WO2008123802A1

WO2008123802A1 - Device for producing fullerene-containing soot

Info

Publication number: WO2008123802A1
Application number: PCT/RU2008/000223
Authority: WO
Inventors: Nikolay Nikolaevich Bolstren; Vladimir Maksimovich Oichenko; Gennady Nikolaevich Druzhinin; Valery Aleksandrovich Belov
Original assignee: Obschestvo S Ogranichennoy Otvetsvennostju, 'nauchno-Proizvodstvennaya Kompaniya 'neotekprodakt'
Priority date: 2007-04-06
Filing date: 2008-04-03
Publication date: 2008-10-16
Also published as: RU2343111C1; RU2007114019A

Abstract

The inventive device for producing fullerene-containing soot comprises a horizontal sealed discharge chamber (1) and an inert gas cycling system (10) with means (14) for catching fullerene-containing soot. The discharge chamber (1) is designed in the form of two truncated cones which are connected by the large bases thereof and are closed by spherical covers. Two graphite electrodes (2, 3) are arranged in coolable current leads (8, 9) along the axis of the chamber (1). The inert gas cycling system (10) comprises at least two nozzles (29, 30) which are placed at the end walls of the discharge chamber (1) tangentially to the side wall thereof in planes perpendicular to the axis of the electrodes (2, 3).

Description

INSTALLATION FOR THE PRODUCTION OF FULLERY-CONTAINING SOOT

Technical field

The invention relates to the production of fullerene-containing carbon black - a product containing a new form of a carbon element, which is an electron-deficient superalken with weakly conjugated double bonds, including compounds with a strictly defined molecular, and not only crystalline structure, including closed-chain superalkenes - fullerenes, which find application in chemistry, physics, engineering, energy, electronics, biology, medicine and other fields. State of the art

To obtain fullerene-containing soot, various devices are used, based, for example, on the evaporation of graphite and the pyrolysis of hydrocarbons, however, not all devices can be used for industrial production due to unproductive consumption of raw materials, low yield of target products, and difficulties in scaling.

A device for the production of fullerene-containing soot (see patent RU 2085484, IPC, published July 27, 1997), including an emitter installed with the possibility of movement inside a vacuum vessel, an emitter heating system, as well as soot collectors and collectors for separating fullerenes.

The disadvantages of this device are the inability to remove soot not containing fullerenes during the process and the termination of the process due to the filling of the reactor with soot.

A device is known for producing fullerene-containing soot (see patent RU 2184700, IPC C01 B 31/02, published July 10, 2002) comprising a housing containing a working chamber connected to a channel for product withdrawal, means for supplying carbon-containing material and a process control unit. The housing is equipped with a thin-walled cylinder in the form of a cup placed in the working chamber, the bottom of which has an opening connected to a hollow cone for removal and collection of fullerene-containing material. At the base of the cylinder there is a bearing assembly having a remote magnetic drive in the form of plates of electromagnets fixed outside the walls of the housing. The carbon-containing material supply means is adapted to be fed in portions and made in the form of a magazine holder with nests for graphite rods located around its circumference, with the possibility of its axial rotation and equipped with a clamping and fixing unit for graphite rods in the working chamber. Cone cavity

SUBSTITUTE SHEET (RULE 26) equipped with a filter for trapping and accumulating fullerene particles.

The clamping and fixing unit of graphite rods is made in the form of spring-loaded screw grips and longitudinal ring guides. The capture and accumulation of fullerene particles is carried out due to the location of the filter in the cavity of the cylinder and cone; as the filter material take a multilayer fine mesh with layers of foil having pores.

The disadvantages of this device are the immobility of the second electrode, which leads to the deposition of the cathode deposit and the inability to remove solid graphite residues from the reaction volume without disassembling the device.

A device is known for producing fullerene-containing soot (see application RU 98105520, IPC C01 B 31/02, published January 27, 2000) containing an electric current source, the poles of which are connected to the first and second electrical inputs with electrodes fixed in them, one of which is made from a carbon-containing material, for example, graphite, as well as a cooled first sealed chamber connected by means of a first gas duct to a vacuum pump and by means of a second one with an inert gas supply unit to the sealed chamber. A vacuum-tight first electrical input with an electrode in the form of a rod is installed on the inside of the chamber wall, opposite which, coaxially with it, a second electrical input with an electrode in the form of a rod is mounted on the wall of the sealed chamber, mounted in a vacuum seal mounted on the wall of the sealed chamber. The rods are installed with the ends facing each other, and the second electrical input has the ability to move along its geometric axis relative to the first electrical input with an electrode. On the outside of the sealed chamber, the second electrical input is connected to the block of its movement along its axis while maintaining the discharge gap between the rods. The sealed chamber is made in the form of a hollow body with a ratio of the width of the cavity to its length equal to 0.02 - 1, 0, with the first electrical input connected to the positive pole of the electric current source, the negative pole of which is connected to the second electrical input, and the first and second electrical bushings with rods are installed along the length of the cavity in the sealed chamber. In the known device, it is necessary to interrupt the process to remove soot from the reactor and remove the remnants of the electrodes. The disadvantages of the device should also include large losses of evaporated carbon (up to 50%) on the SUBSTITUTE SHEET (RULE 26) the formation of a cathode deposit on one of the electrodes and the low yield of fullerenes when using catalysts.

A device for the production of fullerene-containing soot (see patent for utility model RU 39129, IPC C01 B 31/00, published July 20, 2004), including a plasma reactor in the form of a sealed cylindrical chamber with two graphite rod electrodes placed along the chamber axis - anode and cathode fixed in cooled current leads, while the anode is equipped with axial displacement means, the reactor is equipped with means for supplying an inert gas and swirling the flow along the axis of the electrodes, which can be performed with the possibility of the inert gas supply from the cathode side in the form of a nozzle oriented tangentially to the side surface of the chamber or in the form of a nozzle, which ensure twisting of the gas flow along the side wall of the chamber. The installation can be equipped with a container for collecting slag, communicating with the lower part of the chamber, and a device for controlling the size of the gap between the electrodes, and the axial movement of the anode is made possible to control the speed of its movement while maintaining a constant gap between the electrodes. The cathode may be provided with means of reverse rotation about the axis. The disadvantages of the known technical solution are the unreasonable complication of the design by various effects on the arc and the reaction volume, the possibility of burning the chamber as a result of extreme impacts (especially at peak loads), the inability to remove the cathode deposit formed without stopping the process, changing the geometric position of the arc, the possibility of arc breaking by a swirling inert stream gas and, as a consequence, the non-stationary nature of the process and the low yield of fullerenes in the specified device.

A device is known for the production of nanotubes, fullerenes and their derivatives (see patent US 7125525, IPC BOU 19/08, published October 24, 2006), including: a vacuum reactor equipped with inlet and vacuum nozzles; a graphite electrode mounted in a vacuum reactor; means for evaporating said electrode and simultaneously forming a high-temperature plasma around said graphite electrode, which comprise an inductor installed inside the vacuum reactor and a power generator associated with it and designed to create a high-frequency electromagnetic field with vortex flows; and

SUBSTITUTE SHEET (RULE 26) an inert gas source set so that gas flows around the inductor and the graphite electrode.

The disadvantages of the known device are the complexity of the practical implementation associated with the presence of an inductor inside a vacuum reactor, i.e. in the process zone and the difficulty of its functioning in the formation of soot, as well as the impossibility of removing residual electrodes from the reaction volume.

A device for the production of carbon nanostructures (see patent US 6902655, IPC B01 J19 / 08, published 07.05.2005), consisting of two opposite electrodes, a node for creating a voltage between them and a node for creating a magnetic field, the multidirectional lines of which intersect the feed direction voltage.

The disadvantages of this device are the need to interrupt its operation to install new electrodes instead of evaporated ones, to remove soot and electrode residues from the reactor, to deposit a cathode deposit on one of the electrodes (up to 50% of the evaporated carbon) and low fullerene yield when using catalysts.

A device for the production of fullerene-containing soot (see patent US 6358375, IPC H05H1 / 42, published July 20, 2004), including a plasma reactor and sequentially descending heated and cooled separators.

The disadvantages of this device are the lack of degassing of the electrodes, deposition of a cathode deposit on a fixed electrode (loss of evaporated carbon up to 50%), deposition of a large amount of soot in the reactor, the need to stop the device to replace burned electrodes and remove from the reaction volume electrode fragments, the cause of which is usually considered heterogeneity of the electrodes and a high voltage drop in the plasma.

A device for the continuous production of carbon nanotubes and fullerenes is known (see application US 20050019245, IPC D01 F 9/12, published

01/27/2005), which is a closed system and includes a sealed water-cooled chamber, consisting of an arc discharge section with a vapor generation zone between two graphite electrodes, an anode supply section with a device for automatically connecting individual graphite electrodes and gradually supplying them to the vapor generation zone and sections catalyst supply with a device for continuous supply of catalyst through a central hole in the cathode body into the generation zone

SUBSTITUTE SHEET (RULE 26) vapor. The anode feed section includes a replaceable sealed cartridge containing several graphite electrodes to ensure continuous operation. The catalyst supply section includes a replaceable sealed cartridge containing a catalyst in the form of a metal wire or metal powder to ensure continuous operation of the device. The device also comprises: means for maintaining an optimum surface temperature of the anode and an optimal concentration of carbon vapors in the vapor generation zone containing at least one gas a nozzle and at least one gas distributor located inside the arc discharge section of the sealed chamber. In addition, the device comprises means for transporting gas of condensing vapor and inert gas recirculation; a heat exchanger for maintaining a constant temperature of the circulating inert gas stream, comprising means for continuously cleaning the internal walls of the heat exchanger from condensing vapors; a filter for separating condensing vapors from the inert gas stream, including means for automatically cleaning the filter; and also a storage hopper for filtered vapor condensate, including a device for automatically discharging vapor condensate from the storage hopper. The disadvantages of this device are the lack of degassing of the electrodes, the need to interrupt the process for periodically cleaning the walls of the heat exchanger and removing fragments of electrodes from the reaction volume, the absence of automatic self-cleaning of the filter and the inability to remove the cathode deposit. The closest set of features to the claimed technical solution is the installation for producing fullerene-containing soot (see RU 2234457, IPC C01 B 31/02, published 10.06.2003), including a plasma reactor in the form of a sealed cylindrical chamber with an inert gas circulation system with a trapping means fullerene-containing soot, with two graphite rod electrodes placed along the chamber axis, one of which is fixedly mounted in the cooled current lead, and the other is installed in the second cooled current lead axial translational displacement. The reactor is additionally equipped with a chamber for degassing the movable graphite electrode with a glow discharge, the inert gas circulation system is equipped with an annular slot nozzle placed coaxially to the electrodes, and the means for collecting fullerene-containing soot SUBSTITUTE SHEET (RULE 26) equipped with an electrostatic precipitator installed at the inlet of the inert gas circulation system.

In the known installation of the prototype is the degassing of one of the electrodes. Its disadvantages include the deposition of a cathode deposit on the second electrode, which causes the destruction of the material when the polarity changes, relatively low productivity of soot and fullerenes at significant energy costs, insufficient removal of fullerene-containing soot from the reactor volume during the process.

SUMMARY OF THE INVENTION The objective of the present technical solution is to develop such a plant for the production of fullerene-containing soot, which would provide higher productivity for soot and fullerenes with minimal energy consumption, sufficiently complete removal of fullerene-containing soot during the process. The problem is solved in that the installation for the production of fullerene-containing soot includes a horizontal sealed discharge chamber with two graphite rod electrodes installed in the cooled current leads and with an outlet pipe opposite the interelectrode gap, an inert gas circulation system with a means of trapping fullerene-containing at least one glow discharge degassing chamber. The discharge chamber is made in the form of two truncated cones connected by spherical covers connected by wide bases. At least one of the electrodes is mounted axially reciprocating. The inert gas circulation system connected to the outlet nozzle is provided with at least two nozzles mounted at the end walls of the discharge chamber tangentially to its side wall and lying in planes perpendicular to the axis of the electrodes.

As the studies conducted by the applicant have shown, the gas dynamics of the process in the discharge chamber is crucial for the performance of the device and the quality of the resulting product. When inert gas is supplied along the axis of the electrodes or the flow is twisted along the electrodes, which takes place in a prototype installation, there is a danger of arc breaking by a swirling gas flow and the device’s malfunction. In addition, part of the swirling flow captures the generated carbon vapor and deposits it on the side walls of the chamber. A flow directed or swirling along the axis of the electrodes moves the steam and soot to the chamber lid with a mounted SUBSTITUTE SHEET (RULE 26) current lead. In addition, the linear velocity of the gas along the chamber varies, which also contributes to the non-stationary nature of the process of carbon evaporation and, thus, reduces the device’s performance for fullerene-containing soot and fullerenes. These disadvantages are overcome in the inventive installation by supplying an inert gas from the side wall through the nozzles of at least two points tangentially with a flow swirling on both sides of the arc region. The carbon vapor generated in the electric arc is captured by the gas stream in the region of fullerene formation, i.e. in a torus with a radius of 8-10 radii of the electrode, and moves to the outlet pipe located against the interelectrode gap. It was also found that the optimal shape of the discharge chamber is a shape close to the sphere. Given the technological difficulties of manufacturing a spherical chamber, it was made in the form of two truncated cones connected by wide bases closed by spherical covers, which brings its shape closer to spherical.

The inert gas circulation system can be equipped with two pairs of nozzles, while the mentioned pairs of nozzles are 180 ° apart from each other.

The walls of the discharge chamber can be made cooled. At least one of the electrodes may be axially rotatable.

The horizontal location of the discharge chamber allows you to articulate with it in the arc region a collection of electrode residues directed vertically downward, which also increases the period of operation of the device until it is unloaded. The collection of graphite residues can be made cooled.

The collection of residual graphite can be equipped with a vacuum tight shutter. In this case, there is no need to stop the installation to remove fragments of electrodes from the reaction volume,

Means for capturing fullerene-containing soot can be made in the form of one or more cyclones with a tangential gas inlet installed at the inlet of the inert gas circulation system.

At least one cyclone can be made cooled (the first along the gas, which has a high temperature at the outlet of the discharge chamber). Cyclones can be equipped with a vacuum tight shutter, which allows them to be unloaded without stopping the device.

SUBSTITUTE SHEET (RULE 26) Additionally, the means for trapping fullerene-containing soot can be equipped with a bag filter at the outlet for complete trapping of soot when it can slip through the cyclone at high plant performance. The installation may be equipped with at least one device for supplying a graphite electrode to the discharge chamber.

The degassing chamber may be provided with a viewing window on the side surface.

The discharge chamber may be provided with a viewing window located opposite the zone of the electric arc.

The installation can be equipped with at least one device for supplying a graphite electrode to the discharge chamber to automate the operation of the device.

Both graphite electrodes can be mounted with the possibility of axial reciprocating movement.

Means for capturing fullerene-containing soot can be made in the form of two or three series-connected cyclones with a tangential gas inlet.

A brief description of the figures of the drawings The claimed invention is illustrated in the drawing, where in FIG. 1 shows a General view of the installation for the production of fullerene-containing soot, top view; in FIG. 2 shows a variant of the parallel axis of the electrodes of the gas flow in the installation of the prototype; in FIG. 3 shows a variant of a gas flow swirling along electrodes in a prototype installation; in FIG. 4 shows the nature of the gas flow in the inventive installation; in FIG. 5 is a longitudinal section of a discharge chamber; in FIG. 6 shows a section through the discharge chamber along A-A; in FIG. 7 shows one of the degassing chambers, a sectional side view; in FIG. 8 is a plan view of the camera of FIG. 7. FIG. 9 is a rear view of the current lead; in FIG. 10 shows a section through a current lead along B-B; in FIG. 11 is a sectional side view of a cyclone; in FIG. 12 is a C-C cyclone sectional view;

SUBSTITUTE SHEET (RULE 26) Embodiments of the invention

Installation for the production of fullerene-containing soot (see Fig. 1, Fig. 5) includes a horizontal sealed discharge chamber 1, in which along its axis there are two graphite rod electrodes 2, 3; nodes 4, 5 supply of graphite electrodes 2, 3; which can be supplemented by chambers 6, 7 by glow discharge degassing; cooled current leads 8, 9; an inert gas circulation system 10 (mainly helium) including a gas blower 11 for generating an inert gas stream and supplying it to the discharge chamber 1, a pipe 12 supplying an inert gas, a pipe 13 discharging fullerene soot and gas, and a means for collecting fullerene-containing soot 14, for example, in the form of three cyclones 15, 16 and 17 with a tangential inert gas inlet installed at the inlet of the inert gas circulation system 10. At the outlet of means 14, a known bag filter (not shown) can be installed. The electrodes 2, 3 can be installed with the possibility of axial reciprocating movement, and can also rotate around its axis. The discharge chamber 1 (see Fig. 5, Fig. 6) contains a housing 18 in the form of two truncated cones connected by wide bases, for example, with double side walls 19, 20, closed by removable convex spherical covers 21, 22, respectively, with flanges 23, 24 . In the center of the covers 21, 22 are made, respectively, windows 25, 26 for passage of the electrodes 2, 3. The inner wall 19 can be provided with two pairs of tangentially entering the wall 19 through the wall 20 of the nozzles 27, spaced 180 ° apart from the axis of the electrodes 2, 3. , 28 and 29, 30 connected to the pipe 12. The mouth of the nozzles 27, 28 and 29, 30 are separated from the axis of the electrodes 2, 3 at a distance of R> 45 mm. Between the pairs of nozzles 27, 28 and 29, 30, an outlet pipe 31 is cut into the wall 19, opposite the interelectrode gap, to remove the formed fullerene-containing soot from the discharge chamber 1 by the gas flow into the pipeline 13 and then into the cyclones 15, 16, 17. The discharge chamber 1 can be equipped with a cooled viewing window 32 for monitoring the electric arc and taking measurements of the temperature of the arc. The wall 20 and the flanges 23, 24 can be equipped with fittings 33, 34, 35, 36 for supplying a cooling agent, for example water, into the space between the walls 19 and 20, in the cavity between the covers 21, 22 and flanges 23, 24, respectively, for cooling discharge chamber 1. From the bottom, the chamber 1 is connected by a cooled pipe 37 with a collection of 38 residues. Residue collector 38 can be equipped with a vacuum-tight shutter (not shown in the drawing) to discharge residues without stopping the operation of the device. Electrodes 2 and 3 may be a SUBSTITUTE SHEET (RULE 26) pass respectively into the chamber 6, 7 degassing by glow discharge (see Fig. 7, Fig. 8) through the well-known seals 39, 40 Wilson (see, for example, Danilin B. S, Minaichev V. E. Fundamentals of designing vacuum systems. - M., Energy, 1971, S. 221), ensuring the tightness of the cavities of the chambers 6, 7. Each chamber 6, 7 (see Fig. 7, Fig. 8) contains a cylindrical body 41, along the axis of which a perforated cylindrical electrode 42 is installed, providing uniform volume distribution of plasma. The fitting 43 is connected to a vacuum system (not shown in the drawing). Each chamber 6, 7 can be equipped with a viewing window 44 for monitoring the state of the glow discharge, and is also equipped with nozzles 45, 46, respectively, for supplying and discharging inert gas (preferably argon), a fitting 47 for pumping out the internal cavities of the Wilson seals 40 and a 48 an insulating housing 49 for connecting to the positive terminal of a glow discharge power supply 50 (see FIG. 1). Terminals 51, 52 of current leads 8, 9 are connected through a switch 53 to an arc power source 54. The switch 53 allows you to change the polarity of the electrodes 2, 3. The outputs of the arc power source 54 are isolated from the ground. The nodes 4, 5 for supplying graphite electrodes 2, 3 can be of any known design (for example, in the form of a drum magazine holder, as in patent RU 2184700, IPC C01 B 31/02, published July 10, 2002; cassette type, as patent RU 39129, IPC C01 B 31/00, published July 20, 2004, in application US 20050019245, IPC B01 F 9/12, published January 27, 2005). Each of the current leads 8, 9 (see Fig. 9, Fig. 10) contains a metal washer 55 located between two curly ring insulators 56, 57. The washer 55 is electrically connected to the switch 53 using respectively terminals 51, 52 (see Fig. . one). Set: insulator 56, washer 55 and insulator 57 are clamped with studs 58 with nuts 59 between flange 60 and spacer 61 flange 61. Lower prismatic guide 63 with limiter 64 is rigidly attached to washer 55. Upper movable prismatic guide 65 is attached to spring washer 55 suspension 66 L-shaped with a bolt 67. The suspension 66 is made of a set of thin plates rigidly fastened at the ends, and provides vertical and horizontal movement of the upper movable prismatic guide 65 relative to the lower prismatic th guide 63. In the washer 55 channels 68 are made, connected to fittings 69, 70 for supplying and discharging a cooling agent. In the center of the washer 55, a centering hole 71 is made for the passage of the electrode (2 or 3). Spacer 62 may be provided with a viewing window 72 and a backlight 73 for REPLACEMENT SHEET (RULE 26) visual control over the location of the rails 63, 65. The cyclone 15 (see Fig. 11, Fig. 12) may include a cooled outer casing 74 with an inlet pipe 75, a cooled inner casing 76 with an outlet pipe 77 and a cooled receiver 78. The receiver 78 may be equipped with a vacuum tight damper (not shown in the drawing) for unloading soot without stopping the operation of the device. Since the temperature of the inert gas at the inlet to cyclones 16 and 17 is no longer as high as that at the inlet of cyclone 15, cyclones 16 and 17 may no longer require forced cooling. The fittings 79, 80, 81, 82, 83, 84 and 85 are intended for supplying a cooling agent to the outer casing 74, the inner casing 76 and the receiver 78 and for removing the cooling agent from them.

The production of fullerene-containing soot in the inventive installation is as follows. Graphite electrodes 2 and 3 are fed into current leads 8, 9 from nodes 4, 5, respectively. The internal volume of chamber 1, the inert gas circulation system 10, the internal cavities of Wilson seals 39, 40 and chambers 6, 7 are pumped out to a pressure of 410 ^"2 Torr s using a fore-vacuum pump equipped with a trap with liquid nitrogen, then the internal volume of the chamber 1 and the inert gas circulation system 10 of the installation is filled with an inert gas or a mixture of inert gases at a pressure of 50 Torr to atmospheric pressure (preferably up to a pressure of 50-300 Torr). 7 through n Tubes 45, 46 set the dynamic pressure of an inert gas (preferably argon) from 0.1 to 10 Torr (preferably 1 Torr). Plus 50 glow discharge sources are supplied to the cylindrical electrodes of 42 chambers 6, 7 and a glow discharge is ignited with a current from 1 to 100 mA (preferably 10 mA). The internal cavities of the Wilson 40 seals are pumped out continuously during the entire soot production process. Graphite electrodes 2 and 3 fed into the current leads 8, 9 from nodes 4, 5 respectively pass a glow discharge zone in chambers 6, 7. Electrodes 2 and 3 are fixed upper movable prismatic guide 65 and lower guide prism 63. The material of the electrodes 2 and 3 are normally circular graphite rods of 12 mm diameter and 400 mm in length. The gas supercharger 11 is turned on, while the inert gas emerging from the nozzles 27, 28 and 29, 30 is twisted on both sides of the interelectrode gap into two circular flows. The cooling agent is supplied to the current leads 8, 9 and in the cavity between the walls 19 and 20 of the covers 21, 22 and the flanges 23, 24. A voltage of negative polarity is applied to one of the electrodes 2 and 3, and a positive polarity from the source 53 of the arc discharge power supply to the other . A welding rectifier with a REPLACEMENT SHEET (RULE 26) can be used as a power source reverse current. The arc discharge is ignited between the electrodes 2, 3 and the operating mode of combustion is set (the set discharge current and the distance between the electrodes are 1, 0-5.0 mm), observing through the viewing window 32. Using a node 4 or 5 (depending on the polarity of the electrode) respectively supply a graphite electrode 2 or 3 (for example, electrode 2), set the feed rate necessary to maintain the interelectrode gap constant, and translate electrode 2 progressively, compensating for its evaporation in the arc discharge. At the same time, it can be rotated at a speed of 0.2-3.0 rpm / min (you can also rotate the electrode 3 in the opposite direction). The carbon vaporized from the electrode 2 leaves the arc zone in the radial direction and can partially be deposited on the electrode 3. After a certain time (preferably in the range of 2-30 minutes), the polarity of the electrodes 2 and 3 is reversed to evaporate the electrode 3, while unit 4 is stopped and turn on the node 5. The time of reversing the polarity of the discharge is chosen so that a deposit does not form on the electrodes 2, 3. After that, the polarity of the electrodes 2, 3 is changed again, the node 5 is stopped and the node 4 is turned on, and the process is repeated. Since the electrodes 2, 3 are made of graphite rods of finite length, as the electrodes 2, 3 evaporate, the following graphite rods are attached to their outer ends (for this purpose, for example, a cylindrical groove is made at one end of each rod, and the corresponding to this groove a ledge). Thus, ensure the continuous operation of the device. The electrodes 2, 3 during their movements passing through the chambers 6, 7, can be gassed in a glow discharge. The degassing products are removed from the chambers 6, 7 by pumping inert gas through the nozzles 45, 46. The annular flows of inert gas leaving the nozzles 27, 28 and 29, 30 pick up the formed products of the transformation of carbon atoms and transfer them from the discharge chamber through the outlet pipe 31 1 into the pipeline 13 and further into cyclones 15, 16, 17, where they are deposited in the form of fullerene-containing soot in the receivers 68. When supplying the collector 38, cyclones 15, 16, 17, vacuum-tight valves, the unloading of the residues of graphite and fullerene-containing soot can be made without stopping the mustache tanovki.

Industrial Applicability Examples. At the installation, the same as in FIG. 1, but with two cyclones 15, 16, experiments were carried out to obtain fullerene-containing soot. In the experiments, graphite rods with a diameter of 12 mm were used as electrodes 2, 3. Graphite was evaporated at an energy flow of 120-180 W / mm ² into a SUBSTITUTE SHEET (RULE 26) Helium was used as an inert gas at a pressure of 100 Torr, the interelectrode distance was changed in the range of 1.0–5.0 mm and outside this interval. The helium flow rate at the nozzle exit did not exceed 5 m / s. The electrodes passed through chambers 6, 7, in which their S degassing in a glow discharge took place. The electrodes were rotated around the axis at a speed of 0.2-3.0 rpm / min, and in some experiments they were not rotated. The amount of soot collected in cyclones 15, 16, and in the discharge chamber 1 was determined by the gravimetric method. The fullerenes contained in fullerene-containing soot were extracted by exhaustive extraction, and their concentration was determined by spectrophotometric method. The experimental results are shown in the table.

Table

^* α is the mass content of fullerenes; the difference up to 100% applies to fragments of graphite. 5 At the same time, comparative tests were carried out of the inventive installation and the experimental prototype installation of the applicant according to the patent of the Russian Federation N ° 2234457. The inventive installation works for several months in normal mode and stops only for a routine inspection.

The prototype installation had to be turned off 2-3 times a day due to arc failure. 0 On the second day of operation, the prototype installation failed due to burnout of the discharge chamber. The performance of the claimed installation was 2 times higher compared to the installation of the prototype.

SUBSTITUTE SHEET (RULE 26) As can be seen from the table, with an energy flow of 120-180 W / mm ² and the gas supply indicated above, a sufficiently complete removal of fullerene-containing soot from the chamber into cyclones and a stably high yield of fullerenes are achieved. In this case, there was no breakdown of the arc and burn-through of the chamber walls during the long-term operation of the inventive installation. Compared with a cylindrical discharge chamber, the inventive discharge chamber in the form of two truncated cones connected by wide bases closed by spherical caps provides the best gas dynamics of the process, which effectively affects the performance of the installation and minimizes product deposition on the chamber walls.

SUBSTITUTE SHEET (RULE 26)

Claims

CLAIM

1. Installation for the production of fullerene-containing soot, including a horizontal sealed discharge chamber with two graphite 5 rod electrodes placed in the cooled current leads and with an outlet pipe opposite the interelectrode gap, an inert gas circulation system with means for capturing the fullerene-containing soot, made in the form of two truncated cones connected by wide bases closed by spherical covers, at least one of

10 electrodes are mounted with the possibility of axial reciprocating movement, the inert gas circulation system connected to the said outlet pipe is provided with at least two nozzles mounted at the end walls of the discharge chamber tangentially to its side wall and lying in planes perpendicular to the axis of the electrodes.

15 2. The apparatus of claim 1, wherein the apparatus further includes at least one degassing chamber of said electrodes by a glow discharge.

3. Installation according to claim 1, characterized in that at least one of the electrodes is mounted with axial rotation.

20 4. Installation according to claim 1, characterized in that the inert gas circulation system is provided with two pairs of nozzles, while the said pairs of nozzles are 180 ° apart from each other,

5. Installation according to claim 1, characterized in that the walls of the discharge chamber are made cooled.

25 6. Installation according to claim 1, characterized in that the discharge chamber is equipped with a collection of graphite residues.

7. Installation according to claim 6, characterized in that the collection of graphite residues is made cooled.

8. Installation according to claim 6, characterized in that the collection of residues of graphite 30 is equipped with a vacuum-tight shutter.

9. Installation according to claim 1, characterized in that the means for collecting fullerene-containing soot is made in the form of at least one cyclone with a tangential gas inlet installed at the inlet of the inert gas circulation system.

35 10. Installation according to claim 9, characterized in that at least one cyclone is made cooled.

SUBSTITUTE SHEET (RULE 26)

11. Installation according to claim 9, characterized in that at least one cyclone is equipped with a vacuum tight damper.

12. Installation according to claim 1, characterized in that the discharge chamber is equipped with an inspection window located opposite the zone of the electric arc.

13. Installation according to claim 1, characterized in that it is equipped with at least one device for supplying a graphite electrode to the discharge chamber.

14. Installation according to claim 1, characterized in that the degassing chamber is provided with a viewing window on the side surface.

15. The device according to claim 1, characterized in that the means for collecting fullerene-containing soot is provided with a bag filter at the outlet.

SUBSTITUTE SHEET (RULE 26)