JP7582711B2 - Continuous production system and method for single-walled carbon nanotubes - Google Patents

Description

The present invention belongs to the field of new materials technology and relates to nanocarbon materials, and in particular to a continuous production system and production method for single-walled carbon nanotubes.

In the field of carbon nanotubes, efforts are being made on how to reduce the amount of defects and improve the structural integrity, and the development is moving in the direction of small tube diameters, low defects and high graphitization. The development of high-performance electronic devices will further promote the development of semiconducting carbon materials, with single-walled carbon nanotubes with controllable structures as the ultimate goal. In order to control the size of the catalyst during the growth of carbon nanotubes, efficiency must be sacrificed. The catalyst is kept at a fairly low concentration so that the particle size of the catalyst is small, and the growth temperature is controlled to avoid agglomeration growth under high temperature conditions. However, due to the small tube diameter and large surface curvature of single-walled carbon nanotubes, a larger activation energy is required to build a stable C-C covalent bond structure, and the high crystallization also depends on high temperature conditions. Therefore, the key point in the production technology of high-quality single-walled carbon nanotubes is to require a higher production reaction temperature, and at the same time, to obtain a highly active catalyst with a stable atomic state that can be sustained, thereby realizing high-efficiency continuous production.

At present, the main methods for producing single-walled carbon nanotubes are chemical vapor deposition, arc ablation, laser, plasma, etc. Chemical vapor deposition is a commonly used method, but it has the disadvantage that the crystallinity of carbon nanotubes is low due to its inherent low reaction temperature, so the single-walled carbon nanotubes produced by chemical vapor deposition have a high defect content. Li Qingwen et al. (Li Qingwen, Yan Hao, Cheng Yan, Zhang Jin, Liu Zhongfan, A scalable CVD synthesis of high-purity single-walled carbon nanotubes with porous MgO as support material, J. Mater. Chem., 2002, 12, 1179-1183) discloses a method for producing single-walled carbon nanotubes by chemical vapor deposition using magnesium oxide as a support and iron as a catalyst. The floating chemical vapor deposition method adopts a gas-phase reaction process without a support, and the purity and quality of the single-walled carbon nanotube product are obviously improved. H.M. Cheng et al. H.M. Cheng, F. Li, X. Sun, S.D.M. Brown, M.A. Pimenta, A. Marucci, G. Dresselhaus, M.S. Dresselhaus, Bulk morphology and diameter distribution of single-walled carbon nanotubes synthesized by catalytic decomposition of hydrocarbons, Chemical Physics Letters 289, 1998. 602-610, discloses a floating chemical vapor deposition method using ferrocene and thiophene as catalysts and ethanol as a carbon source. The aerogel-like single-walled carbon nanotube product can be continuously blown out from the tail end of the tubular furnace, and in subsequent studies, the quality of the single-walled carbon nanotubes was significantly improved by increasing the reaction temperature and adjusting the co-catalyst. Chinese Patent 202010326890.0 discloses an improved floating chemical vapor deposition method for producing single-walled carbon nanotubes. A vertical structure and bottom-to-top gas supply reaction model are adopted, utilizing the natural tendency of the airflow to rise, allowing continuous collection at the top. Chinese Patent 201010234322.4 discloses a method for producing single-walled carbon nanotubes with controllable diameter. Using the high-temperature arc ablation method, carbon powder and metal catalyst are filled into a carbon electrode, and single-walled carbon nanotubes are produced by directly ablation using an arc.

However, due to the huge surface area of single-walled carbon nanotubes, they are very prone to agglomeration and form a membrane. With conventional cyclone separation or filtration methods, the filtration equipment is prone to clogging within a short period of time, making continuous operation impossible. Stable, continuous collection without affecting the high-temperature reaction remains a difficult challenge.

The primary objective of the present invention is to overcome the deficiencies of the prior art and provide an apparatus and method for continuous production of single-walled carbon nanotubes.

In order to achieve the above object of the invention, the technical solution of the present invention is as follows: A continuous single-walled carbon nanotube manufacturing system, the carbon nanotube manufacturing apparatus includes:
a high-temperature reaction chamber for generating a direct current arc flame, evaporating a metal catalyst agent as a counter electrode, and combining with the high-temperature pyrolyzed organic carbon source to catalyze the production of single-walled carbon nanotubes;
a collector for cooling the produced single-walled carbon nanotubes, separating and concentrating the cooled single-walled carbon nanotubes by a magnetic separation method, and collecting the single-walled carbon nanotubes by using a gas blowback;
and an auxiliary unit to assist the high temperature reaction chamber and the collection device to complete the continuous production of single-walled carbon nanotubes.

The high-temperature reaction chamber and the collection device are connected in series. The auxiliary unit is connected to each of the high-temperature reaction chamber and the collection device.

Furthermore, the auxiliary unit includes a vacuum unit, a gas flow passage unit, a power supply unit and a supply unit.

A bottom electrode is placed at the bottom of the high-temperature reaction chamber. A crucible for placing a catalytic agent is placed on the bottom electrode, and the internal arc gun of the high-temperature reaction chamber is inserted at an angle and positioned vertically above the bottom electrode.

An organic carbon source mixed gas connection port is provided on the side wall of the high temperature reaction chamber and extends tangentially along the side wall of the high temperature reaction chamber to the inside of the high temperature reaction chamber, and the height at which the organic carbon source mixed gas connection port is located on the side wall of the high temperature reaction chamber is not higher than the height of the crucible.
The top of the high temperature reaction chamber has an opening facing straight up that is connected to the collector via piping. A supply connection is provided on one side of the top of the high temperature reactor, diagonally above the bottom electrode.

The vacuum unit is connected to the exhaust gas outlet of the gas-solid separator. The gas flow passage unit is connected to the organic carbon source mixed gas connection port and the carrier gas inlet of the high-temperature reaction chamber.

The power supply unit supplies power.

The supply unit is connected to the supply connection port of the high-temperature reaction chamber.

Furthermore, the number of collection devices is one or two.

The collection device includes a transport pipe, a cooling unit, a gas-solid separator and a powder material collection tank.

One end of the transport pipe is connected to the top of the high-temperature reaction chamber, and the other end is connected to the gas-solid separator and the powdered material collection tank via a three-way pipe. An intermediate valve is disposed between the gas-solid separator and the powdered material collection tank. The cooling unit is installed in the transport pipe, so that a cooling chamber is formed inside the transport pipe in which the cooling unit is installed.

The gas-solid separator is provided with an exhaust gas outlet and a blowback inlet, and the blowback inlet is connected to the gas flow path unit.

Furthermore, the high temperature reaction chamber is constructed of a double water-cooled stainless steel housing including a high temperature ceramic lining and a high temperature insulation layer. The lining is corundum or mullite. The high temperature insulation layer is porous ceramic, ceramic fiber felt, hollow ceramic beads, graphite, or graphite felt.

The separation method used in the gas-solid separator is an electronically controlled magnetic separation method. The magnetic field-rich region of the gas-solid separator is formed by converging multiple quartz tubes wrapped with electromagnetic coils.

Another object of the present invention is to provide a method for producing single-walled carbon nanotubes using the above-mentioned continuous single-walled carbon nanotube production system. The method utilizes the high temperature generated by the DC arc flame to evaporate a metal catalyst as a counter electrode, forming catalyst microparticles, which combine with an organic carbon source pyrolyzed at high temperature to catalyze the production of single-walled carbon nanotubes, and then cooling. After cooling, the resulting single-walled carbon nanotube powder is concentrated and separated by a magnetic separation method, and finally, the gas-solid separator is blown back with gas (gas blowback) to obtain single-walled carbon nanotubes with high purity, high productivity, and uniform structure.

More specifically, the method includes the following steps:
S1) Discharge all the air in the system and inject protective gas into the high temperature reaction chamber. Turn on the DC arc gun and form a stable arc with the bottom electrode, then gradually lift the DC arc gun to obtain a specified length of arc flame.
S2) The catalyst is fed into the crucible of the bottom electrode, and the catalyst is evaporated by the action of the arc flame. At the same time, the organic carbon source mixed gas is fed through the mixed gas inlet. The organic carbon source mixed gas forms a spiral upward current and combines with the catalyst microparticles formed by evaporation, and the growth of carbon nanotubes begins.
S3) Using magnetic separation techniques, the cooled carbon nanotubes are concentrated on the inner walls of a collection device.
S4) After the reaction is completed, close the exhaust port of the high temperature reaction chamber, open the collection valve, remove the magnetic field, and use the inert gas blowback to blow the concentrated carbon nanotube product into the powder material collection tank to obtain the final product.

Furthermore, the protective gas in S1) is any one of nitrogen gas, argon gas, and helium gas, or a mixture of these gases.

The arc start gas for the DC arc gun is argon gas or helium gas.

The power of the DC arc gun is greater than 10 kW, the current is 50-600 A, and the arc flame length is 2-50 cm.

Furthermore, the catalyst agent in S2) is a metal catalyst agent.

The metal catalyst is one of iron, cobalt, and nickel, or contains other alloying elements including iron, cobalt, or nickel.

Furthermore, the flow rate of the organic carbon source mixed gas in step S2) is 1 to 50 L/min.

The organic carbon source mixed gas includes an organic carbon source gas, an inert carrier gas, and hydrogen gas.

The volume percentage of the organic carbon source gas is 5-40%, the volume percentage of hydrogen gas is 0.1-40%, and the remainder is an inert carrier gas.

The organic carbon source gas is one or more of methane, ethane, ethylene, acetylene, propylene, propane, ethanol, and methanol.

The inert carrier gas is one of nitrogen gas, argon gas, and helium gas.

Furthermore, in step S3), the product is cooled in a cooling chamber until the temperature is lower than 300°C. The inert gas in step S4) is any one of nitrogen gas, argon gas, and helium gas, or a mixture of any of these gases.

Beneficial Effects of the Invention By using the above technical solutions, the features of the method of the present invention are as follows:

(1) By evaporating the metal catalyst at high arc temperatures, very fine catalyst particles can be obtained and rapidly bonded to the pyrolytic carbon source in situ. This is an effective way to maintain very fine particle size and high activity of the catalyst, avoiding the aggregation and growth of catalyst particles during heating and transportation in the conventional chemical vapor deposition process. This allows the production of single-walled carbon nanotubes with high purity, high yield, and uniform structure.
(2) A high-temperature arc is used as a heat source for evaporating the catalyst and for the chemical reaction. The temperature at the center of the arc flame theoretically reaches 20,000°C, which makes it easier for single-walled carbon nanotubes to grow beyond a large potential barrier, making it possible to produce high-quality single-walled carbon nanotubes. The average Raman IG/ID is significantly higher than that of conventional chemical vapor deposition methods.
(3) Using the principle of electromagnetism to control the separation of gas and solid particles. The magnetic properties of the catalyst in the single-walled carbon nanotube product are utilized to adsorb it onto the quartz tube wall, achieving concentration and separation. Due to the tendency of single-walled carbon nanotubes to adhere and aggregate, the clogging problem caused by the conventional particle filtration separation method can be avoided, and the gas blowback method can be used to realize circulation operation.
(4) The dual system of magnetic gas-solid separator can be used alternately to realize continuous production and collection of the entire system, which is highly efficient, easy to operate, and has high system reliability.

FIG. 1 is a schematic diagram of an apparatus for continuously producing carbon nanotubes using a single collection system according to the present invention. FIG. 2 is a schematic diagram of an apparatus for continuous production of carbon nanotubes using a bottom feed and single collection system according to the present invention. FIG. 3 is a schematic diagram of a continuous carbon nanotube production apparatus using a dual collection system according to the present invention. FIG. 4 is a scanning electron microscope photograph of the single-walled carbon nanotubes produced in the first embodiment. FIG. 5 is a transmission electron microscope photograph of the single-walled carbon nanotubes produced in the first embodiment. FIG. 6 is a diagram showing the Raman spectrum distribution of the single-walled carbon nanotubes produced in the first embodiment. FIG. 7 is a scanning electron microscope photograph of the single-walled carbon nanotubes produced in the second embodiment. FIG. 8 is a transmission electron microscope photograph of the single-walled carbon nanotubes produced in the second embodiment. FIG. 9 is a Raman spectrum curve diagram of the single-walled carbon nanotube produced in the second embodiment.

The technical solution of the present invention is further described below in conjunction with drawings and specific embodiments.

As shown in FIG. 1, in the continuous single-walled carbon nanotube production system of the present invention, the carbon nanotube production apparatus includes the high-temperature reaction chamber 3 for generating a DC arc flame, evaporating a metal catalyst agent as a counter electrode, combining with a high-temperature pyrolyzed organic carbon source, and catalyzing the production of single-walled carbon nanotubes, the collection device for cooling the produced single-walled carbon nanotubes, separating and concentrating the cooled single-walled carbon nanotubes by a magnetic separation method, and collecting them using gas blowback, and the auxiliary unit (not shown) for assisting the high-temperature reaction chamber and collection device and completing the continuous production of single-walled carbon nanotubes.

The high-temperature reaction chamber 3 and the collection device are connected in series. The auxiliary unit is connected to the high-temperature reaction chamber 3 and the collection device, respectively.

The auxiliary unit includes a vacuum unit, a gas flow path unit, a power supply unit, and a supply unit.

A bottom electrode is placed at the bottom of the high-temperature reaction chamber 3. A crucible for placing a catalytic agent is placed on the bottom electrode, and the internal DC arc gun 4 of the high-temperature reaction chamber 3 is inserted at an angle and positioned vertically above the bottom electrode.

An organic carbon source mixed gas connection port 1 is provided on the side wall of the high temperature reaction chamber 3 and extends tangentially along the side wall of the high temperature reaction chamber 3 to the inside of the high temperature reaction chamber 3. The height at which the organic carbon source mixed gas connection port 1 is located on the side wall of the high temperature reaction chamber 3 is not higher than the height of the crucible.
An opening facing directly upward at the top of the high temperature reaction chamber 3 is connected to the collection device via piping. A supply connection port 5 is provided on one side of the top of the high temperature reaction chamber 3, located diagonally above the bottom electrode.

The vacuum unit is connected to the exhaust gas outlet 7 of the gas-solid separator 9. The gas flow passage unit is connected to the organic carbon source mixed gas connection port 1 and the carrier gas inlet of the high-temperature reaction chamber 3.

The power supply unit supplies power.

The supply unit is connected to the supply connection port of the high-temperature reaction chamber.

The number of collection devices is one or two.

The collection device includes a transport pipe 6, a cooling unit, a gas-solid separator 9 and a powder material collection tank 11.

One end of the transport pipe 6 is connected to the top of the high-temperature reaction chamber, and the other end is connected to the gas-solid separator 9 and the powdered material collection tank 11 via a three-way pipe. An intermediate valve 10 is disposed between the gas-solid separator 9 and the powdered material collection tank 11. The cooling unit 13 is installed in the transport pipe 6, so that a cooling chamber is formed inside the transport pipe 6 in which the cooling unit is installed.

The gas-solid separator 9 is provided with an exhaust gas outlet 7 and a blowback inlet 8, and the blowback inlet is connected to the gas flow path unit.

The high temperature reaction chamber 3 is constructed of a double water-cooled stainless steel housing including a high temperature ceramic lining and a high temperature insulation layer. The lining is corundum or mullite. The high temperature insulation layer is porous ceramic, ceramic fiber felt, hollow ceramic beads, graphite or graphite felt.

The separation method used in the gas-solid separator 9 is an electrically controlled magnetic separation method. The magnetic field-rich region of the gas-solid separator is formed by converging multiple quartz tubes wrapped with electromagnetic coils.

A method for producing single-walled carbon nanotubes using the above-mentioned continuous single-walled carbon nanotube production system, in which the method utilizes the high temperature generated by the DC arc flame to evaporate the metal catalyst agent as a counter electrode, form catalyst agent microparticles, combine with the high-temperature pyrolyzed organic carbon source, catalyze the production of single-walled carbon nanotubes, and cool. After cooling, the resulting single-walled carbon nanotube powder is concentrated and separated by a magnetic separation method, and finally, the gas-solid separator is blown back with gas to obtain single-walled carbon nanotubes with high purity, high yield, and uniform structure.

Specifically, the method includes the following steps:

S1) Discharge all the air in the system and inject protective gas into the high temperature reaction chamber. Turn on the DC arc gun and form a stable arc with the bottom electrode, then gradually lift the DC arc gun to obtain a specified length of arc flame.
S2) The catalyst is fed into the crucible of the bottom electrode, and the catalyst is evaporated by the action of the arc flame. At the same time, the organic carbon source mixed gas is fed through the mixed gas inlet. The organic carbon source mixed gas forms a spiral upward current and combines with the catalyst microparticles formed by evaporation, and the growth of carbon nanotubes begins.
S3) Using magnetic separation techniques, the cooled carbon nanotubes are condensed onto the inner walls of a collection device.
S4) After the reaction is completed, close the exhaust port of the high temperature reaction chamber, open the collection valve, remove the magnetic field, and use the inert gas blowback to blow the condensed carbon nanotube product into the powder material collection tank to obtain the final product.

Furthermore, the protective gas in S1) is any one of nitrogen gas, argon gas, and helium gas, or a mixture of these gases.

The arc start gas for the DC arc gun is argon gas or helium gas.

The power of the DC arc gun is greater than 10 kW, the current is 50-600 A, and the arc flame length is 2-50 cm.

Furthermore, the catalyst agent in S2) is a metal catalyst agent.

The metal catalyst is one of iron, cobalt, and nickel, or contains other alloying elements including iron, cobalt, or nickel.

The flow rate of the organic carbon source mixed gas in step S2) is 1 to 50 L/min.

The organic carbon source mixed gas includes an organic carbon source gas, an inert carrier gas, and hydrogen gas.

The volume percentage of the organic carbon source gas is 5-40%, the volume percentage of hydrogen gas is 0.1-40%, and the remainder is an inert carrier gas.

The organic carbon source gas is one or more of methane, ethane, ethylene, acetylene, propylene, propane, ethanol, and methanol.

The inert carrier gas is one of nitrogen gas, argon gas, and helium gas.

In step S3), the product is cooled in a cooling chamber to a temperature lower than 300°C. The inert gas in step S4 is any one of nitrogen gas, argon gas, and helium gas, or a mixture of any of these gases.

The organic carbon source mixed gas connection port may be located at the bottom of the high-temperature reaction chamber. The organic carbon source mixed gas connection port is located on one side of the bottom electrode and crucible 2, as shown in FIG. 2.

The crucible is made of graphite.

The cooling unit is a water-cooled machine.

<Embodiment 1>
The continuous single-walled carbon nanotube production system using the single collection system is configured by connecting a high-temperature reaction chamber 3, a cooling chamber and a gas-solid separator 9 in series, as shown in the schematic diagram of FIG. 1, and is controlled by valves. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is made of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of corundum. A bottom electrode is disposed at the bottom of the high-temperature reaction chamber, and a graphite crucible is provided for containing the catalytic agent. An arc gun is inserted obliquely into the high-temperature reaction chamber and faces the bottom electrode. The organic carbon source mixed gas connection port 1 is provided on the side wall of the high-temperature reaction chamber, so that the organic carbon source mixed gas forms a spiral upward air current and is reliably bonded to the catalytic agent fine particles formed by evaporation. The high-temperature reactor is provided with a supply connection port 5 at an obliquely upward position, so that the catalytic agent supplied from the upper end falls reliably and directly onto the bottom electrode. The gas-solid separator 9 is divided into two parts: a magnetic field-rich region and a powder material collection tank 11, which are connected by an intermediate valve 10. The magnetic field-rich region is provided with an exhaust gas outlet 7 and a blowback inlet 8.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 10 kW, and form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 200 A and a voltage of 50 V to obtain an arc flame with a length of 30 cm. S2) Feed the catalyst agent, which is iron, into the graphite crucible of the bottom electrode by the supply system, and at the same time, put in the organic carbon source gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 45% methane, 50% helium gas, and 5% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic separator, and use magnetic separation technology to concentrate the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After the reaction is completed, close the exhaust port of the high-temperature reaction chamber, open the collection valve, and remove the magnetic field. The quartz tube is blown back using argon gas, an inert gas, and the concentrated carbon nanotube product is blown into a collection tank to obtain the final product.

Product characteristics As shown in Figure 4, which is a scanning electron microscope photograph of the obtained product, the product is pure and the tube bundle is elongated and straight. As shown in Figure 5, which shows a transmission electron microscope photograph, it can be seen that the product is a single-walled carbon nanotube from the isolated single carbon nanotube. As shown in Figure 6, which shows the Raman spectrum curve, the excitation wavelength is 532 nm, and the product has a clear RBM peak (radial breathing mode peak) and a relatively high G/D ratio value, IG/ID = 52.

<Embodiment 2>
The continuous production system for single-walled carbon nanotubes using a dual collection system is constructed by connecting a high-temperature reaction chamber 3 and a collection device in series, as shown in the schematic diagram of FIG. 2, and is controlled by a high-temperature valve 12. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber 3 is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of mullite. A bottom electrode is disposed at the bottom of the high-temperature reaction chamber, and a graphite crucible is provided for containing a catalytic agent. An arc gun is inserted obliquely into the high-temperature reaction chamber and faces the bottom electrode and the crucible 2. An organic carbon source mixed gas connection port 1 is provided at the bottom of the high-temperature reaction chamber 3, so that the reactive gas can reliably enter the high-temperature reaction chamber from the bottom. A supply connection port 5 is provided at the diagonal upper part of the high-temperature reaction chamber, so that the catalytic agent supplied from the upper end can reliably fall directly onto the bottom electrode. Two high-temperature valves 12 are respectively arranged in the transport pipe 6 and the high-temperature reaction chamber 3. The two gas-solid separators 9 are divided into two parts: one is a magnetic field-rich region and the other is a powder material collection tank 11, which are connected respectively by two intermediate valves 10. Each magnetic field-rich region is provided with an exhaust gas outlet 7 and a blowback inlet 8.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 100 kW, and form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 500 A and a voltage of 200 V to obtain an arc flame with a length of 50 cm. S2) Feed the iron catalyst agent into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 5% ethylene, 85% argon gas, and 10% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic gas-solid separator 9, and use magnetic separation technology to condense the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After reacting for a certain time, close the high-temperature valve 12, open the intermediate valve 10, and at the same time, turn on the electromagnetic field of the magnetic gas-solid separator 9 to continue collecting the product. S5) Close the exhaust gas outlet 7, open the intermediate valve 10, and remove the electromagnetic field of the gas-solid separator 9. Supply argon gas from the blowback inlet 8 to blow the product into the powder material collection tank 11 to obtain the final product. S6) Circulate the two gas-solid separators 9 for repeated use and collection. Then, use the supply system to replenish the catalyst agent into the high-temperature reaction chamber from the supply connection port 5, achieving continuous non-stop production.

Product characteristics As shown in the scanning electron microscope photograph of the obtained product in FIG. 6, the product is pure and the tube bundle is elongated and straight. As shown in the transmission electron microscope photograph in FIG. 7, the product is found to be single-walled carbon nanotubes from the isolated single carbon nanotube. As shown in the Raman spectrum curve diagram in FIG. 8, the excitation wavelength is 532 nm, and the product has a clear RBM peak (radial breathing mode peak) and a relatively high G/D ratio value, IG/ID=61.

<Embodiment 3>
The continuous production system of single-walled carbon nanotubes using a single collection system is formed by connecting a high-temperature reaction chamber 3 and a gas-solid separator 9 in series, as shown in the schematic diagram of FIG. 1, and controlled by a valve. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is made of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of corundum. A bottom electrode is arranged at the bottom of the high-temperature reaction chamber, and a graphite crucible is provided for containing the catalytic agent. An arc gun is inserted obliquely into the high-temperature reaction chamber and faces the bottom electrode. An organic carbon source mixed gas connection port 1 is provided at the bottom of the high-temperature reaction chamber, so that the reactive gas can be reliably introduced into the high-temperature reaction chamber from the side wall. A supply connection port 5 is provided at the oblique upper part of the high-temperature reactor, so that the catalytic agent supplied from the upper end can be reliably dropped directly onto the bottom electrode. The gas-solid separator 9 is divided into two parts. One is a magnetic field rich region and the other is a powder material collection tank 11, which are connected by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 17.5 kW, form a stable arc with the bottom electrode, and gradually lift the electrode at a current of 250 A and a voltage of 70 V to obtain an arc flame with a length of 35 cm. S2) Feed the iron catalyst into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 30% acetylene, 55% argon gas, and 15% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic separator, and use magnetic separation technology to concentrate the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After the reaction is completed, close the exhaust port of the high-temperature reaction chamber, open the collection valve, and remove the magnetic field. The quartz tube is blown back using argon gas, an inert gas, and the concentrated carbon nanotube product is blown into a collection tank to obtain the final product.

<Embodiment 4>
The continuous production system for single-walled carbon nanotubes using a dual collection system is constructed by connecting a high-temperature reaction chamber 3 and two sets of collection devices in series, as shown in the schematic diagram of FIG. 3, and controlled by valves. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of mullite. A bottom electrode and a crucible 2 are arranged at the bottom of the high-temperature reaction chamber, and the bottom electrode is equipped with a graphite crucible for containing a catalytic agent. An arc gun inserted obliquely into the high-temperature reaction chamber faces the bottom electrode and the crucible 2. An organic carbon source mixed gas connection port 1 is provided on the side wall of the high-temperature reaction chamber 3, so that the reactive gas can reliably enter the high-temperature reaction chamber 3 from the side wall. A supply connection port 5 is provided at the diagonal upper part of the high-temperature reactor 3, so that the catalytic agent supplied from the upper end can reliably fall directly onto the bottom electrode. Two transport pipes 6 are connected to the high-temperature reaction chamber 3, and high-temperature valves 12 are respectively arranged on the two transport pipes 6. The two gas-solid separators 9 each include a magnetic field rich region and a powdery material collection tank 11, which are connected to the magnetic field rich region by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 120 kW, form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 600 A and a voltage of 200 V to obtain an arc flame with a length of 47 cm. S2) Feed the iron catalyst agent into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 10% ethanol, 75% helium gas, and 15% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic gas-solid separator 9, and use magnetic separation technology to condense the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After reacting for a certain time, close the high-temperature valve 12 and open the intermediate valve 10. At the same time, turn on the electromagnetic field of the magnetic gas-solid separator 9 to continue collecting the product. S5) Close the exhaust gas outlet 7, open the blowback valve, and remove the electromagnetic field of the gas-solid separator 9. Inject argon gas from the blowback inlet 8 to blow the product into the powder material collection tank 11 to obtain the final product. S6) Circulate the gas-solid separator 9 for repeated use and collection. Then, use the supply system to replenish the catalyst agent from the supply connection port 5 to the high-temperature reaction chamber, achieving continuous non-stop production.

<Embodiment 5>
The continuous single-walled carbon nanotube production system using a single collection system is configured by connecting a high-temperature reaction chamber 3, a cooling chamber and a gas-solid separator 9 in series, as shown in the schematic diagram of FIG. 2, and controlled by valves. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is made of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of corundum. A bottom electrode is arranged at the bottom of the high-temperature reaction chamber, and a graphite crucible is provided for containing the catalytic agent. An arc gun is inserted obliquely into the high-temperature reaction chamber and faces the bottom electrode. An organic carbon source mixed gas connection port 1 is provided at the bottom of the high-temperature reaction chamber, so that the reactive gas can be reliably introduced into the high-temperature reaction chamber from the bottom. A supply connection port 5 is provided at the oblique upper part of the high-temperature reactor, so that the catalytic agent fed from the upper end can be reliably dropped directly onto the bottom electrode. The gas-solid separator 9 is divided into two parts. One is a magnetic field rich region and the other is a powder material collection tank 11, which are connected by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 48 kW, form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 400 A and a voltage of 120 V to obtain an arc flame with a length of 40 cm. S2) Feed the iron catalyst agent into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas consists of 38% methane, 2% ethylene, 40% argon gas, and 20% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic separator, and use magnetic separation technology to concentrate the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After the reaction is completed, close the exhaust port of the high-temperature reaction chamber, open the collection valve, and remove the magnetic field. The quartz tube is blown back using argon gas, an inert gas, and the concentrated carbon nanotube product is blown into a collection tank to obtain the final product.

<Embodiment 6>
The continuous production system for single-walled carbon nanotubes using a dual collection system is constructed by connecting a high-temperature reaction chamber 3 and two collection devices in series, as shown in the schematic diagram of FIG. 3, and controlled by valves. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of mullite. A bottom electrode and a crucible 2 are arranged at the bottom of the high-temperature reaction chamber, and a graphite crucible is provided for containing a catalytic agent. An arc gun inserted obliquely into the high-temperature reaction chamber faces the bottom electrode and the crucible 2. An organic carbon source mixed gas connection port 1 is provided on the side wall of the high-temperature reaction chamber, so that the reactive gas can reliably enter the high-temperature reaction chamber from the bottom. A supply connection port 5 is provided at the diagonal upper part of the high-temperature reactor, so that the catalytic agent fed from the upper end can reliably fall directly onto the bottom electrode. Two transport pipes 6 are connected to the high-temperature reaction chamber 3, and each of the two transport pipes 6 is provided with a high-temperature valve 12. The two gas-solid separators 9 each have a magnetic field-rich region, one part of which is a powder material collection tank 11, and are connected to each other by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field-rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 90 kW, and form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 500 A and a voltage of 180 V to obtain an arc flame with a length of 46 cm. S2) Feed the iron catalyst into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 25% propane, 55% helium gas, and 20% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic gas-solid separator 9, and use magnetic separation technology to condense the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After reacting for a certain time, close the high-temperature valve 12, open the intermediate valve 10, and at the same time, turn on the electromagnetic field of the magnetic gas-solid separator 9 to continue collecting the product. S5) Close the exhaust gas outlet 7, open the blowback valve, and remove the electromagnetic field from the gas-solid separator 9. Argon gas is introduced from the blowback inlet 8, and the product is blown into the powder material collection tank 11 to obtain the final product. S6) The gas-solid separator 9 is circulated to be repeatedly used and collected. Then, the supply system is used to replenish the catalyst agent from the supply connection port 5 to the high-temperature reaction chamber, achieving continuous non-stop production.

<Embodiment 7>
The continuous production system of single-walled carbon nanotubes using a single collection system is constructed by connecting a high-temperature reaction chamber 3 and a collection device in series, as shown in the schematic diagram of FIG. 1, and controlled by a valve. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of corundum. A bottom electrode and a crucible 2 are arranged at the bottom of the high-temperature reaction chamber. The crucible is used to put the catalyst agent and is made of graphite. The arc gun, which is inserted obliquely into the high-temperature reaction chamber, faces the bottom electrode. The organic carbon source mixed gas connection port 1 is provided at the bottom of the high-temperature reaction chamber, so that the reaction gas can be surely introduced into the high-temperature reaction chamber from the bottom. A supply connection port 5 is provided obliquely above the high-temperature reactor, so that the catalyst agent supplied from the upper end can be surely dropped directly to the bottom electrode. The gas-solid separator 9 is divided into two parts. One is a magnetic field rich region and the other is a powder material collection tank 11, which are connected by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 80 kW, and form a stable arc with the bottom electrode, and gradually lift the electrode at a current of 450 A and a voltage of 150 V to obtain an arc flame with a length of 43 cm. S2) Feed the iron catalyst agent into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 20% ethane, 5% propylene, 50% helium gas, and 25% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic separator, and use magnetic separation technology to concentrate the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After the reaction is completed, close the exhaust port of the high-temperature reaction chamber, open the collection valve, and remove the magnetic field. The quartz tube is blown back using argon gas, an inert gas, and the concentrated carbon nanotube product is blown into a collection tank to obtain the final product.

<Embodiment 8>
The continuous production system for single-walled carbon nanotubes using a dual collection system is constructed by connecting a high-temperature reaction chamber 3 and two collection devices in series, as shown in the schematic diagram of FIG. 3, and is controlled by a high-temperature valve 12. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber 3 is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of mullite. A bottom electrode and a crucible 2 are arranged at the bottom of the high-temperature reaction chamber 3, and a catalyst agent is placed in the graphite crucible. An arc gun inserted obliquely into the high-temperature reaction chamber faces the bottom electrode and the crucible 2. An organic carbon source mixed gas connection port 1 is provided on the side wall of the high-temperature reaction chamber, so that the reaction gas can reliably enter the high-temperature reaction chamber 3 in a spiral shape from the side wall. A supply connection port 5 is provided diagonally above the high-temperature reactor, so that the catalyst agent supplied from the upper end can reliably fall directly onto the bottom electrode. Two transport pipes 6 are connected to the high-temperature reaction chamber 3, and each of the two transport pipes 6 is provided with a high-temperature valve 12. The gas-solid separator 9 is divided into a magnetic field enriched region, one part of which is a powder material collection tank 11, and is connected by an intermediate valve 10. The magnetic field enriched region is provided with an exhaust gas outlet 7 and a blowback inlet 8.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 50 kW, form a stable arc with the bottom electrode, and gradually lift the electrode at a current of 400 A and a voltage of 120 V to obtain an arc flame with a length of 38 cm. S2) Feed the iron catalyst into the graphite crucible of the bottom electrode by the feeding system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas is 30% acetylene, 55% argon gas, and 15% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic gas-solid separator 9, and use magnetic separation technology to condense the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After reacting for a certain time, close the high-temperature valve 12 and open the intermediate valve 10. At the same time, turn on the electromagnetic field of the magnetic gas-solid separator 9 to continue collecting the product. S5) Close the exhaust gas outlet 7, open the blowback valve, and remove the electromagnetic field of the gas-solid separator 9. Inject argon gas from the blowback inlet 8, and blow the product into the powder material collection tank 11 to obtain the final product. S6) Circulate the gas-solid separator 9 for repeated use and collection. Then, use the supply system to replenish the catalyst agent from the supply connection port 5 to the high-temperature reaction chamber, achieving continuous non-stop production.

<Embodiment 9>
The continuous production system of single-walled carbon nanotubes using a double collection system is formed by connecting a high-temperature reaction chamber 3 and a collection device in series, and controlled by a valve, as shown in the schematic diagram of FIG. 3. In addition, the auxiliary system includes vacuum, gas flow path, control, cooling and supply systems, etc. The outer layer of the high-temperature reaction chamber is composed of a double water-cooled stainless steel housing including a graphite lining and a high-temperature insulation layer, and the inner wall is made of mullite. A bottom electrode and a crucible 2 are arranged on the side wall of the high-temperature reaction chamber, and a catalyst agent is placed in the graphite crucible. An arc gun inserted obliquely into the high-temperature reaction chamber 3 faces the bottom electrode and the crucible 2. An organic carbon source mixed gas connection port 1 is provided on the side wall of the high-temperature reaction chamber, so that the reaction gas can be reliably introduced into the high-temperature reaction chamber from the bottom. A supply connection port 5 is provided at the oblique upper part of the high-temperature reactor, which ensures that the catalyst agent fed from the top falls directly onto the bottom electrode. A high-temperature valve 12 is disposed in the transport pipe 6 and the high-temperature reaction chamber 3, respectively. The gas-solid separator is divided into two parts: a magnetic field-rich region and a powder material collection tank 11, which are connected by an intermediate valve 10. An exhaust gas outlet 7 and a blowback inlet 8 are provided in the magnetic field-rich region.

Manufacturing process S1) Turn on the vacuum system, exhaust all the air in the entire system, and inject argon protective gas. Then, turn on the DC arc gun with a power of 100 kW, form a stable arc with the bottom electrode, and gradually lift the electrode with a current of 500 A and a voltage of 200 V to obtain an arc flame with a length of 50 cm. S2) Feed the iron catalyst agent into the graphite crucible of the bottom electrode by the supply system, and at the same time, feed the organic carbon source mixed gas from the mixed gas inlet. Here, the organic carbon source mixed gas consists of 40% methane, 2% ethylene, 3% ethanol, 40% argon gas, and 15% hydrogen gas. The growth of carbon nanotubes begins. S3) Turn on the electromagnetic field of the magnetic gas-solid separator 9, and use magnetic separation technology to condense the carbon nanotubes cooled in the cooling chamber on the inner wall of the quartz tube. S4) After reacting for a certain time, close the high-temperature valve 12 and open the left high-temperature valve 12. At the same time, turn on the electromagnetic field of the magnetic gas-solid separator 9 and continue to collect the product. S5) Close the exhaust gas outlet 7, open the intermediate valve 10, and remove the electromagnetic field of the gas-solid separator 9. Argon gas is introduced from the blowback inlet 8, and the product is blown into the powder material collection tank 11 to obtain the final product. S6) Circulate the gas-solid separator 9 for repeated use and collection. Then, use the supply system to replenish the catalyst agent from the supply connection port 15 to the high-temperature reaction chamber, achieving continuous non-stop production.

The above content is intended to explain the technical concept of the present invention, and does not limit the scope of protection of the present invention. Any modifications that can be made based on the technical solution means in accordance with the technical concept of the present invention are included in the scope of protection of the claims of the present invention.

1: Organic carbon source mixed gas inlet 2: Bottom electrode and crucible 3: High temperature reaction chamber 4: DC arc gun 5: Supply connection port 6: Transport pipe 7: Exhaust gas outlet 8: Blowback inlet 9: Gas-solid separator 10: Intermediate valve 11: Powdered material collection tank 12: High temperature valve 13: Cooling unit

Claims (10)

A continuous production system for single-walled carbon nanotubes, comprising:
a high-temperature reaction chamber for generating a direct current arc flame, evaporating a metal catalyst agent as a counter electrode, and combining with the high-temperature pyrolyzed organic carbon source to catalyze the production of single-walled carbon nanotubes;
a collecting device for cooling the produced single-walled carbon nanotubes, separating and concentrating the cooled single-walled carbon nanotubes by a magnetic separation method, and collecting the single-walled carbon nanotubes by using a gas blowback;
and an auxiliary unit for assisting the high temperature reaction chamber and the collection device to complete the continuous production of single-walled carbon nanotubes;
A continuous production system for single-walled carbon nanotubes, characterized in that the high-temperature reaction chamber and the collection device are connected in series, and the auxiliary unit is connected to each of the high-temperature reaction chamber and the collection device. A system for continuously producing single-walled carbon nanotubes, comprising:
The auxiliary unit includes a vacuum unit, a gas flow passage unit, a power supply unit, and a supply unit;
A bottom electrode is disposed at the bottom of the high-temperature reaction chamber, a crucible for placing a catalytic agent is disposed on the bottom electrode, and an internal arc gun inserted obliquely into the high-temperature reaction chamber is positioned vertically above the bottom electrode;
an organic carbon source mixed gas connection port is provided on a side wall of the high-temperature reaction chamber, and extends tangentially along the side wall of the high-temperature reaction chamber to the inside of the high-temperature reaction chamber, and the height at which the organic carbon source mixed gas connection port is located on the side wall of the high-temperature reaction chamber is not higher than the height of the crucible;
The opening facing directly upward at the top of the high temperature reaction chamber is connected to the collector via a pipe, and a supply connection port is provided on one side of the top of the high temperature reaction chamber, which is located diagonally above the bottom electrode;
The vacuum unit is connected to an exhaust gas outlet of the gas-solid separator, and the gas flow passage unit is connected to an organic carbon source mixed gas connection port and a carrier gas inlet of a high-temperature reaction chamber, respectively;
The power supply unit supplies power;
2. The system for continuously producing single-walled carbon nanotubes according to claim 1, wherein the supply unit is connected to a supply connection port of a high-temperature reaction chamber. The number of the collection devices is one or two;
The collection device includes a transport pipe, a cooling unit, a gas-solid separator, and a powder material collection tank;
One end of the transport pipe is connected to the top of the high temperature reaction chamber, and the other end is connected to the gas-solid separator and the powder material collection tank through a three-way pipe, and an intermediate valve is disposed between the gas-solid separator and the powder material collection tank. The cooling unit is installed in the transport pipe, so that a cooling chamber is formed inside the transport pipe in which the cooling unit is installed.
3. The continuous production system for single-walled carbon nanotubes according to claim 2, characterized in that the gas-solid separator is provided with an exhaust gas outlet and a blowback inlet, and the blowback inlet is connected to the gas flow path unit. The continuous single-walled carbon nanotube production system according to claim 2, characterized in that the high-temperature reaction chamber is comprised of a double water-cooled stainless steel housing including a high-temperature ceramic lining and a high-temperature insulation layer, the lining being corundum or mullite, and the high-temperature insulation layer being porous ceramic, ceramic fiber felt, hollow ceramic beads, graphite or graphite felt. The continuous single-walled carbon nanotube production system according to claim 3, characterized in that the separation method used in the gas-solid separator is an electronically controlled magnetic separation method, and the magnetic field-rich region of the gas-solid separator is formed by converging multiple quartz tubes around which electromagnetic coils are wound. A method for producing single-walled carbon nanotubes using the continuous single-walled carbon nanotube production system according to any one of claims 1 to 5, the method comprising: utilizing high temperatures generated by a DC arc flame to evaporate a metal catalyst as a counter electrode, forming fine particles of the catalyst, combining with a high-temperature pyrolyzed organic carbon source, catalyzing the production of single-walled carbon nanotubes, cooling, concentrating and separating the resulting single-walled carbon nanotube powder by a magnetic separation method after cooling, and finally blowing back the gas-solid separator with a gas to obtain single-walled carbon nanotubes with high purity, high yield, and uniform structure. S1) Discharge all the air in the system, inject protective gas into the high temperature reaction chamber, turn on the DC arc gun, form a stable arc with the bottom electrode, gradually lift the DC arc gun to obtain a specified length of arc flame;
S2) supplying a catalytic agent into the crucible of the bottom electrode, and evaporating the catalytic agent by the action of the arc flame; at the same time, feeding an organic carbon source mixed gas from the mixed gas inlet, the organic carbon source mixed gas forms a spiral upward air current, and combines with the catalytic agent microparticles formed by evaporation, and carbon nanotube growth begins;
S3) Condensing the cooled carbon nanotubes onto the inner wall of a collection device using a magnetic separation technique;
S4) after the reaction is completed, closing the exhaust port of the high-temperature reaction chamber, opening the collection valve, removing the magnetic field, and using the inert gas blowback to blow the condensed carbon nanotube product into a powder material collection tank to obtain the final product. The protective gas in S1) is any one of nitrogen gas, argon gas, and helium gas, or a mixture thereof;
The arc start gas of the DC arc gun is argon gas or helium gas,
8. The method according to claim 7, wherein the power of the DC arc gun is greater than 10 kW, the current is 50-600 A, and the flame length of the arc is 2-50 cm. The catalyst in S2) is a metal catalyst;
The metal catalyst is any one of iron, cobalt, and nickel, or contains other alloy elements including iron, cobalt, or nickel;
The flow rate of the organic carbon source mixed gas in the step S2) is 1 to 50 L/min;
The organic carbon source mixed gas comprises an organic carbon source gas, an inert carrier gas, and a hydrogen gas;
the volume percent of said organic carbon source gas is between 5 and 40%, the volume percent of hydrogen gas is between 0.1 and 40%, and the remainder is an inert carrier gas;
the organic carbon source gas is one or more of methane, ethane, ethylene, acetylene, propylene, propane, ethanol, and methanol;
8. The method according to claim 7, wherein the inert carrier gas is any one of nitrogen gas, argon gas, and helium gas. The method according to claim 7, characterized in that in step S3), the product is cooled in a cooling chamber to a temperature lower than 300°C, and in step S4), the inert gas is any one of nitrogen gas, argon gas, and helium gas, or a mixture thereof.

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