Catalyst for producing carbon nanotubes and carbon nanotubes produced using same

Patent metadata

Field	Value
Publication number	US-9956546-B2
Application number	US-201414439168-A
Country	US
Kind code	B2
Filing date	Sep 30, 2014
Priority date	Sep 30, 2013
Publication date	May 1, 2018
Grant date	May 1, 2018

Abstract

Provided is a supported catalyst for producing carbon nanotubes with a large specific surface area. The supported catalyst enables the production of carbon nanotubes with a large specific surface area in high yield. Therefore, the catalyst can be used in various fields. Also provided are carbon nanotubes produced using the supported catalyst.

First claim

What is claimed is:

1. A catalyst for producing carbon nanotubes, comprising a support and a graphitization metal catalyst supported on the support and having a maximum diffraction peak at a 2θ angle of 35 to 38° in the XRD pattern recorded in the 2θ range of 10° to 80° wherein when the intensity of the maximum diffraction peak and the intensity of a diffraction peak at a 2θ angle of 17 to 22° are defined as “a” and “b”, respectively, the ratio b/a is 0.09 to 0.15,
wherein when the intensity of a diffraction peak at a 2θ angle of 63 to 67° is defined as “c”, the ratio c/a is in a range of 0.3 to 0.5,
wherein the graphitization metal catalyst is a multi-component metal catalyst comprising a main catalyst and an auxiliary catalyst,
wherein the main catalyst is selected from Co, Fe, and mixtures thereof and the auxiliary catalyst is V, and
wherein the catalyst is a supported catalyst obtained by calcining aluminum hydroxide at a primary calcination temperature of 250° C. to 500° C. to form the support, supporting a catalytic metal precursor on the support, and calcining the catalytic metal precursor supported on the support at a secondary calcination temperature of 450° C. to 800° C., the secondary calcination temperature being higher by 200 to 400° C. than the primary calcination temperature, and
wherein the catalyst has a crystal size of 3 to 50 nm.

2. The catalyst according to claim 1 , wherein the catalyst further has one or more diffraction peaks at 2θ angles of 30 to 33°, 43 to 46°, and 57 to 60.

3. The catalyst according to claim 1 , wherein the catalyst is adjusted to have a particle size of 30 to 150 μm and a number average particle diameter of 40 to 80 μm by sorting.

4. The catalyst according to claim 1 , wherein the graphitization metal catalyst comprises 0.1-10 moles of the auxiliary catalyst, based on 10 moles of the main catalyst.

5. The catalyst according to claim 1 , wherein the graphitization metal catalyst is supported in an amount of 5 to 40 parts by weight, based on 100 parts by weight of the catalyst.

6. A carbon nanotube aggregate comprising carbon nanotubes grown on the catalyst according to claim 1 wherein the carbon nanotube aggregate has a BET specific surface area of at least 200 m 2 /g and the BET specific surface area and the crystal size of the catalyst satisfy the following relationship:
y≤− 2.1 x+ 400
where y is the BET specific surface area (m 2 /g) and x is the crystal size of the catalyst (nm).

7. The carbon nanotube aggregate according to claim 6 , wherein the BET specific surface area of the carbon nanotube aggregate and the crystal size of the catalyst satisfy the following relationship:
−2.1 x+ 200≤ y≤− 2.1 x+ 400

where y is the BET specific surface area (m 2 /g) and x is the crystal size of the catalyst (nm).

8. A composite material comprising the carbon nanotube aggregate according to claim 6 .

9. The composite material according to claim 8 , wherein the composite material has a conductivity inversely proportional to the crystal size of the catalyst.

10. A method for producing a carbon nanotube aggregate, comprising bringing the catalyst according to claim 1 into contact with a carbon source in the gas phase to form carbon nanotubes (CNTs).

11. The method according to claim 10 , wherein the carbon source in the gas phase is selected from the group consisting of carbon monoxide, methane, ethane, ethylene, ethanol, acetylene, propane, propylene, butane, butadiene, pentane, pentene, cyclopentadiene, hexane, cyclohexane, benzene, toluene, and mixtures thereof.

12. The method according to claim 10 , wherein the catalyst reacts with the carbon source at a temperature of 600° C. to 750° C.

Assignees

• Lg Chemical Ltd

Inventors

• Kim Sungjin
• Cho Dong Hyun
• Kang Kyungyeon
• Son Seungyong
• Cha Jinmyung
• Jang Hyungsik
• Lee Seungyong
• Woo Jihee

Classifications

• C01B32/16

  Preparation · CPC title

• B01J23/8472 Primary

  Vanadium · CPC title

• B82Y30/00

  Nanotechnology for materials or surface science, e.g. nanocomposites · CPC title

• B01J37/10

  in the presence of water, e.g. steam · CPC title

• B01J23/8906

  Iron and noble metals · CPC title