CN103911006B - Heat transfer composite and manufacture method - Google Patents
Heat transfer composite and manufacture method Download PDFInfo
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- CN103911006B CN103911006B CN201310001028.2A CN201310001028A CN103911006B CN 103911006 B CN103911006 B CN 103911006B CN 201310001028 A CN201310001028 A CN 201310001028A CN 103911006 B CN103911006 B CN 103911006B
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Abstract
A kind of heat transfer composite and manufacture method, the composite include：High molecular polymer, the high polymer material comprising free redical reaction and the peroxide that the high polymer material can be polymerize with radical reaction；Heat filling, including at least the compatible Heat Conduction Material of two kinds of properties；And silane thing, including at least two kinds of different functional groups, a kind of functional group may participate in the high molecular polymer Raolical polymerizable, and another functional group can be in the heat filling Surface Creation chemical bonded refractory.The present invention has effects that reduction thermal contact resistance and material thermal resistance.
Description
Technical field
The present invention is relevant a kind of heat transfer composite and manufacture method, espespecially a kind of to have reduction thermal contact resistance and material
Expect the design of thermal resistance effect.
Background technology
The exploitation of electronic product is more and more compact, and the thing followed is that the stability of product is more beneficial important, therefore more
Seem importance in terms of heat management；Regardless of whether being which kind of kenel (such as notebook computer, desktop computer, mobile phone or other
Apparatus), hot working at high speed of the generation from electronic building brick, its heat produced (being referred to as thermal source), if not in the short time
Interior its temperature of reduction, by hot migration low temperature (hot well), then electronic building brick has the possibility of damage, causes the electronic product life-span to reduce
Or quality it is unstable the problem of.
However, by heat by thermal source migration hot well, it has three approach, respectively radiation, convection current and conduction, and to conduct most
To be effective；When removing heat, can be one of them approach, or two kinds of approach merge, and hold the heat management side of visual equipment device
Depending on formula.Situation inside electronic building brick or apparatus, it is in the majority with convection current and pathway, and the effect of pathway
Better than convection current approach, this be because the thermal impedance of solid is far below the thermal impedance of gas therefore.Furthermore, thermal source and hot well are each other
The point of contact is more, and its thermal impedance is lower, and when heat source surface more tends to be smooth with hot well surface, when the contact of this two flat surface
When, the remaining space not touched is fewer, and the effect of heat transfer is better, because there is low thermal impedance.
Therefore, when the heat source surface space produced because contacting with hot well surface is fewer, thermal convection current approach is changed into hot biography then
Approach is led, and this hot well is big well known heat sink material, Heat Conduction Material or interface Heat Conduction Material；What this approach changed
Meanwhile, the purpose is to be to reduce the thermal impedance of contact surface, therefore thermal impedance is lower, is more to be conducive to heat source surface heat
Remove；But, in addition to the thermal impedance of heat source surface and hot well surface contact interface, connecing between each raw material when hot well is manufactured
Contacting surface, is also to influence another key of thermal impedance.
In addition, the TWI325752 of tw Taiwan discloses one graphitic sheet of heat radiation sheet metal assembly and on its surface
On one layer electric insulation elastic layer, elastic layer is formed by a kind of elastic constituent, elastic constituent include a kind of particulate
The conducting filler of shape；The TWM412971 of tw Taiwan discloses a kind of heat radiator, including a heat sink body and a protection
Layer, heat sink body is a graphite substrate, and protective layer at least partly coats the graphite substrate, and the wherein material of protective layer is set for synthesis
Fat or natural resin, face in graphite substrate by setting protective layer to improve the shortcoming of heat radiator dry linting；TaiWan, China
The TW201024399 of province discloses a kind of carbon containing metallic composite and preparation method thereof, and carbon containing metallic composite includes multiple
Graphite, multiple heat conduction particles and a metal matrix.
Therefore, patent is above taken off, as is well known graphite, aluminum oxide, zinc oxide, aluminium nitride, boron nitride, aluminium powder, copper powder
Deng being all the heat filling with very good thermal conduction effect；If however, with single filler kenel exist, such as it is single
Graphite heat conducting conforming layer or graphite substrate, and multiple material is formed for a basic substance without the compound with tool chemical bonded refractory, graphite guide
Hot conforming layer, graphite substrate or metallic composite, engineering properties will not be better than the compound with chemical bonded refractory, for example, bend
Property and flexibility impose small strength outside, and its structure has the anxiety of disintegration；Moreover graphite heat conducting passes conforming layer, graphite substrate
Or carbon containing metallic composite, for the contact interface of pyrotoxin, its thermal contact resistance can be higher than the compound with chemical bonded refractory,
Reduce thermal conduction effect.
In addition, the TWM308849 of tw Taiwan discloses a kind of multilayer materials, comprising one or some heat-conducting layer and
One or some electromagnetic wave absorbing layer, and stacked and touch and constitute with interaction each other between each layer, from ratio 10%~70% it
Between one or two kinds of glue materials and 90%~30% between one or two kinds of heat transfer powders collocation be heat-conducting layer；TaiWan, China
The heat dissipation film that the TWM390642 of province is disclosed, is formed, the filler in resin material by a graphite material and a resin material
For zirconium oxide, cerium oxide, aluminum oxide, carbon nanotube, iron oxide, magnesia, zinc oxide, titanium oxide and nm oxide；China
The TW201012910 in Taiwan Province discloses a kind of heat transfer composite bed, includes gel heat-conducting layer and release layer, heat-conducting layer filling
Thing includes alumina powder, boron nitride powder, aln precipitation powder, magnesium oxide powder, Zinc oxide powder, silicon carbide powder
End, quartz powder, aluminium-hydroxide powder, carbon fiber powder, diamond powder, powdered graphite, the single one or more of aluminium powder
Combination；The TWI273118 of tw Taiwan discloses multiple material, by the native graphite of boracic, Delanium, expanded graphite, carbon black, carbon
Matter fiber, vapor phase method carbon fibre, carbon nanotubes, with phenol resin, unsaturated polyester resin, epoxy resin, vinylester resin,
Acrylate resins are made；The TW200837083 of tw Taiwan discloses the multiple material of conductibility, is expanded by a polyolefin polymer and one
Graphite composition；The TWM401536 of tw Taiwan discloses convenient again glutinous appropriate compound radiating structure, by one layer of pottery magnetic powder
Constituent and the pottery thermosetting cement of magnetic powder, a metal base and one layer are filled in from stickiness silica gel composition, pottery magnetic powder composition
Thing can be replaced by carborundum, aluminium nitride, zinc oxide, aluminum oxide or by graphite.
Then, the Heat Conduction Material of patent making is above taken off, the heat filling used is well-known skill with sizing material, but its
Heat filling is kneaded each other with glue material, whether using one or more kinds of heat filling or one or more
Glue material, it is most important that the compatibility of storeroom, therefore compatible between different heat filling or between glue material and heat filling
Property will height, made Heat Conduction Material just has low thermal impedance；Therefore, if using two or more heat fillings, then
From the high heat filling of similitude, the compatibility allowed between heat filling is lifted, and to heat filling and uses interface modification agent, is changed
Kind compatibility between heat filling and glue material, so could make preferably Heat Conduction Material.
The content of the invention
Technical problem underlying to be solved by this invention is, overcomes the drawbacks described above of prior art presence, and provides one
Heat transfer composite and manufacture method are planted, it has effects that reduction thermal contact resistance and material thermal resistance.
The technical solution adopted for the present invention to solve the technical problems is：
A kind of heat transfer composite, it is characterised in that including：High molecular polymer, the height reacted comprising free redical
Molecular material and the peroxide that the high polymer material can be polymerize with radical reaction；Heat filling, including at least two kinds of property
The compatible Heat Conduction Material of matter；And silane thing, including at least two kinds of different functional groups, a kind of functional group may participate in the macromolecule
Free polymer readical polymerisation, another functional group can be in the heat filling Surface Creation chemical bonded refractory.
In addition, the high polymer material is the dimethyl silicone polymer containing at least two vinyl functional groups；The heat conduction is filled out
Composite inorganic material of graphite composite powder of the material containing tool hole and compressibility with wrapping up graphite with nickel；The silane thing contains vinyl
With alkoxy.Also, the blending that the heat filling wraps up the composite inorganic material and graphite composite powder of graphite with nickel has compressibility, with
Reduce the space after graphite composite powder formation sheet and reduce thermal impedance；The acidity of graphite essence and the characteristic of absorption moisture content, are caused
The chemical reaction of hydrolytic condensation occurs therewith for the alkoxy of the silane thing, and in graphite surface formation chemical bond so that graphite table
Face because and the silane thing combination and there is vinyl, and then participate in the polymerization that the high polymer material occurs by peroxide
Reaction, causes graphite and high molecular polymer formation chemical bond, is reduced with reducing the space between high molecular polymer and filler
Thermal impedance.Furthermore, cementing layer further is combined at least one side of the heat transfer composite, the cementing layer can be glutinous and non-sticky
Hand does not have tackness completely, and end is suited the particular use, the cementing layer be made up of add-on type liquid macroimolecule material and with the high score
The high polymer material of sub- polymer free redical reaction is all the add-on type liquid macroimolecule material using siloxanes macromolecule as main chain
Material is formed by two kinds of high polymer materials at least containing vinyl and hydrogen-based through polyaddition reaction.In addition, the high molecular polymer
The temperature of polymerisation is 150~200 DEG C, and the time is 2~10 minutes.
The heat transfer method for composite material of the present invention, comprises the following steps：A. the high score of free redical reaction is taken
Sub- material, and the amount of taking accounts for more than the 50% of high polymer material aggregate demand；B. add free containing may participate in high polymer material
Base react with can in the silane thing of heat filling Surface Creation chemical bonded refractory, and addition account for silane thing aggregate demand 50% with
Under, and the silane thing of addition is mixed with the step a high polymer materials taken；C. add and led including at least two kinds of property compatibilities
The heat filling of hot material, and addition accounts for heat filling aggregate demand below 50%, and by the heat filling of addition and completion
Step b mixture mixing, until light is presented in mixture outward appearance or occurs without obvious filler；D. add and step b identicals
Silane thing, and addition accounts for silane thing aggregate demand below 50%, and the silane thing of addition is mixed with completing step c mixture
Close；E. add with step c identical heat fillings, and addition accounts for heat filling aggregate demand below 50%, and by addition
Heat filling is mixed with completing step d mixture, until light is presented in mixture outward appearance or occurs without obvious filler；F. repeat
Step d and step e, until the aggregate demand of silane thing and heat filling is added completely into；G. adding can be by high polymer material with certainly
Mixed by the peroxide of base reactive polymeric and the mixture of remaining high polymer material with completing step f mixture；And
H. take out the mixture for completing step g, high-pressure and vacuumize and be molded.
Another person, the step a high polymer material amount of taking accounts for high polymer material aggregate demand 85~95%, step b and step d
Silane thing addition account for silane thing aggregate demand 25~40%, step c and step e heat filling addition account for heat filling
Aggregate demand 25~40%.Also, the step a high polymer material amount of taking accounts for high polymer material aggregate demand 90%, step b and step
Rapid d silane thing addition accounts for silane thing aggregate demand 33.3%, and step c and step e heat filling addition account for heat conduction and filled out
Expect aggregate demand 33.3%.Furthermore, step c to step f is carried out in depressurizing and being warming up to 100~130 DEG C of environment, and auxiliary is mixed
Mix effect；Step g is carried out in the environment of room temperature；Step h is carried out in 150~200 DEG C of environment is warming up to.In addition, step c is extremely
Step f is carried out in depressurizing and being warming up to 110 DEG C of environment；Step h is carried out in 170 DEG C of environment is warming up to.
The beneficial effects of the invention are as follows it has effects that reduction thermal contact resistance and material thermal resistance.
Brief description of the drawings
The present invention is further described with reference to the accompanying drawings and examples.
Fig. 1 is the heat transfer composite structure schematic diagram of the present invention.
Fig. 2 is the process flow chart of the heat transfer method for composite material of the present invention.
Label declaration in figure：
10 high molecular polymers
20 heat fillings
21 graphite composite powders
22 composite inorganic materials
30 silane things
Embodiment
First, refer to shown in " Fig. 1 ", heat transfer composite of the invention, it with high molecular polymer 10 is base material to be
Mix heat filling 20 and the thing of base silane containing function 30；The high molecular polymer 10 contains the macromolecule of free redical reaction
Material and the peroxide that the high polymer material can be polymerize with radical reaction, and the temperature of polymerisation is preferably 150
~200 DEG C, the time is 2~10 minutes, and more preferably temperature is 170 DEG C, and the time is 5 minutes, and then obtains the polyphosphazene polymer of curing
Compound, the high polymer material is the dimethyl silicone polymer containing at least two vinyl functional groups；The heat filling 20 is at least
The heat conductivity thing of two kinds of properties extremely compatibility is contained, one of which is has the graphite composite powder 21 of hole and compressibility, separately
It is a kind of be using nickel be outer layer covers graphite as internal layer composite inorganic material 22；The thing of base silane containing function 30 is at least containing two kinds of differences
Functional group, one of which functional group can simultaneously participate in the high polymer material of above-mentioned free redical reaction, and to carry out radical polymerization anti-
Should, relatively appropriate functional group is vinyl, and another functional group can be relatively more appropriate in graphite packing Surface Creation chemical bonded refractory
Functional group be alkoxy.
Furthermore, refer to shown in " Fig. 2 ", heat transfer method for composite material of the invention first, takes aggregate demand
The high polymer material of 85%~95% free redical reaction, relatively appropriate consumption are 90%；Continue, add aggregate demand 25
~40% thing of base silane containing function mixing, relatively appropriate consumption are 33.3%, will using two rollers, pug mill type mixer or three rollers
It is well mixed, and relatively appropriate machine is pug mill type mixer；Continue, the heat filling for adding aggregate demand 25~40% is (mixed in advance
Close and comprise at least the compatible Heat Conduction Material of two kinds of properties) mixing, relatively appropriate consumption is 33.3%, while in pressure-reducing ring
Carried out in border, now can outside hot water or hot coal oil until mixture outward appearance presents bright, glossy or occurs without obvious filler
100~130 DEG C are heated to Deng medium, relatively appropriate temperature is 110 DEG C, auxiliary puddles effect；Continue, aggregate demand is added again
The thing of base silane containing the function mixing of amount 25~40%, relatively appropriate consumption is 33.3%, with identical mixer and identical
Temperature and identical reduced pressure atmosphere are well mixed；Continue, the heat filling mixing of aggregate demand 25~40% is added again, is compared
Appropriate consumption is 33.3%, is well mixed with identical mixer with identical temperature and identical reduced pressure atmosphere, until mixed
Compound outward appearance is presented bright, glossy or occurred without obvious filler；Continue, the remaining thing of base silane containing function mixing is added, with phase
Same mixer is well mixed with identical temperature skill identical reduced pressure atmosphere；Continue, add remaining heat filling mixing, with
Identical mixer is well mixed with identical temperature and identical reduced pressure atmosphere, until mixture outward appearance is presented bright, glossy
Or presented without obvious filler；Continue, be passed through the medium such as cold water or cold kerosene, external temperature is down to room temperature；Continue, addition can be by
Peroxide and the mixture of remaining high polymer material that high polymer material is polymerize with radical reaction, with identical mixer
It is well mixed with identical temperature and identical reduced pressure atmosphere；Continue, take out final mixture, then by means of hydraulic press is with high pressure and takes out
Vacuum forming, needs heating-up temperature to 150~200 DEG C during shaping, relatively more desired temperature is 170 DEG C；Whereby, via procedure above
Producing can closely press between the compatible heat filling of two properties in heat filling and have chemistry between filler and high polymer material
The heat transfer composite of bond.
Based on above-mentioned composition, in the heat filling that the present invention is used, using nickel be outer layer covers graphite as internal layer compound nothing
Machine material, in addition to having compatibility well with graphite composite powder, has compressibility when it is with graphite composite powder blending, can be by graphite powder
Space after bodily form slabbing is filled, and reducing free space in filler, there is provided the solution route of reduction material thermal resistance；
In addition, by the acidity and the characteristic of absorption moisture content of graphite essence, the alkoxy of the thing of base silane containing function can be hydrolyzed therewith
The chemical reaction of condensation, that is, the thing of base silane containing function can in graphite surface formation chemical bond so that graphite surface because with containing official
Can base silane thing combination and with vinyl, when the high polymer material that free redical reacts, by peroxide to occur polymerization anti-
At once, vinyl can participate in this polymerisation in the lump, cause graphite and high molecular polymer formation chemical bond, except compound rear material
Material surfacing and reduce the free space between high molecular polymer and filler there is provided reduction thermal contact resistance and material thermal resistance
Solution route.
It is so that the present invention is that asymptotic expression forms chemical bond on heat filling surface with complete, that is, first addition heat conduction is filled out
Before material, the existing mixture for the high polymer material that the thing of base silane containing function and free redical react, now heat filling is herein
Solid content in mixture is low, therefore has splendid blending effect, and heat filling may be homogenously dispersed in mixture, therefore control
Outside heating-up temperature and because of the essential acidic nature of heat filling and the moisture content of absorption, alkoxy that can be with the thing of base silane containing function
Condensation chemical reaction is hydrolyzed and chemical bonded refractory is formed, and then reaches the mixture of expected low-viscosity；When the addition that continues
The secondary thing of base silane containing function is in this mixture, in addition to obtaining and having the mixture of more low-viscosity, also creates and first
Secondary identical hybird environment, is conducive to the expected hydrolytic condensation chemistry of blending and generation for adding second of heat filling anti-
Should；The hydrolytic condensation chemistry expected from the addition third time thing of base silane containing function and the generation of third time conducting filler that continues is anti-
Should；By such program, but it is not limited to three times, it can be divided into four times or five times, it is considered to time cost, relatively appropriate number of times is
Three times, homogeneous mixture can be now obtained, when peroxide is added, its high polymer material reacted using free redical is carries
Body, contribute to peroxide it is dispersed in the mixture, while shorten the blending time；And the charging side of this gradation asymptotic expression
Formula, helps to complete the surfaction in filler Surface Creation chemical bonded refractory while blending.
Another person, the present invention still further provides cementing layer, and the gluing in the one or both sides of heat transfer composite
Layer is made to strengthen the functional of heat transfer composite, and the cementing layer can stick together to be glutinous without touching with one's hand or not having completely
Property, end is suited the particular use, and the cementing layer is made up of add-on type liquid macroimolecule material, the add-on type liquid macroimolecule material with it is upper
The high polymer material for stating free redical reaction is same type, that is, is all the add-on type liquid using siloxanes macromolecule as main chain
High polymer material is formed by least two high polymer materials through polyaddition reaction, and it is respectively to contain vinyl and hydrogen-based, its
Can be via catalyst, relatively appropriate catalyst is the catalyst of platiniferous composition, and it can be by vinyl and hydrogen-based with appropriate ratio
Example is in 130~170 DEG C, and relatively appropriate temperature was 150 DEG C, through 1~10 minute, compares reasonable time for 5 minutes, can obtain
Obtain cementing layer.However, not yet generation cementing layer before, can prior to heat transfer composite one side in the way of spraying it is appropriate
Addition delayed-action activator, solvent can be added if necessary, then with above-mentioned temperature and time, occur addition polymerization with continous way processing procedure anti-
Should, can be obtained in the one side of heat transfer composite can generate chemical bonded refractory, and then shape with the vinyl of heat transfer composite
Into the glutinous cementing layer without touching with one's hand；Also, typically make the multiple material of heat conduction it is glutinous without touch with one's hand cementing layer when, be in mixture base material
Silicone oil is added, such a mode there must be the situation that silicone oil oozes out, and present invention application base material adjusts vinyl and hydrogen in itself
The proper proportion of base, does not have the problem of silicone oil oozes out.
The above described is only a preferred embodiment of the present invention, any formal limitation not is made to the present invention, it is all
It is any simple modification, equivalent variations and the modification made according to the technical spirit of the present invention to above example, still falls within
In the range of technical solution of the present invention.
In summary, the present invention is in structure design, using in practicality and cost benefit, complying fully with industry development institute
Need, and disclosed structure is also, with unprecedented innovative structure, with novelty, creativeness, practicality, to meet relevant
The regulation of patent of invention important document, therefore lift application in accordance with the law.
Claims (4)
1. a kind of heat transfer composite, it is characterised in that including：
Macromolecule mixture, the high polymer material comprising free redical reaction is with that can mix the high polymer material with radical reaction
The peroxide of conjunction；
Heat filling, including at least the compatible Heat Conduction Material of two kinds of properties；And
Silane thing, including at least two kinds of different functional groups, a kind of functional group may participate in macromolecule mixture free radical mixing
Reaction, another functional group can be in the heat filling Surface Creation chemical bonded refractory；
The high polymer material is the dimethyl silicone polymer containing at least two vinyl functional groups；The heat filling contains tool
The composite inorganic material of hole and the graphite composite powder of compressibility with wrapping up graphite with nickel；The silane thing contains vinyl and alcoxyl
Base.
2. heat transfer composite according to claim 1, it is characterised in that the heat filling wraps up graphite with nickel
The blending of composite inorganic material and graphite composite powder has compressibility, is reduced with reducing the space after graphite composite powder formation sheet
Thermal impedance；The acidity of graphite essence and the characteristic of absorption moisture content, cause the alkoxy of the silane thing that hydrolytic condensation occurs therewith
Chemical reaction, and in graphite surface formation chemical bond so that graphite surface because and the silane thing combination and there is vinyl, enter
And the reaction that the high polymer material occurs by peroxide is participated in, cause graphite and macromolecule mixture formation chemical bond,
Thermal impedance is reduced to reduce the space between macromolecule mixture and filler.
3. heat transfer composite according to claim 1 or 2, it is characterised in that further compound in the heat transfer
At least one side of material is combined cementing layer, and the cementing layer can be to be glutinous without touching with one's hand or not having completely tackness, and the cementing layer is by adding
The high polymer material that shaping liquid high polymer material is made and reacted with the macromolecule mixture free redical is all with siloxanes
Macromolecule is main chain, and the add-on type liquid macroimolecule material is by two kinds of high polymer materials at least containing vinyl and hydrogen-based through adding
Formed into reaction.
4. heat transfer composite according to claim 3, it is characterised in that the temperature of the macromolecule mixture reaction
For 150~200 DEG C, the time is 2~10 minutes.
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| CN201310001028.2A CN103911006B (en) | 2013-01-04 | 2013-01-04 | Heat transfer composite and manufacture method |
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| CN201310001028.2A CN103911006B (en) | 2013-01-04 | 2013-01-04 | Heat transfer composite and manufacture method |
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| CN103911006B true CN103911006B (en) | 2017-07-28 |
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Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105271938B (en) * | 2015-10-16 | 2017-04-19 | 孙刚 | Heat-transfer joint sealing material |
| TWI614332B (en) * | 2016-09-22 | 2018-02-11 | 國立交通大學 | Polymeric composites having thermal conductivity and manufacturing method thereof |
| CN109111742B (en) * | 2018-07-10 | 2021-09-10 | 江门市硅成新材料有限公司 | Heat-conducting silicone grease for computer CPU and preparation method thereof |
| JP2020037634A (en) * | 2018-09-03 | 2020-03-12 | トヨタ自動車株式会社 | Thermally conductive material, production method thereof and thermally conductive composition |
| CN113861623A (en) * | 2021-10-25 | 2021-12-31 | 宁夏清研高分子新材料有限公司 | Preparation method of heat-conducting LCP composite material |
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| CN102827480A (en) * | 2012-09-03 | 2012-12-19 | 华东理工大学 | Method for preparing high-heat-conducting silicon rubber compound material |
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| JP4214203B2 (en) * | 1999-05-18 | 2009-01-28 | オリヱント化学工業株式会社 | Organic-inorganic composite material and method for producing the same |
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| CN102220006A (en) * | 2011-04-28 | 2011-10-19 | 天津大学 | Mixed filling type thermal conductive silicone rubber composite and preparation method thereof |
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