Synthesis of micron and nanoscale carbon spheres and structures using hydrothemal carbonization

Patent metadata

Field	Value
Publication number	US-11724941-B2
Application number	US-201916970265-A
Country	US
Kind code	B2
Filing date	Feb 15, 2019
Priority date	Feb 15, 2018
Publication date	Aug 15, 2023
Grant date	Aug 15, 2023

Abstract

Provided are methods for preparing carbon powders and activated carbon powders from cellulose-containing liquids. In some embodiments, the methods include exposing a cellulose-containing liquid to a hydrothermal carbonization process to convert the carbonaceous material present therein into a carbon powder. Also provided are methods for activating carbon powders, methods for producing carbon powder-containing polymer matrices, and carbon powders, activated carbon powders, and polymer matrices that that include the disclosed carbon powders and/or activated carbon powders that are produced by the presently disclosed methods.

First claim

What is claimed is:

1. A method for preparing a carbon powder from a cellulose-containing liquid, the method comprising exposing the cellulose-containing liquid to a hydrothermal carbonization process to convert carbonaceous material present therein into a carbon powder;
wherein the cellulose-containing liquid comprises about 5% micro—and/or nanofibrillated cellulose by weight in water.

2. The method of claim 1 , wherein the cellulose-containing liquid comprises agricultural waste residue.

3. The method of claim 2 , wherein the agricultural waste residue has been grinded to a powder.

4. The method of claim 1 , wherein the cellulose present in the cellulose-containing liquid comprises cellulose nanocrystals (CNCs).

5. The method of claim 4 , wherein the CNCs have been generated from plant cellulose pulp by acid hydrolysis.

6. The method of claim 1 , wherein the hydrothermal carbonization process is performed under conditions sufficient to carbonize at least 60%, at least 65%, at least 70% but less than 95%, less than 90%, less than 85%, less than 80%, or less than 75% of the carbonaceous material present in the cellulose-containing liquid.

7. The method of claim 1 , wherein hydrothermal carbonization process comprises exposing the cellulose-containing liquid to the hydrothermal carbonization process at temperatures from about 170° C. to 350° C.

8. The method of claim 1 , wherein the cellulose-containing liquid is subjected to a hydrothermal carbonization at temperatures in the range from about 180° C. to about 250° C.

9. The method of claim 8 , wherein the cellulose-containing liquid is subjected to a hydrothermal carbonization at 250° C.

10. The method of claim 8 , wherein the cellulose-containing liquid is subjected to a hydrothermal carbonization 225° C.

11. The method of claim 1 , wherein the hydrothermal carbonization process comprises exposing the cellulose-containing liquid to the hydrothermal carbonization process in a closed reactor at a temperature of about 250° C. for about 25 minutes before allowing the processed material to cool to room temperature.

12. The method of claim 1 , wherein performing the hydrothermal carbonization process in the closed reactor results in an autogenous pressure of about 10 to about 50 bars within the closed reactor.

13. The method of claim 1 , wherein the carbon powder has an average grain size of about 100 nm or less, about 250 nm or less, about 500 nm or less, about 750 nm or less, about 1000 nm or less, about 1.25 μm or less, about 1.5 m or less, about 2.0 μm or less, or about 5.0 μm or less.

14. The method of claim 1 , wherein the carbon powder is configured for use in an application selected from the group consisting of a metal-carbon composite, an activated carbon for CO 2 capture, an active surface, a structural composite, an absorbent, an electronics application, and energy storage.

15. The method of claim 1 , wherein the hydrothermal carbonization process is a batch hydrothermal carbonization process.

16. The method of claim 1 , wherein the hydrothermal carbonization process is a continuous hydrothermal carbonization process.

17. The method of claim 1 , further comprising separating the carbon powder from liquid containing the carbon powder after the hydrothermal carbonization process is performed.

18. The method of claim 17 , wherein the liquid containing the carbon powder comprises one or more of furfurals and organic acids after the hydrothermal carbonization process is performed.

19. The method of claim 18 , further comprising isolating at least one of the one or more chemicals of interest from the liquid after the hydrothermal carbonization process is performed.

20. A method for preparing a carbon powder from a cellulose-containing liquid, the method comprising
exposing the cellulose-containing liquid to a hydrothermal carbonization process to convert carbonaceous material present therein into a carbon powder; and
exposing the carbon powder to an activation process;
wherein the cellulose-containing liquid comprises about 5% micro—and/or nanofibrillated cellulose by weight in water.

21. The method of claim 20 , wherein the cellulose-containing liquid comprises agricultural waste residue.

22. The method of claim 21 , wherein agricultural waste residue has been grinded to a powder.

23. The method of claim 20 , wherein the cellulose present in the cellulose-containing liquid comprises cellulose nanocrystals (CNCs).

24. The method of claim 23 , wherein the CNCs have been generated from plant cellulose pulp by acid hydrolysis.

25. The method of claim 20 , comprising exposing the carbon powder to an activation process selected from the group consisting of exposure to steam at a temperature of at least 800° C. and chemical activation.

26. The method of claim 25 , wherein the chemical activation is chemical activation with phosphoric acid and zinc chloride treated with sodium hydroxide.

27. The method of claim 20 , wherein the hydrothermal carbonization process is performed under conditions sufficient to carbonize at least 60%, at least 65%, at least 70% but less than 95%, less than 90%, less than 85%, less than 80%, or less than 75% of the carbonaceous material present in the cellulose-containing liquid.

28. The method of claim 20 , wherein hydrothermal carbonization process comprises exposing the cellulose-containing liquid to the hydrothermal carbonization process at temperatures from about 170° C. to 350° C.

29. The method of claim 20 , wherein the cellulose-containing liquid is subjected to a hydrothermal carbonization at temperatures in the range from about 180° C. to about 250° C.

30. The method of claim 29 , wherein the cellulose-containing liquid is subjected to a hydrothermal carbonization at 250° C.

31. The method of claim 20 , wherein the hydrothermal carbonization process comprises exposing the cellulose-containing liquid to the hydrothermal carbonization process in a closed reactor at a temperature of about 250° C. for about 25 minutes before allowing the processed material to cool to room temperature.

32. The method of claim 20 , wherein performing the hydrothermal carbonization process in the closed reactor results in an autogenous pressure of about 10 to about 50 bars within the closed reactor.

33. The method of claim 20 , wherein the carbon powder has an average grain size of about 100 nm or less, about 250 nm or less, about 500 nm or less, about 750 nm or less, about 1000 nm or less, about 1.25 μm or less, about 1.5 m or less, about 2.0 μm or less, or about 5.0 μm or less.

34. The method of claim 20 , wherein the carbon powder is configured for use in an application selected from the group consisting of a metal-carbon composite, an activated carbon for CO 2 capture, an active surface, a structural composite, an absorbent, an electronics application, and energy storage.

35. The method of claim 20 , wherein the hydrothermal carbonization process is a batch hydrothermal carbonization process.

36. The method of claim 20 , wherein the hydrothermal carbonization process is a continuous hydrothermal carbonization process.

37. The method of claim 20 , further comprising separating the carbon powder from liquid containing the ca

Assignees

• Univ North Carolina State

Inventors

• Hakovirta Marko
• Saloni Daniel
• Venditti Richard

Classifications

• C01B32/318 Primary

  characterised by the starting materials · CPC title

• C01B32/05

  Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30 · CPC title

• C01P2002/85

  by XPS, EDX or EDAX data · CPC title

• C01P2004/03

  obtained by SEM · CPC title

• C01P2004/61

  Micrometer sized, i.e. from 1-100 micrometer · CPC title