CN111646456A

CN111646456A - Device and method for large-scale continuous synthesis of carbon nanotubes by flame method

Info

Publication number: CN111646456A
Application number: CN202010551572.4A
Authority: CN
Inventors: 楚化强; 董世林; 韩伟伟; 牙宇晨
Original assignee: Anhui University of Technology AHUT
Current assignee: Anhui University of Technology AHUT
Priority date: 2020-06-17
Filing date: 2020-06-17
Publication date: 2020-09-11
Anticipated expiration: 2040-06-17
Also published as: CN111646456B

Abstract

The invention discloses a device and a method for large-scale continuous synthesis of carbon nanotubes by a flame method, and belongs to the technical field of synthesis of carbon nanotubes. The device includes: a combustion section providing a source of carbon and energy for synthesis; a circulation transfer substrate for synthesizing and transferring the carbon nanotubes; a driving member for driving the cyclic transfer substrate; a coating member for coating a catalyst on the circulating substrate; a collecting member for taking the carbon nanotubes from the circulating transport substrate; and the control component is used for controlling the operation of the combustion component, the driving component, the coating component and the collecting component. The carbon nano tube is synthesized by adopting methane/ethylene laminar diffusion flame, the computer end is combined with the PLC and the circulating transmission substrate, the synthesis process of the carbon nano tube can be directly controlled by the computer end configuration module, the operation flow of synthesizing the carbon nano tube by the flame method is greatly simplified, the preparation cost can be reduced on the premise of ensuring the quality of the carbon nano tube, and the synthesis efficiency is effectively improved.

Description

Device and method for large-scale continuous synthesis of carbon nanotubes by flame method

Technical Field

The invention relates to the technical field of carbon nanotube synthesis, in particular to a device and a method for continuously synthesizing carbon nanotubes on a large scale by a flame method.

Background

The carbon nanotube is a one-dimensional nanometer quantum material with a special structure, and mainly comprises a single-layer or a plurality of layers of coaxial circular tubes with six-membered ring structures (hybridized by carbon atoms sp 2), wherein the distance between the layers is about 0.34 nm. Carbon nanotubes can be regarded as being formed by winding graphene sheets, and can be classified into single-walled carbon nanotubes and multi-walled carbon nanotubes according to the number of graphene sheets. The unique structure (bent graphite, small diameter and high aspect ratio) of the carbon nano tube determines that the carbon nano tube has a plurality of special physical and chemical properties, such as high mechanical strength and elasticity, excellent semiconductor characteristics, high specific surface area and strong adsorption characteristics, so that the carbon nano tube has huge application prospects in the fields of catalyst carriers, hydrogen storage materials, high-energy capacitors, battery electrode materials and the like.

Since the discovery of carbon nanotubes by the japanese electron microscope expert Iijima under a high-resolution transmission scanning electron microscope, the methods for preparing carbon nanotubes are continuously perfected, mainly including an arc method, a chemical vapor deposition method and a laser evaporation method, which can prepare high-quality carbon nanotubes, but all need additional energy, increase the cost, are not easy to prepare in a large scale, and particularly for the fields of composite materials and the like, large-scale low-cost carbon nanotubes are needed.

There are three key factors in carbon nanotube synthesis: a carbon source, a heat source, and a catalyst. At present, the flame method for preparing the carbon nano tube mainly has the following problems: 1) the quality and yield of the carbon nano tube are influenced by a plurality of factors (such as the size of catalyst particles, the type and the temperature of a carbon source, the type and the proportion of mixed gas and the like), and how to realize continuous batch industrial production of the carbon nano tube meeting different requirements on the basis of low cost; 2) the mechanism for preparing the carbon nano tube is not clear enough, the structure (diameter, tube length, spiral line, tube wall thickness, graphite carbon crystallinity on the surface of the tube and the like) of the carbon nano tube cannot be adjusted and controlled at will, and the carbon nano tube is difficult to regulate and control growth from the mechanism; 3) the carbon nano tube prepared in the flame has more impurities, and the later purification of the carbon nano tube needs further optimization.

The flame method for preparing the carbon nano material has wide application prospect. In conclusion, the perfection and mechanism research of the carbon nanotube flame preparation method are still the focus of the current research. Panchuxu et al use ethanol alcohol lamps as heat and carbon sources, and place the synthetic substrate above them to prepare carbon nanotubes, but this method can only perform single preparation, cannot synthesize carbon nanotubes on a large scale, and cannot accurately control the preparation time (reference: keen, strong, Zhang Yupeng, etc.. research progress on one-dimensional carbon nanomaterials grown in ethanol flame [ J ] Chinese non-ferrous metals bulletin, 2011,21(9): 2119-2125.); mohd Syair et al use a support to support the substrate for sampling, but the sampling height is not easily adjusted and the sampling time is difficult to control precisely (ref: Mohd Syahir M S, Chong CT. Synthesis of carbon nanotubes from particulate premix/air flame [ J ]. Applied Mechanics and materials,2014,699:136 materials 140).

In the publication No. CN108946702A, a thermophoresis probe sampling system capable of controlling the sampling time of carbon nanotubes at millisecond level is designed by using an air cylinder, a signal generator, etc., so as to realize sampling in the formation process of carbon nanotubes. Both publication numbers CN204714524U and CN103708439A propose a device or method capable of continuously synthesizing carbon nanotubes, the former is provided with a crawler-type acquisition probe and realizes separation of flame combustion and carbon nanotube synthesis, thereby ensuring synthesis stability, and realizing batch and continuous synthesis of carbon nanotubes to a certain extent, but both catalyst coating and carbon nanotube collection need manual intervention; in addition, the speed of the collecting probe is respectively controlled by the accessory parts, so that the synthesis efficiency of the carbon nano tube is reduced; the latter realizes the continuous synthesis of the carbon nano tube by driving the substrate conveying rotating shaft and the recycling rotating shaft through the motor, and sets the coating and drying of the catalyst in the conveying process of the substrate, thereby reducing the manual intervention and improving the synthesis efficiency.

Disclosure of Invention

1. Problems to be solved

Aiming at the problem of low synthesis efficiency of the carbon nano tube, the invention provides a device and a method for synthesizing the carbon nano tube in a large scale by a flame method, which can reduce the preparation cost and effectively improve the synthesis efficiency on the premise of ensuring the quality of the carbon nano tube.

2. Technical scheme

In order to solve the problems, the technical scheme adopted by the invention is as follows:

the apparatus for synthesizing carbon nanotubes on a large scale by a flame method of the present invention comprises:

a combustion section providing a source of carbon and energy for synthesis;

a circulation transfer substrate for synthesizing and transferring the carbon nanotubes;

a driving means for driving the endless transfer substrate;

a coating member for coating a catalyst on the circulating transport substrate;

a collecting member for taking the carbon nanotubes from the circulating transport substrate;

and the control component is used for controlling the operation of the combustion component, the driving component, the coating component and the collecting component.

In a possible embodiment of the invention, the combustion part comprises a multi-burner combustor, a gas mixing chamber, a fuel bottle, a nitrogen gas bottle, an oxygen bottle and a gas mass flowmeter, the nitrogen gas bottle and the oxygen bottle are connected with the gas mass flowmeter to the gas mixing chamber through pipelines, the fuel bottle is connected with the gas mass flowmeter to the multi-burner combustor through pipelines, the circular conveying substrate is conveyed above flame formed by the multi-burner combustor, the multi-burner combustor is provided with a windproof cover, the upper end and the lower end of the windproof cover are open, and the left end and the right end of the windproof cover are provided with openings from the middle to the bottom for the circular conveying substrate to rotate and pass through.

In a possible embodiment of the present invention, the driving component includes a speed-adjustable motor and a plurality of rotating shafts, the rotating shafts are connected to the speed-adjustable motor, and the circular conveying substrate is mounted on the rotating shafts; or the control part comprises a computer end and a PLC (programmable logic controller) connected with the computer end, the adjustable-speed motor is connected to the PLC, and the computer end controls the PLC through the configuration module so as to control the adjustable-speed motor to rotate.

In a possible embodiment of the present invention, the coating unit includes a catalyst dripping pipe, a rolling brush, and a coating dryer, the catalyst dripping pipe is disposed above the rolling brush and conveys a catalyst solution to the rolling brush, the rolling brush is in contact with the surface of the substrate to be circularly transferred, the rolling direction is opposite to the overall movement direction of the substrate to be circularly transferred, and the catalyst is coated on the surface of the substrate to be circularly transferred while rolling, and is dried by the coating dryer.

In one possible embodiment of the present invention, the collecting means comprises a primary collector and a secondary collector; the primary collector comprises a first blade and a first container, wherein the first blade scrapes carbon nanotubes formed on the surface of the circularly conveyed substrate and falls into the first container; the secondary collector comprises a second blade and a second container, and the second blade scrapes residual carbon nanotubes on the surface of the circularly conveyed substrate and falls into the second container.

In one possible embodiment of the present invention, the substrate cleaning apparatus further includes a substrate cleaning unit, the substrate cleaning unit includes an alcohol nozzle, an alcohol collection container, and a cleaning dryer, the alcohol nozzle sprays an alcohol solution onto the surface of the substrate to clean the surface of the substrate, excess alcohol sprayed onto the substrate is collected by the alcohol collection container, and the substrate cleaned by the alcohol spray is sent to the cleaning dryer to be dried.

In a possible embodiment of the present invention, the substrate cleaning device further comprises a substrate cleaning component, wherein the substrate cleaning component comprises a plurality of integrated rolling cleaning brushes, the rolling direction is opposite to the overall movement direction of the circularly conveyed substrate, and the substrate cleaning component cleans the carbon nanotubes remaining on the scraped circularly conveyed substrate.

In a possible embodiment of the present invention, the driving unit further includes a plurality of supporting shafts disposed between the rotating shafts for supporting the circular transfer substrate and controlling a traveling path of the circular transfer substrate during the transfer process.

The invention also provides a method for continuously synthesizing the carbon nano tube in a large scale by adopting the device, which comprises the following steps:

the speed-adjustable motor is connected with the PLC, the PLC is connected with the computer end, the working cycle of the speed-adjustable motor is 10 seconds, the speed-adjustable motor stops for 1-10 minutes, the cycle time and the stop time are input and controlled by the computer end configuration module, and the supporting rotating shaft is used for supporting and fixing the position of the circular transmission substrate; when the speed-adjustable motor stops, the catalyst dropper conveys the catalyst solution to the rolling brush, the rolling brush coats the catalyst solution on the surface of the circular conveying substrate, the catalyst solution on the surface of the circular conveying substrate is dried at a dryer, the carbon nano tube is prepared at a combustion part, the alcohol nozzle sprays the alcohol solution on the surface of the circular conveying substrate, and then the circular conveying substrate is dried in the dryer; when the speed-adjustable motor rotates, the circular conveying substrate moves along the rotating shaft, the carbon nano tube collecting component scrapes and collects the carbon nano tubes on the surface of the circular conveying substrate, and the scraped circular conveying substrate is cleaned by the rolling cleaning brush.

In one possible embodiment of the present invention, the material of the circular conveying substrate is copper and is made into a thin sheet, the catalyst is nickel nitrate, and the processing method is as follows: 29.079g of nickel nitrate hexahydrate is dissolved in a test tube containing 100mL of absolute ethanol to prepare a 1mol/L nickel nitrate solution, and ultrasonic oscillation is carried out for 10 minutes.

3. Advantageous effects

Compared with the prior art, the invention has the beneficial effects that:

according to the device for synthesizing the carbon nano tubes in a large scale by the flame method, the carbon nano tubes are synthesized by adopting methane/ethylene laminar diffusion flame, the computer end is combined with the PLC and the circular transmission substrate, the synthesis process of the carbon nano tubes can be directly controlled by the computer end configuration module, the operation flow of synthesizing the carbon nano tubes by the flame method is greatly simplified, the manual intervention is reduced, meanwhile, the windproof device is arranged, the preparation cost can be reduced on the premise of ensuring the quality of the carbon nano tubes, and the process is simpler and more convenient; a continuous conveying circulating device is designed, so that the synthesis efficiency is effectively improved, the substrate is conveyed circularly and enters the preparation process again through secondary cleaning, the substrate can be recycled, and the cost is further reduced; the coating method of the catalyst on the substrate is improved, so that the catalyst is more uniformly and conveniently coated;

compared with the traditional method, the carbon-hydrogen flame is used for synthesizing the carbon nano tube by utilizing the carbon source generated by burning the carbon-hydrogen fuel under the action of the catalyst, can simultaneously provide the carbon source and the heat source required by preparing the carbon nano tube, has the advantages of high energy efficiency and low cost, can rapidly produce the carbon nano tube in a large batch and continuously in tens of seconds, and provides an effective way for the commercial production of the carbon nano tube.

Drawings

The technical solutions of the present invention will be described in further detail below with reference to the accompanying drawings and examples, but it should be understood that these drawings are designed for illustrative purposes only and thus do not limit the scope of the present invention. Furthermore, unless otherwise indicated, the drawings are intended to be illustrative of the structural configurations described herein and are not necessarily drawn to scale.

FIG. 1 is a schematic view of an apparatus for large-scale continuous synthesis of carbon nanotubes by a flame method according to the present invention.

The notation in the figure is:

100. a combustion component; 110. a multi-burner; 120. a windshield; 130. a gas mixing chamber; 140. a fuel bottle; 150. a nitrogen gas cylinder; 160. an oxygen cylinder; 170. a gas mass flow meter;

200. circularly conveying the substrate;

300. a drive member; 310. a speed adjustable motor; 320. rotating the rotating shaft; 330. a support shaft;

400. coating the component; 410. a catalyst dropper; 420. a rolling brush; 430. a coating dryer;

500. a collecting member; 510. a primary collector; 511. a first blade; 512. a first container; 520. a secondary collector; 521. a second blade; 522. a second container;

600. a control component; 610. a PLC controller; 620. a computer terminal;

700. a substrate cleaning member; 710. an integral rolling cleaning brush;

800. a substrate cleaning member; 810. an alcohol nozzle; 820. an alcohol collection vessel; 830. cleaning and drying the device;

Detailed Description

The following detailed description of exemplary embodiments of the invention refers to the accompanying drawings, which form a part hereof, and in which is shown by way of illustration exemplary embodiments in which the invention may be practiced. Although these exemplary embodiments are described in sufficient detail to enable those skilled in the art to practice the invention, it should be understood that other embodiments may be realized and that various changes to the invention may be made without departing from the spirit and scope of the present invention. The following more detailed description of the embodiments of the invention is not intended to limit the scope of the invention, as claimed, but is presented for purposes of illustration only and not limitation to describe the features and characteristics of the invention, to set forth the best mode of carrying out the invention, and to sufficiently enable one skilled in the art to practice the invention. Accordingly, the scope of the invention is to be limited only by the following claims.

The detailed description and exemplary embodiments of the invention will be better understood when read in conjunction with the appended drawings, where the elements and features of the invention are identified by reference numerals.

Examples

As shown in fig. 1, the arrows in the figure indicate the direction of the drive. The apparatus for synthesizing carbon nanotubes on a large scale by the flame method of this embodiment includes: a combustion section 100 providing a carbon source and energy required for synthesis; a circulation transfer substrate 200 for synthesizing and transferring carbon nanotubes; a driving part 300 for driving the circulation transfer substrate 200; a coating member 400 for coating a catalyst on the circulating transport substrate 200; a collecting member 500 for taking the carbon nanotubes from the circulating transfer substrate 200; a substrate cleaning part 800 for cleaning the substrate; a substrate cleaning member 700 for cleaning a substrate; and a control part 600 for controlling the operations of the combustion part 100, the driving part 300, the coating part 400, the collecting part 500, the substrate cleaning part 800, and the substrate cleaning part 700.

In this embodiment, the material of the circular transfer substrate 200 is copper, and is made into a sheet. The catalyst is nickel nitrate, and the treatment method comprises the following steps: 29.079g of nickel nitrate hexahydrate is dissolved in a test tube containing 100mL of absolute ethanol to prepare a 1mol/L nickel nitrate solution, and ultrasonic oscillation is carried out for 10 minutes.

In this embodiment, the control unit 600 includes a computer terminal 620 and a PLC controller 610 connected to the computer terminal 620. The computer 620 has a configuration module, which can be designed by existing software, such as DCS module, and can control the operation of the component 600 by setting relevant parameters in the configuration module.

Further, the driving part 300 includes an adjustable speed motor 310, a plurality of supporting rotating shafts 330 disposed between the rotating shafts 320, and a plurality of rotating shafts 320, the rotating shafts 320 are connected to the adjustable speed motor 310, and the circular conveying substrate 200 is carried on the rotating shafts 320; the adjustable speed motor 310 is connected to the PLC controller 610, and the computer terminal 620 controls the PLC controller 610 through the configuration module, so as to control the adjustable speed motor 310 to rotate. As shown in fig. 1, the support shaft 330 is used for supporting the circular transfer substrate 200 and controlling the travel path of the circular transfer substrate 200 during the transfer process.

Further, the combustion part 100 comprises a multi-burner combustor 110, a gas mixing chamber 130, a fuel bottle 140, a nitrogen bottle 150, an oxygen bottle 160 and a gas mass flow meter 170, wherein the nitrogen bottle 150 and the oxygen bottle 160 are connected with the gas mass flow meter 170 to the gas mixing chamber 130 through pipelines, the fuel bottle 140 is connected with the gas mass flow meter 170 to the multi-burner combustor 110 through pipelines, the circular conveying substrate 200 is conveyed above flames formed by the multi-burner combustor 110, a windshield 120 is arranged on the multi-burner combustor 110, the upper end and the lower end of the windshield 120 are open, and openings which are vertically arranged from the middle to the bottom are formed in the left end and the right end of the windshield 120, so that the circular conveying substrate 200 can rotate circularly.

The multi-burner combustor 110 of the embodiment is a methane/ethylene laminar diffusion flame combustor, methane/ethylene fuel is introduced into the multi-burner combustor 110 through an air inlet at the bottom of the multi-burner combustor 110, nitrogen and oxygen enter a gas mixing chamber 130 to be mixed and then enter the multi-burner combustor 110 through air inlets at two sides of the multi-burner combustor 110, and the windshield 120 can reduce disturbance of ambient air flow and keep combustion flame stable; the specific flow rate of each gas is 320mL/min of methane, 160mL/min of ethylene and 48L/min of air flow; the inner diameter of the fuel pipe is 10.8mm, and the outer diameter is 12.8 mm; the inner diameter of the oxidant pipe is 89.0 mm.

It should be emphasized that, according to the "solvation-dispersion-precipitation" catalytic mechanism theory proposed by Vander Wal et al, the growth process of the carbon nanotubes is: the hydrocarbon gas is cracked to generate carbon atoms, the carbon atoms are adsorbed, dissolved or diffused on the catalyst, and finally a graphite carbon layer is separated out on the surface of the catalyst to generate the carbon nano tube. Therefore, the coating unit 400 is provided in the apparatus, the coating unit 400 includes a catalyst dripping pipe 410, a rolling brush 420, and a coating dryer 430, the catalyst dripping pipe 410 is disposed above the rolling brush 420 and conveys a catalyst solution to the rolling brush 420, the rolling brush 420 is in contact with the surface of the substrate 200, the rolling direction is opposite to the overall moving direction of the substrate 200 (opposite to the direction of the arrow in the drawing), and the catalyst is coated on the surface of the substrate 200 during rolling and dried by the coating dryer 430.

Further, in order to collect the synthesized carbon nanotubes more sufficiently, the collecting part 500 includes a primary collector 510 and a secondary collector 520; the primary collector 510 includes a first blade 511 and a first container 512, the first blade 511 scrapes carbon nanotubes formed on the surface of the cyclic transfer substrate 200 and drops into the first container 512; the secondary collector 520 includes a second blade 521 and a second container 522, and the second blade 521 scrapes residual carbon nanotubes on the surface of the circulating transfer substrate 200 and drops into the second container 522.

It should be noted that the apparatus of the present invention realizes the synthesis of the carbon nanotubes by using the reciprocating manner of the substrate 200 for reciprocating and conveying, and firstly solves the problem of how to synthesize the carbon nanotubes, and in addition, solves the problem of recycling the substrate 200 for reciprocating and conveying in the reciprocating and circulating process.

The carbon nanotubes remaining on the substrate 200 are cleaned to prevent the influence of the next synthesis efficiency, and therefore, a substrate cleaning member 700 is provided, in which the substrate cleaning member 700 includes a plurality of integrated rolling cleaning brushes 710, and the rolling direction is opposite to the overall movement direction of the substrate 200 (opposite to the arrow direction in the figure), so as to clean the carbon nanotubes remaining on the scraped substrate 200.

In addition, the substrate cleaning part 800 includes an alcohol nozzle 810, an alcohol collection container 820, and a cleaning dryer 830, the alcohol nozzle 810 sprays an alcohol solution onto the surface of the circulation transfer substrate 200 to clean the surface thereof, excess alcohol sprayed onto the circulation transfer substrate 200 is collected by the alcohol collection container 820, and the circulation transfer substrate 200 cleaned by the alcohol spraying is sent to the cleaning dryer 830 to be dried. The circular conveying substrate 200 enters the preparation flow again after being cleaned, so that the circular conveying substrate can be recycled, and the cost is further reduced.

On the basis of the device, the method for continuously synthesizing the carbon nano tubes in large scale by adopting the device comprises the following steps: the speed-adjustable motor 310 is connected with the PLC 610, the PLC 610 is connected with the computer end 620, the working cycle of the speed-adjustable motor 310 is 10 seconds, the speed-adjustable motor stops for 1-10 minutes, the cycle time and the stop time are input and controlled by the configuration module of the computer end 620, and the supporting rotating shaft 330 is used for supporting and fixing the position of the circular transmission substrate 200; when the speed-adjustable motor 310 stops, the catalyst dropper 410 delivers the catalyst solution to the rolling brush 420, the rolling brush 420 coats the catalyst solution on the surface of the circular transfer substrate 200, the catalyst solution on the surface of the circular transfer substrate 200 is dried at the dryer, the carbon nanotube is prepared at the combustion part 100, the alcohol nozzle 810 sprays the alcohol solution on the surface of the circular transfer substrate 200, and then the circular transfer substrate 200 is dried in the dryer; when the speed-adjustable motor 310 rotates, the circular transfer substrate 200 moves along the rotation shaft 320, the carbon nanotubes on the surface of the circular transfer substrate 200 are scraped and collected by the carbon nanotube collecting member 500, and the scraped circular transfer substrate 200 is cleaned by the integrated rolling cleaning brush 710.

The above examples are only preferred embodiments of the present invention, it should be noted that: it will be apparent to those skilled in the art that various modifications and equivalents can be made without departing from the spirit of the invention, and it is intended that all such modifications and equivalents fall within the scope of the invention as defined in the claims.

Claims

1. An apparatus for large-scale synthesis of carbon nanotubes by flame method, comprising:

a combustion section (100) providing a carbon source and energy required for synthesis;

a circulation transfer substrate (200) for synthesizing and transferring carbon nanotubes;

a driving means (300) for driving the circulating transfer substrate (200);

a coating member (400) for coating a catalyst on the circulating transport substrate (200);

a collecting member (500) for taking the carbon nanotubes from the circulating transfer substrate (200);

a control part (600) for controlling the operation of the combustion part (100), the driving part (300), the coating part (400) and the collecting part (500).

2. The apparatus for flame mass synthesis of carbon nanotubes according to claim 1, the combustion part (100) comprises a multi-burner (110), a gas mixing chamber (130), a fuel bottle (140), a nitrogen bottle (150), an oxygen bottle (160) and a gas mass flowmeter (170), the nitrogen gas bottle (150) and the oxygen gas bottle (160) are connected with a gas mass flow meter (170) to the gas mixing chamber (130) through pipelines, the fuel bottle (140) is connected with a gas mass flow meter (170) to the multi-burner (110) through a pipeline, the circular conveying substrate (200) is conveyed to pass above the flame formed by the multi-burner (110), a windproof cover (120) is arranged on the multi-burner (110), the upper end and the lower end of the windproof cover (120) are opened, and the left and right ends are provided with openings which are vertically arranged from the middle to the bottom and are used for the circular rotation of the circular transmission substrate (200) to pass through.

3. The apparatus for flame-mass synthesis of carbon nanotubes according to claim 1, wherein the driving unit (300) comprises a speed-adjustable motor (310) and a plurality of rotating shafts (320), the rotating shafts (320) are connected to the speed-adjustable motor (310), and the circulating transport substrate (200) is mounted on the rotating shafts (320); or the control part (600) comprises a computer end (620) and a PLC (610) connected with the computer end (620), the adjustable speed motor (310) is connected to the PLC (610), and the computer end (620) controls the PLC (610) through a configuration module, so that the adjustable speed motor (310) is controlled to rotate.

4. The apparatus for synthesizing carbon nanotubes on a large scale by flame method according to claim 1, wherein the coating unit (400) comprises a catalyst dripping pipe (410), a rolling brush (420), and a coating dryer (430), the catalyst dripping pipe (410) is disposed above the rolling brush (420) and delivers a catalyst solution to the rolling brush (420), the rolling brush (420) is in contact with the surface of the substrate (200) for circulation transfer, the rolling direction is opposite to the direction of the overall movement of the substrate (200) for circulation transfer, and the catalyst is coated on the surface of the substrate (200) for circulation transfer when rolling, and is dried by the coating dryer (430).

5. The apparatus for flame-process mass synthesis of carbon nanotubes according to claim 1, wherein the collecting member (500) comprises a primary collector (510) and a secondary collector (520); the primary collector (510) comprises a first blade (511) and a first container (512), the first blade (511) scrapes carbon nanotubes formed on the surface of the circular conveying substrate (200) and falls into the first container (512); the secondary collector (520) comprises a second blade (521) and a second container (522), wherein the second blade (521) scrapes residual carbon nanotubes on the surface of the circular conveying substrate (200) and falls into the second container (522).

6. The apparatus for flame-mass synthesis of carbon nanotubes according to claim 1, further comprising a substrate cleaning unit (800), wherein the substrate cleaning unit (800) comprises an alcohol nozzle (810), an alcohol collection container (820), and a cleaning dryer (830), the alcohol nozzle (810) sprays an alcohol solution onto the surface of the circulation transport substrate (200) to clean the surface, excess alcohol sprayed onto the circulation transport substrate (200) is collected by the alcohol collection container (820), and the circulation transport substrate (200) cleaned by the alcohol spraying is sent to the dryer (830) to be dried.

7. The apparatus for flame-mass synthesis of carbon nanotubes according to claim 1, further comprising a substrate cleaning member (700), wherein the substrate cleaning member (700) comprises a plurality of integrated rolling cleaning brushes (710), the rolling direction of the integrated rolling cleaning brushes is opposite to the overall movement direction of the circularly transported substrate (200), and the substrate cleaning member cleans the scraped circularly transported substrate (200) of residual carbon nanotubes.

8. The apparatus for flame-mass synthesizing carbon nanotubes according to claim 3, wherein the driving unit (300) further comprises a plurality of supporting shafts (330) disposed between the rotating shafts (320) for supporting the circulating transport substrate (200) and controlling a traveling path of the circulating transport substrate (200) during the transport.

9. A method for large-scale continuous synthesis of carbon nanotubes using the apparatus of claim 1, comprising the steps of:

the speed-adjustable motor (310) is connected with the PLC (610), the PLC (610) is connected with the computer end (620), the working cycle of the speed-adjustable motor (310) is 10 seconds and stops for 1-10 minutes, the cycle time and the stop time are input and controlled by the configuration module of the computer end (620), and the supporting rotating shaft (330) is used for supporting and fixing the position of the circular transmission substrate (200); when the speed-adjustable motor (310) stops, the catalyst dropper (410) conveys a catalyst solution to the rolling brush (420), the rolling brush (420) coats the catalyst solution on the surface of the circular conveying substrate (200), the catalyst solution on the surface of the circular conveying substrate (200) is dried at the coating dryer (430), carbon nanotubes are prepared at the combustion part (100), the alcohol nozzle (810) sprays an alcohol solution on the surface of the circular conveying substrate (200), and then the circular conveying substrate (200) is dried in the cleaning dryer (830); when the speed-adjustable motor (310) rotates, the circular conveying substrate (200) moves along the rotating shaft (320), the carbon nano tubes on the surface of the circular conveying substrate (200) are scraped and collected by the carbon nano tube collecting component (500), and the scraped circular conveying substrate (200) is cleaned by the rolling cleaning brush.

10. The apparatus for mass-continuous synthesis of carbon nanotubes according to claim 9, wherein the material of the circulating transport substrate (200) is copper and is made into a thin sheet, the catalyst is nickel nitrate, and the treatment method is as follows: 29.079g of nickel nitrate hexahydrate is dissolved in a test tube containing 100mL of absolute ethanol to prepare a 1mol/L nickel nitrate solution, and ultrasonic oscillation is carried out for 10 minutes.