IP Library Granted Patent US 12,286,352
Granted Patent B2
US 12,286,352 · App. 17/554,293 · Granted Apr 29, 2025

Flame-synthesis of monolayer and nano-defective graphene

Inventors: Stephen D. Tse (Warren, NJ); Hua Hong (Weehawken, NJ); Bernard H. Kear (Whitehouse Station, NJ)
Assignee: Rutgers, the State University of New Jersey
C01B32/184B82Y40/00C01P2002/52C01P2002/82
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Quick Facts
Patent No.
US 12,286,352
App. No.
17/554,293
Granted
Apr 29, 2025
Kind
B2
Abstract

Methods for the production of carbon-based and other nanostructures are provided.

Claims (41)

1. An ultrafiltration membrane, wherein said ultrafiltration membrane comprises a nano-defective graphene film, wherein the nano-defective graphene film has an ID/IG ratio of 1.2 or higher, and wherein said nano-defective graphene film is a monolayer.

2. The ultrafiltration membrane of claim 1 , wherein said nano-defective graphene film is selected from the group consisting of sheets, plates, and discs.

3. The ultrafiltration membrane of claim 1 , wherein the nano-defective graphene film is synthesized by reacting an oxidizer and a fuel in a modified multiple, inverse-diffusion flame burner,

wherein said modified multiple, inverse-diffusion flame burner comprises delivery tubes for the fuel extending beyond a main burner surface, wherein said method comprises:

a) reducing a metal substrate in said modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel;

b) adding a hydrocarbon precursor through the fuel lines extending beyond the main burner surface of the modified, multiple inverse-diffusion flame burner to synthesize the graphene on said substrate; and, optionally,

c) annealing the flame-synthesized graphene of step b) by running the modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel.

4. The ultrafiltration membrane of claim 3 , wherein said method comprises annealing the flame-synthesized graphene of step b) by running the modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel.

5. The ultrafiltration membrane of claim 3 , wherein said metal substrate is less than 99.9% pure.

6. The ultrafiltration membrane of claim 3 , where the modified, multiple, inverse-diffusion-flame burner comprises an array of stabilized flames that form radially uniform temperature and species distribution downstream.

7. The ultrafiltration membrane of claim 3 , wherein the oxidizer is air, O 2 , or an oxidizing agent.

8. The ultrafiltration membrane of claim 3 , wherein the metal substrate is copper, nickel, steel, transition metals, alloys thereof, or spinels thereof.

9. The ultrafiltration membrane of claim 3 , where the fuel contains at least one additive, thereby forming doped nano-defective graphene films.

10. The ultrafiltration membrane of claim 9 , wherein the additive is a nitrogen species or a boron species.

11. The ultrafiltration membrane of claim 1 , wherein said nano-defective graphene film is doped with ions.

12. The ultrafiltration membrane of claim 11 , wherein said nano-defective graphene film is doped with ions in vacant atomic sites.

13. The ultrafiltration membrane of claim 11 , wherein said ions are metal ions.

14. A method of ultrafiltration, said method comprising passing a gas or liquid through the ultrafiltration membrane of claim 1 .

15. The method of claim 14 , wherein said ultrafiltration is ion selection, gas separation, water desalination, or gas molecule sensing.

16. The method of claim 14 , said method further comprising synthesizing said nano-defective graphene film.

17. The ultrafiltration membrane of claim 1 , wherein said nano-defective graphene film is a sheet.

18. An ultrafiltration membrane, wherein said ultrafiltration membrane comprises a nano-defective graphene film, wherein the nano-defective graphene film has an I D /I G ratio of 1.2 or higher, wherein said nano-defective graphene film is a sheet.

19. The ultrafiltration membrane of claim 18 , wherein said nano-defective graphene film is a monolayer or a few layer.

20. A method of ultrafiltration, said method comprising passing a gas or liquid through the ultrafiltration membrane of claim 18 .

21. The ultrafiltration membrane of claim 18 , wherein said nano-defective graphene film is a monolayer sheet.

22. A method of ultrafiltration, said method comprising passing a gas or liquid through the ultrafiltration membrane of claim 18 .

23. The method of claim 22 , wherein said ultrafiltration is ion selection, gas separation, water desalination, or gas molecule sensing.

24. An ultrafiltration membrane, wherein said ultrafiltration membrane consists of a nano-defective graphene film, wherein the nano-defective graphene film has an I D /I G ratio of about 0.6 or higher, and wherein said nano-defective graphene film is a monolayer.

25. A method of ultrafiltration, said method comprising passing a gas or liquid through the ultrafiltration membrane of claim 24 .

26. The method of claim 25 , wherein said ultrafiltration is ion selection, gas separation, water desalination, or gas molecule sensing.

27. An ultrafiltration membrane, wherein said ultrafiltration membrane consists of a nano-defective graphene film, wherein the nano-defective graphene film has an I D /I G ratio of about 0.6 or higher, wherein said nano-defective graphene film is a sheet.

28. A method of ultrafiltration, said method comprising passing a gas or liquid through the ultrafiltration membrane of claim 27 .

29. The method of claim 28 , wherein said ultrafiltration is ion selection, gas separation, water desalination, or gas molecule sensing.

30. A method of synthesizing an ultrafiltration membrane, wherein said ultrafiltration membrane comprises a nano-defective graphene film, wherein the nano-defective graphene film has an I D /I G ratio of about 0.6 or higher, said method comprising synthesizing the nano-defective graphene film by

a) reducing a metal substrate in said modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel, wherein said modified multiple, inverse-diffusion flame burner comprises delivery tubes for the fuel extending beyond a main burner surface;

b) adding a hydrocarbon precursor through the fuel lines extending beyond the main burner surface of the modified, multiple inverse-diffusion flame burner to synthesize the graphene on said substrate; and

c) annealing the flame-synthesized graphene of step b) by running the modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel.

31. A method of ultrafiltration, said method comprising passing a gas or liquid through an ultrafiltration membrane, wherein said ultrafiltration membrane comprises a nano-defective graphene film, wherein the nano-defective graphene film has an I D /I G ratio of about 0.6 or higher, said method further comprising synthesizing said nano-defective graphene film by:

a) reducing a metal substrate in a modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel, wherein said modified multiple, inverse-diffusion flame burner comprises delivery tubes for the fuel extending beyond a main burner surface;

b) adding a hydrocarbon precursor through the fuel lines extending beyond the main burner surface of the modified, multiple inverse-diffusion flame burner to synthesize the graphene on said substrate; and, optionally,

c) annealing the flame-synthesized graphene of step b) by running the modified, multiple inverse-diffusion flame burner wherein hydrogen (H 2 ) is the only fuel.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 19, 2022
From: TSE, STEPHEN D.; KEAR, BERNARD H.; HONG, HUA
To: RUTGERS, THE STATE UNIVERSITY OF NEW JERSEY
Reel/Frame 061232/0963 →
Continuity (3)
Continuation 16229055 · Dec 21, 2018
Provisional Application 62608739 · Dec 21, 2017
Related Publication 20220250913A1 · Aug 11, 2022
References Cited (42)
US 5000779A · German et al. · 1991 [cited by applicant]
US 5498278A · Edlund · 1996 [cited by applicant]
US 5604037A · Ting et al. · 1997 [cited by applicant]
US 5876683A · Glumac et al. · 1999 [cited by applicant]
US 6882094B2 · Dimitrijevic et al. · 2005 [cited by applicant]
US 6979433B1 · Saito et al. · 2005 [cited by applicant]
US 7157069B2 · Jurng et al. · 2007 [cited by applicant]
US 7279222B2 · Hearley et al. · 2007 [cited by applicant]
US 7323034B2 · Buxbaum · 2008 [cited by applicant]
US 7335344B2 · Height et al. · 2008 [cited by applicant]
US 7371065B2 · Aigner et al. · 2008 [cited by applicant]
US 7396520B2 · Howard et al. · 2008 [cited by applicant]
US 8845768B2 · Wachsman et al. · 2014 [cited by applicant]
US 9388042B2 · Tse et al. · 2016 [cited by applicant]
US 10099928B2 · Tse et al. · 2018 [cited by applicant]
US 20040050207A1 · Wooldridge et al. · 2004 [cited by applicant]
US 20110084237A1 · Wachsman et al. · 2011 [cited by applicant]
US 20110108521A1 · Woo et al. · 2011 [cited by applicant]
US 20130156678A1 · Banerjee et al. · 2013 [cited by applicant]
US 20130302693A1 · Sun · 2013 [cited by examiner]
US 20140054505A1 · Tse · 2014 [cited by examiner]
US 20140230653A1 · Yu · 2014 [cited by examiner]
US 20170125320A1 · Sung et al. · 2017 [cited by applicant]
WO 2009020958A2 · 2009 [cited by applicant]
Park, et al., Porous graphene-based membranes for water purification from metal ions at low differential pressures, Nanoscale 2016; 8: 9563-9571 (Year: 2016). [cited by examiner]
Memon, et al., Flame synthesis of graphene films in open environments, Carbon 2011; 49: 5064-5070 (Year: 2011). [cited by examiner]
Ossler, F., et al., “Sheet-Like Carbon Particles with Graphene Structures Obtained from a Bunsen Flame,” Carbon (2010) 48:4203-4206. [cited by applicant]
Xu, et al. “Synthesis of carbon nanotubes on metal alloy substrates with voltage bias in methane inverse diffusion flames” Carbon (2006) 44:570-577. [cited by applicant]
Rao, et al. “Fullerenes, nanotubes, onions and related carbon structures” Materials Science and Engineering (1995) R15:209-262. [cited by applicant]
Hu, et al. “Experimental and numerical investigation of non-premixed tubular flames” Proceedings of Combustion Institute (2007) 31:1093-1099. [cited by applicant]
Merchan-Merchan, et al. “Combustion synthesis of carbon nanotubes and related nanostructures” Process in Energy and Combustion (2010) 36:696-727. [cited by applicant]
Memon, et al. “Scalable Flame Synthesis of Carbon Nanotubes on Substrates” 2010 Materials Research Society Fall Meeting & Exhibit. Nov. 29, 2010; Abstract C4.10. Accessed online Aug. 8, 2013 <http://www.mrs.org/f10-abst… [cited by applicant]
Murayama, et al., “Uniform Deposition of Diamond Films using a Flat Flame Stabilized in the Stagnation-point Flow” J. Appl. Phy. (1991) 69(11):7924-7926. [cited by applicant]
Zhou, et al., “Synthesis of Carbon Nanotubes by Sequential Pyrolysis and Combustion of Polyethylene” (2010) Carbon 48:4024-4034. [cited by applicant]
Xu, F., “Investigating Flame-Based Synthesis of Carbon Nanotubes and Metal-Oxide Nanowires” (2007) Ph.D. Dissertation, Rutgers, The State University of New Jersey. [cited by applicant]
Rao, et al., “Fullerenes, Nanotubes, Onions and Related Carbon Structures” Mater. Sci. Engr. (1995) R15:209-262. [cited by applicant]
Liu, et al., “Rapid flame synthesis of multilayer graphene on SiO2/Si substrate” J Mater Sci: Mater Electron (2016) 27:2795-2799. [cited by applicant]
Yao, et al., “Monolayer graphene growth using additional etching process in atmospheric pressure chemical vapor deposition” Carbon (2012) 50:5203-5209. [cited by applicant]
Park, et al., “Porous graphene-based membranes for water purification from metal ions at low differential pressures” Nanoscale (2016) 8:9563-9571. [cited by applicant]
Huang, et al., “Graphene-Based Membranes for Molecular Separation” J. Phys. Chem. Lett. (2015) 6:2806-2815. [cited by applicant]
Perreault, et al., “Environmental applications of graphene-based nanomaterials” Chem. Soc. Rev. (2015) 44:5861-5896. [cited by applicant]
Liu, et al., “Graphene-based membranes” Chem. Soc. Rev. (2015) 44:5016-5030. [cited by applicant]