Mesophase pitch for carbon fiber production using supercritical carbon dioxide

Patent metadata

Field	Value
Publication number	US-12152198-B2
Application number	US-202318446298-A
Country	US
Kind code	B2
Filing date	Aug 8, 2023
Priority date	Mar 18, 2019
Publication date	Nov 26, 2024
Grant date	Nov 26, 2024

Abstract

Embodiments of methods for improving mesophase pitch for carbon fiber production using supercritical carbon dioxide are described. The methods improve the relative amount and quality of mesophase pitch in feedstocks, such as coal tar, already having at least some mesophase pitch. One particular method includes performing a sCO2/toluene extraction on the coal tar to obtain a toluene insoluble fraction of the coal tar; mixing the toluene insoluble fraction with sCO2 to obtain a sCO2/toluene insoluble fraction mixture; and extruding the sCO2/toluene insoluble fraction mixture, thereby separating the sCO2 from the toluene insoluble fraction to obtain fibers of mesophase pitch.

First claim

What is claimed:

1. A method of manufacturing carbon fibers comprising:
contacting a coal derivative with a supercritical fluid solvent and first co-solvent mixture, thereby removing at least some soluble components from the coal derivative to obtain an insoluble coal derivative fraction;
after contacting the coal derivative with the supercritical fluid solvent and the first co-solvent mixture, separating the supercritical fluid solvent and first co-solvent mixture from the insoluble coal derivative fraction;
after separating the supercritical fluid solvent and first co-solvent mixture from the insoluble coal derivative fraction, mixing the insoluble coal derivative fraction with a supercritical fluid to obtain a supercritical fluid/insoluble fraction mixture; and
after mixing the insoluble coal derivative fraction with the supercritical fluid, separating the supercritical fluid from the insoluble fraction to obtain the carbon fibers.

2. The method of claim 1 , wherein the coal derivative comprises coal tar.

3. The method of claim 1 , wherein:
the coal derivative comprises a mesophase pitch precursor; and
the carbon fibers comprise fibers of mesophase pitch.

4. The method of claim 1 , wherein the supercritical fluid comprises sCO 2 .

5. The method of claim 1 , wherein separating the supercritical fluid from the insoluble fraction comprises passing the supercritical fluid/insoluble fraction mixture through an extruder.

6. The method of claim 1 , further comprising:
washing the insoluble coal derivative fraction with a second co-solvent to obtain a second co-solvent and second co-solvent-soluble fraction mixture and a second co-solvent-insoluble fraction of the first insoluble fraction;
separating the second co-solvent from the second co-solvent-soluble fraction of the insoluble fraction; and
mixing the second co-solvent-soluble fraction of the insoluble fraction with the supercritical fluid to obtain the supercritical fluid/insoluble fraction mixture.

7. The method of claim 6 , wherein the second co-solvent comprises one or more of benzene, xylene, tetralin, tetrahydrofuran, pyridine, and quinoline.

8. The method of claim 6 , further comprising:
heating the second co-solvent-soluble fraction of the insoluble fraction to a temperature in a range of 300 to 400° C. for less than 24 hours before mixing the second co-solvent-soluble fraction with the supercritical fluid; and
contacting the second co-solvent-soluble fraction with the supercritical fluid heated to a temperature between 300 to 400° C. for up to 24 hours.

9. The method of claim 1 , further comprising performing one of:
a stabilization operation on the carbon fibers;
a carbonization operation on the carbon fibers; and
a graphitization operation on the carbon fibers.

10. The method of claim 6 , wherein at least one of the first co-solvent and the second co-solvent comprises an aromatic organic solvent.

11. The method of claim 6 , wherein at least one of the first co-solvent and the second co-solvent comprises one or more of benzene, xylene, tetralin, tetrahydrofuran, pyridine, and quinoline.

12. The method of claim 1 , wherein the supercritical fluid solvent comprises one or more of carbon dioxide, water, methane, nitrous oxide, ethane, propane, ethylene, propylene, methanol, ethanol, and acetone.

13. The method of claim 1 , wherein the coal derivative is
created by:
pyrolyzing a combination of carbonaceous feedstock at a first temperature and first pressure and for a first period of time to generate C 1 -C 4 gases;
increasing the combination to a second temperature greater than the first temperature;
pyrolyzing the combination at the second temperature and for a second period of time to generate coal derivative; and
extracting coal derivative from the combination.

14. The method of claim 13 , wherein:
the first temperature is in a range of 150 to 350° C.;
the second temperature is in a range of 350 to 550° C.; and
the first pressure is in a range of 7 to 30 MPa.

15. The method of claim 13 , wherein the first period is in a range of 1 to 120 minutes.

16. The method of claim 13 , wherein the second period of time is in a range of 1 minute to 24 hours.

17. The method of claim 13 , wherein pyrolyzing the carbonaceous feedstock at the first temperature and first pressure is performed in a first pyrolysis reaction chamber.

18. The method of claim 13 , wherein pyrolyzing the carbonaceous feedstock at the first temperature and first pressure is performed in a carbon dioxide atmosphere.

19. The method of claim 13 , wherein extracting the coal derivative includes transferring the carbon dioxide atmosphere to a separation system.

20. The method of claim 13 , wherein extracting the coal derivative includes lowering at least one of the temperature or the pressure of the carbon dioxide atmosphere.

Assignees

• Terrapower Llc

Inventors

• Goodrich Benjamin L
• Kim Pyoungchung
• Targett Matthew
• Walter Joshua C

Classifications

• D01F9/145

  from pitch or distillation residues · CPC title

• D01F9/15

  from coal pitch · CPC title

• C10C3/08 Primary

  by selective extraction · CPC title

• C10C1/18 Primary

  by extraction with selective solvents (preparation of hydrocarbon oils from tar oils C10G21/00) · CPC title

• Y02P20/54

  using solvents, e.g. supercritical solvents or ionic liquids · CPC title