Method of preparing nitrogen-doped graphene and method of producing composite heat dispatching plate thereof

Patent metadata

Field	Value
Publication number	US-2016369149-A1
Application number	US-201615168097-A
Country	US
Kind code	A1
Filing date	May 30, 2016
Priority date	Jun 22, 2015
Publication date	Dec 22, 2016
Grant date	—

Abstract

The present invention relates to a method of preparing nitrogen-doped graphene, comprising: mixing at least one solid-state nitrogen containing precursor with a graphene to form a mixture, and sintering the mixture under a reducing atmosphere to obtain the nitrogen-doped graphene. The present invention further provides a method of producing a composite heat dispatching plate coated with nitrogen-doped graphene film, comprising: mixing a nitrogen-doped graphene obtained aforementioned with a polymer bonding agent to form a mixture slurry, coating the mixture slurry onto at least one surface of a metal substrate to form a composite material, drying the composite material, and obtaining the composite heat dispatching plate with a film of nitrogen-doped graphene. Structural defects of graphene lattices are reduced during doping process so that crystallinity and thermal conductivity are improved. Methods of the present invention may be conducted under normal pressure using commercially available solid-state nitrogen sources without adding polluting solvents to provide a safe, stable and cost effective preparation of composite heat dispatching material.

First claim

What is claimed is:

1 . A method of preparing nitrogen-doped graphene, comprising:
mixing at least one solid-state nitrogen containing precursor with a graphene to form a mixture; and sintering said mixture under a reducing atmosphere to obtain said nitrogen-doped graphene.

2 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said solid-state nitrogen containing precursor and said graphene are mixed to form said mixture using a solid phase mixing method.

3 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said solid-state nitrogen containing precursor is an organic solid-state nitrogen source, and said organic solid-state nitrogen source is selected from at least one of the following: C 6 H 12 N 4 , C 6 H 5 COONH 4 , (NH 4 ) 2 CO 3 , HOC(CO 2 NH 4 )(CH 2 CO 2 NH 4 ) 2 , HCO 2 NH 4 , C 11 H 7 N, C 3 H 3 N 6 , C 10 H 6 (CN) 2 and C 12 H 7 NO 2 .

4 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said solid-state nitrogen containing precursor is an inorganic solid-state nitrogen source, and said inorganic solid-state nitrogen source is selected from at least one of NH 4 NO 3 and other inorganic nitrate salts.

5 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said solid-state nitrogen containing precursor is a combination of an organic solid-state nitrogen source and an inorganic solid-state nitrogen source; said organic solid-state nitrogen source is selected from at least one of the following: C 6 H 12 N 4 , C 6 H 5 COONH 4 , (NH 4 ) 2 CO 3 , HOC(CO 2 NH 4 )(CH 2 CO 2 NH 4 ) 2 , HCO 2 NH 4 , C 11 H 7 N, C 3 H 3 N 6 , C 10 H 6 (CN) 2 and C 12 H 7 NO 2 ; and said inorganic solid-state nitrogen source is selected from at least one of NH 4 NO 3 and other inorganic nitrate salts.

6 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said graphene is selected from at least one of monolayer graphene, multilayer graphene, graphene oxide, reduced graphene oxide and graphene derivatives.

7 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said nitrogen-doped graphene has bonding configurations of Pyridinic N(398.1˜399.3 eV) and Graphitic N(401.1˜402.7 eV).

8 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein a mass mixing ratio between said solid-state nitrogen containing precursor and said graphene is over 1.

9 . The method of preparing nitrogen-doped graphene according to claim 8 , wherein a mass mixing ratio between said graphene and said solid-state nitrogen containing precursor is between 1:1 and 1:30.

10 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein a nitrogen content of said nitrogen-doped graphene is between 0.04 and 5 wt %.

11 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said mixture is sintered under a temperature between 300° C. and 800° C. .

12 . The method of preparing nitrogen-doped graphene according to claim 1 , wherein said mixture is sintered for 0.5 to 10 hours.

13 . A method of producing a composite heat dispatching plate, comprising:
mixing a nitrogen-doped graphene with a polymer bonding agent to form a mixture slurry, wherein said nitrogen-doped graphene is prepared using any of the methods of claim 1 to claim 12 ; coating said mixture slurry onto at least one surface of a metal substrate to form a composite material; drying said composite material; and obtaining said composite heat dispatching plate with a coating of nitrogen-doped graphene.

14 . The method of producing a composite heat dispatching plate according to claim 13 , wherein said polymer bonding agent is Carboxymethyl Cellulose(CMC).

15 . The method of producing a composite heat dispatching plate according to claim 13 , wherein said mixture slurry further comprising an electricity conductive agent, an adhesive agent, or a combination thereof.

16 . The method of producing a composite heat dispatching plate according to claim 13 , wherein said nitrogen-doped graphene content in said mixture slurry is between 50 and 93 wt %.

17 . The method of producing a composite heat dispatching plate according to claim 16 , wherein said nitrogen-doped graphene content in said mixture slurry is between 89 and 92 wt %.

18 . The method of producing a composite heat dispatching plate according to claim 13 , wherein said metal substrate is a copper foil.

19 . The method of producing a composite heat dispatching plate according to claim 13 , wherein a thickness of said nitrogen doped graphene coating is between 15 and 65 μm.

Assignees

• Univ Chung Yuan Christian
• The-Hydroxyl® Applied Carbon Tech Inc

Inventors

• Liu Wei Jen
• Xie zheng zhe
• Shen Jun

Classifications

• H10W40/25

  characterised by their materials · CPC title

• C01B32/194

  After-treatment · CPC title

• C09K5/14 Primary

  Solid materials, e.g. powdery or granular · CPC title

• B82Y40/00 Primary

  Manufacture or treatment of nanostructures · CPC title

• C09D101/286

  substituted with acid radicals (C09D101/282 takes precedence) · CPC title