Method for preparing uniform single walled carbon nanotubes

• US 7,951,351 B2
• Filed: 03/29/2007
• Issued: 05/31/2011
• Est. Priority Date: 03/29/2006
• Status: Expired due to Fees

• Current Assignee: Hyperion Catalysis International Incorporated
• Original Assignee: Hyperion Catalysis International Incorporated
• Inventors: Ma, Jun, Tennent, Howard
• Primary Examiner(s): Michener; Jennifer K.
• Assistant Examiner(s): Barcena; Carlos
• Application Number:
  US11/693,261
• Publication Number:
  US 20080279751A1
• Time in Patent Office: 1,524 Days
• Field of Search: 423/447.3, 423/447.1, 423/445.R, 997/734, 977/735, 977/742, 977/750
• US Class Current: 423/447.3
• 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 2202/02 Single-walled nanotubes
• CPC Class Codes: C01B 2202/36 Diameter
• CPC Class Codes: C01B 32/154 Preparation
• CPC Class Codes: C01B 32/156 After-treatment
• CPC Class Codes: C01B 32/16 Preparation
• CPC Class Codes: C01B 32/162 characterised by catalysts
• CPC Class Codes: Y10S 977/735 Carbon buckyball
• CPC Class Codes: Y10S 977/742 Carbon nanotubes, CNTs
• CPC Class Codes: Y10S 977/75 Single-walled
• CPC Class Codes: Y10T 428/13 Hollow or container type article [e.g., tube, vase, etc.]
• CPC Class Codes: Y10T 428/2918 including free carbon or carbide or therewith [not as steel]

Abstract

Methods of preparing single walled carbon nanotubes from a metal catalyst having deposited thereon fullerenes are provided. Fullerenes are deposited onto a metal catalyst precursor or metal catalyst. In the presence of a carbon containing gas, the metal catalyst precursor/fullerene composition is then exposed to conditions suitable for reducing the metal catalyst precursor, for subliming the fullerene and for growing single walled carbon nanotubes. The fullerenes form the end caps for the resulting single walled carbon nanotubes, which are uniform in diameter.

Claims

1. A method for producing single walled carbon nanotubes comprising:

(a) reacting a carbon containing gas under reaction conditions with a composition comprising

fullerene on a precursor of a metal catalyst, wherein the precursor of a metal catalyst is coated with a thin film of fullerene, and

wherein said reaction conditions are suitable for reducing said metal catalyst precursor, said conditions being at atmospheric pressure or greater; and

(b) growing single walled carbon nanotubes, wherein said fullerene serves as a seed for growth of the single walled carbon nanotubes.

2. The method of claim 1, wherein said metal catalyst precursor comprises a metal selected from the group consisting of Fe, Co, Mn, Ni and Mo.

3. The method of claim 1, wherein said reaction conditions are suitable for non-subliming said fullerene, and wherein the temperature of said reaction condition is lower than the sublimation temperature of said fullerene.

4. The method of claim 1, wherein said single walled carbon nanotubes comprise a multiplicity of single walled carbon nanotubes, wherein at least 80% of the single walled carbon nanotubes in said multiplicity have a diameter within ±

5% of a single walled carbon nanotube diameter D present in said multiplicity, said diameter D being in the range between 0.6-2.2 nm.

5. The method of claim 4, wherein the diameter D is within the range of 1.0 to 1.8 nm.

6. The method of claim 4, wherein the diameter D is within the range of 1.2 to 1.6 nm.

7. The method of claim 1, wherein the composition comprising fullerene on a precursor of a metal catalyst is formed by a method comprising:

mixing fullerene into a solution of toluene;

adding a precursor of a metal catalyst to the solution;

mixing the precursor of a metal catalyst in the solution; and

evaporating the solution, thereby resulting in deposition of fullerene on the precursor of a metal catalyst.

8. The method of claim 1, wherein said metal catalyst precursor comprises a form selected from the group consisting of an oxide, chloride, oxalate, acetate, nitrate and carbonate.

9. The method of claim 1, wherein said metal catalyst precursor comprises a form selected from the group consisting of an chloride, oxalate, acetate, and carbonate.

10. A method for producing single walled carbon nanotubes comprising:

(a) forming a composition comprising fullerene on a precursor of a metal catalyst, wherein the precursor of a metal catalyst is coated with a thin film of fullerene,

(b) reacting a carbon containing gas in the presence of said composition under reaction conditions suitable for reducing said metal catalyst precursor, wherein the temperature of said reaction condition is lower than the sublimation temperature of said fullerene and the pressure of said reaction condition is 1 atmosphere or greater, and

(c) growing single walled carbon nanotubes having a single raman peak in the RBM region, wherein said fullerene serves as a seed for growth of the single walled carbon nanotubes.

11. The method of claim 10, wherein said single walled carbon nanotubes comprise a multiplicity of single walled carbon nanotubes, wherein at least 80% of the single walled carbon nanotubes in said multiplicity have a diameter within ±

5% of a single walled carbon nanotube diameter D present in said multiplicity, said diameter D being in the range between 0.6-2.2 nm.

12. The method of claim 11, wherein the diameter D is within the range of 1.2 to 1.6 nm.

13. A method for producing single walled carbon nanotubes comprising:

(a) forming a composition comprising fullerene on a metal catalyst, wherein the metal catalyst is coated with a thin film of fullerene,

(b) reacting a carbon containing gas in the presence of said composition at a temperature lower than the sublimation temperature of said fullerene and at atmospheric pressure or greater, and

(c) growing a multiplicity of single walled carbon nanotubes, wherein at least 80% of the single walled carbon nanotubes in said multiplicity have a diameter within ±

5% of a single walled carbon nanotube diameter D present in said multiplicity, said diameter D being in the range between 0.6-2.2 nm, wherein said fullerene serves as a seed for growth of the single walled carbon nanotubes.

14. The method of claim 13, wherein the diameter D is within the range of 1.2 to 1.6 nm.

15. The method of claim 13, wherein forming a composition comprising fullerene on a metal catalyst comprises:

mixing fullerene into a solution of toluene;

adding the metal catalyst to the solution;

mixing the metal catalyst in the solution; and

evaporating the solution, thereby resulting in deposition of fullerene on the metal catalyst.