DIRECT GROWTH OF GRAPHENE FILMS ON NON-CATALYST SURFACES

• US 20140120270A1
• Filed: 09/09/2011
• Published: 05/01/2014
• Est. Priority Date: 04/25/2011
• Status: Abandoned Application

• Current Assignee: Rice University
• Original Assignee: Rice University
• Inventors: Tour, James M., Yan, Zheng, Peng, Zhiwei, Sun, Zhengzong
• Application Number:
  US14/113,856
• Publication Number:
  US 20140120270A1
• Time in Patent Office: Days
• US Class Current: 427/596
• CPC Class Codes: B01J 23/755 Nickel
• 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 32/184 Preparation
• CPC Class Codes: C01B 32/186 by chemical vapour deposition [CVD]
• CPC Class Codes: C23C 16/26 Deposition of carbon only
• CPC Class Codes: H01L 21/02115 the material being carbon, e.g. alpha-C, diamond or hydrogen doped carbon
• CPC Class Codes: H01L 21/02263 deposition from the gas or vapour phase

Abstract

The present invention provides methods of forming graphene films on various non-catalyst surfaces by applying a carbon source and a catalyst to the surface and initiating graphene film formation. In some embodiments, graphene film formation may be initiated by induction heating. In some embodiments, the carbon source is applied to the non-catalyst surface before the catalyst is applied to the surface. In other embodiments, the catalyst is applied to the non-catalyst surface before the carbon source is applied to the surface. In further embodiments, the catalyst and the carbon source are applied to the non-catalyst surface at the same time. Further embodiments of the present invention may also include a step of separating the catalyst from the formed graphene film, such as by acid etching.

Claims

1. A method of growing a graphene film on a non-catalyst surface, wherein the method comprises:

(a) applying a carbon source and a catalyst to the non-catalyst surface; and

(b) initiating the formation of the graphene film from the carbon source on the non-catalyst surface.

2. The method of claim 1, wherein the carbon source is applied to the non-catalyst surface before the catalyst is applied to the surface, and wherein the carbon source forms a layer directly above the non-catalyst surface.

3. The method of claim 1, wherein the catalyst is applied to the non-catalyst surface before the carbon source is applied to the non-catalyst surface, and wherein the catalyst forms a layer directly above the non-catalyst surface.

4. The method of claim 1, wherein the catalyst and the carbon source are applied to the non-catalyst surface at approximately the same time.

5. The method of claim 1, wherein the non-catalyst surface is a non-metal substrate.

6. The method of claim 1, wherein the non-catalyst surface is an insulating substrate.

7. The method of claim 1, wherein the non-catalyst surface is selected from the group consisting of silicon (Si), silicon oxide (SiO₂), SiO₂/Si, silicon nitride (Si₃N₄), hexagonal boron nitride (h-BN), sapphire (Al₂O₃), and combinations thereof.

8. The method of claim 1, wherein the carbon source is selected from the group consisting of polymers, self-assembly carbon monolayers, organic compounds, non-polymeric carbon sources, non-gaseous carbon sources, gaseous carbon sources, and combinations thereof.

9. The method of claim 1, wherein the carbon source is a polymer selected from the group consisting of poly(2-phenylpropyl)methysiloxane (PPMS), poly(methyl methacrylate) (PMMA), polystyrene (PS), acrylonitrile butadiene styrene (ABS), high impact polystyrene (HIPS), polyacrylonitrile and combinations thereof.

10. The method of claim 1, wherein the carbon source comprises a nitrogen-doped carbon source.

11. The method of claim 1, wherein the carbon source is applied to the non-catalyst surface by a process selected from the group consisting of thermal evaporation, spin-coating, spray coating, dip coating, drop casting, doctor-blading, inkjet printing, gravure printing, screen printing, chemical vapor deposition, and combinations thereof.

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

13. The method of claim 1, wherein the catalyst is applied to the non-catalyst surface by a process selected from the group consisting of thermal evaporation, electron beam evaporation, sputtering, film pressing, film rolling, printing, ink jet printing, gravure printing, compression, vacuum compression, and combinations thereof.

14. The method of claim 1, wherein initiating graphene film formation comprises induction heating.

15. The method of claim 1, wherein the graphene film is formed in the presence of an inert gas selected from the group consisting of H₂, N₂, Ar and combinations thereof.

16. The method of claim 1, wherein the graphene film is formed at a temperature range between about 800°

C. and about 1100°

C.

17. The method of claim 1, wherein the formed graphene film is a bilayer.

18. The method of claim 1, further comprising separating the catalyst from the formed graphene film.

19. The method of claim 1, wherein a thickness of the graphene film is controlled by adjusting reaction conditions, wherein the reaction conditions are selected from the group consisting of carbon source type, carbon source concentration, carbon source thickness on the non-catalyst surface, inert gas flow rate, pressure, temperature, reaction time, reaction time at elevated temperatures, non-catalyst surface type, cooling rate and combinations thereof.

20. A method of growing a graphene film on a non-catalyst surface, wherein the method comprises:

(a) applying a carbon source and a metal catalyst to the non-catalyst surface;

(b) initiating the formation of the graphene film from the carbon source on the non-catalyst surface; and

(c) separating the metal catalyst from the formed graphene film.

21. The method of claim 20, wherein the non-catalyst surface is selected from the group consisting of silicon (Si), silicon oxide (SiO₂), silicon nitride (Si₃N₄), hexagonal boron nitride (h-BN), sapphire (Al₂O₃), and combinations thereof.

22. The method of claim 20, wherein the carbon source is selected from the group consisting of polymers, self-assembly carbon monolayers, organic compounds, non-polymeric carbon sources, non-gaseous carbon sources, gaseous carbon sources, and combinations thereof.

23. The method of claim 20, wherein the carbon source is a polymer selected from the group consisting of poly(2-phenylpropyl)methysiloxane (PPMS), poly(methyl methacrylate) (PMMA), polystyrene (PS), acrylonitrile butadiene styrene (ABS), high impact polystyrene (HIPS), polyacrylonitrile and combinations thereof.

24. The method of claim 20, wherein the metal catalyst is selected from the group consisting of Ni, Co, Fe, Pt, Au, Al, Cr, Cu, Mg, Mn, Mo, Rh, Si, Ta, Ti, W, U, V, Zr and combinations thereof.

25. The method of claim 20, wherein initiating graphene film formation comprises induction heating.

26. The method of claim 20, wherein the graphene film is formed in the presence of an inert gas selected from the group consisting of H₂, N₂, Ar, and combinations thereof.

27. The method of claim 20, wherein separating the metal catalyst from the formed graphene film comprises acid etching.

28. The method of claim 20, wherein a thickness of the graphene film is controlled by adjusting reaction conditions, wherein reaction conditions are selected from the group consisting of carbon source type, carbon source concentration, carbon source thickness on the non-catalyst surface, inert gas flow rate, pressure, temperature, reaction time, reaction time at elevated temperatures, non-catalyst surface type, cooling rate and combinations thereof.

29. The method of claim 20, wherein the formed graphene film is a bilayer.