Copper foil-graphene composite material based on CVD (Chemical Vapor Deposition) and hot rolling embedding method and preparation process of copper foil-graphene composite material

Abstract

The invention discloses a copper foil-graphene composite material based on CVD (chemical vapor deposition) and a hot rolling embedding method and a preparation process of the copper foil-graphene composite material. The preparation method comprises the following steps: by taking a copper foil of 0.5 mm as a substrate, introducing CH1 / H2 mixed gas (CH15-15sccm and H2 30-70sccm) at 1000-1100 DEG C through a CVD (Chemical Vapor Deposition) method to grow double-layer graphene; and then heating to 380-400 DEG C under the protection of argon, and carrying out single-pass hot rolling in a two-roller mill (the reduction rate is 15%, the total deformation is 75%, the roller speed is 0.3-0.7 m / s, and the rolling force is 150-250 kN). According to the technology, a specific temperature window is matched with single-pass large-deformation rolling, copper matrix dynamic recrystallization and graphene low-damage embedding are achieved, the damage rate of graphene is reduced to be smaller than 5%, the interface bonding strength is improved to 150-180 MPa (improved by 80% compared with a traditional technology), and meanwhile the production period is shortened by 50% or above. The obtained composite material has high conductivity (gt; 5.8 * 10 < 7 > S / m), high strength (the tensile strength is improved by 40%) and excellent thermal conductivity (450W / (m * K)), and is suitable for high-performance electronic devices and energy storage electrodes.

Description

Technical Field

[0001] The present invention belongs to the field of materials science, and specifically relates to a copper foil-graphene composite material and a preparation method thereof, which is suitable for fields requiring high-performance composite materials such as electronic devices and energy storage. Background Art

[0002] Copper foil is widely used in electronics due to its conductivity, but it suffers from drawbacks such as low strength and susceptibility to oxidation. Graphene possesses excellent mechanical, electrical, and thermal properties, but existing composite processes suffer from issues such as loose graphene bonding, uneven layer number, long production cycles, and high interfacial stress (e.g., multiple rolling passes can result in graphene damage rates exceeding 20% ​​and bond strengths of only 80-100 MPa). A highly efficient and stable composite process is urgently needed. Summary of the Invention

[0003] The present invention provides a copper foil-graphene composite material and a preparation process thereof. By CVD growth of double-layer graphene and 380-400°C single-pass large deformation hot rolling, graphene is embedded in copper foil grains with low damage (<5%), significantly improving the interface bonding strength (150-180MPa).

[0004] Technical Solution

[0005] Composite material structure: Double-layer graphene is composited on the surface of copper foil. After hot rolling at 380-400℃, the graphene is embedded in the copper grains to form a tight composite.

[0006] Preparation process:

[0007] CVD growth of graphene: Using 0.5mm copper foil as the substrate, introduce CH4 (5-15sccm) and H2 (30-70sccm) at 1000-1100°C for 20-40 minutes to grow double-layer graphene;

[0008] Atmosphere protection heating: heat the composite to 380-400℃ under argon protection;

[0009] Single-pass hot rolling: single-pass rolling on a two-roll mill (roll speed 0.3-0.7 m / s, rolling force 150-250 kN), with a reduction rate of 15% and a total deformation of 75%.

[0010] Beneficial effects

[0011] Low-damage composite: Single-pass large deformation rolling causes graphene to be rolled into copper grains, with a damage rate of <5% (conventional process >20%);

[0012] High bonding strength: interface bonding strength reaches 150-180MPa (traditional process 80-100MPa);

[0013] Efficient production: a single rolling pass replaces 4-6 processes, shortening the cycle by more than 50%;

[0014] Performance improvement: electrical conductivity of composite materials>5.8×10 7 S / m, tensile strength increased by 40%, and thermal conductivity reached 450W / (m·K). DETAILED DESCRIPTION

[0015] The present invention is further described below with reference to specific examples, but the protection scope of the present invention is not limited to these examples.

[0016] Example 1

[0017] The CVD method is used to composite two layers of graphene on copper foil: the copper foil is placed in a reactor, methane and hydrogen are used as reaction gases, the methane flow rate is controlled to be 10 sccm, the hydrogen flow rate is 50 sccm, the reaction temperature is 1050°C, and the reaction time is 30 minutes, so that graphene grows on the surface of the copper foil to form a two-layer graphene structure.

[0018] The copper foil composited with graphene is placed in an atmosphere furnace: argon is used as the protective gas, heated to 380°C, and hot rolled.

[0019] After heat treatment in an atmosphere furnace, the copper foil-graphene composite was hot-rolled on a two-roll mill at a roll speed of 0.5 m / s and a rolling force of 200 kN to a 50% reduction. This further refined the copper foil grains and further thinned the bilayer graphene during the hot rolling process, resulting in the final copper foil-graphene composite. Performance testing of the resulting copper foil-graphene composite revealed excellent electrical conductivity, high strength, and high thermal conductivity, meeting the application requirements of high-performance composite materials.

[0020] Example 2

[0021] CVD graphene growth: Using the CVD method, a two-layer graphene layer is grown on copper foil. The copper foil is placed in a reactor. Methane and hydrogen are used as the reaction gases, with a methane flow rate of 8 sccm and a hydrogen flow rate of 60 sccm. The reaction temperature is raised to 1080°C and the reaction time is extended to 35 minutes. This promotes the growth of graphene on the copper foil surface, forming a uniform two-layer graphene structure.

[0022] Atmosphere furnace heating: The copper foil composited with graphene is sent into the atmosphere furnace, argon gas is introduced for protection, and heated to 390°C in preparation for the hot rolling process.

[0023] Hot Rolling: The copper foil-graphene composite, heated in an atmosphere furnace, was hot rolled using a two-roll mill. The roll speed was maintained at 0.4 m / s, the rolling force was adjusted to 220 kN, and the rolling reduction was 60%. During this process, the copper foil grains became more refined, the bilayer graphene was further thinned, and more evenly incorporated into the grains, resulting in a copper foil-graphene composite material. Testing has shown that this composite exhibits excellent electrical conductivity, strength, and thermal conductivity, demonstrating good suitability for practical applications.

[0024] Example 3

[0025] CVD process: Two layers of graphene are grown on copper foil using the CVD method. In a reactor, the copper foil serves as the substrate, and methane and hydrogen are used as the reaction gases. The methane flow rate is controlled at 12 sccm, the hydrogen flow rate is 40 sccm, the reaction temperature is set at 1020°C, and the reaction time is 25 minutes. The graphene is successfully grown into a two-layer structure on the copper foil surface.

[0026] Atmosphere furnace operation: The copper foil composited with graphene is placed into an atmosphere furnace and heated to 400°C under argon protection to make the copper foil reach a state suitable for hot rolling.

[0027] Hot Rolling: The heated copper foil-graphene composite is hot rolled using a two-roll mill at a roll speed of 0.6 m / s and a rolling force of 180 kN, reaching a 40% reduction. The resulting copper foil-graphene composite exhibits excellent grain refinement and a close bond between the graphene and copper foil. Performance testing confirms that all performance indicators meet the standards for high-performance composite materials, demonstrating its potential for application in related fields.

[0028] Example 4

[0029] CVD graphene production: CVD technology was used to composite two layers of graphene onto the copper foil surface. The reaction gases used were methane and hydrogen, with a methane flow rate of 9 sccm and a hydrogen flow rate of 55 sccm. The reaction temperature was maintained at 1060°C for 32 minutes, achieving uniform growth of graphene on the copper foil, forming a two-layer structure.

[0030] Atmosphere furnace heating stage: put the copper foil compounded with graphene into the atmosphere furnace, introduce argon protection, and heat it to 385℃ to ensure that the copper foil is ready for subsequent hot rolling.

[0031] Hot Rolling: The copper foil-graphene composite is hot rolled on a two-roll mill at a roll speed of 0.55 m / s and a rolling force of 210 kN, reaching a 55% reduction. The resulting copper foil-graphene composite material exhibits uniform structure and excellent performance, with outstanding electrical conductivity, strength, and thermal conductivity, meeting the needs of a variety of high-performance applications.

[0032] Example 5

[0033] CVD growth: A two-layer graphene structure is formed on copper foil using the CVD method. In the reactor, methane and hydrogen are used as reactant gases, with a methane flow rate of 11 sccm and a hydrogen flow rate of 45 sccm. The reaction temperature is 1040°C, and the reaction time is controlled within 28 minutes, allowing the graphene to grow on the copper foil surface, forming a two-layer structure.

[0034] Atmosphere furnace heating: The copper foil composited with graphene is fed into an atmosphere furnace and heated to 395°C under argon protection to provide a suitable material state for hot rolling.

[0035] Hot Rolling: The heated copper foil-graphene composite is hot rolled on a two-roll mill at a roll speed of 0.45 m / s and a rolling force of 230 kN, reaching a 45% reduction. The resulting copper foil-graphene composite material has been tested to exhibit excellent overall performance and has potential applications in electronics, energy, and other fields.

[0036] The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent replacements, improvements, etc. made within the spirit and principles of the present invention shall be included in the scope of protection of the present invention.

Claims

1. A process for preparing a copper foil-graphene composite material, characterized in that include: (a) Double-layer graphene was grown on the surface of copper foil by CVD method; (b) heating the material obtained in step (a) to 380-400° C. in an inert atmosphere; (c) Single-pass hot rolling, 15% reduction, 75% total deformation.

2. The process according to claim 1, characterized in that: The CVD reaction gas is a mixture of CH1 and H2, with a CH1 flow rate of 5-15 sccm, a H2 flow rate of 30-70 sccm, a temperature of 1000-1100° C., and a time of 20-40 minutes.

3. The process according to claim 1, characterized in that: Hot rolling is carried out on a two-roll mill with a roll speed of 0.3-0.7 m / s and a rolling force of 150-250 kN.

4. A copper foil-graphene composite material obtained by the process of any one of claims 1 to 3, characterized in that: The graphene damage rate is less than 5%, and the interface bonding strength is 150-180MPa.