CN115157714A - Foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material and preparation method thereof - Google Patents
Foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material and preparation method thereof Download PDFInfo
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Images
Classifications
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- B32B5/18—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by features of a layer of foamed material
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Abstract
The invention provides a foam metal/oriented graphene laminated composite high-heat-conductivity flexible interface material and a preparation method thereof. The test result shows that the composite material maintains excellent flexibility and compressibility while having high thermal conductivity coefficient, and provides a feasible method for breaking through the technical bottleneck.
Description
Technical Field
The invention belongs to the technical field of heat management, and particularly relates to a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material and a preparation method thereof.
Background
With the continuous development of communication technology, the electronic industry tends to be more and more developed to be light, thin, highly integrated and miniaturized. With the size reduction and the integration and power density increase of the chip, the heat generated by the chip during operation increases more and more, which leads to the temperature rise of the chip, and seriously affects the service performance, reliability and service life of the final electronic component. The thermal interface material is widely applied to the field of electronic element heat dissipation, and mainly used for filling the space between a chip and a heat sink and between the heat sink and a radiator to expel air in the space, so that heat generated by the chip can be more quickly transferred to the outside through the thermal interface material, and the important functions of reducing the working temperature and prolonging the service life are achieved.
In recent years, the industry of thermal interface materials in China has been rapidly developed, but the market of high-end heat conduction materials is still occupied by developed countries such as the United states and Japan. The substrates commonly used in current thermal interface materials are polymers and liquid metals. The polymer matrix has good fluidity and processability, but high thermal conductivity interface materials are difficult to obtain by filling thermal conductive fillers; liquid metal has high thermal conductivity, but too high fluidity causes migration problems, which causes circuit pollution of electronic components and even short circuit.
Disclosure of Invention
Aiming at the technical problems, the invention provides a high-thermal-conductivity flexible interface material with a foam metal/oriented graphene laminated composite structure and a preparation method thereof.
The technical scheme of the invention is as follows:
a preparation method of a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material comprises the following operation steps:
s1, preparing graphene coated by magnetic nanoparticles: dispersing a certain amount of graphene in deionized water, sequentially performing electrostatic adsorption treatment by using poly (4-sodium styrene sulfonate) (PSS) and poly (diallyldimethylammonium chloride) (PDDA) to obtain positive charge-coated graphene, and then adding negatively charged ferroferric oxide to react to obtain magnetic particle-coated graphene;
s2, preparing a graphene-containing silica gel prepolymer: weighing a proper amount of vinyl-terminated polydimethylsiloxane, methyl hydrogen-containing silicone oil, a catalyst, an inhibitor and the graphene coated with the magnetic particles prepared in the step S1, mixing, and then stirring in vacuum to obtain a graphene silica gel prepolymer;
s3, preparing an oriented silica gel sheet: transferring the graphene silica gel prepolymer obtained in the step S2 into a mold, and carrying out magnetic field orientation until the graphene silica gel prepolymer is preliminarily cured; drying after primary curing to obtain an oriented silica gel sheet;
s4, coating a graphene silica gel prepolymer on the surface of the foam metal: coating the graphene silica gel prepolymer obtained in the step S2 on the surface of the foam metal plate, and drying to obtain a coated foam metal plate;
s5, preparing a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material: and (5) taking the oriented silica gel sheet in the step (S3) and the coated foam metal plate in the step (S4), and assembling and compounding the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet to obtain the high-heat-conductivity flexible interface material.
In the prior art, in order to increase the heat conductivity of silica gel, certain graphene is added into the silica gel
According to the technical scheme, firstly, graphene is processed through PSS to enable the graphene to be charged with negative charges, then the graphene with the negative charges is processed through cationic polyelectrolyte PDDA to enable the graphene to be combined with ammonium ions in the PDDA, and finally, ferroferric oxide particles with the negative charges are added into the graphene to enable the ferroferric oxide particles to be combined on the surface of graphite to obtain graphene coated with magnetic particles, the graphene is added into a silica gel prepolymer and then oriented through a magnetic field, and the graphene can be directionally arranged in silica gel sheets after being solidified; according to the method, magnetic nanoparticles are adopted to coat graphene, the orientation of the graphene on a silica gel matrix is accurately controlled by a magnetic field induction method, a graphene compound with ferroferric oxide particles covered on the surface is directionally arranged along the magnetic field direction in an end-to-end connection mode, and the compound shows strong anisotropy due to the two-dimensional planar structure of the graphene, so that the thermal conductivity of the compound in the axial direction is far higher than that in the parallel direction, under the condition of high directional arrangement, the dosage of a heat-conducting filler can be properly reduced under the condition of not reducing the heat-conducting efficiency of a silica gel sheet so as to improve the flexibility of a heat-conducting interface material, and the high thermal conductivity and the flexibility of the heat-conducting interface material are considered; meanwhile, in an end-to-end structure formed by orienting ferroferric oxide particles coated on the end part of graphene, a ferroferric oxide particle bridge for connecting two adjacent graphenes in a communication manner is formed under the traction action of charges on the graphene, so that the thermal stability of the silica gel sheet is improved, the directional arrangement of the graphene is not disturbed easily due to expansion in the silica gel sheet in overheating, and the service life of the heat dissipation material is prolonged.
Preferably, in step S1, the amount of the ferroferric oxide is 0.02% to 0.1% of the graphene content.
In the above aspect of the present invention, preferably, in step S3, the magnetic field strength is 0.5t to 6t.
Preferably, in step S3, the direction of the magnetic field is perpendicular to the plane of the metal foam plate or the plane of the mold.
Preferably, in the step S1, the mass ratio of the PSS to the graphene is 10% to 50%; the mass ratio of the PDDA to the graphene is 10-50%.
Preferably, in the above technical solution of the present invention, in step S2, the content of the magnetic particle-coated graphene is 5% to 25%.
Preferably, in the step S2, the viscosity of the vinyl-terminated polydimethylsiloxane ranges from 500 to 30000mPa.s, and the content of the vinyl-terminated polydimethylsiloxane ranges from 70% to 80%;
preferably, in the step S2, the viscosity of the methyl hydrogen silicone oil ranges from 50 to 600mPa.s, and the content of the methyl hydrogen silicone oil ranges from 0.4% to 8%;
preferably, in the step S2, the catalyst is selected from the group consisting of 0.03% to 0.8% of a platinum catalyst, and the effective concentration of platinum is 0.5% to 1.0%;
preferably, in the step S2, the inhibitor is preferably 1-ethynylcyclohexanol, and the content of the inhibitor is 0.05-1% of the sum of the mass of the vinyl-terminated polydimethylsiloxane and the mass of the methyl hydrogen silicone oil.
The invention also aims to provide a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material, which is prepared according to the preparation method of the foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material.
In the technical scheme, the vinyl-terminated polydimethylsiloxane and the methyl hydrogen-containing silicone oil are used as organic matrixes, the graphene coated with magnetic-field-oriented magnetic particles is used as a heat-conducting filler, the foam metal is used as a heat-conducting framework, and the foam metal/oriented graphene laminated composite structure heat-conducting interface material is prepared. The test result shows that the composite material maintains excellent flexibility and compressibility while having high thermal conductivity coefficient, and provides a feasible method for breaking through the technical bottleneck.
Preferably, in the above technical solution of the present invention, the material of the middle skeleton layer is selected from one of nickel foam, copper foam, titanium foam, cobalt foam, tungsten foam, molybdenum foam, chromium foam, iron nickel foam, and aluminum foam.
Preferably, in the above technical solution of the present invention, the thickness of the middle skeleton layer is 0.15 to 0.30mm.
Preferably, in the above technical solution of the present invention, the thickness of the heat conducting silica gel layer is 1.0 to 1.5mm.
Compared with the prior art, the invention has the beneficial effects that:
1. the heat-conducting interface material disclosed by the invention is formed by compounding a flexible foam metal serving as a heat-conducting framework and a heat-conducting silica gel sheet containing oriented graphene in a laminated manner, so that a multistage continuous heat-conducting passage is constructed, and the heat-conducting property of the material is effectively improved;
2. according to the method, magnetic nanoparticles are adopted to coat graphene, and the orientation of the graphene on a silica gel matrix is accurately controlled by using a magnetic field induction method, so that the vertical directional arrangement of the graphene is realized; by utilizing the ultrahigh heat conduction characteristic of the oriented graphene, the using amount of the heat conduction filler is further reduced, and the high heat conduction and flexibility of the heat conduction interface material are considered;
3. the heat-conducting interface material prepared by the invention has stable structure and longer service life;
4. the heat-conducting interface material with the foam metal/graphene laminated composite structure is prepared in situ by adopting a series of forming processes such as magnetic field orientation, coating, thermosetting forming and the like, and is simple in process, high in production efficiency, low in cost, green and environment-friendly.
Drawings
FIG. 1 is a schematic structural diagram of a thermal interface material according to the present invention;
in the figure, 1-middle framework layer, 2-heat-conducting silica gel and 21-graphene.
Detailed Description
The invention will now be further illustrated by the following examples, without limiting the scope of the invention thereto.
A preparation method of a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material comprises the following operation steps:
s1, preparing graphene coated by magnetic nanoparticles: dispersing a certain amount of graphene in deionized water, sequentially performing electrostatic adsorption treatment by using poly (4-sodium styrene sulfonate) (PSS) and poly (diallyldimethylammonium chloride) (PDDA) to obtain positive charge-coated graphene, then adding ferroferric oxide with negative charge, and reacting to obtain magnetic particle-coated graphene;
s2, preparing a graphene-containing silica gel prepolymer: weighing a proper amount of vinyl-terminated polydimethylsiloxane, methyl hydrogen-containing silicone oil, a catalyst, an inhibitor and the graphene coated with the magnetic particles prepared in the S1, mixing, and then stirring in vacuum to obtain a graphene silica gel prepolymer;
s3, preparing an oriented silica gel sheet: transferring the graphene silica gel prepolymer obtained in the step S2 into a mold, and carrying out magnetic field orientation until the graphene silica gel prepolymer is preliminarily cured; drying after primary curing to obtain an oriented silica gel sheet;
s4, coating a graphene silica gel prepolymer on the surface of the foam metal: coating the graphene silica gel prepolymer obtained in the step S2 on the surface of the foam metal plate, and drying to obtain a coated foam metal plate;
s5, preparing a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material: and (4) combining the oriented silica gel sheet in the step (S3) and the coated foam metal plate in the step (S4) according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet to obtain the high-heat-conductivity flexible interface material.
Wherein, step S1 includes the following steps:
step 1: weighing 5 to 25g of graphene and 0.8 to 7.5g of PSS poly (4-sodium styrene sulfonate) into a beaker, adding a proper amount of deionized water, and magnetically stirring for 30min;
and 2, step: ultrasonically dispersing the mixed solution prepared in the step 1 for 30min, and then putting the mixed solution into an oven to keep the temperature for 12h, wherein the temperature is set to 50 ℃;
and step 3: and (3) putting the mixed solution subjected to heat preservation in the step (2) into a high-speed centrifuge for high-speed centrifugation for 3 times, wherein the rotating speed is 12000r/min, and each time is 30min. After the centrifugation is finished, removing the supernatant to remove the PSS and reserving the lower solution;
and 4, step 4: adding 0.8-4.5 g of PDDA (poly diallyl dimethyl ammonium chloride) into the solution obtained in the step (3), adding a proper amount of deionized water, and magnetically stirring for 30min;
and 5: and (4) carrying out ultrasonic dispersion treatment on the mixed solution in the step (4) for 30min, and putting the mixed solution into a centrifuge for high-speed centrifugation for 3 times, wherein the rotating speed is 12000r/min, and each time is 30min. After the centrifugation is finished, removing supernatant, removing PDDA and reserving lower solution;
step 6: and (3) adding 0.005 to 0.25g of ferroferric oxide into the mixed solution in the step (5), and magnetically stirring for 30min to obtain the magnetic particle coated graphene.
The step S2 includes the steps of:
and 7: stirring in vacuum. Weighing a proper amount of vinyl-terminated polydimethylsiloxane, methyl hydrogen-containing silicone oil, a Kanstedt platinum catalyst and an inhibitor, and adding a proper amount of the magnetic particle-coated graphene prepared in the step (I) into the mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
the content of the magnetic particle-coated graphene is 5% -25%. The viscosity range of the vinyl-terminated polydimethylsiloxane is 500 to 30000mPa.s, and the content of the vinyl-terminated polydimethylsiloxane is 70 to 80 percent; the viscosity range of the methyl hydrogen-containing silicone oil is 50 to 600mPa.s, and the content is 0.4 to 8 percent; the catalyst is selected from a Kanst platinum catalyst, the content of the catalyst is 0.03-0.8%, and the effective concentration of platinum is 0.5-1.0%; the inhibitor is selected from 1-ethynylcyclohexanol, and the content of the inhibitor is 0.05-1% of the mass sum of the vinyl-terminated polydimethylsiloxane and the methyl hydrogen-containing silicone oil.
The step S3 includes the steps of:
and 8: the magnetic field is oriented. Transferring the graphene silica gel prepolymer obtained in the step S2 into a polytetrafluoroethylene mold, and carrying out magnetic field orientation in the direction vertical to the magnetic field of the mold, wherein the magnetic field intensity is 0.5T to 6T, and the orientation time is 12h until the graphene silica gel prepolymer is primarily cured;
and step 9: and (5) drying. Placing the graphene silica gel prepolymer prepared in the step 2 in an oven for drying, setting the temperature to be 85 ℃ and the time to be 6 hours, and obtaining a pre-cured magnetic graphene oriented silica gel sheet;
step S4 includes the following steps:
step 10: and (4) coating. Uniformly coating the graphene silica gel prepolymer prepared in the step S2 on the surface of the foam metal by adopting a coating process; the amount of the graphene silica gel prepolymer coated on the surface of the foam metal in the step is very small, so that when the foam metal and the silica gel sheet are subjected to thermosetting bonding in the step S5, a better adhesion effect can be obtained, and the obtained composite material has higher bonding strength.
Step 11: drying in an oven at a set temperature of 80 ℃ for 2h.
Step S5 includes the steps of:
step 12: taking the coated foam metal plate in the step 11 and the oriented silica gel sheet in the step 9, and assembling blanks according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet;
step 13: and (3) placing the blank obtained in the step (12) into a flat vulcanizing machine for thermosetting at the temperature of 155 ℃, under the pressure of 15MPa for 10min to obtain the high-thermal-conductivity flexible interface material with the foam metal/oriented graphene laminated composite structure.
Another object of the present invention is to provide a foam metal/oriented graphene laminated composite high thermal conductive flexible interface material, which is prepared according to the above preparation method, wherein the interface material includes a middle skeleton layer 1 and thermal conductive silica gel layers 2 disposed on the upper and lower surfaces of the middle skeleton layer, the thermal conductive silica gel layers are added with graphene 21, and at least some of the graphene molecules have the same orientation; the thickness of the middle framework layer is 0.15 to 0.30mm, and the thickness of the heat conduction silica gel layer is 1.0 to 1.5mm.
The material of the middle framework layer 1 is selected from one of foamed nickel, foamed copper, foamed titanium, foamed cobalt, foamed tungsten, foamed molybdenum, foamed chromium, foamed iron nickel and foamed aluminum; further, the flexible foam metal is foam copper or foam nickel. Wherein the porosity of the foam metal is 60% -80%, and the average pore diameter is 8 mu m-1 mm.
Example 1
A preparation method of a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material comprises the following steps:
preparation of (I) magnetic nanoparticle coated graphene
Step 1: weighing 5g of graphene and 0.8g of PSS (poly (sodium 4-styrenesulfonate)) into a beaker, adding a proper amount of deionized water, and magnetically stirring for 30min;
and 2, step: ultrasonically dispersing the mixed solution prepared in the step 1 for 30min, and then drying the mixed solution in an oven for 12h, wherein the temperature is set to 50 ℃;
and 3, step 3: and (3) putting the mixed solution dried in the step (2) into a high-speed centrifuge for high-speed centrifugation for 3 times, wherein the rotating speed is 12000r/min, and each time is 30min. After the centrifugation is finished, removing the supernatant, removing the PSS, and reserving the lower solution;
and 4, step 4: adding 0.8g of PDDA (poly diallyl dimethyl ammonium chloride) into the solution obtained in the step (3), adding a proper amount of deionized water, and magnetically stirring for 30min;
and 5: and (5) carrying out ultrasonic dispersion treatment on the mixed solution in the step (4) for 30min, and putting the mixed solution into a centrifuge for high-speed centrifugation for 3 times, wherein the rotating speed is 12000r/min, and each time is 30min. After the centrifugation is finished, removing the supernatant, removing PDDA, and keeping the lower solution;
step 6: and (5) adding 0.05g of ferroferric oxide into the mixed solution in the step (5), and magnetically stirring for 30min to obtain the magnetic particle coated graphene.
(II) preparation of heat-conducting silica gel sheet containing oriented graphene
Step 1: stirring in vacuum. 84g of vinyl-terminated polydimethylsiloxane, 6g of methyl hydrogen silicone oil, 0.80g of Kansted platinum catalyst and 0.63g of inhibitor were weighed, and 8g of the magnetic particle-coated graphene prepared above was added to the above mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
step 2: the magnetic field is oriented. Transferring the graphene silica gel prepolymer obtained in the step (1) into a polytetrafluoroethylene mold, and carrying out magnetic field orientation in a magnetic field with the direction vertical to the mold, wherein the magnetic field intensity is 2T, and the orientation time is 12h until the graphene silica gel prepolymer is preliminarily cured;
and step 3: and (5) drying. And (3) placing the whole device in the step (2) in an oven for drying, setting the temperature to be 85 ℃ and the time to be 6h, and obtaining the oriented silica gel sheet containing the oriented graphene.
(III) coating graphene silica gel prepolymer on surface of flexible foam copper
Step 1: stirring in vacuum. Weighing 84g of vinyl-terminated polydimethylsiloxane, 6g of methyl hydrogen silicone oil, 0.80g of Kanstedt platinum catalyst and 0.63g of inhibitor, adding 5g of the magnetic particle-coated graphene prepared in the step (I) into the mixture, and stirring in a planetary stirrer in vacuum for 1 hour to obtain a graphene silica gel prepolymer;
step 2: and (4) coating. Uniformly coating 5g of the graphene silica gel prepolymer prepared in the step 1 on the surface of the foam copper by adopting a coating process;
and step 3: and (5) drying. And (3) putting the material prepared in the step (2) into an oven for drying to obtain the coated foam metal plate. The temperature was set at 80 ℃ for 2h.
Preparation of heat-conducting interface material with (IV) foamy copper/oriented graphene laminated composite structure
Step 1: and (5) laminating and compounding. Taking a coated foam metal plate and an oriented silica gel sheet to form a blank according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet;
step 2: and (4) performing heat curing molding. Placing the blank obtained in the step 1 into a flat vulcanizing instrument for thermosetting at the temperature of 155 ℃ and the pressure of 15MPa for 10min to obtain the heat-conducting interface material with the foamy copper/oriented graphene laminated composite structure; the interface material comprises a middle framework layer 1 and heat conduction silica gel layers 2 arranged on the upper surface and the lower surface of the middle framework layer, wherein graphene 21 is added into the heat conduction silica gel layers, and at least part of graphene molecules are consistent in orientation; the thickness of the middle framework layer is 0.15mm, and the thickness of the heat-conducting silica gel layer is 1.0mm; the middle framework layer 1 is made of foam copper.
Example 2
Preparing magnetic nanoparticle coated graphene: same as example 1
(II) preparation of heat-conducting silica gel sheet containing oriented graphene
Step 1: stirring in vacuum. 80g of vinyl-terminated polydimethylsiloxane, 5g of methyl hydrogen silicone oil, 0.65g of Kansted platinum catalyst and 0.64g of inhibitor were weighed, and 15g of the magnetic particle-coated graphene prepared above was added to the mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
step 2: the magnetic field is oriented. Transferring the graphene silica gel prepolymer obtained in the step (1) into a polytetrafluoroethylene mold, and carrying out magnetic field orientation, wherein the magnetic field intensity is 3.5T, and the orientation time is 12h until the graphene silica gel prepolymer is preliminarily cured;
and step 3: and (5) drying. And (3) placing the whole device obtained in the step (2) in an oven for drying, setting the temperature to be 85 ℃ and the time to be 6h, and obtaining the heat-conducting silica gel sheet containing the oriented graphene.
(III) coating graphene silica gel prepolymer on surface of flexible foam copper
Step 1: stirring in vacuum. Weighing 80g of vinyl-terminated polydimethylsiloxane, 5g of methyl hydrogen silicone oil, 0.65g of Karsted platinum catalyst and 0.64g of inhibitor, and adding 15g of the magnetic particle-coated graphene prepared in the step (I) into the mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
step 2: and (4) coating. Uniformly coating 5g of the graphene silica gel prepolymer prepared in the step 1 on the surface of the foam copper by adopting a coating process;
and step 3: and (5) drying. And (3) putting the material prepared in the step (2) into an oven for drying. The temperature was set at 80 ℃ for 2h.
Preparation of heat-conducting interface material with (four) foamy copper/oriented graphene laminated composite structure
Step 1: and (5) laminating and compounding. Taking a coated foam metal plate and an oriented silica gel sheet to form a blank according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet;
step 2: and (5) thermosetting and forming. Placing the blank obtained in the step 1 into a flat vulcanizing instrument for thermosetting at the temperature of 155 ℃ and the pressure of 15MPa for 10min to obtain a heat-conducting interface material with a foamy copper/oriented graphene laminated composite structure; the interface material comprises a middle framework layer 1 and heat conduction silica gel layers 2 arranged on the upper surface and the lower surface of the middle framework layer, wherein graphene 21 is added into the heat conduction silica gel layers, and at least part of graphene molecules are consistent in orientation; the thickness of the middle framework layer is 0.15mm, and the thickness of the heat-conducting silica gel layer is 1.0mm; the middle framework layer 1 is made of foam copper.
Example 3
Preparing magnetic nanoparticle coated graphene: same as example 1
(II) preparing a heat-conducting silica gel sheet containing oriented graphene
Step 1: stirring in vacuum. 76g of vinyl-terminated polydimethylsiloxane, 4.5g of methyl hydrogen silicone oil, 0.70g of Kansted platinum catalyst and 0.68g of inhibitor were weighed, and 20g of the magnetic particle-coated graphene prepared above was added to the mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
and 2, step: the magnetic field is oriented. And (3) transferring the graphene silica gel prepolymer obtained in the step (1) into a polytetrafluoroethylene mold, and carrying out magnetic field orientation. The magnetic field intensity is 5T, the orientation time is 12h, and the graphene silica gel prepolymer is primarily cured;
and step 3: and (5) drying. And (3) placing the whole device in the step (2) in an oven for drying, setting the temperature to be 85 ℃ and the time to be 6h, and obtaining the heat-conducting silica gel sheet containing the oriented graphene.
(III) foam copper surface coating graphene silica gel prepolymer
Step 1: stirring in vacuum. 76g of vinyl-terminated polydimethylsiloxane, 4.5g of methyl hydrogen silicone oil, 0.70g of Kansted platinum catalyst and 0.68g of inhibitor were weighed, and 20g of the magnetic particle-coated graphene prepared in step (one) was added to the above mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
step 2: and (4) coating. Uniformly coating 5g of the graphene silica gel prepolymer prepared in the step 1 on the surface of the foam copper by adopting a coating process;
and 3, step 3: and (5) drying. And (3) putting the material prepared in the step (2) into an oven for drying. The temperature was set at 80 ℃ for 2h.
Preparation of heat-conducting interface material with (IV) foamy copper/oriented graphene laminated composite structure
Step 1: and (5) laminating and compounding. Taking a coated foam metal plate and an oriented silica gel sheet to form a blank according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet;
and 2, step: and (4) performing heat curing molding. Placing the blank obtained in the step 1 into a flat vulcanizing instrument for thermosetting at the temperature of 155 ℃ and the pressure of 15MPa for 10min to obtain a heat-conducting interface material with a foamy copper/oriented graphene laminated composite structure; the interface material comprises a middle framework layer 1 and heat conduction silica gel layers 2 arranged on the upper surface and the lower surface of the middle framework layer, wherein graphene 21 is added into the heat conduction silica gel layers, and at least part of graphene molecules are consistent in orientation; the thickness of the middle framework layer is 0.15mm, and the thickness of the heat-conducting silica gel layer is 1.0mm; the middle framework layer 1 is made of foam copper.
Example 4
Preparing magnetic nanoparticle coated graphene: same as example 1
(II) preparation of heat-conducting silica gel sheet containing oriented graphene
Step 1: stirring in vacuum. 70g of vinyl terminated polydimethylsiloxane, 4g of methyl hydrogen silicone oil, 0.64g of Kansted platinum catalyst and 0.60g of inhibitor were weighed, and 25g of the magnetic particle-coated graphene prepared above was added to the above mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
and 2, step: the magnetic field is oriented. And (3) transferring the graphene silica gel prepolymer obtained in the step (1) into a polytetrafluoroethylene mold, and carrying out magnetic field orientation. The magnetic field intensity is 6T, the orientation time is 12h, and the graphene silica gel prepolymer is initially cured;
and 3, step 3: and (5) drying. And (3) placing the whole device obtained in the step (2) in an oven for drying, setting the temperature to be 85 ℃ and the time to be 6h, and obtaining the heat-conducting silica gel sheet containing the oriented graphene.
(III) foam copper surface coating graphene silica gel prepolymer
Step 1: stirring in vacuum. Weighing 70g of vinyl-terminated polydimethylsiloxane, 4g of methyl hydrogen silicone oil, 0.64g of Kansted platinum catalyst and 0.60g of inhibitor, and adding 25g of the magnetic particle-coated graphene prepared in the step (one) into the mixture. Stirring in a planetary stirrer for 1h in vacuum to obtain a graphene silica gel prepolymer;
and 2, step: and (4) coating. Uniformly coating 5g of the graphene silica gel prepolymer prepared in the step 1 on the surface of the foam copper by adopting a coating process;
and 3, step 3: and (5) drying. And (3) putting the material prepared in the step (2) into an oven for drying. The temperature was set at 80 ℃ for 2h.
Preparation of heat-conducting interface material with (IV) foamy copper/oriented graphene laminated composite structure
Step 1: and (5) laminating and compounding. Taking a coated foam metal plate and an oriented silica gel sheet to form a blank according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet;
step 2: and (4) performing heat curing molding. Placing the blank obtained in the step 1 into a flat vulcanizing instrument for thermosetting at the temperature of 155 ℃ and the pressure of 15MPa for 10min to obtain the heat-conducting interface material with the foamy copper/oriented graphene laminated composite structure; the interface material comprises a middle framework layer 1 and heat conduction silica gel layers 2 arranged on the upper surface and the lower surface of the middle framework layer, wherein graphene 21 is added into the heat conduction silica gel layers, and at least part of graphene molecules are consistent in orientation; the thickness of the middle framework layer is 0.15mm, and the thickness of the heat-conducting silica gel layer is 1.0mm; the middle framework layer 1 is made of foam copper.
Comparative example
Compared to example 3, the conditions were kept unchanged except that the magnetic-particle-coated graphene in step (two) was not subjected to magnetic field orientation.
The inventors conducted the following tests for the above examples 1 to 4 and comparative examples:
the heat conductivity is measured by adopting a heat conduction instrument adopting a protective hot plate method, the test adopts the ASTM D5470 standard, the test sample is a round sample with the thickness of 3mm and the diameter of 100mm, the test is repeated for three times, and the average value is taken.
The density test adopts a balance method to measure, the test adopts GB4472-84 standard, the sample is a square sample with the thickness of 3mm and the side length of 50mm, the test is repeated for three times, and the average value is taken.
The shore hardness test adopts a shore hardness meter, the test adopts an ASTM D2240 standard, the test sample is a square sample with the thickness of 5mm and the side length of 50mm, the test is repeated for three times, and an average value is taken.
The breakdown voltage is measured by an electrical strength tester, the test adopts the ASTM D149 standard, and the test sample is a circular sample with the thickness of 1mm and the diameter of 25 mm. And measuring 8 to 10 test points and taking an average value.
The test results were as follows:
compared with the embodiment 1, the content and the magnetic field strength of the magnetic particle coated graphene are improved, and the high heat conduction characteristic of the oriented graphene is benefited, so that according to analysis of test results, compared with the embodiment 1, the prepared composite material has the advantages that the heat conduction coefficient is improved, the hardness is improved, but the breakdown voltage is reduced, which is influenced by the electric conductivity of the graphene and the foam copper;
example 3 compared to example 2, the content of the magnetic particle-coated graphene and the magnetic field strength were continuously increased. According to the analysis of the test result, the thermal conductivity and the hardness are further improved, but the breakdown voltage is further reduced;
example 4 the content of the magnetic particle-coated graphene and the magnetic field strength were continuously increased as compared with example 3. According to the analysis of the test result, the thermal conductivity coefficient is reduced, and the inventor analyzes that the content of the graphene coated by the magnetic particles is too high, so that the graphene can not be completely oriented by a magnetic field; in addition, excessive magnetic particle coated graphene is difficult to disperse in an organic matrix and easy to agglomerate, and the adverse factors influence the heat conduction performance of the composite material. On the other hand, in example 4, the hardness was further improved and the breakdown voltage was reduced as compared with example 3.
Comparative example compared to example 3, non-oriented magnetic particle coated graphene was used as the thermally conductive filler, and the remaining conditions were maintained. And analyzing according to the test result. Compared with the embodiment 3, the thermal conductivity of the prepared composite material is greatly reduced, because the non-oriented magnetic particle coated graphene cannot construct a thermal conduction path in the vertical direction, the thermal conduction performance of the composite material is reduced, and meanwhile, the thermal conductivity of the composite material prepared by the comparative embodiment is far lower than that of other embodiments, further proving that the magnetic field oriented magnetic particle coated graphene can effectively construct a thermal conduction path in an organic matrix and forms a good synergistic effect with the copper foam.
The above description is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, any modification, equivalence, replacement and improvement, etc. related to the filler proportion and processing method of the present invention are included in the protection scope of the present invention without departing from the principle of the present invention.
Claims (10)
1. A preparation method of a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material comprises the following operation steps:
s1, preparing graphene coated with magnetic nanoparticles: dispersing a certain amount of graphene in deionized water, sequentially performing electrostatic adsorption treatment by using poly (4-sodium styrene sulfonate) (PSS) and poly (diallyldimethylammonium chloride) (PDDA) to obtain positive charge-coated graphene, and then adding negatively charged ferroferric oxide for reaction to obtain magnetic particle-coated graphene;
s2, preparing a graphene-containing silica gel prepolymer: weighing a proper amount of vinyl-terminated polydimethylsiloxane, methyl hydrogen-containing silicone oil, a catalyst, an inhibitor and the graphene coated with the magnetic particles prepared in the step S1, mixing, and then stirring in vacuum to obtain a graphene silica gel prepolymer;
s3, preparing an oriented silica gel sheet: transferring the graphene silica gel prepolymer obtained in the step S2 into a mold, and performing magnetic field orientation until the graphene silica gel prepolymer is primarily cured; drying after primary curing to obtain an oriented silica gel sheet;
s4, coating a graphene silica gel prepolymer on the surface of the foam metal: coating the graphene silica gel prepolymer obtained in the step S2 on the surface of the foam metal plate, and drying to obtain a coated foam metal plate;
s5, preparing a foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material: and (5) taking the oriented silica gel sheet in the step (S3) and the coated foam metal plate in the step (S4), and assembling and compounding the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet according to the structure of the oriented silica gel sheet/the coated foam metal plate/the oriented silica gel sheet to obtain the high-heat-conductivity flexible interface material.
2. The preparation method of the foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material according to claim 1, wherein in the step S1, the dosage of ferroferric oxide is 0.02% -0.1% of the graphene content.
3. The method for preparing the foamed metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material according to claim 1, wherein in the step S3, the magnetic field strength is 0.5T to 6T.
4. The method for preparing a foam metal/oriented graphene laminated composite high thermal conductivity flexible interface material according to claim 1, wherein in step S3, the direction of the magnetic field is perpendicular to the mold plane.
5. The preparation method of the foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material according to claim 1, wherein in the step S1, the mass ratio of the PSS to the graphene is 10% -50%; the mass ratio of the PDDA to the graphene is 10-50%.
6. The method for preparing the foam metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material according to claim 1, wherein in the step S2, the content of the magnetic particle-coated graphene is 5% to 25%.
7. A foamed metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material is characterized by being prepared according to the preparation method of the foamed metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material in any one of claims 1 to 6, wherein the interface material comprises a middle framework layer and thermal-conductivity silica gel layers arranged on the upper surface and the lower surface of the middle framework layer, graphene is added into the thermal-conductivity silica gel layers, and at least part of the graphene is oriented by an external magnetic field and then is directionally arranged.
8. The method for preparing a metal foam/oriented graphene laminated composite high thermal conductivity flexible interface material according to claim 7, wherein the material of the middle skeleton layer is selected from one of nickel foam, copper foam, titanium foam, cobalt foam, tungsten foam, molybdenum foam, chromium foam, iron nickel foam and aluminum foam.
9. The method for preparing the foamed metal/oriented graphene laminated composite high-thermal-conductivity flexible interface material according to claim 7, wherein the thickness of the middle skeleton layer is 0.15-0.30mm.
10. The method for preparing the high-thermal-conductivity flexible interface material laminated and compounded by the foamed metal and the oriented graphene according to claim 7, wherein the thickness of the thermal-conductivity silica gel layer is 1.0-1.5 mm.
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