Apparatus and method for manufacturing fullerenes

Abstract

Provided is a fullerene production apparatus capable of improving the yield of fullerene. The fullerene production apparatus includes: a reaction furnace (2) that generates fullerene through incomplete combustion of a raw material gas containing a hydrocarbon; a first injection portion (23c) that injects the raw material gas into the reaction furnace (2) while causing the raw material gas to undergo incomplete combustion, thereby forming a first combustion flame; and a second injection portion (25a) that injects an auxiliary gas containing a hydrocarbon that is the same as or different from the raw material gas into the reaction furnace (2) while causing the auxiliary gas to undergo combustion, thereby forming a second combustion flame.

Description

Technical Field

[0001] The present invention relates to a device and method for producing fullerene.

[0002] This application claims priority based on Japanese Patent Application No. 2020-209111 filed in Japan on December 17, 2020, the contents of which are cited herein. Background Art

[0003] Known methods for producing fullerenes include a combustion method in which a raw material gas containing hydrocarbons (hereinafter also referred to as "raw material gas") is incompletely combusted in a reactor to produce fullerenes, and a thermal decomposition method in which a raw material gas containing hydrocarbons is thermally decomposed to produce fullerenes (see, for example, Patent Documents 1 to 4).

[0004] Prior art literature

[0005] Patent Literature

[0006] Patent Document 1: Japanese Patent Application Laid-Open No. 2003-160316

[0007] Patent Document 2: Japanese Patent Application Laid-Open No. 2003-171106

[0008] Patent Document 3: Japanese Patent Application Laid-Open No. 2003-221216

[0009] Patent Document 4: Chinese Patent No. 102757032 Summary of the Invention

[0010] Problems to be solved by the invention

[0011] Furthermore, to increase the fullerene yield, it is preferable to increase the temperature within the production apparatus. However, in the fullerene production apparatuses and methods described in Patent Documents 1 to 4, it is difficult to achieve or maintain a high temperature within the reaction apparatus, resulting in a low fullerene yield. Therefore, it is desirable to increase the fullerene yield and further reduce the fullerene production cost.

[0012] One aspect of the present invention has been made in view of the above-mentioned problems, and one object of the present invention is to provide a fullerene production apparatus and a fullerene production method capable of improving the fullerene yield.

[0013] Means for solving problems

[0014] In order to solve the above-mentioned problems, one aspect of the present invention provides the following means.

[0015] (1) A fullerene production apparatus comprising:

[0016] a reactor for producing fullerenes by incomplete combustion of a raw material gas containing hydrocarbons;

[0017] a first injection unit configured to inject the raw material gas and a first oxygen-containing gas into the reaction furnace while causing incomplete combustion of the raw material gas to form a first combustion flame; and

[0018] The second injection unit injects an assist gas containing hydrocarbons that are the same as or different from the raw material gas and a second oxygen-containing gas into the reactor, thereby burning the assist gas to form a second combustion flame.

[0019] (2) The fullerene production apparatus according to the above item (1), characterized by comprising:

[0020] a first flow rate adjustment unit configured to adjust a ratio A1 of the number of carbon atoms in the raw material gas to the number of oxygen atoms in the first oxygen-containing gas to 0.60 to 2.00, and supply the raw material gas and the first oxygen-containing gas to the first injection unit; and

[0021] The second flow rate adjustment unit adjusts the ratio A2 of the number of carbon atoms in the assist gas to the number of oxygen atoms in the second oxygen-containing gas to 0.30<A2<A1, and supplies the assist gas and the second oxygen-containing gas to the second injection unit.

[0022] (3) The fullerene production apparatus according to the above item (1) or (2), characterized in that one of the first ejection unit and the second ejection unit is disposed so as to surround the other one.

[0023] (4) The fullerene production apparatus according to the above item (1) or (2), characterized in that at least a portion of the first ejecting portion and at least a portion of the second ejecting portion are alternately arranged in a concentric circle.

[0024] (5) The fullerene production apparatus according to any one of the above (1) to (3), wherein a partition is provided between the first injection section and the second injection section.

[0025] (6) The fullerene production apparatus according to the above item (1) or (2), characterized in that the first injection unit injects the raw material gas from one end side toward the other end side of the reactor,

[0026] The second injection unit injects the assist gas from a periphery between one end side and the other end side of the reactor.

[0027] (7) The fullerene production apparatus according to any one of the above (1) to (6), further comprising a decompression mechanism for reducing the pressure in the reactor while suctioning the reactor.

[0028] (8) A method for producing fullerene, characterized in that:

[0029] The method comprises the steps of generating fullerenes in a reactor by incomplete combustion of a raw material gas containing hydrocarbons,

[0030] In the above step, the raw material gas and the first oxygen-containing gas are injected into the reaction furnace while the raw material gas is incompletely combusted to form a first combustion flame, and

[0031] While injecting an assist gas containing a hydrocarbon that is the same as or different from the raw gas and a second oxygen-containing gas into the reactor, the assist gas is combusted to form a second combustion flame, thereby heating the reactor.

[0032] The ratio A1 of the number of carbon atoms in the raw material gas to the number of oxygen atoms in the first oxygen-containing gas is set to 0.60 to 2.00.

[0033] The ratio A2 of the number of carbon atoms in the assist gas to the number of oxygen atoms in the second oxygen-containing gas is set to 0.30<A2<A1.

[0034] (9) The method for producing fullerene according to the above item (8), wherein the temperature in the reaction furnace is set to 1000 to 2000°C.

[0035] (10) The method for producing fullerene according to the above item (8) or (9), characterized in that, in the above step, the inside of the reaction furnace is brought into a reduced pressure state while suction is being performed inside the reaction furnace.

[0036] (11) The method for producing fullerene according to the above item (10), wherein the pressure in the reaction furnace is set to 1 to 30 kPa.

[0037] Effects of the Invention

[0038] According to one embodiment of the present invention, the yield of fullerenes can be improved. BRIEF DESCRIPTION OF THE DRAWINGS

[0039] Figure 1 This is a structural diagram showing an example of a fullerene production apparatus according to one embodiment of the present invention.

[0040] Figure 2 It is a cross-sectional view showing the structure of a reactor including the burner 9A and the burner 10A according to the first embodiment of the present invention.

[0041] Figure 3 This is an example Figure 2 The illustrated diagram is a plan view of the structure of the tip end surface of the injection portion of the burner 9A and the burner 10A.

[0042] Figure 4 It is a cross-sectional view showing the structure of a reactor including a burner 9B and a burner 10B according to a second embodiment of the present invention.

[0043] Figure 5 It shows Figure 4 The illustrated diagram is a plan view of the structure of the tip end surface of the injection portion of the burner 9B and the burner 10B.

[0044] Figure 6 It is a cross-sectional view showing the structure of a reactor including a burner 9C and a burner 10C according to a third embodiment of the present invention.

[0045] Figure 7 This is an example Figure 6 The illustrated diagram is a plan view of the structure of the tip end surface of the injection portion of the burner 9C and the burner 10C.

[0046] Figure 8 It is a cross-sectional view showing the structure of a reactor including a burner 9D and a burner 10D according to a fourth embodiment of the present invention.

[0047] Figure 9 This is an example Figure 8 A longitudinal sectional view showing the shapes and arrangements of a second injection portion 25d and second injection ports 22a included in the combustor 10D shown.

[0048] Figure 10 This is an example Figure 8 The illustrated cross-sectional view is a view showing the arrangement of the second injection ports 22a of the second injection portion 25d included in the combustor 10D. DETAILED DESCRIPTION

[0049] Hereinafter, a fullerene production apparatus and a fullerene production method to which the present invention is applied will be described in detail with reference to the accompanying drawings.

[0050] Note that, in the drawings used in the following description, characteristic portions may be schematically shown for convenience in order to facilitate understanding of the characteristics, and the dimensional ratios of the components are not necessarily the same as the actual ones.

[0051] (Fullerene Production Apparatus)

[0052] First, as one embodiment of the present invention, for example Figure 1 The fullerene production apparatus 1 shown in FIG.

[0053] It should be noted that Figure 1 1 is a structural diagram showing an example of a fullerene production apparatus 1 .

[0054] like Figure 1 As shown, the fullerene manufacturing device 1 of this embodiment includes: a reactor 2, which generates a coal-like material containing fullerenes through incomplete combustion of a raw material gas containing hydrocarbons; a recovery mechanism 3, which recovers the coal-like material generated in the reactor 2; a cooling mechanism 4, which cools the gas after passing through the recovery mechanism 3; and a pressure reducing mechanism 5, which draws in the gas cooled by the cooling mechanism 4 while making the reactor 2 a reduced pressure state.

[0055] The fullerene production apparatus 1 also includes 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 decompression mechanism 5 .

[0056] Reactor 2 is arranged vertically upright, comprising a cylindrical peripheral wall portion 2a, an upper wall portion 2b that closes the upper end (one end) of peripheral wall portion 2a, and a lower wall portion 2c that closes the lower end (the other end) of peripheral wall portion 2a. Reactor 2 may also include a sapphire glass window 2d for measuring internal temperature.

[0057] It should be noted that the material of the reaction furnace 2 includes, for example, heat-resistant materials such as zirconium oxide (ZrO2), tungsten (W), tantalum (Ta), platinum (Pt), titanium (Ti), titanium nitride (TiN), aluminum oxide (Al2O3), and silicon carbide (SiC). Furthermore, at least a portion of the outside and inside of the reaction furnace 2 may be lined with a heat-insulating material such as alumina refractory bricks or alumina monolithic refractory materials.

[0058] It should be noted that, regarding the placement of the reactor 2, it is preferably arranged in the aforementioned vertical direction to minimize the impact of coal-like material retention. Furthermore, when the reactor 2 is arranged in the vertical direction, it is preferred to supply the raw gas from above. Alternatively, the reactor 2 may be arranged in a tilted position, for example, horizontally or in an inclined direction.

[0059] The first pipe 6 is connected to an exhaust gas outlet 30d (hereinafter referred to as "exhaust gas outlet 30d") provided on the lower wall portion 2c of the reactor 2. Meanwhile, burners 9 and 10 are provided on the upper wall portion 2b of the reactor 2. In the reactor 2, the raw material gas injected from the burner 9 and the first oxygen-containing gas are incompletely combusted, thereby generating a coal-like material containing fullerenes.

[0060] Furthermore, the assist gas and the second oxygen-containing gas injected from the burner 10 into the reactor 2 are combusted, thereby heating the interior of the reactor 2. As a result, high-temperature exhaust gas containing soot, carbon monoxide, carbon dioxide, water vapor, and the like generated by the combustion of the raw gas and the assist gas passes through the first pipe 6 and reaches the recovery mechanism 3.

[0061] The recovery mechanism 3 includes a trap 12 housing a filter 11 , a tank 14 connected to the upper end (one end) of the trap 12 via a solenoid valve 13 , and a discharge valve 15 provided at the lower end (the other end) of the trap 12 .

[0062] The first pipe 6 is connected to the side surface of the upper portion of the trap 12. The second pipe 7 is connected to the upper portion of the trap 12. A sintered metal filter, for example, is used as the filter 11. A solenoid valve 13 is branched from the second pipe 7 and connected thereto. A high-pressure inert gas, such as nitrogen (N2) or argon (Ar), is stored in the tank 14.

[0063] In the recovery mechanism 3, after the soot-like matter contained in the exhaust gas supplied from the first pipe 6 is captured by the filter 11, the solenoid valve 13 is periodically opened to spray inert gas from the tank 14 toward the collector 12. This causes the soot-like matter adhering to the filter 11 to fall off. The soot-like matter accumulated in the collector 12 can then be recovered by opening the discharge valve 15.

[0064] The cooling mechanism 4 has a structure similar to or the same as that of a general heat exchanger, and one end (upper end) thereof is connected to the second pipe 7 , while the other end (lower end) thereof is connected to the third pipe 8 .

[0065] The gas that has passed through the recovery mechanism 3 is cooled in the cooling mechanism 4. In addition, the unreacted hydrocarbons and water vapor in the gas can be liquefied in the cooling mechanism 4 and discharged from the discharge passage 16 provided on the lower side.

[0066] It should be noted that, unlike the cooling mechanism 4 , since the exhaust gas passing through the first pipe 6 is at a high temperature, the first pipe 6 may be cooled.

[0067] The decompression mechanism 5 is composed of a vacuum pump and sucks the gas cooled by the cooling mechanism 4 after passing through the third pipe 8. This creates a negative pressure between the reactor 2 and the decompression mechanism 5, while discharging the coal-like material generated in the reactor 2 to the recovery mechanism 3 through the first pipe 6.

[0068] Examples of hydrocarbons included 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 and carboxylic acid oils; ethylenically unsaturated hydrocarbons; acetylene-based unsaturated hydrocarbons; and aliphatic saturated hydrocarbons such as pentane and hexane. Furthermore, a mixture of two or more of these hydrocarbons may be used. The raw material gas preferably includes aromatic hydrocarbons among the above hydrocarbons. It should be noted that the raw material gas may also be diluted with an inert gas such as nitrogen or argon, as needed.

[0069] The hydrocarbons contained in the auxiliary gas may be the same as or different from the above-mentioned raw material gas. For example, there may be mentioned alkanes with carbon numbers of 1 to 8, olefins with carbon numbers of 2 to 8, alkynes with carbon numbers of 2 to 8, aromatic hydrocarbons with carbon numbers of 6 to 15 such as benzene, toluene, xylene, naphthalene, methylnaphthalene, anthracene, and phenanthrene, coal-based hydrocarbons such as creosote and carboxylic acid oil, aliphatic saturated hydrocarbons such as pentane and hexane, ethers such as dimethyl ether, diethyl ether, and ethyl methyl ether, alcohols such as methanol and ethanol, ketones such as acetone, methyl ethyl ketone, and diethyl ketone. In addition, two or more of the above-mentioned hydrocarbons may be used in combination. The auxiliary gas preferably contains alkanes with carbon numbers of 1 to 8, olefins with carbon numbers of 2 to 8, and alkynes with carbon numbers of 2 to 8 among the above-mentioned hydrocarbons. It should be noted that the auxiliary gas may also be diluted with an inert gas such as nitrogen or argon as needed.

[0070] The first oxygen-containing gas and the second oxygen-containing gas are gases containing oxygen molecules, and examples thereof include oxygen gas and air. The first oxygen-containing gas and the second oxygen-containing gas may be supplied to the reactor 2 separately from the raw material gas and the auxiliary gas, or the raw material gas and the auxiliary gas may be mixed separately in advance and then supplied to the reactor 2.

[0071] Examples of the generated fullerenes include C 60 Fullerene (C 60 ), C 70 Fullerene (C 70 ), C 76 、C 78 、C 84 、C 90 、C 96 and other higher-order fullerenes.

[0072] (Method for producing fullerene)

[0073] Next, a method for producing fullerene using the above-described fullerene production apparatus 1 will be described.

[0074] The method for producing fullerenes according to the present embodiment is characterized in that it includes a step of generating fullerenes by incompletely combusting a raw material gas containing hydrocarbons in a reactor 2. In this step, the raw material gas and a first oxygen-containing gas are injected into the reactor 2 to incompletely combust the raw material gas to form a first combustion flame, and an auxiliary gas and a second oxygen-containing gas are injected into the reactor 2 to combust the auxiliary gas to form a second combustion flame, thereby heating the interior of the reactor 2.

[0075] The ratio A1 of the number of carbon atoms in the raw material gas to the number of oxygen atoms in the first oxygen-containing gas injected into the reactor 2 is preferably 0.60 to 2.00, more preferably 0.80 to 1.70, and even more preferably 1.00 to 1.50. This can increase the yield of fullerenes.

[0076] For example, in the case of toluene (carbon number: 7) being vaporized as the raw material gas, the carbon number in the raw material gas when the raw material gas supply rate is 20 g / min, that is, 0.217 mol / min, is 7×0.217×6.02×10 23 When the supply rate of oxygen molecules is 13 NL / min (0.582 mol / min), the supply rate of oxygen atoms becomes 2×0.582×6.02×10 23 Therefore, A1 is calculated as (7×0.217) / (2×0.582)=1.31. The same is true for A2.

[0077] Furthermore, the ratio A2 of the number of carbon atoms in the assist gas injected into reactor 2 to the number of oxygen atoms in the second oxygen-containing gas preferably satisfies 0.30 < A2 < A1. When A2 is greater than 0.30, the excess of the second oxygen-containing gas is eliminated or minimized, thereby minimizing the impact of incomplete combustion of the raw material gas. On the other hand, when A2 is less than A1, the second combustion flame generated by the combustion of the assist gas is higher in intensity than the first combustion flame (incomplete combustion flame) generated by the incomplete combustion of the raw material gas, allowing the second combustion flame to heat the interior of reactor 2.

[0078] A2 satisfies 0.30<A2<A1, and is preferably 0.35 to 0.85, more preferably 0.35 to 0.55. A2 of 0.35 to 0.85 is preferred because the assist gas is burned completely or nearly completely, and the temperature of the generated second combustion flame is high.

[0079] Typically, the temperature of the first combustion flame for generating fullerenes is 500°C to 2000°C. Meanwhile, the temperature of the second combustion flame generated by burning the assist gas is preferably 1000°C to 2500°C, more preferably 1100°C to 2200°C. This allows the temperature (atmosphere) within the reactor 2 to be maintained at a high temperature.

[0080] Furthermore, the raw material gas is incompletely combusted in the high-temperature reactor 2 to generate a soot-like material, thereby increasing the yield of fullerenes contained in the generated soot-like material.

[0081] From the perspective of increasing the yield of fullerenes, the temperature within the reactor 2 after heating by the second combustion flame is preferably 1000-2000°C, more preferably 1500-2000°C. If the temperature within the reactor 2 is below 1000°C, the effect of increasing the yield of fullerenes is low. On the other hand, if the temperature within the reactor 2 exceeds 2000°C, a large amount of assist gas is required to increase the temperature within the reactor 2, resulting in low efficiency. The temperature within the reactor 2 can be measured using an ultra-high temperature thermocouple or a radiation thermometer.

[0082] The pressure in the reactor 2 is preferably 1 to 30 kPa, more preferably 1 to 10 kPa. If the pressure in the reactor 2 is less than 1 kPa, the load on the pressure reducing mechanism 5 increases. On the other hand, if the pressure in the reactor 2 exceeds 30 kPa, the flame may flash back.

[0083] (First embodiment)

[0084] Next, a fullerene production apparatus 1 according to a first embodiment of the present invention will be described.

[0085] The fullerene production apparatus 1 according to the first embodiment of the present invention includes Figure 2 The burner 9 (hereinafter referred to as "burner 9A") and the burner 10 (hereinafter referred to as "burner 10A") are shown.

[0086] It should be noted that Figure 2 It is a cross-sectional view showing the structure of the reactor 2 including the burner 9A and the burner 10A. Figure 3 (A) and (B) are plan views illustrating the configuration of the distal end surfaces of a first injection portion 23c and a second injection portion 25a described later.

[0087] The combustor 9A of the present embodiment has a top-cylindrical combustor holder 23 installed in a state of penetrating the upper wall portion 2b of the reaction furnace 2, and a first premixing chamber 23a, a pressure accumulation chamber 23b, and a first injection portion 23c provided in this order on the inner side of the combustor holder 23 from the upper side. In addition, a pipe 24a for introducing a raw material gas and a pipe 24b for introducing a first oxygen-containing gas are connected to the upper portion of the combustor holder 23.

[0088] A first flowmeter 35a that controls the flow rate of the raw material gas (or liquid hydrocarbon) is provided in the pipe 24a. Note that a gasification device such as a heating device that gasifies the liquid hydrocarbon can also be provided in the pipe 24a between the first flowmeter 35a and the upper portion of the combustor holder 23.

[0089] A first flowmeter 35b that controls the flow rate of the first oxygen-containing gas is provided in the pipe 24b. The first flow rate adjustment portion adjusts the ratio A1 of the number of carbon atoms of the raw material gas to the number of oxygen atoms of the first oxygen-containing gas to 0.60 to 2.00 using the first flowmeters 35a, 35b, and supplies the raw material gas and the first oxygen-containing gas to the first injection portion 23c.

[0090] Note that the first flowmeters 35a, 35b can be any device that can adjust the raw material gas (or liquid hydrocarbon) and the first oxygen-containing gas to a prescribed flow rate, and for example, a commercially available mass flow controller or the like can be used.

[0091] The first premixing chamber 23a uniformly mixes the raw material gas introduced from the pipe 24a and the first oxygen-containing gas introduced from the pipe 24b. The pressure accumulation chamber 23b accumulates the raw material gas and the first oxygen-containing gas (hereinafter also referred to as "first mixed gas") mixed in the first premixing chamber 23a at a prescribed pressure. The first injection portion 23c has a plurality of first injection ports 21a and injects the first mixed gas accumulated in the pressure accumulation chamber 23b from the first injection ports 21a toward the lower side (toward the direction of the exhaust gas discharge port 30d). The first injection portion 23c can also be composed of a porous ceramic sintered body or a sintered body of metal powder.

[0092] In addition, in the present embodiment, the first premixing chamber 23a, the pressure accumulation chamber 23b, and the first injection portion 23c are provided on the inner side of the combustor holder 23, but the first premixing chamber 23a can also be omitted. Also, the first premixing chamber 23a and the pressure accumulation chamber 23b can also be provided outside the combustor holder 23 as needed.

[0093] The combustor 10A has a second injection portion 25a, a second premixing chamber 26 disposed outside the reaction furnace 2, and a connection pipe 27 that connects between the second injection portion 25a and the second premixing chamber 26.

[0094] The second injection portion 25a is, for example, a tube having a certain thickness, and is provided at its top end with a second injection port 22a for injecting the assist gas and the second oxygen-containing gas into the reactor 2. Furthermore, a passage 22b is provided inside the second injection portion 25a, connecting the second injection port 22a to the connecting pipe 27. The second injection portion 25a is arranged so as to surround the first injection portion 23c.

[0095] There are no particular limitations on the shape and number of the second injection ports 22a. For example, Figure 3 (A) shows a circular shape. Figure 3 In (A), the distal end surface of the second injection portion 25a is annular, and the plurality of second injection ports 22a are evenly arranged on the distal end surface of the second injection portion 25a.

[0096] In addition, if Figure 3 As shown in FIG. 2 (B), an annular second injection port 22a may be arranged on the distal end surface of the annular second injection portion 25a.

[0097] The second premixing chamber 26 is connected to a pipe 28 a for introducing an assist gas and a pipe 28 b for introducing a second oxygen-containing gas.

[0098] A second flowmeter 36a for controlling the flow rate of assist gas (or liquid hydrocarbons) is provided in the piping 28a. A vaporizing device such as a heater for vaporizing the liquid hydrocarbons may be provided in the piping 28a between the second flowmeter 36a and the second premixing chamber 26.

[0099] A second flowmeter 36b for controlling the flow rate of the second oxygen-containing gas is installed in the pipe 28b. The second flow rate adjustment unit uses the second flowmeters 36a and 36b to adjust the ratio A2 of the number of carbon atoms in the assist gas to the number of oxygen atoms in the second oxygen-containing gas to 0.30 < A2 < A1, and then supplies the assist gas and the second oxygen-containing gas to the second injection unit 25a.

[0100] It should be noted that the second flow meters 36 a and 36 b only need to be able to adjust the assist gas (or liquid hydrocarbon) and the second oxygen-containing gas to predetermined flow rates, and for example, commercially available mass flow controllers can be used.

[0101] The second premixing chamber 26 uniformly mixes the assist gas introduced from the pipe 28 a and the second oxygen-containing gas introduced from the pipe 28 b .

[0102] The connecting pipe 27, while extending through the upper portion of the peripheral wall 2a of the reactor 2, supplies the assist gas and the second oxygen-containing gas (hereinafter referred to as the "second mixed gas") mixed in the second premixing chamber 26 to the second injection unit 25a. Alternatively, the connecting pipe 27 can extend through the upper wall 2b of the reactor 2 to supply the second mixed gas to the second injection unit 25a. The second injection unit 25a injects the second mixed gas supplied via the connecting pipe 27 downward (toward the exhaust gas outlet 30d) from the second injection port 22a.

[0103] A partition 29 is provided between the first injection section 23c and the second injection section 25a. The partition 29 has a partition wall 29a protruding from between the first injection port 21a and the second injection port 22a toward a position below the first injection port 21a and the second injection port 22a on the top surfaces of the first injection section 23c and the second injection section 25a.

[0104] The partition 29 may be formed integrally with a heat insulating member 30 disposed within the reactor 2. The heat insulating member 30 includes a cylindrical peripheral wall 30a disposed along the inner peripheral wall portion 2a of the reactor 2; a bottom wall 30b disposed along the inner lower wall portion 2c of the reactor 2; and a top wall 30c that closes the upper portion of the peripheral wall 30a.

[0105] The burner holder 23 and the second injection portion 25a extend through the top wall 30c, with the first injection port 21a and the second injection port 22a facing the inside of the heat insulating member 30. Furthermore, the bottom wall 30b is provided with an exhaust gas outlet 30d that communicates with the first pipe 6. The heat insulating member 30 may be made of, for example, alumina refractory bricks or alumina monolithic refractory materials.

[0106] Furthermore, an ignition mechanism 31 for igniting the raw material gas and the assist gas is provided near a position to which the first pipe 6 of the reactor 2 is connected.

[0107] The burner 9A and the burner 10A of this embodiment having the above-mentioned structure inject raw gas and the first oxygen-containing gas from the above-mentioned first injection port 21a, while causing the raw gas to be incompletely burned to form a first combustion flame for generating a coal-like material containing fullerenes in the reactor 2, and at the same time inject auxiliary gas and the second oxygen-containing gas from the above-mentioned second injection port 22a, while causing the auxiliary gas to burn to form a second combustion flame (preferably a complete combustion flame) with a higher temperature than the first combustion flame, thereby heating the inside of the reactor 2.

[0108] Thus, in the fullerene production apparatus 1 including the burners 9A and 10A of the present embodiment, the temperature inside the reactor 2 can be maintained at a high temperature, and the yield of fullerenes contained in the generated soot-like material can be increased.

[0109] Furthermore, in the burners 9A and 10A of this embodiment, a partition 29 is provided between the first injection portion 23c (first injection port 21a) and the second injection portion 25a (second injection port 22a). This prevents the first combustion flame and the second combustion flame, which are injected in the same direction, from mixing. This prevents fullerenes contained in the generated soot-like material from being burned by the second combustion flame.

[0110] (Second embodiment)

[0111] Next, a fullerene production apparatus 1 according to a second embodiment of the present invention will be described.

[0112] A fullerene production apparatus 1 according to a second embodiment of the present invention includes: Figure 4 and Figure 5 The burner 9 (hereinafter referred to as "burner 9B") and the burner 10 (hereinafter referred to as "burner 10B") are shown.

[0113] It should be noted that Figure 4 It is a cross-sectional view showing the structure of the reactor 2 including the burners 9B and 10B. Figure 5 This is a top view showing the structure of the top surface of the first injection portion 23c of the burner 9B and the second injection portion 25b of the burner 10B, which will be described later. In the following description, description of parts equivalent to those of the burners 9A and 10A will be omitted, and the same reference numerals will be assigned in the drawings.

[0114] In this embodiment, if Figure 4 As shown, the burner 10B has a tubular second injection portion 25b. The second injection portion 25b is provided at the inner center of the burner holder 23 and vertically penetrates the first premixing chamber 23a, the pressure accumulator chamber 23b, and the first injection portion 23c. Thus, the second injection portion 25b is surrounded by the first injection portion 23c. Figure 5 As shown, the second injection port 22a is provided at the top end of the second injection portion 25b and is surrounded by the first injection port 21a of the first injection portion 23c. It should be noted that the second injection portion 25b is directly connected to the second premixing chamber 26.

[0115] The burner 9B has the same structure as the burner 9A, except that the first premixing chamber 23a, the pressure accumulation chamber 23b, and the first injection portion 23c are vertically penetrated by the second injection portion 25b.

[0116] Furthermore, the tip (lower end) of the second jet portion 25b protrudes downward from the tip (lower end) of the first jet portion 23c. Consequently, the first jet port 21a and the second jet port 22a are positioned differently in the jetting direction (toward the exhaust gas outlet 30d). Specifically, the second jet port 22a is positioned lower than the first jet port 21a.

[0117] The burner 9B and the burner 10B of this embodiment having the above-mentioned structure inject raw gas and the first oxygen-containing gas from the above-mentioned first injection port 21a, while causing the raw gas to be incompletely burned to form a first combustion flame for generating a coal-like material containing fullerenes in the reactor 2, and at the same time inject auxiliary gas and the second oxygen-containing gas from the above-mentioned second injection port 22a, while causing the auxiliary gas to burn to form a second combustion flame (preferably a complete combustion flame) with a higher temperature than the first combustion flame, thereby heating the inside of the reactor 2.

[0118] Thus, in the fullerene production apparatus 1 including the burners 9B and 10B of the present embodiment, the temperature inside the reactor 2 can be maintained at a high temperature, and the yield of fullerenes contained in the generated soot-like material can be increased.

[0119] Furthermore, in the burners 9B and 10B of this embodiment, the first and second injection ports 21a and 22a are positioned in different directions in their injection directions, thereby preventing the first and second combustion flames, which are injected in the same direction, from mixing. This prevents fullerenes contained in the generated soot-like material from being burned by the second combustion flame.

[0120] (Third embodiment)

[0121] Next, a fullerene production apparatus 1 according to a third embodiment of the present invention will be described.

[0122] A fullerene production apparatus 1 according to a third embodiment of the present invention includes: Figure 6 and Figure 7 The burner 9 (hereinafter referred to as "burner 9C") and the burner 10 (hereinafter referred to as "burner 10C") are shown.

[0123] It should be noted that Figure 6 It is a cross-sectional view showing the structure of the reactor 2 including the burner 9C and the burner 10C. Figure 7(A) and (B) are plan views illustrating the top end surfaces of the first injection portion 23c of the burner 9C and the second injection portion 25c of the burner 10B, described later. In the following description, descriptions of components identical to those of the burners 9A and 10A will be omitted, and the same reference numerals will be assigned in the accompanying drawings.

[0124] In this embodiment, if Figure 6 As shown, the burner 10C includes a second injection section 25c disposed within the burner holder 23. The second injection section 25c includes a plurality of nozzle sections 34 branching from a connecting pipe 27. The nozzle sections 34 are arranged to vertically penetrate the pressure accumulation chamber 23b and the first injection section 23c. Furthermore, the connecting pipe 27 extends through the upper center portion of the burner holder 23, connecting the second injection section 25c to the second premixing chamber 26.

[0125] Specifically, the nozzle portion 34 may be, for example, tubular or cylindrical with a certain thickness. The second injection port 22a is arranged on the top surface of the nozzle portion 34. In addition, when the nozzle portion 34 is cylindrical, a passage 22c is provided inside the nozzle portion 34 to connect the connecting pipe 27 to the second injection port 22a. The second injection portion 25c may have only one of the tubular nozzle portion 34 (hereinafter also referred to as the "nozzle portion 34a") and the cylindrical nozzle portion 34 (hereinafter also referred to as the "nozzle portion 34b"), or both.

[0126] For example, Figure 7 The second injection section 25c of the burner 10C shown in FIG. 1 (A) includes multiple nozzle sections 34a. Each nozzle section 34a has a second injection port 22a with a circular opening at the tip of the first injection section 23c and the second injection section 25c. As a result, the second injection section 25c (second injection port 22a) is surrounded by the first injection section 23c (first injection port 21a).

[0127] on the other hand, Figure 7 The second injection section 25c of the burner 10C shown in FIG. 1B has a single nozzle section 34a at its center, with multiple nozzle sections 34b arranged around nozzle section 34a. At the top ends of the first and second injection sections 23c and 25c, nozzle section 34a has multiple second injection ports 22a opening in a circular shape, while nozzle section 34b has multiple second injection ports 22a opening in an annular shape.

[0128] The nozzle portion 34a (second injection port 22a) is surrounded by the first injection port 23c (first injection port 21a), and the nozzle portion 34b (second injection port 22a) and a portion of the first injection port 23c (first injection port 21a) are alternately arranged concentrically.

[0129] The burner 9C has the same structure as the burner 9A except that the first premixing chamber 23 a , the pressure accumulation chamber 23 b , and the first injection portion 23 c are vertically connected via a connecting pipe 27 and a nozzle portion 34 .

[0130] Furthermore, the tip (lower end) of the nozzle portion 34 protrudes downward from the tip (lower end) of the first injection portion 23c. Consequently, the first injection port 21a and the second injection port 22a are positioned differently in the injection direction (toward the exhaust gas outlet 30d). Specifically, the second injection port 22a is positioned lower than the first injection port 21a.

[0131] In the burner 9C and the burner 10C of the present embodiment having the above-mentioned structure, the raw gas and the first oxygen-containing gas are injected from the above-mentioned first injection port 21a, and the raw gas is incompletely burned to form a first combustion flame for generating a coal-like material containing fullerenes in the reactor 2. The auxiliary gas and the second oxygen-containing gas are injected from the above-mentioned second injection port 22a, and the auxiliary gas is burned to form a second combustion flame (preferably a complete combustion flame) with a higher temperature than the first combustion flame, thereby heating the inside of the reactor 2.

[0132] Thus, in the fullerene production apparatus 1 including the burners 9C and 10C of the present embodiment, the temperature inside the reactor 2 can be maintained at a high temperature, and the yield of fullerenes contained in the generated soot-like material can be increased.

[0133] Furthermore, in the burners 9C and 10C of this embodiment, the first and second injection ports 21a and 22a are positioned in different directions in their injection directions, thereby preventing the first and second combustion flames, which are injected in the same direction, from mixing. This prevents fullerenes contained in the generated soot-like material from being burned by the second combustion flame.

[0134] (Fourth embodiment)

[0135] Next, a fullerene production apparatus 1 according to a fourth embodiment of the present invention will be described.

[0136] A fullerene production apparatus 1 according to a fourth embodiment of the present invention includes: Figure 8 and Figure 9 The burner 9 (hereinafter referred to as "burner 9D") and the burner 10 (hereinafter referred to as "burner 10D") are shown.

[0137] It should be noted that Figure 8 It is a cross-sectional view showing the structure of the reactor 2 including the burner 9D and the burner 10D. Figure 9It is a longitudinal sectional view illustrating the shape and arrangement of the second injection portion 25d and the second injection port 22a included in the combustor 10D. Figure 10 This is a cross-sectional view illustrating the arrangement of the second injection ports 22a of the second injection portion 25d included in the burner 10D. In the following description, descriptions of parts equivalent to those of the burners 9A and 10A are omitted, and the same reference numerals are used in the drawings.

[0138] The burner 9D of this embodiment has the same structure as the above-mentioned burner 9A.

[0139] The burner 10D has Figure 8 The second injection portion 25d has a cylindrical shape extending downward from a position surrounding the burner holder 23 and is provided around the reactor 2 between one end (the upper wall 2b side) and the other end (the lower wall 2c side).

[0140] A plurality of second injection ports 22a are arranged on the inner circumference of the second injection section 25d. Furthermore, a passage 22d is provided inside the second injection section 25d, connecting the connecting pipe 27 to the second injection ports 22a. This allows the second injection section 25d to inject assist gas into the reactor 2 from the second injection ports 22a.

[0141] The second injection port 22a on the inner peripheral surface of the second injection portion 25d may have a Figure 9 The shapes and configurations shown in (A), (B), and (C) are as follows. For example, Figure 9 The plurality of second injection ports 22a shown in FIG. 1(A) are each opened in a slit shape in the axial direction of the second injection portion 25d and are arranged in a row in the circumferential direction of the second injection portion 25d.

[0142] on the other hand, Figure 9 The plurality of second injection ports 22a shown in FIG. 1(B) are each opened in a circular shape and are arranged in a row along the circumferential direction and the axial direction of the second injection portion 25d.

[0143] on the other hand, Figure 9 The plurality of second injection ports 22a shown in FIG. 5(C) are each opened in a slit shape in the circumferential direction of the second injection portion 25d and are arranged side by side in the axial direction of the second injection portion 25d.

[0144] In addition, the second injection portion 25d has a Figure 9 In the case of a plurality of second injection ports 22a as shown in (A) and (B), the plurality of second injection ports 22a may be arranged in a manner as follows: Figure 10 For example, Figure 10The plurality of second injection ports 22a shown in FIG. 2A are formed by protrusions 33 that open obliquely in the same direction on the inner peripheral surface of the second injection portion 25d. This allows the assist gas injected from each second injection port 22a to form a vortex flow.

[0145] on the other hand, Figure 10 The plurality of second injection ports 22a shown in FIG. 2B open in the circumferential direction of the second injection portion 25d toward the center of the reactor 2. Thus, the assist gas injected from each second injection port 22a can be injected toward the center of the reactor 2.

[0146] In this embodiment, the first injection portion 23c can inject the raw material gas from the first injection port 21a located at one end side (the upper wall 2b side) of the reactor 2 toward the other end side (the lower wall 2c side). The second injection portion 25d can inject the assist gas from the second injection port 22a located around the reactor 2 between the one end side (the upper wall 2b side) and the other end side (the lower wall 2c side).

[0147] In the burner 9D and the burner 10D of the present embodiment having the above-mentioned structure, the raw material gas and the first oxygen-containing gas are injected from the above-mentioned first injection port 21a, and the raw material gas is incompletely burned to form a first combustion flame for generating a coal-like material containing fullerenes in the reactor 2. At the same time, the auxiliary gas and the second oxygen-containing gas are injected from the above-mentioned second injection port 22a, and the auxiliary gas is burned to form a second combustion flame (preferably a complete combustion flame) with a higher temperature than the first combustion flame, thereby heating the inside of the reactor 2.

[0148] Thus, in the fullerene production apparatus 1 including the burners 9D and 10D of the present embodiment, the temperature inside the reactor 2 can be maintained at a high temperature, and the yield of fullerenes contained in the generated soot-like material can be increased.

[0149] It should be noted that 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.

[0150] [Example]

[0151] The effects of the present invention will be further clarified by way of the following examples. It should be noted that the present invention is not limited to the following examples, and can be implemented by making appropriate changes without departing from the spirit of the present invention.

[0152] [Calculation of fullerenes]

[0153] In the following Examples 1 to 7 and Comparative Example 1, C 60 and C 70 The total of the yields was calculated as the fullerene yield.

[0154] In addition, according to "JIS Z 8981", the content of C 60 and C 70 in the recovered coal-like substance was measured as follows.

[0155] Specifically, 15 g of 1,2,3,5-tetramethylbenzene (TMB) was added to 0.05 g of the recovered coal-like substance, and ultrasonic treatment was performed for 15 minutes to obtain a suspension. The obtained suspension was filtered with a membrane filter having a pore size of 0.5 μm, and the filtrate (sample solution) was analyzed by high performance liquid chromatography (HPLC) to quantify C 60 and C 70 , and the content [mass %] of C 60 and C 70 in the coal-like substance was calculated.

[0156] Here, in calculating the content of C 60 and C 70 in the coal-like substance, a standard curve was used which was prepared in advance from TMB solutions having a plurality of known concentrations of C 60 and C 70 .

[0157] The measurement conditions of HPLC were as follows.

[0158] Apparatus: Infinity 1260 (manufactured by Agilent)

[0159] Injection amount of sample solution: 5 μL

[0160] Eluent: toluene (47 vol %) / methanol (53 vol %) mixed solvent

[0161] Flow rate of eluent: 1 ml / min

[0162] Column: YMC-Pack ODS-AM 100*4.6 mm ID S-3 μm, 12 nm

[0163] Measurement temperature: 40°C

[0164] Detector: UV 325 nm (JIS)

[0165] Next, the fullerene yield [mass %] was calculated by the formula {(amount of recovered coal-like substance [g]) / (amount of consumed raw gas [g])} x (content of fullerene [mass %]) based on the content of fullerene (the total of the contents of C 60 and C 70 ) contained in the coal-like substance.

[0166] "Measurement of the temperature in the reaction furnace"

[0167] The temperature in the reactor 2 of Examples 1 to 7 and Comparative Example 1 described below was measured using a high-performance single-color thermometer Marathon MM (manufactured by Raytek) through a sapphire glass window 2 d.

[0168] (Example 1)

[0169] Use with Figure 2 The fullerene production apparatus 1 of the reactor 2 shown in FIG. produces fullerene. The top end of the second injection part 25a has Figure 3 The structure shown in (A).

[0170] Here, the reactor 2 is an alumina cylinder arranged in the vertical direction, with a height of 1000 mm and an inner diameter of 200 mm. A burner 9A is provided so as to penetrate the upper wall 2b of the reactor 2. A 60 mm x 60 mm sapphire glass window 2d is provided in the reactor 2, and the upper side of the sapphire glass window 2d is parallel to the top surface of the first injection part 23c. The first injection part 23c is composed of a porous ceramic sintered body in the shape of a disk with a diameter of 100 mm. In this ceramic sintered body, a hole is formed every 1 cm. 2 60 to 80 holes (first injection ports 21 a ) having a diameter of approximately 0.5 mm to 1.0 mm are formed.

[0171] The second injection section 25a of the burner 10A is a stainless steel cylinder with an inner diameter of 160 mm and an internal cooling water channel. Forty second injection ports 22a with a diameter of 10 mm are evenly spaced at the top surface of the second injection section 25a. Vertically, the top surface of the second injection section 25a is at the same height as the top surface of the first injection section 23c. Furthermore, an alumina partition wall 29a is provided between the first and second injection sections 23c, protruding 40 mm below the top surfaces of the first and second injection sections 23c, 25a.

[0172] Toluene was used as the raw material gas, and pure oxygen (purity 99.9% by volume) was used as the first oxygen-containing gas. Here, toluene was heated in a gasification device installed in the pipe 24a to form a gas, and then supplied to the burner 9A.

[0173] The flow rate of toluene was controlled by a mass controller (Aera SFC168, manufactured by Hitachi Metals) as the first flowmeter 35a, and the flow rate of pure oxygen was controlled by a mass flowmeter (Mass Controller Aera, FC-7810CD, manufactured by Hitachi Metals) as the first flowmeter 35b.

[0174] The flow rate of toluene was set to 20 g / min, and the flow rate of pure oxygen was set to 13 NL / min. In addition, the ratio A1 of the number of carbon atoms in the raw material gas supplied to the reactor 2 to the number of oxygen atoms in the first oxygen-containing gas was 1.31.

[0175] Toluene was used as the assist gas, and pure oxygen (purity 99.9% by volume) was used as the second oxygen-containing gas. Here, toluene was heated in a vaporizer installed in the pipe 28a to form a gas, and then supplied to the burner 10A.

[0176] The flow rate of toluene was controlled by a mass controller (Aera SFC168, manufactured by Hitachi Metals) as the second flow meter 36a, and the flow rate of pure oxygen was controlled by a mass flow meter (Mass Controller Aera, FC-7810CD, manufactured by Hitachi Metals) as the second flow meter 36b.

[0177] The flow rate of toluene was set to 20 g / min, and the flow rate of pure oxygen was set to 18 NL / min. Furthermore, during fullerene production, the pressure inside the reactor 2 was maintained at 5.33 kPa. Furthermore, the ratio of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas was set to A2, which was 0.95, satisfying the following conditions: 0.30 < A2 (0.95) < A1 (1.31).

[0178] The temperature inside the reactor 2 during fullerene production was 1120°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 1.2%.

[0179] (Example 2)

[0180] Fullerenes were produced in the same manner as in Example 1, except that the flow rate of toluene as the assist gas was set to 20 g / min and the flow rate of pure oxygen as the second oxygen-containing gas was set to 21 NL / min. Furthermore, the ratio of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas, A2, was 0.81, satisfying the following conditions: 0.30 < A2 (0.81) < A1 (1.31).

[0181] The temperature of the reactor 2 during fullerene production was 1680°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 1.5%.

[0182] (Example 3)

[0183] Fullerenes were produced in the same manner as in Example 1, except that the flow rate of toluene as the assist gas was set to 20 g / min and the flow rate of pure oxygen as the second oxygen-containing gas was set to 25 NL / min. Furthermore, the ratio A2 of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas was 0.68, which satisfies the condition 0.30<A2(0.68)<A1(1.31).

[0184] The temperature of the reactor 2 during fullerene production was 1870°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 2.1%.

[0185] (Example 4)

[0186] Fullerenes were produced in the same manner as in Example 5, except that 1-hexene was used as the assist gas at a flow rate of 13 g / min and the flow rate of pure oxygen as the second oxygen-containing gas was set at 25 NL / min. The ratio of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas, A2, was 0.42, satisfying the following conditions: 0.30 < A2 (0.42) < A1 (1.31).

[0187] The temperature of the reactor 2 during fullerene production was 1810°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 1.9%.

[0188] (Example 5)

[0189] Use with Figure 4 The fullerene production apparatus 1 having the reactor 2 shown produces fullerene.

[0190] The second injection portion 25b of the burner 10B is a zirconia tube. A circular second injection port 22a with a diameter of 20 mm is provided at the tip of the second injection portion 25b. The tip of the second injection portion 25b is 40 mm lower than the tip of the first injection portion 23c in the vertical direction.

[0191] Fullerenes were produced in the same manner as in Example 1, except that the flow rate of toluene as the assist gas was set to 20 g / min and the flow rate of pure oxygen as the second oxygen-containing gas was set to 21 NL / min. Furthermore, the ratio of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas, A2, was 0.81, satisfying the following conditions: 0.30 < A2 (0.81) < A1 (1.31).

[0192] The temperature of the reactor 2 during fullerene production was 1300°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 1.1%.

[0193] (Example 6)

[0194] Fullerenes were produced in the same manner as in Example 4, except that the flow rate of toluene as the assist gas was set to 20 g / min and the flow rate of pure oxygen as the second oxygen-containing gas was set to 25 NL / min. Furthermore, the ratio of the number of carbon atoms in the assist gas supplied to the reactor 2 to the number of oxygen atoms in the second oxygen-containing gas, A2, was 0.68, satisfying the following conditions: 0.30<A2(0.68)<A1(1.31).

[0195] The temperature of the reactor 2 during fullerene production was 1500°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 1.4%.

[0196] (Example 7)

[0197] Use with Figure 6 The fullerene production apparatus 1 having the reactor 2 shown produces fullerene.

[0198] The tip of the second injection portion 25c has Figure 7 The nozzle portion 34a of the second injection section 25c of the burner 10C is made of zirconia. A circular second injection port 22a with a diameter of 8 mm is located at the tip of the nozzle portion 34a. Furthermore, the second injection section 25c has 16 nozzle portions 34a, spaced evenly apart. Vertically, the tip of the second injection section 25c is 40 mm lower than the tip of the first injection section 23c.

[0199] The flow rate of toluene as the auxiliary gas was set to 20 g / min, and the flow rate of pure oxygen as the second oxygen-containing gas was set to 25 NL / min. Other than the above, fullerene was produced in the same manner as in Example 1. In addition, the ratio of the number of carbon atoms of the auxiliary gas supplied to the reaction furnace 2 to the number of oxygen atoms of the second oxygen-containing gas: A2 was 0.68, and 0.30 < A2 (0.68) < Al (1.31).

[0200] The temperature of the reaction furnace 2 at the time of production of fullerene was 1830°C. In addition, under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the coal-like substance produced was recovered from the recovery mechanism 3. In addition, the content ratio of fullerene contained in the recovered coal-like substance was measured using the method described in the above [Calculation of Fullerene], and then the yield of fullerene was calculated. As a result, the yield of fullerene was 1.9%.

[0201] (Example 8)

[0202] A fullerene production apparatus 1 having a reaction furnace 2 as shown in FIG. 1 was used to produce fullerene. Figure 8

[0203] The burner 10D had a second injection port 22a as shown in (A) of FIG. 2. In addition, the second injection port 22a was opened as in (B) of FIG. 2. The second injection portion 25d of the burner 10D was a cylinder made of zirconia, and the inner diameter of the cylinder was 160 mm and the height was 400 mm. On the inner peripheral surface of the second injection portion 25d, 16 second injection ports 22a in the form of slits having a width of 8 mm and a height of 45 mm were arranged at equal distances from each other. In the vertical direction, the upper side of the second injection port 22a in the form of a slit was at the same height as the top end surface of the burner 9D. Figure 9 Figure 10 The flow rate of toluene as the auxiliary gas was set to 20 g / min, and the flow rate of pure oxygen as the second oxygen-containing gas was set to 25 NL / min. Other than the above, fullerene was produced in the same manner as in Example 1. In addition, the ratio of the number of carbon atoms of the auxiliary gas supplied to the reaction furnace 2 to the number of oxygen atoms of the second oxygen-containing gas: A2 was 0.68, and 0.30 < A2 (0.68) < Al (1.31).

[0204] The temperature of the reaction furnace 2 at the time of production of fullerene was 1960°C. In addition, under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the coal-like substance produced was recovered from the recovery mechanism 3. In addition, the content ratio of fullerene contained in the recovered coal-like substance was measured using the method described in the above [Calculation of Fullerene], and then the yield of fullerene was calculated. As a result, the yield of fullerene was 2.2%.

[0205] The temperature of the reaction furnace 2 at the time of production of fullerene was 1960°C. In addition, under the above conditions, the fullerene production apparatus 1 was operated for 3 hours, and the coal-like substance produced was recovered from the recovery mechanism 3. In addition, the content ratio of fullerene contained in the recovered coal-like substance was measured using the method described in the above [Calculation of Fullerene], and then the yield of fullerene was calculated. As a result, the yield of fullerene was 2.2%.

[0206] (Comparative Example 1) ​​

[0207] Fullerene was produced in the same manner as in Example 1 except that the fullerene production apparatus 1 without the burner 10A was used. The ratio A1 of the number of carbon atoms in the raw material gas supplied to the reactor 2 to the number of oxygen atoms in the first oxygen-containing gas was 1.31.

[0208] The temperature of the reactor 2 during fullerene production was 500°C. Furthermore, the fullerene production apparatus 1 was operated for 3 hours under the above conditions, and the generated coal-like material was recovered from the recovery mechanism 3. Furthermore, the fullerene content in the recovered coal-like material was measured using the method described in [Calculation of Fullerenes] above, and the fullerene yield was calculated. The result was a fullerene yield of 0.6%.

[0209] As can be seen from the above, Examples 1 to 7 have improved fullerene yields compared to Comparative Example 1. That is, the fullerene yield can be improved by maintaining the temperature inside the reactor 2 using the second combustion flame.

[0210] Description of Reference Numerals

[0211] 1...Fullerene production apparatus 2...Reaction furnace 3...Recovery mechanism 4...Cooling mechanism 5...Decompression mechanism (vacuum pump) 6...First pipe 7...Second pipe 8...Third pipe 9, 9A to 9D...Burner 10, 10A to 10D...Burner 11...Filter 12...Collector 13...Solenoid valve 14...Tank 15...Discharge valve 16...Discharge passage 21a...First injection port 22a...Second injection port 23...Burner holder 23a...First preheater Mixing chamber 23b... Accumulator chamber 23c... First injection unit 24a... Pipe 24b... Pipes 25a to 25d... Second injection unit 26... Second premixing chamber 27... Connecting pipe 28a... Pipe 28b... Pipe 29... Partition 30... Heat insulating member 31... Ignition mechanism 34, 34a, 34b... Nozzle 35a, 35b... First flowmeter (first flow rate regulator) 36a, 36b... Second flowmeter (second flow rate regulator)

Claims

1. A fullerene production device, characterized in that: have: a reactor for producing fullerenes by incomplete combustion of a raw material gas containing hydrocarbons; a first injection unit configured to inject the raw material gas and the first oxygen-containing gas into the reaction furnace while causing incomplete combustion of the raw material gas to form a first combustion flame; a second injection unit, wherein the second injection unit injects an auxiliary gas containing hydrocarbons that are the same as or different from the raw material gas and a second oxygen-containing gas into the reaction furnace, and burns the auxiliary gas to form a second combustion flame; a first flow rate adjustment unit configured to adjust a ratio A1 of the number of carbon atoms in the raw material gas to the number of oxygen atoms in the first oxygen-containing gas to 0.60 to 2.00, and supply the raw material gas and the first oxygen-containing gas to the first injection unit; as well as The second flow rate adjustment unit adjusts the ratio A2 of the number of carbon atoms in the assist gas to the number of oxygen atoms in the second oxygen-containing gas to 0.30<A2<A1, and supplies the assist gas and the second oxygen-containing gas to the second injection unit.

2. The fullerene production apparatus according to claim 1, wherein One of the first ejecting portion and the second ejecting portion is disposed so as to surround the other ejecting portion.

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

4. The fullerene production apparatus according to claim 1, wherein A partition is provided between the first injection portion and the second injection portion.

5. The fullerene production apparatus according to claim 1, wherein The first injection unit injects the raw material gas from one end side toward the other end side of the reaction furnace. The second injection unit injects the assist gas from a periphery between one end side and the other end side of the reactor.

6. The fullerene production apparatus according to any one of claims 1 to 5, characterized in that: A decompression mechanism is provided for bringing the interior of the reaction furnace into a decompressed state while suctioning the interior of the reaction furnace. 7 . The fullerene production apparatus according to claim 1 , wherein the second injection unit is arranged to surround the first injection unit.

8. A method for producing fullerene, characterized in that: The method comprises the steps of generating fullerenes in a reactor by incomplete combustion of a raw material gas containing hydrocarbons, In the above step, the raw material gas and the first oxygen-containing gas are injected into the reaction furnace while the raw material gas is incompletely combusted to form a first combustion flame, and While injecting an assist gas containing a hydrocarbon that is the same as or different from the raw gas and a second oxygen-containing gas into the reactor, the assist gas is combusted to form a second combustion flame, thereby heating the reactor. The ratio A1 of the number of carbon atoms in the raw material gas to the number of oxygen atoms in the first oxygen-containing gas is set to 0.60 to 2.

00. The ratio A2 of the number of carbon atoms in the assist gas to the number of oxygen atoms in the second oxygen-containing gas is set to 0.30<A2<A1.

9. The method for producing fullerene according to claim 8, wherein: The temperature in the reaction furnace is set to 1000 to 2000°C.

10. The method for producing fullerene according to claim 8 or 9, wherein: In the above step, the inside of the reaction furnace is brought into a reduced pressure state while suction is being applied to the inside of the reaction furnace.

11. The method for producing fullerene according to claim 10, wherein: The pressure in the reaction furnace is set to 1 to 30 kPa. 12 . The method for producing fullerene according to claim 10 , wherein the first combustion flame and the second combustion flame are formed so that the first combustion flame is surrounded by the second combustion flame.

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