Continuous multilayer copper-graphene composite film and preparation device thereof

By stacking the continuous growth and deposition of graphene film and copper film on the surface of the copper foil, a layered structure with microscopic contact is formed, which solves the problems of low production efficiency and insufficient interface bonding strength of copper-graphene composite materials in the prior art, and improves high conductivity and mechanical properties.

CN223266423UActive Publication Date: 2025-08-26NINGBO INST OF MATERIALS TECH & ENG CHINESE ACAD OF SCI

Patent Information

Application Number
CN202422622049.2
Authority / Receiving Office
CN · China
Patent Type
Utility models(China)
Current Assignee / Owner
Filing Date
2024-10-29
Publication Date
2025-08-26
Estimated Expiration
2034-10-29

AI Technical Summary

Technical Problem

In the prior art, when preparing copper-graphene composite materials, there are problems such as low production efficiency, low yield and insufficient interface bonding strength. Especially in the cold rolling composite process, it is difficult to obtain excellent combination of high conductivity and mechanical properties.

Method used

A continuous multi-layer copper-graphene composite film preparation device is adopted. By stacking graphene films and copper films in sequence on the surface of the copper foil, the CVD growth area and the coating area are used to achieve continuous growth and deposition of graphene films and copper films, forming a micro-contact layered structure, avoiding subsequent pressing treatment.

Benefits of technology

The high conductivity and mechanical properties of copper-graphene composite materials have been improved, the continuity and stability of the preparation process have been ensured, and the problem of low efficiency in the prior art has been solved.

✦ Generated by Eureka AI based on patent content.

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Abstract

The utility model discloses a continuous multilayer copper-graphene composite film and a preparation device thereof, and belongs to the field of copper-graphene composite film preparation. According to the device disclosed by the utility model, the copper-graphene composite film layer is prepared on the surface of the copper foil by arranging the copper-graphene composite film layer preparation unit, and a graphene film in the prepared copper-graphene composite film layer can keep integrity; in the whole preparation process, the composite film can be continuously prepared and obtained only by keeping continuous winding and unwinding of the copper carrying roller and the composite material winding roller, a subsequent pressing treatment procedure is not needed, the phenomenon of poor quality caused in the pressing process is avoided, the continuity and stability of the preparation process of the composite film are guaranteed, and the production efficiency is improved. The layered composite film with good combination can be obtained, and the technical problem that an existing device is low in preparation efficiency is solved.
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Description

Technical Field

[0001] The utility model belongs to the field of copper-graphene composite material preparation, and relates to a continuous multi-layer copper-graphene composite film and a preparation device thereof. Background Art

[0002] Graphene is a carbon material with a single-layer two-dimensional honeycomb lattice structure formed by densely stacked sp2 hybridized carbon atoms. It has excellent comprehensive properties, including a tensile strength of 125GPa, an elastic modulus of 1.0TPa, a thermal conductivity of 5300W / (m〃K), and an electron mobility of 2×10 5 cm 2 (v〃s), therefore, graphene is often used as an ideal filler to prepare composite materials.

[0003] Coating technologies encompass a variety of methods, such as vacuum evaporation, magnetron sputtering, and ion plating. These advanced techniques enable the deposition of specific materials onto the surfaces of other materials. For example, these coating techniques can effectively deposit copper onto graphene films, creating copper-graphene composites.

[0004] In existing technology, copper-based graphene composites can be produced by methods such as chemical vapor deposition (CVD) to decompose a carbon source and then deposit and grow graphene on the surface of copper foil. In this case, graphene can be deposited on the surface of a regularly shaped copper substrate to form an ordered heterostructure, achieving highly oriented graphene and thus high electrical conductivity. However, in practical applications, in order to achieve high electrical conductivity and improved mechanical properties, the copper-based graphene composite material needs to be further compounded.

[0005] Chinese patent application number CN112281012B discloses a method for preparing a copper-coated graphene aluminum-based composite material. This method involves subjecting graphene to solution-coated copper to produce copper-coated graphene powder; mixing the copper-coated graphene powder with aluminum powder to produce a copper-coated graphene aluminum composite powder; and spark plasma sintering the copper-coated graphene aluminum composite powder to produce the copper-coated graphene aluminum-based composite material. The resulting powder is irregularly arranged, making it difficult to obtain an ordered layered structure and, therefore, to achieve ideal electrical properties.

[0006] During lamination, rolling lamination is a common method for preparing composite materials, which mainly includes hot rolling lamination and cold rolling lamination. It has good advantages in production efficiency, material utilization, continuity and automation. Among them, hot rolling lamination can effectively achieve metallurgical bonding between the interfaces of the metal plates and strips to be laminated, resulting in high-quality composite materials. However, the high heating temperature and long heating time required can easily cause brittle intermetallic compounds to form at the composite interface of copper and graphene. In addition, hot rolling production efficiency is low and the yield rate is low. Cold rolling lamination is carried out below the recrystallization temperature of the metal materials, which allows for greater freedom in metal combination and a wide range of applications. However, the interfacial bonding strength of the plate and strip composite materials obtained by cold rolling lamination is low, which will lead to a significant decrease in the mechanical strength of the copper-based graphene composite materials, and still poses a significant obstacle to the preparation of the materials. Therefore, it is imperative to develop a method suitable for the preparation of continuous multilayer copper-graphene composite materials.

[0007] In the preparation of copper-graphene composites, graphene powder is often mixed with copper powder. After plastic forming, it is difficult to obtain an ordered layered structure, and therefore, it is difficult to achieve ideal electrical properties. Chinese patent application publication number CN118060332A discloses a method for preparing long, continuous graphene-copper composites. However, this method uses a hot rolling process to achieve metallurgical bonding of multiple layers of copper-based graphene. However, the high heating temperature and long heating time required can easily lead to the formation of brittle intermetallic compounds at the composite interface between copper and graphene, affecting the quality of the composite material. This results in low production efficiency and yield. Utility Model Content

[0008] The purpose of the utility model is to provide a continuous multi-layer copper-graphene composite film and a preparation device thereof, so as to solve the technical problem of low preparation efficiency of existing devices.

[0009] In order to achieve the above purpose, the present invention adopts the following technical solutions:

[0010] The utility model discloses a continuous multi-layer copper-graphene composite film. The continuous multi-layer copper-graphene composite film comprises a copper foil, and a surface of the copper foil is provided with a plurality of copper-graphene composite film layers stacked in sequence.

[0011] Furthermore, the copper-graphene composite film layer includes a graphene film and a copper film stacked in sequence on the surface of the copper foil.

[0012] Furthermore, the copper foil has a thickness of 5-1000 μm and a width of 1-100 cm.

[0013] Furthermore, the number of layers of the graphene film is 1-10.

[0014] Furthermore, the copper film has a thickness of 0.1-10 μm.

[0015] The present invention also discloses a continuous multi-layer copper-graphene composite film preparation device for preparing the above-mentioned continuous multi-layer copper-graphene composite film, comprising a copper-carrying roller; the discharge port of the copper-carrying roller is connected to a plurality of copper-graphene composite film layer preparation units for preparing copper-graphene composite film layers; the discharge ports of the plurality of copper-graphene composite film layer preparation units are connected to a composite material winding roller;

[0016] The plurality of copper-graphene composite film layer preparation units are connected in sequence.

[0017] Furthermore, the copper-graphene composite film preparation unit includes a CVD growth area for growing a graphene film and a coating area for depositing a copper film;

[0018] The CVD growth area and the copper film deposition area are connected in sequence.

[0019] Furthermore, the discharge port of the copper-carrying roller is connected to the CVD growth area.

[0020] Furthermore, the number of the copper-graphene composite film layer preparation units is 2 to 100.

[0021] Furthermore, the number of the copper-graphene composite film layer preparation units is 5.

[0022] Compared with the prior art, the present invention has the following beneficial effects:

[0023] The utility model discloses a continuous multilayer copper-graphene composite film. The continuous multilayer copper-graphene composite film is prepared by a copper-graphene composite film layer preparation unit on the surface of a copper foil to prepare mutually stacked graphene films and copper films. Since the mutually stacked copper-graphene composite materials are in microscopic contact, good interface bonding is guaranteed, and the layered structure ensures that the distribution of graphene in the copper matrix is ​​orderly, which can bring into play the high electron migration ability of graphene and help improve the conductive performance of the composite material. The obtained composite film has high conductivity.

[0024] The present invention also discloses a device for preparing the above-mentioned continuous multi-layer copper-graphene composite film. By setting a copper-graphene composite film layer preparation unit, the preparation of the copper-graphene composite film layer on the surface of the copper foil is realized. The graphene film in the prepared copper-graphene composite film layer can maintain integrity. During the entire preparation process, it is only necessary to maintain the continuous winding and unwinding of the copper-carrying roller and the composite material winding roller to continuously prepare the composite material. No subsequent pressing process is required, which avoids the poor quality caused by the pressing process, ensures the continuity and stability of the composite material preparation process, and can obtain a well-bonded layered composite material, thereby solving the technical problem of low preparation efficiency of the existing device. BRIEF DESCRIPTION OF THE DRAWINGS

[0025] Figure 1 This is a structural diagram of the device for preparing continuous multi-layer copper-graphene composite films of the utility model;

[0026] Figure 2 Schematic diagram of the cross-sectional structure of the multilayer copper-graphene composite film of the present invention;

[0027] Among them: 1-copper-carrying roller; 2-CVD growth area; 3-coating area; 4-copper foil; 5-graphene film; 6-copper film; 7-composite material winding roller. DETAILED DESCRIPTION

[0028] In order to help those skilled in the art better understand the present invention, the following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the embodiments described are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative efforts should fall within the scope of protection of the present invention.

[0029] It should be noted that the terms "first", "second", etc. in the specification and claims of the present invention and the above-mentioned drawings are used to distinguish similar objects and are not necessarily used to describe a specific order or sequence. It should be understood that the numbers used in this way can be interchanged where appropriate, so that the embodiments of the present invention described herein can be implemented in an order other than those illustrated or described herein. In addition, the terms "including" and "having" and any variations thereof are intended to cover non-exclusive inclusions. For example, a process, method, system, product or device that includes a series of steps or units is not necessarily limited to those steps or units clearly listed, but may include other steps or units that are not clearly listed or inherent to these processes, methods, products or devices.

[0030] The first aspect of the present invention discloses a continuous multi-layer copper-graphene composite film preparation device, which mainly includes a copper-carrying roller 1, a plurality of copper-graphene composite film layer preparation units connected in sequence and a composite material winding roller 7 connected at the end; wherein, the copper-graphene composite film layer preparation unit is used to prepare a copper-graphene composite film layer on the surface of a copper foil 4.

[0031] Preferably, the copper-graphene composite film preparation unit includes a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film.

[0032] Preferably, the number of the copper-graphene composite film layer preparation units is 2 to 100.

[0033] The second aspect of the present invention discloses a continuous multilayer copper-graphene composite film prepared by the above-mentioned device, wherein the cross-sectional structure of the continuous multilayer copper-graphene composite film includes a copper foil 4, and a plurality of copper-graphene composite film layers stacked in sequence are provided on the surface of the copper foil 4.

[0034] Preferably, the copper-graphene composite film layer comprises a graphene film 5 and a copper film 6 stacked in sequence.

[0035] Preferably, the copper foil 4 has a thickness of 5-1000 μm and a width of 1-100 cm.

[0036] Preferably, the number of layers of the graphene film 5 is 1-10; the thickness of the copper film 6 is 0.1-10 μm.

[0037] The third aspect of the present invention discloses a process for preparing a continuous multilayer copper-graphene composite film using the above-mentioned device:

[0038] First, a copper foil 4 is installed on a copper-carrying roller 1. The copper foil 4 is purchased commercially, and the thickness of the selected copper foil 4 is 5-1000 μm and the width is 1-100 cm. Secondly, the copper foil 4 on the copper-carrying roller 1 is sequentially passed through a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film at a certain tension and speed. In the CVD growth area 2, a graphene film 5 is grown on the surface of the copper foil 4 and the copper film 6. The gases are preferably CH4 and H2. The number of layers of the obtained graphene film 5 is 1-10 layers. The copper film 6 is deposited on the surface of the graphene film 5 through the coating area 3. The coating technology can be vacuum evaporation coating, magnetron sputtering coating, ion plating and other coating technologies. The thickness of the obtained copper film 6 is 0.1-10 μm. The above steps are repeated in this cycle, and the composite material is continuously wound on a winding roller 7 to obtain a continuous multi-layer copper-graphene composite film.

[0039] Example 1

[0040] like Figure 1 As shown, the utility model discloses a continuous multi-layer copper-graphene composite film preparation device, including a copper-carrying roller 1, the discharge port of the copper-carrying roller 1 is connected to two copper-graphene composite film layer preparation units, the discharge ports of the several copper-graphene composite film layer preparation units are connected to a composite material winding roller 7; wherein the two copper-graphene composite film layers are connected to each other.

[0041] Example 2

[0042] The utility model discloses a continuous multi-layer copper-graphene composite film preparation device, comprising a copper-carrying roller 1, wherein the discharge port of the copper-carrying roller 1 is connected to three copper-graphene composite film layer preparation units, and the discharge ports of the several copper-graphene composite film layer preparation units are connected to a composite material winding roller 7; wherein the three copper-graphene composite film layers are connected to each other.

[0043] Example 3

[0044] The utility model discloses a continuous multi-layer copper-graphene composite film preparation device, comprising a copper-carrying roller 1, wherein the discharge port of the copper-carrying roller 1 is connected to four copper-graphene composite film layer preparation units, and the discharge ports of the several copper-graphene composite film layer preparation units are connected to a composite material winding roller 7; wherein the four copper-graphene composite film layers are connected to each other.

[0045] Example 4

[0046] The utility model discloses a continuous multi-layer copper-graphene composite film preparation device, comprising a copper-carrying roller 1, wherein the discharge port of the copper-carrying roller 1 is connected to five copper-graphene composite film layer preparation units, and the discharge ports of the several copper-graphene composite film layer preparation units are connected to a composite material winding roller 7; wherein the five copper-graphene composite film layers are connected to each other.

[0047] Example 5

[0048] When a continuous multilayer copper-graphene composite film is prepared using the continuous multilayer copper-graphene composite film preparation device disclosed in Example 1, the following steps are included:

[0049] First, a copper foil 4 is installed on a copper-carrying roller 1. The copper foil 4 is purchased commercially, and the selected copper foil 4 has a thickness of 50 μm and a width of 4 cm. Secondly, the copper foil 4 on the copper-carrying roller 1 is sequentially passed through a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film at a certain tension and speed. In the CVD growth area 2, a graphene film 5 is grown on the surface of the copper foil 4 and the copper film 6. The gases are CH4 and H2, and the number of layers of the obtained graphene film 5 is 2. The copper film 6 is deposited on the surface of the graphene film 5 through the coating area 3. The coating technology can be vacuum evaporation coating, magnetron sputtering coating, ion plating and other coating technologies. The thickness of the obtained copper film 6 is 0.2 μm. The above coating steps are repeated twice to obtain a continuous multi-layer copper-graphene composite film.

[0050] Example 6

[0051] When a continuous multilayer copper-graphene composite film is prepared using the continuous multilayer copper-graphene composite film preparation device disclosed in Example 2, the following steps are included:

[0052] First, a copper foil 4 is installed on a copper-carrying roller 1. The copper foil 4 is purchased commercially, and the selected copper foil 4 has a thickness of 100 μm and a width of 10 cm. Secondly, the copper foil 4 on the copper-carrying roller 1 is sequentially passed through a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film under a certain tension and speed. In the CVD growth area 2, a graphene film 5 is grown on the surface of the copper foil 4 and the copper film 6. The gases are CH4 and H2, and the number of layers of the obtained graphene film 5 is 4. The copper film 6 is deposited on the surface of the graphene film 5 through the coating area 3. The coating technology can be vacuum evaporation coating, magnetron sputtering coating, ion plating and other coating technologies. The thickness of the obtained copper film 6 is 1 μm. The above coating steps are repeated 3 times to obtain a continuous multi-layer copper-graphene composite film.

[0053] Example 7

[0054] When a continuous multilayer copper-graphene composite film is prepared using the continuous multilayer copper-graphene composite film preparation device disclosed in Example 3, the following steps are included:

[0055] First, a copper foil 4 is installed on a copper-carrying roller 1. The copper foil 4 is purchased commercially, and the selected copper foil 4 has a thickness of 500 μm and a width of 20 cm. Secondly, the copper foil 4 on the copper-carrying roller 1 is sequentially passed through a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film at a certain tension and speed. In the CVD growth area 2, a graphene film 5 is grown on the surface of the copper foil 4 and the copper film 6. The gases are CH4 and H2, and the number of layers of the obtained graphene film 5 is 5. The copper film 6 is deposited on the surface of the graphene film 5 through the coating area 3. The coating technology can be vacuum evaporation coating, magnetron sputtering coating, ion plating and other coating technologies. The thickness of the obtained copper film 6 is 5 μm. The above coating steps are repeated 4 times to obtain a continuous multi-layer copper-graphene composite film.

[0056] Example 8

[0057] When a continuous multilayer copper-graphene composite film is prepared using the continuous multilayer copper-graphene composite film preparation device disclosed in Example 4, the following steps are included:

[0058] First, a copper foil 4 is installed on a copper-carrying roller 1. The copper foil 4 is purchased from a commercial source. The thickness of the selected copper foil 4 is 25 μm and the width is 20 cm. Secondly, the copper foil 4 on the copper-carrying roller 1 is sequentially passed through a CVD growth area 2 for growing a graphene film and a coating area 3 for depositing a copper film at a certain tension and speed. In the CVD growth area 2, a graphene film 5 is grown on the surface of the copper foil 4 and the copper film 6. The gases are CH4 and H2. The number of layers of the obtained graphene film 5 is 1. The copper film 6 is deposited on the surface of the graphene film 5 through the coating area 3. The coating technology can be vacuum evaporation coating, magnetron sputtering coating, ion plating and other coating technologies. The thickness of the obtained copper film 6 is 0.1 μm. The above coating steps are repeated 5 times to obtain a continuous multi-layer copper-graphene composite film with a cross-sectional structure as shown in FIG. Figure 2 shown.

[0059] The above content is only for explaining the technical idea of ​​the present invention and cannot be used to limit the protection scope of the present invention. Any changes made on the basis of the technical solution in accordance with the technical idea proposed by the present invention shall fall within the protection scope of the claims of the present invention.

Claims

1. A continuous multilayer copper-graphene composite film, characterized in that The continuous multilayer copper-graphene composite film comprises a copper foil (4), and a surface of the copper foil (4) is provided with a plurality of copper-graphene composite film layers stacked in sequence.

2. A continuous multilayer copper-graphene composite film according to claim 1, characterized in that: The copper-graphene composite film layer comprises a graphene film (5) and a copper film (6) stacked in sequence on the surface of a copper foil (4).

3. A continuous multilayer copper-graphene composite film according to claim 2, characterized in that: The copper foil (4) has a thickness of 5-1000 μm and a width of 1-100 cm.

4. A continuous multilayer copper-graphene composite film according to claim 3, characterized in that: The number of layers of the graphene film (5) is 1-10.

5. A continuous multilayer copper-graphene composite film according to claim 3, characterized in that: The copper film (6) has a thickness of 0.1-10 μm.

6. A continuous multilayer copper-graphene composite film preparation device, characterized in that: Used for preparing the continuous multilayer copper-graphene composite film according to any one of claims 1 to 5, comprising a copper-carrying roller (1); the discharge port of the copper-carrying roller (1) is connected to a plurality of copper-graphene composite film layer preparation units for preparing copper-graphene composite film layers; the discharge ports of the plurality of copper-graphene composite film layer preparation units are connected to a composite material winding roller (7); The plurality of copper-graphene composite film layer preparation units are connected in sequence.

7. A continuous multi-layer copper-graphene composite film preparation device according to claim 6, characterized in that: The copper-graphene composite film preparation unit comprises a CVD growth area (2) for growing a graphene film (5) and a coating area (3) for depositing a copper film (6); The CVD growth area (2) and the copper film deposition area (3) are connected in sequence.

8. The device for preparing a continuous multilayer copper-graphene composite film according to claim 7, characterized in that: The discharge port of the copper-carrying roller (1) is connected to the CVD growth area (2).

9. The device for preparing a continuous multilayer copper-graphene composite film according to claim 6, characterized in that: The number of the copper-graphene composite film layer preparation units is 2 to 100.

10. The continuous multi-layer copper-graphene composite film preparation device according to claim 6, characterized in that: The number of the copper-graphene composite film layer preparation units is 5.

Citation Information

Patent Citations

  • A copper-plated graphene aluminum-based composite material and its preparation method

    CN112281012B

  • Method for preparing graphene-copper composite material

    CN118060332A

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