WO2012067546A2 - Device for producing of fullerene-containing soot - Google Patents
Device for producing of fullerene-containing soot Download PDFInfo
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- WO2012067546A2 WO2012067546A2 PCT/RU2011/000891 RU2011000891W WO2012067546A2 WO 2012067546 A2 WO2012067546 A2 WO 2012067546A2 RU 2011000891 W RU2011000891 W RU 2011000891W WO 2012067546 A2 WO2012067546 A2 WO 2012067546A2
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/02—Apparatus characterised by being constructed of material selected for its chemically-resistant properties
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
- B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/152—Fullerenes
- C01B32/154—Preparation
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/02—Apparatus characterised by their chemically-resistant properties
- B01J2219/025—Apparatus characterised by their chemically-resistant properties characterised by the construction materials of the reactor vessel proper
- B01J2219/0277—Metal based
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
- B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
- B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
- B01J2219/0816—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes involving moving electrodes
- B01J2219/0818—Rotating electrodes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
- B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
- B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
- B01J2219/0816—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes involving moving electrodes
- B01J2219/082—Sliding electrodes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
- B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
- B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
- B01J2219/0822—The electrode being consumed
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0873—Materials to be treated
- B01J2219/0879—Solid
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0894—Processes carried out in the presence of a plasma
Definitions
- the invention relates to the field of fullerene-containing soot production.
- Carbon materials, including fullerene-containing soot and fullerenes itself have great prospects of usage in industry and medicine. But the latter is limiting by insufficiently elaborated technology of fullerenes synthesis and high prices as a consequence.
- the set is known for fullerene-containing soot production (Patent UM RU N Q 39129, C01 B 31/00, published 20.07.2004), containing plasma reactor implemented as cylindrical chamber with two graphite rod electrodes located along chamber axis - anode and cathode - fixed in cooled current-suppliers, thereby anode is equipped by axial movement device, reactor has a mean for inert gas supply and flow whirling coaxial to electrodes axis; gas supply gadget is accomplished providing the possibility of gas supply from cathode side. Gadget for inert gas supply is made as short pipe oriented tangentially to the side surface of chamber or as a nozzle, both providing gas flow whirling along chamber side wall.
- the set is known for fullerene-containing soot production
- Patent RU 2234457, C01 B 31/02, published 20.08.2004 including plasma reactor accomplished as hermetical cylindrical vaporization chamber with system of inert gas circulation, set for fullerene soot trapping and two graphite rod electrodes located along chamber axis.
- Circulation system is equipped by circular slot nozzle placed coaxially to electrodes. Slot nozzle may contain deflector for twisting of circular flow around said electrodes axis.
- Reactor is equipped additionally by chamber for degassing of movable graphite electrode by glowing discharge.
- the device is known for fullerene-containing soot production (Patent RU 2343111 , C01B 31/00, published 10.01.2009 WO 08123802) in accordance with which coaxial graphite electrodes, located in cooled current-suppliers, are mounted in horizontal hermetical discharge chamber equipped by waste collector.
- Fullerene-containing soot is producing in electric arc between electrodes. At least one of electrodes is mounted with ability of axial reciprocating movement or axial rotation. Discharge chamber is accomplished as two cutoff cones, connected by wide bases and closed by spherical lids. Inert gas circulation system is supplied by two pairs of nozzles, mounted at discharge chamber frontal walls tangentially to its side wall and laying at surfaces perpendicular to electrodes axis. Mean for fullerene-containing soot trapping is made as at least one cyclone with tangential gas input. Said apparatus is soot and fullerenes productive at minimum energy consumption; fullerene-containing soot is removed completely in course of the process.
- At least one of electrodes is mounted with ability of axial reciprocating displacement, circulation system has at least two nozzles mounted at frontal walls of cylindrical discharge chamber tangentially to its side wall and laying at surfaces perpendicular to electrodes axis, mean of soot trapping is implemented as at least one cyclone with tangential gas input and discharge chamber has waste collector.
- the known apparatus drawbacks are as follows: impossibility of optimization of temperature field in reactor independently from arc current, what prevents reaching of maximum fullerene output; significant part ( 25-30 %) of graphite evaporated in arc forms solid fragments of carbon stuff not containing fullerenes, i.e. is going in waste.
- the invention is directed to elaboration of effective arrangement for getting of fullerene-containing soot, enlarging of fullerene amount in soot and waste lessening.
- Device for fullerene-containing soot production includes cylindrical plasma reactor with two graphite electrodes mounted along reactor axis, at this graphite evaporation is occurred between said coaxially located graphite electrodes in cylindrical discharge chamber.
- the set includes system of inert gas circulation and system of fullerene-containing soot filtration, hereby inside said reactor the hollow cylinder and end lids of high-melting material are placed.
- Orifices for inert gas input and output are made in cylinder and portholes for graphite electrodes supply are implemented in end lids. Hollow cylinder and high-melting stuff end lids may touch tightly the inside metal walls of reactor. In other version the gap filled with inert gas may exist between hollow cylinder, end lids and reactor metal walls.
- Hollow cylinder and end lids may be manufactured from carbide of transient metal (titanium or zirconium or niobium) or from high- temperature ceramics. It is reasonable to produce the hollow cylinder and end lids from graphite. Thickness of mentioned hollow graphite cylinder and end graphite lids is not less than 5 mm. Inside surface of end lids may be made in shape of spherical segment.
- Hollow cylinder and end lids may be manufactured from carbide of transient metal (titanium or zirconium or niobium) or high-temperature ceramics.
- the most suitable material for present invention aim is graphite.
- Arrangement for fullerene-containing soot production includes cylindrical plasma reactor containing: horizontal cylindrical hermetical discharge chamber 1 with two graphite rod electrodes 2 , 3 at its axis; system 4 of inert gas (mostly helium) circulation, including gas supercharger 5 for creation of inert gas flow and its supply to discharge chamber 1 , pipeline 6 supplying soot-free inert gas, pipeline 7 pulling fullerene soot and gas out and mean 8 for fullerene-containing soot trapping , for example as a three cyclones 9, 10 and 11 with tangential input of inert gas, mounted at the input of system 4 of inert gas circulation .
- system 4 of inert gas (mostly helium) circulation including gas supercharger 5 for creation of inert gas flow and its supply to discharge chamber 1 , pipeline 6 supplying soot-free inert gas, pipeline 7 pulling fullerene soot and gas out and mean 8 for fullerene-containing soot trapping , for
- Electrodes 2, 3 are installed with ability of axial reciprocating movement and can also rotate around their axis. Hollow cylinder 12 and end lids 13, 14 of high-melted material are additionally mounted into discharge chamber 1. In cylinder 12 and in chamber casing the orifices are made: 15, 16 - for supply and 17 - for output of inert gas, and at end lids 13, 14 the orifices 18, 19 are provided for feeding of said graphite electrodes.
- Discharge chamber 1 may have cooled watching window for electrical arc monitoring. Discharge chamber may be cooled, for instance, by means of water flow. The same with cyclone 9. Inert gas temperature at cyclones 10, 11 input is not so high as at the cyclone 9 input, so cyclones 10, 11 may not need forced cooling.
- Arrangement for fullerene-containing soot production is functioning as follows. For instance, cylindrical graphite rods of 12 mm diameter and 400 mm length are used as electrodes. Out pumping of chamber 1 inner volume is carried out in system 4 of inert gas circulation till the pressure of 4.10-2 torr by means of forvacuum pump, equipped by trap with liquid nitrogen. Then inner volume of chamber 1 and inert gas circulation system 4 of apparatus are filled by inert gas or inert gases mixture at pressure from 50 torr till atmospheric (preferably till 100 - 300 torr). Then gas supercharger 5 is switched on. Agent for cooling chamber 1 and cyclone 9 is supplied. At one of electrodes 2 and 3 negative voltage is supplied and positive voltage at the other one from power supply unit for arc discharge.
- Welding rectifier with device for current polarity changing may be used as supply unit.
- Arc discharge between electrodes 2 and 3 is ignited, then operating burning mode is adjusted (proper discharge current and gap between electrodes 1.0 - 5.0 mm) .
- Feed of graphite electrode (e.g. 2) is switched on, feed velocity is tuned, needed for keeping of constant inter-electrodes gap and electrode 2 is moved straight forward for compensating its evaporation into arc discharge. Carbon evaporated from electrode 2 leaves arc zone radially.
- Graphite electrodes 2,3 are made as rods having limited length, so in process of their evaporation to the end of each the next rods are fixing (for that purpose each rod has slot at its one end and corresponding lug at the other) , providing by that incessant working process. Formed products of carbon atoms association are catched by inert gas streams and are transferred from discharge chamber 1 through pipeline 7 into cyclones 9, 10, 11 where they are deposited as a fullerene-containing soot. In case of providing of cyclones 9, 10, 11 by vacuum-tight dampers it is possible to unload fullerene- containing soot not stopping the operation of equipment.
- Content of fullerenes in soot is 10 - 12 %.
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Abstract
Device for fullerene-containing soot production comprises cylindrical plasma reactor, including horizontal cylindrical hermetical discharge chamber (1), where two graphite rod electrodes (2,3) are located along chamber axis; system of inert gas (mostly helium) circulation, comprising gas supercharger (5) for creation of inert gas flow and its supply into discharge chamber (1), pipeline (6) conducting soot-free inert gas, pipeline (7) taking out fullerene-containing soot and gas and mean (8) of fullerene soot trapping, for instance as a three cyclones (9, 10 and 11) with tangential supply of inert gas, mounted at the input of system (4) of inert gas circulation. Electrodes (2, 3) are installed with allowance of axial reciprocal movement. Hollow cylinder (12) and end lids (13, 14) of high-melted material are installed additionally into discharge chamber (1). Cylinder (12) and chamber casing have orifices for inert gas supply (15, 16) and output (17) and end lids (13, 14) have holes (18, 19) for feeding of said graphite electrodes.
Description
DEVICE FOR PRODUCING OF FULLERENE-CONTAINING SOOT
FIELD OF TECHNIQUE
The invention relates to the field of fullerene-containing soot production. Carbon materials, including fullerene-containing soot and fullerenes itself have great prospects of usage in industry and medicine. But the latter is limiting by insufficiently elaborated technology of fullerenes synthesis and high prices as a consequence.
BACKGROUND OF THE INVENTION
Well known method of fullerene-containing soot synthesis now is the arc method [A.Bogdanov, D.Dyninger, G.Diydzev. «Prospects of development of industrial methods for fullerenes production» JTPH, 2000, v.70, iss.5, p.1-7].
In arc reactor with graphite electrodes the erosion of anode electrode is occurred during arc ignition and the vapor arises from small carbon clusters which remove from arc nucleus towards reactor walls to the less temperature side. Over there in optimum temperatures zone - from 3000°K till 2000°K - various big carbon clusters are formed, including fullerenes predecessors and fullerenes itself (C60, C70 and heavier ones). The main part of big carbon clusters are further transforms into soot. Usually the mass yield of fullerenes is 10 -15 % of soot mass. Evidently that for reaching of maximum output of fullerenes it's necessary that the flow with optimum carbon vapor density would gone through optimum temperatures zone during optimal period. To reach optimum relation of mentioned parameters in common arc reactor is really impossible because they are changing simultaneously when arc current is changing
In issue [X.Song, Y.Liu, J.Zhu. The effect of furnace temperature on fullerene yield by a temperature controlled arc discharge. Carbon. 2006. V.44.N8. P.1584-1586.9] the influence was investigated of reactor wall temperature on fullerene yield inside direct current arc discharge. Stainless steel reactor was mounted in vacuum chamber and was able to be power-heated till 700 °C what lead to the heating of gas in reactor. In the center of reactor the arc was ignited between electrodes. Experiments showed that at rising of reactor temperature fullerenes yield is enlarged at first and reaches maximum 30.6 % at 200°C and then drops. The recession of fullerene yield at 200 - 400 °C has no physical grounding and most likely is explained by fullerenes sublimation from reactor walls and their outflow into vacuum chamber.
During laser ablation of graphite fullerenes are not formed in macroscopic amounts at temperature of buffer gas, surrounding graphite target, till 500 °C.
At further temperature rising the fullerenes appear in soot. Their yield reaches maximum of 20 % at 1200 °C .
The experimental results inevitably confirm the strong influence of temperature distribution in reactor at fullerenes yield as at laser so at arc synthesis
The set is known for fullerene-containing soot production (Patent UM RU NQ 39129, C01 B 31/00, published 20.07.2004), containing plasma reactor implemented as cylindrical chamber with two graphite rod electrodes located along chamber axis - anode and cathode - fixed in cooled current-suppliers, thereby anode is equipped by axial movement device, reactor has a mean for inert gas supply and flow whirling coaxial to electrodes axis; gas supply gadget
is accomplished providing the possibility of gas supply from cathode side. Gadget for inert gas supply is made as short pipe oriented tangentially to the side surface of chamber or as a nozzle, both providing gas flow whirling along chamber side wall.
The set is known for fullerene-containing soot production
(Patent RU 2234457, C01 B 31/02, published 20.08.2004), including plasma reactor accomplished as hermetical cylindrical vaporization chamber with system of inert gas circulation, set for fullerene soot trapping and two graphite rod electrodes located along chamber axis. Circulation system is equipped by circular slot nozzle placed coaxially to electrodes. Slot nozzle may contain deflector for twisting of circular flow around said electrodes axis. Reactor is equipped additionally by chamber for degassing of movable graphite electrode by glowing discharge.
Some of known set drawbacks are great amount of waste stuff and comparatively low soot yield.
The device is known for fullerene-containing soot production (Patent RU 2343111 , C01B 31/00, published 10.01.2009 WO 08123802) in accordance with which coaxial graphite electrodes, located in cooled current-suppliers, are mounted in horizontal hermetical discharge chamber equipped by waste collector.
Fullerene-containing soot is producing in electric arc between electrodes. At least one of electrodes is mounted with ability of axial reciprocating movement or axial rotation. Discharge chamber is accomplished as two cutoff cones, connected by wide bases and closed by spherical lids. Inert gas circulation system is supplied by two pairs of nozzles, mounted at discharge chamber frontal walls tangentially to its side wall and laying at surfaces perpendicular to
electrodes axis. Mean for fullerene-containing soot trapping is made as at least one cyclone with tangential gas input. Said apparatus is soot and fullerenes productive at minimum energy consumption; fullerene-containing soot is removed completely in course of the process.
Technically closest to claimed device is the arrangement for fullerene-contained soot production (Patent RU 2341451 , C01B 31/00 published 20.12.2008), containing horizontal, hermetical, cylindrical discharge chamber, two graphite electrodes located at chamber axis in cooled current-suppliers, gas circulation system equipped by fullerene-containing soot trapping mean.
Thereby at least one of electrodes is mounted with ability of axial reciprocating displacement, circulation system has at least two nozzles mounted at frontal walls of cylindrical discharge chamber tangentially to its side wall and laying at surfaces perpendicular to electrodes axis, mean of soot trapping is implemented as at least one cyclone with tangential gas input and discharge chamber has waste collector. The known apparatus drawbacks are as follows: impossibility of optimization of temperature field in reactor independently from arc current, what prevents reaching of maximum fullerene output; significant part ( 25-30 %) of graphite evaporated in arc forms solid fragments of carbon stuff not containing fullerenes, i.e. is going in waste.
DISCLOSURE OF THE INVENTION
The invention is directed to elaboration of effective arrangement for getting of fullerene-containing soot, enlarging of fullerene amount in soot and waste lessening. Device for fullerene-containing soot production includes cylindrical plasma reactor with two graphite
electrodes mounted along reactor axis, at this graphite evaporation is occurred between said coaxially located graphite electrodes in cylindrical discharge chamber. The set includes system of inert gas circulation and system of fullerene-containing soot filtration, hereby inside said reactor the hollow cylinder and end lids of high-melting material are placed. Orifices for inert gas input and output are made in cylinder and portholes for graphite electrodes supply are implemented in end lids. Hollow cylinder and high-melting stuff end lids may touch tightly the inside metal walls of reactor. In other version the gap filled with inert gas may exist between hollow cylinder, end lids and reactor metal walls.
Hollow cylinder and end lids may be manufactured from carbide of transient metal (titanium or zirconium or niobium) or from high- temperature ceramics. It is reasonable to produce the hollow cylinder and end lids from graphite. Thickness of mentioned hollow graphite cylinder and end graphite lids is not less than 5 mm. Inside surface of end lids may be made in shape of spherical segment.
The mounting of shallow cylinder and high-melting material end lids inside the reactor allows to rise sharply the temperature of inner walls of these elements in comparison with temperature of inner surface of metal walls water-cooled reactor itself which is close to 100 °C. Depending on material and dimensions of said elements, their disposal inside reactor , arc temperature and mode, temperature of their inner surface may lay in range of 1000 - 1500 °K. Such sharp rising of wall temperature leads to significant growth of zone length for temperatures optimal for fullerene synthesis (2000 - 3000 °K) what results in rising of effectiveness of fullerenes formation and enlarging of fullerenes content in the soot. Application of high-melted materials
for producing of mentioned cylinder and lids allows to use heat arising into arc itself for their heating till high temperatures. That permits to exclude the active heating of said elements by conducting the current through special heater and to rise by that reactor productivity, simplifying its design. Hollow cylinder and end lids may be manufactured from carbide of transient metal (titanium or zirconium or niobium) or high-temperature ceramics. The most suitable material for present invention aim is graphite.
BRIEF DESCRIPTION OF DRAWINGS
Fig.1 General view of for fullerene-containing soot production
Fig.2 Cut view of discharge chamber
a) version with junction oh discharge chamber 1 and hollow cylinder 12;
b) version with gap between chamber and cylinder;
Arrangement for fullerene-containing soot production (see fig.1 and fig.2) includes cylindrical plasma reactor containing: horizontal cylindrical hermetical discharge chamber 1 with two graphite rod electrodes 2 , 3 at its axis; system 4 of inert gas (mostly helium) circulation, including gas supercharger 5 for creation of inert gas flow and its supply to discharge chamber 1 , pipeline 6 supplying soot-free inert gas, pipeline 7 pulling fullerene soot and gas out and mean 8 for fullerene-containing soot trapping , for example as a three cyclones 9, 10 and 11 with tangential input of inert gas, mounted at the input of system 4 of inert gas circulation . At system exit 8 the known sleeve filter can be fixed ( not seen at the drawing). Electrodes 2, 3 are installed with ability of axial reciprocating movement and can also rotate around their axis. Hollow cylinder 12 and end lids 13, 14 of high-melted material are additionally mounted into discharge chamber
1. In cylinder 12 and in chamber casing the orifices are made: 15, 16 - for supply and 17 - for output of inert gas, and at end lids 13, 14 the orifices 18, 19 are provided for feeding of said graphite electrodes. Discharge chamber 1 may have cooled watching window for electrical arc monitoring. Discharge chamber may be cooled, for instance, by means of water flow. The same with cyclone 9. Inert gas temperature at cyclones 10, 11 input is not so high as at the cyclone 9 input, so cyclones 10, 11 may not need forced cooling.
BEST MODE FOR INVENTION ACCOMPLISHMENT
Arrangement for fullerene-containing soot production is functioning as follows. For instance, cylindrical graphite rods of 12 mm diameter and 400 mm length are used as electrodes. Out pumping of chamber 1 inner volume is carried out in system 4 of inert gas circulation till the pressure of 4.10-2 torr by means of forvacuum pump, equipped by trap with liquid nitrogen. Then inner volume of chamber 1 and inert gas circulation system 4 of apparatus are filled by inert gas or inert gases mixture at pressure from 50 torr till atmospheric (preferably till 100 - 300 torr). Then gas supercharger 5 is switched on. Agent for cooling chamber 1 and cyclone 9 is supplied. At one of electrodes 2 and 3 negative voltage is supplied and positive voltage at the other one from power supply unit for arc discharge. Welding rectifier with device for current polarity changing may be used as supply unit. Arc discharge between electrodes 2 and 3 is ignited, then operating burning mode is adjusted (proper discharge current and gap between electrodes 1.0 - 5.0 mm) . Feed of graphite electrode (e.g. 2) is switched on, feed velocity is tuned, needed for keeping of constant inter-electrodes gap and electrode 2 is moved straight forward for compensating its evaporation into arc
discharge. Carbon evaporated from electrode 2 leaves arc zone radially. Graphite electrodes 2,3 are made as rods having limited length, so in process of their evaporation to the end of each the next rods are fixing ( for that purpose each rod has slot at its one end and corresponding lug at the other) , providing by that incessant working process. Formed products of carbon atoms association are catched by inert gas streams and are transferred from discharge chamber 1 through pipeline 7 into cyclones 9, 10, 11 where they are deposited as a fullerene-containing soot. In case of providing of cyclones 9, 10, 11 by vacuum-tight dampers it is possible to unload fullerene- containing soot not stopping the operation of equipment.
INDUSTRIAL APPLICABILITY
Results of fullerene-containing soot production set are as follows.
Discharge current in range 300 - 400 A at inter-electrode gap
1.0 - 5.0 mm. Velocity of graphite electrode feed 8 - 20 mm/min. Waste in shape of solid fractions of carbon stuff not containing fullerenes - 15 - 20 %.
Content of fullerenes in soot is 10 - 12 %.
Claims
1. Device for producing of fullerene-containing soot is characterized by presence of cylindrical plasma reactor with two graphite electrodes located along reactor's axis, presence of inert gas circulation system and system of filtration of fullerene-containing soot, additional mounting of hollow cylinder equipped by end lids of high- melted material inside said reactor, hereby two orifices are implemented for inert gas input and output, and end lids have holes for feeding of said electrodes.
2. Device of claim 1 , characterized in that, hollow cylinder and end lids are in tight contact with inner metal walls of reactor.
3. Device of claim 1^ characterized in that, between hollow cylinder, end lids and reactor metal walls there is gap filled by inert gas.
4. Device of claim 1 , characterized in that, hollow cylinder and end lids are made from transient metal (titanium or zirconium or niobium) carbide.
5. Device of claim 1 , characterized in that, hollow cylinder and end lids are made from high-temperature ceramics.
6. Device of claim 1 , characterized in that, hollow cylinder and end lids are made from graphite.
7. Device of claim 1 , characterized in that, thickness of hollow graphite cylinder and end graphite lids is not less than 5 mm.
8. Device of claim 1 , characterized in that, inner surface of said end lids is implemented in shape of spherical segment.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| RU2010147069 | 2010-11-19 | ||
| RU2010147069 | 2010-11-19 |
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| WO2012067546A2 true WO2012067546A2 (en) | 2012-05-24 |
| WO2012067546A3 WO2012067546A3 (en) | 2012-08-30 |
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|---|---|---|---|
| PCT/RU2011/000891 Ceased WO2012067546A2 (en) | 2010-11-19 | 2011-11-14 | Device for producing of fullerene-containing soot |
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Cited By (19)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
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Family Cites Families (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE420529C (en) * | 1924-11-26 | 1925-10-26 | Georg Schaefer | Butyrometer |
| RU2259942C2 (en) * | 2003-09-09 | 2005-09-10 | Закрытое акционерное общество "ФУЛЛЕРЕН-ЦЕНТР" (ЗАО "ФУЛЛЕРЕН-ЦЕНТР") | Method of production of $$$ and $$$ fullerenes and reactor for production of fullerene black |
| RU2341451C1 (en) * | 2007-03-30 | 2008-12-20 | Общество с ограниченной ответственностью "Научно-производственная компания "НеоТекПродакт" | Method of production of fullerene-containing soot and device to this end |
| RU2343111C1 (en) * | 2007-04-06 | 2009-01-10 | Общество с ограниченной ответственностью "Научно-производственная компания "НеоТекПродакт" | Plant for fullerene soot production |
-
2011
- 2011-11-14 WO PCT/RU2011/000891 patent/WO2012067546A2/en not_active Ceased
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