof

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1201770A (en) * 1970-03-24 1970-08-12 Zd Y Jana Svermy Narodni Podni Improvements in or relating to sintered carbides
JPS6191344A (en) * 1984-10-11 1986-05-09 Toshiba Tungaloy Co Ltd High hardness sintered body
CN101545057A (en) * 2009-05-15 2009-09-30 北京科技大学 Method for preparing diamond/Cu composite material with high heat conductivity
CN101831584A (en) * 2009-03-10 2010-09-15 北京有色金属研究总院 High heat-conducting copper-based composite material and preparation method thereof
CN102383014A (en) * 2011-11-11 2012-03-21 华中科技大学 Method for preparing diamond-copper composite material by virtue of metallization of high-temperature blending surface

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1201770A (en) * 1970-03-24 1970-08-12 Zd Y Jana Svermy Narodni Podni Improvements in or relating to sintered carbides
JPS6191344A (en) * 1984-10-11 1986-05-09 Toshiba Tungaloy Co Ltd High hardness sintered body
CN101831584A (en) * 2009-03-10 2010-09-15 北京有色金属研究总院 High heat-conducting copper-based composite material and preparation method thereof
CN101545057A (en) * 2009-05-15 2009-09-30 北京科技大学 Method for preparing diamond/Cu composite material with high heat conductivity
CN102383014A (en) * 2011-11-11 2012-03-21 华中科技大学 Method for preparing diamond-copper composite material by virtue of metallization of high-temperature blending surface

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
HAIBO HU等: ""Improved Thermal Performance of Diamond-copper Composite with Boron Carbide Coating"", 《JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE》 *

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108179004A (en) * 2016-12-08 2018-06-19 中国科学院宁波材料技术与工程研究所 A kind of PcBN composite and its preparation and application
CN108179004B (en) * 2016-12-08 2020-07-17 中国科学院宁波材料技术与工程研究所 Cubic boron nitride complex and preparation and application thereof
CN107419133A (en) * 2017-05-12 2017-12-01 南通鑫祥锌业有限公司 High-volume fractional diamond zinc composite
CN107649688A (en) * 2017-08-21 2018-02-02 武汉速博酷新材料科技有限公司 A kind of diamond heat-conducting composite of easy processing and its preparation method and application
CN107937783A (en) * 2017-11-17 2018-04-20 湖南大学 Increase the method for binding ability between diamond and metallic matrix
CN109371303A (en) * 2018-11-07 2019-02-22 中国科学院宁波材料技术与工程研究所 Heat-conductive composite material and preparation method thereof, radiating piece
CN113210602A (en) * 2021-05-18 2021-08-06 许昌学院 Preparation method of copper-aluminum alloy coated diamond complex
CN113210602B (en) * 2021-05-18 2022-11-29 许昌学院 Preparation method of copper-aluminum alloy coated diamond composite
CN115323211A (en) * 2022-08-15 2022-11-11 广东奔朗新材料股份有限公司 Diamond-copper composite material and preparation method thereof

Also Published As

Publication number Publication date
CN105986158B (en) 2018-03-06

Similar Documents

Publication Publication Date Title
CN105986158B (en) A kind of high heat-conductive diamond metallic composite and preparation method thereof
CN102383014B (en) Method for preparing diamond-copper composite material by virtue of metallization of high-temperature blending surface
CN107649688B (en) A kind of the diamond heat-conducting composite material and preparation method and application of easy processing
ZA200303525B (en) A heat conductive material.
CN101151384A (en) High-heat-conduction composite with graphite grain dispersed and process for producing the same
CN112981164B (en) Preparation method of diamond reinforced metal matrix composite material with high reliability and high thermal conductivity
CN108746637A (en) Aluminium silicon/aluminium silicon carbide gradient composites and preparation method thereof
CN103966533B (en) A kind of diamond heat-conducting composite and preparation method thereof
CN102071332A (en) Method for preparing diamond enhanced copper based composite with high volume fraction
CN112935249B (en) Efficient preparation method of diamond/metal-based composite material
CN108925108A (en) The conductive structure and its manufacturing method of aluminium alloy are inlayed in a kind of graphene-based composite substrate
CN114309596A (en) Preparation method of high-thermal-conductivity surface metallized diamond/copper composite substrate
CN104707996B (en) A kind of diamond complex and Ways of Metallizing Cladding onto Diamond Surface
CN104707995B (en) A kind of diamond complex and preparation method thereof
CN109371303B (en) Heat-conducting composite material, preparation method thereof and heat dissipation piece
CN105385902B (en) A kind of AlN and AlB2Particle enhanced aluminum-based composite material and preparation method thereof
Wu et al. Fabrication and characterization of highly thermal conductive Si3N4/diamond composite materials
CN109321882B (en) Coating and method for improving interface bonding of diamond/magnesium composite electronic packaging material
Xie et al. Fabrication and evaluation of high-performance 3D interpenetrated network structures SiC/Al composites with high-purity plate-like α-SiC framework
CN116987924B (en) Preparation method of SiC/Al composite material
CN105803427A (en) Method for preparing diamond with thinned surface plating layer
CN113122188A (en) Heat-conducting composite material, preparation method and application thereof
Xie et al. Fabrication of high-performance 3D-interpenetrated network structures SiC/Al composites with SiC equiaxed grain frameworks
CN112091219B (en) Graphite-titanium composite material and preparation method and application thereof
CN108588461B (en) Polyimide-based graphite-metal composite material and preparation method thereof

Legal Events

Date Code Title Description
C06 Publication
PB01 Publication
C10 Entry into substantive examination
SE01 Entry into force of request for substantive examination
GR01 Patent grant
GR01 Patent grant