CN111572119A - Thermal interface material and preparation method thereof - Google Patents
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Abstract
The invention provides a thermal interface material and a preparation method thereof, wherein the preparation method comprises the following steps: preparing a carbon nano tube film by adopting a floating catalysis method; preparing a nano-scale silicon dioxide powder and graphene oxide mixed dispersion solution; uniformly distributing the mixed dispersion solution on the surface of a layer of carbon nanotube film by adopting a spraying method, covering a layer of carbon nanotube film, and repeatedly spraying until a set number of layers is reached to form a carbon nanotube-nano silicon dioxide-graphene oxide composite film; and carrying out rapid thermal treatment on the composite film in an inert protective atmosphere, reducing graphene oxide into graphene, generating silicon carbide nanowires by using a carbothermic reduction reaction, and forming a three-dimensional network structure between the carbon nanotubes and the graphene to form the carbon nanotube-graphene-silicon carbide nanowire composite film. The thermal interface material and the preparation method thereof improve the compressibility and the thermal conductivity.
Description
Technical Field
The invention relates to the technical field of thermal interface materials, in particular to a thermal interface material for manufacturing a thermal interface material by adopting a carbon nano tube and a silicon carbide nano wire and a preparation method thereof.
Background
In recent years, with the continuous improvement of the integration level of electronic devices and intelligent terminals, the heat dissipation problem becomes one of the key factors restricting the performance of the devices and the terminals, and under the background, the important academic and engineering concept of 'heat management materials and technologies' is created, and the thermal interface material is a hot point direction of the recent development of the heat management material, particularly under the condition of rapid development of the 5G technology, the high-performance thermal interface material with higher heat conductivity coefficient has important application value and potential.
The conventional thermal interface material mainly includes thermal grease, thermal silica gel, heat sink, phase change material, phase change metal, and thermal adhesive (curing type). Of these materials, the most thermally conductive is a phase change metal sheet, such as a pure indium sheet, an indium/silver alloy sheet, a tin/silver/copper alloy sheet, an indium/tin/bismuth alloy sheet. However, the phase change metal sheet is completely melted during use, and voids are generated, which seriously affect the stability of the thermal interface material. Therefore, a more mature and stable thermal interface material with a higher thermal conductivity is sought.
The carbon nanotube material is a thermal interface material with development prospect developed in recent years, has certain directionality and compressibility for a carbon nanotube film prepared by a spinning method, has better thermal diffusion performance in the film according to the spinning direction, and has more advantages compared with other materials. However, the biggest problem of the spun carbon nanotube film material is that the longitudinal thermal conductivity is not superior.
In recent years, the excellent heat-conducting property of the silicon carbide quasi-one-dimensional nano material is gradually developed and has practical application value. The carbon nano tube and the silicon carbide nano wire (quasi-one-dimensional material) are combined, namely, the carbon nano tube-silicon carbide nano wire composite heat conduction material is generated in situ on the basis of the carbon nano tube film, and the silicon carbide nano wire and the carbon nano tube are combined with excellent heat conduction performance to form a good thermal interface material with a three-dimensional heat conduction structure, so that the carbon nano tube-silicon carbide nano wire composite heat conduction material has an excellent development prospect.
The statements in the background section are merely prior art as they are known to the inventors and do not, of course, represent prior art in the field.
Disclosure of Invention
To address one or more of the problems of the prior art, the present invention provides a method for preparing a thermal interface material, comprising:
preparing a carbon nano tube film by adopting a floating catalysis method;
preparing a nano-scale silicon dioxide powder and graphene oxide mixed dispersion solution;
uniformly distributing the mixed dispersion solution of nanoscale silicon dioxide powder and graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, covering a layer of carbon nanotube film, and repeatedly spraying the mixed dispersion solution of nanoscale silicon dioxide powder and graphene oxide until a set number of layers is reached to form a carbon nanotube-nanosilicon dioxide-graphene oxide composite film, wherein a nanosilicon dioxide and graphene oxide coating 2 is sprayed between two layers of carbon nanotube films 1 as shown in figure 1;
performing rapid thermal treatment on the carbon nanotube-nanosilicon dioxide-graphene oxide composite film in an inert protective atmosphere, reducing graphene oxide into graphene, generating a silicon carbide nanowire by using a carbothermic reduction reaction, forming a three-dimensional network structure between the carbon nanotube and the graphene to form the carbon nanotube-graphene-silicon carbide nanowire composite film, wherein the internal structure of the carbon nanotube-nanosilicon dioxide-graphene oxide before thermal treatment is shown in fig. 2, and the three-dimensional network structure of the carbon nanotube-graphene-silicon carbide nanowire formed after thermal treatment is shown in fig. 3.
Preferably, the step of preparing the carbon nanotube film by using a floating catalyst method comprises:
preparing a carbon source/catalyst solution: dissolving a catalyst and a promoter in a carbon source solvent, wherein the content of the catalyst is 0.1-5 wt%, preferably 2 wt%, and the content of the promoter is 0.1-5 wt%, preferably 1 wt%;
heating the reaction cavity to 1000-1300 ℃, preferably 1200 ℃; then introducing inert carrier gas, wherein the flow rate of the introduced mixed gas is 1-30L/min, preferably 10L/min; injecting a carbon source/catalyst solution into the reaction cavity at a rate of 10-40mL/h and 20 mL/h; preferably, the inert carrier is argon and hydrogen (Ar/H)2) And the volume ratio of argon gas to hydrogen gas is 10: (8-10), further, preferably, the volume ratio of argon gas to hydrogen gas is 10: 10;
the carbon nano tube film is driven by inert carrier gas to float out of the tube tail, and is continuously rolled into a film through a collecting roller
Preferably, the carbon source solvent is absolute ethyl alcohol, ethylene glycol, methanol or benzyl alcohol, the catalyst is ferrocene, and the promoter is thiophene.
Preferably, the step of preparing the mixed dispersion solution of nano-scale silica powder and graphene oxide includes:
adding nanoscale silicon dioxide powder and graphene oxide powder into a solvent, adding a dispersing agent, stirring and mixing uniformly, wherein the size of the nanoscale silicon dioxide powder is 1-100 nanometers, and preferably 1-5 nanometers; the size of the graphene oxide material sheet layer is 1-100 micrometers, preferably 2-5 micrometers;
stirring and dispersing by using water and/or N-methyl pyrrolidone (NMP) and absolute ethyl alcohol as solvents and one or more of polyvinylpyrrolidone (PVP), polyvinyl alcohol (PVA), Sodium Dodecyl Sulfate (SDS), Sodium Dodecyl Benzene Sulfonate (SDBS) and carboxymethyl cellulose (CMC) as dispersing agents;
in the mixed dispersion liquid, the mass concentration of graphene in the mixed dispersion liquid is 1-50 wt%, preferably 35 wt%; the mass concentration of the nano-scale silicon dioxide in the mixed dispersion liquid is 1-10 wt%, preferably 5 wt%; the mass concentration of the dispersant is 0.1-5 wt%, preferably 1-2 wt%.
Preferably, the forming step of the carbon nanotube-nanosilicon dioxide-graphene oxide composite film comprises:
spraying the nano-scale silicon dioxide and graphene oxide dispersion liquid on the surface of the carbon nanotube film by adopting spraying equipment, wherein the average spraying thickness of the surface of the carbon nanotube film is 1-100 micrometers, and preferably 30-50 micrometers;
covering a layer of carbon nanotube film to form a carbon nanotube film/nano-scale silicon dioxide-graphene oxide/carbon nanotube film composite structure;
repeating the two steps to form a multi-layer carbon nanotube film/nano-scale silicon dioxide-graphene oxide/carbon nanotube film laminated structure.
Preferably, the step of performing rapid thermal treatment on the carbon nanotube-nanosilicon dioxide-graphene oxide composite film in an inert protective atmosphere includes:
putting the coiled carbon nanotube-nano silicon dioxide-graphene oxide composite film prepared by spraying and compounding into a vacuum heat treatment furnace;
vacuumizing the vacuum heat treatment furnace, introducing argon protective gas after the background vacuum degree reaches 3Pa, heating to 1400-1600 ℃, preferably 1500 ℃, and carrying out heat treatment, wherein the heat preservation time is 30-180min, preferably 100-120min, and the argon introduction rate is 800ml/min, preferably 200-400ml/min during heat preservation;
after the treatment in the high-temperature heat preservation stage is finished, the temperature of the heat treatment furnace is reduced to 150-; the cooling rate is 3-10 ℃/min, preferably 4-5 ℃/min;
and taking out the carbon nano tube-graphene-silicon carbide nanowire composite film obtained after the heat treatment.
Preferably, the method further comprises the following steps: and (3) carrying out rolling and shaping treatment on the carbon nano tube-graphene-silicon carbide nanowire composite film.
Further, it is preferable that the rolling pressure in the rolling setting treatment is 0.2 to 2MPa, preferably 0.2 to 0.7 MPa.
In addition, preferably, the longitudinal thermal conductivity of the rolled and shaped carbon nanotube-graphene-silicon carbide nanowire composite film is 5-50W/m.K according to different process conditions.
According to another aspect of the present invention, there is provided a thermal interface material comprising a plurality of units, each unit comprising two carbon nanotube films and a thermally reduced graphene nanoplatelet and a silicon carbide nanowire sandwiched between the two carbon nanotube films.
According to the thermal interface material based on the carbon nanotube film-silicon carbide nanowire composite structure and the preparation method thereof, the carbon nanotube-graphene-silicon carbide composite structure film is used as the thermal interface material for the first time, the characteristic of high transverse thermal conductivity coefficient of the carbon nanotube and the graphene is utilized, and the silicon carbide nanowires generated by in-situ carbothermic reduction are combined to be communicated into the three-dimensional thermal conductivity structure, so that the thermal interface material with excellent transverse and longitudinal thermal conductivity coefficients is formed, the technical requirements of electronic equipment on the thermal interface material can be met, and the comprehensive performance of an integrated electronic device is improved.
The thermal interface material is a carbon nano tube-graphene-silicon carbide three-dimensional composite heat-conducting film, has more internal pores, and is used as the thermal interface material, so that better compressibility is ensured;
drawings
FIG. 1 is a schematic cross-sectional structure of a carbon nanotube-nanosilica-graphene oxide composite film according to the present invention;
FIG. 2 is a schematic diagram of the internal structure of the carbon nanotube-nanosilica-graphene oxide of the present invention,
FIG. 3 is a schematic diagram of a three-dimensional network structure of a carbon nanotube-graphene-silicon carbide nanowire formed after heat treatment according to the present invention;
FIG. 4 is a schematic view of a process flow of the carbon nanotube-graphene-silicon carbide nanowire composite film according to the present invention;
the preparation method comprises the following steps of 1-carbon nanotube film, 2-nano silicon dioxide and graphene oxide coating, 201-graphene oxide, 202-nano silicon dioxide, 203-silicon carbide nanowire and 204-thermally reduced graphene microchip.
Detailed Description
In the following, only certain exemplary embodiments are briefly described. As those skilled in the art will recognize, the described embodiments may be modified in various different ways, all without departing from the spirit or scope of the present invention. Accordingly, the drawings and description are to be regarded as illustrative in nature, and not as restrictive.
The first embodiment is as follows:
a preparation method of a carbon nanotube-graphene-silicon carbide composite thermal interface material is shown in figure 4, wherein A-E is a process flow, namely, a layer of nanoscale silicon oxide and graphene oxide coating is compounded on a single-layer carbon nanotube film, and then the process is repeated until a multi-layer composite carbon nanotube film is formed. The method specifically comprises the following steps:
1) preparing a carbon nanotube film by a floating catalysis method, and rolling the carbon nanotube film, wherein the rolling length is 200m, and the average thickness of a layer of carbon nanotube film on a rolling shaft is 2 microns;
2) preparing a nano silicon dioxide and graphene oxide mixed dispersion solution, wherein the mass concentration of graphene is 25 wt%, and the mass concentration of nano silicon dioxide is 5 wt%; adopting water as a solvent, Sodium Dodecyl Benzene Sulfonate (SDBS) as a dispersant with the mass concentration of 2 wt%, and stirring for dispersion;
3) uniformly coating the mixed dispersion solution of nano silicon dioxide and graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, and then covering a layer of carbon nanotube film; repeatedly spraying the nano silicon dioxide and graphene oxide mixed dispersion solution, and repeatedly covering a carbon nanotube film, wherein the carbon nanotube film is 4 layers;
4) in an argon protective atmosphere, carrying out heat treatment on the carbon nanotube film/nano silicon dioxide-graphene oxide/carbon nanotube film, wherein the heat treatment conditions are as follows: the temperature is 1500 ℃, and the heat preservation time is 120 min;
5) performing rolling and shaping treatment on the carbon nanotube film/silicon carbide-graphene/carbon nanotube film obtained after the heat treatment, wherein the rolling pressure is 0.5 MPa;
the final product forms a composite structure of 4 layers of carbon nanotube films and 3 layers of silicon carbide-graphene, and the longitudinal thermal conductivity coefficient of the composite structure is 22W/m.K.
Example two:
a preparation method of a carbon nanotube-graphene-silicon carbide composite thermal interface material is shown in figure 4, wherein A-E is a process flow, namely, a layer of nanoscale silicon oxide and graphene oxide coating is compounded on a single-layer carbon nanotube film, and then the process is repeated until a multi-layer composite carbon nanotube film is formed. The method specifically comprises the following steps:
1) preparing a carbon nanotube film by a floating catalysis method, and rolling the carbon nanotube film, wherein the rolling length is 200m, and the average thickness of a layer of carbon nanotube film on a rolling shaft is 2 microns;
2) preparing a nano silicon dioxide and graphene oxide mixed dispersion solution, wherein the mass concentration of graphene is 30 wt%, and the mass concentration of nano silicon dioxide is 5 wt%; NMP is used as a solvent, Sodium Dodecyl Benzene Sulfonate (SDBS) is used as a dispersing agent, the concentration of the dispersing agent is 2 wt%, and the dispersing agent is stirred and dispersed;
3) uniformly coating the mixed dispersion solution of nano silicon dioxide and graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, and then covering a layer of carbon nanotube film; repeatedly spraying the nano silicon dioxide and graphene oxide mixed dispersion solution, and repeatedly covering a carbon nanotube film, wherein the carbon nanotube film reaches 5 layers;
4) in an argon protective atmosphere, carrying out heat treatment on the carbon nanotube film/nano silicon dioxide-graphene oxide/carbon nanotube film, wherein the heat treatment conditions are as follows: the temperature is 1500 ℃, and the heat preservation time is 120 min;
5) performing rolling and shaping treatment on the carbon nanotube film/silicon carbide-graphene/carbon nanotube film obtained after the heat treatment, wherein the rolling pressure is 0.7 MPa;
the final product forms a composite structure of 5 layers of carbon nanotube films and 4 layers of silicon carbide-graphene, and the longitudinal thermal conductivity coefficient of the composite structure is 28W/m.K.
Example three:
a preparation method of a carbon nanotube-graphene-silicon carbide composite thermal interface material is shown in figure 4, wherein A-E is a process flow, namely, a layer of nanoscale silicon oxide and graphene oxide coating is compounded on a single-layer carbon nanotube film, and then the process is repeated until a multi-layer composite carbon nanotube film is formed. The method specifically comprises the following steps:
1) preparing a carbon nanotube film by a floating catalysis method, and rolling the carbon nanotube film, wherein the rolling length is 200m, and the average thickness of a layer of carbon nanotube film on a rolling shaft is 2 microns;
2) preparing a nano silicon dioxide and graphene oxide mixed dispersion solution, wherein the mass concentration of graphene is 20 wt%, and the mass concentration of nano silicon dioxide is 3 wt%; water and NMP (mass concentration ratio is 10: 1) are used as solvents, Sodium Dodecyl Sulfate (SDS) is used as a dispersant, the concentration of the dispersant is 1 wt%, and the mixture is stirred and dispersed;
3) uniformly coating the mixed dispersion solution of nano silicon dioxide and graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, and then covering a layer of carbon nanotube film; repeatedly spraying the nano silicon dioxide and graphene oxide mixed dispersion solution, and repeatedly covering a carbon nanotube film, wherein the carbon nanotube film is 4 layers;
4) in an argon protective atmosphere, carrying out heat treatment on the carbon nanotube film/nano silicon dioxide-graphene oxide/carbon nanotube film, wherein the heat treatment conditions are as follows: the temperature is 1500 ℃, and the heat preservation time is 120 min;
5) performing rolling and shaping treatment on the carbon nanotube film/silicon carbide-graphene/carbon nanotube film obtained after the heat treatment, wherein the rolling pressure is 0.3 MPa;
the final product forms a composite structure of 4 layers of carbon nanotube films and 3 layers of silicon carbide-graphene, and the longitudinal thermal conductivity coefficient of the composite structure is 19W/m.K.
Example four:
a preparation method of a carbon nanotube-graphene-silicon carbide composite thermal interface material is shown in figure 4, wherein A-E is a process flow, namely, a layer of nanoscale silicon oxide and graphene oxide coating is compounded on a single-layer carbon nanotube film, and then the process is repeated until a multi-layer composite carbon nanotube film is formed. The method specifically comprises the following steps:
1) preparing a carbon nanotube film by a floating catalysis method, and rolling the carbon nanotube film, wherein the rolling length is 200m, and the average thickness of a layer of carbon nanotube film on a rolling shaft is 2 microns;
2) preparing a nano silicon dioxide and graphene oxide mixed dispersion solution, wherein the mass concentration of graphene is 30 wt%, and the mass concentration of nano silicon dioxide is 5 wt%; water and NMP (mass concentration ratio is 10: 1) are used as solvents, Sodium Dodecyl Sulfate (SDS) is used as a dispersant, the concentration of the dispersant is 1.5 wt%, and the mixture is stirred and dispersed;
3) uniformly coating the mixed dispersion solution of nano silicon dioxide and graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, and then covering a layer of carbon nanotube film; repeatedly spraying the nano silicon dioxide and graphene oxide mixed dispersion solution, and repeatedly covering a carbon nanotube film, wherein the carbon nanotube film reaches 5 layers;
4) in an argon protective atmosphere, carrying out heat treatment on the carbon nanotube film/nano silicon dioxide-graphene oxide/carbon nanotube film, wherein the heat treatment conditions are as follows: the temperature is 1500 ℃, and the heat preservation time is 120 min;
5) performing rolling and shaping treatment on the carbon nanotube film/silicon carbide-graphene/carbon nanotube film obtained after the heat treatment, wherein the rolling pressure is 0.7 MPa;
the final product forms a composite structure of 5 layers of carbon nanotube films and 4 layers of silicon carbide-graphene, and the longitudinal thermal conductivity coefficient of the composite structure is 26W/m.K.
Comparative example one:
1) preparing a carbon nanotube film by a floating catalysis method, and rolling the carbon nanotube film, wherein the rolling length is 200m, and the average thickness of a layer of carbon nanotube film on a rolling shaft is 2 microns;
2) preparing a graphene oxide mixed dispersion solution, wherein the mass concentration of graphene is 25 wt%, adopting an aqueous solvent and Sodium Dodecyl Sulfate (SDS) as a dispersant, the concentration of the dispersant is 1 wt%, and stirring for dispersion;
3) uniformly coating the graphene oxide mixed dispersion solution on the surface of a layer of carbon nanotube film by adopting a spraying method, and then covering a layer of carbon nanotube film; repeating the graphene oxide mixed dispersion solution, and repeatedly covering the carbon nanotube film, wherein the carbon nanotube film has 5 layers;
4) and (2) carrying out heat treatment on the carbon nanotube film/graphene oxide/carbon nanotube film in an argon protective atmosphere, wherein the heat treatment conditions are as follows: the temperature is 1500 ℃, and the heat preservation time is 120 min;
5) performing rolling and shaping treatment on the carbon nanotube film/graphene/carbon nanotube film obtained after the heat treatment, wherein the rolling pressure is 0.7 MPa;
the final product forms a composite structure of 5 layers of carbon nanotube films and 4 layers of graphene, and the longitudinal thermal conductivity coefficient of the composite structure is 5W/m.K.
The thermal interface materials of examples one to four and comparative example one were evaluated as follows:
the longitudinal thermal conductivity is measured by adopting a steady-state heat flow method, the transverse thermal conductivity is measured by adopting a laser flash method, and the detection is carried out by specifically referring to a carbon material thermal conductivity determination method (GB/T8722-2019).
Serial number | Sample (I) | Longitudinal thermal conductivity (W/m. K) | Transverse coefficient of thermal conductivity (W/m. K) |
1 | Example 1 | 22 | 500 |
2 | Example 2 | 28 | 560 |
3 | Example 3 | 19 | 440 |
4 | Example 4 | 26 | 530 |
5 | Comparative example 1 | 5 | 380 |
As can be seen from the above table, the thermal interface material of the invention has a longitudinal thermal conductivity of more than 18W/mK and a transverse thermal conductivity of more than 400W/mK, and has better performance compared with the common thermal interface material.
Finally, it should be noted that: although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that changes may be made in the embodiments and/or equivalents thereof without departing from the spirit and scope of the invention. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A method of making a thermal interface material, comprising:
preparing a carbon nano tube film by adopting a floating catalysis method;
preparing a nano-scale silicon dioxide powder and graphene oxide mixed dispersion solution;
uniformly distributing the mixed dispersion solution of the nano-scale silicon dioxide powder and the graphene oxide on the surface of a layer of carbon nanotube film by adopting a spraying method, covering a layer of carbon nanotube film, and repeatedly spraying the mixed dispersion solution of the nano-scale silicon dioxide powder and the graphene oxide until a set number of layers is reached to form a carbon nanotube-nano silicon dioxide-graphene oxide composite film;
and carrying out rapid thermal treatment on the carbon nanotube-nano silicon dioxide-graphene oxide composite film in an inert protective atmosphere, reducing graphene oxide into graphene, generating silicon carbide nanowires by utilizing a carbothermic reduction reaction, and forming a three-dimensional network structure between the carbon nanotube and the graphene to form the carbon nanotube-graphene-silicon carbide nanowire composite film.
2. The method for preparing a thermal interface material according to claim 1, wherein the step of preparing the carbon nanotube film by using a floating catalyst method comprises:
preparing a carbon source/catalyst solution: dissolving a catalyst and a promoter in a carbon source solvent, wherein the content of the catalyst is 0.1-5 wt%, and the content of the promoter is 0.1-5 wt%;
heating the reaction cavity to the high temperature of 1000-1300 ℃; then introducing inert carrier gas, wherein the flow rate of the introduced mixed gas is 1-30L/min, preferably 10L/min; injecting a carbon source/catalyst solution into the reaction cavity at a rate of 10-40mL/h and 20 mL/h; preferably, the inert carrier is argon and hydrogen (Ar/H)2) And the volume ratio of argon gas to hydrogen gas is 10: (8-10);
the carbon nano tube film is driven by inert carrier gas to float out of the tube tail, and is continuously rolled by a collecting roller.
3. The method for preparing a thermal interface material according to claim 2, wherein the carbon source solvent is absolute ethyl alcohol, ethylene glycol, methanol or benzyl alcohol, the catalyst is ferrocene, and the accelerator is thiophene.
4. The method for preparing a thermal interface material according to claim 1, wherein the step of preparing a mixed dispersion solution of nano-sized silica powder and graphene oxide comprises:
adding nanoscale silicon dioxide powder and graphene oxide powder into a solvent, adding a dispersing agent, stirring and mixing uniformly, wherein the size of the nanoscale silicon dioxide powder is 1-100 nanometers, and preferably 1-5 nanometers; the size of the graphene oxide material sheet layer is 1-100 micrometers, preferably 2-5 micrometers;
stirring and dispersing by using water and/or N-methyl pyrrolidone (NMP) and absolute ethyl alcohol as solvents and one or more of polyvinylpyrrolidone (PVP), polyvinyl alcohol (PVA), Sodium Dodecyl Sulfate (SDS), Sodium Dodecyl Benzene Sulfonate (SDBS) and carboxymethyl cellulose (CMC) as dispersing agents;
in the mixed dispersion liquid, the mass concentration of graphene in the mixed dispersion liquid is 1-50 wt%, preferably 35 wt%; the mass concentration of the nano-scale silicon dioxide in the mixed dispersion liquid is 1-10 wt%, preferably 5 wt%; the mass concentration of the dispersant is 0.1-5 wt%, preferably 1-2 wt%.
5. The method for preparing a thermal interface material according to claim 1, wherein the step of forming the carbon nanotube-nanosilica-graphene oxide composite film comprises:
spraying the nano-scale silicon dioxide and graphene oxide dispersion liquid on the surface of the carbon nanotube film by adopting spraying equipment, wherein the average spraying thickness of the surface of the carbon nanotube film is 1-100 micrometers, and preferably 30-50 micrometers;
covering a layer of carbon nanotube film to form a carbon nanotube film/nano-scale silicon dioxide-graphene oxide/carbon nanotube film composite structure;
repeating the above two steps to form a multi-layer carbon nanotube film/nano-scale silicon dioxide-graphene oxide/carbon nanotube film laminated structure.
6. The method for preparing a thermal interface material according to claim 1, wherein the step of performing rapid thermal treatment on the carbon nanotube-nanosilica-graphene oxide composite film in an inert protective atmosphere comprises:
putting the coiled carbon nanotube-nano silicon dioxide-graphene oxide composite film prepared by spraying and compounding into a vacuum heat treatment furnace;
vacuumizing the vacuum heat treatment furnace, introducing argon protective gas after the background vacuum degree reaches 3Pa, heating to 1400-1600 ℃, preferably 1500 ℃, and carrying out heat treatment, wherein the heat preservation time is 30-180min, preferably 100-120min, and the argon introduction rate is 800ml/min, preferably 200-400ml/min during heat preservation;
after the treatment in the high-temperature heat preservation stage is finished, the temperature of the heat treatment furnace is reduced to 150-300 ℃, and preferably 200 ℃; the cooling rate is 3-10 ℃/min, preferably 4-5 ℃/min;
and taking out the carbon nano tube-graphene-silicon carbide nanowire composite film obtained after the heat treatment.
7. The method of claim 1, further comprising: and (3) carrying out rolling and shaping treatment on the carbon nano tube-graphene-silicon carbide nanowire composite film.
8. The method for preparing a thermal interface material according to claim 7, wherein the rolling pressure is 0.2 to 2MPa, preferably 0.2 to 0.7MPa, in the rolling and setting treatment.
9. The method for preparing a thermal interface material according to claim 7, wherein the longitudinal thermal conductivity of the rolled and shaped carbon nanotube-graphene-silicon carbide nanowire composite film is 5-50W/m.K according to different process conditions.
10. A thermal interface material is characterized by comprising a plurality of units, wherein each unit comprises two layers of carbon nanotube films, and a graphene microchip and a silicon carbide nanowire which are sandwiched between the two layers of carbon nanotube films and subjected to thermal reduction.
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