A bubbling reaction device and method for continuous production of graphene

By optimizing the structure and components of the bubbling reactor, the intermittent production problem of the liquid metal catalytic reactor was solved, enabling continuous production and stable gas supply of graphene, thus improving production efficiency and environmental friendliness.

CN121695782BActive Publication Date: 2026-05-19TSINGHUA UNIVERSITY +1
View PDF 1 Cites 0 Cited by

Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
TSINGHUA UNIVERSITY
Filing Date
2026-02-14
Publication Date
2026-05-19

AI Technical Summary

Technical Problem

Existing liquid metal catalytic bubbling column reactors can only achieve intermittent production and cannot achieve long-term, large-scale, continuous and stable graphene production. Furthermore, the gas inlet funnel and reaction crucible are inconvenient to clean, and the supply of carbon source gas is unstable.

Method used

Design a bubbling reaction device, including a reactor, an inlet funnel, and a reaction crucible. The outlet end of the inlet funnel is inserted below the surface of the liquid metal catalyst. Gaps are provided between the inlet funnel and the reaction crucible, and between the reaction crucible and the reactor, forming a graphene discharge channel. Stable support is provided by annular baffles and fan-shaped baffles. Combined with a differential pressure transmitter and a tail gas collection pipe, stable gas supply and tail gas treatment are ensured.

Benefits of technology

This enables continuous production of graphene, reduces powder accumulation, improves production stability and environmental friendliness, ensures a stable supply of carbon source gas and timely treatment of exhaust gas, and enhances production efficiency and safety.

✦ Generated by Eureka AI based on patent content.

Smart Images

  • Figure CN121695782B_ABST
    Figure CN121695782B_ABST
Patent Text Reader

Abstract

The application discloses a bubbling type reaction device and method for continuous production of graphene, and belongs to the technical field of graphene preparation equipment, and is used for solving at least one problem in the prior art that a bubbling column type reactor can only realize intermittent production, an air inlet funnel and a reaction crucible are inconvenient to clean, and carbon source gas supply is unstable. In the device, an air inlet is formed in the top end of the reactor, a discharge port is formed in the bottom end, the top end of the reaction crucible is open and the bottom end is closed, the air outlet end of the air inlet funnel is inserted below the liquid level of the liquid metal catalyst of the reaction crucible, the air inlet funnel and the reactor are in sealing connection, the air inlet funnel and the reaction crucible have a first gap, and the reaction crucible and the reactor have a second gap. The method comprises the following steps: preheating the reactor; supplying carbon source gas into the reaction crucible; and performing catalytic pyrolysis reaction of the carbon source gas and the liquid metal catalyst. The application can be used for continuous production of graphene.
Need to check novelty before this filing date? Find Prior Art

Description

Technical Field

[0001] This invention belongs to the technical field of graphene preparation equipment, and particularly relates to a bubbling reaction device and method for continuous graphene production. Background Technology

[0002] Graphene is a natural two-dimensional material composed of sp. 2 Hybridized carbon atoms are connected to three adjacent carbon atoms through σ bonds, forming a hexagonal planar two-dimensional crystal. The electron orbitals in the pz direction are perpendicular to the graphene plane and form large π bonds with surrounding atoms, giving graphene excellent electrical and thermal conductivity as well as mechanical properties, with an electron mobility as high as 200,000 cm⁻¹. 2 With a strength of 130 GPa and an electrical conductivity of 10⁶ S / m, a thermal conductivity of up to 5000 W / (m·K), and a strength of up to 130 GPa, graphene has enormous potential applications in optoelectronic components, chemical power sources, metal corrosion protection, electromagnetic shielding, and thermal conductive materials.

[0003] Graphene powder can be prepared by passing a carbon source gas into a liquid metal catalyst. The generated graphene can float on the surface of the liquid metal catalyst, providing a natural advantage for the low-cost separation and purification of graphene. Compared with traditional solid metal catalysts, liquid metal catalysts have unique advantages such as no carbon deposition, resistance to sintering, and no deactivation, while greatly simplifying the separation process of graphene from the catalyst.

[0004] Currently, the bubble column reactor commonly used in liquid metal catalysis is usually a closed reaction chamber, with carbon source gas supplied from above the closed reaction chamber through an inlet pipe.

[0005] However, since the generated graphene powder floats on the surface of the liquid metal catalyst, as the reaction proceeds, a large amount of graphene powder accumulates, filling the closed reaction chamber and cannot be discharged in time. Therefore, the existing bubble column reactor can only achieve intermittent production and cannot achieve long-term, large-scale, continuous and stable production, which restricts its industrial application. Summary of the Invention

[0006] Based on the above analysis, the present invention aims to provide a bubbling reaction apparatus and method for continuous graphene production, which solves at least one of the following problems in the prior art: the bubbling column reactor can only achieve intermittent production, the gas inlet funnel and reaction crucible are inconvenient to clean, and the carbon source gas supply is unstable.

[0007] The objective of this invention is mainly achieved through the following technical solutions.

[0008] In a first aspect, the present invention provides a bubbling reaction apparatus for continuous graphene production, comprising a reactor and an inlet funnel and a reaction crucible disposed within the reactor; an inlet is provided at the top of the reactor and an outlet is provided at the bottom of the reactor; the top of the reaction crucible is open and the bottom is closed; the outlet of the inlet funnel is inserted below the liquid surface of the liquid metal catalyst in the reaction crucible; the inlet funnel and the reactor are sealed together; a first gap is provided between the inlet funnel and the reaction crucible; a second gap is provided between the reaction crucible and the reactor; the first gap, the second gap, and the outlet are sequentially connected to each other, serving as a graphene discharge channel.

[0009] Furthermore, the inlet funnel includes a first narrowed section and a second narrowed section connected sequentially along the flow direction of the carbon source gas. The slope of the first narrowed section is greater than that of the second narrowed section. The first narrowed section is located outside the reaction crucible, and the second narrowed section is partially inserted below the liquid surface of the liquid metal catalyst in the reaction crucible.

[0010] Furthermore, the bubbling reaction device also includes an annular baffle, which is disposed on the inner wall of the reactor. The outer edge of the annular baffle is fixedly connected to the inner wall of the reactor and conforms to the inner wall of the reactor. The air inlet funnel is placed on the inner edge of the annular baffle, and the inner edge of the annular baffle conforms to the corresponding part of the air inlet funnel.

[0011] Furthermore, the annular baffle is a solid ring structure, with multiple guide and limiting grooves opened on the inner wall of the top of the annular baffle, and guide and limiting blocks provided on the outer wall of the top of the air intake funnel. The guide and limiting blocks are inserted into the guide and limiting grooves and cooperate with each other. The air intake funnel is located in the inner ring area of ​​the annular baffle and the two cooperate with each other.

[0012] Furthermore, the bubbling reaction device also includes a fan-shaped baffle, which is disposed on the inner wall of the reactor. The outer edge of the fan-shaped baffle is fixedly connected to the corresponding part of the inner wall of the reactor. The outer edge of the fan-shaped baffle is conformal to the corresponding part of the inner wall of the reactor. The reaction crucible is placed on the inner edge of the fan-shaped baffle, and the inner edge of the fan-shaped baffle is conformal to the corresponding part of the reaction crucible.

[0013] Furthermore, the bubbling reactor also includes an upper flange head, an opening at the top of the reactor, and the upper flange head is detachably connected to the top of the reactor.

[0014] Furthermore, the bubbling reaction device also includes a lifting ring and a lifting rod. The lifting ring is fixedly connected to the top of the air inlet funnel, one end of the lifting rod is fixedly connected to the lifting ring, and the other end of the lifting rod is fixedly connected to the upper flange head.

[0015] Furthermore, the bubbling reaction device also includes a differential pressure transmitter and / or a pressure gauge installed on the carbon source gas inlet pipe. The differential pressure transmitter is used to monitor the pressure difference in the carbon source gas inlet pipe, and the pressure gauge is used to display the pressure value in the carbon source gas inlet pipe.

[0016] Furthermore, the bubbling reactor also includes a tail gas collection pipe, one end of which is connected to the space above the inlet funnel inside the reactor, and the other end extends to the outside of the reactor and is connected to the tail gas treatment system.

[0017] Secondly, the present invention also provides a continuous production method for graphene, employing the aforementioned bubble-type reaction apparatus for continuous graphene production; the continuous production method includes the following steps:

[0018] Step 1: Preheat the reactor;

[0019] Step 2: Supply carbon source gas from the gas inlet at the top of the reactor and feed it into the reaction crucible through the gas inlet funnel;

[0020] Step 3: The carbon source gas is brought into contact with the liquid metal catalyst to carry out a catalytic pyrolysis reaction, yielding graphene powder;

[0021] Step 4: Graphene powder is discharged from the reactor through the discharge channel.

[0022] Compared with the prior art, the present invention can achieve at least one of the following beneficial effects:

[0023] A) The bubbling reactor for continuous graphene production provided by this invention changes the gas inlet and outlet positions of the reactor. Simultaneously, by setting up a gas inlet funnel and optimizing the positions of the gas inlet funnel, reaction crucible, and reactor, a first gap exists between the gas inlet funnel and the reaction crucible, and a second gap exists between the reaction crucible and the reactor. The first gap, the second gap, and the outlet are sequentially connected to form a graphene discharge channel. This allows the generated graphene powder to be discharged promptly from the top of the reaction crucible along the first gap, the second gap, and the outlet, reducing the accumulation of graphene powder in the reactor and reaction crucible. This enables continuous graphene production and achieves efficient, stable, and continuous conversion of carbon source gas into graphene.

[0024] B) The bubbling reaction device for continuous graphene production provided by the present invention has an outlet end of the gas inlet funnel that extends below the surface of the liquid metal catalyst. This ensures that the gas is in full contact with the liquid metal catalyst and reduces the waste and environmental pollution caused by carbon source gas escaping from the liquid surface, thereby further improving the environmental protection and safety of the production process.

[0025] In this invention, the above-described technical solutions can be combined with each other to achieve more preferred combinations. Other features and advantages of this invention will be set forth in the following description, and some advantages may become apparent from the description or be learned by practicing the invention. The objects and other advantages of this invention can be realized and obtained from what is particularly pointed out in the description and drawings. Attached Figure Description

[0026] The accompanying drawings are for illustrative purposes only and are not intended to limit the invention. Throughout the drawings, the same reference numerals denote the same parts.

[0027] Figure 1 This is a three-dimensional structural schematic diagram of a bubble-type reaction device for continuous graphene production provided in Embodiment 1 of the present invention.

[0028] Figure 2 This is a schematic diagram of the internal structure of a bubble-type reaction device for continuous graphene production provided in Embodiment 1 of the present invention.

[0029] Figure 3 This is a three-dimensional structural diagram of the gas inlet funnel in the bubbling reactor for continuous graphene production provided in Embodiment 2 of the present invention.

[0030] Figure 4 This is a front view of the annular baffle in the bubbling reactor for continuous graphene production provided in Embodiment 2 of the present invention.

[0031] Figure 5 This is a top view of the annular baffle in the bubbling reactor for continuous graphene production provided in Embodiment 2 of the present invention.

[0032] Figure label:

[0033] 1-Reactor; 2-Upper flange end cap; 3-Carbon source gas inlet pipe; 4-Lifting rod; 5-Tail gas collection pipe; 6-Sand core; 7-Lower flange interface; 8-Inlet funnel; 81-First diameter reduction section; 82-Second diameter reduction section; 83-Guide limiting block; 9-Reaction crucible; 10-Fan-shaped baffle; 11-Annular baffle; 111-Guide limiting groove. Detailed Implementation

[0034] Preferred embodiments of the present invention will now be described in detail with reference to the accompanying drawings, which form part of this application and are used together with the embodiments of the present invention to illustrate the principles of the present invention, but are not intended to limit the scope of the present invention.

[0035] Example 1

[0036] This embodiment provides a bubble-type reaction apparatus for continuous graphene production. See [link to relevant documentation]. Figures 1 to 2The reactor includes a reactor 1 and an inlet funnel 8 and a reaction crucible 9 (e.g., a graphite crucible) disposed within the reactor 1. The reactor 1 has an inlet at its top and an outlet at its bottom. The reaction crucible 9 has an open top and a closed bottom. The outlet of the inlet funnel 8 is inserted below the liquid surface of the liquid metal catalyst in the reaction crucible 9. The inlet funnel 8 and the reactor 1 are sealed together. There is a first gap between the inlet funnel 8 and the reaction crucible 9, and a second gap between the reaction crucible 9 and the reactor 1. The first gap, the second gap, and the outlet are connected in sequence to serve as a discharge channel for graphene.

[0037] Compared with the prior art, the bubbling reactor for continuous graphene production provided in this embodiment changes the inlet and outlet positions of reactor 1. Simultaneously, by setting an inlet funnel 8 and optimizing the positions of the inlet funnel 8, reaction crucible 9, and reactor 1, a first gap exists between the inlet funnel 8 and the reaction crucible 9, and a second gap exists between the reaction crucible 9 and reactor 1. The first gap, the second gap, and the outlet are sequentially connected to form a graphene discharge channel. This allows the generated graphene powder to be discharged promptly from the top of the reaction crucible 9 along the first gap, the second gap, and the outlet, reducing the accumulation of graphene powder in reactor 1 and reaction crucible 9. This enables continuous graphene production and achieves efficient, stable, and continuous conversion of carbon source gas into graphene.

[0038] In addition, the outlet end of the inlet funnel 8 is submerged below the surface of the liquid metal catalyst. This ensures that the gas is in full contact with the liquid metal catalyst and reduces the waste and environmental pollution caused by carbon source gas escaping from the liquid surface, thereby further improving the environmental friendliness and safety of the production process.

[0039] It should be noted that the lugs of the reaction crucible 9 are chamfered to reduce the accumulation of graphene powder at this location.

[0040] To address the inconvenience of cleaning the inlet funnel 8 and reaction crucible 9, the aforementioned bubbling reactor for continuous graphene production also includes an upper flange head 2, with an opening at the top of the reactor 1. The upper flange head 2 is detachably connected to the top of the reactor 1. This allows for easy cleaning of the reactor 1's interior simply by removing the upper flange head 2 when cleaning the inlet funnel 8 and reaction crucible 9 is required. This effectively solves the cleaning inconvenience problem in existing technologies and improves the maintenance efficiency and operability of the bubbling reactor.

[0041] To enable the connection between the top of reactor 1 and the carbon source gas supply unit, the aforementioned bubbling reactor for continuous graphene production also includes a carbon source gas inlet pipe 3. The inlet end of the carbon source gas inlet pipe 3 is connected to the carbon source gas supply unit, and the outlet end of the carbon source gas inlet pipe 3 is connected to the space above the gas inlet funnel 8 inside reactor 1 through an inlet hole on the upper flange head 2. In this way, the carbon source gas can smoothly enter reactor 1 through the carbon source gas inlet pipe 3 and fully contact the liquid metal catalyst, thereby reacting to generate graphene.

[0042] It is worth noting that, since part of the inlet funnel 8 needs to be inserted into the liquid metal catalyst, a drop in temperature may cause the inlet funnel 8 to become impossible to remove. Therefore, the aforementioned bubbling reactor for continuous graphene production also includes a lifting rod 4. One end of the lifting rod 4 is fixedly connected to the inlet funnel 8, and the other end is fixedly connected to the upper flange head 2. In this way, by setting up the lifting ring and lifting rod 4, when it is necessary to remove the inlet funnel 8, it can be easily lifted out of the liquid metal catalyst simply by operating the upper flange head, effectively reducing the problem of the inlet funnel 8 becoming impossible to remove due to temperature drops.

[0043] To address the issue of unstable carbon source gas supply and ensure its stability, the aforementioned bubbling reactor for continuous graphene production also includes a differential pressure transmitter and / or pressure gauge mounted on the carbon source gas inlet pipe 3. The differential pressure transmitter monitors the pressure difference within the carbon source gas inlet pipe 3, while the pressure gauge displays the current pressure value. Through their combined use, the carbon source gas supply can be monitored in real time. In case of abnormal supply, such as excessive pressure fluctuations or insufficient supply, timely adjustments can be made to ensure the stability and continuity of the entire graphene production process.

[0044] Meanwhile, in order to prevent the exhaust gas generated during the reaction from accumulating in reactor 1 and affecting the normal progress of the reaction, the above-mentioned bubbling reaction device for continuous graphene production also includes an exhaust gas collection pipe 5. One end of the exhaust gas collection pipe 5 is connected to the space above the air inlet funnel 8 in reactor 1, and the other end extends to the outside of reactor 1 and is connected to the exhaust gas treatment system. In this way, the exhaust gas generated by the reaction can be discharged from reactor 1 in a timely manner through the exhaust gas collection pipe 5, avoiding the exhaust gas from interfering with the reaction and ensuring the cleanliness and safety of the production environment.

[0045] It is worth noting that a certain amount of exhaust gas is generated during the reaction process. Since the exhaust gas has a high calorific value, the outlet of the aforementioned exhaust gas treatment system is connected to a waste heat recovery unit. This allows for the effective recovery and utilization of the calorific value in the exhaust gas, which not only improves energy efficiency and reduces production costs but also reduces thermal pollution caused by direct exhaust gas emissions, further enhancing the environmental performance of the bubbling reactor.

[0046] For example, the distance between the exhaust gas collection pipe 5 and the discharge port at the bottom of the reactor 1 is 8cm to 15cm. In this way, the exhaust gas can blow off the graphene accumulated in the reactor 1, reducing the accumulation and blockage of graphene powder.

[0047] In order to further optimize the gas distribution in the reaction device, the above-mentioned bubbling reaction device for continuous graphene production also includes a sand core 6 located at the gas inlet end of the tail gas collection pipe 5. The sand core 6 has a uniform pore structure and can filter the graphene powder in the tail gas, reducing the amount of graphene powder flowing out of the tail gas collection pipe 5.

[0048] To facilitate graphene collection, the aforementioned bubbling reactor for continuous graphene production also includes a material storage tank, which is detachably connected to the outlet of reactor 1 via a lower flange interface 7. This allows the graphene powder discharged from reactor 1 to smoothly enter the material storage tank for collection. Furthermore, the detachable connection between the material storage tank and reactor 1 facilitates subsequent processing and transfer of the collected graphene, as well as cleaning and maintenance of the material storage tank.

[0049] To address the issue of swaying in the inlet funnel 8 during graphene production, which affects the stability of the gas supply, the aforementioned bubbling reactor for continuous graphene production further includes an annular baffle 11. The annular baffle 11 is disposed on the inner wall of the reactor 1, with its outer edge fixedly connected to the inner wall. The outer edge of the annular baffle 11 is conformal to the inner wall of the reactor 1. The inlet funnel 8 is placed on the inner edge of the annular baffle 11, with the inner edge of the annular baffle 11 conforming to the corresponding portion of the inlet funnel 8. In this way, the annular baffle 11 provides stable support for the inlet funnel 8, effectively reducing swaying during the reaction, thereby ensuring the stability of the carbon source gas supply and guaranteeing the smooth operation of the graphene production process.

[0050] Similarly, to address the issue of reaction crucible 9 shaking and affecting reaction stability during graphene production, the aforementioned bubbling reaction apparatus for continuous graphene production further includes a fan-shaped baffle 10. The fan-shaped baffle 10 is disposed on the inner wall of the reactor 1, with its outer edge fixedly connected to the corresponding portion of the inner wall of the reactor 1. The outer edge of the fan-shaped baffle 10 is conformal to the corresponding portion of the inner wall of the reactor 1. The reaction crucible 9 is placed on the inner edge of the fan-shaped baffle 10, which is also conformal to the corresponding portion of the reaction crucible 9. In this way, the fan-shaped baffle 10 provides stable support for the reaction crucible 9, effectively reducing shaking during the reaction and ensuring reaction stability, thus guaranteeing the efficient operation of the graphene production process.

[0051] For example, there are multiple fan-shaped baffles 10, which are uniformly arranged along the circumference of the reactor 1, with gaps between adjacent fan-shaped baffles 10 so that graphene can pass through smoothly.

[0052] Example 2

[0053] This embodiment provides a bubble-type reaction device for continuous graphene production, the structure of which is basically the same as the bubble-type reaction device for continuous graphene production provided in Embodiment 1, the difference being:

[0054] Considering that the accumulation of graphene powder at the top of the reaction crucible 9 could cause blockage of the first gap and affect the discharge of graphene powder, the structure of the gas inlet funnel 8 is specifically described in [reference needed]. Figure 3 It includes a first narrowed section 81 and a second narrowed section 82 connected sequentially along the direction of carbon source gas flow. The slope of the first narrowed section 81 is greater than that of the second narrowed section 82. The first narrowed section 81 is located outside the reaction crucible 9, and the second narrowed section 82 is partially inserted below the liquid surface of the liquid metal catalyst in the reaction crucible 9.

[0055] It should be noted that the structure of the aforementioned air intake funnel 8 is not a simple improvement in shape, but rather has the following effects:

[0056] As the reaction proceeds, the graphene powder accumulates and becomes more compact. The pressure of the graphene powder received by the second narrowed section 82, which is below the liquid surface of the liquid metal catalyst inserted into the reaction crucible 9, gradually increases. However, since the slope of the first narrowed section 81 is greater than that of the second narrowed section 82, this structure causes the graphene powder to exert an upward thrust on the first narrowed section 81 when it accumulates upward to the junction of the first and second narrowed sections 81 and 82. This causes the inlet funnel 8 to move upward a certain distance. Because the inlet funnel 8 has a narrowed structure, its upward movement increases the first gap, thereby increasing the discharge speed of the graphene powder. This effectively reduces the problem of blockage in the first gap caused by the accumulation of graphene powder, ensuring that graphene can be continuously and stably discharged from the reaction crucible 9, further improving the efficiency and stability of continuous graphene production.

[0057] Furthermore, the upward movement of the inlet funnel 8 reduces the distance between its outlet end and the surface of the liquid metal catalyst in the reaction crucible 9, decreasing the sufficiency of the reaction and consequently reducing the amount of graphene powder produced. Conversely, as the graphene powder's packing density decreases, the upward thrust of the graphene powder on the first narrowing section 81 decreases, causing the inlet funnel 8 to move downwards. This increases the distance between the inlet funnel 8 and the surface of the liquid metal catalyst in the reaction crucible 9, further enhancing the sufficiency of the reaction and resulting in a larger amount of graphene powder produced. Thus, the inlet funnel 8 can automatically adjust its insertion distance into the liquid metal catalyst based on the packing density of the graphene powder, effectively reducing blockage in the first gap while ensuring sufficient reaction density, thereby achieving continuous and stable graphene production.

[0058] It is worth noting that, in order to ensure the airtightness between the air inlet funnel 8 and the reactor 1 during vertical movement, the annular baffle 11 has the following structure: specifically, the annular baffle 11 is a solid ring structure, and multiple guide and limiting grooves 111 are formed on the inner wall of the top of the annular baffle 11. (See [reference]). Figures 4 to 5 Correspondingly, a guide limiting block 83 is provided on the outer wall of the top of the air intake funnel 8, see [reference]. Figure 3The guide limiting block 83 is inserted into the guide limiting groove 111 and they cooperate with each other, meaning that the size of the guide limiting block 83 is the same as the size of the guide limiting groove 111. The air inlet funnel 8 is located in the inner ring area of ​​the annular baffle 11 and the two cooperate with each other, meaning that the outer diameter of the top of the air inlet funnel 8 is equal to the inner diameter of the top of the annular baffle 11. In this way, the cooperation between the guide limiting block 83 and the guide limiting groove 111 can restrict the movement of the air inlet funnel 8 in the horizontal direction, ensuring that the air inlet funnel 8 moves only in the vertical direction. At the same time, the tight cooperation between the annular baffle 11 and the air inlet funnel 8, as well as the sealing effect of the guide limiting block 83 and the guide limiting groove 111, can effectively ensure the airtightness between the air inlet funnel 8 and the reactor 1 during the movement, prevent the leakage of carbon source gas, and ensure the smooth progress of the reaction.

[0059] Example 3

[0060] This embodiment provides a continuous production method for graphene, using the bubble-type reaction apparatus for continuous graphene production provided in Embodiment 1 or Embodiment 2.

[0061] The continuous production method in this embodiment includes the following steps:

[0062] Step 1: Preheat the reactor using an electric heating furnace to a temperature of 700℃~800℃;

[0063] Step 2: Supply carbon source gas from the gas inlet at the top of the reactor and feed it into the reaction crucible through the gas inlet funnel;

[0064] Step 3: The carbon source gas is brought into contact with the liquid metal catalyst to carry out a catalytic pyrolysis reaction, yielding graphene powder;

[0065] Step 4: Graphene powder is discharged from the reactor through the discharge channel.

[0066] Compared with the prior art, the beneficial effects of the continuous graphene production method provided in this embodiment are basically the same as those of the bubble reaction device for continuous graphene production provided in Embodiment 1, and will not be described in detail here.

[0067] The above description is only a preferred embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any changes or substitutions that can be easily conceived by those skilled in the art within the scope of the technology disclosed in the present invention should be included within the scope of protection of the present invention.

Claims

1. A bubble-type reaction device for continuous graphene production, characterized in that, The device includes a reactor and an inlet funnel and a reaction crucible disposed within the reactor. The reactor has an inlet at its top and an outlet at its bottom. The reaction crucible is open at its top and closed at its bottom. The outlet of the inlet funnel is inserted below the surface of the liquid metal catalyst in the reaction crucible. The inlet funnel and the reactor are sealed together. A first gap exists between the inlet funnel and the reaction crucible, and a second gap exists between the reaction crucible and the reactor. The first gap, the second gap, and the outlet are sequentially connected, serving as a graphene discharge channel. The gas inlet funnel includes a first narrowed section and a second narrowed section connected sequentially along the flow direction of the carbon source gas. The slope of the first narrowed section is greater than that of the second narrowed section. The first narrowed section is located outside the reaction crucible, and the second narrowed section is partially inserted below the liquid surface of the liquid metal catalyst in the reaction crucible.

2. The bubble-type reaction apparatus for continuous graphene production according to claim 1, characterized in that, The bubbling reaction device also includes an annular baffle, which is disposed on the inner wall of the reactor. The outer edge of the annular baffle is fixedly connected to the inner wall of the reactor and conforms to the inner wall of the reactor. The air inlet funnel is placed on the inner edge of the annular baffle, and the inner edge of the annular baffle conforms to the corresponding part of the air inlet funnel.

3. The bubble-type reaction apparatus for continuous graphene production according to claim 2, characterized in that, The annular baffle is a solid ring structure. Multiple guide and limiting grooves are opened on the inner wall of the top of the annular baffle. A guide and limiting block is provided on the outer wall of the top of the air intake funnel. The guide and limiting block is inserted into the guide and limiting groove and cooperates with each other. The air intake funnel is located in the inner ring area of ​​the annular baffle and the two cooperate with each other.

4. The bubble-type reaction apparatus for continuous graphene production according to claim 1, characterized in that, The bubbling reaction device also includes a fan-shaped baffle, which is disposed on the inner wall of the reactor. The outer edge of the fan-shaped baffle is fixedly connected to the corresponding part of the inner wall of the reactor. The outer edge of the fan-shaped baffle is conformal to the corresponding part of the inner wall of the reactor. The reaction crucible is placed on the inner edge of the fan-shaped baffle, and the inner edge of the fan-shaped baffle is conformal to the corresponding part of the reaction crucible.

5. The bubble-type reaction apparatus for continuous graphene production according to claim 1, characterized in that, The bubbling reactor also includes an upper flange head, an opening at the top of the reactor, and the upper flange head is detachably connected to the top of the reactor.

6. The bubble-type reaction apparatus for continuous graphene production according to claim 5, characterized in that, The bubbling reaction device also includes a lifting ring and a lifting rod. The lifting ring is fixedly connected to the top of the air inlet funnel, one end of the lifting rod is fixedly connected to the lifting ring, and the other end of the lifting rod is fixedly connected to the upper flange head.

7. The bubble-type reaction apparatus for continuous graphene production according to claim 1, characterized in that, The bubbling reaction device also includes a differential pressure transmitter and / or a pressure gauge installed on the carbon source gas inlet pipe. The differential pressure transmitter is used to monitor the pressure difference in the carbon source gas inlet pipe, and the pressure gauge is used to display the pressure value in the carbon source gas inlet pipe.

8. The bubble-type reaction apparatus for continuous graphene production according to claim 1, characterized in that, The bubbling reactor also includes a tail gas collection pipe, one end of which is connected to the space above the air inlet funnel inside the reactor, and the other end extends to the outside of the reactor and is connected to the tail gas treatment system.

9. A continuous production method for graphene, characterized in that, The continuous production method employs a bubble-type reactor for graphene production as described in any one of claims 1 to 8, comprising the following steps: Step 1: Preheat the reactor; Step 2: Supply carbon source gas from the gas inlet at the top of the reactor and feed it into the reaction crucible through the gas inlet funnel; Step 3: The carbon source gas is contacted with a liquid metal catalyst to carry out a catalytic pyrolysis reaction to obtain graphene powder; Step 4: The graphene powder is discharged from the reactor through the discharge channel.