Process for the synthesis of fullerenes

• US 5,395,496 A
• Filed: 04/23/1993
• Issued: 03/07/1995
• Est. Priority Date: 04/07/1992
• Status: Expired due to Term

• Current Assignee: Pyrogenesis Canada, Inc.
• Original Assignee: Pegasus Refractory Materials, Inc.
• Inventors: Tsantrizos, Peter G., Grenier, Serge
• Primary Examiner(s): Lewis, Michael
• Assistant Examiner(s): KALINCHAK, STEPHEN
• Application Number:
  US08/051,556
• Time in Patent Office: 683 Days
• Field of Search: 423/445 B, 423/1, 204/173, 204/157.47
• US Class Current: 204/173
• CPC Class Codes: B82Y 30/00 Nanotechnology for materials or surface science, e.g. nanocomposites
• CPC Class Codes: B82Y 40/00 Manufacture or treatment of nanostructures
• CPC Class Codes: C01B 32/15 Nano-sized carbon materials
• CPC Class Codes: C01B 32/154 Preparation
• CPC Class Codes: Y10S 977/843 Gas phase catalytic growth, i.e. chemical vapor deposition

Abstract

A process is disclosed to synthesize fullerenes in a plasma reactor. It comprises introducing various amounts of carbon halides as the plasma forming gas in a plasma torch capable of producing a high enough temperature flame to dissociate the carbon bearing molecules into carbon and halogen atoms, hence forming a carbon cloud which condenses into a soot containing fullerenes. Also hydrocarbons can be introduced in the torch as the plasma forming gas and reacted with carbon halides or halogens injected therewith or directly into the plasma flame at the exit of the torch. Moreover, an inert gas, such as helium, may also be used as the plasma forming gas. The process can use a high enthalpy non-transferred d.c. plasma torch or an induction plasma torch as the plasma generating device.

Claims

1. A process for the synthesis of fullerenes which comprises:

a) feeding a plasma forming gas into a reactor and generating a plasma of said plasma forming gas within said reactor in the form of a plasma flame, said plasma forming gas consisting essentially of a carbon and halogen containing gas selected from the group-consisting of a carbon halide gas, a mixture of a carbon halide gas and a halogen gas, a mixture of a hydrocarbon gas and a halogen gas, a mixture of a hydrocarbon gas and a carbon halide gas, and a mixture of a hydrocarbon gas, a carbon halide gas and a halogen gas,

b) dissociating said plasma forming gas in said plasma flame into carbon and halogen atoms produced in the form of a cloud; and

then

c) allowing substantially all of the carbon atoms in said cloud to recombine and condense as soot on a surface outside of said plasma flame, said soot containing the fullerenes being formed from essentially only the carbon and halogen containing gas.

2. Process as defined in claim 1, in which the plasma forming gas is a carbon halide gas.

3. Process as defined in claim 2, in which the carbon halide gas is a CFC.

4. Process as defined in claim 2, in which the carbon halide gas is selected from CBrF₃ and C₂ Cl₄.

5. Process as defined in claim 1, in which the hydrocarbon gas is selected from CH₄ and C₂ H₂.

6. Process as defined in claim 1, in which the halogen gas is chlorine.

7. Process as defined in claim 1, in which the plasma forming gas is used in admixture with an inert gas.

8. Process as defined in claim 7, in which the inert gas is selected from helium and argon.

9. Process as defined in claim 1, in which the plasma forming gas is a mixture of a hydrocarbon gas and a halogen gas.

10. Process as defined in claim 1, in which the plasma forming gas is dissociated at temperatures between about 5,000°

C. and 20,000°

C.

11. Process as defined in claim 1, in which the reactor uses a non-transferred d.c. plasma torch for generating the plasma flame.

12. Process as defined in claim 1, in which the reactor uses an induction plasma torch for generating the plasma flame.

13. Process as defined in claim 1, in which soot with an admixture of C₆₀ and C₇₀ fullerenes is produced.

14. A process for the synthesis of fullerenes which comprises:

a) feeding a plasma forming gas into a reactor and generating a plasma of said plasma forming gas within said reactor in the form of a plasma flame, said plasma forming gas consisting essentially of a gas selected from the group consisting of a hydrocarbon gas and a mixture of a hydrocarbon gas and an inert gas;

b) feeding a halogen containing gas into said reactor, said halogen containing gas consisting essentially of a gas selected from the group consisting of a halogen gas, a carbon halide gas, a mixture of a halogen gas and a carbon halide gas, a mixture of a halogen gas and an inert gas, a mixture of a carbon halide gas and an inert gas, and a mixture of a halogen gas, a carbon halide gas and an inert gas,

c) dissociating said plasma forming gas and said halogen containing gas in said plasma flame into carbon and halogen atoms produced in the form of a cloud; and

then

d) allowing substantially all of the carbon atoms in said cloud to recombine and condense as soot on a surface outside of said plasma flame, said soot containing the fullerenes being formed from essentially only the carbon and halogen containing gas.

15. Process as defined in claim 14, in which the plasma forming gas is used to form the plasma flame and the halogen containing gas is injected into said plasma flame.

16. Process as defined in claim 14, in which the hydrocarbon gas is selected from CH₄ and C₂ H₂.

17. Process as defined in claim 14, in Which the inert gas in the plasma forming gas is helium.

18. Process as defined in claim 14, in which the halogen gas is chlorine.

19. Process as defined in claim 14, in which the carbon halide gas is selected from CBrF₃ and C₂ Cl₄.

20. Process as defined in claim 14, in which the inert gas in the halogen containing gas is argon.

21. Process as defined in claim 14, in which the plasma forming gas is dissociated at temperatures between about 5,000°

C. and 20,000°

C.

22. A process for the synthesis of fullerenes which comprises:

a) feeding a plasma forming gas consisting essentially of an inert gas into a reactor and generating a plasma of said plasma forming gas within said reactor in the form of a plasma flame;

b) injecting a carbon and halogen containing gas into said plasma flame, said carbon and halogen containing gas consisting essentially of a gas selected from the group consisting of a carbon halide gas, a mixture of a carbon halide gas and a halogen gas, a mixture of a hydrocarbon gas and a halogen gas, a mixture of a hydrocarbon gas and a carbon halide gas, and a mixture of a hydrocarbon gas, a carbon halide gas and a halogen gas;

c) dissociating said carbon and halogen containing gas in said plasma flame into carbon and halogen atoms produced in the form of a cloud; and

then

d) allowing substantially all of the carbon atoms in said cloud to recombine and condense as soot on a surface outside of said plasma flame, said soot containing the fullerenes being formed from essentially only the carbon and halogen containing gas.

23. Process as defined in claim 22, in which the inert plasma forming gas is helium.

24. Process as defined in claim 22, in which the carbon and halogen containing gas is a carbon halide gas.

25. Process as defined in claim 24, in which the carbon halide gas is selected from CBrF₃ and C₂ Cl₄.

26. Process as defined in claim 22, in which the carbon and halogen containing gas is used in admixture with an inert gas.

27. Process as defined in claim 26, in which the inert gas used with the carbon and halogen containing gas is argon.

28. Process as defined in claim 22, in which the plasma forming gas is dissociated at temperatures between about 5,000°

C. and 20,000°

C.