Preparation equipment of single-walled carbon nanotube

Abstract

The invention discloses preparation equipment of a single-walled carbon nanotube, and belongs to the technical field of carbon nanotube production. The preparation equipment comprises a main reactor, the main reactor comprises a catalyst gasification cavity and a carbon nanotube generation cavity, the catalyst gasification cavity extends in the horizontal direction, a feeding port is formed in the first end of the catalyst gasification cavity, the carbon nanotube generation cavity extends in the vertical direction, and a discharging port is formed in the lower end of the carbon nanotube generation cavity; the arc plasma torch assembly and the catalyst assembly are mounted on the upper side and the lower side of the catalyst gasification cavity respectively; feeding gas enters the catalyst gasification cavity along the feeding hole, and an electric arc is generated between the electric arc plasma torch assembly and the catalyst assembly; a reaction product enters the carbon nanotube generation cavity along the catalyst gasification cavity and is discharged along the discharge port after growth is completed. According to the invention, continuous production of the single-walled carbon nanotubes can be realized.

Description

Technical Field

[0001] The invention relates to the technical field of carbon nanotube production, and in particular to a preparation device for single-walled carbon nanotubes. Background Art

[0002] Single-walled carbon nanotubes are a type of carbon nanotubes with unique structures and properties. They have broad application prospects in the fields of materials science, electronics, and biomedicine. At present, the main methods for preparing single-walled carbon nanotubes include arc discharge, laser evaporation, chemical vapor deposition (CVD), pyrolysis, etc. Among them, arc discharge is one of the most commonly used preparation methods. Its principle is to introduce carbon-containing gases such as methane into a vacuum container, use transition metals as catalysts to form a receiving electrode, and use tungsten needles as anodes. Argon gas is broken down and ionized by the high voltage between the cathode and anode to form a stable arc. During the arc discharge process, the metal catalyst in the receiving electrode is vaporized and forms nano-scale droplets in the reaction container. The carbon-containing gas attaches to the metal droplets and dehydrogenates under the high temperature environment in the reaction container, thereby producing single-walled carbon nanotubes.

[0003] The arc discharge method for preparing single-walled carbon nanotubes has high requirements on the thermal insulation of the manufacturing equipment due to the arc temperature of 3000℃-3700℃. At the same time, the droplets formed after the metal catalyst is vaporized are easy to adhere to the reactor tube wall. If too many metal catalyst droplets accumulate on the reactor tube wall, the production efficiency of the product will be affected. Summary of the invention

[0004] To this end, the present invention provides a single-walled carbon nanotube preparation device with high production efficiency.

[0005] In view of the above technical problems, the present invention provides the following technical solutions:

[0006] A single-wall carbon nanotube preparation device comprises: a main reactor, the main reactor comprises a catalyst gasification chamber and a carbon nanotube generation chamber, the catalyst gasification chamber extends in a horizontal direction and a feed port is provided at a first end thereof, the carbon nanotube generation chamber extends in a vertical direction and a discharge port is provided at a lower end thereof; an arc plasma torch assembly and a catalyst assembly, both of which are respectively installed at the upper and lower sides of the catalyst gasification chamber; feed gas enters the catalyst gasification chamber through the feed port, an arc is generated between the arc plasma torch assembly and the catalyst assembly; reaction products enter the carbon nanotube generation chamber through the catalyst gasification chamber and are discharged through the discharge port after growth is completed.

[0007] In some embodiments of the present invention, the main reactor is an inverted L-shaped tube as a whole, and the flow cross-sectional area of ​​the catalyst gasification chamber is larger than the flow cross-sectional area of ​​the carbon nanotube generation chamber.

[0008] In some embodiments of the present invention, the arc plasma torch assembly has an angle other than 0° with the horizontal direction, and the catalyst assembly extends in the vertical direction.

[0009] In some embodiments of the present invention, a reactor shell is further included which is covered on the outside of the main reactor, and a heat-insulating material is filled between the reactor shell and the main reactor.

[0010] In some embodiments of the present invention, the arc plasma torch assembly and the catalyst assembly extend along the reactor shell into the inner side of the main reactor.

[0011] In some embodiments of the present invention, the main reactor is provided with an insulation device on the outside of the carbon nanotube generation chamber, and the insulation device includes an electric heating sleeve, an insulation shell and an insulation material located therebetween; the electric heating sleeve is coated on the outer side wall of the carbon nanotube generation chamber, the insulation shell is coated on the outside of the electric heating sleeve and there is a cavity between the two, and the insulation material is located in the cavity.

[0012] In some embodiments of the present invention, the main reactor is provided with at least one water spray outlet in the area between the heat preservation device and the discharge port, and the water spray outlet is connected to the cooling liquid circulation system.

[0013] In some embodiments of the present invention, a first temperature sensor for detecting the temperature of the catalyst gasification chamber is further included, and the first temperature sensor extends along the reactor shell into the catalyst gasification chamber of the main reactor.

[0014] In some embodiments of the present invention, a second temperature sensor and a third temperature sensor for detecting the inlet temperature and outlet temperature of the carbon nanotube generation chamber are also included. The second temperature sensor and the third temperature sensor respectively extend along the reactor shell into the side wall of the main reactor, and the second temperature sensor is located on the upper side of the insulation device, and the third temperature sensor is located on the lower side of the insulation device.

[0015] In some embodiments of the present invention, the main reactor is provided with a catalyst replenishing port at a position directly opposite to the catalyst assembly, and the catalyst replenishing port is connected to the catalyst supply system via a catalyst replenishing pipeline penetrating the reactor shell.

[0016] The technical solution of the present invention has the following technical effects compared with the prior art:

[0017] In the single-walled carbon nanotube preparation equipment provided by the present invention, an arc plasma torch assembly and a catalyst assembly are located at the upper and lower sides of a main reactor, and an arc can be generated between the two, so that the metal catalyst in the catalyst assembly is gasified and enters a catalyst gasification chamber to form nanometer-level droplets; the feed gas enters the catalyst gasification chamber in a horizontal direction, so that the feed gas can be fully cracked and dehydrogenated in the catalyst gasification chamber, and the reaction product is attached to the catalyst droplets and enters a carbon nanotube generation chamber extending in a vertical direction along the catalyst gasification chamber to complete growth and finally form a single-walled carbon nanotube, and is discharged along the discharge port on the lower side thereof, so that the metal catalyst droplets are prevented from accumulating in the chamber extending in the horizontal direction of the main reactor, thereby improving the production efficiency of the single-walled carbon nanotubes and realizing the continuous preparation of the single-walled carbon nanotubes. BRIEF DESCRIPTION OF THE DRAWINGS

[0018] The preferred embodiments of the present invention will be described in detail below with reference to the accompanying drawings, which will help to understand the objects and advantages of the present invention, wherein:

[0019] Figure 1 A schematic diagram of a specific embodiment of the single-walled carbon nanotube preparation device of the present invention;

[0020] Figure 2 It is a structural schematic diagram of a specific embodiment of an arc plasma torch assembly in the single-walled carbon nanotube preparation device of the present invention;

[0021] Figure 3 A partial schematic diagram of a specific embodiment of the single-walled carbon nanotube preparation device of the present invention;

[0022] Figure 4 It is a schematic structural diagram of the support part in the single-walled carbon nanotube preparation device of the present invention. DETAILED DESCRIPTION

[0023] The technical solution of the present invention will be described clearly and completely below in conjunction with the accompanying drawings. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0024] In the description of the present invention, it should be noted that the terms "center", "upper", "lower", "left", "right", "vertical", "horizontal", "inner", "outer", etc., indicating the orientation or positional relationship, are based on the orientation or positional relationship shown in the drawings, and are only for the convenience of describing the present invention and simplifying the description, rather than indicating or implying that the device or element referred to must have a specific orientation, be constructed and operated in a specific orientation, and therefore cannot be understood as limiting the present invention. In addition, the terms "first", "second", and "third" are used for descriptive purposes only, and cannot be understood as indicating or implying relative importance.

[0025] In the description of the present invention, it should be noted that, unless otherwise clearly specified and limited, the terms "installed", "connected", and "connected" should be understood in a broad sense, for example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a direct connection, or an indirect connection through an intermediate medium, or it can be the internal communication of two components. For ordinary technicians in this field, the specific meanings of the above terms in the present invention can be understood according to specific circumstances.

[0026] In addition, the technical features involved in the different embodiments of the present invention described below can be combined with each other as long as they do not conflict with each other.

[0027] like Figure 1 The figure shows a specific embodiment of the single-walled carbon nanotube preparation device of the present invention, which comprises a main reactor 10, wherein the main reactor 10 comprises a catalyst gasification chamber 10a and a carbon nanotube generation chamber 10b which are interconnected, wherein the catalyst gasification chamber 10a extends in a horizontal direction and a feed port 13 is provided at a first end thereof, and the carbon nanotube generation chamber 10b extends in a vertical direction and a discharge port 14 is provided at a lower end thereof; and an arc plasma torch assembly 20 and a catalyst assembly 30 respectively installed at the upper and lower sides of the catalyst gasification chamber 10a; the arc plasma torch assembly 20 is connected to an arc generator, such as an arc generator, an arc generator, etc. An electric arc is generated between the plasma torch assembly 20 and the catalyst assembly 30, so that the metal catalyst in the catalyst assembly 30 is vaporized and enters the catalyst gasification chamber 10a to form nanometer-scale droplets; the feed gas (such as carbon-containing organic matter such as methane) enters the catalyst gasification chamber 10a along the feed port 13 of the main reactor 10 and is cracked and dehydrogenated in a high-temperature environment of more than 3000°C, and the reaction product is attached to the catalyst droplets and enters the carbon nanotube generation chamber 10b along the catalyst gasification chamber 10a to complete the growth and finally form single-walled carbon nanotubes and are discharged along the discharge port, thereby realizing the continuous preparation of single-walled carbon nanotubes.

[0028] In the above-mentioned preparation equipment, the catalyst gasification chamber 10a of the main reactor 10 extends in the horizontal direction, which allows the feed gas to fully undergo cracking reaction in the catalyst gasification chamber 10a, while the carbon nanotube generation chamber 10b extends in the vertical direction and is provided with a discharge port at its lower end, which allows the metal catalyst droplets vaporized in the horizontally extended catalyst gasification chamber 10a to quickly flow into the vertically extended carbon nanotube generation chamber 10b and finally be discharged from the lower outlet, thereby avoiding the accumulation of metal catalyst droplets in the chamber of the main reactor 10 extending in the horizontal direction, thereby improving the production efficiency of single-walled carbon nanotubes.

[0029] Specifically, Figure 1 As shown, the main reactor 10 is an inverted L-shaped tube as a whole, and at least part of the horizontal branch of the L-shaped tube forms the catalyst gasification chamber 10a, and at least part of the vertical branch of the L-shaped tube forms the carbon nanotube generation chamber 10b. The catalyst gasification chamber 10a is connected to the carbon nanotube generation chamber 10b through an arc-shaped transition chamber, which can facilitate the rapid discharge of the reaction product into the carbon nanotube generation chamber 10b. Among them, the flow cross-sectional area of ​​the catalyst gasification chamber 10a is larger than the flow cross-sectional area of ​​the carbon nanotube generation chamber 10b, which can make the chamber volume of the catalyst gasification chamber 10a larger, the temperature field distribution is uniform, which is conducive to the feed gas in each area of ​​the space The cracking reaction is more complete and the reaction effect is good. Among them, the flow cross-sectional area of ​​the carbon nanotube generation chamber 10b is determined according to the set flow rate of the reactants in this chamber. By setting the flow cross-sectional size of the carbon nanotube generation chamber 10b, the flow rate of the reaction products in this chamber can be changed, and then the residence time of the reaction products in this chamber can be changed. After the heat-insulating flow for the set residence time, the production quality of the single-walled carbon nanotube product can be guaranteed.

[0030] Specifically, in an optional implementation manner, Figure 2 As shown, the arc plasma torch assembly 20 includes a plasma generating body 21 and an emitter 22 installed inside the plasma generating body 21, the emitter 22 includes a conductive tube 221 extending along a first direction and an emitter nozzle 222 located at the end of the conductive tube 221; wherein the emitter nozzle 222 is made of metal tungsten, and the conductive tube 221 is made of metal copper, the emitter nozzle 222 is plugged into the end of the conductive tube 221, the conductive tube 221 is electrically connected to the arc generator, and the arc generator is controlled to be turned on so that an arc can be generated between the emitter 22 of the arc plasma torch assembly 20 and the catalyst surface of the catalyst assembly 30; a gas channel 22a is provided in the conductive tube 221 and the emitter nozzle 222 for supplying a protective gas, specifically, the protective gas is argon, and the argon is broken down and ionized by the high voltage between the cathode and anode to form a stable arc.

[0031] Specifically, in an optional implementation manner, Figure 3 As shown, the catalyst assembly 30 includes a catalyst containing part 31 with an upper opening, the catalyst containing part 31 is used to contain a solid catalyst 32 with a shape matching therewith, and a connection hole for connecting a receiving pole 33 is provided at the bottom of the catalyst containing part 31, and the receiving pole 33 is connected to the solid catalyst 32 through the connection hole. The solid catalyst 32 is usually made of metal materials such as iron, cobalt, nickel, and molybdenum, and the receiving pole 33 is usually made of metal materials such as copper and silver.

[0032] Specifically, in an optional embodiment, the arc plasma torch assembly 20 has an angle with the horizontal direction that is not 0°, that is, the extension direction of the plasma generating body 21 or the emitter 22 is inclined relative to the horizontal direction; the catalyst assembly 30 extends in the vertical direction, that is, the catalyst receiving portion 31 extends in the vertical direction so that the upper surface of the solid catalyst 32 located therein extends in the horizontal direction. When the arc heats the solid catalyst at high temperature, the high-temperature catalyst liquid will sputter to the surroundings, and the emission nozzle 222 and the surface of the solid catalyst 32 form a certain angle so that the argon gas blown out from the emission nozzle 222 can quickly blow away the sputtered droplets, thereby avoiding the emission nozzle from being ablated. More specifically, the angle a between the arc plasma torch assembly 20 and the horizontal direction is between 30° and 60°, for example, the angle a is 45°.

[0033] Specifically, Figure 1 , Figure 3 As shown, the preparation equipment also includes a reactor shell 40 covered on the outside of the main reactor 10, the arc plasma torch assembly 20 and the catalyst assembly 30 extend into the inside of the main reactor 10 along the reactor shell 40, and the reactor shell 40 and the main reactor 10 are filled with insulation material. Since the single-walled carbon nanotubes have high requirements for the reaction temperature, in order to ensure the temperature stability of the catalyst gasification chamber 10a and the carbon nanotube generation chamber 10b, the insulation material between the reactor shell 40 and the main reactor 10 can avoid excessive changes in the reaction temperature. More specifically, the inner wall of the reactor shell 40 is provided with a heat insulation layer, which can isolate the temperature field of the outside and inside of the reactor shell 40, avoiding the safety hazard caused by the excessively high temperature of the outside of the reactor shell 40.

[0034] Specifically, the preparation equipment also includes a first temperature sensor 51 for detecting the temperature of the catalyst gasification chamber 10a. The first temperature sensor 51 extends along the reactor shell 40 into the inner side of the catalyst gasification chamber 10a of the main reactor 10, so as to facilitate the operator to monitor the temperature of the catalyst gasification chamber 10a.

[0035] Specifically, in an optional embodiment, the catalyst containing portion 31 is detachably connected to the main reactor 10 via a supporting portion 34. Figure 3 As shown, the main reactor 10 is provided with a first mounting seat 11, the first mounting seat 11 extends to the outside of the reactor shell 40, and is provided with a connecting edge 111 at its end, and the connecting edge 111 is provided with a connecting hole, and the catalyst containing portion 31 is detachably connected to the first mounting seat 11 through a supporting portion 34. Figure 4 As shown, the support portion 34 includes a support plate 341 and a support sleeve 342 arranged on one side of the support plate 341, the support plate 341 is provided with a through hole connected to the support sleeve 342, the catalyst containing portion 31 is supported on the upper side of the support plate 341, and the receiving pole 33 is inserted into the support sleeve 342 and extends along the through hole to the inner side of the catalyst containing portion 31.

[0036] In order to avoid the problem that the receiving electrode 33 melts or deforms at too high a temperature, Figure 3 , Figure 4 As shown, the catalyst assembly 30 further includes a receiving electrode cooling portion 35, and the receiving electrode cooling portion 35 includes a cooling cavity 351 surrounding the outside of the receiving electrode 33, and the cooling cavity 351 is connected to a cooling circulation pipeline (not shown in the figure). The receiving electrode 33 can be cooled by opening the cooling circulation pipeline and controlling the flow rate of the coolant in the cooling circulation pipeline.

[0037] Since the catalyst containing part 31 is detachably connected to the first mounting seat 11, in order to facilitate the removal of the catalyst containing part 31, it is spaced apart from the inner wall of the first mounting seat 11. In order to prevent the high-temperature gas in the catalyst gasification chamber 10a from passing through the gap between the first mounting seat 11 and the catalyst containing part 31 as much as possible, at least one annular extension edge 112 is provided on the inner wall of the first mounting seat 11, and the inner side wall of the annular extension edge 112 abuts against the outer wall of the catalyst containing part 31 to isolate the catalyst gasification chamber 10a from the outer area of ​​the main reactor 10, thereby ensuring the temperature stability of the catalyst gasification chamber 10a.

[0038] Specifically, when an arc is generated between the arc plasma torch assembly 20 and the catalyst assembly 30 to gasify the metal catalyst, the amount of catalyst in the catalyst receiving portion 31 gradually decreases, which causes the gap between the arc plasma torch assembly 20 and the catalyst assembly 30 to be too large, and the gap between the two is not enough to generate an arc, which eventually leads to the problem of production interruption. In order to ensure the continuous preparation of single-walled carbon nanotubes, such as Figure 1As shown, the main reactor 10 is provided with a catalyst replenishing port 12 at a position directly opposite to the catalyst assembly 30, and the catalyst replenishing port 12 is connected to the catalyst supply system through a catalyst replenishing pipeline 60 penetrating the reactor shell 40. When the gap between the arc plasma torch assembly 20 and the catalyst assembly 30 is greater than a set threshold, the granular metal catalyst is allowed to enter the catalyst containing portion 31 along the catalyst replenishing pipeline 60 and the catalyst replenishing port 12 by controlling the switch valve on the catalyst replenishing pipeline 60.

[0039] Specifically, in order to further ensure the stability of the temperature field during the carbon nanotube generation process, as Figure 1 As shown, the main reactor 10 is provided with a heat preservation device 70 outside the carbon nanotube generation chamber 10b, and the heat preservation device 70 includes an electric heating sleeve 71, a heat preservation shell 73 and a heat preservation material 72 located therebetween; the electric heating sleeve 71 is coated on the outer wall of the carbon nanotube generation chamber 10b, the heat preservation shell 73 is coated on the outer side of the electric heating sleeve 71, and there is a cavity between the two, and the heat preservation material 72 is located in the cavity; the lead wire of the electric heating sleeve 71 is led out to the outside of the reactor shell 40 through the heat preservation shell 73. The electric heating sleeve 71 is controlled to start, and the carbon nanotube generation chamber 10b can be heated to keep its temperature in a set temperature range. At the same time, the heat preservation material 72 located between the electric heating sleeve 71 and the heat preservation shell 73 can ensure that the temperature field is in a stable temperature range as much as possible.

[0040] Among them, the electric heating sleeve 71 includes a ceramic sleeve and an electric heating wire embedded in the ceramic sleeve, which surrounds the entire extension length direction of the carbon nanotube generation chamber 10b. One or more electric heating sleeves 71 are provided, and the winding density of the electric heating wire on each electric heating sleeve is the same or different. Multiple electric heating sleeves 71 are connected in parallel to achieve independent heating of different areas of the carbon nanotube generation chamber 10b.

[0041] Specifically, in order to more accurately control the electric heating temperature of the carbon nanotube generation chamber 10b, the preparation equipment further includes a second temperature sensor 52 and a third temperature sensor 53 for detecting the inlet temperature and the outlet temperature of the carbon nanotube generation chamber 10b, the second temperature sensor 52 and the third temperature sensor 53 are respectively extended into the side wall of the main reactor 10 along the reactor shell 40, and the second temperature sensor 52 is located on the upper side of the heat preservation device 70, and the third temperature sensor 53 is located on the lower side of the heat preservation device 70. The opening or closing of the electric heating jacket 71 can be controlled according to the temperature value detected by the second temperature sensor 52 and / or the third temperature sensor 53. More specifically, when the carbon nanotube generation chamber 10b is provided with a plurality of electric heating jackets 71 connected in parallel, the opening and closing of the electric heating jackets 71 in different regions can be controlled according to the detection values ​​of the second temperature sensor 52 and the third temperature sensor 53, thereby achieving more accurate temperature control and improving the production quality of single-walled carbon nanotubes.

[0042] Specifically, in order to rapidly cool down the single-walled carbon nanotubes after passing through the carbon nanotube generation chamber 10b, as Figure 1 As shown, the main reactor 10 is provided with at least one water spray outlet 80 in the area between the insulation device 70 and the discharge port. The water spray outlet 80 is connected to the coolant circulation system (not shown in the figure). After the single-walled carbon nanotubes are cooled by cooling water, they can be discharged to the next station through the discharge port to avoid excessive temperature which reduces the service life of the next station device.

[0043] Obviously, the above embodiments are merely examples for the purpose of clear explanation, and are not intended to limit the implementation methods. For those skilled in the art, other different forms of changes or modifications can be made based on the above description. It is not necessary and impossible to list all the implementation methods here. However, the obvious changes or modifications derived therefrom are still within the scope of protection of the present invention.

Claims

1. A single-walled carbon nanotube preparation device, characterized in that: include: A main reactor, the main reactor comprising a catalyst gasification chamber and a carbon nanotube generation chamber, the catalyst gasification chamber extending in a horizontal direction and having a feed port at a first end thereof, the carbon nanotube generation chamber extending in a vertical direction and having a discharge port at a lower end thereof; An arc plasma torch assembly and a catalyst assembly are respectively installed on the upper and lower sides of the catalyst gasification chamber; The feed gas enters the catalyst gasification chamber through the feed port, and an arc is generated between the arc plasma torch assembly and the catalyst assembly; the reaction product enters the carbon nanotube generation chamber through the catalyst gasification chamber, completes growth, and is discharged through the discharge port.

2. The single-walled carbon nanotube preparation device according to claim 1, characterized in that: The main reactor is in an inverted L-shaped tube as a whole, and the flow cross-sectional area of ​​the catalyst gasification chamber is larger than the flow cross-sectional area of ​​the carbon nanotube generation chamber.

3. The single-walled carbon nanotube preparation device according to claim 1, characterized in that: The arc plasma torch assembly has an angle with the horizontal direction that is not 0°, and the catalyst assembly extends in the vertical direction.

4. The single-walled carbon nanotube preparation device according to claim 1, characterized in that: It also includes a reactor shell which is covered on the outside of the main reactor, and a heat-insulating material is filled between the reactor shell and the main reactor.

5. The single-walled carbon nanotube preparation device according to claim 4, characterized in that: The arc plasma torch assembly and the catalyst assembly extend along the reactor shell into the inner side of the main reactor.

6. The single-walled carbon nanotube preparation device according to claim 4, characterized in that: The main reactor is provided with an insulation device on the outside of the carbon nanotube generation chamber, and the insulation device includes an electric heating sleeve, an insulation shell and an insulation material located therebetween; the electric heating sleeve is coated on the outer wall of the carbon nanotube generation chamber, the insulation shell is coated on the outside of the electric heating sleeve and there is a cavity between the two, and the insulation material is located in the cavity.

7. The single-walled carbon nanotube preparation device according to claim 6, characterized in that: The main reactor is provided with at least one water spraying port in the area between the heat preservation device and the discharge port, and the water spraying port is connected to the cooling liquid circulation system.

8. The single-walled carbon nanotube preparation device according to claim 4, characterized in that: It also includes a first temperature sensor for detecting the temperature of the catalyst gasification chamber, and the first temperature sensor extends along the reactor shell into the catalyst gasification chamber of the main reactor.

9. The single-walled carbon nanotube preparation device according to claim 6, characterized in that: It also includes a second temperature sensor and a third temperature sensor for detecting the inlet temperature and outlet temperature of the carbon nanotube generation chamber. The second temperature sensor and the third temperature sensor extend into the side wall of the main reactor along the reactor shell respectively, and the second temperature sensor is located on the upper side of the insulation device, and the third temperature sensor is located on the lower side of the insulation device.

10. The single-walled carbon nanotube preparation device according to claim 4, characterized in that: The main reactor is provided with a catalyst replenishing port at a position directly opposite to the catalyst assembly, and the catalyst replenishing port is communicated with a catalyst supply system through a catalyst replenishing pipeline penetrating the reactor shell.

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