Gas reaction device and gas reaction method for preparing graphene

Abstract

The present disclosure relates to a gas reaction device and a gas reaction method for preparing graphene. The device includes a housing and a reaction part and a catalyst circulation mechanism arranged inside the housing; the reaction part includes a catalyst cavity at the lower end for accommodating molten metal catalyst and a gas reaction cavity located above the catalyst cavity. The gas reaction cavity is provided with an air inlet and an air outlet; the catalyst circulation mechanism includes a conveying component and a distribution component. The distribution component is arranged at the top of the gas reaction cavity and has a number of through holes at the bottom. The conveying component continuously conveys the metal catalyst in the catalyst cavity to the distribution component during the gas reaction; the metal catalyst in the cavity of the distribution component oozes out through the through holes, and the reaction gas contacts the catalyst droplets in the gas reaction cavity at the reaction temperature and generates graphene on the surface of the droplets. The graphene drips into the catalyst cavity along with the catalyst; the graphene is separated from the metal catalyst in the catalyst cavity. This device can continuously catalyze the progress of the gas reaction.

Description

Technical Field

[0001] The present disclosure relates to the technical field of gas-phase reactions, and particularly relates to a gas reaction device and a gas reaction method for preparing graphene. Background Art

[0002] Graphene is composed of single or multiple layers of graphite layers and has a two-dimensional hexagonal lattice structure. Due to its unique lattice structure, graphene has many excellent properties, such as: very excellent electron conduction performance, excellent mechanical strength and elasticity, high light transmittance and thermal conductivity. Therefore, since its discovery, graphene has been widely studied and applied in fields such as electronics, optoelectronics, and materials science.

[0003] However, limited by the cost and quality of graphene, the large-scale industrial application of graphene has not been realized. Therefore, to achieve the large-scale application of graphene, the preparation technology of graphene is crucial. The existing graphene preparation technologies mainly include mechanical exfoliation method, oxidation-reduction method, SiC epitaxial growth method, and chemical vapor deposition method (CVD).

[0004] Among them, the mechanical exfoliation method exfoliates graphene from the surface of graphite crystals by mechanical force. This method can ensure the quality of graphene, but its efficiency, yield, and consistency are extremely low, and the cost is extremely high. The oxidation-reduction method prepares graphene through a process of chemical oxidation and reduction. This method can achieve the mass production of graphene, but the prepared graphene has many defects and poor quality. Moreover, this method requires the use of a large amount of strong oxidants, strong acids, and other chemical reagents, posing a high safety risk and possibly causing environmental pollution.

[0005] The SiC epitaxial growth method is to heat a SiC single crystal under high temperature and high vacuum conditions to evaporate the Si atoms on its surface, and the remaining C atoms self-assemble into graphene. The graphene prepared by this method has good quality, but it requires high temperature and vacuum conditions, the preparation method is complex, the yield is low, and the cost is high. The CVD method is that under certain temperature and pressure, a carbon-containing gas (such as methane, ethylene, etc.) thermally cracks into carbon atoms and hydrogen under the catalysis of a substrate (which can be solid or liquid). The carbon atoms adhere to the growth substrate and nucleate and assemble into graphite-like carbon under its catalysis and gradually grow. This method can prepare large-area and high-quality graphene.

[0006] Among the above methods, the graphene produced by the CVD method has very high quality and thus has great potential. However, after graphene grows on the substrate surface, the graphene will completely cover the substrate, making it lose its catalytic activity. Therefore, the existing CVD method can only grow graphene films, that is, it cannot achieve the mass production of graphene powder. Summary of the Invention

[0007] The objective of the present disclosure is to continuously prepare graphene powder by the CVD method, thereby reducing the production cost of graphene powder.

[0008] To achieve the above objective, the present disclosure adopts the following technical solutions:

[0009] Provide a gas reaction device for preparing graphene, including a housing and a reaction part and a catalyst circulation mechanism arranged in the housing;

[0010] The reaction part includes a catalyst cavity arranged at the lower end of the reaction part and a gas reaction cavity located above the catalyst cavity. The catalyst cavity is used to accommodate the melted metal catalyst, and the gas reaction cavity is provided with an air inlet and an air outlet;

[0011] The catalyst circulation mechanism includes a conveying component and a distribution component. The distribution component is arranged at the top of the gas reaction cavity and is provided with a plurality of through holes at the bottom. The conveying component continuously conveys the metal catalyst in the catalyst cavity to the distribution component during the gas reaction;

[0012] The metal catalyst in the distribution component cavity oozes out through the through holes. The reaction gas contacts the dripping metal catalyst droplets at the reaction temperature in the gas reaction cavity and generates graphene on the surface of the metal catalyst droplets. The graphene drips into the catalyst cavity along with the metal catalyst droplets; the graphene is separated from the metal catalyst in the catalyst cavity, and the metal catalyst is copper or an alloy of copper.

[0013] Preferably, the graphene floats on the liquid surface of the metal catalyst with a density greater than itself in the catalyst cavity and is entrained by the airflow introduced into the gas reaction cavity and leaves the gas reaction device through the air outlet.

[0014] Preferably, the aperture of the through hole is 0.1 - 5 mm; or

[0015] A flow guiding member extending towards the catalyst cavity is arranged at the center of the through hole. The metal catalyst oozes out from the gap between the through hole and the flow guiding member and forms a liquid surface on the surface of the flow guiding member. The diameter of the flow guiding member is 5 - 50 mm, and the gap between the flow guiding member and the through hole is 0.1 - 5 mm.

[0016] Preferably, the conveying component includes a conveying channel. The upper end opening of the conveying channel is communicated with the cavity of the distribution component, and the lower end opening of the conveying channel is inserted into the liquid surface of the catalyst cavity;

[0017] A main shaft is arranged inside the conveying channel. The lower end of the main shaft is connected with an axial flow impeller, and the upper end of the main shaft is connected with a motor for controlling the rotation of the main shaft in the conveying channel.

[0018] Preferably, the conveying assembly includes a catalyst turnover bin and a main shaft connecting the catalyst turnover bin, and an opening that can be closed or opened is provided at the lower end of the catalyst turnover bin;

[0019] The upper end of the main shaft is connected to a lifting mechanism that drives the main shaft to reciprocate up and down.

[0020] More preferably, the temperature of the section where the catalyst chamber is located is controlled at 1200 - 1500 °C, the temperature of the section where the distribution assembly and the gas reaction chamber are located is controlled at 900 - 1100 °C, and the temperature of the section where the distribution assembly and the gas reaction chamber are located is 100 - 300 °C lower than the temperature of the section where the catalyst chamber is located.

[0021] Preferably, the gas reaction device generates heat through resistance or induction, and the resistance heating element or the induction heating element is arranged at least around the periphery of the section where the reaction part is located and the section where the distribution assembly is located.

[0022] More preferably, the air inlet is arranged on the bottom side wall of the gas reaction chamber, and the air outlet is arranged on the top side wall of the gas reaction chamber;

[0023] A heat insulation layer is provided in the gap between the reaction part and the catalyst circulation mechanism and the housing, and the heat insulation layer includes a bracket for restraining and supporting the heat insulation material.

[0024] To achieve the above object, the present disclosure also adopts the following technical solutions:

[0025] A gas reaction method for preparing graphene is provided, and the method is carried out in the gas reaction device described in any one of the foregoing items, and includes the following steps:

[0026] 1) Replace the atmosphere in the cavity of the gas reaction device with an inert gas, and then heat the metal catalyst in the catalyst chamber to melting;

[0027] 2) Continuously convey the metal catalyst in the catalyst chamber to the distribution assembly through the conveying assembly, and the metal catalyst oozes out from the through holes of the distribution assembly and drips into the catalyst chamber to form a metal catalyst circulation;

[0028] 3) The reaction gas introduced into the gas reaction chamber contacts the dripping metal catalyst droplets reversely and generates graphene on the surface of the metal catalyst droplets;

[0029] 4) The graphene drops into the catalyst chamber along with the metal catalyst droplets;

[0030] 5) Separate the graphene in the catalyst chamber and continue to circulate the clean metal catalyst to the top of the gas reaction chamber.

[0031] The technical solutions claimed in the present disclosure have achieved the following beneficial effects:

[0032] 1) The graphene on the surface of the liquid metal catalyst can be separated in a timely manner, and the catalyst contacts the reaction gas in a way that continuously circulates and flows to form a new catalyst surface, which can continuously catalyze the gas reaction, improve the gas reaction efficiency, and reduce the gas reaction cost.

[0033] 2) Utilizing the property that the density of graphene is less than that of the catalyst and the interaction force between them causes it to float on the liquid surface of the liquid metal catalyst, the graphene is directly entrained by the gas flow introduced into the gas reaction chamber and leaves the gas reaction device together through the outlet, simplifying the separation of graphene from the catalyst, saving the product separation cost and accelerating the reaction process at the same time.

[0034] 3) The temperatures of the catalyst chamber and the gas reaction chamber are set in a partitioned manner. The surface of the liquid metal catalyst at a higher temperature is conducive to the gas reaction and can rapidly generate graphene; while setting the temperature of the gas reaction chamber lower than that of the catalyst chamber can inhibit the non-catalytic gas-phase cracking of the reaction gas near the catalyst liquid film and reduce the proportion of amorphous carbon in the product. BRIEF DESCRIPTION OF THE DRAWINGS

[0035] In order to more clearly illustrate the technical solutions in the embodiments of the present disclosure, the following will briefly introduce the drawings required for the description of the embodiments. Obviously, the drawings in the following description are only the embodiments of the present disclosure. For those of ordinary skill in the art, without creative efforts, other drawings can also be obtained according to the provided drawings.

[0036] Figure 1 Structural schematic of the gas reaction device Figure 1 。

[0037] Figure 2 Structural schematic of the gas reaction device Figure 2 。

[0038] Reference numerals:

[0039] 1 - housing; 2 - metal catalyst; 3 - inlet; 4 - outlet; 5 - crucible; 6 - heating element; 7 - conveying assembly; 8 - distribution assembly; 9 - through hole; 10 - guiding rod; 11 - heat insulation layer; 12 - motion mechanism; 13 - gas reaction chamber; 14 - catalyst chamber. DETAILED DESCRIPTION OF THE EMBODIMENTS

[0040] To make the objectives, technical solutions, and beneficial effects of the embodiments in the present disclosure clearer, the following will clearly and completely describe the technical solutions in the embodiments of the present disclosure with reference to the accompanying drawings in the embodiments of the present disclosure. Obviously, the described embodiments are some, but not all, of the embodiments of the present disclosure. All other embodiments obtained by those of ordinary skill in the art based on the embodiments in the present disclosure without creative efforts belong to the scope of protection of the present disclosure.

[0041] This embodiment provides a gas reaction device for preparing graphene. Referring to Figure 1 and Figure 2 , the gas reaction device in this embodiment includes a housing 1 and a reaction part and a catalyst circulation mechanism disposed inside the housing 1. The inside of the housing 1 is a sealed cavity. The housing 1 is used to isolate air and maintain the atmosphere and pressure conditions required for the reaction process. Interfaces such as instruments, power supplies, gas inlets and outlets, and power introduction for the catalyst circulation mechanism are provided on the housing.

[0042] The reaction part includes a catalyst cavity disposed at the lower end of the reaction part and a gas reaction cavity located above the catalyst cavity. The catalyst cavity is used to accommodate the molten metal catalyst 2 in a liquid state. The gas reaction cavity is provided with an air inlet 3 and an air outlet 4. The air inlet 3 is disposed on the bottom side wall of the gas reaction cavity, and the air outlet 4 is disposed on the top side wall of the gas reaction cavity, forming an upward gas flow path. The air inlet 3 and the air outlet 4 of the gas reaction cavity are connected to the gas inlet and the gas outlet of the housing 1 through pipelines. In this embodiment, the reaction part can be set as a crucible 5. The metal catalyst is placed at the bottom of the crucible 5. The heat provided by the heating element 6 can melt the metal catalyst to form a molten pool at the bottom of the crucible 5, and the upper section of the crucible 5 is used for gas reaction.

[0043] Exemplarily, the material of the crucible 5 can be graphite, silicon carbide, silicon nitride, alumina, carbon-carbon composite material, and composite materials composed of the above materials. When the crucible 5 is cylindrical, the inner diameter is in the range of 300 - 1500 mm, and the inner height is in the range of 300 - 3000 mm. When the crucible 5 is a rectangular structure, the side length is in the range of 300 - 1500 mm, and the inner height is in the range of 300 - 3000 mm.

[0044] The catalyst circulation mechanism includes a conveying component 7 and a distribution component 8. The distribution component 8 is disposed at the top of the gas reaction cavity and has a plurality of through holes 9 at the bottom. The conveying component 7 continuously conveys the metal catalyst in the catalyst cavity to the distribution component 8 during the gas reaction. The metal catalyst in the cavity of the distribution component 8 oozes out through the through holes 9. The reaction gas contacts the dripping metal catalyst droplets at the reaction temperature in the gas reaction cavity and generates graphene on the surface of the metal catalyst droplets. The graphene drops to the catalyst cavity along with the metal catalyst droplets, and the graphene is separated from the metal catalyst in the catalyst cavity.

[0045] In this embodiment, the function of the conveying component 7 is to lift the molten metal catalyst in the crucible 5 to a certain height and then introduce it into the distribution component 8. After coming into contact with the reaction gas during the dripping process and growing graphene on the surface, the molten metal catalyst will fall back into the crucible 5 and repeat this cycle. Exemplarily, the conveying component 7 is installed on a moving mechanism 12 such as a mechanical lifting mechanism, inserted below the liquid level after the metal catalyst melts, and lifted above the liquid level before the metal catalyst stops heating but solidifies.

[0046] In an exemplary structure, one form of the conveying component 7 can adopt an axial flow blade type. Its main structure includes a conveying channel in the form of a cylinder with open ends. The upper end opening of the cylinder communicates with the cavity of the distribution component 8. A main shaft is arranged in parallel in the cylinder. The lower end of the main shaft is connected to an axial flow blade, and the upper end is connected to a motor. During operation, the lower end of the cylinder and the blade are inserted below the liquid level of the metal catalyst, and the motor drives the axial flow blade to rotate in the cylinder through the main shaft, and the metal catalyst liquid can be lifted along the cylinder and introduced into the distribution component 8.

[0047] Another form of the conveying component 7 can adopt a reciprocating lifting type. Its main structure includes a cylindrical catalyst turnover bin and a main shaft. The lower end of the catalyst turnover bin is provided with an opening that can be closed or opened. The lower end of the main shaft is connected to the catalyst turnover bin, and the upper end is connected to a lifting mechanism that can move up and down reciprocally. The reciprocating lifting mechanism is driven by a motor. Small holes are opened at the bottom of the catalyst turnover bin for the inflow and outflow of the molten metal catalyst. A plug rod is arranged on the small holes to control the closing and opening of the small holes. After starting work, the motor drives the cylinder to be inserted below the liquid level through the reciprocating lifting mechanism, the plug rod is moved away, the molten metal catalyst liquid enters the cylinder, after closing the small holes with the plug holes, the reciprocating mechanism starts to lift upwards. After reaching the cavity of the distribution component, the plug rod is removed, and the molten metal catalyst liquid is introduced into the distribution component 8.

[0048] In this embodiment, the distribution component 8 is used to dynamically generate a new catalyst surface. In an exemplary structure, the distribution component is a buffer melting pool with a through-hole array at the bottom. The aperture of the through-hole 9 is set in the range of 0.1 - 5 mm. The cross-section of the buffer melting pool is the same as that of the crucible 5. After the conveying component 7 introduces the molten metal catalyst liquid into the distribution component 8, the metal catalyst oozes out from the through-hole array under the action of gravity to form metal catalyst droplets, and then drips into the crucible, and then is lifted to the distribution component 8 by the conveying component 7 again. In this way, a large number of new metal catalyst droplets are continuously formed in the reaction section inside the crucible 5.

[0049] In another exemplary structure, refer to Figure 2, the distribution component 8 includes a buffer melting pool with a through-hole array at the bottom, and a diversion rod 10 extending towards the catalyst cavity is assembled at the center of each through-hole 9 (the material of the diversion rod can be selected from graphite, carbon-carbon composite material, tungsten, molybdenum, etc.). The diameter of the diversion rod 10 is 5 - 50 mm, and the length is set to 300 - 3000 mm. An annular gap is formed between the diversion rod 10 and the through-hole 9, and the gap size is between 0.1 - 5 mm. After the metal catalyst liquid is introduced into the cavity of the distribution component 8 by the conveying component 7, the metal catalyst seeps out from the annular gap under the action of gravity and forms a new metal catalyst liquid surface on the surface of the diversion rod 10, and finally flows into the crucible, and then is lifted to the distribution component 8 by the conveying component 7 again. In this way, a new dynamic liquid catalyst surface is continuously formed on the surface of the diversion rod.

[0050] In this embodiment, the temperature of the section where the catalyst cavity is located is controlled at 1200 - 1500 °C, and the temperature of the sections where the distribution component 8 and the gas reaction cavity are located is controlled at 900 - 1100 °C. The temperature of the sections where the distribution component 8 and the gas reaction cavity are located is 100 - 300 °C lower than the temperature of the section where the catalyst cavity is located.

[0051] Exemplarily, the heating element in this embodiment can be composed of a resistive heating material, including iron-chromium-aluminum, silicon carbide rod, silicon molybdenum rod, graphite rod, carbon-carbon composite material, etc. Inside the heat insulation layer, the resistive heating elements are arranged around the crucible and the distribution component on the four sides and the upper and lower surfaces, and can raise the temperature and maintain the temperature within the range of 900 - 1500 °C for a long time.

[0052] In another exemplary structure, the heating element 6 can also be through induction heating. When using induction heating, the induction coil is located outside the heat preservation layer of the gas reaction device, and a conductive cylinder is arranged around the crucible 5 and the distribution component 8 inside the heat preservation layer. When the inductor works, an annular current is formed on the cylinder to generate heat, and then the heat is radiated to the crucible 5 and the distribution component 8.

[0053] In the preferred solution, the gas reaction device in this embodiment also has a heat preservation layer 11 in the gap between the reaction part and the catalyst circulation mechanism and the sealed housing. The heat preservation layer 11 is used to keep the crucible 5 and the metal catalyst inside the crucible warm, reduce heat dissipation, and maintain the temperature of the gas reaction zone. Exemplarily, the heat preservation layer 11 is composed of a heat insulation material and a metal support. The heat insulation material includes mullite fiber cotton, mullite fiber board, carbon felt, carbon fiber felt, etc. or a composite material composed of the above materials combined. The metal support is used to restrain and support the heat insulation material. The heat preservation layer 11 is arranged around the crucible 5 and around and in the upper and lower directions of the distribution component 8 to form a constant temperature space.

[0054] Taking the preparation of graphene as an example, the operation process of the gas reaction device in this embodiment is as follows:

[0055] Before the device starts running, add a metal catalyst (the catalyst is copper and its alloys) into crucible 5. First, displace other atmospheres in the cavity with an inert gas such as nitrogen or argon, and then start heating using heating element 6. The metal in crucible 5 is heated and melted.

[0056] After the device is heated to the preset temperature, insert the lower end of the liquid metal catalyst delivery assembly below the liquid level in the catalyst cavity of crucible 5, and then start the motor of delivery assembly 7 to continuously lift the liquid metal catalyst in the catalyst cavity into distribution assembly 8. After the liquid metal catalyst enters the cavity of distribution assembly 8, it continuously seeps out from the through hole 9 at the bottom and drips downward under the action of gravity, forming a flowing surface of the liquid metal catalyst. The metal catalyst droplets finally enter the catalyst cavity and are then lifted by delivery assembly 7 into distribution assembly 8 again, thus continuously forming a new catalyst surface in a cycle.

[0057] When the circulation of the liquid metal catalyst is established and the system reaches the preset temperature, start introducing gases. The gases include reactive gases (including methane, ethane, propane, ethylene, propylene, and mixtures of the above gases) and carrier gases (including nitrogen, argon, hydrogen, and mixtures of the above gases). It is preferred to use a mixture of methane and nitrogen. In this embodiment, the gas inlet is set at a position of the crucible close to the catalyst liquid level, and the gas outlet is located at the top of crucible 5. The gas flow direction is opposite to the dripping direction of the liquid metal catalyst. During the downward dripping process of the metal catalyst, it meets the reaction gas, and graphene grows on the surface of the metal catalyst. The graphene then flows into the molten pool in the crucible together with the liquid metal catalyst. Since the density of graphene is relatively small, it will be carried away by the gas flow after floating out of the liquid surface and leave the reaction device together from the gas outlet.

[0058] In the solution of this embodiment, the graphene on the surface of the liquid metal catalyst can be separated in time, and the catalyst contacts the reaction gas in a way that continuously circulates and flows to form a new catalyst surface, which can continuously catalyze the gas reaction, improve the gas reaction efficiency, and reduce the gas reaction cost.

[0059] The above-described embodiments are only exemplary descriptions of the present disclosure, and do not limit the scope of the present disclosure. Without departing from the design spirit of the present disclosure, various deformations and improvements made by those of ordinary skill in the art to the technical solutions of the present disclosure shall fall within the protection scope determined by the present disclosure.

Claims

1. A gas reaction device for preparing graphene, characterized in that, It includes a housing and a reaction section and a catalyst circulation mechanism arranged inside the housing; The reaction section includes a catalyst chamber provided at the lower end of the reaction section and a gas reaction chamber located above the catalyst chamber. The catalyst chamber is used to accommodate the melted metal catalyst; the gas reaction chamber is provided with an air inlet on the bottom side wall and an air outlet on the top side wall; The catalyst circulation mechanism includes a conveying component and a distribution component. The distribution component is arranged at the top of the gas reaction chamber and is provided with a number of through holes at the bottom. The conveying component continuously conveys the metal catalyst in the catalyst chamber to the distribution component during the gas reaction; The metal catalyst in the cavity of the distribution component oozes out through the through holes. The reaction gas contacts the dripping metal catalyst droplets in the gas reaction chamber at the reaction temperature and generates graphene on the surface of the metal catalyst droplets. The graphene drops to the catalyst chamber along with the metal catalyst droplets; The graphene is separated from the metal catalyst in the catalyst chamber. The metal catalyst is copper or an alloy of copper; The graphene floats on the liquid surface of the metal catalyst with a density greater than its own in the catalyst chamber and is entrained by the air flow introduced into the gas reaction chamber and leaves the gas reaction device through the air outlet.

2. The gas reaction device according to claim 1, wherein The aperture of the through hole is 0.1 to 5 mm; or A flow guide member extending toward the catalyst chamber is provided at the center of the through hole. The metal catalyst oozes out from the gap between the through hole and the flow guide member and forms a liquid surface on the surface of the flow guide member. The diameter of the flow guide member is 5 to 50 mm, and the gap between the flow guide member and the through hole is 0.1 to 5 mm.

3. The gas reaction device according to claim 1, wherein The conveying component includes a conveying channel. The upper end opening of the conveying channel is communicated with the cavity of the distribution component, and the lower end opening of the conveying channel is inserted into the liquid surface of the catalyst chamber; A main shaft is arranged inside the conveying channel. The lower end of the main shaft is connected with an axial flow impeller, and the upper end of the main shaft is connected with a motor for controlling the rotation of the main shaft in the conveying channel.

4. The gas reaction device according to claim 1, wherein The conveying component includes a catalyst turnover bin and a main shaft connecting the catalyst turnover bin. The lower end of the catalyst turnover bin is provided with an opening that can be closed or opened; The upper end of the main shaft is connected with a lifting mechanism for driving the main shaft to move up and down reciprocally.

5. The gas reaction device according to claim 1, characterized in that, The temperature of the section where the catalyst chamber is located is controlled at 1200 to 1500 °C, the temperature of the section where the distribution component and the gas reaction chamber are located is controlled at 900 to 1100 °C, and the temperature of the section where the distribution component and the gas reaction chamber are located is 100 to 300 °C lower than the temperature of the section where the catalyst chamber is located.

6. The gas reaction device according to claim 5, characterized in that, The gas reaction device is heated by resistance or induction. The resistance heating element or the induction heating element is at least arranged around the periphery of the section where the reaction section is located and the section where the distribution component is located.

7. The gas reaction device according to claim 1, characterized in that, The air inlet is arranged on the bottom side wall of the gas reaction chamber, and the air outlet is arranged on the top side wall of the gas reaction chamber; A heat insulation layer is provided in the gap between the reaction section and the catalyst circulation mechanism and the housing. The heat insulation layer includes a bracket for restraining and supporting the heat insulation material.

8. A gas reaction method for preparing graphene, characterized in that, The method is carried out in the gas reaction device according to any one of claims 1 to 7, and comprises the following steps: 1) Replacing the atmosphere in the cavity of the gas reaction device with an inert gas, and then heating the metal catalyst in the catalyst cavity to melting; 2) Continuously conveying the metal catalyst in the catalyst cavity to the distribution component through the conveying component, and the metal catalyst oozes out from the through holes of the distribution component and drips into the catalyst cavity to form a metal catalyst cycle; 3) The reaction gas introduced into the gas reaction cavity is in reverse contact with the dripping metal catalyst droplets and graphene is generated on the surface of the metal catalyst droplets; 4) The graphene drops into the catalyst cavity along with the metal catalyst droplets; 5) Separating the graphene in the catalyst cavity and continuing to circulate the clean metal catalyst to the top of the gas reaction cavity.

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