CN100411981C - Burner for synthesizing nanometer carbon pipe by V type and conical type pyrolytic flame and its synthesizing method - Google Patents
Burner for synthesizing nanometer carbon pipe by V type and conical type pyrolytic flame and its synthesizing method Download PDFInfo
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- CN100411981C CN100411981C CNB2006100767911A CN200610076791A CN100411981C CN 100411981 C CN100411981 C CN 100411981C CN B2006100767911 A CNB2006100767911 A CN B2006100767911A CN 200610076791 A CN200610076791 A CN 200610076791A CN 100411981 C CN100411981 C CN 100411981C
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Abstract
The present invention discloses a burner and a synthesizing method for synthesizing carbon nanotubes by V-shaped and conical pyrolysis flames, and belongs to the technical field of the synthesis of the carbon nanotubes. In the specific method, inflammable mixed gas is combusted by a V-shaped equicrural body or a cone in the burner to form a stable flame surface, and a high-temperature environment-heat source necessary to the synthesis of the carbon nanotubes is provided. Central gas flow has the three elements, namely the heat source, a carbon source and catalysts, of the synthesis of the carbon nanotubes through reactant mixed gas, inert gas and metal catalyst nanoparticles, wherein the reactant mixed gas, the inert gas and the metal catalyst nanoparticles pass through a central tube, and single-walled carbon nanotubes can be obtained in the burner and at an outlet. Heat and the synthesizing processes of the carbon nanotubes are separated by the pyrolysis flame method, which is favorable for the control of the synthesizing processes. The present invention has the advantage that a sampling mechanism with a continuous conveyor belt is used, and the preparation of the single-walled carbon nanotubes with controllability, continuous batch, large size, a large scale and low cost is realized. In addition, flame temperature can be changed by regulating the wall temperature of the burner, which is favorable for the control of the synthesizing processes.
Description
Technical field
The invention belongs to the carbon nanotube synthesis technical field, the burner and the synthetic method of V-type or pyramid type pyrolysis flame synthesizing carbon nanotubes particularly is provided.
Background technology
1991 Japanese scholar's Iijima (Iijima) at first found carbon nanotube (Carbon nanotubes, CNTs).Carbon current nanotube synthetic method mainly contains four kinds: (chemical vapor deposition is CVD) with flame synthesis method (flame synthesis) for arc discharge method (arc discharge), laser evaporation method (laser vapori zation), chemical Vapor deposition process.First three plants synthetic method equipment complexity, and the cost height is fit to small-scale, small size, interval type operation.The flame synthesis method has preparation continuously under atmospheric condition, and equipment is simple, and is energy-conservation, low cost, the potentiality of large size, extensive batch preparations.Flame synthesis method representative studies mainly contains more following at present:
The Vander wal of NASA etc. use laminar flow diffusion flame synthesizing carbon nanotubes at document " Vander wal RL; Ticich TM; Curtis VE.Diffusion Flme Synthesis of Single-walled Carbon Nanotubes.Chem PhysLett.2000; 354 (1-2): 20-4 " and the Yuan Liming of University of Kentucky etc. in " Yuan LM; SaitoK; Pan CX et al.Nanotubes from Methane Flames.Chem Phys Lett.2001,340 (3-4): 237-41 ".They adopt rich fuel gas from the ejection of 1mm pipe core, are another 5m pipe of blowing air on every side, form taper laminar flow diffusion flame.Sample probe with the containing metal catalyzer obtains multi-walled carbon nano-tubes in the inboard near flame front.Vander wal more uses document " Vander wal RL; Fe-Catalyzed.Single-walled Carbon NanotubesSynthesis within a Flame Environment.Combustion and Flme.2002; 130:37-47 " and " Vander wal RL; HaLi LJ; Berger CM.The Chemistry of PremixedFlame Synthesis of Carbon Nanotubes using Supported Catalysts.Proceedings of the Combustion Institute.2002,29:1079-1085 " to be called " pyrolysis flame " to come synthesizing carbon nanotubes.They adopt external diameter 50mm annular burner structure, and the outer shroud of burner is set up rich fuel premix flat flame as thermal source, and middle 11mm diameter pipe core outlet exports same plane (flushing) with outer shroud.Pipe core leads to containing metal catalyst nano particulate reaction gas mixtures, adds thinner again, reduces temperature.Above near burner, be arranged vertically a diameter 25mm thin-wall circular tube as stable cover.Collect Single Walled Carbon Nanotube in stable cover exit.Illinois university Saveliev etc. adopt head-on collision (adverse current) diffusion plane flame in document " Saveliev AV; Merchan-Merchar W; Kennedy LA.Metal Catalyzed Synthesisof Carbon Nanostructures in an Opposed Flow Methane Oxygen Flame.Combustion and Flame.2003,135:27-33 ".Two bursts of inverted draft head-on collisions of coming out from nozzle, one is rich fuel gas, another strand is oxygenant, obtains multi-walled carbon nano-tubes in fuel one side that forms flat flame with the sample probe that contains catalyzer.Height of Massachusetts Institute Technology and Howard etc. with the 0.067 normal atmosphere low pressure vessel burning acetylene premixed gas of oxygenation and thinner, obtain Single Walled Carbon Nanotube at the different heights place, laminar flow flat flame back of burner outlet in document " Height MT; Howard JB; Tester JW et al.FlameSynthesis of Single-walled Carbon Nanotubes.Carbon.2004; 42:2295-2307 ".The flame structure of above-mentioned representative studies and device all are fundamental researchs, can only obtain small amount of carbon nanotubes.Premix gas-bearing formation with acetylene, air and the thinner of one rich fuel in " NaKazawa S; YoKomori T; Mizomoto M.Flame Synthesis of Carbon Nanotubes in a WallStagnation Flow.Chemical Physics Letter.2005; 403:158-162 " such as Japan NaKazawa etc. flows jet, impact a pottery that catalyst n i layer is arranged in allocating plate, forming a tubaeform flame between the plate at jet exit with in allocating, is not fire reaction gas flow in the tubaeform flame.Generating multi-walled carbon nano-tubes in allocating on the very narrow endless belt of the adjacent flame front of plate.If slab design becomes conveyer structure, so this synthetic method might the bigger carbon nanotube of acquisition amount.But, owing to only generate a carbon nanotube in the extremely narrow endless belt of flame front gauge, if want a large amount of, then take very longly, efficient is lower.
Up to now, but still do not have the flame mode of continuous batch, controlled, large size, extensive synthesizing carbon nanotubes.
Summary of the invention
The object of the present invention is to provide the burner and the synthetic method of V-type or pyramid type pyrolysis flame synthesizing carbon nanotubes.It is characterized in that: the burner of described pyrolysis flame synthesizing carbon nanotubes is V-type isosceles body and pyramid type burner.
The concrete grammar of described pyrolysis flame synthesizing carbon nanotubes is: the inflammable mixture that enters from rectangular parallelepiped burner 3 or pipe burner 6 heads, the V-type isosceles body 1 or the cone 4 of both ends open are set in rectangular parallelepiped burner 3 or pipe burner 6, igniting makes the inflammable mixture burning, form the stationary flame face, provide synthesizing carbon nanotubes necessary hot environment-thermal source.The pipe core 2 that joins with V-type body 1 or cone 4 heads, or center pipe 5 feeds reactant gas mixture, rare gas element and metal-catalyst nanoparticles, reactant gas mixture and because the backflow effect that V-type body or cone cause, from the inflammable mixture of the outside, enter the imperfect combustion hydrocarbon polymer of central section, necessary second key element of synthesizing carbon nanotubes-carbon source is provided; And the metal-catalyst nanoparticles that is added to central gas stream provides necessary the three elements of synthesizing carbon nanotubes-catalyzer; So central gas stream has possessed the three elements of synthesizing carbon nanotubes, can synthesizing carbon nanotubes.Such V-type isosceles bodily form or conical pyrolysis flame separate heat and carbon nanotube building-up process.
Beneficial effect of the present invention is to adopt the continuous conveyor sampling mechanism, can accomplish controlled, continuous batch, large size, extensive, low-cost preparation Single Walled Carbon Nanotube.In addition, pyrolysis flame can change flame temperature by regulating the burner wall temperature, is beneficial to the control of building-up process.
Description of drawings
Fig. 1 is a V-type pyrolysis flame burner synoptic diagram.
Fig. 2 is a pyramid type pyrolysis flame burner synoptic diagram.
Embodiment
The invention reside in burner and synthetic method that V-type or pyramid type pyrolysis flame synthesizing carbon nanotubes are provided, the present invention is illustrated below in conjunction with accompanying drawing.
Figure 1 shows that V-type isosceles body heat separates the flame burner synoptic diagram.In the drawings, the V-type isosceles body 1 of both ends open and the rectangular centre pipe 2 of logical reactant gas mixture, rare gas element and metal-catalyst nanoparticles are set in the rectangular parallelepiped burner 3 of one end opening, pipe core 2 joins with V-type isosceles body 1 head opening end, V-type isosceles body 1 front and back sides flushes, seals with burner 3 front and back sidewalls, the logical inflammable mixture that is entered by burner 3 heads in the space between V-type isosceles body 1 left and right side and burner 3 left and right sides sidewalls.
Figure 2 shows that pyramid type pyrolysis flame burner synoptic diagram.The cone 4 of both ends open and the center pipe 5 of feeding reactant gas mixture, rare gas element and metal-catalyst nanoparticles at one end are set in the pipe burner 6 of opening, and center pipe 5 joins with cone 4 head opening ends.The logical inflammable mixture that enters by burner 6 heads in space between cone 4 sides and pipe burner 6 walls.
Concrete grammar with pyrolysis flame single-wall carbon nanotube synthesizing is example explanation the present invention below, enter inflammable mixture from burner head, described inflammable mixture is the pre-composition of geseous fuel and air (or oxygen), or be the liquid fuel of atomizing and the mixture of air (or oxygen), its fuel equivalence ratio (inverse of excess air ratio) is 1～2.2, and wherein geseous fuel is good with acetylene.The burner igniting, inflammable mixture stable burning.Pipe core feeds reactant gas mixture, rare gas element and metal-catalyst nanoparticles.The central reactant gas mixture can be carbon monoxide, hydrogen and rare gas element (as argon gas, helium, nitrogen), and carbon monoxide is separated out carbon by hydrogenization and hydrogen atom commentaries on classics shape carbon source is provided.To adopting iron is the situation of catalyzer, and reactivity ratio's acetylene of carbon monoxide is much better than, and carbon monoxide can cause the fragmentation of macrobead iron, and reaction surface is increased.Hydrogen makes hydrogenation of carbon monoxide separate out carbon, and Hydrogen Energy promotion dissociative carbon is absorbed the growth of promotion carbon nanotube by the iron particle.In addition, hydrogen can also keep activity of such catalysts.Rare gas element can reduce flame temperature as thinner, regulates flame temperature and reaches carbon nanotube synthetic temperature range (600 ℃～1300 ℃).Rare gas element also works to keep catalyst activity in addition.The throughput ratio of described reactant gas mixture carbon monoxide, hydrogen and rare gas element can be 0.5～1.5/0.5～1.5/0.5～1.5.The central reactant gas mixture is geseous fuel, hydrogen or oxygen and rare gas element also.Metal catalyst is commonly used nickel, iron, cobalt etc., can obtain the catalyst metal nano particle by sublimating technologe or pyrolysis spray technique from the nitrate solution of catalyst metal, and its concentration is between 200～10000ppm.Ferruginous catalyst nano particle is more suitable for the synthetic of Single Walled Carbon Nanotube.The metal catalyst particles size is advisable about with 1 nanometer.
V-type isosceles bodily form pyrolysis flame can enter sampling acquisition Single Walled Carbon Nanotube in the burner from the forward and backward sidewall of burner, also can take a sample at burner outlet.Conical pyrolysis flame can be taken a sample at burner outlet.
Claims (7)
1. the burner of V-type or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: the structure of described V-type burner is V-type isosceles body (1) and the logical reactant gas mixture that both ends open is set in the rectangular parallelepiped burner (3) of opening at one end, the rectangular centre pipe (2) of rare gas element and metal-catalyst nanoparticles, pipe core (2) joins with V-type isosceles body (1) head opening end, V-type isosceles body (1) front and back sides flushes with sidewall before and after the rectangular parallelepiped burner (3), sealing, the inflammable mixture for entering in the space between V-type isosceles body (1) left and right side and rectangular parallelepiped burner (3) left and right sides sidewall by rectangular parallelepiped burner (3) head;
The structure of described pyramid type burner is, the cone (4) of both ends open and the center pipe (5) of logical reactant gas mixture, rare gas element and metal-catalyst nanoparticles at one end are set in the pipe burner (6) of opening, center pipe (5) joins with cone (4) head opening end, the inflammable mixture for being entered by pipe burner (6) head in the space between cone (4) side and pipe burner (6) wall.
2. the method for the burner synthesizing carbon nanotubes of described V-type of claim 1 or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: concrete grammar is: the inflammable mixture that enters from rectangular parallelepiped burner (3) or pipe burner (6) head, by V-type isosceles body (1) in rectangular parallelepiped burner (3) or pipe burner (6) or cone (4) igniting, make the inflammable mixture burning, form the stationary flame face, provide synthesizing carbon nanotubes necessary hot environment-thermal source; The pipe core (2) or the center pipe (5) that join with V-type body (1) or cone (4) head feed reactant gas mixture, rare gas element and metal-catalyst nanoparticles, reactant gas mixture and because the backflow effect that V-type body or cone cause, from the inflammable mixture of the outside, enter the imperfect combustion hydrocarbon polymer of central section, necessary second key element of synthesizing carbon nanotubes-carbon source is provided; And the metal-catalyst nanoparticles that is added to central gas stream provides necessary the three elements of synthesizing carbon nanotubes-catalyzer; So central gas stream has possessed the three elements of synthesizing carbon nanotubes, can synthesizing carbon nanotubes.
3. according to the method for the burner synthesizing carbon nanotubes of described V-type of claim 2 or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: described inflammable mixture is the pre-composition of geseous fuel and air or oxygen, or is the liquid fuel of atomizing and the mixture of air or oxygen.
4. according to the method for the burner synthesizing carbon nanotubes of described V-type of claim 2 or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: described reactant gas mixture is carbon monoxide, hydrogen and rare gas element, or is geseous fuel, hydrogen or oxygen and rare gas element.
5. according to the method for the burner synthesizing carbon nanotubes of claim 2 or 4 described V-types or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: described rare gas element is argon gas, helium or nitrogen.
6. according to the method for the burner synthesizing carbon nanotubes of described V-type of claim 2 or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: described metal-catalyst nanoparticles is nickel, iron or cobalt.
7. according to the method for the burner synthesizing carbon nanotubes of described V-type of claim 2 or pyramid type pyrolysis flame synthesizing carbon nanotubes, it is characterized in that: described pyrolysis flame changes flame temperature by regulating the burner wall temperature.
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| Application Number | Priority Date | Filing Date | Title |
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| CNB2006100767911A CN100411981C (en) | 2006-04-21 | 2006-04-21 | Burner for synthesizing nanometer carbon pipe by V type and conical type pyrolytic flame and its synthesizing method |
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| CNB2006100767911A CN100411981C (en) | 2006-04-21 | 2006-04-21 | Burner for synthesizing nanometer carbon pipe by V type and conical type pyrolytic flame and its synthesizing method |
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| CN100411981C true CN100411981C (en) | 2008-08-20 |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102070139A (en) * | 2010-11-29 | 2011-05-25 | 华北电力大学 | V-shaped flame burner and method for synthesizing carbon nanotube array |
| CN102115075A (en) * | 2011-01-19 | 2011-07-06 | 华北电力大学 | Prismoid type flame combustor and synthesis method of carbon nanotube thereof |
| CN102491308A (en) * | 2011-11-25 | 2012-06-13 | 卓心康 | Method for synthesis of carbon nanostructure material by using organic material |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH05186209A (en) * | 1992-01-14 | 1993-07-27 | Nippon Kasei Chem Co Ltd | Production of carbon cluster c60 |
| CN1288076A (en) * | 1999-09-14 | 2001-03-21 | 鞍山钢铁集团公司 | Acid mist inhibitor for hydochloric acid pickling, and its prodn. method |
| WO2004083120A1 (en) * | 2003-03-14 | 2004-09-30 | Massachusetts Institute Of Technology | Method and apparatus for synthesizing filamentary structures |
| US20040201141A1 (en) * | 2003-04-12 | 2004-10-14 | Jongsoo Jurng | Apparatus and process for synthesis of carbon nanotubes or carbon nanofibers using flames |
| CN1549877A (en) * | 2001-08-30 | 2004-11-24 | TDA�о�����˾ | Burners and combustion apparatus for carbon nanomaterial production |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH05186209A (en) * | 1992-01-14 | 1993-07-27 | Nippon Kasei Chem Co Ltd | Production of carbon cluster c60 |
| CN1288076A (en) * | 1999-09-14 | 2001-03-21 | 鞍山钢铁集团公司 | Acid mist inhibitor for hydochloric acid pickling, and its prodn. method |
| CN1549877A (en) * | 2001-08-30 | 2004-11-24 | TDA�о�����˾ | Burners and combustion apparatus for carbon nanomaterial production |
| WO2004083120A1 (en) * | 2003-03-14 | 2004-09-30 | Massachusetts Institute Of Technology | Method and apparatus for synthesizing filamentary structures |
| US20040201141A1 (en) * | 2003-04-12 | 2004-10-14 | Jongsoo Jurng | Apparatus and process for synthesis of carbon nanotubes or carbon nanofibers using flames |
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