KR20090073341A - Apparatus and method for collection carbon nano tube - Google Patents

Abstract

An apparatus and a method for collecting carbon nanotubes are provided to enable to collect carbon nanotubes from a reactor rapidly and automatically. An apparatus for collecting carbon nanotubes comprises: a collecting tank(710) for collecting carbon nanotubes generated in a reactor; a storage tank(750) for storing the carbon nanotubes collected by the collecting tank; and a transfer member(760) for transferring the carbon nanotubes from the collecting tank to the storage tank. The transfer member consists of: a first transferring portion(762) for pushing the collected carbon nanotubes into the storage tank; and a second transferring portion installed within the storage tank.

Description

Apparatus and method for carbon nanotube recovery {APPARATUS AND METHOD FOR COLLECTION CARBON NANO TUBE}

The present invention relates to a method for producing carbon nanotubes, and more particularly, to a device and a method for recovering carbon nanotubes from a reactor for flowing carbon catalyst particles to produce carbon nanotubes.

Carbon nanotubes (CNTs) are formed by combining three carbon atoms adjacent to one carbon atom to form a hexagonal ring, and the hexagonal ring is formed in a cylindrical or tube form by repeating a plane in a honeycomb form.

Carbon nanotubes are materials that can exhibit metallic or semiconducting conductivity depending on their structure and can be widely applied in various technical fields. For example, carbon nanotubes are applicable to electrodes of electrochemical storage devices such as secondary batteries, fuel cells or supercapacitors, electromagnetic shielding, field emission displays, or gas sensors.

The technology methods for manufacturing such carbon nanotubes are classified into various types such as electric discharge, laser deposition, and pyrolysis vapor deposition. Recently, as mass production of carbon nanotubes is an issue, fluidized bed technology for mass synthesis has emerged. . Fluidized bed technology is a method of producing carbon nanotubes by dispersing and reacting metal catalyst particles and a hydrocarbon-based source gas in a high temperature reactor. That is, carbon nanotubes are grown on the metal catalyst by thermal decomposition of the source gas and the metal catalyst while the metal catalyst is suspended by the source gas in the reactor.

However, this fluidized-bed manufacturing technology is a starting point for research at some universities, and is a basic technical level that is practically impossible to apply to mass production.

It is an object of the present invention to provide an apparatus and method for recovering carbon nanotubes that can quickly recover carbon nanotubes from a reactor.

It is an object of the present invention to provide an apparatus and method for recovering carbon nanotubes that can lower the height of the entire installation.

It is an object of the present invention to provide an apparatus and method for carbon nanotube recovery suitable for mass production systems.

It is an object of the present invention to provide an apparatus and method for carbon nanotube recovery suitable for continuous production systems.

It is an object of the present invention to provide an apparatus and method for carbon nanotube recovery that can contribute to improved productivity.

The present invention provides an apparatus for recovering carbon nanotubes. According to an embodiment of the present invention, an apparatus for recovering carbon nanotubes from a reactor in which carbon nanotubes are generated includes a recovery tank in which carbon nanotubes generated in the reactor are recovered; A storage tank having a space for receiving and storing carbon nanotubes from the recovery tank; And a transfer member for transferring carbon nanotubes from the recovery tank to the storage space of the storage tank.

The transfer member is installed in the recovery tank, the first transporter for pushing the carbon nanotubes recovered in the recovery tank to the storage tank; And a second transporter installed in the storage tank and transporting the carbon nanotubes transported by the first transporter to an upper portion of the storage tank.

The space in which the carbon nanotubes are transported by the second transporter is partitioned from the storage space of the storage tank by a vertical partition wall.

The transfer member further includes a nozzle installed at an upper portion of the storage tank and injecting an inert gas so that the carbon nanotubes transferred by the second transfer unit fall into the storage space.

The first feeder is a pressure plate for pushing the carbon nanotubes stacked on the bottom of the recovery tank to the storage tank through the connection port; And a first driving mechanism for driving the pressure plate.

The second transfer unit is an electromagnet plate for transporting to the upper portion of the storage tank by magnetically attaching the carbon nanotubes provided to the storage tank by the first transfer unit; And a second driving mechanism for elevating the electromagnet.

The transfer member transfers carbon nanotubes from the recovery tank to the upper end of the storage tank by a transfer screw method.

The recovery tank has a discharge port that is opened and closed by a valve at the bottom, the transfer member includes a first transfer screw for transferring the carbon nanotubes dropped through the discharge port of the recovery tank to the storage tank; And a second transfer screw installed in the storage tank and transferring the carbon nanotubes transported by the first transfer screw to an upper end of the storage tank.

The transfer member has a connection port for connecting the lower end of the recovery tank and the lower end of the storage tank; A vertical transfer passage provided vertically in the storage tank to be connected to the connection port and having an upper portion open; A first transporter installed in the recovery tank and configured to push the carbon nanotubes recovered in the recovery tank into the connection port; It is installed in the vertical transport passage, and includes a second transporter for transporting carbon nanotubes introduced into the vertical transport passage through the connection port to the open upper portion of the vertical transport passage to the storage space of the storage tank. .

The apparatus for recovering the carbon nanotubes includes a negative pressure generating member that forms a negative pressure in the inner space of the recovery tank, and recovers the carbon nanotubes generated in the reactor using the negative pressure of the recovery tank.

The present invention provides a method for recovering carbon nanotubes. According to an embodiment of the present invention, a method for recovering carbon nanotubes from a reactor in which carbon nanotubes are generated includes recovering carbon nanotubes from the reactor by making a pressure inside the recovery tank; Transporting the carbon nanotubes recovered to the recovery tank to a large storage tank; The transfer step transfers carbon nanotubes from the recovery tank to the top of the storage tank.

The transfer step may include the steps of: primarily transporting carbon nanotubes stacked in the recovery tank to the storage tank; Including a second transfer step of transferring the carbon nanotubes transferred to the storage tank to an upper end thereof; In the second transfer step, the carbon nanotubes are adsorbed using an electromagnet to the upper end of the storage tank, and then the carbon nanotubes are dropped into the storage space of the storage tank by spraying an inert gas in a state where magnetic force is removed. Drop.

According to the present invention, carbon nanotubes can be recovered quickly and automatically from the reactor.

In addition, according to the present invention, accurate and reliable carbon nanotube recovery is possible.

In addition, according to the present invention, the utilization rate of the equipment can be improved by automating the recovery process of the carbon nanotubes.

Moreover, according to this invention, the height of the whole installation can be reduced.

In addition, according to the system for producing carbon nanotubes to which the present invention is applied, carbon nanotubes can be produced in large quantities.

Further, according to the present invention, the metal catalyst particles can be prevented from adhering to the reaction sidewall and reacting with the reaction sidewall.

In addition, according to the present invention, it is possible to prevent the channeling phenomenon generated while the metal catalyst is accumulated on the dispersion plate.

Moreover, according to this invention, the usage-amount of a source gas can be reduced.

In addition, according to the present invention, carbon nanotubes can be continuously produced.

In addition, according to the present invention, it is possible to improve the productivity of carbon nanotubes and to reduce manufacturing costs.

Hereinafter, exemplary embodiments of the present invention will be described in more detail with reference to FIGS. 1 to 8. The embodiments of the present invention can be modified in various forms, and the scope of the present invention should not be construed as being limited to the following embodiments. This embodiment is provided to more completely explain the present invention to those skilled in the art. Therefore, the shape of the elements in the drawings are exaggerated to emphasize a more clear description.

1 is a schematic view showing an example of a carbon nanotube mass production system of the present invention.

Referring to FIG. 1, the system 1 largely has a flow synthesis apparatus 100, a catalyst supply 300, an exhaust 500, and a recovery 700.

(Flow compounding device)

FIG. 2 is a view for explaining the flow synthesizing apparatus shown in FIG. 1.

Referring to FIG. 2, the fluid synthesis apparatus 100 (also called fluidized bed apparatus) supplies a gaseous carbon-containing gas (source gas) together with a metal catalyst to a heated reactor 112 to pyrolyze the source gas so as to pyrolyze the source gas. Will produce carbon nanotubes. The flow synthesizing apparatus 100 includes a reactor 112, a heater 130, and a rotating body 160.

(Reactor)

The reactor 112 is made of a heat resistant material such as quartz or graphite, and includes a catalyst supply port 118, a gas supply port 115, a recovery port 122, and a dispersion plate 126. It includes.

In detail, the reactor 112 includes a body 114 and a cover 116. The body portion 114 has a cylindrical shape with an upper surface open, and provides a preheating space PHS and a reaction space RS. Here, the preheating space PHS is a space that is preheated before the source gas SG flows into the reaction space RS. The reaction space RS is positioned above the preheating space PHS, and carbon nanotubes CNT are generated by the reaction of the source gas SG and the metal catalyst MC.

The body portion 114 includes a bottom surface 114a and sidewalls 114b extending from the bottom surface 114a to form a preheating space PHS and a reaction space RS. The bottom surface 114a defines a preheating space PHS together with the sidewall 114b and has a gas supply port 115 through which the source gas SG flows. In this embodiment, the body portion 114 has one gas supply port 115, but the number of gas supply ports 115 may increase with the type of gas supplied and the number of gas supply lines.

The side wall 114b of the body part 114 is made of a heat resistant material such as quartz or graphite when the single tube is a single tube. Can be added externally.

The metal catalyst (MC) includes an organometallic compound having a magnetic body, such as iron, cobalt, nickel, and the like. Due to the components of the metal catalyst (MC) it can be synthesized on the side wall in the pyrolysis process for producing carbon nanotubes (CNT). However, such a problem may be prevented by the rotating body 160, and the rotating body 160 will be described in detail later.

The cover part 116 is provided on the upper part of the body part 114. The cover part 116 is coupled to the body part 114 to seal the body part 114. An exhaust port 117 is formed at a central portion of the cover 116 to discharge the exhaust gas EG generated in the process of forming the carbon nanotubes CNT. The exhaust port 117 is connected to the exhaust part 500.

Meanwhile, the catalyst supply port 118 is provided at one side of the body portion 114 to provide the metal catalyst MC to the body portion 114. The catalyst supply port 118 receives a metal catalyst from the catalyst supply unit 300. The output end of the catalyst supply port 118 may be provided in the reaction space RS through the side wall 114b of the body portion 114 and introduce the metal catalyst MC into the reaction space.

The lower portion of the body 114 is provided with a gas supply port 115 connected to the source gas line. In this embodiment, the flow synthesizing apparatus 100 has one gas supply port, but the number of gas supply ports may be increased according to the size of the reactor 112.

The source gas line 151 is connected to the gas supply port 115 of the body 114, and provides the source gas SG to the preheating space PHS of the body 114. Here, as the source gas (SG), a hydrocarbon-based gas such as acetylene, ethylene, methane, hydrogen gas, or the like may be used. The source gas SG flows into the preheating space PHS from the source gas line 151 through the gas supply port 115. The source gas may further include a flowing gas. The flowing gas not only serves to prevent the carbon nanotubes generated by the reaction between the hydrocarbon-based gas and the metal catalyst from falling in the gravity direction due to the increase in weight due to the growth, and also provides a fluidization zone inside the reactor 112. And used to activate the reaction of the hydrocarbon-based gas (ie carbon source) with the metal catalyst. Accordingly, the flowing gas may include an inert gas such as helium, nitrogen, argon, and the like, and, if necessary, a gas such as methane, acetylene, carbon monoxide or carbon dioxide, or a mixed gas of such gas and argon gas may be used as the flowing gas. . Although not shown, an inert gas supply line may be connected to the bottom surface 114a to fill the inside of the reactor 112 with the inert gas.

On the other hand, the dispersion plate 126 is provided at the boundary between the reaction space (RS) and the preheating space (PHS). The dispersion plate 126 faces the bottom surface 114a of the body portion 114 and is disposed below the catalyst supply port 118. The distribution plate 126 has a plurality of distribution holes 126a for uniformly dispersing the source gas SG. The source gas SG is introduced into the preheating space PHS from the source gas line 151, and the source gas SG introduced into the preheating space PHS is transferred to the reaction space RS through the distribution holes 126a. Is dispersed. Since the dispersion plate 126 is less affected by the upper heater 132 and the lower heater 134, it is maintained at a temperature below 400 ° C. lower than the preheating space or the reaction space. The bottom surface of the distribution plate 126 is provided with a mesh 127 to prevent the metal catalyst falling into the preheating space (PHS) through the distribution holes 126a of the distribution plate.

The metal catalyst MC introduced into the upper portion of the distribution plate 126 reacts with the source gas SG while floating in the reaction space RS by the source gas SG passing through the distribution holes 126a. Accordingly, carbon nanotubes (CNTs) are grown on the metal catalysts MC. As described above, since the carbon nanotubes CNT are generated while the metal catalyst MC floats in the reaction space RS, the growth of the carbon nanotubes CNT is activated as the floating of the metal catalyst MC is activated.

On the other hand, carbon nanotubes (CNT) formed in the reaction space (RS) is discharged to the outside through the recovery port 122. That is, the recovery port 122 is connected to the side wall 114b (a position adjacent to the dispersion plate) of the body part 114, and an input terminal through which the carbon nanotubes (CNT) are sucked is provided in the reaction space (RS) so that the dispersion plate ( 126 is disposed on top. The recovery port 122 is connected to the recovery line 711 of the recovery unit 700, the metal catalyst on which carbon nanotubes are grown is recovered through the negative pressure air flow in the recovery unit 700.

(heater)

The heater 130 is characterized in that it is separated into an upper heater 132 and a lower heater 134 based on the distribution plate 126. The upper heater 132 and the lower heater 134 are positioned adjacent to the side wall 114b of the body portion 114 and away from the periphery of the distribution plate 126. The upper heater 132 and the lower heater 134 heat the body 114 to maintain the temperature of the reaction space (RS) and the preheating space (PHS) at an appropriate temperature. Specifically, the lower heater 134 is provided in a region corresponding to the preheating space PHS to raise the temperature of the preheating space PHS to an appropriate temperature. Accordingly, the source gas SG introduced into the preheating space PHS is heated. The upper heater 132 is provided in a region corresponding to the reaction space RS, and maintains the temperature of the reaction space RS at an appropriate temperature (600-900 ° C.) for activating growth of carbon nanotubes (CNT). .

On the other hand, since the upper heater 132 and the lower heater 134 does not directly heat the area corresponding to the dispersion plate 126, the dispersion plate 126 is the upper heater 132 and the lower heater 134 Less thermally affected by Therefore, the temperature of the dispersion plate 126 is lower than the preheating space or the reaction space, and preferably maintained below 400 ° C. As such, when the temperature of the dispersion plate 126 is maintained at 400 ° C. or less, the metal catalysts stacked on the dispersion plate 126 may be prevented from agglomerating at high temperatures.

(Rotary body)

3A to 3C are views showing the rotating bodies.

Referring to FIGS. 3A to 3C, the rotor 160 may improve the fluidization of the metal catalyst in the reaction space RS to prevent the metal catalyst from coalescing on the sidewall 114b of the reactor 112. The rotating body 160 is provided with a driving unit 162 such as a motor installed outside the reactor 112, a rotating shaft 164 installed in the reaction space RS, and receiving a rotating force from the driving unit 162, and a rotating shaft ( 164 includes a rotating frame 166 is installed. The rotating body 160 may be operated regularly or irregularly. The rotating body 160 may be rotated at a low speed (1-10 times per minute) when used to prevent catalyst adhesion on the side wall of the reactor, and may be relatively faster than a low speed rotation when used to improve the fluidized bed in the reaction space. Can be rotated.

The rotating frame 166 has blades 168 that rotate along the edge of the reaction space RS. The rotating frame 166 scrapes and removes the metal catalyst adhering to the side wall 114b of the reactor 112 as the blade 168 rotates along the edge of the reaction space RS. Both ends of the blades 168 are fixed by the support 167, and the support 167 is fixedly connected to the rotating shaft 164 horizontally. The rotating frame 166 has a rectangular frame shape having an opening in the center when viewed from the front. For stable rotation of the rotating frame 166, the lower end of the rotating shaft may be rotatably supported by the distribution plate 126.

Referring to FIG. 3A, the rotation shaft 164 is formed across the center of the rotation frame 166, thereby stably rotating the rotation frame 166. However, the rotating shaft 164 may act as an obstacle when the metal catalyst flows in the carbon nanotube synthesis process. However, as shown in FIG. 3B, when the rotating shaft 164 is connected only to the upper end of the rotating frame 166, the above problem may be minimized.

The rotating body 160 illustrated in FIG. 3C includes a first rotating frame 166-1 and a second rotating frame 166-2, and a first rotating frame 166-1 and a second rotating frame 166. -2) is provided in series with the rotation shaft 164. Here, it can be seen that the first rotation frame 166-1 and the second rotation frame 166-2 are different from each other in directions installed on the rotation shaft 164. That is, the first rotating frame 166-1 is provided in the X-axis direction, and the second rotating frame 166-2 is provided in the Y-axis direction.

As such, the flow synthesis apparatus 100 rotates the rotation body 160 periodically or irregularly in the synthesis space RS of the reactor 112, so that the metal catalyst MC is disposed on the sidewall of the reactor 112. It can be expected to improve product yield and productivity by preventing sticking.

Referring back to FIG. 3A, the rotating frame 166 of the rotating body 160 may include a bottom blade 169 that rotates on the distribution plate 126. The bottom blade 169 is positioned adjacent to the dispersion plate 126 to sweep the metal catalyst (the relatively large metal catalyst particles mentioned above) that accumulate in the dispersion plate 126, resulting from the accumulation of the metal catalyst in the dispersion plate 126. Channeling phenomenon can be prevented. The bottom blade 169 may be additionally installed in a separate configuration to the rotating frame 166. However, since the support 167 installed at the bottom of the rotating frame 166 serves as the bottom blade 169 as shown in Figure 3a, it is not necessary to install additional floor blades separately.

(Catalyst supply)

4 is a view for explaining the catalyst supply unit shown in FIG.

Referring to FIG. 4, the catalyst supply unit 300 includes a catalyst manufacturing apparatus 302, a first reservoir 310, a feeder 320, and an injector 350.

The metal catalyst is produced in the catalyst manufacturing apparatus 302. The metal catalyst produced in the catalyst manufacturing device 302 is stored in the first reservoir 310. The metal catalyst stored in the first reservoir 310 is provided to the feeder 320 as needed.

(1st storage)

The first reservoir 310 includes a first storage tank 312 and a pusher 316. The first storage tank 312 has a space 312a in which the metal catalyst which can be used for several tens of times in the flow synthesizing apparatus 100 and a passage 313 connected to the feeder. The passage 313 is provided at the upper end of the first storage tank 312. The pusher 316 is for pushing the metal catalyst stored in the first storage tank 312 into the passage 313. The pusher 316 includes a pressure plate 317 which is installed to be movable in a vertical direction in the internal space of the first storage tank 312, and a lift driver 318 for lifting the pressure plate 317 up and down. The elevating drive unit 318 is for elevating the pressure plate 317, and a linear driving mechanism such as a cylinder driving method using hydraulic / pneumatic, a motor and a ball screw driving method is applicable, and such a driving mechanism is well known in the art. Detailed description thereof will be omitted. When the metal catalyst stored in the feeder 320 is reduced to a certain amount or less, the pushing machine 316 detects this by a capacity detecting sensor (not shown) installed in the feeder 320 and pushes the detection signal to the pushing machine 316. Will be provided. The pusher 316 raises the pressure plate 317 by a signal received from a capacity detecting sensor (a signal indicating that the metal catalyst has been reduced to a certain amount or less) to raise a portion of the metal catalyst stored in the first storage tank 312. It is provided to the feeder 320 through the passage (313).

(feeder)

The feeder 320 has a second storage tank 321 in which as many metal catalysts as are used in the flow synthesizing apparatus 100 are stored. The second storage tank 321 has an upper surface 322, a side surface 324, and a lower surface 326 on which an outlet 326a is formed. Side 324 is a generally vertical upper portion 324a, a middle side portion 324b extending downwardly therefrom and inclined inwardly downward, and a lower portion extending generally vertically downwardly therefrom and providing a narrow passageway. Has 324c. Due to the above-described structure, a large amount of metal catalyst MC is stored in the space provided by the upper portion 324a in a region corresponding to the same height as compared to the space provided by the lower portion 324c. Due to the shape of the intermediate side portion 324b described above, the catalyst MC in the space provided by the upper portion 324a is smoothly supplied to the space provided by the lower portion 324c.

The second storage tank 321 is provided with a fixed-quantity supply unit 330 to supply the amount of metal catalyst to be used once in the flow synthesis apparatus.

The fixed quantity supply part 330 has an upper blocking plate 334 and a lower blocking plate 332 which can provide a quantitative space 331 in which a set amount of the metal catalyst MC can be contained. The upper blocking plate 334 and the lower blocking plate 332 are provided at the lower portion 324c. The metering space 331 is located above the discharge port 326a of the second storage tank 321, the upper blocking plate 334 is provided to the top of the metering space 331, the lower blocking plate 332 is the metering space 331 is provided at the bottom. The upper blocking plate 334 and the lower blocking plate 332 are opened and closed by a driving means 336 such as a cylinder. When the upper blocking plate 334 is closed while the lower blocking plate 332 is closed, the amount of metal catalyst MC set by the amount set between the lower blocking plate 332 and the upper blocking plate 334 is quantitatively spaced 331. Is filled in.

When the lower blocking plate 332 is opened, the metal catalyst MC contained in the metering space 331 is supplied to the injector 350 through the discharge port 326a. On the other hand, the stirrer 325 which stirs the metal catalyst MC is provided in the middle side part 324b of the 2nd storage tank 321. As shown in FIG. The stirrer 325 rotates before the metal catalyst is supplied to the metering space to remove the empty space inside the second storage tank 321 and induces the metal catalyst MC to be naturally supplied to the metering space 331. Have

(Feeder)

The injector 350 is an inlet gas 352, an inlet pipe 358 through which a metal catalyst is supplied from the inlet tank 352 to the reactor 112, and an inert gas for pressurizing the internal space of the inlet tank 352. It has a supply pipe 357. The inlet end 358a of the input pipe 358 is positioned to be spaced apart from the bottom surface of the input tank 352. And the inert gas supply pipe 357 is made of a double pipe form to surround the input pipe. The input tank 352 has an inlet port 354 through which the metal catalyst provided from the feeder 320 is introduced. The injector 350 uses the inert gas supplied from the inert gas supply pipe and presses a slight negative pressure inside the reactor 110 to supply the metal catalyst filled in the input tank 352 to the reactor 112 through the input pipe 358. ) Will be supplied internally. When the on-off valve 359 installed in the input pipe 358 is opened, the metal catalyst in the input tank 352 is inert gas due to the pressure difference (pressurization of inert gas) between the reactor 110 and the input tank 352. It is sucked into the reactor 112 through the input pipe 358 together. On the other hand, the input tank 352 is provided with a vibrator 360 for applying vibration to the input tank 352 so that the metal catalyst is easily sucked into the input pipe 358. Although not shown, an inert gas (also called a carrier gas) supplied to the input tank 352 is supplied to the reactor through the input pipe 358 together with the metal catalyst.

(Exhaust part)

FIG. 5 is a diagram for describing an exhaust unit illustrated in FIG. 1.

The exhaust unit 500 is a portion for exhausting and treating the unreacted gas generated after the carbon nanotubes are generated from the flow synthesis apparatus 100 and the residual gas (exhaust gas) after the reaction. The exhaust unit 500 includes a cyclone 510, a screwer 530, and a residual gas detector 550.

The cyclone 510 is for separating the metal catalyst from the exhaust gas containing the metal catalyst. The cyclone 510 has a cylindrical cyclone body 512, a suction tube 514 into which the exhaust gas containing the metal catalyst is sucked into the cyclone body 512, and the sucked exhaust gas and the metal catalyst are separated, respectively. An exhaust pipe 516 for discharging only the separated exhaust gas, and a collecting container 518 for discharging and collecting the metal catalyst separated from the exhaust gas. The metal catalyst collected in the collecting vessel may be used in the flow synthesis apparatus 100.

The scrubber 530 removes and purifies exhaust gas that has passed through the cyclone 510. The residual gas detection unit 550 is installed in the discharge pipe 516 connecting the cyclone 510 and the scrubber 530. The residual gas detector 550 performs gas chromatography (GC) and performs residual gas analysis (RGA).

The residual gas detection unit 550 detects whether source gas (particularly hydrogen gas) remaining in the exhaust gas remains, and determines the recovery time of the carbon nanotubes from the reactor 112. Since the residual gas detection unit 172 is constantly pressurized to suck the gas, the residual gas detection unit 172 may detect the residual gas in the exhaust gas only at a necessary stage through a valve (not shown) operation. Carbon nanotube recovery from the flow synthesis apparatus 100 may be performed according to the concentration value of the residual gas detected by the residual gas detector 550. For example, when carbon nanotube synthesis is completed in the fluid synthesis apparatus 100, purge gas (inert gas) is supplied to make the inside of the reactor 112 in an inactive state, and then carbon nanotubes are recovered in the recovery unit 700. The tube will be recovered. If the hydrogen concentration value of the residual gas is detected by the residual gas detection unit 172 or more, the valve 711a provided in the recovery line 711 connecting the reactor 112 and the recovery unit 700 of the flow synthesis apparatus. Keeps the lock). On the contrary, if the residual gas detection unit 172 detects the hydrogen concentration value of the residual gas below a predetermined value (preferably not detected at all), the valve 711a of the recovery line 711 is opened to recover the carbon nanotubes. Allow the process to proceed.

(Collection section)

FIG. 6 is a diagram for describing a recovery unit illustrated in FIG. 1.

Referring to FIG. 6, the recovery unit 700 recovers carbon nanotubes generated in a reactor using a negative pressure. The recovery unit 700 includes a recovery tank 710 and a negative pressure generating member 720, an electromagnet 730, and a cooling pump that makes the recovery space inside the recovery tank 710 lower than the internal pressure of the reactor (negative pressure). The member 740, the transfer member 760, and a large storage tank 750 are included.

The recovery tank 710 has a recovery space 712 of a size capable of recovering the carbon nanotubes generated in the reactor 112 once or three times. The negative pressure generating member 720 is installed at the upper portion of the recovery tank. And a filter 714 is installed directly below the sound pressure generating member 720. The filter 714 prevents the carbon nanotubes recovered into the recovery space 712 from entering the negative pressure generating member 720. On the other hand, the recovery tank 710 is provided with a pipe 718 connected to the screwer 530 of the exhaust unit 500 at the top. If there is residual gas remaining in the reactor 112 in the process of recovering the carbon nanotubes, there is a risk of explosion, so the air exhausted from the recovery tank 710 is a screwer 530 of the exhaust unit 500. Is provided.

The larger the size of the recovery tank 710, the larger the capacity of the negative pressure generating member 720, in particular, the larger the size of the recovery tank 710 takes a long time to form the negative pressure. Therefore, the recovery tank 710 preferably has a size small enough to recover the carbon nanotubes from one to three times from the reactor 112.

The recovery tank 710 is cooled by the cooling member 740. The carbon nanotubes produced in the reactor 112 are at a high temperature, and the carbon nanotubes are acidified when burned in contact with oxygen when the carbon nanotubes are at a high temperature (above 500 ° C.). To this end, the inside of the recovery tank 710 may be filled with an inert gas, but in this case, the maintenance cost is consumed by the enormous use of the inert gas. However, if the carbon nanotubes recovered in the recovery tank 710 are quenched using the cooling member 740 and maintained at 400 ° C. or lower, the carbon nanotubes may be prevented from being oxidized and burned even when they are in contact with oxygen.

The electromagnet 730 is installed on the bottom surface of the recovery tank 710. Electromagnet 730 is to prevent the blowing phenomenon of carbon nanotubes that are recovered to the recovery tank 710. Looking at the recovery process of carbon nanotubes, when negative pressure is generated in the recovery tank 710 by the negative pressure generating member 720, the existing carbon nanotubes are blown out of the recovery space 712 to block the filter 714. do. When the filter 714 is blocked by the carbon nanotubes, the negative pressure gradually decreases, thereby reducing the recovery efficiency. However, when the electromagnet 730 is used, the carbon nanotubes recovered in the recovery tank 710 may be prevented from being blown off by magnetic force, thereby reducing the blockage of the filter 714 by the carbon nanotubes.

On the other hand, since the recovery space of the recovery tank 710 is small, the recovered carbon nanotubes are transferred to the storage tank 750 and stored. The transfer member 760 for transferring from the recovery tank 710 to the storage tank 750 may use a drop method, a press method or an electromagnet method. However, when the drop method is applied, the recovery tank 710 has to be located higher than the storage tank 750, so that the overall height of the installation increases. Therefore, the drop method is not suitable for a facility for mass production of carbon nanotubes. In the present invention, a conveying member 760 in which a pressing method and an electromagnet method are combined are used.

The conveying member 760 includes a first conveyer 762 and a second conveyer. The first transporter 762 is installed in the recovery tank 710, a device for pushing the carbon nanotubes recovered in the recovery tank 710 into the storage tank 750 through the connection port 790. The first transporter 762 is a cylinder for driving the pressure plate 764 and the pressure plate 764 for pushing the carbon nanotubes stacked on the bottom of the recovery tank 710 into the storage tank 750 through the connection port 790. Or a first screw driving mechanism 765 of a lead screw type driven by a motor.

The second conveyer 766 is installed in the storage tank 750. The storage tank 750 provides a vertical transfer passage 753 separated from the storage space 752 by the partition wall 754, and the electromagnet plate 768 of the second transfer unit 766 is provided in the vertical transfer passage 753. ) Is installed. The second transfer unit 766 is a device for transferring the carbon nanotubes transferred by the first transfer unit 762 to the upper portion of the storage tank 750. The recovery tank 710 is positioned so that its height does not differ greatly from the storage tank 750. The connection port 790 has one end connected to a side close to the bottom of the recovery tank 710, and the other end thereof has a storage tank ( 750 is connected to the bottom (corresponding to the bottom of the storage space). Therefore, the carbon nanotubes transported through the connection port 790 are transferred to the upper end of the storage tank 750 by the second transporter 766.

On the other hand, the space in which the carbon nanotubes are transported by the second transfer unit 766 is partitioned from the storage space of the storage tank by the vertical partition 754. The second conveyer 766 includes an electromagnet plate 768 installed in the vertical conveyance passage 753 so as to be vertically movable, and a second driving mechanism 769. The electromagnet plate 768 magnetically attaches the carbon nanotubes provided to the storage tank 750 by driving the first conveyer 762. The second driving mechanism 769 transfers the electromagnet plate 768 to the upper portion of the storage tank 750. As the second drive mechanism 769, various linear drive devices such as a cylinder type or a motor and lead screw type can be used. The driving mechanisms mentioned above are not shown in detail because they can be easily implemented by those skilled in the art, and description thereof will be omitted.

On the other hand, the large-capacity storage tank 750 has a nozzle 770 is installed on the top. The nozzle 770 injects an inert gas so that the carbon nanotubes transported by the second conveyer 766 fall into the storage space 752. At this time, the nozzle 770 is preferably injected with an inert gas in a state in which the magnetic force of the electromagnet plate is removed.

7A and 7B are views for explaining a process of transferring carbon nanotubes from a recovery tank to a storage tank.

7A and 7B, the carbon nanotubes generated from the reactor 112 are recovered to the recovery tank 710 and stacked on the bottom of the recovery tank 710. At this time, the valve 792 of the connection port 790 maintains a locked state. When the recovery of the carbon nanotubes is completed, the valve 711a installed in the recovery line 711 is closed, and an inert gas is supplied into the recovery tank 710 to bring it to atmospheric pressure. The valve 7802 of the connecting port 790 is opened. In this state, when the pressure plate 764 of the first feeder 762 moves forward, the carbon nanotubes stacked on the bottom of the recovery tank 710 are vertically installed in the storage tank 750 through the connection port 790. It is pushed into the transfer passage 753 (upper electromagnet).

When the carbon nanotubes are stacked on the upper portion of the electromagnet plate 768, the electromagnet plate 768 moves to the upper portion of the vertical transfer passage 753 in a state in which the carbon nanotubes are magnetically aggregated. When the electromagnet 768 is moved to the upper portion of the vertical transfer passage 753, the magnetic force is removed, the nozzle 770 is injected by the electromagnet plate 768 by injecting an inert gas toward the electromagnet plate 768 The carbon nanotubes are dropped into the storage space 752 of the storage tank (see FIG. 7B).

8 is a view showing a conveying member of a conveying screw method.

Referring to FIG. 8, the transfer member 760a is a device for transferring carbon nanotubes from the recovery tank 710 to the upper end of the storage tank 750 by a transfer screw method. First, for this purpose, the recovery tank 710 has an outlet 717 which is opened and closed by a valve at the bottom, and the outlet 717 has a horizontal transfer passage in which the first transfer screw 772 of the transfer member 760a is installed. 771). The transfer member 760a includes a first transfer screw 772 and a second transfer screw 774. The first transfer screw 772 transfers the carbon nanotubes falling through the outlet 717 of the recovery tank 710 to the storage tank 750, and the first transfer screw 772 of the storage tank 750. A horizontal transfer passage 771 is connected to the vertical transfer passage 753. The second transfer screw 774 is installed in the vertical transfer passage 753 of the storage tank 750. The second transfer screw 774 transfers the carbon nanotubes transferred by the first transfer screw 772 to the upper end of the storage tank 750.

On the other hand, the carbon nanotubes stored in the storage space of the storage tank 750 are packaged in a fixed quantity in the packing container 780 as necessary later.

Process progress in a system for mass production of carbon nanotubes 30 having such a configuration will be briefly described.

The heater 130 heats the reactor 112 to maintain and raise the temperature of the reaction space RS to an appropriate temperature (about 600 degrees Celsius or more). At this time, the temperature of the dispersion plate 126 is maintained at a temperature lower than the temperature of the reaction space (RS). The catalyst supply unit 300 supplies the metal catalyst to the reaction space RS of the reactor 112, and the source gas is preheated in the preheating space PHS and then provided to the reaction space RS through the dispersion plate 126. do. The metal catalyst reacts with the source gas SG while growing in the reaction space RS by the source gas SG passing through the dispersion holes 126a to grow carbon nanotubes CNT.

In this process, the rotating body 160 rotates at a low speed to prevent the metal catalyst from adhering to the side wall 114b of the reactor 112 or accumulating on the dispersion plate 126. That is, the carbon nanotubes are synthesized in the metal catalyst adhering to the side wall of the reactor 112 to eliminate the problem of narrowing the reaction space by using a physical force using a rotating body. In particular, by increasing the metal catalyst layer expansion in the reaction space by the rotating body 160 can increase the time that the metal catalyst can react with the source gas to increase the production yield. Therefore, the problem of non-flow, non-flow, etc. according to the particle size during the flow reaction of the metal catalyst can be minimized, and the synthesis yield can be improved. In addition, the production cost can be lowered by reducing the amount of source gas used.

Meanwhile, while generating carbon nanotubes (CNTs) in the reactor 112, the exhaust gas EG generated in the reaction space RS passes through the exhaust port 117 on the upper surface of the reactor 112. 500). The exhaust gas provided to the exhaust path includes a metal catalyst (small particles), and the metal catalyst exhausted together with the exhaust gas is sorted in the cyclone 510 and collected in the collecting container and then used later.

When the production of carbon nanotubes (CNT) in the reactor 112 is completed, after filling with an inert gas to remove the source gas in the reactor 112, the carbon catalyst, the carbon nanotubes are grown recovery line 711 It is provided to the recovery unit 700 through). The recovery unit 700 recovers the metal catalyst on which carbon nanotubes are grown by using a negative pressure. In addition, the recovery unit 700 prevents the carbon nanotubes from oxidizing and burning by lowering the temperature of the metal catalyst on which the carbon nanotubes are recovered. The above process is repeated.

Although described with reference to the embodiments above, those skilled in the art will understand that the present invention can be variously modified and changed without departing from the spirit and scope of the invention as set forth in the claims below. Could be.

1 is a schematic view showing an example of a carbon nanotube mass production system of the present invention.

FIG. 2 is a view for explaining the flow synthesizing apparatus shown in FIG. 1.

3A to 3C are views showing the rotating bodies according to the first embodiment.

4 is a view for explaining the catalyst supply unit shown in FIG.

FIG. 5 is a diagram for describing an exhaust unit illustrated in FIG. 1.

FIG. 6 is a diagram for describing a recovery unit illustrated in FIG. 1.

7A and 7B are views for explaining a process of transferring carbon nanotubes from a recovery tank to a storage tank.

8 is a view showing a conveying member of a conveying screw method.

Explanation of symbols on the main parts of the drawings

100: flow synthesis apparatus 112: reactor

160: rotating body 300: catalyst supply

500: exhaust part 700: recovery part

Claims (12)

In an apparatus for recovering carbon nanotubes from a reactor where carbon nanotubes are produced: A recovery tank in which carbon nanotubes generated in the reactor are recovered; A storage tank having a space for receiving and storing carbon nanotubes from the recovery tank; And And a transfer member for transferring the carbon nanotubes from the recovery tank to the storage space of the storage tank. The method of claim 1, The conveying member A first transporter installed in the recovery tank and configured to push the carbon nanotubes recovered in the recovery tank into the storage tank; And a second transporter installed in the storage tank and transporting the carbon nanotubes transported by the first transporter to an upper portion of the storage tank. The method of claim 2, And a space in which the carbon nanotubes are transported by the second transporter is partitioned from a storage space of the storage tank by a vertical partition wall. The method of claim 2, The conveying member The apparatus for recovering carbon nanotubes is installed on the storage tank, and further comprising a nozzle for injecting an inert gas so that the carbon nanotubes transported by the second conveyer fall into the storage space. The method according to any one of claims 2 to 4, The first transfer machine A pressure plate for pushing carbon nanotubes stacked on the bottom of the recovery tank into the storage tank through the connection port; And a first driving mechanism for driving the pressure plate. The method according to any one of claims 2 to 4, The second transfer machine An electromagnet plate attached to the carbon nanotubes provided to the storage tank by the first transporter by magnetic force and transferred to the upper portion of the storage tank; And a second driving mechanism for elevating the electromagnet plate. The method of claim 1, The conveying member Apparatus for recovering carbon nanotubes, characterized in that for transporting carbon nanotubes from the recovery tank to the top of the storage tank by a transfer screw method. The method of claim 1, The recovery tank has an outlet opening and closing at the bottom by a valve, The conveying member A first transfer screw for transferring the carbon nanotubes falling through the discharge port of the recovery tank to the storage tank; And a second transfer screw installed in the storage tank and transferring the carbon nanotubes transferred by the first transfer screw to an upper end of the storage tank. The method of claim 1, The conveying member A connection port connecting a lower end of the recovery tank to a lower end of the storage tank; A vertical transfer passage provided vertically in the storage tank to be connected to the connection port and having an upper portion open; A first transporter installed in the recovery tank and configured to push the carbon nanotubes recovered in the recovery tank into the connection port; A second transfer unit installed in the vertical transfer passage and transferring the carbon nanotubes introduced into the vertical transfer passage through the connection port to an open upper portion of the vertical transfer passage to transfer to the storage space of the storage tank; Apparatus for recovering carbon nanotubes, characterized in that. The method of claim 1, The apparatus for recovering the carbon nanotubes is Including a negative pressure generating member for forming a negative pressure in the inner space of the recovery tank, Apparatus for recovering carbon nanotubes, characterized in that for recovering the carbon nanotubes produced in the reactor using the negative pressure of the recovery tank. In a method for recovering carbon nanotubes from a reactor in which carbon nanotubes are produced: Recovering carbon nanotubes from the reactor by making a pressure inside the recovery tank negative; And transferring the carbon nanotubes recovered to the recovery tank to a large storage tank; The transfer step A method for recovering carbon nanotubes, characterized in that for transporting carbon nanotubes from the recovery tank to the top of the storage tank. The method of claim 11, The transfer step Firstly transporting carbon nanotubes accumulated in the recovery tank to the storage tank; Including a second transfer step of transferring the carbon nanotubes transferred to the storage tank to an upper end thereof; In the second transfer step, the carbon nanotubes are adsorbed using an electromagnet to the upper end of the storage tank, and then the carbon nanotubes are dropped into the storage space of the storage tank by spraying an inert gas in a state of removing magnetic force. Method for recovering carbon nanotubes, characterized in that the floating.

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