Method of producing graphene

Patent metadata

Field	Value
Publication number	US-10865488-B2
Application number	US-201916665220-A
Country	US
Kind code	B2
Filing date	Oct 28, 2019
Priority date	Feb 14, 2014
Publication date	Dec 15, 2020
Grant date	Dec 15, 2020

Abstract

A method of producing graphene sheets comprising the steps of, (a) forming a carbonaceous powder by electrochemical erosion of a graphite electrode in a molten salt comprising hydrogen ions, (b) recovering the resulting carbonaceous powder from the molten salt liquid, and (c) thermally treating the carbonaceous powder by heating the carbonaceous powder in a non-oxidising atmosphere to produce a thermally treated powder comprising graphene sheets.

First claim

The invention claimed is:

1. A method of producing graphene sheets comprising the steps of,
(a) forming a carbonaceous powder by electrochemical erosion of a graphite electrode in a molten salt comprising hydrogen ions,
(b) recovering the resulting carbonaceous powder from the molten salt liquid, and
(c) thermally treating the carbonaceous powder by heating the carbonaceous powder in a non-oxidising atmosphere to produce a thermally treated powder comprising graphene sheets.

2. A method according to claim 1 in which the molten salt comprises a halide salt of lithium, sodium or potassium.

3. A method according to claim 1 in which the temperature of the molten salt during the electrochemical erosion of the graphite electrode is greater than 800° C.

4. A method according to claim 1 in which the molten salt and the carbonaceous powder is recovered from the molten salt by a process comprising steps of cooling and solidifying the molten salt, and washing the solidified salt from the carbonaceous powder.

5. A method according to claim 4 further comprising the step of vacuum filtration of the washed carbonaceous material.

6. A method according to claim 1 in which the carbonaceous powder comprises a metal hydride compound prior to the step of thermal treatment, for example lithium hydride, the metal species in the metal hydride being derived from the molten salt.

7. A method according to claim 1 in which the carbonaceous powder is thermally treated by heating to a temperature of greater than 1,000° C., for example to 1250° C.+/−50° C., in a reducing atmosphere, for example, in a reducing gas atmosphere comprising a mixture of nitrogen and hydrogen.

8. A method according to claim 1 in which the carbonaceous powder is thermally treated by heating in a lower than atmospheric pressure environment.

9. A method according to claim 1 in which the graphene sheets are graphene nanosheets having lateral dimensions of greater than 200 nanometres.

10. A method according to claim 1 in which the current at the graphite electrode during electrochemical erosion of the electrode is greater than 0.5 A/cm 2 .

11. A method according to claim 1 in which graphene sheets are produced at a rate of greater than 1 kg per hour, per square metre of graphite electrode immersed in the ionic liquid.

12. A method according to claim 1 in which the graphite electrode is cathodic in polarity during electrochemical erosion.

13. A method according to claim 1 comprising the step of:
(a) forming a carbonaceous powder by electrochemical erosion of two or more graphite electrodes in a molten salt comprising hydrogen ions, each of the two or more graphite electrodes alternately serving as a negative electrode in connection with a positive counter electrode for periods of time in order to effect the electrochemical erosion.

14. A method of producing graphene sheets comprising the steps of:
(a) forming a carbonaceous powder by electrochemical erosion of a graphite electrode in an ionic liquid, the ionic liquid comprising hydrogen ions,
(b) recovering the resulting carbonaceous powder from the ionic liquid, and
(c) thermally treating the carbonaceous powder by heating the carbonaceous powder in a non-oxidising or reducing atmosphere to produce a thermally treated powder comprising graphene sheets.

15. A method of producing graphene sheets comprising the steps of:
(a) forming a carbonaceous powder by electrochemical intercalation of a metallic species and a hydrogen species into a graphite electrode, the graphite electrode being arranged in contact with an electrolyte, the electrolyte comprising the metallic species and the hydrogen species,
(b) recovering the resulting carbonaceous powder from the electrolyte, and
(c) thermally treating the carbonaceous powder by heating the carbonaceous powder in a non-oxidising or reducing atmosphere to produce a thermally treated powder comprising graphene sheets.

16. A method of producing graphene sheets comprising the steps of:
(a) forming a carbonaceous powder by electrochemical erosion of a graphite electrode in a molten salt, in which electrochemical erosion of the graphite electrode is performed under an atmosphere comprising an inert gas and hydrogen, and
(b) recovering the resulting carbonaceous powder, which comprises graphene sheets, from the molten salt.

17. A method according to claim 16 further comprising the step of:
(c) thermally treating the carbonaceous powder by heating the carbonaceous powder in a non-oxidising atmosphere to produce a thermally treated powder comprising graphene sheets.

18. A method according to claim 16 in which the atmosphere comprises between 2 and 10 mole percent hydrogen and the inert gas is selected from the group consisting of argon and nitrogen.

19. A method according to claim 18 , wherein the atmosphere is a dry atmosphere.

Assignees

• Cambridge Entpr Ltd

Inventors

• Fray Derek
• Kamali Ali

Classifications

• C25B11/044

  Impregnation of carbon · CPC title

• C01B2204/32

  Size or surface area · CPC title

• C01B32/19

  by exfoliation · CPC title

• C25B1/00

  Electrolytic production of inorganic compounds or non-metals · CPC title

• C01B32/184

  Preparation · CPC title