CN107791616B - A kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film - Google Patents
A kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film Download PDFInfo
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- CN107791616B CN107791616B CN201711019866.7A CN201711019866A CN107791616B CN 107791616 B CN107791616 B CN 107791616B CN 201711019866 A CN201711019866 A CN 201711019866A CN 107791616 B CN107791616 B CN 107791616B
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- copper
- graphite film
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- graphite
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
- B32B9/005—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile
- B32B9/007—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile comprising carbon, e.g. graphite, composite carbon
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
- B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B9/041—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/30—Properties of the layers or laminate having particular thermal properties
- B32B2307/302—Conductive
Abstract
The present invention provides a kind of preparation methods of multiple-layer laminated block composite material of copper/graphite film, can be applied to the Electronic Packaging field of IC industry.Composite material raw material selects the netted graphite film of the anisotropic high thermal conductivity of performance and tough cathode powder.It is in the homogeneous mixture solotion of plasticizer that copper powder, which is added to by the binder and repefral of polyvinyl butyral and ethanol solution preparation, and the uniform sizing material being sufficiently stirred as good fluidity, by slurry on netted graphite film uniform drawout, through drying, it cuts, it after degumming, is layering, fine and close graphite film and metallic copper is prepared using Bidirectional-pressure sintering and are layered alternately arranged multiple-layer laminated block composite material.Such composite material can be 1.5-2 times high compared to fine copper along the thermal conductivity of graphite film in-plane, and density can be reduced to the 65-80% of fine copper, can be used for substituting traditional copper tungsten metal thermal conductive material.
Description
Technical field
The present invention relates to a kind of preparation methods of multiple-layer laminated block composite material of copper/graphite film, provide and are led with height
The netted graphite film material of heat is raw material, should in conjunction with the layer structure composite material that specially-shaped and sintering process are prepared
Material can be used for miniature electronic part heat dissipation, belong to integrated circuit, electronic package material field.
Technical background
Being constantly progressive for modern society promotes electronic equipment to rapidly develop, while requiring excellent performance, electronics
Equipment is intended to miniaturization, lightweight development, this inevitably results in calorific value under its unit volume and increases, if cannot dissipate in time
Heat may influence equipment normal operation, or even damage equipment.Traditional heat dissipation has been difficult to meet heat dissipation of today and has wanted
It asks.In the thermal conductivity of Electronic Packaging neighborhood optimization material, this problem can be effectively solved.
The fundamental type of electronic package material has Plastic Package, ceramic package, Metal Packaging and metal-base composites envelope
Dress.Among these, metal-base composites has its unique advantages, and can combine metal material and the advantage of reinforced phase respectively,
With the physical properties such as excellent mechanical property and good thermally conductive, conductive, wear-resisting, low thermal coefficient of expansion.Common Metal Substrate
Body has aluminium and aluminium alloy, copper and copper alloy etc., and reinforcement can be metal, is also possible to inorganic material.
With the development of technology, it can manually synthesize with a thickness of micron-sized graphite film, thermal conductivity is reachable in face
1500W/mK is even higher, and has anisotropy, is good electronic package material.But graphite film intensity itself is low,
Especially interfacial bonding strength is very low, while it can not be connected with each other between metal, difficult between the bulk material interface of formation
It is urgent problem with firm connection.
To finding after the document of last decade, patent retrieval, application No. is a kind of 201410114471.5 patent " high thermal conductivities
Graphite film-carbon/carbon-copper composite material preparation method " first electroless copper, one layer of copper of re-plating on graphite film obtain single layer copper facing stone
The film material of ink film improves material axial thermal conductivity, but the interface cohesion problem of unresolved graphite film and copper, and fails
The block composite material that obtained shape can be processed arbitrarily.Application No. is a kind of 201511019061.3 patent " high thermal conductivity graphite
The preparation method of film surface metal coating " is coated with one layer of copper coating to graphite film surface using PVD equipment, carries out to graphite film
Processing, improves its performance, but coating is only mechanically attached on graphite film, and mutual binding force is weak, and finally obtains still
It is so film material, not formed block composite material.Application No. is a kind of 201510052133.8 patent " high thermal conductivity graphite films
Metal block composite material and preparation method thereof " using graphite film and aluminium foil be superimposed and it is hot-forming, it is compound to have obtained block
Material, although solving the problems, such as to combine between graphite film and metallic matrix interface by the diffusion of aluminium and graphite film, stone
The low problem of ink film itself interlaminar strength does not obtain effective solution, thus leads to the intensity of its block composite material obtained
Not high, the composite material prepared belongs to loose material, and performance is unable to reach best applications state.
Summary of the invention
To improve above-mentioned material performance deficiency, the present invention provides a kind of multiple-layer laminated block composite material of copper/graphite film
Preparation method, selecting tough cathode powder and netted graphite film is raw material, and copper powder slurry is spread to graphite using the tape casting
On film, the good mobility of slurry is sufficient filling with copper powder at the mesh of netted graphite film, thus can be between layers of copper
Be connected with each other, form rivet arrangement, it is low to solve graphite film interlaminar strength, and copper with graphite film interface is uncombined asks
Topic, effectively improves the intensity of composite material.
The present invention is achieved by the following technical programs:
A kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film, it is characterised in that: with fine copper powder and
Artificial synthesized netted graphite film is raw material, is uniformly layered on copper powder on graphite film using casting molding processes, then carry out
It is dry, it cuts, degumming, heap poststack makes composite molding using Bidirectional-pressure sintering process, obtains fine and close high thermal conductivity block
Shape composite material.
Further, tough cathode powder and artificial synthesized graphite film that the raw material are 5-10 μm of partial size, in netted
Structure, with a thickness of 25 μm, the size of mesh and interval can designed, designeds.
Further, casting molding processes sprawl the step of copper powder are as follows: the polyvinyl butyral of configuration quality score 5%
Alcohol mixeding liquid with mass fraction 95% pours into copper powder and stirs evenly to form slurry as binder, copper powder and binder
Mass ratio is 1:1, and instills repefral as plasticizer, and the 1-1.3% of the total slurry of mass fraction Zhan will be starched
Material pours into casting device, uniformly spreads out on graphite film surface, bonds, and adjusting blade height is 50-100 μm, casting belt
Operating rate is 0.4-0.8m/min.
Further, drying steps are as follows: molded casting films are placed in vacuum oven, drying temperature is set as 30
DEG C, vacuum degree≤10-1Pa, drying time 1h.
Further, graphite film is cut into appropriate size, carries out degumming, this process carries out in hydrogen furnace, heats up
To 400-500 DEG C, 2h is kept the temperature, is taken out after cooling, and carry out layered arrangement and be loaded in graphite jig.
Further, pressure sintering is carried out, sintering process carries out in pure nitrogen gas atmosphere, and heating rate is 5 DEG C/min, until
950-1050 DEG C, Bidirectional-pressure pressure is 5-10MPa, heat-insulation pressure keeping 60-90min, and it is more that fine and close copper/graphite film is prepared
Block composite material is closed layer by layer.
Advantages of the present invention
1. the graphite film that the present invention adds has heating conduction in the face of superelevation, its reticular structure makes copper
It can be connected with each other between layer, solve the problems, such as that bulk material interlayer bond strength is too low, prepare with some strength
High thermal conductivity block composite material.
2. the present invention is uniformly spread in copper powder on netted graphite film using the tape casting, it is ensured that copper powder is filled in graphite
At film mesh, rivet arrangement is formed；The volume of graphite and copper in composite material can be controlled by control copper layer thickness simultaneously
Than.
3. the present invention is applied widely, copper is can be selected in metal material, and other thermally conductive good metals and alloy also can be selected.
Specific embodiment
The present invention is described in detail combined with specific embodiments below.Following embodiment is for illustrating original of the invention
Reason feature and has the advantage that, facilitates it is further understood that the present invention, but do not appoint to the present invention
What is limited.It will be apparent to those skilled in the art that being made centainly in the case where not departing from design of the invention to the implementation condition of use
Change and adjustment, belong to protection scope of the present invention.
Embodiment 1
Polyvinyl butyral and alcohol mixeding liquid are configured as binder, copper powder is poured into and stirs evenly to form slurry, and
Repefral is instilled as plasticizer；Casting machine is poured into after slurry agitation is uniform, adjusting blade height is 40 μm,
Uniform drawout on netted graphite film, the width of mesh of graphite film are 1mm, are spaced 2mm；Molded casting films are placed in
It is dry in vacuum oven, then pass through degumming, cut, stacks, be put into graphite jig and carry out pressure sintering, sintering temperature is
1000 DEG C, pressure 5MPa, fine and close block composite material is prepared；Graphite film volume fraction is in composite material
50vol%, measuring composite density using drainage is 5.52g/cm3, composite material thermal conductivity is measured using the laser method of shining
Rate is 590W/mK.
Embodiment 2
Polyvinyl butyral and alcohol mixeding liquid are configured as binder, copper powder is poured into and stirs evenly to form slurry, and
Repefral is instilled as plasticizer；Casting machine is poured into after slurry agitation is uniform, adjusting blade height is 80 μm,
Uniform drawout on netted graphite film, the width of mesh of graphite film are 1mm, are spaced 2mm；Molded casting films are placed in
It is dry in vacuum oven, then pass through degumming, cut, stacks, be put into graphite jig and carry out pressure sintering, sintering temperature is
1000 DEG C, pressure 5MPa；Graphite film volume fraction is 35vol% in composite material, measures composite material using drainage
Density is 6.53g/cm3, measuring heat conductivity using the laser method of shining is 497W/mK.
Claims (2)
1. a kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film, it is characterised in that: using tape casting
Tough cathode slurry material is spread on artificial synthesized netted graphite film by method, is sufficient filling with copper powder in netted graphite film
Mesh at, connection function is provided, then through drying, is cut, degumming, and be layering, the method for utilizing Bidirectional-pressure sintering
Prepare fine and close graphite film and the multiple-layer laminated block composite material of copper；
Wherein: polyvinyl butyral and alcohol mixed solution 1:19 in mass ratio are weighed in the configuration of copper powder slurry, and mixing is equal
It is even, as binder；Then it is added copper powder, the mass ratio of copper powder and binder is 1:1, is stirred as uniform sizing material；Finally, being added
Shape is sufficiently stirred as plasticizer, the 1-1.3% of the total slurry of plasticizer mass fraction Zhan in repefral solution again
At uniform slurry；
Copper slurry is spread on graphite film by the tape casting, key step are as follows: uniform copper slurry is poured into casting device,
Blade is adjusted to proper height, makes casting belt operating rate 0.4-0.8m/min, guarantees that slurry is uniformly spread on graphite film
Expansion；Thickness by controlling metal copper layer can control the volume ratio of graphite and copper in composite material；
Copper slurry is sprawled after graphite film using the tape casting, places it in 1h in vacuum oven, setting temperature is 30 DEG C, very
Reciprocal of duty cycle≤10-1Pa；It is cut into further according to actual conditions suitably sized；Then degumming is carried out, is warming up in a hydrogen atmosphere
400-500 DEG C, the oxidation of copper is prevented, keeps the temperature 2h；
Material after degumming is placed in progress Bidirectional-pressure sintering in graphite jig, sintering temperature is 950-1050 DEG C, pressurization pressure
Power is 5-10MPa, heat-insulation pressure keeping 60-90min；
In the composite, layers of copper and graphite linings layering folded array are in layered composite structure, and thermal conductivity is in anisotropy, edge
The thermal conductivity of graphite film in-plane is reduced to 5.62g/cm up to 590W/mK, the density of composite material3。
2. the preparation method of the multiple-layer laminated block composite material of copper/graphite film as described in the appended claim 1, it is characterised in that:
The tough cathode powder of selection, 5-10 μm of partial size, 25 μm artificial synthesized of high thermal conductivity graphite film thickness is in reticular structure, mesh
Size and mesh between interval can voluntarily adjust as desired.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201711019866.7A CN107791616B (en) | 2017-10-26 | 2017-10-26 | A kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film |
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| CN201711019866.7A CN107791616B (en) | 2017-10-26 | 2017-10-26 | A kind of preparation method of the multiple-layer laminated block composite material of copper/graphite film |
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| CN107791616A CN107791616A (en) | 2018-03-13 |
| CN107791616B true CN107791616B (en) | 2019-09-10 |
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Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN110449590B (en) * | 2018-05-08 | 2021-03-09 | 长飞光纤光缆股份有限公司 | Preparation method and product of graphene-copper-based composite material |
| CN109175356B (en) * | 2018-10-16 | 2020-10-09 | 中国科学院兰州化学物理研究所 | Graphite-copper layered composite material and preparation method thereof |
| CN110340368B (en) * | 2019-08-02 | 2021-05-04 | 中国科学院山西煤炭化学研究所 | Preparation method of high-performance graphite film copper-based composite material |
| CN111114041A (en) * | 2020-01-07 | 2020-05-08 | 中国电子科技集团公司第十六研究所 | Composite material with high-thermal-conductivity graphite-copper interpenetrating structure and preparation method thereof |
| CN112108654A (en) * | 2020-09-23 | 2020-12-22 | 长飞光纤光缆股份有限公司 | Preparation method of high-thermal-conductivity composite material and graphite-aluminum metal composite material |
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| CN104647830A (en) * | 2015-01-30 | 2015-05-27 | 上海交通大学 | High-heat-conductivity graphite film metal block composite material and preparation method of composite material |
| CN107116210A (en) * | 2016-10-27 | 2017-09-01 | 北京科技大学 | Cu-base composites fin of the oriented laminated arrangement of graphite flake and preparation method thereof |
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| TWI375347B (en) * | 2009-11-20 | 2012-10-21 | Ind Tech Res Inst | Manufacture method of bi-polar plates of fuel cell and bi-polar plates thereof |
| US20150166346A1 (en) * | 2013-12-18 | 2015-06-18 | Chung-Shan Institute Of Science And Technology, Armaments Bureau, M.N.D | Method of fabricating graphite films |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104647830A (en) * | 2015-01-30 | 2015-05-27 | 上海交通大学 | High-heat-conductivity graphite film metal block composite material and preparation method of composite material |
| CN107116210A (en) * | 2016-10-27 | 2017-09-01 | 北京科技大学 | Cu-base composites fin of the oriented laminated arrangement of graphite flake and preparation method thereof |
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