JP7359334B2 - Operating method of fullerene production equipment, fullerene production equipment and fullerene production method - Google Patents

Description

The present invention relates to a method of operating a fullerene production device, a fullerene production device, and a fullerene production method.
This application claims priority based on Japanese Patent Application No. 2021-143240 filed in Japan on September 2, 2021, the contents of which are incorporated herein.

As a method for producing fullerene, a combustion method is known in which fullerene is produced by incompletely burning a raw material containing hydrocarbons in a reactor (see, for example, Patent Document 1). Patent Document 1 describes a fullerene in which a hydrocarbon raw material and an oxygen-containing gas are incompletely combusted in a reactor having a cylindrical main body (cylindrical part) and a truncated conical part connected to the lower part of the main body and gradually decreasing in diameter. It describes the manufacturing method of the following types. In the method described in Patent Document 1, a soot-like substance containing fullerene C ₆₀ , fullerene C ₇₀ , and mixed fullerene containing higher fullerenes is continuously recovered from high-temperature gas generated from a reactor. The reactor described in Patent Document 1 has a burner in the upper part of the main body, and the lower end of the truncated cone serves as a discharge part for exhaust gas containing soot.

Japanese Patent Application Publication No. 2005-170695

In the production of fullerene using the combustion method, it is common to continuously supply raw materials containing hydrocarbons and oxygen-containing gas at a constant rate into the reactor equipped in the fullerene production equipment, resulting in incomplete combustion. It is true. The raw materials supplied into the reactor are incompletely combusted within the reactor at a temperature of 1000°C to 2000°C. As a result, a soot-like substance containing fullerene is generated and is discharged from the exhaust port together with the exhaust gas. Most of the soot produced in the reactor is discharged from the exhaust port along with the exhaust gas, and is recovered by a recovery device.

However, when producing fullerene continuously by the combustion method, some of the soot produced in the reactor adheres to the wall of the reactor and remains in the reactor. The thickness of the attached soot increases as the operating time of the fullerene manufacturing equipment increases. If the flow path consisting of the space between the raw material supply means and the discharge port in the reactor is blocked by the thickened soot, incomplete combustion of the raw material may not be able to continue.

Therefore, when producing fullerene continuously by the combustion method, it is necessary to periodically stop the operation of the fullerene production apparatus and perform maintenance work. Maintenance work, for example, involves waiting for the temperature inside the reactor of a production equipment that has stopped operation to drop to room temperature, opening the reactor, and removing soot that has adhered to the walls of the reactor by physical means. Work is underway to remove it. Such maintenance work requires a long time and is labor intensive.

The present invention has been made in view of the above circumstances, and provides a method for operating a fullerene production apparatus that can easily remove soot attached to the walls of a reactor in a short time and that can efficiently produce fullerene by a combustion method. The purpose is to provide
Another object of the present invention is to provide a fullerene manufacturing apparatus used in the operating method of the fullerene manufacturing apparatus of the present invention, and a fullerene manufacturing method using the operating method of the fullerene manufacturing apparatus.

The present invention is a method for operating a fullerene manufacturing apparatus equipped with a reactor that produces soot-like substances containing fullerene, in which raw materials containing hydrocarbons and oxygen-containing gas are supplied into the reactor by a burner, and laminar flow combustion is performed. The soot-like substance forming step in which the raw material is incompletely combusted under the condition of To provide an excellent method for operating a fullerene manufacturing apparatus, which includes a soot-like material removal step for removing soot-like substances.
That is, the first aspect of the present invention is the following method of operating a fullerene production apparatus.
[1] A method for operating a fullerene production device comprising a reactor that produces soot-like material containing fullerene,
A soot-like substance production step of supplying a raw material containing a hydrocarbon and an oxygen-containing gas into the reactor using a burner, and causing incomplete combustion of the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene. and,
After the soot production step, the volume of gas in the reactor is rapidly expanded to generate a pressure wave, and the generated pressure wave causes the reactor to absorb the gas generated in the soot production step. A method for operating a fullerene manufacturing apparatus, comprising a soot-like material removal step of removing the soot-like material adhering to a wall.
In addition, in the operating method of the first aspect of the present invention, it is also preferable that the generated soot is sent to the outside of the reactor in the soot-like generation step.

The operating method of the fullerene production apparatus according to the first aspect of the present invention can preferably include the following features. Two or more of the following features may be preferably combined.
[2] In the soot removal step, at least one of the raw material and the oxygen-containing gas is continuously supplied into the reactor from the soot production step, and the supplied raw material and the oxygen-containing gas are The method for operating a fullerene production apparatus according to [1], wherein the supply amount of at least one of the above is made larger than the supply amount in the soot-like product generation step, and the volume of the gas in the reactor is rapidly expanded. .
[3] In the soot removal step, the feed rate (g/min) of the raw material is 1.5 to 5.0 times the feed rate (g/min) of the raw material in the soot generation step. , the method for operating the fullerene production apparatus according to [2].

[4] In the soot-like substance removal step, the supply amount (NL/min) of the oxygen-containing gas is set to 1.5 to 5. The method for operating a fullerene production apparatus according to [2] or [3], wherein the fullerene manufacturing apparatus is increased to 0 times.
[5] In the soot-like substance removal step, the time for increasing the supply amount of at least one of the raw material and the oxygen-containing gas is 0.5 seconds to 5.0 seconds, [2] to [4] ] The method of operating the fullerene production apparatus according to any one of the above.

[6] In the soot removal step, an inert gas is supplied to the burner or near the discharge part of the burner disposed in the reactor to rapidly expand the volume of gas in the reactor. , a method for operating the fullerene production apparatus according to [1].
[7] In the soot removal step, the inert gas supply amount (NL/min) is 1.5 to 5. The operating method of the fullerene production apparatus according to [6], which is 0 times.
[8] The method for operating a fullerene production apparatus according to [6] or [7], wherein in the soot-like substance removal step, the inert gas is supplied for 0.5 seconds to 5.0 seconds.

[9] The soot removal step includes an extinguishing step of extinguishing the flame in the laminar combustion state generated in the soot generation step;
The method for operating a fullerene manufacturing apparatus according to [1], further comprising a re-ignition step of igniting the raw material in the reactor after the flame-extinguishing step.
[10] The extinguishing step is a step of stopping the supply of the raw material,
The method for operating a fullerene manufacturing apparatus according to [9], wherein the re-ignition step is a step of supplying the raw material into the reactor.

The second aspect of the present invention is the following fullerene production apparatus.
[11] A fullerene production device used in the method for operating the fullerene production device according to any one of [1] to [10],
A reactor that has a burner that supplies a raw material containing hydrocarbons and an oxygen-containing gas, and incompletely burns the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene;
A fullerene production apparatus comprising: pressure wave generating means for rapidly expanding the volume of gas in the reactor to generate pressure waves that remove the soot-like substances adhering to the wall of the reactor. .

The fullerene production apparatus according to the second aspect of the present invention can preferably include the following features. Two or more of the following features may be preferably combined.
[12] The pressure wave generating means may set the feed rate (g/min) of the raw material to 1.5 g/min of the feed rate (g/min) when the raw material is incompletely combusted in the laminar flow combustion state. The fullerene production apparatus according to [11], which has a supply control means that increases the amount by 5 to 5.0 times.
[13] The pressure wave generating means is configured to set the supply amount (NL/min) of the oxygen-containing gas to the supply amount (NL/min) of the oxygen-containing gas when the raw material is incompletely combusted in the laminar flow combustion state. ) The fullerene production apparatus according to [11] or [12], which has a supply control means that increases the amount by 1.5 to 5.0 times.

[14] The pressure wave generating means rapidly expands the volume of gas in the reactor by supplying an inert gas to the burner or near the discharge part of the burner disposed in the reactor. The fullerene production apparatus according to [11], which has an inert gas supply means. [15] The pressure wave generating means includes extinguishing means for extinguishing the flame in the laminar combustion state;
The fullerene manufacturing apparatus according to [11], further comprising a re-ignition means for igniting the raw material in the reactor.
[16] The extinguishing means is a means for stopping the supply of the raw material,
The fullerene manufacturing apparatus according to [15], wherein the re-ignition means is a means for supplying the raw material into the reactor.

The third aspect of the present invention is the following method for producing fullerene.
[17] A fullerene production method using the operating method of the fullerene production apparatus according to any one of [1] to [10],
A soot-like product generation step in which a raw material containing hydrocarbons and an oxygen-containing gas are supplied into the reactor using a burner, and the raw materials are incompletely combusted in a laminar flow combustion state to produce a soot-like product containing fullerene. ,
a soot-like matter removing step of removing soot-like matter containing the fullerene adhering to the wall of the reactor using pressure waves generated by rapidly expanding the volume of gas in the reactor. , fullerene production method.
The method for producing fullerene according to the third aspect of the present invention provides a method for producing fullerene from the soot containing the fullerene produced in the soot production step and the soot removed in the soot removal step. It is also preferable to include a step of recovering.

The operating method of the fullerene production apparatus of the present invention includes a soot-forming step in which a raw material containing hydrocarbons and an oxygen-containing gas are supplied into a reactor using a burner, and the raw materials are incompletely combusted in a laminar combustion state; The method includes a soot removal step of removing the soot adhering to the wall of the reactor using pressure waves generated by rapidly expanding the volume of gas in the reactor. Therefore, even if soot adheres to the wall of the reactor by performing the soot generation step, the soot adhered to the wall of the reactor can be removed by performing the soot removal step. can be easily removed in a short time. Therefore, by using the operating method of the fullerene production apparatus of the present invention, fullerene can be efficiently produced by the combustion method.

The fullerene production apparatus of the present invention has a burner that supplies a raw material containing hydrocarbons and an oxygen-containing gas, and a reactor that incompletely burns the raw material in a laminar combustion state to produce soot containing fullerene. and pressure wave generating means for generating pressure waves that rapidly expand the volume of gas in the reactor and remove the soot-like substances adhering to the walls of the reactor. Therefore, the fullerene manufacturing apparatus of the present invention can easily remove soot attached to the reactor wall in a short time by performing the soot-like matter removal step using the operating method of the present invention. Fullerene can be produced efficiently using the combustion method.

In the fullerene production method of the present invention, since the operating method of the fullerene production apparatus of the present invention is used, even if soot is attached to the wall of the reactor, the soot attached to the wall of the reactor may be removed. can be easily removed in a short time. Therefore, by using the fullerene production method of the present invention, fullerene can be efficiently produced by the combustion method.
In the present invention, the term "means" may mean an apparatus, a process, a method, a member, a part, a mechanism, or the like.

BRIEF DESCRIPTION OF THE DRAWINGS It is a block diagram which shows an example of the fullerene manufacturing apparatus based on 1st Embodiment of this invention. FIG. 2 is a drawing for explaining a state in which soot-like substances 15 adhere to a reactor 11 when fullerene is produced using the fullerene production apparatus 10 shown in FIG. 1. FIG. It is a block diagram which shows an example of the fullerene manufacturing apparatus based on 2nd Embodiment of this invention. 4 is a drawing for explaining a state in which soot-like substances 15 adhere to inside a reactor 11 when fullerene is manufactured using the fullerene manufacturing apparatus 40 shown in FIG. 3. FIG.

The present inventors conducted extensive studies to solve the above problems.
As a result, after producing soot containing fullerene in the reactor, the pressure waves generated by rapidly expanding the volume of gas in the reactor caused soot to adhere to the walls of the reactor. They discovered that it is sufficient to remove the material, and came up with the present invention.

Hereinafter, preferred examples of the operating method of the fullerene production apparatus, the fullerene production apparatus, and the fullerene production method of the present invention will be described in detail with reference to the drawings. Note that the present invention is not limited only to the embodiments shown below. The drawings used in the following explanation may schematically show characteristic parts for convenience in order to make the features of the present invention easier to understand, and the dimensional ratio of each component may not be the same as the actual one. Not exclusively. Within the scope of the present invention, numbers, positions, orders, combinations, types, amounts, strengths, times, ratios, numerical values, sizes, etc. may be omitted, changed, and/or added as necessary. It is.

(First embodiment)
[Fullerene production equipment]
FIG. 1 is a configuration diagram showing an example of a fullerene manufacturing apparatus according to a first embodiment of the present invention. The fullerene manufacturing apparatus 10 of this embodiment can be suitably used when fullerene is continuously manufactured by a combustion method. As shown in FIG. 1, the fullerene manufacturing apparatus 10 of this embodiment includes a reactor 11, piping 19, a fullerene recovery mechanism 16, a cooling mechanism 17, and a pressure reducing device 18. FIG. 2 shows a state in which soot-like material 15 is attached to the wall of the reactor 11 as a result of producing fullerene using the fullerene production apparatus 10 shown in FIG.

In the reactor 11, a raw material contained in a mixed gas of a raw material containing a hydrocarbon and an oxygen-containing gas is incompletely combusted in a laminar combustion state to generate a soot-like substance containing fullerene. Examples of the fullerenes to be produced include higher-order fullerenes such as C ₆₀ fullerene (C ₆₀ ), C ₇₀ fullerene (C ₇₀ ), C ₇₆ , C ₇₈ , C ₈₄ , C ₉₀ , and C ₉₆ . Incomplete combustion of raw materials produces exhaust gas containing carbon monoxide, carbon dioxide, water vapor, etc. as well as soot containing fullerenes. Note that the laminar combustion state may mean a state in which combustion is occurring in a laminar flow and there is no turbulence in the flame front. Moreover, incomplete combustion may mean combustion in a state of insufficient oxygen.

The reactor 11 is preferably cylindrical, more preferably cylindrical.
In the fullerene manufacturing apparatus 10 shown in FIG. 1, a burner 13 for spewing raw materials and oxygen-containing gas into the reactor 11 is installed at the first end (the upper end in FIG. 1) of the cylindrical reactor 11. It is located. Further, an exhaust port 12 is provided at the second end (lower end in FIG. 1) of the reactor 11 to discharge exhaust gas containing soot generated within the reactor 11. The space between the burner 13 and the discharge port 12 in the reactor 11 is a flow path through which raw materials and exhaust gas containing soot containing fullerene produced by incomplete combustion of the raw materials pass.

When the reactor 11 is cylindrical, it is preferably arranged so that the length direction is substantially vertical, as shown in FIG. In this case, the generated soot is less likely to remain in the reactor 11 . In addition, by performing the soot-like material removal process described later, the soot-like material separated from the furnace wall of the reactor 11 is efficiently discharged from the discharge port 12.

The reactor 11 shown in FIG. 1 may be arranged, for example, so that the length direction is horizontal, or it may be arranged obliquely with respect to the vertical direction, depending on the situation of the place where it is installed. It may be placed in

When the reactor 11 is cylindrical, the inner diameter D1 of the reactor 11 is preferably 50 mm to 500 mm, more preferably 50 mm to 300 mm. When the inner diameter D1 of the reactor 11 is 50 mm or more, even if soot containing fullerene adheres to the wall of the reactor 11, the flow inside the reactor 11 can be prevented by performing the soot-like production step described below. The road is less likely to be blocked in a short time. For this reason, the soot-like substance production process described below can be performed continuously for a long time, the time until the soot-like substance removal process is performed, and fullerene can be produced more efficiently. Further, when the inner diameter D1 of the reactor 11 is 500 mm or less, the soot 15 adhering to the furnace wall can be efficiently removed by pressure waves generated in the soot removal process described below.

When the inner diameter D1 of the reactor 11 is 50 mm to 500 mm, the length L of the reactor 11 is preferably 500 mm to 3000 mm, more preferably 1000 mm to 2000 mm. When the length L of the reactor 11 is 500 mm or more, a sufficient volume within the reactor 11 can be secured. Therefore, in the soot-like substance removal process described later, it is possible to suppress the change in the pressure inside the reactor 11 from becoming too large due to the rapid expansion of the volume of the gas inside the reactor 11, resulting in excellent safety. In addition, when the length L of the reactor 11 is 3000 mm or less, the soot 15 adhering to the wall of the reactor 11 can be efficiently removed by performing the soot removal process described below. , maintenance becomes easier.

Examples of materials for the reactor 11 include zirconia (ZrO ₂ ), tungsten (W), tantalum (Ta), platinum (Pt), titanium (Ti), titanium nitride (TiN), alumina (Al ₂ O ₃ ), A material with excellent heat resistance such as silicon carbide (SiC) can be used.
As shown in FIG. 1, a heat insulating layer 14 is preferably provided on the outer surface of the reactor 11 so as to cover part or all of the outer surface of the reactor 11. As the material for the heat insulating layer 14, for example, an alumina refractory brick, an alumina amorphous refractory material, or the like can be used.

A raw material supply pipe 20 and an oxygen-containing gas supply pipe 21 are connected to a burner 13 arranged in the reactor 11 via a flashback prevention device (not shown). As the flashback prevention device, a known device can be used. The raw material supply pipe 20 supplies a raw material containing hydrocarbons to the reactor 11 via the burner 13 . The oxygen-containing gas supply pipe 21 supplies oxygen-containing gas used for combustion of raw materials to the reactor 11 via the burner 13.

The raw material supply pipe 20 is provided with a raw material supply control means 20a (supply control means) that controls the amount of raw material supplied, and a heating device (not shown) that vaporizes the raw material gas. Note that the raw material supply control means 20a may also mean a device, process, member, part, mechanism, etc. that performs raw material supply control. The heating device is provided between the raw material supply control means 20a and the burner 13. The oxygen-containing gas supply pipe 21 is provided with an oxygen-containing gas supply control means 21a (supply control means) that controls the supply amount of the oxygen-containing gas. Note that the supply control means 21a may mean a device, process, member, part, mechanism, etc. that controls the supply of oxygen-containing gas.

The raw material supply control means 20a changes the raw material supply amount (g/min) to the raw material supply amount (g/min) used when the raw material is incompletely combusted in a laminar flow combustion state (hereinafter also referred to as "soot-like substance generation step"). In addition to being able to adjust the amount (g/min), it is also possible to increase the feed rate (g/min) of the raw material for the soot production step. In particular, it is preferable that the raw material supply control means 20a is capable of adjusting the raw material supply rate (g/min) to 1.5 to 5.0 times the raw material supply rate (g/min) for the soot production step. Specifically, an example of the raw material supply control means 20a is a commercially available mass flow controller that satisfies the above conditions.

The oxygen-containing gas supply control means 21a can adjust the supply amount (NL/min) of the oxygen-containing gas to the supply amount (NL/min) of the oxygen-containing gas used in the soot-forming process, and can also control the soot-forming process. It can also be made larger than the supply amount (NL/min) of oxygen-containing gas in the process. In particular, the oxygen-containing gas supply control means 21a increases the supply amount (NL/min) of the oxygen-containing gas to 1.5 to 5.0 times the supply amount (NL/min) of the oxygen-containing gas in the soot production step. Preferably one that can be adjusted. Specifically, a commercially available mass flow controller that satisfies the above conditions can be cited as an example. Here, NL/min is normal liter/min, and represents the volume of gas supplied per minute under standard conditions (pressure 0.1013 MPa, temperature 0° C., humidity 0%).
The piping from the raw material supply control means 20a to the mixing chamber 13a and the piping from the oxygen-containing gas supply control means 21a to the mixing chamber 13a may or may not be connected before entering the mixing chamber 13a. .

The burner 13 includes a mixing chamber 13a that mixes a raw material and an oxygen-containing gas to produce a mixed gas, a pressure accumulation chamber 13b that holds the mixed gas at a predetermined pressure, and a discharge port for discharging the pressure of the mixed gas accumulated in the pressure accumulation chamber 13b. 12 (downward in FIG. 1). The burner 13 may have a configuration in which the mixing chamber 13a is omitted.

The ratio of the raw material and oxygen-containing gas contained in the mixed gas produced in the mixing chamber 13a is determined by the amount of raw material supplied to the burner 13 and the amount of oxygen-containing gas supplied. The amount of raw material supplied is controlled by the raw material supply control means 20a. The supply amount of the oxygen-containing gas is controlled by the oxygen-containing gas supply control means 21a.

The supply amount of the mixed gas jetted into the reactor 11 from the discharge part 13c of the burner 13 can be controlled by the supply amount of the raw material supplied to the burner 13 and the supply amount of the oxygen-containing gas.

Various forms can be used as the discharge part 13c. As the discharge part 13c, for example, one having a plurality of discharge ports made of a porous ceramic sintered body, a metal powder sintered body, etc. can be used.
The planar shape of the discharge portion 13c may be circular or polygonal in plan view. Since the discharge part 13c can discharge the mixed gas more uniformly into the reactor 11, it is preferable that its external shape is similar to the shape of the inner wall surface of the reactor 11. Specifically, the shape of the inner wall surface of the reactor 11 and the outer shape of the discharge portion 13c are preferably circular in plan view.

When the shape of the inner wall surface of the reactor 11 and the external shape of the discharge part 13c are circular in plan view, the diameter D2 of the discharge part 13c is preferably 30 mm to 400 mm, more preferably 40 mm to 350 mm. . When the diameter D2 of the discharge part 13c is 30 mm to 400 mm, the ratio of the inner diameter D1 of the reactor 11 to the diameter D2 of the discharge part 13c (inner diameter D1 of the reactor 11/diameter D2 of the discharge part 13c) is within a preferable range. Cheap.

The ratio between the inner diameter D1 of the reactor 11 and the diameter D2 of the discharge portion 13c is preferably 1.05 to 2.00, more preferably 1.10 to 1.50. When the ratio between the inner diameter D1 of the reactor 11 and the diameter D2 of the discharge part 13c is 1.05 or more, soot 15 is difficult to accumulate around the discharge part 13c in the soot production step described below. Furthermore, if the ratio between the inner diameter D1 of the reactor 11 and the diameter D2 of the discharge portion 13c is 2.00 or less, the soot 15 containing fullerene will be efficiently generated in the soot generation step described below. Productivity is improved.

The discharge portion 13c is preferably provided with a large number of discharge ports having a small opening area. As such a discharge part 13c, for example, one having a large number of discharge ports each having a diameter of 0.1 mm to 5 mm and having a substantially circular shape in a plan view can be mentioned. When the discharge part 13c is provided with a large number of discharge ports having a small opening area, the ratio of the total opening area of the discharge ports to the area of the discharge part 13c is preferably 10% to 95%. It is preferably 50% to 95%.

An ignition mechanism 31 is provided near the outlet 12 of the reactor 11 . The ignition mechanism 31 ignites the raw material and causes incomplete combustion to produce fullerene. As the ignition mechanism 31, an ignition device commonly used in combustion equipment such as a combustion furnace can be used. In particular, it is preferable to use a pressure-resistant and explosion-proof ignition device. The conditions for ignition by the ignition mechanism 31 can be arbitrarily selected.

In the fullerene manufacturing apparatus 10 of the present embodiment, by controlling the raw material supply control means 20a and the oxygen-containing gas supply control means 21a, the raw material is incompletely burnt in a laminar flow state in the soot production process described later. In addition, in the soot removal process, pressure waves are generated to rapidly expand the volume of gas in the reactor 11 and remove soot 15 adhering to the walls of the reactor 11. It can also be generated.

Therefore, in the fullerene manufacturing apparatus 10 of this embodiment, the raw material supply control means 20a and the oxygen-containing gas supply control means 21a function as supply control means for the pressure wave generation means. The pressure wave generating means may mean a device, process, member, part, mechanism, etc. that generates pressure waves.
The pressure wave generating means controls the raw material supply control means 20a and the oxygen-containing gas supply control means 21a, and controls at least the raw material supply amount (g/min) and the oxygen-containing gas supply amount (NL/min). By increasing one side more than when the raw material is incompletely combusted in a laminar flow combustion state, the volume of gas in the reactor 11 can be rapidly expanded.

The pressure wave generating means controls the raw material supply control means 20a to adjust the raw material supply amount (g/min) to 1.5 to 1.5 of the raw material supply amount (g/min) when the raw material is incompletely combusted in a laminar flow combustion state. It is preferable that it can be increased by 5.0 times. The magnification may be 2.0 to 5.0 times, 1.8 to 4.0 times, 2.0 to 3.0 times, etc., as necessary.

The pressure wave generating means also controls the oxygen-containing gas supply control means 21a to adjust the supply amount (NL/min) of the oxygen-containing gas to the supply amount (NL/min) of the oxygen-containing gas when the raw material is incompletely combusted in a laminar flow combustion state. /min) is preferably 1.5 to 5.0 times. The magnification may be 2.0 to 5.0 times, 1.8 to 4.0 times, 2.0 to 3.0 times, etc., as necessary.

Note that the pressure wave generating means is controlled by the raw material supply control means 20a to adjust the raw material supply rate (g/min) to 1. 5 to 5.0 times, and the oxygen-containing gas supply control means 21a changes the supply amount (NL/min) of oxygen-containing gas to the amount of oxygen-containing gas supplied when the raw material is incompletely combusted in a laminar flow combustion state. It is also preferable to be able to increase the speed by 1.5 to 5.0 times (NL/min).

The fullerene manufacturing apparatus 10 of this embodiment includes, as a pressure wave generating means, a flame extinguishing means for extinguishing a flame in a laminar flow combustion state, and a re-ignition means for igniting the raw material in the reactor 11 after the flame is extinguished. Good too. In this case, after the flame is extinguished, the raw material is ignited within the reactor 11 by the re-ignition means, so that the volume of the gas within the reactor 11 rapidly expands and pressure waves are generated. The flame extinguishing means may mean a device, process, member, part, mechanism, etc. that extinguishes flame. The re-ignition means may mean a device, process, member, part, mechanism, etc. that performs re-ignition.

The extinguishing means is not particularly limited, but includes means for controlling the supply amount of the raw material and the oxygen-containing gas so that the flame in the laminar flow combustion state is extinguished. For example, means for stopping at least one of the supply of raw materials and the supply of oxygen gas can be mentioned. Preferably, the extinguishing means is a means for stopping the supply of raw materials.
Therefore, in the fullerene manufacturing apparatus 10 of this embodiment, the raw material supply control means 20a and the oxygen-containing gas supply control means 21a can function as a flame extinguishing means for the pressure wave generation means.

An example of the re-ignition means is a means for supplying the raw material and/or oxygen-containing gas into the reactor 11 after the flame has been extinguished. Specifically, as the re-ignition means, there is a means for supplying raw material and oxygen-containing gas into the reactor 11 in the same amount as in the laminar flow combustion state before the flame is extinguished, after the flame is extinguished by the flame extinguishing means. The re-ignition means may further include an ignition mechanism 31.
Therefore, in the fullerene manufacturing apparatus 10 of the present embodiment, the raw material supply control means 20a, the oxygen-containing gas supply control means 21a, and, if necessary, the ignition mechanism 31 function as a re-ignition means for the pressure wave generation means. can do.

Piping 19 supplies exhaust gas containing soot generated within reactor 11 to collector 29 of fullerene recovery mechanism 16 . As shown in FIG. 1, the piping 19 has a first end connected to the outlet 12 of the reactor 11, and a second end connected to the upper side of the collector 29 of the fullerene recovery mechanism 16. There is.
As the piping 19, a publicly known piping can be used. Specifically, as the piping 19, for example, a pipe made of stainless steel or the like can be used. The inner diameter of the pipe 19 can be appropriately determined depending on the inner diameter of the reactor 11 and the amount of exhaust gas containing the soot-like material 15 discharged from the reactor 11. Further, the length of the pipe 19 can be determined as appropriate depending on the distance between the reactor 11 and the fullerene recovery mechanism 16, etc.

The fullerene recovery mechanism 16 recovers soot from the exhaust gas containing the soot generated in the reactor 11 . The fullerene recovery mechanism 16 includes a collector 29 containing a filter 22, a tank 24 connected via a pipe 23 connected to the upper end (one end) of the collector 29, and an electromagnetic collector provided in the pipe 23. It has a valve 25 and a discharge valve 26 provided at the lower end (other end) side of the collector 29. As will be described later, the solenoid valve 25 can be opened periodically at a favorable timing. By injecting the inert gas in the tank 24 toward the collector 29, the soot attached to the filter 22 can be dropped and deposited on the bottom of the collector 29. The soot can be collected by opening the discharge valve 26 of 29.

As the filter 22, for example, one made of sintered metal can be used. The tank 24 stores high-pressure inert gas such as nitrogen gas (N ₂ ) and argon gas (Ar). The solenoid valve 25 supplies the inert gas stored in the tank 24 to the collector 29 at a predetermined supply amount. As the electromagnetic valve 25, a known one can be used.

The pipe 27 is provided with a valve. The first end of the pipe 27 is connected to the pipe 23 connected to the upper end of the collector 29, as shown in FIG. A second end of the pipe 27 is connected to one end (upper end) of the cooling mechanism 17 . As the pipe 27, a known pipe can be used.

The cooling mechanism 17 cools the exhaust gas that passes through the fullerene recovery mechanism 16 and is supplied via the pipes 23 and 27. As the cooling mechanism 17, for example, one having the same or similar structure to the heat exchanger can be used. A drain 28 is provided on the side surface of the cooling mechanism 17 on the other end (lower end) side. The drain 28 discharges the components liquefied by passing through the cooling mechanism 17.

As shown in FIG. 1, the piping 30 has a first end connected to the other end (lower end) of the cooling mechanism 17, and a second end connected to the pressure reducing device 18. As the piping 30, a publicly known piping can be used.
The pressure reducing device 18 consists of a vacuum pump. The pressure reducing device 18 sucks the exhaust gas cooled by the cooling mechanism 17 through the pipe 30, generates negative pressure between the pressure reducing device 18 and the reactor 11, and brings the inside of the reactor 11 into a reduced pressure state.

[How to operate fullerene production equipment, fullerene production method]
Next, as an example of the operating method of the fullerene producing apparatus and the fullerene producing method of the present invention, the operating method of the fullerene producing apparatus 10 shown in FIG. 1 and the fullerene producing method using this operating method will be described.
The fullerene manufacturing method of this embodiment is a method of manufacturing fullerene by a combustion method. The operating method of the fullerene manufacturing apparatus and the fullerene manufacturing method of the present embodiment include a soot-like material generation step and a soot-like material removal step. It is preferable that the soot-like material generation step and the soot-like material removal step are performed alternately and repeatedly. In this case, fullerene can be produced even more efficiently. The number of repetitions can be selected arbitrarily.

The soot-like material generation step and the soot-like material removal step in this embodiment are performed by suctioning exhaust gas by the pressure reducing device 18 via the pipe 19, the fullerene recovery mechanism 16, the pipes 23, 27, the cooling mechanism 17, and the pipe 30. It is preferable to carry out the reaction in a state where a negative pressure is generated between the pressure reducing device 18 and the reactor 11.

(Soot-like substance generation process)
In the soot-like substance generation step, a raw material in a mixed gas containing a raw material and an oxygen-containing gas is incompletely combusted in a laminar combustion state in the reactor 11 to generate a soot-like substance containing fullerene.

Examples of hydrocarbons contained in the raw materials used in the soot production step and the soot removal step described below include those having 6 to 15 carbon atoms, such as toluene, benzene, xylene, naphthalene, methylnaphthalene, anthracene, and phenanthrene. Examples include aromatic hydrocarbons, coal hydrocarbons such as creosote oil and carboxylic acid oil, acetylenically unsaturated hydrocarbons, ethylene hydrocarbons, and aliphatic saturated hydrocarbons such as pentane and hexane. Among these, it is preferable to use aromatic hydrocarbons, and it is particularly preferable to use toluene because fullerene can be produced efficiently. As the hydrocarbon, only one type of these may be used, or two or more types may be used in combination.

The raw material may be supplied to the burner 13 in a liquid state, or may be supplied to the burner 13 in a vaporized state by a heating device or the like. It is preferable that the raw material is supplied to the burner 13 in a vaporized state by a heating device so that it can sufficiently contact the oxygen-containing gas. The vaporized raw material may be diluted with an inert gas such as nitrogen gas or argon gas, if necessary.

Examples of the oxygen-containing gas used in the soot production step and the soot removal step described below include oxygen gas, air, and the like. As the oxygen-containing gas, it is particularly preferable to use oxygen gas because fullerene can be produced efficiently. Further, the oxygen-containing gas may be diluted with an inert gas such as nitrogen gas or argon gas, if necessary.

In the soot-like substance generation step of the present embodiment, the raw material supply control means 20a and the oxygen-containing gas supply control means 21a are controlled respectively to produce a mixed gas containing a raw material containing hydrocarbons and an oxygen-containing gas at a predetermined ratio. is injected into the reactor 11 from the burner 13 at a predetermined supply amount. The raw material contained in the mixed gas supplied from the burner 13 is ignited by the ignition mechanism 31 and is incompletely combusted in a laminar combustion state. As a result, exhaust gas containing carbon monoxide, carbon dioxide, water vapor, etc. is generated along with soot containing fullerene.

The feed rate (g/min) of the raw material is preferably 10 to 40 g/min, more preferably 10 to 30 g/min, even more preferably 10 to 20 g/min. The amount may be 12 to 18 g/min, 14 to 16 g/min, etc., as necessary. The supply amount (NL/min) of the oxygen-containing gas is adjusted depending on the type and supply amount of the raw material. The ratio between the number of carbon atoms in the raw material and the number of oxygen atoms in the oxygen-containing gas supplied to the burner 13 per minute is preferably 0.60 to 1.60, and preferably 0.80 to 1.40. is more preferable. If necessary, it may be 0.90 to 1.30, 1.00 to 1.20, etc. When the above ratio is within the above range, the yield of fullerene will be high.

The pressure of the mixed gas in the pressure accumulation chamber 13b of the burner 13 is preferably 6 kPa to 27 kPa, more preferably 8 kPa to 24 kPa, and even more preferably 10 kPa to 20 kPa. The pressure may be 6 kPa to 15 kPa, 8 kPa to 13 kPa, etc., as necessary.

The pressure inside the reactor 11 in the soot production step is preferably 1 kPa to 20 kPa, more preferably 1 kPa to 15 kPa, and even more preferably 1 to 10 kPa. The pressure may be 2 to 8 kPa, 4 to 6 kPa, etc., as necessary. It is preferable that the pressure inside the reactor 11 is 1 kPa or more, since it is possible to prevent the load on the vacuum pump of the pressure reducing device 18 from becoming excessively large, and the life of the vacuum pump is extended. When the pressure inside the reactor 11 is 20 kPa or less, backfire can be prevented from occurring in the soot-forming process, resulting in excellent safety.

In the soot production step, the temperature inside the reactor 11 when performing incomplete combustion of the raw material is preferably 1000°C to 2000°C, preferably 1200°C to 1950°C, and preferably 1300°C to 1900°C. It is more preferable that the temperature is ℃. The temperature may be 1400° C. to 1800° C., 1500° C. to 1700° C., etc., as necessary. When the temperature inside the reactor 11 is 1000° C. or higher, soot-like substances containing fullerene are efficiently generated, and the yield of fullerene becomes good. When the temperature inside the reactor 11 is 2000° C. or less, a large amount of energy is not required to raise the temperature inside the reactor 11, and fullerene can be efficiently produced. The temperature inside the reactor 11 can be measured with an ultra-high temperature thermocouple or a radiation thermometer.

In the soot production step, exhaust gas containing soot containing fullerene produced in the reactor 11 is sucked into the pressure reducing device 18 and discharged from the outlet 12 of the reactor 11 . The soot containing fullerene is collected by a collector 29. At this time, a part of the soot generated in the reactor 11 adheres to the wall of the reactor 11 and remains within the reactor 11 . The thickness of the soot 15 (see FIG. 2) attached to the wall of the reactor 11 gradually increases over time after the soot production process is started. Therefore, the thickness of the soot 15 attached to the wall of the reactor 11 becomes thicker as the time from the start of the soot production process to the end of the soot production process is longer.

(Soot removal process)
In the soot removal step, which removes soot from the inner wall of the reactor 11, pressure waves generated by rapidly expanding the volume of gas within the reactor 11 cause soot to be removed from the wall of the reactor 11. Remove the soot-like material 15 (see FIG. 2). The removed soot is collected by a collector 29. The pressure waves generated in the soot removal step collide with the wall of the reactor 11, and the soot 15 adhering to the wall of the reactor 11 is peeled off from the wall and removed. The gas in the reactor 11 may be composed of any gas that can exist in the reactor 11, such as raw materials, oxygen-containing gas, carbon monoxide generated by combustion of the raw materials, carbon dioxide, water vapor, etc. , is a mixed gas. In the soot removal step, the raw material and oxygen-containing gas may be continuously supplied into the reactor from the soot production step, or at least one of the raw material and the oxygen-containing gas may be supplied. It may also include a sub-step that is stopped.

First, a description will be given of an example of the soot-like material removal process in a case where the raw material supply control means 20a and the oxygen-containing gas supply control means 21a function as supply control means for the pressure wave generation means.

First, an example in which only the supply amount of raw materials is changed will be explained. In the soot removal process, only the feed rate (g/min) of the raw material is made larger than in the soot production process, so that the volume of gas in the reactor 11 is rapidly expanded. Then, a pressure wave of sufficient strength is generated to efficiently remove the soot-like material 15 adhering to the wall of the reactor 11. In this case, it is preferable that the feed rate (g/min) of the raw material is 1.5 to 5.0 times the feed rate (g/min) of the raw material in the soot production step, and 2.0 to 5.0 times. More preferably, it is doubled. When the amount of raw material supplied is 1.5 times or more the soot production step, the volume of gas in the reactor 11 expands at a sufficiently high rate. Therefore, it is possible to generate a pressure wave having sufficient strength to efficiently remove the soot-like material 15 adhering to the wall of the reactor 11. If the feed rate (g/min) of the raw material is 5.0 times or less than the soot production step, the volume of gas in the reactor 11 will expand too quickly and the generated pressure waves will become too strong. can be suppressed. Further, in the soot removal step, the supply amount (NL/min) of the oxygen-containing gas may be the same as the supply amount (NL/min) of the oxygen-containing gas in the soot production step, or at least Good, but preferably similar.

An example of changing only the supply amount of oxygen-containing gas will be explained. In the soot removal process, only the supply amount (NL/min) of the oxygen-containing gas is made larger than in the soot production process, thereby rapidly expanding the volume of gas in the reactor 11. Then, a pressure wave of sufficient strength is generated to efficiently remove the soot-like material 15 adhering to the wall of the reactor 11. In this case, it is preferable that the supply amount (NL/min) of the oxygen-containing gas be 1.5 to 5.0 times the supply amount (NL/min) of the oxygen-containing gas in the soot production step, and 2.0 It is more preferable to increase the amount by 5.0 times. When the supply amount (NL/min) of the oxygen-containing gas is 1.5 times or more the soot production step, the volume of the gas in the reactor 11 expands at a sufficiently fast rate. Therefore, it is possible to generate a pressure wave having sufficient strength to efficiently remove the soot-like material 15 adhering to the wall of the reactor 11. If the supply amount (NL/min) of the oxygen-containing gas is 5.0 times or less than the soot production process, the volume of the gas in the reactor 11 will expand too quickly and the generated pressure waves will be strong. You can prevent it from becoming too much. In addition, in the soot-like substance removal process, the feed rate (g/min) of the raw material may be the same as or less than the feed rate (g/min) of the raw material in the soot-like substance generation process; It is preferable that

An example of changing both the supply amount of raw materials and the supply amount of oxygen-containing gas will be described. In the soot-like substance removal process, the feed rate (g/min) of the raw material and the supply rate (NL/min) of the oxygen-containing gas are each made larger than in the soot-like substance generation process. This rapidly expands the volume of gas within the reactor 11 and generates pressure waves strong enough to efficiently remove soot 15 adhering to the walls of the reactor 11. In this case, it is preferable that the feed rate of the raw material (g/min) and the feed rate of the oxygen-containing gas (NL/min) are each 1.5 to 5.0 times the feed rate of the soot production step. , more preferably 1.5 to 3.0 times. When the supply amount of the raw material and oxygen-containing gas is within the above range, the volume of the gas in the reactor 11 expands at a sufficiently fast rate, so that the soot 15 attached to the wall of the reactor 11 is removed. A pressure wave having sufficient strength to efficiently remove the soot is generated, and the soot 15 attached to the wall of the reactor 11 can be effectively removed.

The time for increasing the supply amount of at least one of the raw material and the oxygen-containing gas (supply time) can be arbitrarily selected, but is preferably 0.5 seconds to 5.0 seconds, and preferably 2.0 seconds to 5.0 seconds. It is more preferable that It is preferable that the time for increasing the supply amount of at least one of the raw material and the oxygen-containing gas is 0.5 seconds or more, since this facilitates generation of sufficient pressure waves to remove soot-like substances adhering to the furnace wall. When the time for increasing the supply amount of at least one of the raw material and the oxygen-containing gas is 5.0 seconds or less, the volumetric expansion of the gas does not occur more than necessary, and safety is excellent.

Next, an example will be described in which a sub-step of stopping the supply of at least one of the raw material and the oxygen-containing gas is included. Specifically, the soot-like material removal process will be described in the case where the raw material supply control means 20a and the oxygen-containing gas supply control means 21a function as extinguishing means and re-ignition means of the pressure wave generation means.
In this case, in the soot removal process, the raw material supply control means 20a and the oxygen-containing gas supply control means 21a are controlled to extinguish the flame in the laminar combustion state, and after the flame extinguishing process, the inside of the reactor 11 is By performing a re-ignition step in which the raw material is ignited, the volume of gas in the reactor is rapidly expanded and pressure waves are generated.

An example of the flame-extinguishing process is a process of stopping the supply of raw materials and/or oxygen-containing gas. From the viewpoint that pressure waves with sufficient strength are likely to occur during re-ignition, the flame-extinguishing step is preferably a step in which only the supply of raw materials is stopped. Specifically, by controlling the raw material supply control means 20a and/or the oxygen-containing gas supply control means 21a to stop the supply of the raw material and/or the oxygen-containing gas, laminar diffusion combustion is performed in the soot production process. Extinguish the flame in the state (extinguishing process).

Thereafter, the raw material supply control means 20a and/or the oxygen-containing gas supply control means 21a are controlled to restart the supply of the raw material and/or the oxygen-containing gas into the reactor 11, and the raw material is re-ignited (re-ignition step ). It is preferable to re-ignite the raw material before the temperature inside the reactor 11 decreases due to the flame being extinguished. When the temperature inside the reactor 11 is high, re-ignition can be achieved by simply restarting the supply of the raw material and/or the oxygen-containing gas and as long as the minimum ignition energy of the raw material is exceeded. If re-ignition cannot be achieved simply by restarting the supply of the raw material and/or oxygen-containing gas into the reactor 11, the ignition mechanism 31 can also re-ignite the raw material. As the raw material is re-ignited, the volume of gas within the reactor 11 expands instantaneously, generating strong pressure waves.

The supply amount of the raw material and oxygen-containing gas when restarting the supply of the raw material and/or oxygen-containing gas may be the same as that in the laminar flow combustion state in the soot production process, and the laminar flow combustion state in the soot production process It may be more than the combustion state. For example, the feed rate (g/min) of the raw material is 1.5 to 5.5% of the feed rate (g/min) in the laminar flow combustion state of the soot production process for a few seconds after restarting the feed material supply. 0 times, and thereafter the same supply rate (g/min) as in the laminar flow combustion state in the soot production step.

In the flame extinguishing process, a known method such as a method using a camera installed in the reactor 11 can be used to confirm that the flame has been extinguished. In the re-ignition step, a known method such as a method using a camera installed in the reactor 11 can be used to confirm that the reactor has been re-ignited.
The time from when the flame is extinguished until the supply of the raw material and/or oxygen-containing gas to the reactor 11 is started can be, for example, 1.0 to 5.0 seconds, and the time when the flame is extinguished. In order to prevent the temperature inside the reactor 11 from decreasing due to this, the shorter the time, the more preferable it is.

The timing of performing the soot-like substance removal step can be appropriately determined depending on the size of the reactor 11 and the supply amount of raw materials and oxygen-containing gas. In this embodiment, it is preferable to perform the soot removal step once every time the soot production step is performed for 20 min to 60 min, and the soot removal step is performed each time the soot production step is performed for 20 min to 40 min. It is more preferable to do it once. In this case, a large amount of soot-like material does not adhere to the inside of the reactor 11, and the flow path can be prevented from being blocked by the soot-like material. After performing the soot removal step, the supply amount of the raw material and/or oxygen-containing gas is immediately returned to the supply amount for the soot formation step, and the soot formation step is restarted. In this way, fullerene can be efficiently produced by alternately repeating the soot-like material generation step and the soot-like material removal step.

It is preferable that the pressure waves generated in the soot removal process of this embodiment are generated instantaneously due to rapid expansion of the gas volume. Examples of pressure waves include blast waves generated by explosions.

In the soot-like material generation step and the soot-like material removal step in the fullerene manufacturing method of the present embodiment, the exhaust gas containing soot produced in the reactor 11 is transferred to the exhaust port 1 of the reactor 11 by the suction force of the pressure reducing device 18. and is supplied to the fullerene recovery mechanism 16 via the pipe 19.
The soot contained in the exhaust gas supplied from the pipe 19 is collected by the filter 22 housed in the collector 29 of the fullerene recovery mechanism 16 .

In the fullerene recovery mechanism 16, inert gas is injected from the tank 24 toward the collector 29 by periodically opening the electromagnetic valve 25. As a result, the soot-like substances adhering to and being collected by the filter 22 installed in the collector 29 fall off from the filter 22 and accumulate at the bottom of the collector 29 . The soot deposited on the bottom of the collector 29 is discharged from the fullerene recovery mechanism 16 and recovered by opening the discharge valve 26.

The exhaust gas that has passed through the fullerene recovery mechanism 16 and from which fullerene has already been recovered is supplied to the cooling mechanism 17 via a pipe 27. In the cooling mechanism 17, the exhaust gas that has passed through the fullerene recovery mechanism 16 is cooled. As a result, unreacted hydrocarbons and water vapor contained in the exhaust gas are liquefied and discharged from the drain 28 provided at the lower side of the cooling mechanism 17.

The operating method of the fullerene manufacturing apparatus 10 of the present embodiment includes a soot-like material generation step and a soot-like material removal step. Therefore, even if soot adheres to the wall of the reactor 11 by performing the soot-generating step, the temperature inside the reactor 11 can be maintained without lowering by performing the soot-removing step. The soot 15 attached to the inside of the reactor 11 can be easily removed in a short time while keeping the temperature inside the reactor 11 at a high temperature capable of producing soot containing fullerene. Therefore, by using the fullerene manufacturing method using the operating method of this embodiment, fullerene can be efficiently manufactured by the combustion method.

(Second embodiment)
[Fullerene production equipment]
FIG. 3 is a configuration diagram showing an example of a fullerene manufacturing apparatus according to a second embodiment of the present invention. FIG. 4 shows a state in which soot 15 is attached to the wall of the reactor 11 due to fullerene production using the fullerene production apparatus 40 shown in FIG. 3 . The difference between the fullerene manufacturing apparatus 40 of this embodiment and the fullerene manufacturing apparatus 10 of the first embodiment shown in FIG. A gas supply pipe 32 is also connected thereto.
In the fullerene manufacturing apparatus 40 of this embodiment shown in FIG. 3, the same members as those of the fullerene manufacturing apparatus 10 of the first embodiment shown in FIG.

The inert gas supply piping 32 in the fullerene manufacturing apparatus 40 shown in FIG. 3 is provided with an inert gas supply control means 32a that controls the amount of inert gas supplied. Inert gas can be supplied into the reactor 11 via the burner 13 by the inert gas supply piping 32 by controlling the inert gas supply control means 32a. As an example of the inert gas supply control means 32a, a commercially available mass flow meter or the like can be used, for example.

The pressure wave generating means includes an inert gas supply means that rapidly expands the volume of gas in the reactor 11 by supplying an inert gas to the burner 13 . In the fullerene manufacturing apparatus 40 shown in FIG. 3, an inert gas supply pipe 32, an inert gas supply control means 32a, and an inert gas supply source (for example, an inert gas cylinder) not shown in FIG. It can function as an active gas supply means. The pressure wave generating means adjusts the supply amount (NL/min) of the inert gas in the soot removal process to 1.5 to 5. It is preferable to use one that can be multiplied by 0 times. The magnification may be 2.0 to 5.0 times, 1.8 to 4.0 times, 2.0 to 3.0 times, etc., as necessary.

In the second embodiment, an inert gas is supplied into the reactor 11 via the burner 13 using a fullerene manufacturing apparatus 40 shown in FIG. An example of how to introduce this will be explained. However, the inert gas may be supplied to the vicinity of the discharge portion 13c of the burner 13 disposed in the reactor 11 without passing through the burner 13. As a method for supplying inert gas to the vicinity of the discharge part 13c of the burner 13 without passing through the burner 13, for example, a method of supplying inert gas to the vicinity of the discharge part 13c of the burner 13 separately from the burner 13 is available. One method is to install a department. The vicinity of the discharge part 13c of the burner 13 is the area where the volume of gas in the reactor 11 is rapidly expanded by supplying inert gas, and the soot 15 attached to the wall of the reactor 11 can be removed. This is the range in which pressure waves can be generated.

[How to operate fullerene production equipment, fullerene production method]
Next, a method of operating the fullerene production apparatus 40 shown in FIG. 3 and a method of producing fullerene using the fullerene production apparatus 40 will be described by giving examples.
The operating method of the fullerene manufacturing apparatus 40 includes a soot-like material generation step and a soot-like material removal step. The soot-like substance generation process is the same as the soot-like substance generation process of the first embodiment, so the description thereof will be omitted.

(Soot removal process)
In the soot removal step, an inert gas is supplied into the reactor 11 to rapidly expand the volume of the gas in the reactor 11 . This generates a pressure wave with sufficient strength to remove the soot 15 adhering to the wall of the reactor 11. The gas in the reactor 11 is composed of any gas that may exist in the reactor 11, such as raw materials, oxygen-containing gas, inert gas, carbon monoxide, carbon dioxide, water vapor, etc. generated by combustion of raw materials. It is a mixed gas that may be mixed.

The strength of the pressure waves generated in the soot removal process can be adjusted by controlling the amount of inert gas supplied into the reactor 11.
In the soot removal step, when an inert gas is supplied into the reactor 11 to rapidly expand the gas volume, the amount of inert gas supplied (NL/min) is equal to the oxygen content in the soot production step. It is preferably 1.5 to 5.0 times the gas supply amount (NL/min), and more preferably 2.0 to 5.0 times. The magnification may be 1.8 to 4.0 times, 2.0 to 3.0 times, etc., as necessary. When the amount of inert gas supplied is 1.5 times or more the amount of oxygen-containing gas supplied in the soot production step, the volume of gas in the reactor 11 can expand at a sufficiently fast rate. Therefore, a pressure wave is generated that is strong enough to efficiently remove the soot-like material 15 (see FIG. 4) adhering to the wall of the reactor 11. If the amount of inert gas supplied is less than 5.0 times the amount of oxygen-containing gas in the soot production step, the volume of gas in the reactor 11 will expand too quickly and the generated pressure waves will become stronger. You can prevent too much. In the soot-like substance removal step, the feed rate (g/min) of the raw material and the feed rate (NL/min) of the oxygen-containing gas are preferably the same as in the soot-like substance generation process.

The time for supplying the inert gas by the inert gas supply means (supply time) can be arbitrarily selected, but is preferably 0.5 seconds to 5.0 seconds, and preferably 2.0 seconds to 4.0 seconds. It is more preferable. If the time for supplying the inert gas is 0.5 seconds or more, a pressure wave strong enough to remove the soot 15 (see Figure 4) adhering to the furnace wall is likely to be generated. ,preferable. When the inert gas supply time is 5.0 seconds or less, the soot 15 adhering to the furnace wall can be sufficiently removed, and the soot removal process can be completed in a short time, allowing the soot generation process to proceed. This is preferable because it has less influence.

As the inert gas, for example, an inert gas such as nitrogen gas or argon gas can be used. As the inert gas, only one type of these may be used, or two or more types may be used in combination.

The timing of performing the soot-like substance removal step can be appropriately determined depending on the size of the reactor 11 and the supply amount of raw materials and oxygen-containing gas. In this embodiment, it is preferable to perform the soot removal step once every time the soot production step is performed for 20 min to 60 min, and the soot removal step is performed each time the soot production step is performed for 20 min to 40 min. It is more preferable to do it once. In this case, a large amount of soot-like material does not adhere in the reactor 11, and it is possible to prevent the soot-like material from clogging the flow path. After the supply of inert gas into the reactor 11 (soot removal process) is completed, the inside of the reactor 11 returns to a laminar combustion state in which incomplete combustion of the raw materials is stabilized, and the soot production process is completed. will be started. Therefore, the soot-like material generation step and the soot-like material removal step can be easily repeated alternately, and fullerene can be efficiently produced.

It is preferable that the pressure waves generated in the soot removal process of this embodiment are generated instantaneously due to rapid expansion of the gas volume. Examples of pressure waves include blast waves generated by explosions.

In the operating method of the fullerene production apparatus 40 of this embodiment and the fullerene production method using this operating method, similarly to the first embodiment, raw materials containing hydrocarbons and oxygen-containing gas are supplied into the reactor 11, Due to the soot production process in which raw materials are incompletely combusted in a laminar flow combustion state and the pressure waves generated by rapidly expanding the volume of gas in the reactor 11, soot adhering to the walls of the reactor 11 is removed. and a soot-like material removal step for removing the soot-like material 15. Therefore, even if soot 15 adheres to the interior of the reactor 11 by performing the soot production step, the reaction can be carried out without lowering the temperature inside the reactor 11 by performing the soot removal step. The soot 15 attached to the inside of the reactor 11 can be removed in a short time while keeping the temperature inside the furnace 11 at a high temperature capable of producing soot containing fullerene.

Hereinafter, the present invention will be specifically explained with reference to Examples and Comparative Examples. Note that the examples shown below are provided to facilitate understanding of the contents of the present invention. The present invention is not limited to these examples, and various modifications can be made without departing from the spirit of the present invention.

<Example 1>
Fullerene was manufactured using the fullerene manufacturing apparatus 10 shown in FIG. 1 by the operating method shown below.
The reactor 11 used was one made of alumina, which had a cylindrical shape with a length of 1000 mm and an inner diameter of 60 mm, and was arranged so that the length direction was in the vertical direction.
A heat insulating layer 14 made of alumina was provided all over the outside of the reactor 11.
The temperature inside the reactor 11 during the soot production step was within the range of 1100°C to 2000°C.

As the discharge part 13c of the burner 13, a disc-shaped porous ceramic sintered body with a diameter of 50 mm was used. This ceramic sintered body has 60 to 80 approximately circular discharge ports per 1 cm ² with a diameter of 0.5 mm to 1.5 mm. The ratio between the inner diameter D1 of the reactor 11 and the diameter D2 of the discharge portion 13c was 1.20.
A camera was installed near the discharge port 12 inside the reactor 11, and fullerene was produced while photographing the inside of the reactor 11 with the camera.
As the raw material supply control means 20a, a mass controller (AeraSFC168, manufactured by Hitachi Metals, Ltd.) was used, and as the oxygen-containing gas supply control means 21a, a mass flow meter (mass controller AeraFC-7810CD, manufactured by Hitachi Metals, Ltd.) was used.

(Soot-like substance generation process)
The raw material supply pipe 20 supplies toluene as a raw material vaporized by a heating device (not shown) to the burner 13, and the oxygen-containing gas supply pipe 21 supplies oxygen gas (purity 99.9% by volume) as an oxygen-containing gas. ) was supplied to the burner 13 and ignited using the ignition mechanism 31 to cause incomplete combustion in a laminar flow combustion state and to start the production of soot containing fullerene.

In the soot production step, the pressure of the mixed gas in the pressure accumulator 13b was 10 kPa, and the pressure in the reactor 11 was 5.33 kPa. The amount of toluene supplied into the reactor 11 was set to 15 g/min, the amount of oxygen gas supplied was set to 10 NL/min, and a mixed gas of toluene and oxygen gas was continuously injected into the reactor 11 from the burner 13. , incomplete combustion was continued for 30 minutes. The ratio between the number of carbon atoms in the raw material and the number of oxygen atoms in the oxygen-containing gas supplied to the burner 13 per minute was 1.28.

(Soot removal process)
The amount of oxygen gas supplied remains at 10 NL/min, only the raw material supply control means 20a is controlled, the amount of toluene supplied is set to 2.0 times that of the soot production step (30 g/min), and the reaction is started from the burner 13. It was injected into the furnace 11 for 2.0 seconds. Thereafter, the raw material supply control means 20a is controlled while the oxygen gas supply rate remains at 10 NL/min, and the toluene supply rate is returned from 30 g/min to 15 g/min, which is the toluene supply rate in the soot production step. A second soot production step was started.

Similarly, the soot-like material generation step and the soot-like material removal step were repeated five times. Thereafter, the raw material supply control means 20a was controlled to stop the supply of toluene, the oxygen-containing gas supply control means 21a was controlled to stop the supply of oxygen gas, and the operation of the manufacturing apparatus 10 was stopped.

In Example 1, the flame was not extinguished in the soot-like production process of the manufacturing apparatus 10, and continuous operation was possible.
Further, after the operation of the manufacturing apparatus 10 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, no clogging of the flow path due to soot adhering to the furnace wall was observed in the reactor 11.

Further, in Example 1, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 459.0 g.
Then, the content rate and amount of fullerene in the soot were determined by the method shown below. As a result, the fullerene content was 3.8% by mass, and the fullerene content was 17.40 g.

<Measurement of fullerene content>
In accordance with "JIS Z 8981", the fullerene (C ₆₀ and C ₇₀ ) content contained in the collected soot was measured by the method shown below.
15 g of 1,2,3,5-tetramethylbenzene (TMB) was added to 0.05 g of soot, and subjected to ultrasonication for 15 minutes to obtain a suspension. The resulting suspension was filtered through a membrane filter with a pore size of 0.5 μm. The obtained filtrate (sample liquid) was analyzed using high performance liquid chromatography (HPLC) under the measurement conditions shown below to quantify C 60 and C 70, and the results were used to determine the amount of C ₆₀ and C ₇₀ contained in the soot. The content rate [mass%] of C ₆₀ and C ₇₀ was calculated.
When calculating the content of C ₆₀ and C ₇₀ contained in the soot, a calibration curve prepared in advance from a plurality of TMB solutions of C ₆₀ and C ₇₀ with known concentrations was used.

The HPLC measurement conditions are as follows.
Device: Infinity1260 (manufactured by Agilent)
Injection volume of sample solution: 5μL
Eluent: Toluene (47% by volume)/methanol (53% by volume) mixed solvent Eluent flow rate: 1ml/min Column: YMC-Pack ODS-AM 100*4.6mm ID S-3μm, 12nm (manufactured by YMC)
Measurement temperature: 40℃
Detector: UV 325nm (JIS)

<Example 2>
Using the same fullerene manufacturing apparatus 10 as in Example 1, fullerene was manufactured by the operating method shown below.
(Soot-like substance generation process)
The soot production step was carried out in the same manner as in Example 1.

(Soot removal process)
The soot removal step was carried out in the same manner as in Example 1, except that the toluene supply amount was kept at 15 g/min and the oxygen gas supply amount was twice that of the soot production step (20 NL/min). I did it. Thereafter, the oxygen-containing gas supply control means 21a is controlled while the toluene supply rate remains at 15 g/min, and the oxygen gas supply rate is increased from 20 NL/min to 10 NL/min, which is the oxygen gas supply rate for the soot production step. , and the second soot production step was started.
After repeating the above-mentioned soot-like substance generation step and soot-like substance removal process five times in the same manner, the operation of the manufacturing apparatus 10 was stopped in the same manner as in Example 1.

In Example 2, the flame was not extinguished in the soot production process of the manufacturing apparatus 10, and continuous operation was possible.
Further, after the operation of the manufacturing apparatus 10 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, no clogging of the flow path due to soot adhering to the furnace wall was observed in the reactor 11.

Further, in Example 2, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 431.0 g.
Then, the content rate and amount of fullerene in the soot were determined in the same manner as in Example 1. As a result, the fullerene content was 3.5% by mass, and the fullerene content was 15.08 g.

<Example 3>
Using the same fullerene manufacturing apparatus 10 as in Example 1, fullerene was manufactured by the operating method shown below.
(Soot-like substance generation process)
The soot production step was carried out in the same manner as in Example 1.

(Soot removal process)
The amount of toluene supplied is twice the amount of toluene supplied in the soot production step (30 g/min), and the amount of oxygen gas supplied is twice the amount of oxygen gas supplied in the soot production step (20 NL/min). The soot-like substance removal step was carried out in the same manner as in Example 1, except that. Thereafter, the raw material supply control means 20a and the oxygen-containing gas supply control means 21a are controlled to supply oxygen gas from 30 g/min to the toluene supply amount of 15 g/min in the soot production step. The amount of oxygen gas was returned from 20 NL/min to 10 NL/min for the soot production step, and the second soot production step was started.
After repeating the above-mentioned soot-like substance generation step and soot-like substance removal process five times in the same manner, the operation of the manufacturing apparatus 10 was stopped in the same manner as in Example 1.

In Example 3, the flame was not extinguished in the soot production process of the manufacturing apparatus 10, and continuous operation was possible.
Further, after the operation of the manufacturing apparatus 10 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, no clogging of the flow path due to soot adhering to the furnace wall was observed in the reactor 11.

Further, in Example 3, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 439.0 g.
Then, the content rate and amount of fullerene in the soot were determined in the same manner as in Example 1. As a result, the fullerene content was 3.8% by mass, and the fullerene content was 16.68 g.

<Example 4>
Using the same fullerene manufacturing apparatus 10 as in Example 1, fullerene was manufactured by the operating method shown below.
(Soot-like substance generation process)
The soot production step was carried out in the same manner as in Example 1.

(Soot removal process)
The amount of oxygen gas supplied was kept at 10 NL/min, and only the raw material supply control means 20a was controlled to reduce the amount of toluene supplied to 0 g/min (the supply of toluene was stopped) to extinguish the laminar flame. Using a camera installed in the reactor 11, it is confirmed that the flame has been extinguished, and within 5 seconds after the flame has been extinguished, the raw material supply control means 20a is controlled to increase the supply amount into the reactor 11. The supply of toluene at 15 g/min was restarted. Since the temperature inside the reactor 11 was high, toluene was spontaneously re-ignited the moment it was introduced.

After that, the supply amount of oxygen gas is set to 10 NL/min, which is the supply amount of oxygen gas in the soot production step, and the supply amount of toluene is set to 15 g/min, which is the supply amount of toluene in the soot production step. Combustion was returned to laminar combustion and a second soot production step was started.
After repeating the above-mentioned soot-like substance generation step and soot-like substance removal process five times in the same manner, the operation of the manufacturing apparatus 10 was stopped in the same manner as in Example 1.

In Example 4, after the operation of the manufacturing apparatus 10 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, no clogging of the flow path due to soot adhering to the furnace wall was observed in the reactor 11.

In addition, in Example 4, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 397.0 g.
Then, the content rate and amount of fullerene in the soot were determined in the same manner as in Example 1. As a result, the fullerene content was 4.5% by mass, and the fullerene content was 17.86 g.

<Example 5>
Fullerene was manufactured using the fullerene manufacturing apparatus 40 shown in FIG. 3 by the operating method shown below. As the inert gas supply control means 32a, a mass flow meter (mass controller AeraFC-7810CD, manufactured by Hitachi Metals, Ltd.) was used.
(Soot-like substance generation process)
The soot production step was carried out in the same manner as in Example 1.

(Soot removal process)
While keeping the toluene supply rate at 15 g/min and the oxygen gas supply rate at 10 NL/min, the inert gas supply control means 32a was controlled to inject nitrogen gas from the burner 13 into the reactor 11 for 2 seconds. . The amount of nitrogen gas supplied was 5.0 times (50 NL/min) the amount of oxygen gas supplied (10 NL/min) in the soot production step.
Thereafter, the supply of nitrogen gas was stopped, and the second soot production step was started while keeping the toluene supply rate at 15 g/min and the oxygen gas supply rate at 10 NL/min.
After repeating the above-mentioned soot-like substance generation step and soot-like substance removal process five times in the same manner, the operation of the manufacturing apparatus 40 was stopped in the same manner as in Example 1.

In Example 5, the flame was not extinguished in the soot production process of the manufacturing apparatus 40, and continuous operation was possible.
Further, after the operation of the manufacturing apparatus 40 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, no clogging of the flow path due to soot adhering to the furnace wall was observed in the reactor 11.

In addition, in Example 5, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 386.0 g.
Then, the content rate and amount of fullerene in the soot were determined in the same manner as in Example 1. As a result, the fullerene content was 4.7% by mass, and the fullerene content was 18.14 g.

<Comparative example 1>
Using the same fullerene manufacturing apparatus 10 as in Example 1, fullerene was manufactured by the operating method shown below.
Fullerene was continuously produced in the same soot production step as in Example 1 without performing the soot removal step.
As a result, the flashback prevention device was activated 91 minutes after the start of the soot production process, and the operation of the manufacturing apparatus 10 was stopped.

In Comparative Example 1, after the operation of the manufacturing apparatus 10 was stopped and the temperature inside the reactor 11 returned to room temperature, the burner 13 was removed and the state inside the reactor 11 was visually confirmed. As a result, clogging of the flow path in the reactor 11 due to soot adhering to the furnace wall was observed.

Further, in Comparative Example 1, the soot-like material collected in the collector 29 was collected. The mass of the soot-like substance recovered was 127.0 g.
Then, the content rate and amount of fullerene in the soot were determined in the same manner as in Example 1. As a result, the fullerene content was 3.7% by mass, and the fullerene content was 4.70 g.

In Examples 1 to 4 and Comparative Example 1, fullerene was produced using the fullerene production apparatus 10. However, the fullerene production apparatus 40 can also be used to produce fullerenes as in Examples 1 to 4 and Comparative Example 1. At that time, the mass flow meter, which is the inert gas supply control means 32a of the fullerene production apparatus 40, is controlled to set the inert gas supply amount to zero.

In Examples 1 to 5, by performing the soot-like material removal step, the soot-like material adhering to the inside of the reactor 11 can be easily removed in a short time, and the soot-like material removal step is performed. It was confirmed that fullerene could be produced efficiently by the combustion method compared to Comparative Example 1, which did not have the following conditions.
That is, in Examples 1 to 5, in the soot removal process, the pressure waves generated by rapidly expanding the volume of gas in the reactor 11 remove soot adhering to the wall of the reactor 11. It is presumed that the object 15 was removed.

The present invention provides a method for operating a fullerene production apparatus that can easily remove soot-like substances adhering to the walls of a reactor in a short time and that can efficiently produce fullerene by a combustion method.

DESCRIPTION OF SYMBOLS 10, 40... Fullerene manufacturing apparatus 11... Reaction furnace 12... Discharge port 13... Burner 13a... Mixing chamber 13b... Pressure accumulation chamber 13c... Discharge part 14... Heat insulation layer 15... Soot-like substance 16... Fullerene recovery mechanism 17... Cooling mechanism 18 ... Pressure reducing device 19, 23, 27, 30... Piping 20... Raw material supply piping 20a... Raw material supply control means 21... Oxygen-containing gas supply piping 21a... Oxygen-containing gas supply control means 22... Filter 24... Tank 25... Solenoid valve 26... Discharge valve 28...Drain 29...Collector 31...Ignition mechanism 32...Inert gas supply piping 32a...Inert gas supply control means

Claims (17)

A method of operating a fullerene production device equipped with a reactor that produces soot-like material containing fullerene,
A soot-like substance production step of supplying a raw material containing a hydrocarbon and an oxygen-containing gas into the reactor using a burner, and causing incomplete combustion of the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene. and,
After the soot production step, the volume of gas in the reactor is rapidly expanded to generate a pressure wave, and the generated pressure wave causes the reactor to absorb the gas generated in the soot production step. a soot-like substance removal step of removing the soot-like substance adhering to the wall,
In the soot removal step, at least one of the raw material and the oxygen-containing gas is continuously supplied into the reactor from the soot production step, and at least one of the supplied raw material and the oxygen-containing gas is supplied. A method for operating a fullerene manufacturing apparatus, comprising increasing the amount of gas supplied in the soot production step to rapidly expand the volume of gas in the reactor. In the soot-like substance removal step, the feed rate (g/min) of the raw material is set to 1.5 to 5.0 times the feed rate (g/min) of the raw material in the soot-like substance generation process. Item 1. A method for operating the fullerene production apparatus according to item 1. In the soot removal step, the supply amount (NL/min) of the oxygen-containing gas is 1.5 to 5.0 times the supply amount (NL/min) of the oxygen-containing gas in the soot production step. A method for operating a fullerene production apparatus according to claim 1 or 2. The fullerene according to claim 1 or 2 , wherein in the soot removal step, the time for increasing the supply amount of at least one of the raw material and the oxygen-containing gas is 0.5 seconds to 5.0 seconds. How to operate manufacturing equipment. A method of operating a fullerene production device equipped with a reactor that produces soot-like material containing fullerene,
A soot-like substance production step of supplying a raw material containing a hydrocarbon and an oxygen-containing gas into the reactor using a burner, and causing incomplete combustion of the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene. and,
After the soot production step, the volume of gas in the reactor is rapidly expanded to generate a pressure wave, and the generated pressure wave causes the reactor to absorb the gas generated in the soot production step. a soot-like substance removal step of removing the soot-like substance adhering to the wall,
In the soot removal step, an inert gas is supplied to the burner or near the discharge part of the burner disposed in the reactor to rapidly expand the volume of gas in the reactor, producing fullerene. How to operate the equipment. In the soot removal step, the inert gas supply rate (NL/min) is 1.5 to 5.0 times the oxygen-containing gas supply rate (NL/min) in the soot generation step. A method for operating the fullerene production apparatus according to claim 5. The method for operating a fullerene production apparatus according to claim 5 or 6, wherein in the soot-like substance removal step, the time for supplying the inert gas is 0.5 seconds to 5.0 seconds. A method of operating a fullerene production device equipped with a reactor that produces soot-like material containing fullerene,
A soot-like substance production step of supplying a raw material containing a hydrocarbon and an oxygen-containing gas into the reactor using a burner, and causing incomplete combustion of the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene. and,
After the soot production step, the volume of gas in the reactor is rapidly expanded to generate pressure waves, and the generated pressure waves cause the soot production a soot-like substance removal step of removing the soot-like substance adhering to the wall,
The soot-like material removal step is a flame-extinguishing step of extinguishing the flame in the laminar combustion state generated in the soot-like material generation step;
A method for operating a fullerene manufacturing apparatus, comprising a re-ignition step of igniting the raw material in the reactor after the flame-extinguishing step. The extinguishing step is a step of stopping the supply of the raw material,
The method of operating a fullerene manufacturing apparatus according to claim 8, wherein the re-ignition step is a step of supplying the raw material into the reactor. A method of operating a fullerene production device equipped with a reactor that produces soot-like material containing fullerene,
A soot-like substance production step of supplying a raw material containing a hydrocarbon and an oxygen-containing gas into the reactor using a burner, and causing incomplete combustion of the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene. and,
After the soot production step, the volume of gas in the reactor is rapidly expanded to generate a pressure wave, and the generated pressure wave causes the reactor to absorb the gas generated in the soot production step. A fullerene production device used in a method for operating a fullerene production device, comprising a soot-like substance removal step of removing the soot-like substance adhering to a wall,
A reactor that has a burner that supplies a raw material containing hydrocarbons and an oxygen-containing gas, and incompletely burns the raw material in a laminar flow combustion state to produce a soot-like substance containing fullerene;
Pressure wave generating means for generating a pressure wave that rapidly expands the volume of gas in the reactor to remove the soot attached to the wall of the reactor,
The pressure wave generating means sets the feed rate (g/min) of the raw material to 1.5 to 5 of the feed rate (g/min) when the raw material is incompletely combusted in the laminar flow combustion state. A fullerene manufacturing device that has a supply control means that increases the amount by .0 times. The pressure wave generating means is configured to set the supply amount (NL/min) of the oxygen-containing gas to 1 of the supply amount (NL/min) of the oxygen-containing gas when the raw material is incompletely combusted in the laminar flow combustion state. The fullerene production apparatus according to claim 10, comprising a supply control means for increasing the amount by .5 to 5.0 times. The pressure wave generating means is an inert gas that rapidly expands the volume of gas in the reactor by supplying an inert gas to the burner or near the discharge part of the burner disposed in the reactor. The fullerene production apparatus according to claim 10, comprising a supply means. The pressure wave generating means includes extinguishing means for extinguishing the flame in the laminar combustion state;
The fullerene manufacturing apparatus according to claim 10, further comprising a re-ignition means for igniting the raw material in the reactor. The extinguishing means is a means for stopping the supply of the raw material,
The fullerene manufacturing apparatus according to claim 13, wherein the re-ignition means is means for supplying the raw material into the reactor. A fullerene production method using the operating method of the fullerene production apparatus according to claim 1 or 2 ,
A soot-like product generation step in which a raw material containing hydrocarbons and an oxygen-containing gas are supplied into the reactor using a burner, and the raw materials are incompletely combusted in a laminar flow combustion state to produce a soot-like product containing fullerene. ,
a soot-like matter removing step of removing soot-like matter containing the fullerene adhering to the wall of the reactor using pressure waves generated by rapidly expanding the volume of gas in the reactor. , fullerene production method. 16. The method according to claim 15, comprising the step of recovering fullerene from the soot containing the fullerene produced in the soot production step and the soot removed in the soot removal step. Fullerene manufacturing method. The method of operating a fullerene production apparatus according to claim 1, wherein in the soot-like substance generation step, the generated soot-like substance is sent outside the reactor.

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