Methods of preparing carbonaceous material

• US 8,920,680 B2
• Filed: 04/08/2011
• Issued: 12/30/2014
• Est. Priority Date: 04/08/2010
• Status: Expired due to Fees

• Current Assignee: Pyrotek Incorporated
• Original Assignee: Pyrotek Incorporated
• Inventors: Mao, Zhenhua
• Primary Examiner(s): Kopec, Mark
• Assistant Examiner(s): NGUYEN, HAIDUNG D
• Application Number:
  US13/083,094
• Publication Number:
  US 20110248212A1
• Time in Patent Office: 1,362 Days
• Field of Search: 427/212, 427/220, 423/364, 429/231.8, 252/502
• US Class Current: 252/502
• CPC Class Codes: C01B 32/05 Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
• CPC Class Codes: H01M 10/0525 Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
• CPC Class Codes: H01M 4/587 for inserting or intercalating light metals
• CPC Class Codes: Y02E 60/10 Energy storage using batteries
• CPC Class Codes: Y02E 60/50 Fuel cells

Abstract

Methods and apparatus relate to methods of making carbonaceous material or coating from a precursor. Oxidation of hydrocarbons forming the precursor occurs upon adding an oxidation agent to a mixture of the precursor and a solvent for the precursor. The oxidation of the hydrocarbons yields constituents that are insoluble in the solvent and may not melt. The constituents that are insoluble in the solvent may further coat solid particles, if the solid particles are provided in the mixture. Carbonization of solids recovered by separation from liquids in the mixture increases carbon weight percent of the constituents that are insoluble in the solvent. The methods result in products that provide the carbonaceous material or coating and are suitable for use in electrodes.

Claims

1. A method, comprising:

preparing a mixture containing hydrocarbons and a solvent for the hydrocarbons wherein the boiling point of the hydrocarbons is higher than that of the solvent;

adding an oxidizer to the mixture and reacting the hydrocarbons with the oxidizer to increase concentration of constituents of the mixture that are insoluble in the solvent;

separating the mixture into liquids and solids where the solids are including the constituents that are insoluble in the solvent and such that the solvent is generally separated with the liquid; and

carbonizing the constituents that are insoluble in the solvent to provide carbonaceous material.

2. The method according to claim 1, wherein the oxidizer is liquid and is selected from nitric acid, thionyl chloride, peroxide, perchloric acid and benzoyl peroxide.

3. The method according to claim 1, wherein the oxidizer is gaseous and is selected from oxygen, ozone, nitrogen dioxide and sulfur trioxide.

4. The method according to claim 1, wherein the oxidizer includes ammonium persulfate.

5. The method according to claim 1, wherein the solvent is an organic compound or compound mixture and includes at least one of xylene and toluene.

6. The method according to claim 1, wherein the hydrocarbons are at least one of decant oil, petroleum refinery vacuum residual, thermal cracked oils, pyrolysis tars and coal tars.

7. The method according to claim 1, wherein the oxidizer includes nitric acid, the solvent includes xylene and the hydrocarbons include decant oil having a boiling point above 450°

C.

8. The method according to claim 1, wherein the carbonizing includes heating the solids above 400°

C. in an inert environment.

9. The method according to claim 1, wherein the hydrocarbons do not include any content that is insoluble in the solvent prior to the step of adding oxidizer and reacting of the hydrocarbons with the oxidizer.

10. The method according to claim 1, further comprising incorporating the carbonaceous material into an electrode of an electrochemical energy cell.

11. The method according to claim 1, wherein the mixture further includes carbonaceous suspended particles, which upon the step of adding oxidizer and reacting of the hydrocarbons with the oxidizer are coated by the constituents that are insoluble in the solvent.

12. The method according to claim 1, wherein the mixture further includes coke particles, which upon the step of adding oxidizer and reacting of the hydrocarbons with the oxidizer are coated by the constituents that are insoluble in the solvent.

13. The method according to claim 1, wherein the mixture remains below 120°

C. during the reacting of the hydrocarbons with the oxidizer.

14. The method according to claim 1, wherein the mixture during the reacting of the hydrocarbons with the oxidizer is above 70°

C. and remains below 120°

C.

15. The method according to claim 1, wherein a mass ratio of the solvent to the hydrocarbons is between 0.2 and 10.0.

16. The method according to claim 1, wherein a mass ratio of the hydrocarbons to the oxidizer is between 15 and 1.

23. The method of claim 1, wherein the reaction in the mixture between the oxidizer and the hydrocarbons causes compounds in the hydrocarbons to cross-link, thereby producing heavier hydrocarbons that are not soluble in the solvent.

17. A method, comprising:

preparing a mixture containing hydrocarbons, a solvent for the hydrocarbons, wherein the boiling point of the hydrocarbons is higher than that of the solvent and solid particles suspended in the mixture;

adding an oxidizer to the mixture, wherein the oxidizer reacts with the hydrocarbons to cause a coating to deposit on the solid particles;

separating the coated solid particles from liquids in the mixture; and

carbonizing the coating into carbonaceous material disposed on the particles.

18. The method according to claim 17, wherein the solid particles in the mixture are carbonaceous.

19. The method according to claim 17, wherein the oxidizer is nitric acid, the solvent is xylene and the hydrocarbons are decant oil having a boiling point above 450°

C.

20. The method according to claim 17, further comprising incorporating the solid particles with the coating that is carbonized into an electrode of an electrochemical energy cell.

24. The method of claim 17, wherein the reaction in the mixture between the oxidizer and the hydrocarbons causes compounds in the hydrocarbons to cross-link, thereby producing heavier hydrocarbons that are not soluble in the solvent.

21. A method, comprising:

preparing a mixture containing solvent, solid particles and hydrocarbons, wherein the boiling point of the hydrocarbons is higher than that of the solvent;

adding an oxidizer to the mixture, wherein the oxidizer reacts with the hydrocarbons to form products that are insoluble in the solvent and provide a coating of carbonaceous material on the solid particles;

separating the coated solid particles from liquids in the mixture; and

incorporating the solid particles with the coating into an electrochemical energy cell.

22. The method according to claim 21, further comprising carbonizing the coating on the solid particles.

25. The method of claim 21, wherein the reaction in the mixture between the oxidizer and the hydrocarbons causes compounds in the hydrocarbons to cross-link, thereby producing heavier hydrocarbons that are not soluble in the solvent.

26. The method of claim 21, wherein the mixture containing solvent, solid particles and hydrocarbons does not include other content which is insoluble in the solvent prior to adding the oxidizer.