CN115159511B - Graphene material, preparation method thereof and heat conduction gasket - Google Patents

Graphene material, preparation method thereof and heat conduction gasket Download PDF

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CN115159511B
CN115159511B CN202210938687.8A CN202210938687A CN115159511B CN 115159511 B CN115159511 B CN 115159511B CN 202210938687 A CN202210938687 A CN 202210938687A CN 115159511 B CN115159511 B CN 115159511B
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graphene oxide
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CN115159511A (en
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葛翔
杨淑洁
胡佳佳
周曙
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Changzhou Fuxi Technology Co Ltd
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/15—Nano-sized carbon materials
    • C01B32/182—Graphene
    • C01B32/184—Preparation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/15—Nano-sized carbon materials
    • C01B32/182—Graphene
    • C01B32/194—After-treatment
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    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2204/00—Structure or properties of graphene
    • C01B2204/20—Graphene characterized by its properties
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2204/00—Structure or properties of graphene
    • C01B2204/20—Graphene characterized by its properties
    • C01B2204/24—Thermal properties
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Abstract

The scheme discloses a graphene material, a preparation method thereof and a heat conduction gasket, wherein graphene oxide slurry is coated on the surface of a substrate, and a first layer of template is arranged after the coating; drying graphene oxide slurry between the substrate and the first layer of template to form a first layer of graphene oxide coating; coating graphene oxide slurry on the first layer of template, and setting a second layer of template after coating; drying the graphene oxide slurry between the first layer of templates and the second layer of templates to form a second layer of graphene oxide coating; repeating the steps of coating graphene oxide slurry, setting a template and drying to a preset thickness to obtain graphene oxide blanks; performing heat treatment on the blank to obtain a graphene material which is formed by a plurality of graphene layers, wherein lamellar gaps exist between upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps; wherein the template is made of foaming material; the template is provided with a through hole penetrating through the template along the thickness direction. The graphene material is used for preparing the reinforced composite material, and is simple and easy to implement.

Description

Graphene material, preparation method thereof and heat conduction gasket
Technical Field
The invention relates to the technical field of heat conduction materials, in particular to a graphene material, a preparation method thereof and a heat conduction gasket.
Background
The graphene heat-conducting film is a graphene film structural material with high heat conductivity formed by coating, drying and heat treatment of graphene oxide slurry. The heat-conducting material has good heat-conducting property (the heat conductivity coefficient is more than 1500W/(m.K)), excellent structural strength and excellent flexible folding property, and is widely applied to the fields of smart phones, tablet personal computers, ultrathin notebooks and the like. Meanwhile, the graphene heat-conducting film has wide application prospects in composite materials, particularly high-heat-conducting composite materials. However, when the graphene heat-conducting film is used for preparing the composite material, the composite material has the problems of poor mechanical property, easiness in cracking and the like due to insufficient binding force with matrix materials such as polymers and the like. The reason for this is that the graphene heat conductive film is densified, and the inside thereof is difficult to be immersed in a matrix material such as a polymer. In contrast, patent document CN112852159A, CN113147115A, CN113290958A, CN113510979a discloses that a polymer is filled in a foam structure inside a graphene foam film, and a related composite material is prepared. However, since the pores in the graphene foam film have a small size and are mostly closed pores, it is very difficult to impregnate a matrix material such as a polymer, and only a small amount of pores can be filled. Therefore, the obtained composite material is not compact, has poorer mechanical property and is easy to crack.
Disclosure of Invention
One purpose of the scheme is to provide a preparation method of the graphene material, and the graphene material prepared by the method is used for preparing various reinforced composite materials, and is simple and easy to implement.
Another object of the present invention is to provide a graphene material prepared by the above method, which has a layered void and a through hole formed of graphene and distributed in the layered void.
A third object of the present solution is to provide a graphene thermal pad.
In order to achieve the above purpose, the scheme is as follows:
a preparation method of a graphene material comprises the following steps:
coating graphene oxide slurry on the surface of a substrate, and setting a first layer of template after coating;
drying graphene oxide slurry between the substrate and the first layer of template to form a first layer of graphene oxide coating; coating graphene oxide slurry on the first layer of template, and setting a second layer of template after coating;
drying the graphene oxide slurry between the first layer of templates and the second layer of templates to form a second layer of graphene oxide coating;
repeating the steps of coating graphene oxide slurry, setting a template and drying to a preset thickness to obtain graphene oxide blanks;
carrying out heat treatment on the graphene oxide blank to obtain a graphene material which is formed by a plurality of graphene layers, wherein lamellar gaps exist between upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps;
wherein the template is a foaming material; and a through hole penetrating through the template is formed in the template along the thickness direction.
In the heat treatment process, graphene oxide is thermally reduced to graphene; the template is foamed to form a layered gap, and a small amount of carbon layer formed after heat treatment is integrated with graphene.
Preferably, the layered gap is a layer of gap between upper and lower adjacent graphene layers, the size of the layered gap in the direction parallel to the graphene layers is 50-1000 μm, and the size of the layered gap in the direction perpendicular to the graphene layers is 30-200 μm;
the number of through holes in the template is multiple.
The size of the lamellar gap is lower than 50 μm in the direction parallel to the graphene layer, so that the gap is too small, which is not beneficial to the impregnation of the following high polymer; if the particle size is higher than 1000 mu m, the gap is too large, the overall stability is not facilitated, the gap structure is easy to collapse, and the sample is damaged; in the vertical direction, the gaps are too small below 30 mu m, which is not beneficial to the impregnation of the following high polymer; if the particle diameter is more than 200 mu m, the gap is too large, the overall stability is not facilitated, the gap structure is easy to collapse, and the sample is damaged.
Preferably, the temperature of the heat treatment of the graphene oxide blank is higher than or equal to 2400 ℃, and the temperature is higher than or equal to 2800 ℃ preferably;
the graphene oxide coating is formed by coating and drying graphene oxide slurry; the drying temperature is 40-150 ℃.
Preferably, the weight percentage of the graphene oxide in the graphene oxide slurry is 0.5wt.% to 10wt.%, and preferably the weight percentage of the graphene oxide is 2wt.% to 8wt.%.
The graphene oxide content in the graphene oxide slurry is less than 0.5wt.%, the slurry is too dilute to be coated, and more than 10wt.%, the slurry is too thick to be coated.
Preferably, the thickness of the graphene oxide coating is 0.1 mm-1 mm, and preferably the thickness of the graphene oxide coating is 0.25 mm-0.8 mm. The thickness of the graphene oxide coating is lower than 0.1mm, and precise control cannot be performed; the thickness of the graphene oxide is higher than 1mm, the graphene oxide is coated too thick, the graphene oxide is easy to form own pores, the pores are uncontrolled, and the internal gaps of the whole material are difficult to control
Preferably, the method further comprises peeling the substrate after obtaining a graphene oxide blank of a predetermined thickness;
the substrate comprises polyethylene terephthalate (PET), polypropylene (PP), polyethylene (PE), polyvinyl chloride (PVC), polytetrafluoroethylene (PTFE), copper foil, aluminum film or glass.
Preferably, the thickness of the template is 5-50 μm, preferably the thickness of the template is 10-20 μm; the pore size of the through hole on the template is 50-200 mu m, preferably the pore size of the through hole is 100-150 mu m; the hole spacing between every two through holes on the template is 100-200 mu m, and the hole spacing is 120-160 mu m.
The thickness of the template is less than 5 mu m, the template cannot play a role in excessively thinning, and the formed void structure is not obvious; the thickness is higher than 50 mu m, so that the gap is overlarge, and the mechanical stability of the sample is affected; the pore diameter of the through hole on the template is smaller than 50 mu m, which can cause poor combination between the upper layer graphene and the lower layer graphene, and the pore diameter is larger than 200 mu m, which can cause unsmooth communication between the gaps, and is unfavorable for later immersion in high polymer; the hole spacing between the through holes is lower than 100 mu m, which can cause too small gaps and is not beneficial to the impregnation of the polymer in the later stage; above 200 μm, the resulting voids are too large, which is detrimental to the mechanical stability of the sample.
Preferably, the foaming material is a polymer film, and the foaming material comprises epoxy resin, phenolic resin, furfural resin, polyimide (PI), polyarylacetylene (PAA), polymethyl methacrylate (PMMA), asphalt, ABS, PC-ABS, polyethylene terephthalate (PET) or Polyurethane (PU).
In a second aspect, there is provided a graphene material prepared by the preparation method of any one of the above, wherein the graphene material is composed of a plurality of graphene layers, and a layered gap exists between upper and lower adjacent graphene layers and a plurality of graphene columns are distributed between the layered gaps.
In a third aspect, a graphene heat-conducting gasket is provided, which is made of the graphene material, and the graphene heat-conducting gasket is prepared by immersing the prepared graphene material in a high polymer, taking out the high polymer, and cutting the graphene material into pieces along the thickness direction after curing and forming; in the graphene heat conduction gasket, the weight percentage of graphene is 30-70 wt%, and preferably 40-60 wt%.
The graphene content in the heat conduction gasket is lower than 30 wt%, so that the heat conduction performance of the material is obviously reduced due to the fact that the graphene content is too low; above 70wt.%, the high molecular polymer content is too low and the sample is prone to cracking during use.
The beneficial effects of this scheme are as follows:
1. the preparation method provided by the application prepares the graphene material with the layered gap and the through hole structure between graphene layers;
2. the prepared graphene material can be used for reinforcing a composite material;
3. the enhancement mode is simple and easy to implement;
4. the prepared graphene material can be directly impregnated and reinforced to obtain the graphene heat conduction gasket with excellent heat conduction performance and mechanical property.
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In order to more clearly illustrate the practice of the present solution, the drawings that are required for the description of the embodiments will be briefly described below, it being apparent that the drawings in the following description are only some embodiments of the present solution and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
Fig. 1 is a schematic structural diagram of graphene oxide billets prepared in the examples.
Detailed Description
Embodiments of the present solution are described in further detail below. It is clear that the described embodiments are only some of the embodiments of the present solution, not an exhaustive list of all embodiments. It should be noted that, in the case of no conflict, the embodiments and features in the embodiments in the present solution may be combined with each other.
The terms first, second, and the like in the description and in the claims, if any, are used for distinguishing between similar elements and not necessarily for describing a particular sequential or chronological order. It will be appreciated that the data so used may be interchanged where appropriate. Furthermore, the terms "comprises," "comprising," and "having," and any variations thereof, are intended to cover a non-exclusive inclusion, such that a process, method, system, article, or apparatus that comprises a list of steps or elements is not necessarily limited to those steps or elements that are expressly listed or inherent to such process, method, article, or apparatus.
The inventor of the application provides a graphene material, which consists of a plurality of graphene layers, wherein lamellar gaps exist between the upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps.
After the graphene material is immersed in the high-molecular polymer, the high-molecular polymer immersed in the lamellar gaps of the same layer forms a whole after solidification, so that the graphene of each layer in the obtained composite material is mutually continuous, and the whole is formed by the solidified high-molecular polymer distributed among the graphene layers.
According to the preparation method, the organic silica gel is used as a high molecular polymer, and is combined with the prepared graphene material to obtain the graphene heat conduction gasket with excellent heat conduction performance and good mechanical property.
The application provides a preparation method of a graphene material, which comprises the following steps:
coating graphene oxide slurry on the surface of a substrate, and setting a first layer of template after coating;
drying graphene oxide slurry between the substrate and the first layer of template to form a first layer of graphene oxide coating; coating graphene oxide slurry on the first layer of template, and setting a second layer of template after coating;
drying the graphene oxide slurry between the first layer of templates and the second layer of templates to form a second layer of graphene oxide coating;
repeating the steps of coating graphene oxide slurry, setting a template and drying to a preset thickness to obtain graphene oxide blanks;
carrying out heat treatment on the graphene oxide blank to obtain a graphene material which is formed by a plurality of graphene layers, wherein lamellar gaps exist between upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps;
wherein the template is made of foaming material; the template is provided with a through hole penetrating through the template along the thickness direction.
The thickness direction in this scheme is the direction perpendicular to the plane that the template is located.
In the heat treatment process, graphene oxide is thermally reduced to graphene; the template is foamed to form a layered gap, and a small amount of carbon layer formed after heat treatment is integrated with graphene.
Because each layer of template is provided with a through hole, after the graphene oxide slurry is coated on the template, the graphene oxide slurry flows into the through holes, and when the graphene oxide slurry is subjected to heat treatment later, the graphene oxide slurry in the through holes forms graphene columns.
In one embodiment, the weight percent of graphene oxide in the graphene oxide slurry is 0.5-10 wt.%, preferably the weight percent of graphene oxide is 2-8 wt.%, such as 0.5wt.%,1wt.%,2wt.%,2.5wt.%,3.5wt.%,4wt.%,4.5wt.%,5wt.%,5.5wt.%,6wt.%, 5wt.%,7wt.%, 5wt.%,8wt.%,9wt.% or 10wt.%. The thickness of the graphene oxide coating is 0.1 to 1mm, preferably the thickness of the graphene oxide coating is 0.25 to 0.8mm, such as 0.1mm,0.2mm,0.25mm,0.3mm,0.35mm,0.4mm,0.45mm,0.5mm,0.55mm,0.6mm,0.65mm,0.7mm,0.75mm,0.8mm,0.9mm or 1.0mm.
In one embodiment, the substrate comprises at least one of PET, PP, PE, PVC, PTFE, copper foil, aluminum film and glass.
In one embodiment, the thickness of the template is from 5 μm to 50 μm, preferably the thickness of the template is from 10 μm to 20 μm, such as 5 μm,10 μm,11 μm,12 μm,13 μm,14 μm,15 μm,16 μm,17 μm,18 μm,19 μm,20 μm,25 μm,30 μm,35 μm,40 μm,45 μm or 50 μm; the pore size of the through holes on the template is 50 μm to 200. Mu.m, preferably the pore size of the through holes is 100 μm to 150. Mu.m, such as 50 μm,55 μm,60 μm,65 μm,70 μm,75 μm,80 μm,85 μm,90 μm,95 μm,100 μm,105 μm,110 μm,115 μm,120 μm,125 μm,130 μm,135 μm,140 μm,145 μm,150 μm,155 μm,160 μm,165 μm,170 μm,175 μm,180 μm,185 μm,190 μm,195 μm, or 200 μm; the spacing between every two through holes on the template is 100 μm to 200. Mu.m, preferably 120 μm to 160. Mu.m, such as 100 μm,110 μm,120 μm,125 μm,130 μm,135 μm,140 μm,145 μm,150 μm,155 μm,160 μm,170 μm,180 μm,190 μm or 200 μm.
In one embodiment, the layered void is a layer of void existing between upper and lower adjacent graphene layers, and the size of the layered void in the direction parallel to the graphene layers is 50 μm to 1000 μm, such as 50 μm,100 μm,200 μm,300 μm,400 μm,500 μm,600 μm,700 μm,800 μm,900 μm or 1000 μm; the size of the void in the direction perpendicular to the graphene layer is 30 μm to 200 μm, such as 30 μm,40 μm,50 μm,60 μm,70 μm,80 μm,90 μm,100 μm,110 μm,120 μm,130 μm,140 μm,150 μm,160 μm,170 μm,180 μm,190 μm or 200 μm.
In one embodiment, the plurality of through holes is provided in the template.
In one embodiment, the graphene oxide blank is heat treated at a temperature of 2400 ℃ or higher, preferably at a temperature of 2800 ℃ or higher; the graphene oxide coating is formed by coating and drying graphene oxide slurry; the drying temperature is 40-150 ℃, such as 40 ℃,50 ℃,60 ℃,70 ℃,80 ℃,90 ℃,100 ℃,110 ℃,120 ℃,130 ℃,140 ℃ or 150 ℃.
In one embodiment, the template is a polymeric film, and the foaming material comprises epoxy resin, phenolic resin, furfural resin, polyimide (PI), polyarylacetylene (PAA), polymethyl methacrylate (PMMA), asphalt, ABS, PC-ABS, polyethylene terephthalate (PET) or Polyurethane (PU).
The application provides a graphene material prepared by the preparation method, which consists of a plurality of graphene layers, wherein lamellar gaps exist between the upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps.
The application also provides a graphene heat-conducting gasket which is prepared from the graphene material, and the graphene heat-conducting gasket is prepared by immersing the prepared graphene material in a high-molecular polymer, taking out the graphene material to be solidified and formed, and cutting the graphene material into pieces along the thickness direction; in the prepared graphene heat conduction gasket, the weight percentage of the graphene is 30-70 wt%, preferably 40-60 wt%, such as 30-40 wt%, 45 wt%, 50 wt%, 55 wt%, 60 wt% or 70 wt%.
The thickness of the graphene used for preparing the heat conducting gasket is not particularly limited, and is preferably 25-100 mm in the application.
The present application will be described with reference to specific examples.
A preparation method of a graphene heat conduction gasket comprises the following steps:
coating graphene oxide slurry on the surface of a substrate, and setting a first layer of template after coating;
drying graphene oxide slurry between the substrate and the first layer of template to form a first layer of graphene oxide coating; coating graphene oxide slurry on the first layer of template, and setting a second layer of template after coating;
drying the graphene oxide slurry between the first layer of templates and the second layer of templates to form a second layer of graphene oxide coating;
repeating the steps of coating graphene oxide slurry, setting a template and drying to a preset thickness to obtain graphene oxide blanks;
carrying out heat treatment on the graphene oxide blank to obtain a graphene material which is formed by a plurality of graphene layers, wherein lamellar gaps exist between upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps;
immersing a graphene material with lamellar gaps into a high molecular polymer;
and after solidification and molding, cutting into pieces along the thickness direction to obtain the graphene heat-conducting gasket.
Carrying out performance parameter test on the graphene material with the layered gaps prepared in each embodiment, and testing the thermal diffusion coefficient of the graphene material by referring to an ASTME1461 flashing method;
testing the specific heat capacity of the graphene material with reference to ASTM E1269-2018 differential scanning calorimetry; the density of the graphene material was tested according to GB 4472-1984;
in the application, the thermal conductivity coefficient of the graphene material is calculated by adopting the following formula:
K＝λ·C p ·ρ
k-coefficient of thermal conductivity, unit W/(m.K);
lambda-thermal diffusivity in mm 2 /s；
C p Specific heat capacity, unit J/(g·k);
rho-density in g/cm 3 ；
Testing the heat conductivity coefficient and the application thermal resistance of a graphene heat conduction gasket made of a graphene material by referring to an ASTMD5470 test method, wherein the application thermal resistance in the application is the sum of intrinsic thermal resistance and contact thermal resistance of the upper surface and the lower surface;
the graphene thermal pads were tested for longitudinal compressibility and compression resilience by reference to ASTM D395 assay methods, respectively for the compressibility of the samples at 40psi pressure, and for the resilience after 30 minutes after the samples were compressed to 50% strain.
For convenience of comparison, in the embodiment of the application, the graphene heat conduction gasket is tested for performance such as thermal resistance, compressibility, compression resilience and the like, and samples with the thickness of 0.5mm are uniformly adopted.
Examples 1 to 5
According to the steps for preparing the graphene material and the graphene heat-conducting gasket, the graphene material and the graphene heat-conducting gasket are prepared according to the steps, except that raw materials used for preparing the graphene material, template materials, template thicknesses, the aperture of through holes formed in the template and the intervals between every two through holes when a plurality of through holes are formed, drying conditions of graphene oxide slurry and heat treatment conditions of graphene oxide blank are shown in table 1, the characteristics and performance test results of the graphene material prepared in each embodiment are shown in table 2, and the content of graphene in the graphene heat-conducting gasket prepared in each embodiment and the performance test results of the heat-conducting gasket are shown in table 3. The solid content in the graphene oxide slurry of each embodiment refers to the content of graphene oxide in the graphene oxide slurry. In each embodiment, liquid silica gel is used as an adhesive for bonding the high molecular polymer and the graphene coating, and other types of adhesives are also suitable.
Fig. 1 illustrates a structure of a graphene oxide blank in each embodiment, in which graphene oxide coatings 1 and templates 2 are staggered, and after reaching a predetermined thickness, the graphene oxide blank is subjected to heat treatment, so as to obtain a graphene material with lamellar voids.
TABLE 1
Figure GDA0004234630230000101
TABLE 2
Figure GDA0004234630230000102
TABLE 3 Table 3
Figure GDA0004234630230000103
From the above embodiments, it can be known that, according to the present application, the preparation of the graphene material with the lamellar voids is achieved by performing the coating of the template and the graphene oxide slurry at intervals when preparing the graphene material, wherein the size of the lamellar voids can be regulated and controlled by the size of the template, and the size of the lamellar voids is convenient for the impregnation of the high polymer.
The graphene on the upper layer and the lower layer of the graphene material prepared by the method keep an integral continuous structure, and when the graphene material is applied to a composite material, a heat conduction channel is continuous and uninterrupted, so that the heat conduction effect can be enhanced and maximized; the high molecular polymer immersed in the lamellar gaps of each layer forms a continuous structure, so that the mechanical property of the composite material is improved to the greatest extent; the prepared graphene material is directly immersed and matched with a cutting sheet process, and then the graphene heat conduction gasket product with good heat conduction performance and stable mechanical property can be obtained.
It should be understood that the foregoing examples of the present invention are provided merely for clearly illustrating the present invention and are not intended to limit the embodiments of the present invention, and that various other changes and modifications may be made therein by one skilled in the art without departing from the spirit and scope of the present invention as defined by the appended claims.

Claims (15)

1. The preparation method of the graphene material is characterized by comprising the following steps of:
coating graphene oxide slurry on the surface of a substrate, and setting a first layer of template after coating;
drying graphene oxide slurry between the substrate and the first layer of template to form a first layer of graphene oxide coating; coating graphene oxide slurry on the first layer of template, and setting a second layer of template after coating;
drying the graphene oxide slurry between the first layer of templates and the second layer of templates to form a second layer of graphene oxide coating;
repeating the steps of coating graphene oxide slurry, setting a template and drying to a preset thickness to obtain graphene oxide blanks;
carrying out heat treatment on the graphene oxide blank to obtain a graphene material which is formed by a plurality of graphene layers, wherein lamellar gaps exist between upper and lower adjacent graphene layers, and a plurality of graphene columns are distributed among the lamellar gaps;
wherein the template is a foaming material;
and a through hole penetrating through the template is formed in the template along the thickness direction.
2. The preparation method of claim 1, wherein the layered gap is a layer of gap between upper and lower adjacent graphene layers, the size of the layered gap in the direction parallel to the graphene layers is 50-1000 μm, and the size of the gap in the direction perpendicular to the graphene layers is 30-200 μm;
the number of through holes in the template is multiple.
3. The method according to claim 1, wherein the graphene oxide blank is subjected to heat treatment at a temperature of 2400 ℃ or higher;
the graphene oxide coating is formed by coating and drying graphene oxide slurry; the drying temperature is 40-150 ℃.
4. The method according to claim 3, wherein the graphene oxide blank is heat-treated at a temperature of 2800 ℃ or higher.
5. The preparation method of claim 3, wherein the graphene oxide slurry contains 0.5-10wt.% of graphene oxide.
6. The preparation method of claim 5, wherein the graphene oxide slurry comprises 2-8 wt.% of graphene oxide.
7. The preparation method of claim 1, wherein the graphene oxide coating has a thickness of 0.1-1 mm.
8. The preparation method of claim 7, wherein the graphene oxide coating has a thickness of 0.25-0.8 mm.
9. The method of manufacturing according to claim 1, further comprising peeling the substrate after obtaining a graphene oxide blank of a predetermined thickness;
the substrate comprises polyethylene terephthalate, polypropylene, polyethylene, polyvinyl chloride, polytetrafluoroethylene, copper foil, aluminum film or glass.
10. The method according to claim 2, wherein the thickness of the template is 5-50 μm; the aperture size of the through hole on the template is 50-200 mu m; the hole spacing between every two through holes on the template is 100-200 mu m.
11. The method according to claim 10, wherein the thickness of the template is 10-20 μm; the aperture size of the through hole is 100-150 mu m; the hole spacing is 120-160 mu m.
12. The method of claim 1, wherein the foaming material comprises epoxy resin, phenolic resin, furfural resin, polyimide, polyarylacetylene, polymethyl methacrylate, asphalt, ABS, PC-ABS, polyethylene terephthalate, or polyurethane.
13. A graphene material produced by the production method according to any one of claims 1 to 12, wherein the graphene material is composed of a plurality of graphene layers, and a plurality of graphene columns are distributed between the upper and lower adjacent graphene layers with a layered void therebetween.
14. The graphene heat-conducting gasket is characterized by being prepared from the graphene material according to claim 13, and comprises the steps of immersing the prepared graphene material into a high-molecular polymer, taking out the high-molecular polymer, and cutting the graphene material into pieces along the thickness direction after the high-molecular polymer is cured and molded to prepare the graphene heat-conducting gasket; in the graphene heat conduction gasket, the weight percentage of graphene is 30-70wt%.
15. The graphene heat-conducting gasket of claim 14, wherein the graphene is 40-60 wt%.
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