CN107760278A - Composition as thermal interfacial material - Google Patents
Composition as thermal interfacial material Download PDFInfo
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- CN107760278A CN107760278A CN201610701277.6A CN201610701277A CN107760278A CN 107760278 A CN107760278 A CN 107760278A CN 201610701277 A CN201610701277 A CN 201610701277A CN 107760278 A CN107760278 A CN 107760278A
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- composition
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- heat conduction
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
- C09K5/08—Materials not undergoing a change of physical state when used
- C09K5/14—Solid materials, e.g. powdery or granular
Abstract
The present invention relates to the composition as thermal interfacial material, it includes porous matrix and the packing material being filled in the hole of porous matrix, wherein described packing material includes about 20 80 weight % polymeric substrate and about 20 80 weight % heat conduction additive, and the weight % is the gross weight meter with packing material.
Description
Technical field
The present invention relates to the composition as thermal interfacial material, more particularly to one kind comprising porous matrix and to be filled in porous
The composition of packing material in the hole of matrix, the composition have improved thermal conductivity.
Background technology
In recent years, with the fast development of electronic device integrated technique, the integration degree more and more higher of electronic device, and
Device volume but becomes less and less, its requirement to radiating also more and more higher.In order to meet these needs, various radiating modes
Largely used, such as utilize fan cooling, water-cooling auxiliary heat radiating and heat pipe heat radiation mode, and obtain certain radiating effect
Fruit, but due to the contact interface of radiator and electronic device and out-of-flatness, typically contact with each other only less than 10% area,
There is no preferable contact interface, fundamentally greatly affected the effect that electronic device carries out heat transfer to radiator, therefore
Increase the higher thermal interfacial material of thermal conductivity factor between contact interface of the radiator with electronic device to increase the contact between interface
Area just seems very necessary.
Traditional thermal interfacial material be the higher particle of some thermal conductivity factors is distributed in polymeric material formed it is compound
Material, such as graphite, boron nitride, silica, aluminum oxide, silver or other metals.The heat conductivility of such a material is largely
Property depending on polymer support.Wherein using grease, phase-change material as carrier composite because its using when be liquid and
It can be infiltrated with heat source surface, therefore thermal contact resistance is smaller, and the thermal contact resistance using silica gel and rubber as the composite of carrier just compares
It is larger.One common defects of these materials are that the thermal conductivity factor of whole composite is smaller, about lW/mK, and this is increasingly
Demand of the raising to radiating of semiconductor integrated degree is not adapted to, and the content for increasing heat conduction particle in polymer support arrives
60 weight % and during the above, the thermal conductivity factor of whole composite can be increased by particle is contacted with each other as far as possible with particle, such as certain
Therefore the thermal conductivity factor of a little special boundary materials can reach 2-5W/mK, but when the content of heat conduction particle in polymer support increases
Being added to 85 weight % or more Gao Shihui makes polymer lose required performance, as grease can be hardened, so as to which effect of impregnation can become
Difference, rubber can also be hardened, and so as to lose pliability, this all can substantially reduce thermal interfacial material performance.
Preferable thermal interfacial material is placed between radiator and thermal source (i.e. electronic device), it is desirable to comes from the heat of thermal source
Rapidly it is transmitted to along the vertical direction of thermal source and radiator by thermal interfacial material on radiator, reduces the temperature of thermal source;
It also can quickly be spread by thermal interfacial material along the direction parallel to thermal source and radiator simultaneously, avoid hot-spot from producing heat
Put and form bad point;So as to reach heat transfer and even hot dual purpose, avoiding electronic device, insufficient, temperature is too high because radiating,
The problems such as performance reduces caused by amount of localized heat accumulation, unstable or service life shortens.With electronic device multifunction
With the trend of miniaturization, energy density more and more higher caused by electronic device work, accordingly, it would be desirable to which thermal interfacial material hangs down
Directly to thermal conductivity factor (i.e. along the vertical direction of thermal source with radiator) and the hot coefficient of parallel guide (i.e. along parallel to thermal source and
The direction of radiator) both greater than or equal to 5W/mK.
According to the condition applied in the composition of thermal interfacial material, the shape for measurement, forming method and forming method,
The thermal conductivity factor of thermal interfacial material can have directional dependence, you can to show isotropism or anisotropy.According to melting
Be blended and the mode of hot pressing be by the thermal interfacial material machine-shaping of polymer matrix, heat filling it is random it is scattered in the polymer,
The thermal conductivity factor of resulting thermal interfacial material is isotropic, but all very low in all directions, about lW/mK, it is impossible to full
Sufficient demand.The thermal interfacial material machine-shaping of polymer matrix, thermal interfacial material are being added according to the mode of mold injection molding
Flowed into after heat through over pressurizeed in mould, then by being cooled and shaped so that the thermal conductivity factor after thermal interfacial material shaping shows
The characteristics of anisotropy, thermal conductivity factor when hot interface is molded in material flow direction are typically about 2-8W/mK, are perpendicular to material
3~10 times of the thermal conductivity factor (about 0.6-2W/mK) of direction of flow, that is to say, that the thermal conductivity factor only on a direction
More than 5W/mK, so heat conduction and even hot requirement can not be met simultaneously.
Therefore, it is necessary to can provide a kind of heat conduction isotropic thermal interfacial material, and it is vertically to thermal conductivity factor (i.e. edge
Vertical direction of the thermal source with radiator) it is all big (i.e. along the direction parallel to thermal source and radiator) with the hot coefficient of parallel guide
In or equal to 5W/mK.
The content of the invention
The invention provides a kind of composition as thermal interfacial material, it is included:
(a) porous matrix;With
(b) packing material being filled in the hole of porous matrix;
Wherein, the heat conduction of polymeric substrate and about 20-80 weight % that the packing material includes about 20-80 weight % adds
Add agent, the weight % is the gross weight meter with packing material.
Present invention also offers the hot interface assembly for including the above-mentioned composition as thermal interfacial material.
Present invention also offers the method for manufacturing the above-mentioned composition as thermal interfacial material.
Brief description of the drawings
The sectional view of one embodiment of the composition 10 as thermal interfacial material of Fig. 1 display present invention, it is included:
(a) porous matrix 101 and (b) are filled in the packing material 102 in the hole of porous matrix, and wherein packing material 102 includes poly-
Compound base material 102-1 and heat conduction additive 102-2.
The sectional view of one embodiment of the hot interface assembly 20 of Fig. 2 display present invention, it is included:Radiator 201, heat
Source 203 and the hot interface device 202 being arranged between the thermal source and radiator, wherein, the hot interface device 202 includes this
Invention the composition as thermal interfacial material, x directions represent parallel to thermal source and radiator direction, y directions representative along
The vertical direction of thermal source and radiator.
Detailed description of the invention
If do not otherwise indicated, all publications, patent application, patent and other references that this specification is previously mentioned
Its entirety is expressly incorporated in this specification for all purposes by document by quoting, as having been fully disclosed herein.
Unless otherwise defined, all technologies that otherwise this specification uses have and art of the present invention with scientific terminology
In the identical implication that is generally understood that of those of ordinary skill.In case of conflict, by with the definition in this specification
It is defined.
Unless otherwise indicated, all percentage, number, ratio etc. be all by weight.
As used in this specification, " by ... preparing " this term is synonymous with term "comprising".In this specification
Used, term "comprising", " comprising ", " having ", " containing " or their any other modification are intended to cover nonexcludability
Inclusion.For example, composition, technique, method, product or instrument comprising a series of elements are not necessarily limited to those key elements,
But can include not expressly listed other key elements either this composition, technique, method, product or instrument it is intrinsic
Other key elements.
Conjunction " by ... form " do not include any unspecified key element, step or composition.Will if in right
Ask in book, in addition to impurity generally adjoint with it, this conjunction will be such that claims close to cited material.
When " by ... form " in the subordinate clause of this phrase characteristic for appearing in claims rather than and then preceding prelude
Timesharing, it is limited only within key element listed in the subordinate clause;Other key elements are not precluded from outside the entirety of claims.
Conjunction " substantially by ... form " is used to limit composition, method or instrument, it include except those it is literal on begged for
Material, step, feature, component or key element outside, on condition that these additional material, step, feature, component or key elements are not
Substantially influence the basic feature with novelty of claimed invention.Term " substantially by ... form " is located at
"comprising" and " by ... form " between intermediate range.
Term "comprising" include by " substantially by ... form " and " by ... form " the implementation covered of term
Scheme.Similarly, term " substantially by ... form " includes the embodiment that term " consist of " covers.
When quantity, concentration or other values or parameter are as scope, preferred scope or preferred upper limit value and preferred lower limit value
List when providing, it should be understood that specifically disclose any pair of range limit or preferred value and range lower limit or preferred value institute
All scopes formed, no matter whether scope is individually disclosed.For example, when enumerating the scope of " 1-5 ", disclosed scope should
It is interpreted as including " 1-4 ", " 1-3 ", " 1-2 ", " 1-2 and 4-5 ", " 1-3 and 5 " etc..Numerical value is enumerated in this manual
During scope, unless otherwise indicated, the scope is intended to the end points for including scope and all integers and fraction within the scope of.
When being worth using term " about " description or during the end points of scope, present disclosure should be read to include the specific of meaning
Value or end points.
In addition, unless clearly there is opposite explanation, "or" refers to the "or" of inclusive, rather than exclusive "or".For example,
Any one condition for all meeting A "or" B below:A be true (or presence) and B be false (or in the absence of), A be false (or in the absence of)
And B is true (or presence) and A and B is true (presence).
Embodiment of the present invention described in the Summary of the present invention includes any described in this specification
Other embodiments, and can combine in any way, and subject description in embodiments is directed not only to the present invention's
Composition, further relate to include the hot interface assembly of said composition.
The present invention is described in detail as follows.
The composition as thermal interfacial material of the present invention includes:(a) porous matrix and (b) are filled in the hole of porous material
Packing material in gap, wherein packing material include polymeric substrate and heat conduction additive, and of the invention is used as thermal interfacial material
An embodiment of composition be illustrated in Fig. 1.
(a) porous matrix
In the present invention, the porous matrix (a) is a kind of by being mutually communicated or blind bore gap forms one, two or three-dimensional
The material of space net structure;Preferably by the material for the hole Special composition network structure being mutually communicated, i.e. via material.
The diameter in the aperture of the porous matrix, i.e. hole, is about 50-3000 μm, or about 150-800 μm, or about 300-
500μm.The shape of the hole can be arbitrary shape, such as circular, square, polygon or irregular shape.It is described porous
The porosity of matrix is at least 70%, or at least 80%, and porosity (Porosity) is to characterize the hole portion of porous matrix herein
Point physical quantity, be defined as the volume of hole and the ratio of the cumulative volume of porous matrix, represented with percentage, be 0 to 100% it
Between.The bulk density of the porous matrix is about 0.1-1g/cm3, herein bulk density refer to porous matrix in nature
Under unit volume weight.
The porous matrix for being suitable for the composition of the present invention can be by selected from copper, aluminium, silver, gold, iron, steel and its alloy
Metal material made from foam metal, the foam metal preferably as made from copper.In one embodiment of the invention, this hair
The porous matrix of bright composition is the foam metal of through hole.
Being suitable for the foam metal of the present invention can be made by any conventional known method in this area, specifically, by
The closed-cell foam metal that blind bore gap is formed can be obtained by foam process, as foam melt method, direct blowing gas foam
Method, metal dust and foaming agent mixture densification foaming;The through-hole foamed metal being made up of the hole being mutually communicated can be with
By Seepage Foundry, deposition, powder loose sintering, the technique acquisition for adding pore creating material, porous preform is such as obtained first, it is prefabricated
Part can be sintered body or porous plastics of salt (NaC1) etc., then carry out the works such as seepage flow, deposition, sintering using porous preform
Skill, obtain open-pore metal foam.
The porous matrix being suitable in the composition of the present invention can also be is made porous matrix by nonmetallic materials, such as steeps
Foam carbon, foamed ceramics or by selected from polysiloxanes, polyurethane, polyethylene, rubber, ethylene-vinyl acetate copolymer and its mixing
Foamed polymer is made in thing.The foamed ceramics for being wherein suitable for the present invention can be foamed alumina, foam zirconium oxide, foamy carbon
SiClx or foam silicon nitride.In one embodiment of the invention, the porous matrix of composition of the invention is the poly- silica of foam
Alkane.
Being suitable for the foamy carbon of the present invention can be made with any conventional known method in this area, such as organosilane precursor
Body pressure expansion method or template.The foamed ceramics for being suitable for the present invention can be with any conventional known formula legal system in this area
, such as foaming, sol-gal process, addition pore creating material method or organic precursor infusion process.The foam for being suitable for the present invention gathers
Compound can be made, wherein foaming agent can be chemical hair with any conventional known method in this area, such as foam process
Infusion, gas or water, such as when preparing siloxanes porous material, fluid can be made first, such as carbon dioxide, nitrogen or chlorine fluorine
Alkane, immerse in the block of silicone block copolymer and be copolymerized for a period of time with forming the siloxane blocks of saturated with fluid under stress
Thing, the fluid are dissolved in silicone block copolymer, are nucleated and grow to form siloxanes porous material when removing pressure, institute
Fluid can be gaseous state, liquid or postcritical form.
Porous matrix suitable for the present invention is commercially available, such as the board purchased from Shanghai Zhong Wei new materials Co., Ltd
Number foam copper products for being Cu-10, praise purchased from Kunshan the foam copper that the trade mark of hundred million Sheng electronics new material Co., Ltds is JYS01
Product or the foamed aluminium purchased from Shanghai Zhonghui Foamed Aluminum Product Co., Ltd., the bubble purchased from the magnificent carbon high-tech Co., Ltd in Hunan nine
Foam carbon, purchased from the foam silicon carbon and foamed alumina of Baoding Ning Xin new materials Co., Ltd, purchased from the middle limited public affairs of source porcelain industry
The foam silicon carbon of department or the foamed ethylene acetate ethylene copolymer purchased from Changzhou Fa De plasthetics factory.
Packing material (b)
In the present invention, the composition as thermal interfacial material is also comprising the filling material being filled in the hole of porous matrix
To expect (b), the packing material includes about 20-80 weight % polymeric substrate and about 20-80 weight % heat conduction additive, or
The heat conduction additive of polymeric substrate comprising about 25-75 weight % and about 25-75 weight %, the weight % are to fill material
The gross weight meter of material.
Ethylene methacrylic acid copolymer, ethylene vinyl acetate second are may be selected from for the polymeric substrate in the composition of the present invention
Enoate copolymer, ethylene acrylic acid co polymer elastomer, fluoroelastomer, and their mixture.
In one embodiment of the invention, the polymeric substrate for the composition of the present invention is ethylene methyl propylene
Acid copolymer.
In another embodiment of the present invention, the polymeric substrate for the composition of the present invention is ethylene-vinyl acetate
Ester copolymer.
In yet another embodiment of the present invention, the composition polymeric substrate for the present invention is total to for ethylene acrylic
The mixture of polymers and fluoroelastomer, it includes about 10-40 weight % ethylene acrylic acid co polymer and about 60-90 weight %
Fluoroelastomer, the weight % is the gross weight meter of the mixture with ethylene acrylic acid co polymer and fluoroelastomer.Institute
State fluoroelastomer and include at least about 53 weight % fluorine, specifically, being adapted to the fluoroelastomer of the present invention to include following copolymerization
Unit:Vinylidene fluoride and at least one are iodo- selected from hexafluoropropene, tetrafluoroethene, the bromo- 3,3,4,4- tetrafluoros butene-1s of 4-, 4-
3,3,4,4- tetrafluoros butene-1, perfluor (methyl ethylene) ether, 1,1,3,3,3- pentafluoropropenes or its mixture it is other fluorine-containing
Monomer.
It is adapted to the polymeric substrate of the composition of the present invention commercially available, such as obtained from E.I.Du Pont Company (E.I.du Pont
Nemours and Company.Inc.) trade mark of (being hereinbelow abbreviated as " Du Pont ") is40W ethylene vinyl acetate
Vinyl ester copolymers, the trade mark are599 ethylene methacrylic acid copolymer, the trade mark areDP ethylene propylene
Olefin(e) acid copolymer elastomer or or the trade mark beGF200s fluoroelastomer, purchased from Sumitomo Chemical Co
The trade mark is RB-11 ethylene vinyl acetate copolymer, or is purchased from the trade mark of Taiwan Polymer Chemical Products Co., Ltd.653-04 ethylene vinyl acetate copolymer.
Optionally, other additives can also be included in the packing material, such as crosslinking agent, antioxidant.In the present invention
One embodiment in, about 0.1-5 weight % crosslinking agent is also included in the packing material of composition of the invention, it is described heavy
It is in terms of the weight of the polymeric substrate in packing material to measure %.Wherein described crosslinking agent can be (the tert-butyl group mistakes of 1,1- bis-
Oxygen) -3,3,5- trimethyl-cyclohexanes and/or the peroxidating 2- ethylhexyl carbonate tert-butyl esters.
Heat conduction additive suitable for the composition of the present invention may be selected from expanded graphite, nano graphite flakes, carbon fiber, gold
Belong to particle and its mixture, preferably expanded graphite, nano graphite flakes and its mixture.
In one embodiment of the invention, the heat conduction additive for the composition of the present invention is expanded graphite, institute
The length for stating expanded graphite is 200-500 μm, and width is 50-800 μm, and bulk density is no more than 0.2g/cm3.The expansion
Graphite can be made by expansible graphite, such as expansible graphite is placed in air or inert gas, be heated to about 400-
After 1000 DEG C and insulation about 5-10 minutes are made.Wherein applicable expansible graphite is laminated structure, and lateral dimension is in its piece
About 50-800 μm, its thickness is about 0.5-30 μm.
In another embodiment of the present invention, the heat conduction additive for the composition of the present invention is nano graphite flakes,
The nano graphite flakes are laminated structure, and its thickness is about 1-30nm, or about 10-25nm, and lateral dimension is about 1-15 μ in its piece
m.Described herein interior lateral dimension refers to had along the surface on the surface of expansible graphite lamella or nano graphite flakes lamella
Some full-size.
It is commercially available for the heat conduction additive in the composition of the present invention, such as purchased from the extensive nanometer new material in Ningbo
The silver particles or copper particle of limited company, it is chopped up to the size of composite Co., Ltd for 325 purposes purchased from Nanjing latitude
Carbon fiber powder or the nano graphite flakes purchased from the Nanjing Ji Cang nanosecond science and technology Co., Ltd trade mark for JCGNP10-5.It is swollen for preparing
Swollen graphite is also commercially available for use as the expansible graphite of heat conduction additive, such as purchased from Qingdao Xinghe graphite Co., Ltd
Expansible graphite or purchased from Baoding angstrom can gloomy carbon product Co., Ltd size for 100 mesh, 200 mesh or 50 mesh low-sulfur at
Manage expansible graphite.
The preparation of composition as thermal interfacial material
It is not specifically limited in the present invention for preparing the method for the above-mentioned composition as thermal interfacial material, it can be with
For any conventional known method in this area.For example, methods described may comprise steps of:(i) porous matrix is provided, gathered
Compound base material and heat conduction additive;(ii) by the filling material of hot pressing slabbing after polymeric substrate and heat conduction additive melt blending
Material;(iii) packing material of sheet is placed on porous matrix, then hot pressing so that packing material is pressed into the hole of porous matrix
In gap, the composition as thermal interfacial material of the present invention is obtained.
In one embodiment of the invention, the method for manufacturing the composition as thermal interfacial material of the present invention, comprising
Following steps:
(i) porous matrix, polymeric substrate and heat conduction additive are provided;
(ii) by the packing material of hot pressing slabbing after polymeric substrate and heat conduction additive melt blending;With
(iii) packing material of sheet is placed on porous matrix, then hot pressing so that packing material pressure
In the hole for entering porous matrix, the composition as thermal interfacial material is obtained;
Wherein, the heat conduction of polymeric substrate and about 20-80 weight % that the packing material includes about 20-80 weight % adds
Add agent, the weight % is the gross weight meter with packing material.
Present invention also offers hot interface assembly, the hot interface assembly includes thermal source, radiator and is arranged on the heat
Hot interface device between source and radiator, wherein hot interface device includes the above-mentioned composition as thermal interfacial material.Fig. 2 shows
Show the sectional view of an embodiment of the hot interface assembly of the present invention, it is included:Radiator 201, thermal source 203 and it is arranged on institute
The hot interface device 202 between thermal source and radiator is stated, wherein, the hot interface device 202 is used as hot boundary comprising the present invention's
The composition of plane materiel material, x directions represent the direction parallel to thermal source and radiator, and y directions are represented along thermal source and radiator
Vertical direction.The thermal source of the hot interface assembly can be central processor unit (CPU), graphics processor unit (GPU), place
Manage device integrated heat spreader (IHS), power module or other electronic devices for producing heat.
As it was previously stated, it is expected can obtain a kind of thermal conductivity factor isotropism and sufficiently high thermal interfacial material, i.e., vertically to
Thermal conductivity factor (i.e. along the vertical direction of thermal source with radiator) is with the hot coefficient of parallel guide (i.e. along parallel to thermal source and radiating
The direction of device) both greater than or the thermal interfacial material equal to 5W/mK.In the present invention, can by will include polymeric substrate and
The packing material of heat filling, which is filled in the hole of porous matrix, is made required composition.With polymerizeing comprising same composition
Thing base material and heat filling but composition not comprising porous matrix is compared, composition of the invention it is vertical to thermal conductivity factor and
It is parallel to be not only both greater than 5W/mK to thermal conductivity factor, and show and vertically add about 50% or more to thermal conductivity factor, preferably
About 100% or more, more preferably about 150% or more.
Without further elucidated above, it is believed that use is described above, and those skilled in the art can utilize the present invention to it
At utmost.Therefore, following examples are only illustrative, without limiting the disclosure in any way.
Embodiment
Abbreviation " E " representative " embodiment ", " CE " representative " comparative example ", numeral thereafter show that composition is implemented at which
Prepared in example.Embodiment and comparative example are prepared and tested in a similar manner.
Material
Porous matrix (Cu foam):The foam copper of through hole, size are 5cm × 5cm × 1mm, its hole it is a diameter of about
300-500 μm, porosity is about 80%, a diameter of about 100-200 μm of the single copper wire of hole is formed, with trade mark Cu-10
Purchased from Shanghai Zhong Wei new materials Co., Ltd.
Polymeric substrate -1 (P-1):Ethylene methacrylic acid copolymer, with the trade mark599 are obtained from Du Pont's public affairs
Department.
Polymeric substrate -2 (P-2):Ethylene vinyl acetate copolymer, with the trade mark40W is obtained from E.I.Du Pont Company.
Polymeric substrate -3 (P-3):About 20 weight % ethylene acrylic acid co polymer elastomer and about 80 weight %'s contains
The blend of fluoroelastomer, the weight % are with the total of the mixture of ethylene acrylic acid co polymer elastomer and fluoroelastomer
Weight meter, wherein ethylene acrylic acid co polymer elastomer are with the trade markDP is obtained from E.I.Du Pont Company, and fluoroelastomer is
The trade mark be withGF200s is obtained from E.I.Du Pont Company.
Crosslinking agent:The peroxidating 2- ethylhexyl carbonate tert-butyl esters, CAS No.:3006-82-4, purchased from Chinese medicines group chemistry
Reagent Co., Ltd.
Heat conduction additive -1 (T-1):Expanded graphite, vermiform loose structure, length are about 80-5000 μm, and width is 75 μ
M, bulk density 0.18g/cm3, by purchased from Baoding Chinese mugwort can the specification of gloomy carbon product Co., Ltd be horizontal in 200 mesh and piece
It is made, purchased expansible graphite is placed in Muffle furnace, in air atmosphere to the low-sulfur expansible black lead that size is about 75 μm
It is heated to 400 DEG C to keep no longer changing to volume for 5 minutes, is then cooled to room temperature, that is, obtains the swollen of heat conduction additive -1
Swollen graphite.
Heat conduction additive -2 (T-2):Expanded graphite, vermiform loose structure, length are about 80-5000 μm, width 150
μm, bulk density 0.1g/cm3, by purchased from Baoding Chinese mugwort can the specification of gloomy carbon product Co., Ltd be horizontal in 100 mesh and piece
It is made, purchased expansible graphite is placed in Muffle furnace, in air atmosphere to the low-sulfur expansible black lead that size is about 150 μm
It is heated to 400 DEG C to keep no longer changing to volume for 5 minutes, is then cooled to room temperature, that is, obtains the swollen of heat conduction additive -2
Swollen graphite.
Heat conduction additive -3 (T-3):Expanded graphite, vermiform loose structure, length are about 80-5000 μm, width 300
μm, bulk density 0.04g/cm3, by purchased from Baoding Chinese mugwort can the specification of gloomy carbon product Co., Ltd be horizontal in 50 mesh and piece
It is made, purchased expansible graphite is placed in Muffle furnace, in air atmosphere to the low-sulfur expansible black lead that size is about 300 μm
It is heated to 400 DEG C to keep no longer changing to volume for 5 minutes, is then cooled to room temperature, that is, obtains the swollen of heat conduction additive -3
Swollen graphite.
Heat conduction additive -4 (T-4):Nano graphite flakes, piece Inner lateral dimensions are about 5 μm, and thickness is about 15nm, with the trade mark
JCGNP10-5 is purchased from Nanjing Ji Cang nanosecond science and technology Co., Ltd.
Heat conduction additive -5 (T-5):The tin bismuth of heat conduction additive -3 comprising about 60 weight % and about 40 weight %
(SnBi) mixture of alloyed powder, wherein SnBi alloyed powders are purchased from Hua Yuan Science and Technology Ltd.s of Huizhou City, and its D50 size is about 25
μm。
Prepare E1-E12 and CE1-CE12 composition
1. prepare CE2-CE5, CE7, CE8, CE10 and CE12 composition
Polymeric substrate, crosslinking agent and heat filling are put into banbury (Mixer according to the ratio set in table 1-3
350E, Plasti-Corder Lab-Station, Brabender GmbH&Co.KG) in melted under conditions of about 40 DEG C it is mixed
Close, then by gained mixture thing with flat-bed press (GT-7014-A, GOTECH testing Machines Inc) in sky
Atmosphere, which encloses hot pressing under conditions of middle about 90 DEG C, turns into the sheet material of 1mm thickness, and it is 5cm × 5cm to be cut to planar dimension, is obtained
To the sheet-like composition that size is 5cm × 5cm × 1mm.
2. prepare CE1, CE6, CE9, CE11 and E1-E12 composition
Polymeric substrate, crosslinking agent and optional heat filling are put into banbury according to the ratio set in table 1-3
In (Mixer 350E, Plasti-Corder Lab-Station, Brabender GmbH&Co.KG) under conditions of about 40 DEG C
Melting mixing, filled compositions are obtained, then by the filled compositions of gained flat-bed press (GT-7014-A, GOTECH
Testing Machines Inc) hot pressing turns into the sheet material of about 1mm thickness under conditions of about 90 DEG C in air atmosphere, and cuts
It is 5cm × 5cm into planar dimension, obtains the sheet packing material that size is 5cm × 5cm × 1mm.By the above-mentioned size prepared
It is placed at for 5cm × 5cm × 1mm sheet packing material on the foam copper for the through hole that size is 5cm × 5cm × 1mm so that piece
5cm × 5cm of shape packing material plane is completely covered in 5cm × 5cm of foam copper plane, then using flat board hot pressing
Sheet packing material is heated to 100 by machine (GT-7014-A, GOTECH testing Machines Inc) under air atmosphere
DEG C, with 0.1MP pressure hot pressing 10 minutes so that sheet packing material melts and is pressed completely into the hole of foam metal copper
In;Then rise temperature after continuing hot pressing under 0.1MPa pressure 15 minutes, is taken out simultaneously certainly to 150 DEG C of degree from hot press
Room temperature so is cooled to, obtains corresponding composition.
Method of testing
By the composition obtained by E1-12 and CE1-CE12 cut into a diameter of 2.5mm, thickness be 1mm disc sheet material,
Upper and lower surface even application graphite powder, according to ASTM E1461 method, using laser heat conducting instrument (LFA 447,GmbH) thermal conductivity factor λ in the face of sample is measured∥(W/mK), i.e., it is used for hot interface group
It is parallel to thermal conductivity factor when in part (along the direction parallel to thermal source and radiator).
By the composition obtained by E1-12 and CE1-CE12 cut into a diameter of 6mm, thickness be 1mm disc sheet material, on
Lower surface even application graphite powder, according to ASTM E1461 method, using laser heat conducting instrument (LFA 447,GmbH) come measure sample cross face thermal conductivity factor λ⊥(W/mK), i.e., it is used for hot interface group
It is vertical to thermal conductivity factor when in part (along perpendicular to the direction of thermal source and radiator).
Vertically (the Δ λ of the improvement to thermal conductivity factor⊥%) calculated by following formula:
Δλ⊥%=[(λ⊥n-λ⊥0)/λ⊥0]×100
Wherein λ⊥0For the λ value of reference example;λ⊥nFor the λ for the example compared⊥Value.
Table 1
“a" show the reference example that CE2 is the improvement calculating for E1-E3;“b" show that CE3 is used for E4 and E5 improvement calculating
Reference example;“c" show the reference example that CE4 is the improvement calculating for E6;“d" show that CE5 is used for E7 and E8 improvement calculating
Reference example;“e" show also to include the 2 weight % crosslinking agent peroxidating 2- ethylhexyl carbonate tert-butyl esters in packing material, it is described
Weight % is in terms of the weight of the polymeric substrate in packing material.
By the result of table 1, described below is obvious.
Comparison between E2 and CE2 thermal conductivity factor data shows:Polymeric substrate P-1 (ethylene methyl propylene will be included
Acid copolymer) and heat conduction additive T-1 (expanded graphite) packing material be filled in the hole of porous matrix obtained E2
Composition it is vertical to thermal conductivity ratio include identical weight part P-1 and T-1 CE2 composition it is vertical to heat conduction system
Number significantly increases about 474%.
Comparison between E1 and CE2 thermal conductivity factor data shows:Porous matrix is introduced in E1 composition, although its
Middle T-1 content is only 30 weight %, but is 50 weight % but does not include the CE2 of porous matrix composition with T-1 content
Compare, the vertical of E1 composition does not reduce not only to thermal conductivity factor, adds about 179% on the contrary.
Comparison between E3 and CE2 thermal conductivity factor data shows:Containing for porous matrix and T-1 is introduced in E1 composition
Amount brings up to 70 weight %, with T-1 content for 50 weight % but compared with the composition of the CE2 not comprising porous matrix, E3's
The vertical of composition significantly increases about 553% to thermal conductivity factor.
Likewise, when heat conduction additive is changed to the expanded graphite of other sizes, such as T-2 or T-3, or nano-graphite is changed to
During piece T-4, the vertical of corresponding composition is obtained for unexpected increase to thermal conductivity factor.
Specifically, the comparison between E5 and CE3 thermal conductivity factor data shows:Packing material comprising P-1 and T-2 is filled out
Fill the vertical P-1 and T- for including identical weight part to thermal conductivity ratio of the obtained E5 composition in the hole of porous matrix
The vertical of 2 CE3 composition significantly increases about 472% to thermal conductivity factor.
Comparison between E4 and CE3 thermal conductivity factor data shows:Porous matrix is introduced in E4 composition, although wherein
T-2 content is only 30 weight %, but is 50 weight % but does not include the CE3 of porous matrix composition phase with T-2 content
Than the vertical of E4 composition does not reduce not only to thermal conductivity factor, adds about 180% on the contrary.
Comparison between E6 and CE4 thermal conductivity factor data shows:Porous matrix is introduced in E6 composition, although wherein
T-3 content is only 30 weight %, but is 50 weight % but does not include the CE4 of porous matrix composition phase with T-3 content
Than the vertical of E6 composition does not reduce not only to thermal conductivity factor, adds about 223% on the contrary.
Comparison between E8 and CE5 thermal conductivity factor data shows:Packing material comprising P-1 and T-4 is filled in more
The vertical P-1 and T-4 that identical weight part is included to thermal conductivity ratio of obtained E8 composition CE5 in the hole of hole matrix
The vertical of composition significantly increase about 531% to thermal conductivity factor.
Comparison between E7 and CE5 thermal conductivity factor data shows:Porous matrix is introduced in E7 composition, although wherein
T-4 content is only 30 weight %, but is 50 weight % but does not include the CE3 of porous matrix composition phase with T-4 content
Than the vertical of E7 composition does not reduce not only to thermal conductivity factor, adds about 323% on the contrary.
The above results show, the packing material comprising polymeric substrate and heat conduction additive is filled in the hole of porous matrix
Obtained composition in gap, with the packing material of the polymeric substrate comprising same composition and heat conduction additive but not comprising more
The composition of hole matrix is compared, and it vertically adds at least 470% or more to thermal conductivity factor;Even if will wherein heat conduction additive
Content drop to 30 weight %, it vertically adds at least 179% or more to thermal conductivity factor is also unexpected.
Comparison between E1-E8 and CE1 thermal conductivity factor data also indicates that:Polymeric substrate P-1 will be included and heat conduction adds
Add the packing material of agent be filled in be made in the hole of porous matrix E1-E8 composition with only comprising P-1 and porous matrix
CE1 composition is compared, and it has vertically also significantly increased 5.3-14.3W/mK to thermal conductivity factor from 3.4W/mK, and its is parallel
Also 5.4-12.5W/mK has been significantly increased to thermal conductivity factor from 4.6W/mK.
E1-E8 thermal conductivity factor data are also shown that by will include polymeric substrate P-1 and heat conduction additive filling material
Material be filled in the hole of porous matrix, the composition of the invention found it is vertical to thermal conductivity factor (i.e. along perpendicular to
The direction of thermal source and radiator) it is both greater than 5W/mK;The parallel of composition of the present invention can also be maintained to thermal conductivity factor simultaneously
More than 5W/mK, so as to obtain desired thermal conductivity factor isotropism and the sufficiently high combination that can be used as thermal interfacial material
Thing.
In one embodiment of the invention, the composition as thermal interfacial material includes:
(a) porous matrix;With
(b) packing material being filled in the hole of porous matrix;
Wherein,
The porous matrix is the foam metal as made from copper;
The packing material includes about 25-75 weight % ethylene methacrylic acid copolymer and about 25-75 weight %
Heat conduction additive, the weight % are the gross weight meters with packing material;With
The heat conduction additive is selected from expanded graphite, nano graphite flakes and its mixture.
Table 2
“a" show the reference example that CE7 is the improvement calculating for E9;“b" show that CE8 is used for the reference that E10 improvement calculates
Example;“c" show the reference example that CE10 is the improvement calculating for E11;“d" show also to include 2 weight %'s in packing material
The crosslinking agent peroxidating 2- ethylhexyl carbonate tert-butyl esters, the weight % is with the weight of the polymeric substrate in packing material
Meter.
By the result of table 2, described below is obvious.
E9 and CE7, E10 and CE8, E11 and CE10 thermal conductivity factor data between comparison show:Polymer matrix will be included
Material P-2 (ethylene vinyl acetate copolymer) and heat conduction additive T-3 (expanded graphite) packing material are filled in porous matrix
Hole in obtained E9-E11 composition the vertical P-2 and T-3 for including identical weight part accordingly to thermal conductivity ratio
The vertical of composition about 193%-1000% is unexpectedly added to thermal conductivity factor.
Comparison between E9-E11 and CE6 thermal conductivity factor data also indicates that:Packing material comprising P-2 and T-3 is filled out
Compared with the composition for filling CE6 of the composition that E9-E11 is made in the hole of porous matrix with only including P-2 and porous matrix,
Its vertical thermal conductivity has also significantly increased 13.5-16.1W/mK from 2.8W/mK, its it is parallel to thermal conductivity factor also from
3.6W/mK has significantly increased 10.8-15.2W/mK..
E9-E11 thermal conductivity factor data are also shown that by the way that the packing material comprising P-2 and T-3 is filled in into porous matrix
Hole in, the vertical of composition of the invention found is both greater than 10W/mK or more to thermal conductivity factor;The present invention simultaneously
The parallel of composition can also be maintained at more than 10W/mK to thermal conductivity factor, so as to obtain desired thermal conductivity factor respectively to same
Property and the sufficiently high composition that can be used as thermal interfacial material.
In addition, CE9 and E10 thermal conductivity factor data comparison also shows:When heat conduction additive T-3 is changed to T-5, i.e., comprising about
The mixture of 60 weight % T-3 and about 40 weight % tin bismuth (SnBi) alloyed powder, corresponding composition it is vertical to heat conduction
Coefficient is reduced to 4.6W/mK.
In one embodiment of the invention, the composition as thermal interfacial material includes:
(a) porous matrix;With
(b) packing material being filled in the hole of porous matrix;
Wherein, the porous matrix is the foam metal as made from copper;
The packing material includes about 25-75 weight % ethylene vinyl acetate copolymer and about 25-75 weight %
Expanded graphite, the weight % are the gross weight meters with packing material.
Table 3
“a" show the reference example that CE12 is the improvement calculating for E12;“b" show also to include 2 weights in packing material
The % crosslinking agent peroxidating 2- ethylhexyl carbonate tert-butyl esters are measured, the weight % is with the polymeric substrate in packing material
Weight meter.
By the result of table 3, described below is obvious
Comparison between E12 and CE12 thermal conductivity factor data shows:Polymeric substrate P-3 and heat conduction additive will be included
T-3 (content is 50 weight %) packing material is filled in the composition of obtained E1 in the hole of porous matrix, adds with heat conduction
Add agent T-3 content for 30 weight % but the composition of the CE12 not comprising porous matrix compared, E12 composition it is vertical to
Thermal conductivity factor does not reduce not only, unexpectedly adds about 184% on the contrary.
Comparison between E12 and CE11 thermal conductivity factor data also indicates that:Packing material comprising P-3 and T-3 is filled
Compared with the composition that CE11 of the E12 composition with only including P-3 and porous matrix is made in the hole of porous matrix, it hangs down
7.1W/mK also directly is significantly increased from 4.4W/mK to thermal conductivity factor, its is parallel also notable from 4.8W/mK to thermal conductivity factor
Ground increases 10.2W/mK, that is, the composition of the invention found it is vertical to thermal conductivity factor and the hot coefficient of parallel guide all
More than 7W/mK, so as to obtain desired thermal conductivity factor isotropism and the sufficiently high combination that can be used as thermal interfacial material
Thing.
In one embodiment of the invention, the composition as thermal interfacial material includes:
(a) porous matrix;With
(b) packing material being filled in the hole of porous matrix;
Wherein, the porous matrix is the foam metal as made from copper;
The packing material includes about 25-75 weight % polymeric substrate and about 25-75 weight % expanded graphite, institute
It is the gross weight meter with packing material to state weight %;
About 10-40 weight % ethylene acrylic acid co polymer and about 60-90 weight % is included with the polymeric substrate
Fluoroelastomer, the weight % are the gross weight meters of the mixture with ethylene acrylic acid co polymer and fluoroelastomer.
Although explaining and describing in a typical implementation the present invention, it is not intended to be limited to shown thin
Section, this is due to may have the spirit of various modifications and replacement without departing from the present invention.Therefore, invention disclosed herein is repaiied
Change and can be obtained using only normal experiment by those skilled in the art with equivalent, then it is assumed that all such modification and equivalent
Thing is in the spirit and scope of the present invention limited such as following claims.
Claims (10)
1. a kind of composition as thermal interfacial material, it is included:
(a) porous matrix;With
(b) packing material being filled in the hole of porous matrix;
Wherein:
The packing material includes 20-80 weight % polymeric substrate and 20-80 weight % heat conduction additive, described heavy
Amount % is the gross weight meter with packing material.
2. as claimed in claim 1 be used as thermal interfacial material composition, wherein the porous matrix be by selected from copper, aluminium,
Foam metal made from the metal material of silver, gold, iron, steel and its alloy.
3. it is used as the composition of thermal interfacial material as claimed in claim 1, wherein the porous matrix is with least 70%
Porosity and a diameter of 50-3000 μm of hole.
4. it is used as the composition of thermal interfacial material as claimed in claim 1, wherein the polymeric substrate is selected from ethylene methyl
Acrylic copolymer, ethylene vinyl acetate copolymer, ethylene acrylic acid co polymer, fluoroelastomer and its mixture.
5. as claimed in claim 1 be used as thermal interfacial material composition, wherein the heat conduction additive be selected from expanded graphite,
Nano graphite flakes, carbon fiber, metallic and its mixture.
6. it is used as the composition of thermal interfacial material as claimed in claim 1, wherein the heat conduction additive is expanded graphite, and
The length of the expanded graphite is 200-500 μm, and width is 50-800 μm, and bulk density is less than or equal to 0.2g/cm3。
7. it is used as the composition of thermal interfacial material as claimed in claim 1, wherein the heat conduction additive is nano graphite flakes,
And its thickness is 1-30nm, lateral dimension is 1-10 μm in its piece.
8. being used as the composition of thermal interfacial material as claimed in claim 1, it is vertically with parallel guide heat to thermal conductivity factor
Number is all 5.0W/mK or higher.
9. hot interface assembly, it includes thermal source, radiator and the hot interface device being arranged between the thermal source and radiator,
The hot interface device includes any described compositions as thermal interfacial material of claim 1-8.
10. the method for any described compositions as thermal interfacial material of manufacturing claims 1-8, is comprised the steps of:
(i) porous matrix, polymeric substrate and heat conduction additive are provided;
(ii) by after polymeric substrate and heat conduction additive melt blending, it is mixed the packing material of thing hot pressing slabbing;With
(iii) packing material of sheet is placed on porous matrix, then hot pressing so that packing material is pressed into the hole of porous matrix
In gap, the composition as thermal interfacial material is obtained;
Wherein:
The packing material includes 20-80 weight % polymeric substrate and 20-80 weight % heat conduction additive, described heavy
Amount % is the gross weight meter with packing material.
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