Production of carbon-based oxide and reduced carbon-based oxide on a large scale

Patent metadata

Field	Value
Publication number	US-11097951-B2
Application number	US-201715630758-A
Country	US
Kind code	B2
Filing date	Jun 22, 2017
Priority date	Jun 24, 2016
Publication date	Aug 24, 2021
Grant date	Aug 24, 2021

Abstract

Provided herein are carbon-based oxide (CBO) materials and reduced carbon-based oxide (rCBO) materials, fabrication processes, and devices with improved performance and a high throughput. In some embodiments, the present disclosure provides materials and methods for synthesizing CBO and rCBO materials. Such methods avoid the shortcomings of current synthesizing methods to facilitate facile, high-throughput production of CBO and rCBO materials.

First claim

What is claimed is:

1. A method for producing a carbon-based oxide material comprising:
forming a first solution comprising graphite and an acid;
cooling the first solution to a temperature that is at most about 30° C.;
adding a first oxidizing agent to the first solution to form a second solution;
quenching the second solution to a temperature that is at most about 75° C. to form a carbon-based oxide material, and purifying the carbon-based oxide material, wherein the carbon-based oxide material is filtered until a pH from about 5 to about 7 is achieved, wherein reactions from the first oxidizing agent are neutralized;
forming a third solution comprising the carbon-based oxide material and a second oxidizing agent; and
heating the third solution to a temperature of at least about 45° C.

2. The method of claim 1 , wherein the acid comprises perchloric acid, hydroiodic acid, hydrobromic acid, hydrochloric acid, sulfuric acid, p-toluenesulfonic acid, methanesulfonic acid, or any combination thereof.

3. The method of claim 1 , wherein a mass of the acid is greater than a mass of the graphite by a factor of about 30 to about 180.

4. The method of claim 1 , wherein the first solution comprising the graphite and the acid is cooled to a temperature from about −20° C. to about 30° C.

5. The method of claim 1 , wherein the first oxidizing agent comprises oxygen, ozone, hydrogen peroxide, fluorite dioxide, lithium peroxide, barium peroxide, fluorine, chlorine, nitric acid, nitrate compounds, sulfuric acid, peroxydisulfuric acid, peroxymonosulfuric acid, chlorite, chlorate, perchlorate, halogen compounds, hypochlorite, hypohalite compounds, household bleach, hexavalent chromium compounds, chromic acids, dichromic acids, chromium trioxide, pyridinium chlorochromate, chromate compounds, dichromate compounds, permanganate compounds, potassium permanganate, sodium perborate, nitrous oxide, potassium nitrate, sodium bismuthate, or any combination thereof, and wherein a mass of the first oxidizing agent is greater than a mass of the graphite by a factor of about 1.5 to about 12.

6. The method of claim 1 , wherein the first oxidizing agent is added to the first solution comprising the graphite and the acid over a period of time of about 15 minutes to about 180 minutes.

7. The method of claim 1 , further comprising allowing the second solution comprising the first oxidizing agent to react at a temperature from about 10° C. to about 70° C., prior to quenching said second solution.

8. The method of claim 1 , wherein quenching the second solution occurs via an ice bath, a water bath, one or more cooling coils, ice, water, addition of a third oxidizing agent to the second solution, or any combination thereof, and wherein a temperature of the second solution after quenching is from about 25° C. to about 75° C.

9. The method of claim 8 , wherein the third oxidizing agent comprises oxygen, ozone, hydrogen peroxide, fluorite dioxide, lithium peroxide, barium peroxide, fluorine, chlorine, nitric acid, nitrate compounds, sulfuric acid, peroxydisulfuric acid, peroxymonosulfuric acid, chlorite, chlorate, perchlorate, halogen compounds, hypochlorite, hypohalite compounds, household bleach, hexavalent chromium compounds, chromic acids, dichromic acids, chromium trioxide, pyridinium chlorochromate, chromate compounds, dichromate compounds, permanganate compounds, potassium permanganate, sodium perborate, nitrous oxide, potassium nitrate, sodium bismuthate, or any combination thereof, and wherein a mass of the second oxidizing agent is greater than a mass of the graphite by a factor of about 1.5 to about 6.

10. The method of claim 1 , wherein quenching the second solution occurs over a period of time of about 30 minutes to about 120 minutes.

11. The method of claim 1 , further comprising agitating at least one of 1) the first solution comprising the graphite and acid, and 2) the second solution comprising the graphite, acid and first oxidizing agent, wherein said agitating occurs for a period of time of about 45 minutes to about 360 minutes.

12. The method of claim 1 , further comprising allowing the second solution to react for a period of time of about 15 minutes to about 120 minutes after the second solution is quenched, wherein the second solution during reaction has a temperature that is about 15° C. to about 75° C.

13. The method of claim 1 , wherein purifying the second solution comprises filtering the carbon-based oxide material through a first filter and concentrating the carbon-based oxide material.

14. The method of claim 1 , wherein heating the third solution and adding the second oxidizing agent occur simultaneously.

15. The method of claim 1 , wherein the third solution is heated from about 45° C. to about 180° C., and wherein heating the third solution occurs over a period of time of about 30 minutes to about 120 minutes.

16. The method of claim 1 , wherein the second oxidizing agent comprises oxygen, ozone, hydrogen peroxide, fluorite dioxide, lithium peroxide, barium peroxide, fluorine, chlorine, nitric acid, nitrate compounds, sulfuric acid, peroxydisulfuric acid, peroxymonosulfuric acid, chlorite, chlorate, perchlorate, halogen compounds, hypochlorite, hypohalite compounds, household bleach, hexavalent chromium compounds, chromic acids, dichromic acids, chromium trioxide, pyridinium chlorochromate, chromate compounds, dichromate compounds, permanganate compounds, potassium permanganate, sodium perborate, nitrous oxide, potassium nitrate, sodium bismuthate, or any combination thereof.

17. The method of claim 16 , wherein the second oxidizing agent is hydrogen peroxide.

18. The method of claim 1 , capable of producing a throughput of carbon-based oxide material of about 0.1 pound/day to about 50 pounds/day.

19. The method of claim 1 , further comprising adding a reducing agent to the third solution to form a reduced carbon-based oxide material.

20. The method of claim 19 , wherein the reducing agent comprises sodium ascorbate, calcium ascorbate, potassium ascorbate, magnesium ascorbate, or any combination thereof.

21. The method of claim 19 , wherein the reducing agent is added to the third solution over a period of time of about 10 minutes to about 60 minutes.

22. The method of claim 19 , further comprising allowing the third solution and the reducing agent to react for a period of time of about 45 minutes to about 180 minutes.

23. The method of claim 19 , further comprising agitating the third solution for a period of time of about 45 minutes to about 360 minutes.

24. The method of claim 19 , further comprising purifying the reduced carbon-based oxide material, wherein purifying the reduced carbon-based oxide material comprises filtering with a second filter, flushing the third solution, or any combination thereof.

Assignees

• Univ California

Inventors

• Kowal Matthew
• Kaner Richard B
• El-Kady Maher F

Classifications

• C01B32/23 Primary

  Oxidation · CPC title

• C01B32/198

  Graphene oxide · CPC title

• C01B2204/28

  Solid content in solvents · CPC title

• C01B32/192

  starting from graphitic oxides · CPC title

• C07D307/62 Primary

  Three oxygen atoms, e.g. ascorbic acid · CPC title