METHOD OF MANUFACTURING GRAPHENE USING METAL CATALYST

• US 20140290565A1
• Filed: 10/18/2012
• Published: 10/02/2014
• Est. Priority Date: 10/24/2011
• Status: Active Grant

• Current Assignee: SRC Incorporated
• Original Assignee: SRC Incorporated
• Inventors: Kim, Kang Hyung, Maeng, Kwan Sub, Park, Chol Woo, Cha, Se Won, Hong, Se Youn, Hong, Byung Hee, Jung, Myung Hee, Kim, Kyung Eun, Park, Su Beom
• Granted Patent: US 9,776,875 B2
• Time in Patent Office: Days
• US Class Current: 117/94
• CPC Class Codes: B01J 23/50 Silver
• CPC Class Codes: B01J 23/52 Gold
• CPC Class Codes: B01J 23/72 Copper
• CPC Class Codes: B01J 23/8926 Copper and noble metals
• CPC Class Codes: B01J 35/30 characterised by their physical properties
• CPC Class Codes: B01J 37/18 with gases containing free hydrogen
• CPC Class Codes: B01J 37/348 Electrochemical processes, e.g. electrochemical deposition or anodisation
• 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 32/186 by chemical vapour deposition [CVD]
• CPC Class Codes: C01B 32/188 by epitaxial growth
• CPC Class Codes: C23C 16/0218 in a reactive atmosphere C23C16/0227 takes precedence
• CPC Class Codes: C23C 16/0281 of metallic sub-layers C23C16/029 takes precedence
• CPC Class Codes: C23C 16/26 Deposition of carbon only

Abstract

The present invention relates to a method for producing graphene on a face-centered cubic metal catalyst having a plane oriented in one direction, and more particularly to a method of producing graphene on a metal catalyst having the (100) or (111) crystal structure and a method of producing graphene using a catalyst metal foil having a single orientation, obtained by electroplating a metal catalyst by a pulse wave current and annealing the metal catalyst. The invention also relates to a method of producing graphene using a metal catalyst, and more particularly to a method of producing graphene, comprising the steps of: alloying a metal catalyst with an alloying element; forming step structures on the metal catalyst substrate in an atmosphere of a gas having a molecular weight of carbon; and supplying hydrocarbon and hydrogen gases to the substrate. On unidirectionally oriented metal catalyst prepared according to the present invention, graphene can be grown uniformly and epitaxially. Moreover, a method for producing graphene according to the present invention can form monolayer graphene by epitaxially growing graphene while increasing the growth rate of graphene.

Claims

1. A method of producing graphene, the method comprising:

forming step structures on the surface of a face-centered cubic metal catalyst substrate having a (100) or (111) orientation; and

supplying hydrocarbon to the substrate.

2. The method of claim 1, wherein the metal catalyst is a face-centered cubic metal catalyst having a cold rolling reduction ratio of 85% or higher and a (100) or (111) orientation.

3. The method of claim 1, wherein the metal catalyst has a thickness of 50 μ

m or less.

4. The method of claim 1, wherein the metal catalyst is recrystallization-annealed in a hydrogen or reducing atmosphere, and then heated in an atmosphere of methane and hydrogen to grow graphene thereon.

5. The method of claim 1, wherein the metal catalyst is any one selected from the group consisting of copper, silver, gold, and alloys thereof.

6. The method of claim 1, wherein 95% or more of the graphene is a monolayer graphene thin film.

7. The method of claim 1, wherein the metal catalyst is electroplated by a pulse wave current.

8. The method of claim 1, wherein the step structures are formed by annealing at a temperature of 600°

C. to 1070°

C.

9. The method of claim 7, wherein the pulse wave current is applied at a ratio of current supply time:

rest time of 15;

85 to 85;

15.

10. The method of claim 7, wherein the pulse wave current has a current density of 1-10 A/dm².

11. The method of claim 1, wherein the metal catalyst is a face-centered cubic metal foil obtained by plating a metal on a cathode rotating drum.

12. The method of claim 11, wherein the cathode rotating drum is polished to a roughness (Ra) of Ra 0.35 μ

m or less.

13. The method of claim 1, wherein the metal catalyst is alloyed with an alloying element, in which the alloying element is any one or more selected from among period 2 to period 6 elements among group 3 to group 12 transition metal elements and group 13 to 15 elements.

14. The method of claim 13, wherein the step structures on the metal catalyst are formed in an atmosphere of a gas having a molecular weight higher than the atomic weight of carbon.

15. The method of claim 13, wherein the metal catalyst is aluminum, nickel, autostenitic stainless steel, silver, gold or copper.

16. The method of claim 13, wherein the alloying element is any one or more of transition elements which have solid solubility for hydrogen or form carbides at a temperature ranging from 600 to 1060°

C.

17. The method of claim 13, wherein the alloying element is any one or more selected from among aluminum, indium, silicon, germanium, tin, antimony and bismuth.

18. The method of claim 14, wherein the gas having a molecular weight higher than the atomic weight of carbon is any one or more selected from among neon, argon, krypton, nitrogen, hydrocarbon, carbon dioxide, carbon monoxide and steam (H₂O).