Process for making carbon foam induced by process depressurization

• US 6,576,168 B2
• Filed: 05/22/2001
• Issued: 06/10/2003
• Est. Priority Date: 05/22/2001
• Status: Expired due to Term

• Current Assignee: Poco Graphite Incorporated (Entegris Incorporated)
• Original Assignee: Poco Graphite Incorporated (Entegris Incorporated)
• Inventors: Sheppard, Rex G., Dingus, David F., Hardcastle, Leland A.
• Primary Examiner(s): Kuhns, Allan R.
• Application Number:
  US09/862,560
• Publication Number:
  US 20020190414A1
• Time in Patent Office: 749 Days
• Field of Search: 264/29.1, 264/29.6, 264/42, 264/50, 423/445, 423/448
• US Class Current: 264/29.1
• CPC Class Codes: C01B 32/00 Carbon; Compounds thereof C01B21/00, C01B23/00 take precedence; percarbonates C01B15/10; carbon black C09C1/48
• CPC Class Codes: C04B 2111/00224 Green materials, e.g. porous green ceramic preforms
• CPC Class Codes: C04B 2111/00982 as construction elements for space vehicles or aeroplanes
• CPC Class Codes: C04B 35/52 based on carbon, e.g. graphite
• CPC Class Codes: C04B 35/522 Graphite C04B35/536 takes precedence
• CPC Class Codes: C04B 38/0022 obtained by a chemical conversion or reaction other than those relating to the setting or hardening of cement-like material or to the formation of a sol or a gel, e.g. by carbonising or pyrolysing preformed cellular materials based on polymers, organo-metallic or organo-silicon precursors
• CPC Class Codes: C04B 38/0067 characterised by the density of the end product
• CPC Class Codes: C04B 38/10 by using foaming agents C04B38/02 takes precedenceor by using mechanical means, e.g. adding preformed foam
• CPC Class Codes: C04B 40/0071 making use of a rise in pressure
• CPC Class Codes: C04B 40/0089 making use of vacuum or reduced pressure
• CPC Class Codes: C04B 40/0259 Hardening promoted by a rise in pressure C04B40/024 takes precedence
• CPC Class Codes: C04B 40/0272 Hardening under vacuum or reduced pressure

Abstract

A process for producing molded pitch based foam is shown which provides a more uniform density gradient throughout the ultimate product. The process utilizes a pressure drop during processing in order to induce foaming. By inducing foaming through process depressurization, additional viscosity manipulation can be achieved as well as improved density gradient characteristics in the ultimate product.

Claims

1. A method of producing carbon foam, comprising the steps of:

introducing a solid pitch to an appropriate level in a mold which is placed within a reaction vessel, the initially solid pitch, once melted to a liquid, having a characteristic boiling or foaming point at a given pressure and for a given temperature;

purging air from the reaction vessel;

pressurizing the reaction vessel between a preselected high initial pressure and a final process pressure, the preselected high initial pressure serving to increase the temperature at which the pitch would normally boil in the reaction vessel after being liquified by heating;

wherein the pitch has a given solidification point with continued heating after being heated to liquid and wherein the pitch is heated to liquid within the reaction vessel to a selected temperature which is below the solidification point and above the boiling point of the pitch at the final process pressure but below the boiling point of the pitch at the preselected high initial pressure;

holding the liquid pitch at the selected temperature for a predetermined period of time to increase the viscosity of the liquid pitch;

depressurizing the pitch from the high initial pressure to the final process pressure while maintaining the process temperature above the typical boiling or foaming temperature at the final pressure, whereby boiling and foaming of the pitch begins;

heating the foamed pitch to a temperature that solidifies the foamed pitch;

cooling the solidified foamed pitch to room temperature while allowing natural depressurization during cooling to thereby produce a carbon foam.

2. The method of claim 1, wherein the pitch is introduced in a form selected from the group consisting of granulated pitches, powdered pitches and pelletized pitches.

3. The method of claim 1, wherein the pitch is selected from the group consisting of mesophase and isotropic pitches and mixtures thereof.

4. The method of claim 3, wherein the pitch is a mesophase pitch selected from the group consisting of synthetic pitches, coal based pitches, petroleum based pitches and mixtures thereof.

5. The method of claim 1, wherein the mold is lined with a metal liner.

6. The method of claim 1, wherein the HIP is pressurized to an initial pressure between about 4000 and 16,000 psig with an inert gas.

7. The method of claim 6, wherein the inert gas is selected from the group consisting of nitrogen gas and argon gas.

8. The method of claim 1, wherein the pitch is heated from room temperature to a melting temperature in the range from about 250 to 350°

C. at a rate between about 1.0 and 10.0°

C. per minute.

9. The method of claim 1, wherein the pitch is held at a temperature between about 250 and 350°

C. for up to about 10 hours.

10. The method of claim 1, wherein the pitch is heated between about 250 and 450°

C. at a rate between about 1.0 and 10.0°

C. per minute.

11. The method of claim 1, wherein the pitch is held between 250 and 450°

C. from 0 to 4 hours.

12. The method of claim 1, wherein the HIP is depressurized from the initial pressure to the final pressure at a rate between 50 and 700 psig per minute while maintaining the pre-depressurization temperature.

13. The method of claim 12, wherein the final pressure is between 50 and 4000 psig.

14. The method of claim 12, wherein, after depressurization, the foam is heated from its pre-depressurization temperature to a temperature between 400 and 800°

C. at a rate between 1.0 and 10.0°

C. per minute.

15. The method of claim 14, wherein the foam is held between 400 and 800°

C. from 0 to 4 hours.

16. The method of claim 15, wherein the foam is cooled from between 400 and 800°

C. to room temperature at a rate between 1.0 and 30°

C. per minute.

17. The method of claim 1, further comprising the steps of:

heating the carbon foam in a non-oxidizing atmosphere to a temperature sufficient to carbonize the carbon foam to form a carbonized carbon foam; and

heating the carbonized carbon foam in a non-oxidizing atmosphere to a temperature sufficient to form a thermally conductive essentially graphitic carbon foam.

18. The method of claim 1, wherein the carbon foam is characterized as having a thermal conductivity ranging from about 90 to 244 W/mK.

19. The method of claim 1, wherein the carbon foam is characterized as having an apparent density ranging from about 0.43 to 0.62.

20. The method of claim 1, wherein the carbon foam is characterized by the substantial absence of internal voids.

21. A method of producing carbon foam, comprising the steps of:

selecting an appropriate mold shape;

introducing an initially solid pitch to an appropriate level in the mold, the initially solid pitch, once melted to a liquid, having a characteristic boiling or foaming point at a given pressure and for a given temperature;

desiccating the pitch to assist in removing any residual moisture;

placing the mold within a hot isostatic press and purging air from the press and from the mold;

pressurizing the hot isostatic press between a preselected high initial pressure and a final process pressure, the preselected high initial pressure serving to increase the temperature at which the pitch would normally boil in the hot isostatic press after being liquified by heating;

wherein the pitch has a given solidification point with continued heating after being heated to liquid and wherein the pitch is heated to liquid within the hot isostatic press to a selected temperature which is below the solidification point and above the boiling point of the pitch at the final process pressure but below the boiling point of the pitch at the preselected high initial pressure;

holding the liquid pitch at the selected temperature for a predetermined time to increase the viscosity of the liquid pitch;

depressurizing the pitch from the high initial pressure to the final process pressure while maintaining the process temperature above the typical boiling or foaming temperature at the final pressure, whereby boiling and foaming of the pitch begins;

heating the foamed pitch to a temperature that solidifies the foamed pitch;

cooling the solidified foamed pitch to room temperature while allowing natural depressurization during cooling to thereby produce a carbon foam;

depressurizing the carbon foam to atmospheric pressure; and

removing the carbon foam from the hot isostatic press and from the mold.