Process for preparing carbon nanotube electrode comprising sulfur or metal nanoparticles as a binder

• US 7,531,267 B2
• Filed: 02/19/2004
• Issued: 05/12/2009
• Est. Priority Date: 06/02/2003
• Status: Expired due to Fees

• Current Assignee: KH Chemicals Co., Ltd.
• Original Assignee: KH Chemicals Co., Ltd.
• Inventors: Kim, Young Nam
• Primary Examiner(s): Ruthkosky; Mark
• Assistant Examiner(s): APICELLA, KARIE O
• Application Number:
  US10/783,265
• Publication Number:
  US 20040241532A1
• Time in Patent Office: 1,909 Days
• Field of Search: 429/44, 429/231.8, 502/101, 252/182.1
• US Class Current: 429/409
• CPC Class Codes: B82Y 30/00 Nanotechnology for materials or surface science, e.g. nanocomposites
• CPC Class Codes: H01G 11/28 arranged or disposed on a current collector; Layers or phases between electrodes and current collectors, e.g. adhesives
• CPC Class Codes: H01G 11/36 Nanostructures, e.g. nanofibres, nanotubes or fullerenes
• CPC Class Codes: H01G 11/38 Carbon pastes or blends; Binders or additives therein
• CPC Class Codes: H01G 11/86 specially adapted for electrodes carbonisation or activation of carbon for the manufacture of electrodes H01G11/34
• CPC Class Codes: H01M 4/583 Carbonaceous material, e.g. graphite-intercalation compounds or CFx
• CPC Class Codes: H01M 4/621 Binders
• CPC Class Codes: H01M 4/96 Carbon-based electrodes
• CPC Class Codes: H01M 8/0234 Carbonaceous material
• CPC Class Codes: Y02E 60/10 Energy storage using batteries
• CPC Class Codes: Y02E 60/13 Energy storage using capacitors
• CPC Class Codes: Y02E 60/50 Fuel cells

Abstract

The present invention provides an electrode made of carbon nanotubes or carbon nanofibers and a process for preparing the same. The electrode comprising a current collector, sulfur or metal nanoparicles as a binder, and carbon nanotubes or carbon nanofibers is characterized in that the sulfur or metal nanoparticles are bonded, deposited, or fused on the surfaces of the carbon nanotubes or carbon nanofibers so that the carbon nanotubes or carbon nanofibers are bonded to each other and also bonded to the current collector. The electrode prepared according to the present invention exhibits low internal resistance, strong durability and low equivalent series resistance, and therefore the electrode can be effectively used for secondary batteries, supercapacitors or fuel cells.

Claims

1. A process for preparing a carbon nanotube electrode,consisting:

(1) preparing an electrode material consisting essentially of carbon nanotubes mixed with a binder selected from the group consisting of sulfur having an average particle size of 1 μ

m or less, metal nanoparticles having an average particle size of 1 μ

m or less and both of them;

(2) preparing a pressed electrode material by first pressing the electrode material under a pressure from 1 to 500 atm or about 1.033 to about 516.615 kgf/cm²; and

(3) subsequently pressing under a pressure from 1 to 500 atm or about 1.033 to about 516.615 kgf/cm², or heat-treating at a temperature in the range of the melting point of the sulfur or metal nanoparticles ±

200°

C. in inert gas atmosphere, or simultaneously pressing under the said pressure and heat-treating at the said temperature in inert gas atmosphere the previously pressed electrode material that is placed on a current collector so that the carbon nanotubes are bonded to each other and simultaneously bonded to the current collector, by the binder being bonded, deposited, or fused on the surfaces of the carbon nanotubes;

wherein the binder has the effect of minimizing the internal resistance of the electrode.

2. The process according to claim 1, wherein in (2), the electrode material is uniformly dispersed on a current collector and then pressed, or simultaneously dispersed and pressed.

3. The process according to claim 1, wherein in (1), the mixing of carbon nanotubes with the binder is performed by a method chosen from the group consisting of physical mixing, ultrasonic-mixing, solvent-mixing, and uniformly dispersing the sulfur or metal nanoparticles on the surfaces of the carbon nanotubes.

4. The process according to claim 3, wherein the method of uniformly dispersing sulfur or metal nanoparticles on the surfaces of carbon nanotubes is carried out by a method selected from the group consisting of catalytic impregnation followed by an optional oxidation or reduction, precipitation, chemical vapor deposition (CVD), electrodeposition, plasma spraying, and sputtering.

5. The process according to claim 1, wherein the primary pressing in (2) provides the electrode material in the shape of a disk or thin film.

6. The process according to claim 1, wherein in (3), the pressing and the heat-treatment are carried out simultaneously or consecutively.

7. The process according to claim 1, wherein in (3), the heat-treatment is carried out by a heating method selected from the group of thermal heating, chemical vapor deposition, plasma heating, RF (radio frequency) heating, and microwave heating.

8. A secondary battery comprising the carbon nanotube electrode prepared according to the process of claim 1.

9. A process for preparing a carbon nanotube electrode, comprising:

(1) preparing an electrode material by depositing a binder selected from the group consisting essentially of sulfur having an average particle size of 1 μ

m or less, metal nanoparticles having an average particle size 1 μ

m of or less and both of them on the carbon nanotubes;

(2) preparing a pressed electrode material by first pressing the electrode material under a pressure from 1 to 500 atm or about 1.033 to about 516.615 kgf/cm²; and

(3) subsequently pressing under a pressure from 1 to 500 atm or about 1.033 to about 516.615 kgf/cm², or heat-treating at a temperature in the range of the melting point of the sulfur or metal nanoparticles ±

200°

C. in inert gas atmosphere, or simultaneously pressing under the said pressure and heat-treating at the said temperature in inert gas atmosphere the previously pressed electrode material that is placed on a current collector so that the carbon nanotubes are bonded to each other and simultaneously bonded to the current collector, by the binder being bonded, deposited, or fused on the surfaces of the carbon nanotubes;

wherein the binder has the effect of minimizing the internal resistance of the electrode.

10. The process according to claim 9, wherein in (2), the electrode material is uniformly dispersed on a current collector and then pressed, or simultaneously dispersed and pressed.

11. The process according to claim 9, wherein in (1), the depositing of the binder on the carbon nanotubes is performed by a method chosen from the group consisting of physical mixing, ultrasonic-mixing, solvent-mixing, and uniformly dispersing the sulfur or metal nanoparticles on the surfaces of the carbon nanotubes.

12. The process according to claim 11, wherein the method of uniformly dispersing sulfur or metal nanoparticles on the surfaces of carbon nanotubes is carried out by a method selected from the group consisting of catalytic impregnation followed by an optional oxidation or reduction, precipitation, chemical vapor deposition (CVD), electrodeposition, plasma spraying, and sputtering.

13. The process according to claim 9, wherein the primary pressing in (2) provides the electrode material in the shape of a disk or thin film.

14. The process according to claim 9, wherein in (3), the pressing and the heat-treatment are carried out simultaneously or consecutively.

15. The process according to claim 9, wherein in (3), the heat-treatment is carried out by a heating method selected from the group of thermal heating, chemical vapor deposition, plasma heating, RF (radio frequency) heating, and microwave heating.

16. A secondary battery comprising the carbon nanotube electrode prepared according to the process of claim 9.