KR101691594B1 - Thermally conductive film having metal-graphene carbon and method of manufacturing the same - Google Patents
Thermally conductive film having metal-graphene carbon and method of manufacturing the same Download PDFInfo
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- KR101691594B1 KR101691594B1 KR1020160038623A KR20160038623A KR101691594B1 KR 101691594 B1 KR101691594 B1 KR 101691594B1 KR 1020160038623 A KR1020160038623 A KR 1020160038623A KR 20160038623 A KR20160038623 A KR 20160038623A KR 101691594 B1 KR101691594 B1 KR 101691594B1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
- B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B9/041—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B15/00—Layered products comprising a layer of metal
- B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
- B32B9/005—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile
- B32B9/007—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising one layer of ceramic material, e.g. porcelain, ceramic tile comprising carbon, e.g. graphite, composite carbon
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/02—Pretreatment of the material to be coated
- C23C14/021—Cleaning or etching treatments
- C23C14/022—Cleaning or etching treatments by means of bombardment with energetic particles or radiation
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
- C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
- C23C14/34—Sputtering
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2311/00—Metals, their alloys or their compounds
- B32B2311/12—Copper
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2311/00—Metals, their alloys or their compounds
- B32B2311/18—Titanium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2311/00—Metals, their alloys or their compounds
- B32B2311/24—Aluminium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2313/00—Elements other than metals
- B32B2313/04—Carbon
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- Engineering & Computer Science (AREA)
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- Chemical Kinetics & Catalysis (AREA)
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Abstract
Description
The present invention relates to a metal-graphene carbon thermal conductive film and a method of manufacturing the same, and more particularly, to a metal-graphene carbon thermal conductive film which is formed by spraying, coating, drying and stripping a graphene dispersion not containing an adhesive component on a metal film, To a metal-graphene carbon thermal conductive film capable of sufficiently preventing the occurrence of thermal resistance and improving a thermal conductivity coefficient, and a method of manufacturing the metal-graphene carbon thermal conductive film.
In recent years, the integration of electronic devices with high functionality has resulted in a drastic increase in thermal density due to an increase in resistance due to the driving of the device, and the efficient dispersion and divergence of heat generated due to the fine pitching of the driving circuit, It is becoming the most important factor influencing the reliability increase.
That is, according to miniaturization, high power, and high speed of a microelectronic component, it is necessary to quickly remove high temperature heat generated by the electronic component and operate the electronic component at a safe operating temperature range. , The performance of the electronic component is deteriorated, which seriously affects the reliability and service life of the component.
Graphene, on the other hand, separates one layer of graphite and is a material that forms a two-dimensional planar structure in which carbon atoms are connected in a honeycomb-like hexagonal shape. Such graphene is not only very high in electric conductivity, but also can be applied to flexible displays, electronic paper, and solar cells because it does not lose its electrical properties even when stretched or bent. In particular, graphene is highly transparent and is expected to replace ITO (Indium Tin Oxide), which is currently used as a transparent electrode for touch screens, semiconductors and displays.
That is, graphene is a carbon molecule in which a kind of carbon atoms are arranged in a hexagonal shape and connected to each other, and its structure is very stable, and it is currently the thinnest and hardest nanomaterial in the world. This graphene is almost transparent and absorbs only 2.3% of light. The graphene has a thermal conductivity of 5000 W / mK, a higher thermal conductivity than nano-carbon pipes and diamonds, and an electron transfer rate of 15000 cm 2 / V · s and higher than nano-carbon pipe or silicon crystal. Further, the electric resistivity of yes pin 10 was lower than that of copper, or is a 6 Ω · cm, This graphene has the characteristics of high conductivity, high thermal conductivity, a chapter deceased, high strength, high specific surface area and the like. Due to the characteristics of graphene, it can be widely used in various fields such as electronics, aerospace, military industry, new energy, new material.
Meanwhile, the Chinese patent CN103407268 A discloses a method of manufacturing a composite thermal conductive film containing graphene, which comprises 3 to 5 parts by weight of copper powder, 10 to 20 parts by weight of butyl ester, 5 to 10 parts by weight of guar gum and 1 to 3 parts by weight of magnesium silicate, and then the copper powder, butyl acrylate, guar gum, and magnesium silicate are uniformly mixed at room temperature, And then the resulting composite is uniformly applied to the base material, and the graphene film is coated on the composite and dried at 50 DEG C for 30 minutes (min), and then the composite is uniformly applied to the graphene film And the complex thermal conductive film composite containing graphene is cut to produce a composite thermal conductive film containing graphene.
However, since the graphene-containing composite thermal conductive film contains an adhesive component in the manufacturing process, the thermal conductivity of the heat conductive material such as graphene increases and the thermal conductivity of the thermal conductive film is reduced.
According to the present invention, a graphene dispersion liquid not containing an adhesive component is sprayed, applied, dried and peeled to form a film on the metal film, whereby the thermal conductivity of the graphene can be sufficiently exhibited to prevent the occurrence of thermal resistance, Graphene carbon thermal conductive film and a method of manufacturing the same.
The present invention also provides a metal-graphene carbon thermal conductive film and a method for manufacturing the metal-graphene carbon thermal conductive film which can expand the description of the thermal conduction characteristics of graphene by forming a metal film using a metal such as copper, aluminum or titanium .
The various problems to be solved by the present invention are not limited to the above-mentioned problems, and other problems not mentioned can be clearly understood by those skilled in the art from the following description.
The metal-graphene carbon thermally conductive film according to the present invention is a graphene film; And a metal film on which the graphene film is formed, wherein at least one metal film is deposited on one surface of the graphene film, and the thickness of the graphene film and the metal film is 9: 1.
The metal film may be a copper film, an aluminum film or a titanium film.
In addition, a method of manufacturing a metal-graphene carbon thermal conductive film according to the present invention includes forming a graphene film; And forming a composite film, wherein the step of forming the graphene film is a step of spraying an aqueous graphene dispersion onto a copper foil, coating, drying and peeling the graphene film to form a graphene film, And forming a thermal spray coating on the metal film by applying a metal vacuum ion plating film to the graphene film produced in the forming step.
The graphene film is formed by spraying an aqueous graphene dispersion onto a copper foil and then drying at a temperature of 80 to 100 ° C for 2 to 3 hours. The aqueous graphene dispersion is sprayed onto a copper foil and dried, And pressed by using the automatic press, and then peeled off using a fully automatic bonding separator.
In the step of forming the composite film, a metal vacuum ionic coating is performed using a sputtering deposition facility, a metal vacuum ionic coating is performed using the sputtering deposition facility, and an insulating material is sprayed onto the metal film at 450 to 500 ° C. in an inert gas atmosphere , And can be applied.
As the insulating material, a polymer material having a molecular weight of 1,000,000 to 1,400,000 is used, and as the polymer material, trischloro-isopropyl phosphate (TCPP) may be used.
The details of other embodiments are included in the detailed description.
The metal-graphene carbon thermally conductive film and the method for manufacturing the same according to the present invention can form a film by spraying, coating, drying and peeling a graphene dispersion not containing an adhesive component on a metal film, It is possible to prevent the occurrence of the thermal resistance sufficiently and to improve the thermal conductivity coefficient.
In addition, the metal-graphene carbon thermal conductive film and the method of manufacturing the same according to the present invention can expand and utilize the technology of the thermal conductivity of graphene by forming a metal film using metal such as copper, aluminum or titanium .
It will be appreciated that embodiments of the technical idea of the present invention can provide various effects not specifically mentioned.
Advantages and features of the present invention, and methods of accomplishing the same, will be apparent from and elucidated with reference to the embodiments described hereinafter in detail. However, the present invention is not limited to the embodiments described herein but may be embodied in other forms. Rather, the embodiments disclosed herein are provided so that the disclosure can be thorough and complete, and will fully convey the scope of the invention to those skilled in the art.
The terminology used in this application is used only to describe a specific embodiment and is not intended to limit the invention. The singular expressions include plural expressions unless the context clearly dictates otherwise.
Unless otherwise defined, all terms used herein, including technical or scientific terms, have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Terms such as those defined in commonly used dictionaries are to be interpreted as having a meaning consistent with the meaning in the context of the relevant art and are to be construed as ideal or overly formal in meaning unless explicitly defined in the present application Do not.
Hereinafter, the metal-graphene carbon thermal conductive film and the method of manufacturing the same according to the present invention will be described in detail.
The metal-graphene carbon thermal conductive film according to the present invention can form a film by spraying, applying, drying and peeling a graphene dispersion liquid not containing an adhesive component on a metal film, so that the thermal conductivity of graphene is sufficiently exhibited, And it is possible to improve the heat conduction coefficient.
The metal-graphene carbon thermal conductive film according to the present invention comprises a graphene film and a metal film formed on one side of the graphene film. That is, at least one metal layer is deposited on one surface of the graphene film, and the thickness of the graphene film and the metal film may be 9: 1.
Further, in the metal-graphene carbon thermal conductive film according to the present invention, the metal film may be any one selected from a copper film, an aluminum film and a titanium film.
In addition, the present invention provides a method for producing a metal-graphene carbon thermal conductive film, wherein the method for forming the metal-graphene carbon thermal conductive film includes a step of forming a graphene film and a step of forming a composite film.
That is, in the present invention, the step of forming the graphene film may be a step of spraying an aqueous graphene dispersion onto a copper foil, applying the coating, drying and stripping the graphene film.
Also, in the present invention, the step of forming the composite film may be a step of forming a thermal spray coating film on the metal film by applying a metal vacuum ion plating film to the graphene film produced in the step of forming the graphene film.
In the method of manufacturing a metal-graphene carbon thermal conductive film according to the present invention, the graphene film may be formed by spraying an aqueous graphene dispersion onto a copper foil and drying at a temperature of 80 to 100 ° C for 2 to 3 hours .
Further, in the step of forming the graphene film, an aqueous graphene dispersion may be sprayed onto a copper foil, followed by drying, followed by pressing using a full automatic press.
Further, in the step of forming the graphene film, the green compact can be peeled by using the automatic press separator after being compressed by using the automatic press.
In the method for fabricating a metal-graphene carbon thermal conductive film according to the present invention, a metal vacuum ionic coating may be performed using a sputtering deposition facility.
In the step of forming the composite film, a metal vacuum ion plating film is formed using a sputtering deposition apparatus, and then the metal film is subjected to an ion implantation treatment at 450 to 500 ° C. in an inert gas atmosphere such as helium (He), neon (Ne) The material can be sprayed and applied.
In addition, in the step of forming the composite film, a polymer material having a molecular weight of 1,000,000 to 1,400,000 may be used as the insulating material. For example, trischloro-isopropyl phosphate (TCPP) may be used as the polymer material.
In the method of manufacturing the metal-graphene carbon thermal conductive film according to the present invention, since the metal film is immersed in the graphene film and the adhesive is not used when bonding the metal film and the graphene film, the occurrence of thermal resistance can be prevented, Can be improved.
In the method of manufacturing a metal-graphene carbon thermal conductive film according to the present invention, the thickness of a conventional metal-graphene thermally conductive film is 0.1 to 0.2 mm and the thermal conductivity is 100 to 300 W / (m · K) The thickness of the graphene thermally conductive film thus produced is 0.015 to 0.5 mm and the thermal conductivity coefficient is 600 to 1800 W / (mK).
Accordingly, it is possible to improve the thermal conductivity of the product through the present invention and to produce products having various thicknesses and various thermal conductivities, and it can be applied to various consumable electronic products such as mobile phones, tablet PCs, TVs and the like.
Hereinafter, preferred embodiments of a method of manufacturing a metal-graphene carbon thermal conductive film according to the present invention will be described in more detail.
≪ Example 1 >
One graphene film and one copper film were formed in combination, and the copper film was deposited in the graphene film. The thickness ratio of the graphene film to the copper film was 9: 1.
The method of manufacturing the metal-graphene carbon heat conductive film in the above Example 1 was as follows.
First, an aqueous graphene dispersion was sprayed onto a copper foil and dried at a temperature of 80 to 100 ° C for 2 to 3 hours, followed by compression using a full automatic press. After peeling by using the automatic peeling separator, The formation step of the graphene film to be manufactured was performed.
Subsequently, a metal vacuum ion plating film was formed on the graphene film produced in the step of forming a graphene film by using a sputtering deposition apparatus. After the coating film was formed, a trischloro-isopropyl phosphate (TCPP) polymer The formation of the composite membrane for spraying and applying the material (molecular weight: 1 million to 1.4 million) was carried out.
≪ Example 2 >
One graphene film and one titanium film were formed in combination, and the titanium film was deposited on the graphene film. The thickness ratio of the graphene film to the titanium film was 9: 1.
The method of manufacturing the metal-graphene carbon heat conductive film in the second embodiment was as follows.
First, an aqueous graphene dispersion was sprayed onto a titanium foil, dried at a temperature of 80 to 100 ° C for 2 to 3 hours, compressed using a full automatic press, peeled off using a fully automated bonding separator after the pressing, The formation step of the graphene film to be manufactured was performed.
Subsequently, a metal vacuum ion plating film was formed on the graphene film prepared in the step of forming the graphene film using a sputtering deposition apparatus. After the coating film was formed, a trischloro-isopropyl phosphate (TCPP) polymer The formation of the composite membrane for spraying and applying the material (molecular weight: 1 million to 1.4 million) was carried out.
≪ Example 3 >
One graphene film and one aluminum film were formed in combination, and the aluminum film was deposited on the graphene film. The thickness ratio of the graphene film to the aluminum film was 9: 1.
The method of manufacturing the metal-graphene carbon heat conductive film in the above Example 3 was as follows.
First, an aqueous graphene dispersion was sprayed onto an aluminum foil and dried at a temperature of 80 to 100 ° C for 2 to 3 hours, followed by compression using a full automatic press. After peeling by using the automatic peeling separator after the compression, The formation step of the graphene film to be manufactured was performed.
Then, a metal vacuum ion plating film was formed on the graphene film formed in the graphene film formation step using a sputtering deposition apparatus. After the coating film was formed, a trischloro-isopropyl phosphate (TCPP) polymer The formation of the composite membrane for spraying and applying the material (molecular weight: 1 million to 1.4 million) was carried out.
<Example 4>
One graphene film and two copper films were formed in combination, and the copper film was deposited on the graphene film. The thickness ratio of the graphene film to the copper film was 9: 1.
A method of producing the metal-graphene carbon heat conductive film in the fourth embodiment was as follows.
First, an aqueous graphene dispersion was sprayed onto a copper foil and dried at a temperature of 80 to 100 ° C for 2 to 3 hours, followed by compression using a full automatic press. After peeling by using the automatic peeling separator, The formation step of the graphene film to be manufactured was performed.
Subsequently, a metal vacuum ion plating film was applied twice using a sputtering deposition facility in the graphene film formed in the step of forming the graphene film. After the coating film was formed, 500 ppm of trischloro-isopropyl phosphate (TCPP ) Polymeric materials (molecular weight: 1 million to 1.4 million) were sprayed and applied.
The thickness and thermal conductivity coefficient of the metal-graphene carbon thermally conductive film prepared according to Examples 1 to 4 were measured, and the results are shown in Table 1 below.
While the present invention has been described in connection with what is presently considered to be the most practical and preferred embodiment, it is to be understood that the invention is not limited to the disclosed embodiments, but, on the contrary, It will be possible. It is therefore to be understood that one embodiment described above is illustrative in all aspects and not restrictive.
Claims (6)
Forming a metal-graphene thermally-conductive film including a step of forming a composite film,
The step of forming the graphene film may include the steps of spraying an aqueous graphene dispersion onto a copper foil, coating the same, drying and peeling the graphene film to form a graphene film. The graphene film is formed by spraying an aqueous graphene dispersion onto a copper foil Dried at a temperature of 80 to 100 ° C for 2 to 3 hours, sprayed on the copper foil by spraying the aqueous graphene dispersion, dried and compressed using a full automatic press, compressed using the automatic press, To form a graphene film,
In the step of forming the composite film, a metal vacuum ion plating film is formed on the graphene film formed in the graphene film formation step to form a thermal spray coating film on the metal film. In the step of forming the composite film, Applying a vacuum ion plating film to the metal film and applying an insulating material to the metal film in an inert gas atmosphere at 450 to 500 ° C after applying the metal vacuum ion plating film using the sputtering deposition facility, (TCPP) is used as the polymer material, and tris-chloro-isopropyl phosphate
Wherein the thickness of the graphene film and the metal film is in a ratio of 9: 1, and the metal film is selected from the group consisting of a copper film, an aluminum film, and a titanium film.
Wherein the metal-graphene thermally conductive film has a thickness of 0.015 to 0.5 mm and a thermal conductivity coefficient of 600 to 1800 W / (mK).
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| Application Number | Priority Date | Filing Date | Title |
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| KR1020160038623A KR101691594B1 (en) | 2016-03-30 | 2016-03-30 | Thermally conductive film having metal-graphene carbon and method of manufacturing the same |
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| KR1020160038623A KR101691594B1 (en) | 2016-03-30 | 2016-03-30 | Thermally conductive film having metal-graphene carbon and method of manufacturing the same |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020224258A1 (en) * | 2019-05-05 | 2020-11-12 | 深圳第三代半导体研究院 | Carbon film with high thermal conductivity, and preparation method therefor |
| CN112521881A (en) * | 2020-11-23 | 2021-03-19 | 东莞市鸿亿导热材料有限公司 | High-thermal-conductivity graphene heat dissipation film for 5G communication equipment and preparation method thereof |
| CN113997647A (en) * | 2020-07-28 | 2022-02-01 | Oppo广东移动通信有限公司 | Composite heat-conducting shielding material, preparation method and electronic equipment |
| CN114763020A (en) * | 2021-01-11 | 2022-07-19 | 深圳市汉嵙新材料技术有限公司 | Heat conducting plate |
| CN115092920A (en) * | 2022-06-27 | 2022-09-23 | 常州富烯科技股份有限公司 | Graphene heat-conducting gasket and preparation method thereof |
| CN115534494A (en) * | 2022-10-13 | 2022-12-30 | 合肥工业大学 | Cu/graphene film laminated composite material and preparation method thereof |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2020224258A1 (en) * | 2019-05-05 | 2020-11-12 | 深圳第三代半导体研究院 | Carbon film with high thermal conductivity, and preparation method therefor |
| CN113997647A (en) * | 2020-07-28 | 2022-02-01 | Oppo广东移动通信有限公司 | Composite heat-conducting shielding material, preparation method and electronic equipment |
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| CN112521881A (en) * | 2020-11-23 | 2021-03-19 | 东莞市鸿亿导热材料有限公司 | High-thermal-conductivity graphene heat dissipation film for 5G communication equipment and preparation method thereof |
| CN114763020A (en) * | 2021-01-11 | 2022-07-19 | 深圳市汉嵙新材料技术有限公司 | Heat conducting plate |
| CN115092920A (en) * | 2022-06-27 | 2022-09-23 | 常州富烯科技股份有限公司 | Graphene heat-conducting gasket and preparation method thereof |
| CN115092920B (en) * | 2022-06-27 | 2023-09-26 | 常州富烯科技股份有限公司 | Graphene heat conduction gasket and preparation method thereof |
| CN115534494A (en) * | 2022-10-13 | 2022-12-30 | 合肥工业大学 | Cu/graphene film laminated composite material and preparation method thereof |
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