JP2005194127A - Apparatus and method for producing monolayer carbon nanotube - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an apparatus and method for producing monolayer carbon nanotubes with an enhanced collection efficiency. <P>SOLUTION: The apparatus (1) for producing monolayer carbon nanotubes is characterized as follows: in a reaction vessel (3), a pair of electrodes (13, 15) are arranged so as to face each other with an almost horizontal gap; a gas supply means (7) supplies an atmospheric gas into the reaction vessel (3) so that the atmospheric gas passes through the gap between the electrodes in one direction from below to above; above the gap between the electrodes, a collecting body (9) is installed; and a product containing monolayer carbon nanotubes composed of carbon evaporated from the anode (13) is blown off to above the gap between the electrodes by the atmospheric gas, adheres to the collecting surface (37) of the collecting body (9), and is collected in a high yield. <P>COPYRIGHT: (C)2005,JPO&NCIPI

Description

  The present invention relates to a method for producing single-walled carbon nanotubes and a production apparatus suitable for carrying out the method. Specifically, the present invention relates to a manufacturing apparatus suitable for manufacturing single-walled carbon nanotubes with improved recovery efficiency of the generated single-walled carbon nanotubes, and a manufacturing method thereof.

Single-walled carbon nanotubes are a new material that attracts attention from many fields because of their excellent properties such as conductivity, thermal conductivity, and mechanical strength. Single-walled carbon nanotubes are generally synthesized by placing carbon or a carbon raw material under high temperature conditions in the presence of a catalyst as required. As this manufacturing method, an arc discharge method, a laser evaporation method, and a chemical vapor deposition method (that is, a CVD method) are mainly known.
Among these, the arc discharge method is particularly excellent in that single-walled carbon nanotubes with few defects and good quality can be obtained. In the arc discharge method, by causing an arc discharge between at least a pair of electrodes containing carbon in the anode, carbon is evaporated from the anode, and a product containing single-walled carbon nanotubes in a spider web shape can be obtained. . However, the single-walled carbon nanotubes obtained by the arc discharge method have a lower yield than the CVD method. For this reason, various methods capable of mass production have been developed. For example, Patent Document 1 discloses a method for improving the content of single-walled carbon nanotubes in a product containing single-walled carbon nanotubes by containing a predetermined catalyst in an electrode.

JP 2003-277032 A

However, single-walled carbon nanotubes generated in the reaction vessel by arc discharge are dispersed throughout the vessel. Accordingly, the collection of single-walled carbon nanotubes has to be carried out from the container with a tweezers or the like each time a predetermined amount is produced. Therefore, in recovering single-walled carbon nanotubes, it has been desired to improve the workability and to take out single-walled carbon nanotubes manufactured in a container with a high yield, in other words, to improve the recovery efficiency. .
Therefore, the present invention has been developed to solve such conventional problems, and an object of the present invention is to provide a single-walled carbon nanotube manufacturing apparatus and a manufacturing method thereof that can improve the recovery efficiency.

  A production apparatus suitable for production of single-walled carbon nanotubes according to the present invention has a reaction vessel and a pair of electrodes that are typically horizontally opposed in the reaction vessel. These electrodes are arranged so that a gap between the electrodes is formed in a substantially horizontal direction, and is configured to generate an arc discharge capable of evaporating carbon between the electrodes. The apparatus also includes a gas supply means for supplying an atmospheric gas into the reaction vessel. Typically, it is arranged so that the supplied atmospheric gas passes through the gap between the electrodes in one direction from the bottom to the top. In addition, this apparatus includes a recovery body that can capture the single-walled carbon nanotubes made of the evaporated carbon. This collection body is preferably provided above the gap between the electrodes.

  In the manufacturing apparatus having such a configuration, first, an arc discharge is generated between a pair of electrodes to evaporate carbon between the electrodes. At the same time, the gas supplied from the gas supply means is passed through the gap between the electrodes in one direction from the bottom to the top. As a result, the single-walled carbon nanotubes made of carbon rise with the atmospheric gas from between the electrodes because the gaps between the electrodes are formed in a substantially horizontal direction. Then, the obtained single-walled carbon nanotubes are guided to the collection body provided above the gap between the electrodes and captured there. Thus, in the apparatus of this configuration, the produced single-walled carbon nanotube can be easily captured at a high yield by the recovery body. In addition, since the single-walled carbon nanotubes are captured by being lifted by the gas flow, it is possible to prevent the uneven distribution due to the influence of gravity, and to capture the single-walled carbon nanotubes widely and uniformly dispersed in the recovery body.

  Preferably, the recovery body has a recovery surface to which single-walled carbon nanotubes can be attached, and can include a forced cooling means for cooling the recovery surface to a predetermined temperature. The single-walled carbon nanotubes that have risen due to the gas flow adhere to the recovery surface and are recovered. By cooling the recovery surface by forced cooling means, the attached single-walled carbon nanotubes (that is, heated by arc discharge) can be cooled and peeling from the recovery surface can be facilitated.

  In particular, the forced cooling means may include a coolant supplied to a portion that can conduct heat with the recovery surface. The cooling effect can be easily obtained with a high effect by a simple configuration including a refrigerant.

  Preferably, the recovery body can include a recovery surface moving mechanism that can continuously update the recovery surface with respect to a position where the single-walled carbon nanotube rising with the atmospheric gas can be captured. By updating the recovery surface using the recovery surface transfer mechanism, it is possible to increase the total recovery surface area in the single-walled carbon nanotube production process and recover the single-walled carbon nanotubes thinly and almost evenly on the recovery surface. It becomes. For this reason, a uniform thin-layer single-walled carbon nanotube can be obtained. Further, the recovery efficiency is further improved by increasing the total recovery area.

  In addition, the manufacturing apparatus may further include an auxiliary recovery unit that recovers single-walled carbon nanotubes that have not been recovered by the recovery body. Preferably, it is in communication with the reaction vessel and is provided at a position where single-walled carbon nanotubes can be recovered from the atmospheric gas discharged from the vessel. The produced single-walled carbon nanotubes may not be completely captured by the recovered body, but may be partially removed from the recovered body or remain in the reaction vessel. In this case, the recovery efficiency can be further improved by recovering the single-walled carbon nanotubes that have not been captured by the recovery body by the auxiliary recovery unit.

  Preferably, at least one of the pair of electrodes is provided with an electrode holding portion that can be arranged to be movable toward the other side. The gap between the two electrodes expands during the production of single-walled carbon nanotubes due to the consumption of the anode accompanying carbon evaporation. According to this configuration, one electrode can be moved with the consumption of the anode, and the gap between the two electrodes can be kept constant. For this reason, arc discharge can be stabilized and the production efficiency of single-walled carbon nanotubes can be kept constant.

  Preferably, a stick-shaped carbon molded body is used as at least an anode, and an electrode holding portion is provided that arranges the stick-shaped electrode so as to be rotatable with respect to the central axis thereof. When the anode is stick-shaped, the consumption of the anode tends to progress unevenly on the surface facing the cathode. For this reason, by rotating the anode, the consumption can be made to proceed uniformly on the cathode facing surface.

  As another aspect of the present invention, a method for producing single-walled carbon nanotubes based on arc discharge is provided. In the method for producing single-walled carbon nanotubes according to the present invention, a pair of electrodes are typically arranged horizontally in a reaction vessel so that a gap is formed in a substantially horizontal direction, and an arc is formed between the electrodes. Generate a discharge. As a result, the carbon is evaporated from the electrodes, and the atmospheric gas is passed through the gap between the electrodes in one direction from the bottom to the top. And the single-walled carbon nanotube made of the carbon that has risen with the gas flow above the gap between the electrodes is captured.

  According to the method for producing a single-walled carbon nanotube having such a configuration, the single-walled carbon nanotube can be easily recovered with a high yield above the gap between the electrodes. This production method can be preferably carried out by any single-walled carbon nanotube production apparatus disclosed herein.

  Preferably, a mixed gas containing hydrogen gas and nitrogen gas is used as the atmospheric gas. The mixed gas having this composition can stabilize arc discharge and improve the generation rate of single-walled carbon nanotubes.

Hereinafter, preferred embodiments of the present invention will be described. Note that matters other than the matters specifically mentioned in the present specification (for example, the configuration of the pair of electrodes, the gas supply means, and the recovery body) and the matters necessary for the implementation of the present invention are the prior art in the field. It can be grasped as a design matter of those skilled in the art based on the above. The present invention can be carried out based on the contents disclosed in this specification and common technical knowledge in the field.
In the apparatus of the present invention, it is sufficient that carbon is evaporated from the anode by arc discharge and the obtained single-walled carbon nanotubes can be captured by the recovery body, and various materials and configurations are applied for that purpose. Can do. In addition, although the manufacturing apparatus disclosed here is an apparatus suitable for manufacture of a single-walled carbon nanotube, using it for manufacture of a multi-walled carbon nanotube is not restrict | limited.

Next, a single-walled carbon nanotube manufacturing apparatus according to a specific embodiment of the present invention will be described with reference to the drawings.
FIG. 1 shows a configuration example of a single-walled carbon nanotube production apparatus 1. In general, the apparatus 1 includes a reaction vessel 3, a pair of electrodes 13 and 15, a gas supply unit 7, a single-walled carbon nanotube recovery body 9, and a discharge unit 11.

The reaction vessel 3 is a pressure-resistant vessel that can be sealed, and is made of, for example, stainless steel.
The pair of electrodes 13 and 15 is such that the anode 13 and the cathode 15 are both formed in a stick shape, and the reaction vessel 3 is disposed so as to face each other with its central axis horizontal. In addition, the shape of each electrode 13 and 15 is not restricted to stick shape, What is necessary is just the surface which mutually opposes. Therefore, all of the electrodes may be tablet-like. Although the size of the gap between the anode 13 and the cathode 15 is not particularly limited, for example, 0.1 to 10 mm, particularly about 0.5 to 5 mm, in which the single-walled carbon nanotube generation efficiency by arc discharge is high is suitable. In FIG. 1, the anode 13 and the cathode 15 are both arranged horizontally, but the gap between the anode 13 and the cathode 15 may be formed substantially in the horizontal direction. Therefore, an acute angle arrangement, for example, as shown in FIG. 2, the anode 13a and the cathode 15a may be arranged so as to be inclined in a substantially C shape when viewed from the side. Conversely, as shown in FIG. 3, the anode 13b and the cathode 15b may be arranged in a substantially V shape when viewed from the side. In this case, the angle formed by the anode and the cathode can be 90 ° or less, for example, 5 to 75 °. Connected to the anode 13 and the cathode 15 is a DC power source 23 capable of applying a voltage capable of generating arc discharge between the anode 13 and the cathode 15. Although the power source is a direct current here, an alternating current power source may be used.
From the viewpoint of improving the recovery rate of single-walled carbon nanotubes, the opposing direction of the pair of electrodes used is preferably the horizontal direction as described above, but the opposing pair of electrodes is, for example, the vertical direction (in this case, typically In this case, the single-walled carbon nanotube can be produced by the production apparatus 1 even when the electrodes are arranged in the horizontal direction.

The anode 13 is a heat-resistant conductive material and is made of a material capable of evaporating carbon by arc discharge. For example, various carbon materials can be mentioned, and graphite is particularly preferable. In particular, graphite containing a catalyst for synthesizing single-walled carbon nanotubes, such as iron, nickel, or cobalt, is suitable. Such an anode 13 can be obtained by, for example, blending catalyst powder (for example, iron powder) with graphite powder and compacting it. A solenoid 22 is connected to an end portion (base portion) 19 opposite to the facing surface (tip portion) 17 of the cathode 15 in the anode 13. That is, the solenoid 22 can move the anode 13 (electrode holding portion) held by an electrode holding portion (not shown) in the horizontal direction (that is, the facing surface (tip portion) 25 direction of the cathode 15, particularly leftward in FIG. 1). It is said. Therefore, as the anode 13 is consumed due to carbon evaporation, the anode 13 can be moved to keep the gap between the electrodes 13 and 15 constant. A motor 21 is connected to the cathode 15. The motor 21 is installed so that the cathode 15 held in an electrode holding unit (not shown) can rotate with respect to its long axis.
The consumption amount of the anode 13 may be detected by attaching a sensor, or the consumption amount by the applied voltage may be set in advance and moved by a predetermined distance. Note that the electrodes 13 and 15 may be moved and / or rotated manually without using the solenoid 22 or the motor 21. That is, for example, a stick-like moving and rotating means is provided on the anode or the electrode holding part on the anode side, and one end thereof is disposed outside the container, and the one end is manually operated to horizontally move and rotate the anode or the cathode. It may be allowed.

  The cathode 15 is made of a heat-resistant conductive material, and for example, a metal material such as carbon or copper can be used. In addition, when the power source is an alternating current, carbon (particularly graphite) containing a catalyst for synthesizing single-walled carbon nanotubes is preferable, like the anode 13. The installation location of the solenoid 22 and the motor 21 as the electrode moving and rotating means is not limited to the mode shown in FIG. 1, and the motor, solenoid or manual moving rotating means is provided on either the anode 13 side or the cathode 15 side. May be.

The gas supply means 7 supplies atmospheric gas into the reaction vessel 3. The gas supply means 7 according to the present embodiment includes an atmosphere gas supply cylinder (a plurality of cylinders when a mixed gas of a plurality of types of gases is used as the atmosphere gas; two cylinders 27A and 27B in FIG. 1). A predetermined amount of atmospheric gas can be introduced into the reaction vessel 3 from the gas supply port 31 provided in a part of the reaction vessel 3 (here, the bottom surface 30) by opening and closing the valves 29A and 29B. Here, in the present embodiment, since a mixed gas of H ₂ and N ₂ is used as the atmospheric gas, the valves 29A and 29B communicating with the H ₂ cylinder 27A and the N ₂ cylinder 27B are appropriately adjusted to open and close. Thus, an atmospheric gas (H ₂ / N ₂ ) having a predetermined composition ratio is introduced. The gas supply port 31 has a tip 33 formed in a nozzle shape and is disposed toward the gap between the opposing surfaces 17 and 25 of the anode 13 and the cathode 15. With this configuration, the atmospheric gas is ejected from the gas supply port 31 toward the gap between the electrodes 13 and 15. Here, as the atmospheric gas, a mixed gas containing hydrogen gas is applicable and is not particularly limited. For example, a mixed gas of hydrogen gas and an inert gas such as nitrogen gas, helium gas, neon gas, argon gas, krypton gas, or xenon gas can be given. As in this embodiment, a mixed gas of hydrogen gas and nitrogen gas, or a mixed gas of hydrogen gas and argon gas, particularly a mixed gas of hydrogen gas and nitrogen gas is inexpensive and the production efficiency of single-walled carbon nanotubes is low. It is preferable for improvement.

  The single-walled carbon nanotube recovery body 9 is substantially hemispherical having an inner space 35 and is provided above the reaction vessel 3. The single-walled carbon nanotube recovery body 9 protrudes toward the electrodes 13 and 15 and has a curved surface as the recovery surface 37, and the single-walled carbon nanotubes blown up between the electrodes 13 and 15 are brought into contact with each other and attached. Therefore, it is preferable that the recovery surface 37 is made of a smooth metal surface, for example, stainless steel, because single-walled carbon nanotubes are easily attached by van der Waals force. In a preferred embodiment, a refrigerant supply pipe 41 and a refrigerant discharge pipe 43 are connected to the inner space 35 of the single-walled carbon nanotube recovery body 9 as a forced cooling means so that the refrigerant can be circulated. Although it does not specifically limit as a refrigerant | coolant, For example, liquid nitrogen and cooling water are mentioned, Especially since liquid nitrogen is excellent in the cooling effect among these, it is preferable. In addition, the shape of the collection body 9 is not limited to a substantially hemispherical shape, and may have a collection surface with a shape to which the blown up single-walled carbon nanotubes can adhere. Therefore, for example, a plate shape, a cylindrical shape, a spherical shape, or a sheet shape may be used.

  Here, the single-walled carbon nanotube recovery body 9 can further be provided with a moving mechanism that can update the recovery surface 37. For example, the single-walled carbon nanotube recovery body 91 shown in FIG. 4 is a belt that forms a recovery surface on the side surface of a substantially semi-cylindrical recovery body main body 96 having an inner space provided with a refrigerant supply pipe 94 and a refrigerant discharge pipe 95. 92 is wound. The main body 96 is provided with belt rotating means such as a roller 93, for example. By operating the roller 93 by a motor 98 connected to the main body 96, a recovery surface belt is attached to the side surface of the main body 96. The recovery surface belt 92 to which the single-walled carbon nanotubes are attached can be updated every predetermined time (that is, continuously or intermittently) by rotating the 92. After the single-walled carbon nanotubes adhere to a part or the entire surface of the recovery surface belt 92, a lid (not shown) that can be opened and closed is opened on the front surface of the reaction vessel 3, and the single-walled carbon nanotubes are obtained. It can be renewed to a recovery surface belt (or a recovery surface belt from which single-walled carbon nanotubes have been peeled off).

  The discharge unit 11 is attached above the recovery surface 37 of the single-walled carbon nanotube recovery body 9 above the reaction vessel 3 and outside the side surface 4 of the reaction vessel 3 so that gas can flow. That is, the discharge unit 11 is configured by sequentially connecting an auxiliary recovery unit 47 communicating with a discharge port 45 provided on the side surface 4 of the reaction vessel 3 and a vacuum pump 49 such as an oil rotary pump. The atmospheric gas introduced into the reaction vessel 3 is discharged by being sucked by the vacuum pump 49 from the discharge port 45. The atmospheric gas pressure in the reaction vessel 3 can be adjusted by sucking the gas in the reaction vessel 3 through the discharge unit 11. In the auxiliary recovery part 47, for example, 1 to 10 filters, especially 3 to 7 filters, 5 in FIG. 1, are disposed in the atmosphere gas flow path, and the single-walled carbon nanotube recovery body 9 The single-walled carbon nanotubes that have not been recovered are configured to be captured along with the passage of the atmospheric gas. Note that the auxiliary recovery unit 47 is not limited to the filter 51, and any one that can circulate gas and cannot pass the single-walled carbon nanotube-containing product may be disposed. For example, the net may be used.

  The DC power source 23, the motor 21, and the solenoid 22 (and the motor 98 in the recovery surface moving mechanism if desired) are input with control commands from a control mechanism 53 that operates based on a predetermined program or manual operation. Connected to the output circuit 55, it is possible to control the movement and rotation of the anode 13 by application of voltage (and movement of the recovery surface if desired). Therefore, the arc discharge state is calculated by the control mechanism 53 from the voltage applied between the anode 13 and the cathode 15, and the movement, rotation (and rotation) of the anode 13 according to the growth of the single-walled carbon nanotube-containing product generated by the arc discharge (and The control signal for adjusting the movement of the recovery surface) can be output from the input / output circuit 55 to the motor 21 and the solenoid 22 (and the motor 98 if desired). In this way, arc discharge under stable conditions becomes possible, and a single-walled carbon nanotube-containing product with uniform quality (and a thin layer that is uniformly and widely dispersed as desired) can be obtained.

Next, a method for producing single-walled carbon nanotubes using such a production apparatus 1 will be described. First, the anode 13 and the cathode 15 are prepared, set at a predetermined interval, and placed in an electrode holding portion (not shown) in the reaction vessel 3. And the valve 6a of the exhaust pipe 6 provided in the container 3 is opened, the vacuum pump 5 connected to the exhaust pipe 6 is operated, and the inside of the reaction container 3 is exhausted and depressurized. When the pressure in the container 3 is reduced to a high vacuum of, for example, about 13 to 1.3 × 10 ⁻³ Pa, the valve 6 a is closed, and then the atmospheric gas is introduced by the gas supply means 7. As the atmospheric gas, for example, hydrogen and nitrogen are introduced from the hydrogen gas cylinder 27A and the nitrogen gas cylinder 27B by adjusting the valves 29A and 29B, respectively, in a volume mixing ratio of 20:80 to 80:20. For example, the hydrogen gas in the reaction vessel 3 is adjusted to 1.3 × 10 ⁴ Pa and the nitrogen gas is adjusted to 1.3 × 10 ⁴ Pa by the vacuum pump 49 and the gas supply means 7.

  And a voltage is applied between the anode 13 containing iron (0.5-5 mol%) and the cathode 15, and an electric current (for example, 30-70A) is supplied from the DC power supply 23. FIG. The carbon is evaporated from the anode 13 by the arc heat generated as a result of the arc discharge. The voltage is appropriately selected according to a desired carbon evaporation rate, and is, for example, about 20 to 40V. Also, the arc discharge state is calculated by the control mechanism 53 from the applied voltage, and a control signal is output from the input / output circuit 55 to the motor 21 and the solenoid 22 in accordance with the consumption of the carbon evaporated by the arc discharge. Actuate movement and rotation.

  The evaporated carbon forms a product 60 containing single-walled carbon nanotubes in the gap between the electrodes by arc heat and catalytic action. This product 60 is blown upward of the reaction vessel 3 by the air flow of the supplied atmospheric gas. And most (preferably about 70 mass% or more, especially 90 mass% or more of the manufactured product) adheres to the collection surface 37 of the collection body 9. The ratio of the single-walled carbon nanotube contained therein is 70 mol% or more.

  The single-walled carbon nanotube-containing product 60 adhering to the recovery surface 37 has a lid (not shown) provided on the front surface of the reaction vessel 3 that can be opened and closed after the apparatus is operated to deposit a predetermined amount of single-walled carbon nanotubes. It is recovered by opening it and taking out the recovery body 9. Alternatively, the lid may be opened and peeled off from the collection surface 37 with, for example, tweezers. According to this apparatus, the single-walled carbon nanotube-containing product 60 is widely and uniformly dispersed and attached to the entire recovery surface 37, so that it can be easily taken out with tweezers.

Usually, the product thus obtained contains a catalyst such as iron powder and impurity carbon together with single-walled carbon nanotubes. These catalysts and impurity carbons can be reduced, i.e., the product can be purified. This treatment can include heat treatment and acid treatment. As the heat treatment, for example, heating can be performed at a temperature of 670 to 720 K for 25 to 35 minutes to oxidize impurity carbon in the product to CO or CO _{2 and the} like to remove it as a gas and oxidize the catalyst. In the acid treatment, the oxidized catalyst can be removed by, for example, treatment with hydrochloric acid after the heat treatment.

  According to the production apparatus and / or production method of the present invention, single-walled carbon nanotubes can be obtained in a thin and uniformly spread state. Therefore, for example, as shown in FIG. 5, the single-walled carbon nanotube 80 can be held by sandwiching this state between the two sheets 82 and 83. Although it does not specifically limit as the sheets 82 and 83, For example, the film (commercially available wraps) which consists of aluminum foil, a polyvinylidene chloride, polyethylene, etc. is suitable. In particular, when one sheet is made of aluminum foil and the other sheet is made of polyvinylidene chloride wrap, the shape retention is good and the state of the contents (ie, single-walled carbon nanotubes) can be observed from the outside. It is suitable because it can be done.

  On the other hand, the single-walled carbon nanotube-containing product 60 that has not adhered to the collection surface 37 is sucked by the vacuum pump 49 from the discharge unit 11. Then, it is captured by a filter 51 (for example, a HEPA filter) provided in the auxiliary recovery unit 47. This single-walled carbon nanotube-containing product can be recovered by opening a cover (not shown) of the auxiliary recovery unit 47 and taking out the filter 51. Alternatively, the lid can be opened and peeled off from the filter 51 with tweezers, for example. The filter 51 can be reused after the single-walled carbon nanotube-containing product is taken out. Alternatively, the filter may be replaced with a new filter. The single-walled carbon nanotube-containing product recovered by the auxiliary recovery unit 47 can be subjected to a single-walled carbon nanotube purification process as described above.

The preferred embodiments of the present invention have been described in detail above, but these are only examples and do not limit the scope of the claims. The technology described in the claims includes various modifications and changes of the above-described embodiments.
For example, a recovery surface moving mechanism as shown in FIG. 6 may be provided. That is, as shown in the drawing, a long sheet 102 (hereinafter referred to as “aluminum sheet 102”) made of an aluminum foil having a smooth surface is turned from a supply roll 101 to a rotating body 110 by rotation of guide rolls 103a and 103b. The surface 110a (preferably the surface cooled by liquid nitrogen or the like) is continuously supplied so as to be in close contact. The supplied aluminum sheet 102 is guided by the guide rolls 103a and 103b while being slid on the surface 110a, and is taken up and collected by the collection roll 106. As is apparent from the figure, in this embodiment, the aluminum sheet 102 corresponds to the collection surface of the rotating body 110 that is continuously updated. In such an embodiment, the single-walled carbon nanotubes (see the upward arrow in the figure) supplied (increased) between the electrodes 113 and 115 are continuously captured by the aluminum sheet 102 sliding on the recovery body surface 110a. Can do. The single-walled carbon nanotubes 104 deposited in layers on one surface (that is, the recovery surface) of the aluminum sheet 102 can be continuously recovered by winding the single-walled carbon nanotubes 104 together with the aluminum sheet 102 onto the recovery roll 106.
At this time, a long sheet (film) 105 made of polyvinylidene chloride, polyethylene, or the like is continuously supplied from a separately provided supply roll 108 to the single-walled carbon nanotube 104 deposition surface side of the aluminum sheet 102 via a guide roll 107. May be. As a result, as shown in the drawing, the single-walled carbon nanotubes 104 are collected as a three-layer structure in which the single-walled carbon nanotubes 104 are sandwiched between the long sheet (film) 105 and the aluminum sheet 102. 106 can be continuously collected.
Furthermore, the holding unit 120 holding the anode 113 can hold a plurality of electrodes in a plurality of holding units while being movable by a continuous electrode supply mechanism such as a revolver type (ie, rotating or other movable mechanism). Format). By doing so, it is possible to continuously supply a plurality of anodes 113 and 113a. Such continuous supply of the anode and the use of the recovery surface transfer mechanism (FIGS. 4 and 6) as described above enable continuous and mass production of single-walled carbon nanotubes and efficient recovery.

  The technical elements described in this specification or the drawings exhibit technical usefulness alone or in various combinations, and are not limited to the combinations described in the claims at the time of filing. In addition, the technology illustrated in the present specification or the drawings achieves a plurality of objects at the same time, and has technical utility by achieving one of the objects.

The schematic diagram which shows the structure of the single wall carbon nanotube manufacturing apparatus which concerns on one Embodiment. Explanatory drawing which shows the example of arrangement | positioning of another electrode. Explanatory drawing which shows the example of arrangement | positioning of another electrode. Explanatory drawing which shows an example of a collection | recovery surface moving mechanism. The schematic diagram explaining the storage form of a single-walled carbon nanotube. Explanatory drawing which shows an example of a collection | recovery surface moving mechanism.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 ... Single-walled carbon nanotube manufacturing apparatus 3 ... Reaction container 7 ... Gas supply means 9, 91, 110 ... Single-walled carbon nanotube recovery body 11 ... Discharge part 13 ... Anode 15 ... Cathode 23 ... Power supply 27A, 27B ... Gas cylinder 31 ... Gas supply port 37 ... Recovery surface 41 ... Refrigerant supply pipe 43 ... Refrigerant discharge pipe 47 ... Auxiliary recovery part 49 ... Vacuum pump 51 ... Filter 92 ... Belt (movable recovery surface)
101, 108 ... supply roll 102 ... aluminum sheet (movable recovery surface)
106 ... Recovery roll

Claims (7)

A reaction vessel;
A pair of electrodes arranged opposite to each other in the reaction vessel, the gap between the electrodes being arranged in a substantially horizontal direction, and arc discharge capable of evaporating carbon between the electrodes. A pair of electrodes to be generated;
Gas supply means for supplying an atmospheric gas into the reaction vessel, the gas supply means being arranged so that the supplied atmospheric gas passes through the gap between the electrodes in one direction from the bottom to the top;
A recovery body capable of capturing the single-walled carbon nanotubes made of the evaporated carbon, the recovery body provided above the gap between the electrodes,
A carbon nanotube production apparatus suitable for producing single-walled carbon nanotubes.   The manufacturing apparatus according to claim 1, wherein the recovery body has a recovery surface to which single-walled carbon nanotubes can be attached, and includes a forced cooling means for cooling the recovery surface to a predetermined temperature.   The said forced cooling means is a manufacturing apparatus of Claim 2 provided with the refrigerant | coolant supplied to the site | part which can conduct heat with the said collection | recovery surface.   The said recovery body is provided with the collection | recovery surface moving mechanism which can renew a collection | recovery surface continuously with respect to the position which can capture | acquire the single-walled carbon nanotube which rises with atmospheric gas, The manufacturing of Claim 2 or 3 apparatus.   Any one of Claims 1-4 provided with the auxiliary | assistant collection | recovery part connected with this reaction container which can collect | recover the single-walled carbon nanotube which was not collect | recovered in the said recovery body from the atmospheric gas discharged | emitted from the said reaction container. The manufacturing apparatus of crab. A pair of electrodes facing each other in the reaction vessel are arranged so that the gap is formed in a substantially horizontal direction, and arc discharge is generated between the electrodes,
A single-layer structure that evaporates carbon from the electrodes, passes an atmospheric gas in one direction from below to above the gap between the electrodes, and captures the single-walled carbon nanotube made of carbon above the gap between the electrodes. A method for producing carbon nanotubes.   The manufacturing method according to claim 6, wherein a mixed gas containing hydrogen gas and nitrogen gas is used as the atmospheric gas.

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