IP Library Granted Patent US 9,005,460
Granted Patent B2
US 9,005,460 · App. 13/878,876 · Granted Apr 14, 2015

Layer-by-layer removal of graphene

Inventors: James M. Tour (Bellaire, TX); Ayrat M. Dimiev (Houston, TX); Dmitry V. Kosynkin (Dhahran, SA)
Assignee: William Marsh Rice University
C01B31/0484C01B31/0438C01B31/0469C01B31/0476H01L21/30604H01L21/3085B82Y30/00B82Y40/00
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Quick Facts
Patent No.
US 9,005,460
App. No.
13/878,876
Granted
Apr 14, 2015
Kind
B2
Abstract

The present invention provides methods of selectively removing one or more graphene layers from a graphene material by: (1) applying a metal to a surface of the graphene material; and (2) applying a hydrogen containing solution to the surface of the graphene material that is associated with the metal. The hydrogen containing solution dissolves the metal along with one or more layers of graphene associated with the metal, thereby removing the layer(s) of graphene from the graphene material. In some embodiments, the hydrogen containing solution is an acidic solution, such as hydrochloric acid. In some embodiments, the metal is zinc. In some embodiments, the methods of the present invention are utilized to selectively remove one or more layers of graphene from one or more targeted sites on the surface of a graphene material.

Claims (30)

1. A method of removing a single graphene layer from a graphene material, wherein the method comprises:

a. applying a metal to a surface of the graphene material,

wherein the graphene material has multiple graphene layers; and

b. applying a hydrogen containing solution to the surface of the graphene material that is associated with the metal,

wherein the hydrogen containing solution dissolves the metal along with a single layer of graphene associated with the metal, thereby removing the single layer of graphene from the graphene material.

2. The method of claim 1 , further comprising rinsing the graphene material, wherein the rinsing occurs after applying the hydrogen containing solution to the surface of the graphene material.

3. The method of claim 1 , further comprising drying the graphene material, wherein the drying occurs after applying the hydrogen containing solution to the surface of the graphene material.

4. The method of claim 1 , wherein the metal is applied to a targeted site on the surface of the graphene material.

5. The method of claim 1 , wherein the metal is applied to the entire surface of the graphene material.

6. The method of claim 1 , wherein graphene layers on the graphene material that are not associated with the metal remain intact after the removal of the single layer of graphene from the graphene material.

7. The method of claim 1 , wherein the graphene material is selected from the group consisting of graphene oxide, chemically converted graphene, partially reduced graphene oxide, chemical vapor deposited graphene, micromechanically cleaved graphene, graphite, highly ordered pyrollitic graphite, graphite oxide, and combinations thereof.

8. The method of claim 1 , wherein the metal is applied to the surface of the graphene material by sputtering, thereby forming sputtered metal atoms on the surface of the graphene material.

9. The method of claim 1 , wherein the metal is at least one of Zn, Al and Mg.

10. The method of claim 1 , wherein the metal is selected from the group consisting of Ni, Co, Fe, Pt, Au, Al, Ca, Cr, Cu, Mg, Mn, Mo, Rh, Si, Ta, Ti, W, U, V, Zr, and combinations thereof.

11. The method of claim 1 , wherein the metal has an oxidation potential greater than 0.5 Volts.

12. The method of claim 1 , wherein the hydrogen containing solution is an acidic solution comprising hydrochloric acid.

13. The method of claim 1 , wherein the hydrogen containing solution is a basic solution comprising sodium hydroxide.

14. The method of claim 1 , wherein the hydrogen containing solution is selected from the group consisting of acidic solutions, basic solutions, neutral solutions, aqueous solutions, non-aqueous solutions, and combinations thereof.

15. A method of selectively removing one or more graphene layers from a graphene material, wherein the method comprises:

a. applying a metal to a surface of the graphene material by sputtering,

wherein the graphene material has multiple graphene layers; and

b. applying a hydrogen containing solution to the surface of the graphene material that is associated with the metal,

wherein the hydrogen containing solution dissolves the metal along with one or more layers of graphene associated with the metal, thereby removing the one or more layers of graphene from the graphene material.

16. The method of claim 15 , wherein the number of graphene layers removed from the graphene material is controlled by sputtering power.

17. The method of claim 16 , wherein a single layer of graphene is removed from the graphene material.

18. The method of claim 16 , wherein two layers of graphene are removed from the graphene material.

19. The method of claim 15 , wherein the metal is applied to a targeted site on the surface of the graphene material.

20. The method of claim 15 , wherein the graphene material is selected from the group consisting of graphene oxide, chemically converted graphene, partially reduced graphene oxide, chemical vapor deposited graphene, micromechanically cleaved graphene, and combinations thereof.

21. The method of claim 15 , wherein the metal is at least one of Zn, Al and Mg.

22. The method of claim 15 , wherein the hydrogen containing solution is selected from the group consisting of acidic solutions, basic solutions, neutral solutions, aqueous solutions, non-aqueous solutions, and combinations thereof.

Assignments (3)
CONFIRMATORY LICENSE Recorded Oct 15, 2019
From: RICE UNIVERSITY
To: NAVY, SECRETARY OF THE UNITED STATES OF AMERICA
Reel/Frame 050730/0948 →
EXECUTIVE ORDER 9424, CONFIRMATORY LICENSE Recorded Jun 10, 2019
From: RICE UNIVERSITY
To: NAVY, SECRETARY OF THE UNITED STATES OF AMERICA
Reel/Frame 049890/0301 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 24, 2013
From: TOUR, JAMES M.; DIMIEV, AYRAT M.; KOSYNKIN, DMITRI V.
To: WILLIAM MARSH RICE UNIVERSITY
Reel/Frame 030483/0896 →
Continuity (2)
Provisional Application 61391936 · Oct 11, 2010
Related Publication 20130319973A1 · Dec 5, 2013