Apparatus and method for producing fullerene

Abstract

To provide an apparatus and a method for manufacturing fullerene capable of improving a yield of fullerene.SOLUTION: An apparatus for manufacturing fullerene is configured to generate fullerene by incomplete combustion of a raw material gas containing hydrocarbon. The apparatus for manufacturing fullerene includes: a reaction furnace 2; a burner 9A having a first injection part 23c configured to inject a raw material gas containing hydrocarbon to an inside of the reaction furnace; and an inert gas introduction part 10A having a second injection part 25a configured to inject an inert gas to the inside of the reaction furnace and a heating part 26.SELECTED DRAWING: Figure 2

Description

[Technical field]

[0001] The present invention relates to an apparatus and method for producing fullerenes. [Background technology]

[0002] As a method for producing fullerenes, a combustion method is known in which fullerenes are produced by incompletely combusting a raw material gas containing hydrocarbons (hereinafter also referred to as "raw material gas") in a reactor (see, for example, Patent Documents 1 and 2). This combustion method makes it possible to mass-produce fullerenes contained in soot-like matter produced by incomplete combustion of the raw material gas at low cost. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2003-160316 A [Patent Document 1] JP 2003-171106 A Summary of the Invention [Problem to be solved by the invention]

[0004] However, in the above-mentioned conventional combustion method, the yield of fullerenes contained in the soot-like matter is not high, and therefore it is desired to increase the yield of fullerenes and further reduce the production cost of fullerenes.

[0005] The present invention has been proposed in view of the above-mentioned conventional circumstances, and has an object to provide an apparatus and method for producing fullerenes that make it possible to improve the yield of fullerenes. [Means for solving the problem]

[0006] The present invention provides the following means. (1) A fullerene production apparatus for producing fullerenes by incomplete combustion of a raw material gas containing a hydrocarbon, comprising a reactor, a burner having a first injection section for injecting the raw material gas containing a hydrocarbon into the reactor, and an inert gas introduction section having a second injection section for injecting an inert gas into the reactor and a heating section. (2) The fullerene producing apparatus according to the preceding item (1), wherein either the first injection part or the second injection part is disposed so as to surround the other one of them. (3) The fullerene production apparatus according to the preceding paragraph (1), wherein at least a portion of the first injection portion and at least a portion of the second injection portion are arranged alternately in a concentric circle. (4) The fullerene production apparatus according to the preceding paragraph (1), characterized in that the first injection section injects the raw material gas from one end side of the reactor toward the other end side, and the second injection section injects the inert gas from the periphery between the one end side and the other end side of the reactor. (5) The fullerene producing apparatus according to any one of (1) to (4) above, further comprising a pressure reducing mechanism for reducing the pressure inside the reactor by evacuating the inside of the reactor. (6) A method for producing fullerenes, comprising: a heating step of heating an inert gas; a production step of producing fullerenes in a reactor by incomplete combustion of a raw material gas containing a hydrocarbon; and an injection step of injecting the heated inert gas into the reactor simultaneously with the production step. (7) The method for producing fullerenes according to (6) above, wherein in the heating step, the temperature of the heated inert gas is 1000 to 2500°C. (8) The method for producing fullerenes according to (6) or (7) above, characterized in that the inside of the reaction furnace is evacuated while the inside of the reaction furnace is kept under reduced pressure. (9) The method for producing fullerenes according to (8) above, wherein the pressure inside the reaction furnace is set to 1 to 30 kPa. Effect of the Invention

[0007] As described above, according to the present invention, it is possible to improve the yield of fullerenes. [Brief description of the drawings]

[0008] [Figure 1] 1 is a configuration diagram showing an example of a fullerene production apparatus according to an embodiment of the present invention. [Diagram 2] 1 is a cross-sectional view showing a configuration of a reactor equipped with a burner 9A and an inert gas introduction section 10A according to a first embodiment of the present invention. [Diagram 3] 3 is a plan view illustrating the configuration of the tip end surface of the burner 9A and the injection part of the inert gas introduction part 10A shown in FIG. 2. FIG. [Figure 4] FIG. 11 is a cross-sectional view showing the configuration of a reactor equipped with a burner 9B and an inert gas introduction section 10B according to a second embodiment of the present invention. [Diagram 5] 5 is a plan view showing the configuration of a tip surface of a burner 9B and an injection portion of an inert gas introducing portion 10B shown in FIG. [Figure 6] FIG. 11 is a cross-sectional view showing the configuration of a reactor including a burner 9C and an inert gas inlet section 10C according to a third embodiment of the present invention. [Figure 7] 7 is a plan view illustrating the configuration of the tip end surface of the injection part of the burner 9C and the inert gas introduction part 10C shown in FIG. 6. FIG. [Figure 8] FIG. 11 is a cross-sectional view showing the configuration of a reactor equipped with a burner 9D and an inert gas inlet section 10D according to a fourth embodiment of the present invention. [Figure 9] 9 is a vertical cross-sectional view illustrating an example of the shape and arrangement of a second injection part 25d and a second injection port 22a included in the inert gas introduction part 10D shown in FIG. [Figure 10] 9 is a cross-sectional view illustrating an example of the arrangement of second injection ports 22a of a second injection part 25d included in the inert gas introduction part 10D shown in FIG. 8. FIG. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0009] Hereinafter, a fullerene producing apparatus to which the present invention is applied will be described in detail with reference to the drawings. In addition, the drawings used in the following explanation may show characteristic parts diagrammatically for convenience in order to make the features easier to understand, and the dimensional ratios of each component may not necessarily be the same as the actual ones.

[0010] (Fullerene manufacturing equipment) First, as one embodiment of the present invention, a fullerene production apparatus 1 shown in FIG. 1 will be described. FIG. 1 is a configuration diagram showing an example of a fullerene production apparatus 1.

[0011] As shown in FIG. 1, the fullerene production apparatus 1 of this embodiment includes a reactor 2 that produces a soot-like material containing fullerenes by incomplete combustion of a raw material gas containing hydrocarbons, a recovery mechanism 3 that recovers the soot-like material produced in the reactor 2, a cooling mechanism 4 that cools the gas that has passed through the recovery mechanism 3, and a pressure reduction mechanism 5 that creates a reduced pressure state inside the reactor 2 while sucking in the gas cooled by the cooling mechanism 4.

[0012] In addition, this fullerene production apparatus 1 has a first pipe 6 connecting the reactor 2 and the recovery mechanism 3, a second pipe 7 connecting the recovery mechanism 3 and the cooling mechanism 4, and a third pipe 8 connecting the cooling mechanism 4 and the pressure reduction mechanism 5.

[0013] The reactor 2 has a cylindrical peripheral wall portion 2a, an upper wall portion 2b closing the upper end (one end) side of the peripheral wall portion 2a, and a lower wall portion 2c closing the lower end (the other end) side of the peripheral wall portion 2a, and is arranged in an upright position in the vertical direction.

[0014] The reactor 2 may be made of heat-resistant materials such as zirconia (ZrO2), tungsten (W), tantalum (Ta), platinum (Pt), titanium (Ti), titanium nitride (TiN), alumina (Al2O3), silicon carbide (SiC), etc. At least a portion of the outside and inside of the reactor 2 may be lined with a heat insulating material such as alumina firebricks or alumina castable firebricks.

[0015] Regarding the arrangement of the reactor 2, it is preferable to arrange it in the vertical direction as described above, since the influence of the soot-like matter retention is small. When the arrangement direction of the reactor 2 is vertical, it is preferable to supply the raw material gas from above. On the other hand, the reactor 2 can also be arranged, for example, in the horizontal direction or inclined at an angle.

[0016] The first pipe 6 is connected to an exhaust port 30d (hereinafter also referred to as "exhaust gas exhaust port 30d") for discharging exhaust gas, which is provided in the bottom wall 2c of the reactor 2. Meanwhile, a burner 9 and an inert gas introduction section 10 are provided on the upper wall 2b side of the reactor 2. In the reactor 2, the raw material gas and the oxygen-containing gas injected from the burner 9 are incompletely combusted to generate a soot-like material containing fullerenes.

[0017] The inside of the reactor 2 is heated by the heated inert gas injected into the reactor 2 from the inert gas introduction part 10. Exhaust gas containing soot generated by incomplete combustion of the raw material gas, carbon monoxide, carbon dioxide, water vapor, etc., and the inert gas pass through the first pipe 6 and reach the recovery mechanism 3.

[0018] The recovery mechanism 3 has a collector 12 housing a filter 11, a tank 14 connected to the upper end (one end) of the collector 12 via an solenoid valve 13, and a discharge valve 15 provided on the lower end (other end) of the collector 12.

[0019] The first pipe 6 is connected to the side of the upper portion of the collector 12. The second pipe 7 is connected to the upper portion of the collector 12. For example, a sintered metal filter is used as the filter 11. The solenoid valve 13 is branched off and connected to the second pipe 7. The tank 14 stores a high-pressure inert gas such as nitrogen gas (N2) or argon gas (Ar).

[0020] In the recovery mechanism 3, the soot-like matter contained in the exhaust gas supplied from the first pipe 6 is collected by the filter 11, and then the solenoid valve 13 is periodically opened to inject an inert gas from the tank 14 toward the collector 12. This causes the soot-like matter adhering to the filter 11 to fall off. Thereafter, the discharge valve 15 is opened to enable the soot-like matter accumulated in the collector 12 to be recovered.

[0021] The cooling mechanism 4 has a structure identical to or similar to that of a normal heat exchanger, and one end (upper end) thereof is connected to the second piping 7 and the other end (lower end) thereof is connected to the third piping 8.

[0022] The cooling mechanism 4 cools the gas that has passed through the recovery mechanism 3. The cooling mechanism 4 also liquefies unreacted hydrocarbons and water vapor in the gas, and is capable of discharging the liquefied gas from a drain 16 provided on the lower side.

[0023] In addition to the cooling mechanism 4, the first piping 6 may be configured to be cooled since the exhaust gas and inert gas passing through the first piping 6 are at high temperatures.

[0024] The decompression mechanism 5 is composed of a vacuum pump, and sucks the gas cooled by the cooling mechanism 4 through the third pipe 8. This makes it possible to discharge the soot-like matter generated in the reaction furnace 2 to the recovery mechanism 3 side through the first pipe 6 while generating a negative pressure between the reaction furnace 2 and the gas.

[0025] Examples of the hydrocarbons contained in the raw material gas include aromatic hydrocarbons having 6 to 15 carbon atoms, such as toluene, benzene, xylene, naphthalene, methylnaphthalene, anthracene, and phenanthrene; coal-based hydrocarbons, such as creosote oil and carboxylic acid oil; acetylene-based unsaturated hydrocarbons; ethylene-based hydrocarbons; and aliphatic saturated hydrocarbons, such as pentane and hexane. Two or more of these hydrocarbons may be mixed and used. Among the above-mentioned hydrocarbons, the raw material gas preferably contains aromatic hydrocarbons. The raw material gas may be diluted with an inert gas, such as nitrogen or argon, as necessary.

[0026] The oxygen-containing gas is a gas that contains oxygen, and examples of the gas include oxygen and air. The oxygen-containing gas may be supplied to the reaction furnace 2 separately from the raw material gas, or may be mixed with the raw material gas in advance and then supplied to the reaction furnace 2.

[0027] On the other hand, the inert gas is not particularly limited as long as it does not react with the raw material gas, oxygen gas, and exhaust gas generated by incomplete combustion of the raw material gas. For example, nitrogen gas, argon gas, helium gas, carbon dioxide gas, etc. may be mentioned. Two or more of these inert gases may be mixed and used.

[0028] The fullerenes produced are, for example, C 60 Fullerene (C 60 ), C 70 Fullerene (C 70 ), C 76 , C 78 , C 84 , C 90 , C 96 and the like.

[0029] (Production method of fullerene) Next, a method for producing fullerenes using the above-mentioned fullerene production apparatus 1 will be described. The method for producing fullerenes in this embodiment includes a heating step of heating an inert gas, a production step of producing fullerenes in a reactor 2 by incomplete combustion of a raw material gas containing a hydrocarbon, and an injection step of injecting the heated inert gas into the reactor 2 simultaneously with the production step, and the inside of the reactor 2 is heated by the heated inert gas.

[0030] In the fullerene production method of this embodiment, the temperature of the combustion flame generated by incompletely combusting the raw material gas is 500° C. to 1500° C. Meanwhile, the temperature of the inert gas heated in the heating step is preferably 1000° C. to 2500° C., more preferably 1100° C. to 2200° C. This makes it possible to keep the temperature (atmosphere) in the reaction furnace 2 high.

[0031] Then, the above-mentioned raw material gas is incompletely combusted in the high-temperature reactor 2 to generate soot-like matter. This makes it possible to improve the yield of fullerenes contained in the generated soot-like matter.

[0032] The pressure inside the reactor 2 is preferably 1 to 30 kPa, and more preferably 1 to 10 kPa. If the pressure inside the reactor 2 is within this range, it is possible to prevent overload of the pressure reducing mechanism 5 and backfire of the flame.

[0033] (First embodiment) Next, a fullerene production apparatus 1 according to a first embodiment of the present invention will be described. The fullerene production apparatus 1 according to the first embodiment of the present invention includes a burner 9 (hereinafter referred to as "burner 9A") and an inert gas introduction section 10 (hereinafter referred to as "inert gas introduction section 10A") shown in FIG. 2.

[0034] 2 is a cross-sectional view showing the configuration of the reactor 2 equipped with a burner 9A and an inert gas introduction part 10A. The reactor 2 is arranged in the vertical direction. Figs. 3(A) and (B) are plan views showing examples of the configuration of the tip surfaces of a first injection part 23c and a second injection part 25a described later.

[0035] The burner 9A has a cylindrical burner holder 23 with a top that is attached in a state of penetrating the upper wall portion 2b of the reactor 2, and a premixing chamber 23a, a pressure accumulation chamber 23b, and a first injection portion 23c that are provided in this order from the top inside the burner holder 23. In addition, a pipe 24a for introducing a raw material gas and a pipe 24b for introducing an oxygen-containing gas are connected to the top of the burner holder 23.

[0036] The premixing chamber 23a mixes the raw material gas introduced from the pipe 24a and the oxygen-containing gas introduced from the pipe 24b at a predetermined ratio. The pressure accumulation chamber 23b accumulates the raw material gas and the oxygen-containing gas mixed in the premixing chamber 23a at a predetermined pressure. The first injection part 23c has a plurality of first injection ports 21a at its tip surface, and injects the raw material gas and the oxygen-containing gas accumulated in the pressure accumulation chamber 23b downward (toward the exhaust gas discharge port 30d) from the first injection ports 21a. The first injection part 23c may be composed of a porous ceramic sintered body or a sintered body of metal powder.

[0037] In the present embodiment, the premixing chamber 23a, the pressure accumulation chamber 23b, and the first injection portion 23c are provided inside the burner holder 23, but the premixing chamber 23a may be omitted. Furthermore, the premixing chamber 23a and the pressure accumulation chamber 23b may be provided outside the burner holder 23 as necessary.

[0038] The inert gas introduction section 10A has a second injection section 25a, a heating section 26 arranged outside the reaction furnace 2, and a connection pipe 27 connecting the second injection section 25a and the heating section 26.

[0039] The second injection part 25a is, for example, a tube having a certain thickness, and is provided with a second injection port 22a for injecting an inert gas at its tip end surface. A passage is provided inside the second injection part 25a to connect the second injection port 22a and the connection pipe 27. The second injection part 25a is disposed so as to surround the periphery of the first injection part 23c.

[0040] The shape and number of the second injection ports 22a are not particularly limited, but as an example, they are circular as shown in Fig. 3(A) . In Fig. 3(A), the tip surface of the second injection part 25a is in a link shape, and the multiple second injection ports 22a are evenly arranged on the tip surface of the second injection part 25a.

[0041] Furthermore, as shown in FIG. 3(B), a ring-shaped second injection port 22a may be disposed on the tip surface of a ring-shaped second injection part 25a.

[0042] In addition, the tip surface of the first ejection portion 23c and the tip surface of the second ejection portion 25a may have the same height position in the vertical direction or may have different height positions, but it is preferable that they have the same height positions.

[0043] A pipe 28 for introducing an inert gas is connected to the heating unit 26. The heating unit 26 heats the inert gas introduced from the pipe 28. The heating unit 26 is not particularly limited as long as it is a heating device that can raise the temperature to a set heating temperature. For example, the heating unit 26 may have a tube made of graphite, tungsten, molybdenum, or the like, a heat insulating material made of an alumina-based amorphous refractory material arranged on the outside of the tube, and an induction heating coil. In addition, a high-temperature resistant thermocouple is provided to measure the temperature inside the heating unit 26. The temperature of the heated inert gas is the set heating temperature of the heating unit 26.

[0044] The connection pipe 27 supplies the inert gas heated by the heating unit 26 to the second injection unit 25a while penetrating the upper part of the peripheral wall 2a of the reactor 2. The connection pipe 27 may also supply the heated inert gas to the second injection unit 25a by penetrating the upper wall 2b of the reactor 2. The second injection unit 25a injects the heated inert gas supplied via the connection pipe 27 from the second injection port 22a downward (in the direction toward the exhaust gas discharge port 30d).

[0045] An insulating member 30 is arranged in the reactor 2, and the insulating member 30 has a cylindrical peripheral wall 30a arranged along the inner peripheral wall portion 2a of the reactor 2, a bottom wall 30b arranged along the inner bottom wall portion 2c of the reactor 2, and a top wall 30c that closes the upper part of the peripheral wall 30a.

[0046] The burner holder 23 and the second injection part 25a penetrate the top wall 30c, and the first injection port 21a and the second injection port 22a are exposed to the inside of the heat insulating member 30. The bottom wall 30b is provided with an exhaust gas discharge port 30d that communicates with the first piping 6. The material of the heat insulating member 30 may be, for example, alumina firebrick or alumina amorphous firebrick.

[0047] Further, an ignition mechanism 31 for igniting the raw material gas is provided near the position where the first pipe 6 of the reactor 2 is connected.

[0048] The burner 9A and inert gas introduction section 10A of this embodiment having the above-mentioned configuration inject raw material gas and oxygen-containing gas from the above-mentioned first injection port 21a, while injecting the raw material gas incompletely to generate a soot-like material containing fullerenes in the reaction furnace 2, and at the same time injecting heated inert gas from the above-mentioned second injection port 22a into the reaction furnace 2 to heat the inside of the reaction furnace 2.

[0049] As a result, in the fullerene production apparatus 1 equipped with the burner 9A and inert gas introduction section 10A of this embodiment, the temperature inside the reaction furnace 2 can be maintained at a high temperature, making it possible to improve the yield of fullerenes contained in the generated soot-like material.

[0050] Second embodiment Next, a fullerene production apparatus 1 according to a second embodiment of the present invention will be described. The fullerene production apparatus 1 according to the second embodiment of the present invention is equipped with a burner 9 (hereinafter referred to as "burner 9B") and an inert gas introduction section 10 (hereinafter referred to as "inert gas introduction section 10B") shown in Figures 4 and 5.

[0051] FIG. 4 is a cross-sectional view showing the configuration of the reactor 2 equipped with the burner 9B and the inert gas introduction part 10B. The reactor 2 is arranged in the vertical direction. FIG. 5 is a plan view showing the configuration of the tip surface of the first injection part 23c of the burner 9B and the second injection part 25b (described later) of the inert gas introduction part 10B. In the following description, the description of the same parts as the burner 9A and the inert gas introduction part 10A will be omitted and the same reference numerals will be used in the drawings.

[0052] In this embodiment, as shown in FIG. 4, the inert gas introduction section 10B has a tubular second injection section 25b. The second injection section 25b is installed in the center inside the burner holder 23 and penetrates the premixing chamber 23a, the pressure accumulation chamber 23b, and the first injection section 23c in the vertical direction. As a result, the second injection section 25b is surrounded by the first injection section 23c. Also, as shown in FIG. 5, the second injection section 25b has a second injection port 22a on the tip surface thereof and is surrounded by the first injection port 21a of the first injection section 23c. The second injection section 25b is directly connected to the heating section 26.

[0053] The burner 9B has a similar structure to the burner 9A, except that the premixing chamber 23a, the pressure accumulator chamber 23b, and the first injection portion 23c are vertically penetrated by the second injection portion 25b.

[0054] Furthermore, the tip surface of the first ejection portion 23c and the tip surface of the second ejection portion 25b may have the same height position in the vertical direction or may have different height positions, but it is preferable that they have the same height positions.

[0055] The burner 9B and inert gas introduction section 10B of this embodiment having the above-mentioned configuration inject raw material gas and oxygen-containing gas from the above-mentioned first injection port 21a, while injecting the raw material gas incompletely to generate a soot-like material containing fullerenes in the reaction furnace 2, and at the same time injecting heated inert gas from the above-mentioned second injection port 22a into the reaction furnace 2 to heat the inside of the reaction furnace 2.

[0056] As a result, in the fullerene production apparatus 1 equipped with the burner 9B and inert gas introduction section 10B of this embodiment, the temperature inside the reaction furnace 2 can be kept high, making it possible to improve the yield of fullerenes contained in the generated soot-like material.

[0057] (Third embodiment) Next, a fullerene production apparatus 1 according to a third embodiment of the present invention will be described. The fullerene production apparatus 1 according to the third embodiment of the present invention is equipped with a burner 9 (hereinafter referred to as "burner 9C") and an inert gas introduction section 10 (hereinafter referred to as "inert gas introduction section 10C") shown in Figures 6 and 7.

[0058] FIG. 6 is a cross-sectional view showing the configuration of the reactor 2 equipped with the burner 9C and the inert gas introduction part 10C. The reactor 2 is arranged in the vertical direction. FIGS. 7(A) and 7(B) are plan views showing the configuration of the tip surface of the first injection part 23c of the burner 9C and the second injection part 25c (described later) of the inert gas introduction part 10B. In the following description, the description of the same parts as the burner 9A and the inert gas introduction part 10A will be omitted and the same reference numerals will be used in the drawings.

[0059] In this embodiment, the inert gas introduction section 10C has a second injection section 25c provided in the burner holder 23, as shown in FIG. 6. The second injection section 25c has a plurality of nozzle sections 34 branched off from the connection pipe 27. The nozzle sections 34 are arranged in a state in which they penetrate the pressure accumulator chamber 23b and the first injection section 23c in the vertical direction. As a result, the second injection section 25c is surrounded by the first injection section 23c. In addition, the connection pipe 27 connects between the second injection section 25c and the heating section 26 while penetrating the upper center part of the burner holder 23.

[0060] Specifically, the nozzle portion 34 may be, for example, tubular or cylindrical with a certain thickness. The second injection port 22a is disposed on the tip surface of the nozzle portion 34. When the nozzle portion 34 is cylindrical, a passage connecting the connection pipe 27 and the second injection port 22a is provided inside the nozzle portion 34. The second injection portion 25c may include only one of the tubular nozzle portion 34 (hereinafter referred to as "nozzle portion 34a") and the cylindrical nozzle portion 34 (hereinafter referred to as "nozzle portion 34b"), or may include both.

[0061] For example, the second injection part 25c of the inert gas introduction part 10C shown in Fig. 7(A) has a plurality of nozzle parts 34a. At the tip surface of the first injection part 23c and the second injection part 25c, each nozzle part 34a has a second injection port 22a that opens in a circular shape. As a result, the second injection part 25c (second injection port 22a) is surrounded by the first injection part 23c (first injection port 21a).

[0062] 7B, the second injection part 25c of the inert gas introduction part 10C has one nozzle part 34a arranged in the center, and a plurality of nozzle parts 34b arranged around the nozzle part 34a. At the tip surface of the first injection part 23c and the second injection part 25c, the nozzle part 34a has the second injection port 22a opening in a circular shape, and the nozzle part 34b has the second injection port 22a opening in a ring shape.

[0063] Nozzle portion 34a (second ejection port 22a) is surrounded by first ejection portion 23c (first ejection port 21a), and nozzle portion 34b and parts of first ejection portion 23c are arranged alternately in a concentric circle.

[0064] The burner 9C has a similar structure to the burner 9A, except that the premixing chamber 23a, the pressure accumulator chamber 23b, and the first injection portion 23c are vertically penetrated by the connection pipe 27 and the nozzle portion .

[0065] Furthermore, the tip surface of the first ejection portion 23c and the tip surface of the second ejection portion 25c (nozzle portion 34a, nozzle portion 34b) may have the same height position in the vertical direction or may have different height positions, but it is preferable that they have the same height positions.

[0066] In the burner 9C and inert gas introduction section 10C of this embodiment having the above-mentioned configuration, raw material gas and oxygen-containing gas are injected from the above-mentioned first injection port 21a, and the raw material gas is incompletely combusted to generate a soot-like material containing fullerenes in the reaction furnace 2, and at the same time, heated inert gas is injected from the above-mentioned second injection port 22a into the reaction furnace 2 to heat the inside of the reaction furnace 2.

[0067] As a result, in the fullerene production apparatus 1 equipped with the burner 9C and inert gas introduction section 10C of this embodiment, the temperature inside the reactor 2 can be maintained at a high temperature, making it possible to improve the yield of fullerenes contained in the generated soot-like material.

[0068] (Fourth embodiment) Next, a fullerene production apparatus 1 according to a fourth embodiment of the present invention will be described. The fullerene production apparatus 1 according to the fourth embodiment of the present invention is equipped with a burner 9 (hereinafter referred to as "burner 9D") and an inert gas introduction section 10 (hereinafter referred to as "inert gas introduction section 10D") shown in Figures 8 and 9.

[0069] FIG. 8 is a cross-sectional view showing the configuration of the reactor 2 equipped with the burner 9D and the inert gas introduction part 10D. The reactor 2 is arranged in the vertical direction. FIG. 9 is a longitudinal cross-sectional view illustrating the shape and arrangement of the second injection part 25d and the second injection port 22a equipped in the inert gas introduction part 10D. FIG. 10 is a transverse cross-sectional view illustrating the arrangement of the second injection port 22a of the second injection part 25d equipped in the inert gas introduction part 10D. In the following description, the description of the same parts as the burner 9A and the inert gas introduction part 10A will be omitted and the same reference numerals will be given in the drawings.

[0070] The burner 9D of this embodiment has the same configuration as the burner 9A.

[0071] The inert gas introduction part 10D has a second injection part 25d as shown in Fig. 8. The second injection part 25d has a cylindrical shape extending downward from a position surrounding the periphery of the burner holder 23.

[0072] A plurality of second injection ports 22a are arranged in a row on the inner peripheral surface of the second injection part 25d. A passage connecting the connection pipe 27 and the second injection port 22a is provided inside the second injection part 25d. This allows the second injection part 25d to inject heated inert gas into the reactor 2 from the second injection port 22a.

[0073] The second injection ports 22a in the inner peripheral surface of the second injection part 25d may have shapes and arrangements as shown in Fig. 9(A), (B), and (C) in the axial direction of the second injection part 25d. For example, the multiple second injection ports 22a shown in Fig. 9(A) are opened in the axial direction of the second injection part 25d in the form of slits, and are arranged side by side in the circumferential direction of the second injection part 25d.

[0074] On the other hand, the multiple second injection ports 22a shown in FIG. 9(B) are each opened in a circular shape, and are arranged side by side in the circumferential and axial directions of the second injection part 25d.

[0075] On the other hand, the multiple second injection ports 22a shown in FIG. 9(C) are each opened in the form of a slit in the circumferential direction of the second injection part 25d, and are arranged side by side in the axial direction of the second injection part 25d.

[0076] In addition, when the second injection part 25d has a plurality of second injection ports 22a in the circumferential direction as shown in Fig. 9(A) and (B), the plurality of second injection ports 22a may be formed as shown in Fig. 10. For example, the plurality of second injection ports 22a shown in Fig. 10(A) are formed by protrusions 33 that open obliquely in the same direction on the inner circumferential surface of the second injection part 25d. This makes it possible to form a vortex flow of the inert gas injected from each of the second injection ports 22a.

[0077] 10(B) are open toward the center of the reactor 2 in the circumferential direction of the second injection part 25d. This allows the inert gas injected from each of the second injection ports 22a to be injected toward the center of the reactor 2.

[0078] In the burner 9D and inert gas introduction section 10D of this embodiment having the above-mentioned configuration, raw material gas is injected from the above-mentioned first injection port 21a, and this raw material gas is incompletely combusted to generate a soot-like material containing fullerenes in the reaction furnace 2, and at the same time, heated inert gas is injected from the above-mentioned second injection port 22a into the reaction furnace 2 to heat the inside of the reaction furnace 2.

[0079] As a result, in the fullerene production apparatus 1 equipped with the burner 9D and inert gas introduction section 10D of this embodiment, the temperature inside the reaction furnace 2 can be maintained at a high temperature, making it possible to improve the yield of fullerenes contained in the generated soot-like material.

[0080] The present invention is not necessarily limited to the above-described embodiment, and various modifications can be made without departing from the spirit of the present invention. EXAMPLES

[0081] The effects of the present invention will be more clearly understood by the following examples. Note that the present invention is not limited to the following examples, and can be modified as appropriate without departing from the spirit and scope of the present invention.

[0082] [Calculation of fullerene yield] In Examples 1 to 7 and Comparative Example 1, C 60 and C 70 The total yield of fullerene was calculated as the yield of fullerene. In addition, in accordance with "JIS Z 8981", the C contained in the collected soot-like matter was 60 and C 70 The content was measured as follows.

[0083] Specifically, 15 g of 1,2,3,5-tetramethylbenzene (TMB) was added to 0.05 g of the collected soot-like material, and then ultrasonic treatment was performed for 15 minutes to obtain a suspension. The obtained suspension was filtered through a membrane filter with a pore size of 0.5 μm, and the filtrate (sample liquid) was analyzed by high performance liquid chromatography (HPLC) to obtain the following: 60 and C 70 The amount of C contained in the soot was determined. 60 and C 70 The content [mass %] was calculated.

[0084] Here, the C contained in the soot 60 and C 70 When calculating the content of C, several known concentrations of C 60 and C 70 A calibration curve was prepared using a TMB solution.

[0085] The HPLC measurement conditions are as follows. Equipment: Infinity1260 (Agilent) Sample injection volume: 5μL Eluent: toluene (47% by volume) / methanol (53% by volume) mixed solvent Eluent flow rate: 1 ml / min Column: YMC-Pack ODS-AM 100*4.6mmID S-3μm,12nm Measurement temperature: 40℃ Detector: UV 325nm (JIS)

[0086] Next, the fullerene content (C 60 and C70 From the total content of the soot, the fullerene yield [mass %] was calculated by the formula {(amount of soot recovered [g]) / (amount of raw material gas consumed [g])}×(fullerene content [mass %]).

[0087] Example 1 Fullerenes were produced using a fullerene production apparatus 1 having a reactor 2 shown in Fig. 2. The tip of the second ejection part 25a has the structure shown in Fig. 3(A).

[0088] Here, the reactor 2 is an alumina cylinder arranged vertically, with a height of 1000 mm and an inner diameter of 200 mm. A burner 9A is provided so as to penetrate the wall 2b of the reactor 2. The first injection part 23c is made of a disk-shaped porous ceramic sintered body with a diameter of 100 mm, and this ceramic sintered body has holes (first injection ports 21a) with a diameter of about 0.5 mm to 1.0 mm, which are formed over a distance of 1 cm. 2 There are 60 to 80 of them formed around each area.

[0089] The second injection part 25a of the inert gas introduction part 10A is made of zirconia and is a cylinder with an inner diameter of 160 mm. Forty second injection ports 22a, each having a diameter of 10 mm, are uniformly arranged on the tip surface of the second injection part 25a.

[0090] The heating section 26 of the inert gas introduction section 10A is an induction heating device having a graphite tube. The inert gas is heated by passing through the graphite tube. The heating temperature of the heating section 26 was set to 1700°C. In the vertical direction, the tip surface of the second injection section 25a has the same height position as the tip surface of the first injection section 23c.

[0091] Toluene was used as the raw material gas, and pure oxygen gas (purity 99.9% by volume) was used as the oxygen-containing gas. Here, the toluene was once heated in a vaporizer installed in the pipe 24a to become gaseous, and then supplied to the burner 9A. The oxygen-containing gas was supplied to the burner 9A via the pipe 24b. The flow rate of the toluene gas was set to 20 g / min, and the flow rate of the pure oxygen was set to 13 NL / min.

[0092] Nitrogen gas (purity 99.9% by volume) was used as the inert gas, and the flow rate of the nitrogen gas was set to 15 NL / min.

[0093] When producing fullerenes, the pressure inside the reaction furnace 2 was set to 5.33 kPa.

[0094] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the generated soot-like material was collected from the collection mechanism 3. The fullerene content was measured by the method described in [Calculation of fullerene yield], and the fullerene yield was calculated. As a result, the fullerene yield was 2.5%.

[0095] Example 2 Except for setting the heating temperature of the heating unit 26 to 1000°C, fullerenes were produced in the same manner as in Example 1.

[0096] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 1.8%.

[0097] Example 3 Fullerenes were produced in the same manner as in Example 1, except that the flow rate of the nitrogen gas was set to 25 NL / min.

[0098] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 2.8%.

[0099] Example 4 Fullerenes were produced using a fullerene production apparatus 1 having a reactor 2 shown in FIG.

[0100] The second injection part 25b of the inert gas introduction part 10B is a tube made of zirconia. A circular second injection port 22a having a diameter of 20 mm is provided at the tip of the second injection part 25b. In the vertical direction, the tip surface of the second injection part 25b has the same height position as the tip surface of the first injection part 23c.

[0101] Fullerenes were produced in the same manner as in Example 1, except that the heating temperature of the heating unit 26 was set to 1200° C. and heated nitrogen gas was injected into the reactor 2 from the second nozzle 22a of the second injection unit 25b.

[0102] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 1.5%.

[0103] Example 5 Except for setting the heating temperature of the heating unit 26 to 1500°C, fullerenes were produced in the same manner as in Example 4.

[0104] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 1.8%.

[0105] Example 6 Fullerenes were produced using a fullerene production apparatus 1 having a reactor 2 shown in FIG.

[0106] The tip of the second injection part 25c has a structure as shown in Fig. 7(A). The nozzle 34a of the second injection part 25c of the inert gas introduction part 10C is made of zirconia. A circular second injection port 22a having a diameter of 8 mm is disposed at the tip of the nozzle 34a. The second injection part 25c has 16 nozzles 34a, which are disposed at equal distances from each other. In the vertical direction, the tip surface of the second ejection portion 25c has the same height position as the tip surface of the first ejection portion 23c.

[0107] Fullerenes were produced in the same manner as in Example 1, except that the heating temperature of the heating unit 26 was set to 1600° C. and heated nitrogen gas was injected into the reactor 2 from the second nozzle 22a of the second injection unit 25c.

[0108] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 2.0%.

[0109] Example 7 Fullerenes were produced using a fullerene production apparatus 1 having a reactor 2 shown in FIG.

[0110] The inert gas introduction part 10D has a second nozzle 22a shown in FIG. 9(A). The second nozzle 22a is open as shown in FIG. 10(B). The second injection part 25d of the inert gas introduction part 10D is a cylinder made of zirconia, and the cylinder has an inner diameter of 160 mm and a height of 400 mm. The inner peripheral surface of the second injection part 25d has 16 slit-shaped second nozzles 22a with a width of 8 mm and a height of 45 mm, which are arranged at equal distances from each other. In the vertical direction, the upper side of the slit-shaped second nozzles 22a is at the same height as the tip surface of the burner 9D.

[0111] The heating temperature of the heating unit 26 was set to 1600° C., and heated nitrogen gas was injected from the second injection port 22a of the second injection unit 25d into the reactor 2. Fullerenes were produced in the same manner as in Example 1 except for the above.

[0112] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 2.1%.

[0113] Comparative Example 1 Fullerenes were produced in the same manner as in Example 1, except that fullerenes were produced using a fullerene production apparatus 1 not having an inert gas introduction section 10A.

[0114] Under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the soot-like material produced was recovered from the recovery mechanism 3 in the same manner as in Example 1, and the fullerene yield was calculated. As a result, the fullerene yield was 0.6%.

[0115] From the above, it is found that the yield of fullerenes is improved in Examples 1 to 7 compared to Comparative Example 1. That is, by maintaining the inside of the reaction furnace 2 at a high temperature by using the heated inert gas, it is possible to improve the yield of fullerenes. [Explanation of symbols]

[0116] REFERENCE SIGNS LIST 1...Fullerene manufacturing apparatus 2...Reactor 3...Recovery mechanism 4...Cooling mechanism 5...Pressure reduction mechanism (vacuum pump) 6...First pipe 7...Second pipe 8...Third pipe 9,9A-9D...Burner 10,10A-10D...Inert gas introduction section 11...Filter 12...Collector 13...Solenoid valve 14...Tank 15...Discharge valve 16...Drain 21a...First nozzle 22a...Second nozzle 23...Burner holder 23a...Premixing chamber 23b...Accumulator 23c...First injection section 24a...Pipe 24b...Pipe 25a-25d...Second injection section 26...Heating section 27...Connecting pipe 28...Pipe 30...Insulating member 31...Ignition mechanism 34,34a,34b...Nozzle section

Claims

1. An apparatus for producing fullerenes by incomplete combustion of a raw material gas containing a hydrocarbon, comprising: A reactor; a burner including a first injection part that injects the raw material gas containing the hydrocarbon into the reactor; an inert gas introduction unit disposed outside the reactor, the inert gas introduction unit including a heating unit for heating the inert gas to 1000 to 2500°C, and a second injection unit for injecting the heated inert gas into the reactor; a tip surface of the first injection part in the reactor has a first injection port, The apparatus for producing fullerenes, wherein a tip surface of the second injection part in the reaction furnace has a second injection port.

2. 2. The fullerene producing apparatus according to claim 1, wherein either one of the first injection part and the second injection part is disposed so as to surround the other one of the first injection part and the second injection part.

3. 2. The fullerene producing apparatus according to claim 1, wherein at least a portion of said first injection portion and at least a portion of said second injection portion are arranged alternately in a concentric circle shape.

4. the first injection unit injects the raw material gas from one end side to the other end side of the reaction furnace, 2. The fullerene producing apparatus according to claim 1, wherein the second injection section injects the inert gas from a periphery between one end side and the other end side of the reaction furnace.

5. 5. The fullerene producing apparatus according to claim 1, further comprising a pressure reducing mechanism for reducing the pressure inside the reactor by evacuating the inside of the reactor.

6. A fullerene manufacturing apparatus as described in any one of claims 1 to 5, wherein the second injection section injects the heated inert gas into the reaction furnace at a flow rate of 15 to 25 NL / min.

7. A heating step of heating an inert gas to 1000 to 2500°C; a generating step of injecting a raw material gas containing a hydrocarbon and an oxygen-containing gas into a reactor and generating fullerenes in the reactor by incomplete combustion of the raw material gas containing the hydrocarbon; and an injection step of injecting the heated inert gas into the reaction furnace simultaneously with the generation step.

8. 8. The method for producing fullerenes according to claim 7, wherein the inside of the reaction furnace is evacuated while the inside of the reaction furnace is brought into a reduced pressure state.

9. 9. The method for producing fullerenes according to claim 8, wherein the pressure in the reaction furnace is set to 1 to 30 kPa.

10. The method for producing fullerenes according to any one of claims 7 to 9, wherein in the injection step, the heated inert gas is injected into the reaction furnace at a flow rate of 15 to 25 NL / min.

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