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

Patent metadata

Field	Value
Publication number	US-2017369323-A1
Application number	US-201715630758-A
Country	US
Kind code	A1
Filing date	Jun 22, 2017
Priority date	Jun 24, 2016
Publication date	Dec 28, 2017
Grant date	—

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 first temperature; adding a first oxidizing agent to the first solution to form a second solution; and quenching the second solution to a second temperature to form a carbon-based oxide material.

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 the mass of the acid is greater than the mass of the graphite by a factor of about 30 to about 180.

4 . The method of claim 1 , wherein the first temperature is 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 the mass of the first oxidizing agent is greater than the 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 over a period of time of about 15 minutes to about 180 minutes.

7 . The method of claim 1 , wherein a temperature of the second solution during the addition of the first oxidizing agent is less than about 30° C.

8 . The method of claim 1 , further comprising allowing the second solution to react at a third temperature over a first period of time wherein the third temperature is about 10° C. to about 70° C., and wherein the first period of time is about 15 minutes to about 120 minutes.

9 . The method of claim 1 , wherein the second solution is quenched to the second temperature by an ice bath, a water bath, one or more cooling coils, ice, water, by adding a second oxidizing agent to the second solution, or any combination thereof, and wherein the second temperature is about 25° C. to about 75° C.

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 9 , 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, and wherein a mass of the second oxidizing agent is greater than the mass of the graphite by a factor of about 1.5 to about 6.

12 . The method of claim 1 , further comprising agitating at least one of the first solution, and the second solution for a period of time of about 45 minutes to about 360 minutes.

13 . 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.

14 . The method of claim 1 , further comprising purifying the second solution, purifying the second solution comprises filtering the carbon-based oxide material through a filter and concentrating the carbon-based oxide material.

15 . The method of claim 14 , wherein the carbon-based oxide material is filtered until its pH is about 3 to about 7.

16 . The method of claim 1 , further comprising:
forming a third solution comprising the carbon-based oxide material and a third oxidizing agent; heating the third solution to a fourth temperature for a period of time; and adding a mineral ascorbate to the third solution to form a reduced carbon-based oxide material.

17 . The method of claim 16 , wherein heating the carbon-based oxide material to the fourth temperature, and adding a first quantity of the third oxidizing agent to the carbon-based oxide material, occur simultaneously.

18 . The method of claim 16 , wherein the fourth temperature is about 45° C. to about 180° C., and wherein heating the third solution to a fourth temperature occurs over a period of time of about 30 minutes to about 120 minutes.

19 . The method of claim 16 , 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 the mass of a second quantity of the third oxidizing agent is greater than the mass of the graphite by a factor of about 1.1 to about 6.

20 . The method of claim 16 , wherein the mineral ascorbate comprises sodium ascorbate, calcium ascorbate, potassium ascorbate, magnesium ascorbate, or any combination thereof.

21 . The method of claim 16 , wherein the mass of the mineral ascorbate is greater than the mass of the graphite by a factor of about 2 to about 10.

22 . The method of claim 16 , wherein the mineral ascorbate is added to the third solution over a period of time of about 10 minutes to about 60 minutes.

23 . The method of claim 16 , further comprising allowing the third solution and the mineral ascorbate to react for a period of time of about 45 minutes to about 180 minutes.

24 . The method of claim 16 , further comprising agitating the third solution for a period of time of about 45 minutes to about 360 minutes.

25 . The method of claim 16 , 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.

26 . The method of claim 16 , capable of producing a throughput of carbon-based oxide material of about 0.1 pound/day to about 50 pounds/day.

Assignees

• Univ California

Inventors

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

Classifications

• C01B7/00

  Halogens; Halogen acids (oxyacids C01B11/00) · CPC title

• C01B32/198

  Graphene oxide · CPC title

• C07D307/62 Primary

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

• C01B32/23 Primary

  Oxidation · CPC title

• C01B32/192

  starting from graphitic oxides · CPC title