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HETEROELEMENT-CONTAINING GRAPHENE

Foreign code F210010327
File No. AF39-05WO
Posted date Feb 1, 2021
Country Republic of Korea
Application number 20207011964
Gazette No. 20200060454
Date of filing Sep 28, 2018
Gazette Date May 29, 2020
International application number JP2018036399
International publication number WO2019066013
Date of international filing Sep 28, 2018
Date of international publication Apr 4, 2019
Priority data
  • P2017-190683 (Sep 29, 2017) JP
  • 2018JP36399 (Sep 28, 2018) WO
Title HETEROELEMENT-CONTAINING GRAPHENE
Abstract An object of the present invention is to provide a highly crystalline heteroelement-containing graphene. A heteroelement-containing graphene disclosed herein includes carbon (C) and, as a heteroelement (X), at least one element selected from the group consisting of nitrogen (N), phosphorus (P), arsenic (As), sulfur (S), boron (B), and silicon (Si). Also, spots belonging to either the orthorhombic system or the hexagonal system and having the symmetry of a single crystal are observed in the selected area electron diffraction.
(From EP3689819 A1)
Outline of related art and contending technology BACKGROUND ART
Hexane ring carbon atoms in the graphene structure from the prior art, in addition to carbon atoms of the hetero element is introduced into the graphene containing hetero element has attracted attention. In the hetero element containing graphene, for example nitrogen and the like of the edge portions of the zigzag graphene valley of introduction of the foreign elements, heterologous elements relative to the carbon atom adjacent to the physical, chemical Works. As a result, the carbon atom adjacent to the oxygen reduction characteristics are known to be expressed. From this, the graphene may contain a hetero element, is used as the catalyst material has been studied (for example, see Patent documents 1 to 3).
Patent document 1 discloses, on the surface of the carbon support to form a nitrogen containing graphite, for an electrode catalyst carrier is disclosed. Patent document 1 is a nitrogen containing graphite, π electrons on the surface of the carbon support having formed therein. In Patent document 1, the nitrogen containing graphite based on the Raman spectrum of crystalline ID/IG and evaluated by the value, the value ID/IG is 0.8 to 1. 2 To be disclosed.
Patent document 2 discloses, solvot thermal heteroatoms such as nitrogen by reaction of the heteroatom containing graphene can be synthesized is disclosed. In the embodiment of patent document 2, a nitrogen atom is a heteroatom containing graphene 14. 8 Atom % of the doped ratio described. However, in Patent document 2, the heteroatom in relation to the crystallinity of the graphene is not disclosed at all.
Patent document 3 discloses, the stoichiometric ratio of silicon nitride having a graphite phase (g CH C3 N4) is disclosed. The carbon nitride disclosed in Patent document 3 graphite phase, the nitrogen and carbon atoms of the ring member 3 that includes 6 triangles sharing C field N each having a crystal structure for melon ((C6 N9 H3) X) is, at least one nitrogen atom in the polymerization of a vertex having the structure of the present invention.
In addition, the inventors have found that, in Patent document 4, a large amount of 10 atom % or more of the different elements as nitrogen heteroatom containing a carbon catalyst to provide a production method of the present invention. According to these methods, the carrier does not contain a hetero atom containing graphene can be produced.
In addition, patent document 5 in which, on the electrode catalyst is formed having a redox potential of the carbon atoms are described.
Scope of claims [claim1]
1. In the electron diffraction, rectangular and hexagonal and hexagonal belongs, the symmetry of the single crystal and having a spot is observed, and the carbon (C), nitrogen as hetero (N) (X), phosphorus (P), arsenic (As), sulfur (S), boron and silicon (B) selected from the group consisting of (Si) at least one element 1 containing a hetero element comprising graphene.

[claim2]
2. Method according to claim 1, said spots, said rectangular belongs to orthorhombic, [101] in the direction of incidence of the electron diffraction image and which, reciprocal 11-1,-111,-202, 1-1-1, 20-2 and-1-11 of the amino acid sequence of the graphene and containing a hetero element.

[claim3]
3. Method according to claim 1 or 2, wherein X ray diffraction half width of the diffraction peak from the surface, (002) is not less than 3 and containing a hetero element graphene.

[claim4]
4. Method according to any one of claims 1-3, wherein the diffraction peak X from cotton, (002) the diffraction peak intensity for the diffraction peak intensity I (002) I (101) from the surface (101) of at least 0.1 () /I (002) I (101) characterized in that the hetero element containing graphene.

[claim5]
5. Method according to claim 3 or 4, X ray diffraction of claim 3, (002) the planes of the interval. 5 Å Or less graphene and containing a hetero element.

[claim6]
6. Method according to any one of claims 1-5, X ray photoelectron spectroscopy is calculated on the basis of, carbon and a hetero element (C) (X/C) is an atomic ratio of (X) is at least 0.1 and containing a hetero element in the graphene.

[claim7]
7. Method according to any one of claims 1-6, based on the X ray photoelectron spectroscopy, the bottom side of the nitrogen doped chemically bonded to a cationic nitrogen status and possibly, the Hall effect measurement is determined by the carrier type and P type hetero element containing graphene.

[claim8]
8. Method according to any one of claims 1-7, with an excitation wavelength of 532nm in the Raman spectroscopic analysis of, 1350cm-1 appearing near the D band intensity I (D) and, 1580cm-1 around G band intensity I (G) ratio (I (D) /I (G) ) is 1 or less and, further, the half width of the band 50cm G-1 or less graphene and containing a hetero element.

[claim9]
9. Method according to any one of claims 1-8, in the Raman spectroscopic analysis, 2700cm-1 appearing near the intensity of the (2D) and 2D I, wherein the ratio of the intensity of G I (G) ((2D) /I I (G) ) is 0.5 or more heteroatoms and containing graphene.

[claim10]
10. Method according to any one of claims 1-9, in the Raman spectroscopic analysis, 2700cm-1 appearing near a half value width of the band 2D 80cm-1 hetero containing less graphene.

[claim11]
11. Method according to any one of claims 1-10, the heterocycle containing a substrate supporting the graphene and graphene does not contain a hetero element.

[claim12]
12. Method according to any one of claims 1-11, the carbon atom of the hetero element (C) (X) and the chemically bonded with, in addition, the carbon atom of sp (C) mainly2 configured by binding of the graphene sheet and, wherein the graphene sheet, comprising a single layer structure or a 2 to 1 layers of at least one layer of 5 or less and containing a hetero element having a laminate structure of graphene.

[claim13]
13. Method according to any one of claims 1-12, and having an average particle diameter of 1nm or more than 10 graphene powder containing hetero m.

[claim14]
14. 5-Membered ring structure and having at least a portion of, the 5-membered, nitrogeN, phosphorus (P), arsenic (As), sulfur (S), boron and silicon (B) (Si) 1 is selected from the group consisting of at least one hetero element and (X), carbon (C) constituted by a 5-membered heterocyclic compound is, dissolved in a polar aprotic solvent to prepare a raw material containing liquid, and, in the raw material containing liquid by generating plasma, wherein the heterocyclic ring compound by polymerizing 5, containing a hetero element and to obtain graphene comprising, in a selected area electron diffraction, rectangular and hexagonal belongs to any one of hexagonal, single crystal having the symmetry of the spot is observed and, together with the carbon (C), hetero (N) nitrogen (X), phosphorus (P), arsenic (As), sulfur (S), boron and silicon (B) selected from the group consisting of (Si) at least one kind of element 1 SiO and containing a hetero element.
  • Applicant
  • JAPAN SCIENCE AND TECHNOLOGY AGENCY
  • Inventor
  • Saito Nagahiro
IPC(International Patent Classification)
Reference ( R and D project ) CREST Establishment of molecular technology towards the Creation of New Functions AREA
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