KR20120095708A

KR20120095708A - Synthetic apparatus of continuous and large surface area graphene

Info

Publication number: KR20120095708A
Application number: KR1020110015191A
Authority: KR
Inventors: 강득주; 김주희
Original assignee: 주식회사 제이오
Priority date: 2011-02-21
Filing date: 2011-02-21
Publication date: 2012-08-29

Abstract

PURPOSE: An apparatus for continuously synthesizing plenty of continuously connected large sized graphene is provided to improve the uniformity of large sized graphene by maintaining the internal atmosphere of a reactor. CONSTITUTION: An apparatus for continuously synthesizing plenty of continuously connected large sized graphene includes a reactor(10), a graphene synthesizing unit(80), a metal catalyst sheet transporting unit, a gas supplying unit(100), and a gas sealing unit(110). The reactor includes at least one inlet and outlet. The graphene synthesizing unit synthesizes graphene based on a metal catalyst sheet(20) which is introduced through the inlet. The metal catalyst sheet transporting unit introduces the metal catalyst sheet to pass through the graphene synthesizing unit. The gas supplying unit supplies a carbon source gas into the reactor. The gas sealing unit supplies inert gas to the reactor in order to maintain the pressure of gas in the reactor.

Description

Synthetic apparatus of continuous and large surface area graphene

The present invention relates to a graphene synthesizing apparatus, and more particularly, to a device capable of synthesizing a large amount of continuous large-area graphene that can not be synthesized by a conventional synthesis method using a gas phase synthesis method.

In general, carbon has amorphous carbon and crystalline carbon, and there are diamonds, graphite, natural carbon, and soot, which are made in a natural state, and artificially made fullerene, carbon nanotubes, and graphene.

Soot is a black powder produced by random attachment of carbon. Incompletely burning gas fires, candles, and wood fires, carbon is released by heat, but it does not oxidize due to lack of oxygen.

Diamond is a material in which all the sp outermost electrons of carbon atoms are covalently bonded to surrounding carbon atoms, and are optically transparent because all the electrons are bound to carbon atoms. It is difficult to remove because of the very hard characteristics. In addition, diamond has the highest refractive index and thermal conductivity among all natural materials, but it is considered to be useful as a semiconductor manufacturing substrate because it is not the only conductive material among the materials with high thermal conductivity, and artificial manufacturing methods have been studied in various ways.

Graphite is a crystal in which three electrons are covalently bonded to surrounding carbon and one electron is not used for covalent bonds. When one atom makes three covalent bonds, the tendency to form a plane is so strong that the graphite crystals look like layered layers, while the other electrons move relatively freely between layers. One electron per atom, which is free to move around without being bound to a specific atom, is usually called free electrons. Graphite works well because there are free electrons.

Fullerenes are crystals in which 60 carbon atoms are ball-shaped together. Some atoms use three electrons and four electrons for covalent bonds, so a small number of electrons become free electrons, and these electrons cause superconductivity, and because the center is empty, large atoms such as platinum (Pt) or hydrogen It is expected that many applications will be made by trapping or storing small molecules such as (H) molecules. It does not form well in nature because it usually requires large pressures and temperatures when made.

Carbon nanotubes are crystals in which hundreds to tens of thousands of carbon atoms are killed. Except for the cylindrical shape, the superconducting phenomenon occurs because the atomic state in the crystal is similar to that of fullerene. Electromagnetic waves can be formed in the central hole to form nanowells. Nano wells are typically used as the principle that LEDs and semiconductor lasers are made. Therefore, it is expected that if a large number can be regularly arranged on the plane, a good display device can be made. In addition, carbon nanotubes are expected to make ropes that are stronger than steel because they are very strong.

Graphene is a stripped off layer of graphite. Because electrons are suspended in a thin film about 1Å thick, the electrons of the crystals are swarmed unlike other materials, and various quantum mechanical phenomena appear. This quantum mechanical phenomenon makes graphene a semiconductor.

Semiconductors currently used in industrial sites make holes or surplus electrons of any kind and move them into electric fields. Therefore, the operating speed is slow, and the operation of a lot of electrons. FETs with improved performance over transistors also require more electrons. The large number of electrons required for operation is a source of heat, causing large limits on size and operating speed. However, since graphene is a form of electrons moving directly and a thin film is one atom thick, the operating speed is theoretically 100 times faster than that of conventional semiconductors, making a small semiconductor, and a semiconductor that operates with very few electrons. As it is thin, it does not break when I steam it.

As described above, graphene has been studied for its manufacturing method due to its excellent electrical and mechanical properties, and it has been reported that mechanical stripping, high thermal decomposition, chemical reduction, lamination, chemical vapor deposition, epitaxy synthesis, organic synthesis, and the like can be used.

The mechanical peeling method is that the scotch tape is attached to the graphite, and then to the other scotch tape is repeatedly attached and detached to make the graphite powder thinner and thinner. However, this is not a method of obtaining graphene in large areas because the number of layers is not constant and the shape is not constant due to the torn shape of the paper.

The pyrolysis method is a principle in which a graphene sheet is produced by the remaining carbon (C) when the SiC single crystal is heated to decompose SiC on the surface and Si is removed. However, in such a pyrolysis method, SiC single crystal used as a starting material is very expensive, and there is a problem that it is very difficult to obtain graphene in a large area.

In chemical vapor deposition, a graphene growth catalyst is coated on a SiC substrate, heated, carbon is injected into a deposition medium, deposited, and the catalyst is removed to obtain graphene. However, the graphene may be damaged during the catalyst removal process.

Chemical exfoliation means dispersing graphene flakes from a graphite crystal onto a solution by a chemical method. After oxidizing the graphite and crushed by ultrasonic, etc., it is possible to make graphene oxide dispersed in an aqueous solution, which can be returned to graphene again using a reducing agent such as hydrazine. The dispersed graphene solution may form a large area film through a self-assembly process. However, since graphene oxide is not completely reduced and leaves many defects, electrical properties are inferior.

Epitaxy synthesis involves the carbon adsorbed or contained in a crystal at high temperatures to grow into graphene along the surface grains. In the case of SiC, the carbon contained in the crystal at high temperature is separated into the surface and grows into graphene. In Ru, etc., the adsorbed graphene diffuses from the surface to form a graphene-specific honeycomb structure. In both cases, it can be seen that the pattern of the crystal surface fits well with the crystal structure of graphene. Using this method, it is possible to synthesize graphene films with uniform crystallinity up to the size of wafers, but the electrical properties are not as good as those of graphene grown by mechanical exfoliation or CVD. The disadvantage is that it is very difficult to do.

The organic synthesis method uses tetraphenyl benzene. Using carbon-carbon bonds to tetraphenylbenzene, two aromatics are combined to form hexaphenylbenzene. When iron chloride is used as the oxidizing agent, condensation polymerization of hexaphenylbenzene is possible. This results in polyphenylbenzene, and the formation of graphene as bonds are formed between these carbons. This method has the advantage of making graphene safe and easy, but it is difficult to make large graphene. On the other hand, graphene formation method using acetaldehyde decomposition control method has been reported.

In the thermal plasma method, the isocyanate functionalized graphite oxide is exfoliated by sonication in DMF by expanding the graphite into thermal plasma and mechanically dispersing the expanded graphite with ultrasonic waves and other dispersers. Polystyrene is added to the resulting dispersion in DMF and then the dispersed material is reduced to dimethylhydrazine and the DMF solution is added to a large volume of methanol to coagulate into the polymer composite. Graphene can be obtained by isolating the condensed complex and pulverizing it into a powder.

In the expanded graphite method, artificial graphite is immersed in a mixture of concentrated sulfuric acid and concentrated acetic acid, and then rapidly heated to produce artificial graphite. The artificial graphite is formed into a film by high pressure press after the acid is removed by washing. Is generated. However, the film-like graphite produced in this way has a weak strength, not enough other physical property values, and there are also problems such as the influence of residual acid.

Meanwhile, a graphene synthesis apparatus using a gas phase synthesis method has also been proposed. However, the graphene synthesis apparatus according to the conventional gas phase synthesis method is a batch, in which the metal catalyst sheet metal is injected into the reactor, the reactor is heated and reacted for a predetermined time, and then the process of cooling the reactor is repeated to synthesize graphene. That's the way it is. However, the graphene synthesis apparatus using the conventional gas phase synthesis method is not only expensive but also very low in productivity because it is necessary to repeat the individual process in every batch, and it is difficult to meet the same process conditions in every batch, so that the homogeneity of the graphene There was a problem falling.

The present invention has been made to solve the above problems of the prior art, by continuously passing the metal catalyst sheet through the reactor to enable the synthesis and recovery of graphene using a gas phase synthesis method, the catalyst is added every time as in the prior art And stabilized the reaction conditions, and then synthesized graphene, without having to collect the synthesized graphene in the form of a platelet of a certain size, continuous large area that is connected continuously to synthesize the large area graphene of the continuous form The purpose is to provide a continuous mass synthesis apparatus of graphene.

Continuous mass-synthesizing apparatus of continuous large area graphene connected in accordance with the present invention for achieving the above object, the reactor having at least one inlet and outlet open to the outside air; Graphene synthesis unit for synthesizing graphene via a metal catalyst sheet introduced through the inlet of the reactor; A metal catalyst sheet transfer unit for transferring the metal catalyst sheet such that the metal catalyst sheet flows through the inlet and passes through the graphene synthesis unit; A gas supply unit supplying an inert gas or a carbon source gas for synthesizing the graphene into the reactor; And gas sealing means for supplying the inert gas again at the inlet and the outlet side of the reactor to maintain the gas pressure in the reactor to be equal to or higher than a predetermined pressure to block the external air from entering the reactor.

Here, the graphene recovery unit for recovering the graphene synthesized on the metal catalyst sheet passed through the reactor via a transfer body; further comprising, the metal catalyst sheet transfer unit, the continuously connected At least one of an upper surface or a lower surface of the metal catalyst sheet may be transferred to the metal catalyst sheet in an exposed state in the reactor.

In addition, when the graphene synthesized in the metal catalyst sheet through the reactor is recovered in the graphene recovery unit, the metal catalyst sheet may be added to the reactor again.

The metal catalyst sheet transfer unit may include one or more mounting units rotatably mounted with the metal catalyst sheets continuously connected to each other and to transfer the metal catalyst sheets with rotational power; And one or more rollers supporting the metal catalyst sheet at a predetermined point at both ends of the metal catalyst sheet which is continuously connected to each other.

The metal catalyst sheet transfer unit may include one or more mounting units rotatably mounted with the metal catalyst sheets continuously connected to each other; A mesh-shaped mesh belt supporting the metal catalyst sheet at a lower portion of the metal catalyst sheet which is continuously connected to the metal catalyst sheet; And a mesh belt transfer unit rotatably mounted to the mesh belt and configured to transfer the metal catalyst sheet on the mesh belt by transferring the mesh belt with rotational power.

The graphene recovery unit may further include a transfer body mounting unit in which a transfer body to which the graphene is to be transferred is mounted in a roll form; Located at the outlet of the reactor outside the transfer to transfer the graphene synthesized on the metal catalyst sheet to the transfer body by passing the metal catalyst sheet and the transfer body mounted on the transfer unit mounting unit facing each other Drive unit; And a transfer unit driving unit wound around the transfer member transferred through the transfer driving unit to the graphene in a roll form.

In addition, the metal catalyst sheet transfer unit, the first mounting unit is mounted to the metal catalyst sheet in the form of a roll; When the metal catalyst sheet mounted on the first mounting unit passes through the inside of the reactor and the graphene is synthesized, the second mounting unit for winding the metal catalyst sheet synthesized with the graphene in the form of a roll; And one or more rollers supporting the metal catalyst sheet at a predetermined point at both ends of the metal catalyst sheet.

Here, the graphene synthesis unit, the reaction zone is formed in the reactor and is blocked from the outside air by the inert gas filled in the reactor; Carbon injecting the carbon source gas supplied from the gas supply unit to the reaction zone so that the metal catalyst sheet transferred into the reaction zone by the metal catalyst sheet transfer unit reacts with the carbon source gas to synthesize the graphene. Source injection mechanisms; And heating means for heating the reaction zone.

In addition, the inert gas may include hydrogen gas.

The apparatus may further include a cooling unit cooling one region of the reactor adjacent to the outlet to cool the graphene.

And, a plurality of gates that can be opened and closed to isolate the space from the inlet to the outlet of the reactor in a certain section; And a gate driver opening and closing the gate.

The present invention synthesizes and recovers graphene by using a gas phase synthesis method and a method of continuously passing a metal catalyst sheet through a reactor, thereby continuously connecting large area graphene that cannot be synthesized by a conventional synthesis method. You can get it.

In addition, since it is possible to continuously inject the metal catalyst sheet from the outside to the inside of the reactor, it is possible to maintain a constant without changing the atmosphere inside the reactor without interrupting the synthesis process, a large area that is homogeneous and continuously connected Graphene can be synthesized in continuous mass.

Also, the moving speed of the metal catalyst sheet. By controlling the reaction temperature, the width and thickness of the metal catalyst sheet, the injection amount of carbon source gas, the amount of hydrogen gas, etc., it is possible to synthesize large area graphene that is continuously connected with various widths, thicknesses, and properties.

In addition, since the reduction process of the metal catalyst sheet, the synthesis process of graphene, and the cooling process are continuously performed, production cost is reduced.

BRIEF DESCRIPTION OF THE DRAWINGS Fig. 1 is a schematic diagram for explaining a continuous mass synthesizing apparatus of large area graphene connected in series using a vapor phase synthesis method according to a first embodiment of the present invention.
Figure 2 is a view for explaining the structure of the roller in the apparatus shown in Figure 1;
Figure 3 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using a gas phase synthesis method according to a second embodiment of the present invention.
Figure 4 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using a gas phase synthesis method according to a third embodiment of the present invention.
Fig. 5 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using vapor phase synthesis according to a fourth embodiment of the present invention.
Figure 6 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using the gas phase synthesis method according to a fifth embodiment of the present invention.
Figure 7 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using the gas phase synthesis method according to a sixth embodiment of the present invention.
8 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene connected in series using a vapor phase synthesis method according to a seventh embodiment of the present invention.

DETAILED DESCRIPTION Hereinafter, exemplary embodiments of the present invention will be described with reference to the accompanying drawings, but some components irrelevant to the gist of the present invention will be omitted or compressed, but the omitted elements are not necessarily required in the present invention. The invention can be used in combination by those skilled in the art.

1 is a schematic cross-sectional view for explaining a continuous mass synthesis apparatus (hereinafter, referred to as a graphene synthesis apparatus) of large-area graphene continuously connected according to a first embodiment of the present invention. As shown in FIG. 1, the graphene synthesis apparatus according to the first embodiment of the present invention includes a reactor 10 having a predetermined space therein, and a reduction unit 70 for reducing the metal catalyst sheet 20. The gas suitable for the graphene synthesis unit 80 for synthesizing the graphene 1 from the reduced metal catalyst sheet 20, the cooling unit 90 for cooling the synthesized graphene 1, and the reactor 10 It includes a gas supply unit 100 for supplying and the gas sealing means 110 to block the outside air from penetrating into the reactor (10).

The reactor 10 has an open structure open to the outside air, and the openings 11 and 12 including the reactor inlet 11 and the reactor outlet 12 are open to the outside, where the reactor inlet 11 and the reactor outlet are open. 12 is preferably formed only to the extent that the metal catalyst sheet 20 passes in order to block the outside and the inside of the reactor 10 as much as possible.

In addition, a first depression 13 is formed in the central portion of the reactor 10 to be recessed to form a space. The first recess 13 serves to collect and maintain the carbon source gas and may be referred to as a 'carbon source gas constrained part'. The metal catalyst sheet 20 may be introduced through the reactor inlet 11 of the reactor 10 and the metal catalyst sheet 20 may exit through the reactor outlet 12, and the metal catalyst sheet 20 may be a metal catalyst. It is conveyed by the sheet conveying unit. The description of the metal catalyst sheet transfer unit will be described later.

The gas supply unit includes a carbon source gas tank 110 (for example, an ethylene gas tank), an argon gas tank or a nitrogen gas tank 120 (an inert gas tank), and a hydrogen gas tank 130, each of which is a gas tank. Gases are supplied into the reactor 10 through the supply pipes. The gas tanks also each have a purifier. The purifier purifies the carbon source gas mixture, the inert gas mixture, and the hydrogen gas mixture, respectively, by adsorption, to supply high purity carbon source gas, inert gas, and hydrogen gas. Examples of the carbon source gas include methane, ethane, ethylene, acetylene, propylene, butane, butylene, butadiene, nucleic acid, heptane, toluene, benzene, xylene, gasoline, propane, liquefied propane gas (LPG), liquefied natural gas (LNG) ), Naphtha, carbon monoxide and alcohols.

The reduction unit 70 is for reducing the metal catalyst sheet 20 or removing foreign matters from the metal catalyst sheet 20 introduced into the reactor 10. The reduction unit 70 is connected to the reactor 10 to inert gas such as argon. A first gas nozzle 72 for injecting gas, nitrogen gas, or hydrogen gas, and first heating means 71 provided outside the reactor 10 to reduce oxides of the metal catalyst sheet 20. . The first heating means 71 is a heating device for heating the inside of the reactor 10 and is provided with a temperature sensor (not shown) to adjust the temperature of the inside of the reactor 10 to 600 ℃ to 1200 ℃. When the metal catalyst sheet 20 is not oxidized, the reduction unit performs only a function of removing foreign substances.

The graphene synthesis unit 80 synthesizes the graphene 1 by synthesizing the large area graphene 1 continuously connected by reacting the metal catalyst sheet 20 introduced into the reactor 10 with carbon source gas. A first shower head having a plurality of nozzles connected to the reactor 10 to uniformly discharge the carbon source gas, including a reaction zone (inner space formed by the first depression 13) in which the reaction is performed. (83) and the second heating means (81) installed outside the reactor (10). Since the shower head is arranged with a plurality of nozzles to evenly inject a carbon source gas to a predetermined region in the reactor 10, the graphene (1) is evenly synthesized throughout the reaction region in the reactor (10). The second heating means 81 is a heating device for heating the inside of the reactor 10 and is provided with a temperature sensor (not shown) to adjust the temperature of the inside of the reactor 10 to 600 ℃ to 1200 ℃.

The cooling unit 90 is installed in the reactor 10 and has cooling means 91 for cooling the inside of the reactor 10, and is connected to the reactor 10 so that an inert gas such as argon gas or nitrogen is introduced into the reactor 10. In addition, a third gas nozzle 92 for injecting hydrogen gas is included. The cooling means 91 may be a water cooling jacket or the like, and is formed to surround the periphery of the reactor 10. Hydrogen supplied through the third gas nozzle 92 not only forms the inside of the reactor 10 in a hydrogen atmosphere, but also serves to clean the synthesized graphene 1.

Meanwhile, the graphene 1 synthesized at the high temperature state of the graphene synthesis unit 80 exits the reactor outlet 12 and is recovered by the transfer body 66 in a transfer manner, if the graphene 1 and the metal are If the catalyst sheet 20 maintains a high temperature state, the transfer body 66 of the polymer film may be deformed, thereby preventing the smooth recovery of the graphene 1. Therefore, the cooling unit 90 is such that the graphene 1 and the metal on the metal catalyst sheet 20 passing through the reactor 10 can be smoothly recovered without affecting the transfer body 66. It also serves to cool the catalyst sheet 20.

On the other hand, the heating means (71, 81) and the cooling means (91) is formed to surround the reactor 10 to prevent convection in the entire space inside the reactor 10 can be maintained almost uniform temperature.

Since the reactor inlet 11 and the reactor outlet 12 are open to allow the metal catalyst sheet 20 to continuously enter and exit, the outside air may be penetrated. Therefore, the gas sealing means 110 supplies the inert gas such as hydrogen again from the reactor inlet 11 and the reactor outlet 12 to the inside of the reactor 10 so that the pressure of the inert gas inside the reactor 10 is increased. Do not become less than. Therefore, outside air is blocked from penetrating into the reactor 10. To this end, the gas sealing means 110 is provided with a nozzle for supplying an inert gas such as hydrogen or nitrogen from the gas supply unit 100 into the reactor 10.

Of course, if the pressure of the inert gas such as hydrogen gas in the reactor 10 is greater than the pressure of the outside air, the hydrogen gas may be discharged to the outside through the reactor inlet 11 and the reactor outlet 12, the hydrogen gas is external Emissions are dangerous. Therefore, the first gas discharge pipe 15 and the second gas discharge pipe 16 are formed in the reactor 10 adjacent to the reactor inlet 11 and the reactor outlet 12, so that the pressure of the hydrogen gas is higher than the pressure of the external air. When it becomes large, the hydrogen gas is discharged through the first gas discharge pipe 15 and the second gas discharge pipe 16 so that the pressure of the hydrogen gas inside the reactor 10 and the pressure of the external air are balanced.

The metal catalyst sheets 20 connected in series are circulated and transported outside and inside the reactor 10 by the metal catalyst sheet transfer unit. The metal catalyst sheet transfer unit includes a first mounting unit 41, a second mounting unit 42, and a plurality of rollers 30. The first mounting unit 41 and the second mounting unit 42 are shown in FIG. 1. As shown in FIG. 2, a metal catalyst sheet 20, which is located outside the reactor 10 and is continuously connected in a belt shape, is rotatably mounted to the first mounting unit 41 and the second mounting unit 42. . Thus, a predetermined region of the metal catalyst sheet 20 mounted on the first mounting unit 41 and the second mounting unit 42 is located in the reactor 10, and the metal catalyst sheet 20 is located outside the reactor outlet 12. ) Passes through the transfer drive unit 65 of the graphene recovery unit. Accordingly, the first and second metal catalyst sheets 20 in which at least one mounting unit of the first mounting unit 41 and the second mounting unit 42 are connected by rotation by a power source such as a motor (not shown) are connected to the first mounting unit. (41)-reactor inlet (11)-inside of reactor (10)-reactor outlet (12)-transfer drive unit (65)-second mounting unit (42)-first mounting unit (41)-reactor inlet (11) ... can be cycled in order. That is, the metal catalyst sheet transfer unit allows a metal catalyst sheet 20 continuously connected to a kind of conveyor system to infinitely circulate inside and outside of the reactor 10, thereby providing a catalyst for synthesizing graphene (1). The sheet 20 can be recycled.

On the other hand, in the metal catalyst sheet 20 located inside the reactor 10, since the graphene synthesis process is performed on the surface, at least one of the upper and lower surfaces of the metal catalyst sheet 20 should be transferred in an exposed state. . In addition, the metal catalyst sheet 20 should be transported to a predetermined height from the bottom of the reactor 10, a plurality of rollers 30 to support the metal catalyst sheet 20 for this purpose.

2 is a schematic perspective view for explaining a state in which the roller 30 supports the metal catalyst sheet 20. As shown in FIG. 2, the roller 30 has a pair of the metal catalyst sheet 20 facing each other on the upper and lower surfaces of the metal catalyst sheet 20 to prevent the metal catalyst sheet 20 from floating upward or sinking downward. I support it. The roller 30 is rotatably coupled to the roller driving unit 31. In addition, the roller 30 facing from the upper and lower parts is supported at both ends of the metal catalyst sheet 20. At this time, the roller 30 supports only one portion from both ends of the metal catalyst sheet 20.

That is, the graphene 1 is synthesized on the surface of the metal catalyst sheet 20. In particular, the purpose of the present invention is to allow a large area of graphene (1) connected in series to be synthesized on the metal catalyst sheet (20). Therefore, the surface of the metal catalyst sheet 20 is to be continuously exposed while passing through the reactor 10, but inevitably blocked exposure in the area passing through the roller 30, Accordingly, it is desirable to reduce the area supported by the roller 30 at both ends of the metal catalyst sheet 20 as much as possible. That is, even if only a portion of the roller 30 is supported at both ends in the width direction of the metal catalyst sheet 20 as shown in Figure 2, the metal catalyst sheet 20 can be transported without falling down, the metal catalyst sheet ( The surface of 20) is transported while keeping as much exposure as possible.

On the other hand, if the first mounting unit 41 or the second mounting unit 42 is provided with a power source, even if there is no separate power source can be circulated and transported the metal catalyst sheet 20, a separate roller drive unit 31 A power source (not shown) may be provided to support the transfer of the metal catalyst sheet 20 by rotating the roller 30.

Here, the first mounting unit 41, the second mounting unit 42, the roller drive unit 31 or the first transfer member 66 mounting unit of the graphene recovery unit described below, the transfer drive unit 65 At least one of the motor (not shown) may be linked to generate rotational power. If the metal catalyst sheet 20 is transferred and transferred by two or more power sources, the rotational power does not collide with each other. It is preferable that the driving speeds of two or more power sources are controlled so as to facilitate the transfer and transfer of the metal catalyst sheet 20.

In addition, since the movement speed of the metal catalyst sheet 20 can be controlled through the control of the motor, the time for reducing the metal catalyst sheet 20 and the synthesis time of the graphene 1 can be adjusted.

On the other hand, in consideration of the width of the graphene (1) necessary to use the metal catalyst sheet 20 having an appropriate width to this, accordingly the distance between the rollers 30 supporting at both ends of the metal catalyst sheet (20) It is also possible to take the graphene 1 having a desired width by adjusting.

In the graphene synthesizing apparatus according to the first embodiment of the present invention as described above, the reduction unit 70, the graphene synthesis unit 80, and the cooling unit 90 are continuously disposed and are continuously connected to the metal catalyst. Since the sheet 20 is continuously passed, a continuous graphene (1) synthesis process is possible.

Briefly describing the graphene synthesis method using the graphene synthesis apparatus shown in Figure 1, the metal catalyst sheet 20 is introduced into the reactor 10 from the outside of the reactor 10. Here, since the metal catalyst sheet 20 always maintains the state mounted on the first mounting unit 41 and the second mounting unit 42 over the inside and outside of the reactor 10, the inside of the reactor 10 is maintained. The metal catalyst sheet 20 is introduced into the reactor 10, and the metal catalyst sheet 20 in which the graphene 1 is recovered from the graphene recovery unit comes back into the reactor 10. Means that. Subsequently, the metal catalyst sheet 20 passes through the reduction unit 70, the graphene synthesis unit 80, and the cooling unit 90, and then is discharged to the outside through the reactor outlet 12. Therefore, the large-area graphene (1) continuously connected to the metal catalyst sheet (20) discharged through the reactor outlet (12) is synthesized, and the large-area graphene (1) is continuously connected in this way. The silver is recovered by the transfer method in the graphene recovery unit, and the metal catalyst sheet 20 is again introduced into the reactor inlet 11 through the second mounting unit 42 and the first mounting unit 41.

The graphene recovery unit located outside the reactor outlet 12 includes a first transfer unit mounting unit 61, a transfer drive unit 65, and a first transfer unit drive unit 62.

The transfer member 66 to which the graphene 1 is to be transferred may be a polymer film such as polyethylene terephthalate (PET). The transfer member 66 is mounted to the first transfer member mounting unit 61 in the form of a roll, the end of which is coupled to the first transfer member drive unit 62 through the transfer driving unit 65 to be wound. . That is, the first transfer member mounting unit 61 is a unit that stores the transfer member 66 before the graphene 1 is transferred, and the first transfer member drive unit 62 is transferred from the transfer drive unit 65 to the graph. It is a unit which winds up the transfer body 66 to which the pin 1 was transferred. Therefore, a power source (not shown) such as a motor may be connected to the first transfer member driving unit 62 to wind the transfer member 66 to which the graphene 1 is transferred in the form of a roll by rotational power.

The transfer drive unit 65 is provided in the form of a pair of rollers having a length approximately corresponding to the width of the metal catalyst sheet 20. That is, the metal catalyst sheet 20 and the transfer member 66 may pass between the roller driving member 65 in a state where they face each other. Therefore, the graphene 1 continuously synthesized on the metal catalyst sheet 20 is transferred to the transfer member 66 which is a polymer film while passing between the rollers of the transfer driving unit 65. In other words, the graphene 1 moves from the metal catalyst sheet 20 to the transfer body 66 and sticks. At this time, the width of the transfer member 66 is preferably equal to or slightly larger than the width of the metal catalyst sheet 20 so that the graphene 1 synthesized in the metal catalyst sheet 20 can be recovered in its entirety.

Thus, the metal catalyst sheet 20 passes through the transfer driving unit 65 in a state facing the transfer body 66, thereby allowing the large-area graphene 1 to be continuously connected through the transfer body 66. It can be recovered.

The graphene synthesis apparatus according to the present embodiment repeats this continuous process to synthesize a large amount of graphene (1) of a large area connected in series.

Referring to the occupied state of the gas in the reactor 10, first, the inside of the reactor 10, in which the reactor inlet 11 and the reactor outlet 12 are open to the outside, is filled with hydrogen gas and carbon source gas, and the reactor 10 The inside of) is cut off from the outside air.

The carbon source gas is uniformly supplied through the first shower head 83 connected to the gas supply unit, and hydrogen gas, which is one of the inert gases, is supplied to the reactor through the first gas nozzle 72 and the third gas nozzle 92. 10) supplied into. The inert gas is not limited to hydrogen but includes helium, neon, argon, xenon, nitrogen and the like.

Reactor inlet 11 and the reactor outlet 12 side is provided with a gas sealing means 110, the outside air can not be introduced into the reactor (10).

Since the first depression 13 of the reactor 10 is located lower than the adjacent portion, the carbon source gas injected through the first showerhead 83 directly above the first depression 13 is compared with the surrounding hydrogen. Since the specific gravity is large, it descends as it is from the first shower head 83 and is collected in the first recess 13 to form a carbon source gas layer.

A predetermined amount of hydrogen introduced into the reactor 10 is the first gas discharge pipe 15 and the second gas discharge pipe 16 formed adjacent to the reactor inlet 11 and the reactor outlet 12 of the reactor 10 It is discharged to the outside of the reactor 10 through. This is to ensure that the hydrogen present inside the reactor 10 maintains a higher pressure than the air present outside the reactor 10 so as to reliably block outside air from penetrating into the reactor 10. Excess hydrogen is injected into the reactor 10 through the first gas nozzle 72 and the third gas nozzle 92, and a predetermined amount of the hydrogen is injected into the first gas discharge pipe 15 and the second gas discharge pipe. It is discharged through (16). In addition, in order to block the discharge of hydrogen to the outside of the reactor 10 through the reactor inlet 11 without passing through the gas discharge pipes 15 and 16, a reactor zone for generating a combustion reaction with respect to hydrogen is provided at the reactor inlet 11. You can also make it.

Hereinafter, a method of continuous mass synthesis of large area graphene 1 continuously connected through the continuous mass synthesis apparatus of large area graphene continuously connected to FIG. 1 will be described.

Specifically, the reduction unit 70 and the graphene synthesis unit 80 of the reactor 10 by using the first heating means 71 and the second heating means 81 to a desired temperature, for example, 600 ℃ to 1200 ℃ Hold (step 1).

Next, an inert gas such as nitrogen gas or argon gas is supplied to the reactor 10 using the gas supply unit 100 (step 2). Accordingly, the foreign matter in the reactor 10 is removed and the atmosphere inside the reactor 10 is made an inert gas atmosphere.

Next, hydrogen gas is supplied into the reactor 10 using the gas supply unit 100 (step 3).

Thereafter, a metal catalyst sheet 20 having a thickness of 1 to 100 micrometers and a width of 1 to several hundred centimeters is supplied from the outside to the inside of the reactor 10 through the reactor inlet 11 (step 4). The metal catalyst sheet 20 is supplied by the metal catalyst sheet transfer unit.

The metal catalyst sheet 20 supplied into the reactor 10 may be copper, cobalt, nickel, platinum, molybdenum, or an alloy thereof.

In the metal catalyst sheet 20 moved into the reactor 10, oxides and foreign substances are removed by the reduction treatment of the reduction unit 70 (step 5).

The metal catalyst sheet 20 passing through the reduction unit 70 is moved to the graphene synthesis unit 80. The metal catalyst sheet 20 transferred to the graphene synthesis unit 80 reacts with the carbon source gas to synthesize graphene 1 (step 6).

Synthesis of the graphene (1) is carried out in a hydrogen atmosphere, the hydrogen removes the metal oxide formed on the surface of the metal catalyst sheet 20 particles, the carbon atom is excessively supplied to the surface of the metal catalyst sheet 20 Suppress it. In addition, the hydrogen removes the amorphous carbon material adsorbed on the surface of the metal catalyst sheet 20 and suppresses the attachment of the amorphous carbon mass or carbon particles to the outer wall of the graphene 1 to be grown. Of course, by controlling the carbon source gas flow rate and the synthesis temperature when the graphene (1) is synthesized, the growth rate, the number of walls, and the crystallinity of the graphene (1) may be controlled.

The metal catalyst sheet 20 in which the graphene 1 is synthesized is moved to the cooling unit 90 and forcedly cooled by the cooling means 91 (step 7).

The synthesized high purity continuous large area graphene 1 is cooled to room temperature while passing through the cooling unit 90, and the synthesized continuous large area graphene 1 is washed in a hydrogen atmosphere. Repeat.

Finally, the synthesized continuous large area graphene 1 is discharged to the outside through the reactor outlet 12 in accordance with the transfer of the metal catalyst sheet 20 (step 8). Continuously connected large-area graphene (1) contained in the discharged metal catalyst sheet 20 is transferred to the transfer member 66 by the transfer driving unit 65 of the graphene recovery unit is recovered, the graphene The transfer member 66 to which the pin 1 has been transferred is wound around and stored in the first transfer object drive unit 62 (step 9). Since the metal catalyst sheet 20 is introduced into the reactor 10 again, the graphene (1) synthesis process is repeated, so that large-scale synthesis of large-area graphene (1) continuously connected is possible.

This continuous large area graphene continuous mass synthesis apparatus according to the present invention must be sure to block the ingress of air inside.

When oxygen is present inside the reactor 10 due to air infiltration, oxygen does not instantly react with carbon source gas to obtain graphene (1), and oxygen may react with hydrogen to cause an explosion. Therefore, the inside of the reactor 10 is required to be a state in which oxygen is excluded.

The conventional batch graphene synthesis apparatus using gas phase synthesis method adopts a structure that completely blocks the inside of the reactor from the outside in order to make the inside of the reactor oxygen-excluded, and the inside of the reactor is filled with inert gas.

However, in this structure, the graphene (1) was synthesized by heating the inside of the reactor every step, and after the synthesis was completed, the process of cooling the inside of the reactor again was repeated. Therefore, apart from the time to synthesize the graphene (1), the preparation time for the graphene (1) synthesis takes a lot, there was a limit to the productivity.

In contrast, in the present invention, the internal state of the reactor 10 is always maintained in a reaction environment in which graphene 1 is synthesized, and is not changed. Therefore, the graphene synthesis apparatus according to the embodiment of the present invention does not stop at any moment when the operation of the apparatus is started, and the graphene synthesis process is performed while the metal catalyst sheet 20 continuously connected is continuously passed. Accordingly, the synthesis of large-area graphene (1) connected in series can be made.

Continuous maintenance of such a reaction environment is possible because the metal catalyst sheet 20 continuously flows into the reactor 10 in a state in which the inside of the reactor 10 is completely opened to the outside. In addition, since the graphene 1 is synthesized even at the moment when the metal catalyst sheet 20 is continuously introduced, it is possible to continuously maintain the reaction environment. In other words, although the graphene 1 is being synthesized, new metal catalyst sheets 20 (ie, metal catalyst sheets 20 connected in series) can be continuously introduced into the reactor 10. will be.

To this end, the inside of the reactor 10 is completely open to the outside, but a specific gas occupying a certain area of the reactor 10 completely blocks the inflow of outside air. That is, the reactor inlet 11 and the reactor outlet 12 are formed to be large enough to allow the metal catalyst sheet 20 to pass therethrough, and an inert gas such as hydrogen in the reactor 10 through the gas sealing means 110. By supplying again to maintain the pressure of the hydrogen not lower than the pressure of the outside air, the outside air is blocked from penetrating the inside of the reactor (10).

FIG. 3 is a schematic diagram for explaining a continuous mass synthesis apparatus (hereinafter, referred to as a graphene synthesis apparatus) of large-area graphene continuously connected according to a second embodiment of the present invention. As shown in FIG. 3, the graphene synthesizing apparatus according to the second embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the first embodiment shown in FIG. 1. The configuration of the unit 80, the cooling unit 90 and the gas sealing means 110, etc., and the description of the configuration having the same reference numeral as in Fig. 1 will be replaced by the description in the first embodiment.

In the graphene synthesis apparatus according to the second embodiment shown in FIG. 3, the metal catalyst sheet transfer unit is different from that in the first embodiment, and the metal catalyst sheet transfer unit in the graphene synthesis apparatus according to the second embodiment may be made. The first mounting unit 41, the second mounting unit 42, the mesh belt 51 and the mesh belt transfer unit 52 is implemented.

The first mounting unit 41 and the second mounting unit 42 are located outside the reactor 10, and the metal catalyst sheet 20 continuously connected in a belt shape is mounted with the first mounting unit 41 and the second mounting unit. It is attached to the unit 42 rotatably. Thus, a predetermined region of the metal catalyst sheet 20 mounted on the first mounting unit 41 and the second mounting unit 42 is located in the reactor 10, and the metal catalyst sheet 20 is located outside the reactor outlet 12. ) Passes through the transfer drive unit 65 of the graphene recovery unit.

In addition, the mesh belt 51 supports the metal catalyst sheet 20 from the bottom so that the metal catalyst sheet 20 is transferred from the bottom of the reactor 10 to a predetermined height. That is, the mesh belt 51 is rotatably mounted to the mesh belt conveying unit 52 located outside the reactor 10, and is provided by a power source such as a motor (not shown) associated with the mesh belt conveying unit 52. Due to the generated rotational force, the mesh belt 51 may be circulated to pass through the inside of the reactor 10. Therefore, since the mesh belt 51 supports the metal catalyst sheet 20 in the reactor 10, the metal catalyst sheet 20 may be transferred together by the transfer of the mesh belt 51. In this case, a separate power source for transmitting power to the first mounting unit 41 and the second mounting unit 42 may not be implemented to transfer the metal catalyst sheet 20. However, according to the embodiment, the first mounting unit 41 or the second mounting unit 42 is connected to a power source controlled at an appropriate rotational speed so that the metal catalyst sheet 20 and the mesh belt 51 are transported together by rotational power. You can also

Here, the mesh belt 51 may be supported by a separate roller (not shown) inside the reactor 10. A roller (not shown) for supporting the mesh belt 51 may include the roller 30 shown in FIG. It does not need to be shaped to support only a partial area of both ends.

Thus, in the graphene synthesis apparatus according to the second embodiment, since the metal catalyst sheet 20 introduced into the reactor 10 is transported while being supported by the mesh belt 51, the upper surface of the metal catalyst sheet 20 is provided. Can always be transported exposed. Therefore, there is an advantage that the graphene synthesis process is performed in all regions of the upper portion of the metal catalyst sheet 20.

In addition, since a plurality of perforations are formed in the mesh belt 51, most of the area of the lower surface of the metal catalyst sheet 20 is also transferred to the exposed state inside the reactor 10 by the perforations. Therefore, the graphene 1 may be synthesized on the lower surface of the metal catalyst sheet 20, and may be recovered by using the graphene 1 synthesized on the lower surface of the metal catalyst sheet 20. have.

Meanwhile, components not described in the graphene synthesizing apparatus according to the second embodiment shown in FIG. 3 are replaced by descriptions in the first embodiment in which the components having the same reference numerals are described.

4 is a schematic diagram for explaining a continuous mass synthesis apparatus (hereinafter, referred to as a graphene synthesis apparatus) of large-area graphene continuously connected according to a third embodiment of the present invention. As shown in FIG. 5, the graphene synthesizing apparatus according to the third embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the first embodiment shown in FIG. 1. The unit 80, the cooling unit 90, and the gas sealing means 110 is provided.

However, in the graphene synthesis apparatus according to the third embodiment, the first recessed portion 13 and the second recessed portion 14 are formed in the reactor 10, and accordingly, the metal catalyst is more than in the reactor in the first embodiment. The length of the section through which the sheet 20 passes becomes longer. In addition, the gas is supplied through the first gas nozzle 72 at the front end of the first recess 13 to supply an inert gas to the space inside the reactor 10 which is longer, and the first recess 13 and the first recess 13 are provided. Gas is supplied between the second depressions 14 through the second gas nozzle 73, and gas is supplied from the rear end of the second depressions 14 through the third gas nozzle 92.

In addition, an inert gas is supplied to the first recess 13 through the first shower head 83, and a carbon source gas is supplied to the second recess 14 through the second shower head 84.

In addition, heat is supplied to the front end of the first recess 13 and the second heating means 81 is provided from the first recess 13 to the front end of the second recess 14. Heat is supplied through the second recess 14, and heat is supplied through the third heating means 82. The cooling means 91 is provided at the rear end of the second recess 14.

The graphene synthesizing apparatus according to the third embodiment will be described below with respect to the difference from the first embodiment.

First, in the first embodiment, the metal catalyst sheet 20 passes through a relatively short section and undergoes a reduction process, a graphene synthesis process, and a cooling process. Thus, it may pass through a sufficient hydrogen atmosphere and not be preheated. In contrast, the third embodiment fills a relatively long section in the reactor 10 with a hydrogen atmosphere so that the metal catalyst sheet 20 passes through a long hydrogen gas and is heated to remove oxides and foreign substances. In addition, since hydrogen is confined in the space formed by the first recess 13, the reduction and washing process can be more surely performed.

Therefore, in this case, the reduction unit 70 includes the first gas nozzle 72, the first shower head 83, and the second gas nozzle 73, which supply an inert gas from the front end of the second depression 14, and heat. It comprises a first heating means 71 and the second heating means 81 for supplying the.

In addition, the metal catalyst sheet 20 reacts with the carbon source gas in the reaction region of the second recess 14 having the second shower head 84 to synthesize graphene 1, and the second recess 14 Cool through). Therefore, the graphene synthesis unit 80 includes a second shower head 84 for supplying carbon source gas from the second recess 14 and a third heating means 82 for supplying heat, and the cooling unit ( 90 includes a third gas nozzle 92 for supplying an inert gas from the rear end of the second recess 14 and cooling means 91 for cooling the inside of the reactor 10.

On the other hand, the components not described in the graphene synthesis apparatus according to the third embodiment shown in FIG. 4 are replaced with the description in the first embodiment, which describes the components having the same reference numerals.

FIG. 5 is a schematic diagram for explaining a continuous mass synthesis apparatus (hereinafter, referred to as a graphene synthesis apparatus) of large area graphene continuously connected according to a fourth embodiment of the present invention. As shown in FIG. 5, the graphene synthesizing apparatus according to the fourth embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the case of the third embodiment illustrated in FIG. 4. The unit 80, the cooling unit 90, and the gas sealing means 110 is provided.

However, in the graphene synthesis apparatus according to the fourth embodiment, the graphene recovery unit is applied to recover the graphene 1 from both the upper and lower surfaces of the metal catalyst sheet 20.

That is, in the fourth embodiment, the graphene recovery unit includes the first transfer body mounting unit 61, the first transfer body driving unit 62, the second transfer body mounting unit 63, and the second transfer body driving unit 64. ) And a transfer driving unit 65.

The transfer member 66, which is a polymer film such as PET, is mounted in a roll form on the first transfer member mounting unit 61, and an end thereof passes through the transfer driving unit 65 to the first transfer member drive unit 62. Combined and wound. At this time, when the transfer body 66 mounted on the first transfer member mounting unit 61 passes through the transfer driving unit 65 in a state facing the upper surface of the metal catalyst sheet 20, the first transfer member drive unit Is coupled to (62). That is, the first transfer member mounting unit 61 and the first transfer member drive unit 62 are configured to recover the graphene 1 synthesized on the upper surface of the metal catalyst sheet 20.

In addition, the transfer body 66 is also mounted on the second transfer body mounting unit 63, and an end of the transfer body 66 mounted on the second transfer body mounting unit 63 passes through the transfer driving unit 65. It is coupled to the second transfer object driving unit 64 to be wound. At this time, when the transfer body 66 mounted on the second transfer member mounting unit 63 passes through the transfer driving unit 65 in a state facing the lower surface of the metal catalyst sheet 20, the second transfer member drive unit Coupled to 64. That is, the second transfer member mounting unit 63 and the second transfer member drive unit 64 are configured to recover the graphene 1 synthesized on the lower surface of the metal catalyst sheet 20.

The metal catalyst sheet 20 is transported in a state in which only a portion of both ends thereof are supported by the rollers 30 in the reactor 10. Accordingly, the upper and lower surfaces of the metal catalyst sheet 20 are both exposed to the reactor. (10) to pass through the interior. Therefore, when the metal catalyst sheet 20 passes through the reactor 10, the graphene 1 is synthesized not only on the top surface but also on the bottom surface of the metal catalyst sheet 20. Therefore, as in the fourth embodiment, the metal catalyst sheet 20 exiting the reactor outlet 12 is passed through the transfer driving unit 65 while the transfer body 66 is formed on both the upper and lower surfaces of the metal catalyst sheet 20. When passing through each facing), it is possible to recover all the graphene (1) synthesized in the upper and lower metal catalyst sheet 20, the productivity of the large area graphene (1) connected in succession accordingly That's nearly double the improvement.

On the other hand, components not described in the graphene synthesis apparatus according to the fourth embodiment shown in FIG. 5 are replaced with the descriptions in the first and third embodiments having the same reference numerals.

FIG. 6 is a schematic diagram for explaining a continuous mass synthesis apparatus (hereinafter, referred to as a graphene synthesis apparatus) of large-area graphene continuously connected according to a fifth embodiment of the present invention. As shown in FIG. 6, the graphene synthesizing apparatus according to the fifth embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the first embodiment of FIG. 1. The configuration of the unit 80, the cooling unit 90 and the gas sealing means 110, etc., and the description of the configuration having the same reference numeral as in Fig. 1 will be replaced by the description in the first embodiment.

In the graphene synthesis apparatus according to the fifth embodiment shown in FIG. 6, the metal catalyst sheet transfer unit and the graphene recovery unit are different from those in the first embodiment, and the metal catalyst in the graphene synthesis apparatus according to the fifth embodiment The sheet transfer unit also serves as a graphene recovery unit. That is, the metal catalyst sheet transfer unit in the graphene synthesizing apparatus according to the fifth embodiment includes a first mounting unit 42 ', a second mounting unit 41', and a roller 30. In the first embodiment, The configuration of the transfer driving unit 65, the first transfer member mounting unit 61, and the first transfer member drive unit 62, which are the components for recovering the synthesized graphene 1, are not included.

The first mounting unit 42 'and the second mounting unit 41' are respectively located outside the reactor inlet 11 and the reactor outlet 12 side of the reactor 10, and the graphene 1 is to be synthesized with metal. Both ends of the catalyst sheet 20 pass through the reactor 10 and are coupled to the first mounting unit 42 'and the second mounting unit 41'.

That is, the metal catalyst sheet 20 is mounted in the form of a roll in the first mounting unit 42 ′, and the end is passed through the inside of the reactor 10 to be coupled to and wound around the second mounting unit 41 ′. That is, the first mounting unit 42 'is a unit for storing the metal catalyst sheet 20 before the graphene 1 is synthesized, and the second mounting unit 41' is a graphene (1) in the reactor 10. ) Is a unit for winding and storing the synthesized metal catalyst sheet (20). Therefore, a power source (not shown) such as a motor may be connected to the second mounting unit 41 ′ to wind the metal catalyst sheet 20 in which the graphene 1 is synthesized in a roll form by rotating power.

Thus, the metal catalyst sheet 20 wound in the form of a roll in the first mounting unit 42 'passes through the reactor 10, and graphene 1 is synthesized, and the graphene 1 metal catalyst sheet is synthesized ( 20 is wound around the second mounting unit 41 'and recovered, whereby the large-area graphene 1 continuously connected can be recovered.

The metal catalyst sheet 20 in the state in which the graphene 1 wound around the second mounting unit 41 ′ is synthesized may be supplied as it is in a roll form, or may be cut and supplied at a predetermined interval. In addition, if necessary, only the graphene 1 may be scraped and supplied from the metal catalyst sheet 20, or the graphene 1 may be transferred to a polymer film such as PET.

Meanwhile, components not described in the graphene synthesizing apparatus according to the fifth embodiment shown in FIG. 6 will be replaced with the descriptions in the first embodiment describing the components having the same reference numerals.

7 is a schematic diagram for explaining a continuous mass synthesis apparatus of large area graphene (hereinafter referred to as a "graphene synthesis apparatus") continuously connected according to a sixth embodiment of the present invention. As shown in FIG. 7, the graphene synthesizing apparatus according to the sixth embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the first embodiment shown in FIG. 1. The configuration of the unit 80, the cooling unit 90 and the gas sealing means 110, etc., and the description of the configuration having the same reference numeral as in Fig. 1 will be replaced by the description in the first embodiment.

In the graphene synthesis apparatus according to the sixth embodiment of FIG. 7, the metal catalyst sheet transfer unit and the graphene recovery unit are different from those in the first embodiment, and the metal catalyst in the graphene synthesis apparatus according to the sixth embodiment The sheet transfer unit also serves as a graphene recovery unit. That is, the metal catalyst sheet transfer unit in the graphene synthesis apparatus according to the sixth embodiment includes a first mounting unit 42 ', a second mounting unit 41', a mesh belt 51 and a mesh belt conveying unit 52. Is implemented.

That is, the metal catalyst sheet 20 is mounted in the form of a roll in the first mounting unit 42 ′, and the end is passed through the inside of the reactor 10 to be coupled to and wound around the second mounting unit 41 ′. That is, the first mounting unit 42 'is a unit for storing the metal catalyst sheet 20 before the graphene 1 is synthesized, and the second mounting unit 41' is a graphene (1) in the reactor 10. ) Is a unit for winding and storing the synthesized metal catalyst sheet (20).

That is, the metal catalyst sheet 20 is mounted on the first mounting unit 42 'and the second mounting unit 41', and the method for recovering the metal catalyst sheet 20 in the state where the graphene 1 is synthesized is performed. It will be fully understood from the description in the fifth embodiment.

However, in the sixth embodiment, the mesh belt 51 supports the metal catalyst sheet 20 from the bottom in order to transfer the metal catalyst sheet 20 to a state in which the height of the metal catalyst sheet 20 is raised from the bottom of the reactor 10.

That is, the mesh belt 51 is rotatably mounted to the mesh belt conveying unit 52 located outside the reactor 10, and is provided by a power source such as a motor (not shown) associated with the mesh belt conveying unit 52. Due to the generated rotational force, the mesh belt 51 may be circulated to pass through the inside of the reactor 10. Therefore, since the mesh belt 51 supports the metal catalyst sheet 20 in the reactor 10, the metal catalyst sheet 20 may be transferred together by the transfer of the mesh belt 51. In this case, a separate power source for transmitting power to the second mounting unit 41 ′ to transfer the metal catalyst sheet 20 may not be implemented. However, according to the implementation, a power source controlled at an appropriate rotational speed may also be linked to the second mounting unit 41 'so that the metal catalyst sheet 20 and the mesh belt 51 may be transferred together by rotational power.

The manner of transferring the metal catalyst sheet 20 through the mesh belt 51 and the mesh belt conveying unit 52 will be fully understood through the description in the second embodiment.

8 is a schematic view for explaining a graphene synthesis device according to a seventh embodiment of the present invention. As shown in FIG. 8, the graphene synthesizing apparatus according to the seventh embodiment of the present invention has a reduction unit 70, a gas supply unit 100, and graphene synthesis similarly to the first embodiment shown in FIG. 1. The configuration of the unit 80, the cooling unit 90 and the gas sealing means 110, etc., and the description of the configuration having the same reference numeral as in Fig. 1 will be replaced by the description in the first embodiment.

The graphene synthesis apparatus according to the seventh embodiment shown in FIG. 8 further includes a gate 17 and a gate driver 18 to isolate certain sections of the reactor 10 from each other. In addition, the metal catalyst sheet 21 cut to a length that can be located between the gates 17 rather than the metal catalyst sheet connected to both the reactor inlet 11 and the reactor outlet 12 is graphene (1). A metal catalyst sheet supply unit 32, a roller 30, and a metal catalyst sheet recovery unit 67, which are supplied for synthesis and are capable of supplying, transporting and recovering the metal catalyst sheet 21.

That is, the gate 17 is between the reactor inlet 11, the gas sealing means 110 on the reactor inlet 11 side and the first heating means 71, the first heating means 71 and the second heating means 81. Between the second heating means 81 and the cooling means 91, between the cooling means 91 and the gas sealing means 110 on the reactor outlet 12 side, and at the reactor outlet 12, respectively. 17 are opened and closed by the gate driver 18.

If the gates 17 are all closed, the reactor 10 is completely separated into a sealing section-reduction section-synthesis section-cooling section-sealing section.

Thus, having the gate 17 to separate the inside of the reactor 10 into each section, the atmosphere in each section to minimize the influence on the atmosphere of the other section, the air outside the reactor 10 It is to be able to block even more completely.

Therefore, after the inert gas is filled in the reactor 10, the metal catalyst sheet 21 is reduced, the graphene 1 is synthesized, and the cooling is performed. All gates 17 are closed to completely separate each section. It is done in the state.

To this end, the metal catalyst sheet 21 supplied in the seventh embodiment is supplied in a state of being cut to a predetermined length. That is, the metal catalyst sheet supply unit 32 is loaded with the metal catalyst sheet 21 in a state cut into a predetermined length, and sequentially into the reactor 10 through the reactor inlet 11 according to the driving of the roller 30. The metal catalyst sheet 21 is supplied.

At this time, when the metal catalyst sheet 21 is located within the section separated by the gate 17, the metal catalyst sheet 17 must be kept for a predetermined time since reduction, graphene synthesis or cooling should be performed for a predetermined time. It must be stopped at a very long time or conveyed at a very slow speed, and quickly transferred when the gate 17 is opened and the metal catalyst sheet 17 is to be transferred to the next section. The operation of the gate driver 18 to open and close the gate 17 and the speed control of the roller 30 are appropriately performed through separate control means (not shown).

When the graphene 1 is synthesized via each section in which the metal catalyst sheet 21 is isolated by the gates 17, the metal catalyst sheet 21 in the state where the graphene 1 is synthesized is a metal catalyst. The sheet recovery unit 67 recovers the sheets.

The metal catalyst sheet recovery unit 67 may recover the metal catalyst sheet 21 which has exited the reactor outlet 12 in a sequential manner, but only the graphene 1 may be transferred to the PET or the like according to the method. It can also be recovered by transferring.

As described in detail above, according to the graphene synthesis apparatus and method according to the present invention, by synthesis and recovery of graphene using a gas phase synthesis method and a method of continuously passing the metal catalyst sheet through the reactor, the conventional synthesis method It is possible to obtain a large area of graphene that is continuously connected, which could not be achieved.

Preferred embodiments of the present invention described above are disclosed for the purpose of illustration, and those skilled in the art will be able to make various modifications, changes and additions within the spirit and scope of the present invention. And additions should be considered to be within the scope of the claims of the present invention.

1: graphene
10: reactor
11: reactor inlet 12: reactor outlet
13: first recessed portion 14: second recessed portion
15: first gas discharge pipe 16: second gas discharge pipe
20,21: Metal Catalyst Sheet
30: roller 31: roller drive unit
32: metal catalyst sheet supply unit
41,42 ': 1st mounting unit 42,41': 2nd mounting unit
51: mesh belt 52: mesh belt transfer unit
61: first transfer member mounting unit 62: first transfer member drive unit
63: second transfer member mounting unit 64: second transfer member drive unit
65: transcription driving unit
66: transcript
67: metal catalyst sheet recovery unit
70: reduction unit
71: first heating means
72: first gas nozzle 73: second gas nozzle
80: graphene synthesis unit
81: second heating means 82: third heating means
83: first showerhead 84: second showerhead
90 cooling unit
91: cooling means
92: third gas nozzle
100: gas supply unit
110: carbon source gas tank
120: inert gas tank
130: hydrogen gas tank
110: gas sealing means

Claims

A reactor having at least one inlet and outlet open to outside air;
Graphene synthesis unit for synthesizing graphene via a metal catalyst sheet introduced through the inlet of the reactor;
A metal catalyst sheet transfer unit for transferring the metal catalyst sheet such that the metal catalyst sheet flows through the inlet and passes through the graphene synthesis unit;
A gas supply unit supplying an inert gas or a carbon source gas for synthesizing the graphene into the reactor; And
A gas sealing means for supplying the inert gas again at the inlet and the outlet side of the reactor to maintain the gas pressure in the reactor to be above a predetermined pressure to block the outside air from entering the reactor; and Continuous mass synthesis apparatus of large area graphene connected continuously.

The method of claim 1,
And a graphene recovery unit for recovering the graphene synthesized on the metal catalyst sheet passing through the reactor through a transfer body.
The metal catalyst sheet transfer unit,
Continuous mass of large-area continuously connected graphene, characterized in that for transporting the metal catalyst sheet at least one of the upper surface or the lower surface of the continuously connected metal catalyst sheet exposed in the reactor. Synthetic device.

The method of claim 2,
When the graphene synthesized in the metal catalyst sheet through the reactor is recovered in the graphene recovery unit, the continuous mass of large area graphene continuously connected to the metal catalyst sheet is introduced into the reactor. Synthetic device.

The method of claim 2,
The metal catalyst sheet transfer unit,
At least one mounting unit rotatably mounted to the continuously connected metal catalyst sheet and transferring the metal catalyst sheet with rotational power; And
And at least one roller supporting the metal catalyst sheet at predetermined points of both ends of the continuously connected metal catalyst sheets.

The method of claim 2,
The metal catalyst sheet transfer unit,
At least one mounting unit to which the metal catalyst sheets which are continuously connected are rotatably mounted;
A mesh-shaped mesh belt supporting the metal catalyst sheet at a lower portion of the metal catalyst sheet which is continuously connected to the metal catalyst sheet; And
The mesh belt is rotatably mounted, and a mesh belt transfer unit configured to transfer the metal catalyst sheet on the mesh belt by transferring the mesh belt with rotational power. Continuous mass synthesis device of area graphene.

The method of claim 2,
The graphene recovery unit,
A transfer unit mounting unit to which the transfer member to which the graphene is to be transferred is mounted in a roll form;
Located at the outlet of the reactor outside the transfer to transfer the graphene synthesized on the metal catalyst sheet to the transfer body by passing the metal catalyst sheet and the transfer body mounted on the transfer unit mounting unit facing each other Drive unit; And
And a transfer body driving unit for winding the transfer body in which the graphene is passed through the transfer driving unit in the form of a roll.

The method of claim 1,
The metal catalyst sheet transfer unit,
A first mounting unit to which the metal catalyst sheet is mounted in a roll shape;
When the metal catalyst sheet mounted on the first mounting unit passes through the inside of the reactor and the graphene is synthesized, the second mounting unit for winding the metal catalyst sheet synthesized with the graphene in the form of a roll; And
And at least one roller supporting the metal catalyst sheet at predetermined points of both ends of the metal catalyst sheet.

The method of claim 1,
The graphene synthesis unit,
A reaction zone formed inside the reactor and blocked from the outside air by an inert gas filled in the reactor;
Carbon injecting the carbon source gas supplied from the gas supply unit to the reaction zone so that the metal catalyst sheet transferred into the reaction zone by the metal catalyst sheet transfer unit reacts with the carbon source gas to synthesize the graphene. Source injection mechanisms; And
And a heating means for heating the reaction zone. Continuous continuous mass synthesis of large-area graphene, characterized in that it comprises a.

The method of claim 1,
The continuous mass synthesis apparatus of large area graphene continuously connected, characterized in that the inert gas comprises hydrogen gas.

The method of claim 1,
And a cooling unit for cooling a region of the reactor adjacent to the outlet so that the graphene is cooled.

The method of claim 1,
A plurality of gates capable of opening and closing to isolate a space from an inlet to an outlet of the reactor in a predetermined section; And
And a gate driver for opening and closing the gate. The continuous mass synthesizing apparatus of the large-area graphene connected continuously.