Expansion and exfoliation of graphite to form graphene

Patent metadata

Field	Value
Publication number	US-10787365-B2
Application number	US-201715775203-A
Country	US
Kind code	B2
Filing date	Jan 17, 2017
Priority date	Jan 18, 2016
Publication date	Sep 29, 2020
Grant date	Sep 29, 2020

Abstract

Graphene production methods are described based on subjecting non-covalent graphite intercalated compounds, such as graphite bisulfate, to expansion conditions such as shocks of heat and/or microwaves followed by turbulence-assisted exfoliation to produce few-layer, high quality graphene flakes. Depending on the approach selected for the exfoliation step, free-flowing graphene powder, graphene slurry, or an aqueous graphene mixture can be obtained. Surfactants can aid in dispersion, and graphene inks can be formed. The parameters of the process are simple, efficient and low-cost enabling therefore the scale-up of production. Applications include electrodes and energy storage devices.

First claim

What is claimed is:

1. A method comprising:
subjecting at least one graphite intercalation compound to expansion conditions to produce graphene, wherein the expansion conditions include a thermal shock treatment without previous or parallel exposure to chemicals; and
subjecting the graphene to turbulence-assisted exfoliation to obtain a high quality graphene reaction product,
wherein a particle size of the graphite intercalation compound and an expansion time of the expansion conditions are adapted to provide the high quality graphene reaction product in which an average expansion in a reaction product is at least 10,000, and
wherein the high quality graphene reaction product is characterized by (1) a Raman D/G band ratio of 0.04, (2) an oxygen to carbon ratio of 0.06, and (3) a six fold symmetric electron diffraction pattern.

2. The method of claim 1 , wherein the graphite intercalation compound is in the form of flakes, and the flakes of the graphite intercalation compound are characterized by an average extension along a basal plane of a distance of at least 50 microns.

3. The method of claim 1 , wherein the graphite intercalation compound is expandable graphite.

4. The method of claim 1 , wherein the graphite intercalation compound is a graphite salt.

5. The method of claim 1 , wherein the graphite intercalation compound is intumescent graphite bisulfate.

6. The method of claim 1 , wherein the graphite intercalation compound has a percent carbon of at least 85%.

7. The method of claim 1 , wherein the graphite intercalation compound has sulfur as an intercalated element of highest atomic percent.

8. The method of claim 1 , wherein the graphite intercalation compound has an interlayer spacing larger than a graphitic interlayer spacing of 0.341.

9. The method of claim 1 , wherein the expansion conditions include vaporization of intercalated species.

10. The method of claim 1 , wherein the expansion conditions include electromagnetic waves.

11. The method of claim 1 , wherein the expansion conditions include application of heat, which is applied without microwaves.

12. The method of claim 1 , wherein the time of subjecting the graphite to the expansion conditions is less than 80 seconds.

13. The method of claim 1 , wherein the graphene is in a form having ten or fewer graphene layers.

14. The method of claim 1 , wherein the graphene is subjected to sonication and/or mechanical shear.

15. The method of claim 1 , wherein the graphene is dispersed in a solvent.

16. A composition prepared by the method of claim 1 .

17. An ink composition prepared by the method of claim 1 and comprising at least one solvent vehicle.

18. An energy storage system comprising the composition of claim 16 .

19. A method comprising:
subjecting at least one graphite intercalation compound to expansion conditions to produce graphene, wherein the expansion conditions include a thermal shock treatment without previous or parallel exposure to chemicals; and
subjecting the graphene to turbulence-assisted exfoliation to obtain a high quality graphene reaction product,
wherein a particle size of the graphite intercalation compound and an expansion time of the expansion conditions are adapted to provide the high quality graphene reaction product in which an average separation distance between two adjacent graphene sheets in the reaction product is at least 5 microns, and
wherein the high quality graphene reaction product is characterized by (1) a Raman D/G band ratio of 0.04, (2) an oxygen to carbon ratio of 0.06, and (3) a six fold symmetric electron diffraction pattern.

Assignees

• Univ King Abdullah Sci & Tech

Inventors

• Patole Shashikant P
• Costa Pedro M F J

Classifications

• C01B32/19 Primary

  by exfoliation · CPC title

• H01M10/054

  Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium · CPC title

• B82Y30/00

  Nanotechnology for materials or surface science, e.g. nanocomposites · CPC title

• Y02E60/10

  Energy storage using batteries · CPC title

• B82Y40/00

  Manufacture or treatment of nanostructures · CPC title