Nitrogen-containing carbon material and method of manufacturing the same

Patent metadata

Field	Value
Publication number	US-10046971-B2
Application number	US-201514971685-A
Country	US
Kind code	B2
Filing date	Dec 16, 2015
Priority date	Dec 16, 2014
Publication date	Aug 14, 2018
Grant date	Aug 14, 2018

Abstract

A nitrogen-containing carbon material to the present invention comprises a carbon material having a carbon skeleton formed of carbon atoms and nitrogen atoms introduced into the carbon material, wherein part of carbon atoms in the carbon skeleton are substituted with nitrogen atoms. The nitrogen-containing carbon material according to the present invention can be produced by a production method including the steps of bringing the carbon material into contact with a first treatment gas containing a fluorine-containing gas to subject a surface of the carbon material to a fluorination treatment; and bringing the carbon material after being subjected to the fluorination treatment into contact with a second treatment gas containing a nitrogen-containing gas with heating to perform a nitriding treatment.

First claim

What is claimed is:

1. A nitrogen-containing carbon material comprising:
a carbon material having a carbon skeleton formed of carbon atoms; and
a nitrogen atom introduced into the carbon material,
wherein part of the carbon atoms in the carbon skeleton are replaced with nitrogen atoms, at least one amino group is attached to a surface of the nitrogen-containing carbon material, carbon-fluorine bonds are present on a surface of the nitrogen-containing carbon material and nitrogen-fluorine bonds are not present on the nitrogen-containing carbon material.

2. The nitrogen-containing carbon material according to claim 1 , wherein the nitrogen atoms introduced into the carbon skeleton by replacing part of carbon atoms therewith comprise pyridine-type nitrogen atoms, or pyridine-type nitrogen atoms and pyrrole-type nitrogen atoms.

3. The nitrogen-containing carbon material according to claim 1 , wherein the carbon material before nitrogen atoms are introduced thereinto is at least one kind selected from the group consisting of a carbon nanocoil, graphite, carbon black, diamond-like carbon, a carbon fiber, graphene, amorphous carbon, fullerene, a carbon nanotube and diamond.

4. A method of producing the nitrogen-containing carbon material according to claim 1 , comprising the steps of:
bringing a carbon material having a carbon skeleton formed of carbon atoms into contact with a first treatment gas containing a fluorine-containing gas to subject a surface of the carbon material to a fluorination treatment; and
bringing the carbon material after being subjected to the fluorination treatment into contact with a second treatment gas containing a nitrogen-containing gas to perform a nitriding treatment.

5. The method of producing the nitrogen-containing carbon material according to claim 4 ,
wherein the fluorination treatment is performed under the condition of a treatment period of 1 second to 24 hours and a treatment temperature of 0° C. to 600° C. using a first treatment gas containing a fluorine-containing gas in a content of 0.01 to 100 vol % relative to the whole volume of the first treatment gas, and
the nitriding treatment is performed under the condition of a treatment period of 1 second to 24 hours using a second treatment gas containing a nitrogen-containing gas in a content of 0.01 to 100 vol % relative to the whole volume of the second treatment gas.

6. The method of manufacturing the nitrogen-containing carbon material according to claim 5 , wherein the nitriding treatment is carried out at a treatment temperature higher than or equal to 25° C. and lower than 300° C., to introduce at least one amino group onto a surface of the carbon material and to replace part of the carbon atoms in the carbon skeleton with nitrogen atoms.

7. The method of producing the nitrogen-containing carbon material according to claim 6 , wherein the nitrogen atoms introduced into the carbon skeleton by replacing part of the carbon atoms therewith comprise pyridine-type nitrogen atoms, or pyridine type nitrogen atoms and pyrrole-type nitrogen atoms.

8. The method of producing the nitrogen-containing carbon material according to claim 4 , comprising no step for removing fluorine atoms existing at carbon-fluorine bond moieties on a surface of the nitrogen-containing carbon material after being subjected to the nitriding treatment.

9. The method of producing the nitrogen-containing carbon material according to claim 4 , wherein the carbon material before being subjected to the fluorination treatment is at least one kind selected from the group consisting of a carbon nanocoil, graphite, carbon black, diamond-like carbon, a carbon fiber, graphene, amorphous carbon, fullerene, a carbon nanotube and diamond.

10. An air electrode catalyst for a fuel cell comprising the nitrogen-containing carbon material according to claim 1 .

11. The air electrode catalyst for a fuel cell according to claim 10 , wherein the nitrogen atoms introduced into the carbon skeleton by replacing part of carbon atoms therewith comprise pyridine-type nitrogen atoms, or pyridine-type nitrogen atoms and pyrrole-type nitrogen atoms.

12. The air electrode catalyst for a fuel cell according to claim 11 , wherein the carbon material before nitrogen atoms are introduced thereinto is at least one kind selected from the group consisting of a carbon nanocoil, graphite, carbon black, diamond-like carbon, a carbon fiber, graphene, amorphous carbon, fullerene, a carbon nanotube and diamond.

Assignees

• Stella Chemifa Corp
• Univ Tohoku

Inventors

• Tohji Kazuyuki
• Sato Yoshinori
• Yokoyama Koji
• Hirano Kazutaka
• Sato Yoshinori

Classifications

• H01M4/96

  Carbon-based electrodes · CPC title

• C01B21/082

  Compounds containing nitrogen and non-metals {and optionally metals}(C01B21/06, C01B21/08 take precedence) · CPC title

• C01B32/174 Primary

  Derivatisation; Solubilisation; Dispersion in solvents · CPC title

• C01B2202/02

  Single-walled nanotubes · CPC title

• C01B31/0273 Primary

  Chemistry & Metallurgy · mapped topic