Method for producing graphene with a controllable number of layers

Patent metadata

Field	Value
Publication number	US-9764955-B2
Application number	US-201615000808-A
Country	US
Kind code	B2
Filing date	Jan 19, 2016
Priority date	Jan 19, 2016
Publication date	Sep 19, 2017
Grant date	Sep 19, 2017

Abstract

A method for producing pristine graphene of controllable thickness including monolayer, bilayer and multilayer graphene via microwave irradiation assisted intercalation of graphite with dicarboxylic acids of various molecular chain lengths and subsequent exfoliation is disclosed. The average thickness of the graphene and the number of layers in the graphene produced by the method can be controlled by the molecular chain length of the dicarboxylic acid used for intercalation.

First claim

The invention claimed is:

1. A method for producing graphene nanosheets with a predetermined number of layers of graphene, the predetermined number selected from the group consisting of 1, 2, 3-5, 6-8, and 9-15, the method comprising:
(a) selecting a dicarboxylic acid having a molecular chain length of 0.3-0.5 nm for producing graphene nanosheets with 1 layer of graphene, a molecular chain length of 0.55-0.75 nm for producing graphene nanosheets with 2 layers of graphene, a molecular chain length of 0.95-1.0 nm for producing graphene nanosheets with 3-5 layers of graphene, a molecular chain length of 1.15-1.25 nm for producing graphene nanosheets with 6-8 layers of graphene, and a molecular chain length of 1.3-2.0 nm for producing graphene nanosheets with 9-15 layers of graphene;
(b) treating graphite material with a liquid intercalating agent solution comprising the dicarboxylic acid for a first period of time to form a graphite intercalation compound;
(c) heating the graphite intercalation compound by microwave irradiation at a first power for a second period of time to form an expanded graphite intercalation compound;
(d) dispersing the expanded graphite intercalation compound into an alcohol which does not comprise methanol to form a colloidal suspension of the expanded graphite intercalation compound; and
(e) heating the colloidal suspension of the expanded graphite intercalation compound by microwave irradiation at a second power for a third period of time to exfoliate and/or reduce the expanded graphite intercalation compound and form the graphene nanosheets with the predetermined number of layers of graphene.

2. The method of claim 1 , wherein the graphene nanosheets with 1 layer of graphene have an average thickness of less than 0.4 nm, the graphene nanosheets with 2 layers of graphene have an average thickness of 0.4-0.8 nm, the graphene nanosheets with 3-5 layers of graphene have an average thickness of 1-1.65 nm, the graphene nanosheets with 6-8 layers of graphene have an average thickness of 2-2.7 nm, and the graphene nanosheets with 9-15 layers of graphene have an average thickness of 3-5 nm.

3. The method of claim 1 , wherein the graphene nanosheets with the predetermined number of layers of graphene are pristine graphene with an oxidized graphene content of less than 5% by weight relative to the total weight of the graphene nanosheets.

4. The method of claim 1 , wherein the graphene nanosheets with the predetermined number of layers of graphene are pristine graphene with a carbon content of greater than 95% by weight relative to the total weight of the graphene nanosheets.

5. The method of claim 1 , wherein the graphene nanosheets with the predetermined number of 1 or 2 layers of graphene are at least 80% of the total graphene nanosheets produced.

6. The method of claim 1 , wherein the dicarboxylic acid is at least one selected from the group consisting of a linear unsubstituted dicarboxylic acid, a linear substituted dicarboxylic acid, an aromatic dicarboxylic acid, an alkylitaconate dicarboxylic acid, and a branched-chain dicarboxylic acid.

7. The method of claim 1 , wherein the dicarboxylic acid is a linear dicarboxylic acid and has the general formula HOOC—(CH 2 ) n —COOH, wherein n is a whole number in the range of 0-2 or 4-8.

8. The method of claim 1 , wherein the dicarboxylic acid having a molecular chain length of 0.3-0.5 nm for producing graphene nanosheets with 1 layer of graphene is oxalic acid, the dicarboxylic acid having a molecular chain length of 0.55-0.75 nm for producing graphene nanosheets with 2 layers of graphene is succinic acid, the dicarboxylic acid having a molecular chain length of 0.95-1.0 nm for producing graphene nanosheets with 3-5 layers of graphene is adipic acid, the dicarboxylic acid having a molecular chain length of 1.15-1.25 nm for producing graphene nanosheets with 6-8 layers of graphene is suberic acid, and the dicarboxylic acid having a molecular chain length of 1.3-2.0 nm for producing graphene nanosheets with 9-15 layers of graphene is sebacic acid.

9. The method of claim 1 , wherein the first period of time is 8-30 hours in (b).

10. The method of claim 1 , wherein the graphite intercalation compound is heated at a temperature above 175° C. in (c).

11. The method of claim 1 , wherein the second period of time is 5-300 seconds in (c).

12. The method of claim 1 , wherein the first power of the microwave irradiation in (c) is 200-1000 W.

13. The method of claim 1 , wherein the alcohol in (d) comprises hexanol.

14. The method of claim 1 , wherein the third period of time in (e) is 10-100 minutes.

15. The method of claim 1 , wherein the colloidal suspension of the expanded graphite intercalation compound is heated at a temperature above 175° C. in (e).

16. The method of claim 1 , wherein the second power of the microwave irradiation in (e) is 200-1000 W.

Assignees

• Univ King Abdulaziz

Inventors

• Al-Hazmi Farag Saeed Marshoud
• Al-Ghamdi Ahmed Abdullah Salem
• ELSAYED Waleed Elsayed Mahmoud
• Obaid Abdullah Yousif Abdullah

Classifications

• C01B31/0446 Primary

  Chemistry & Metallurgy · mapped topic

• C01B2204/04

  Specific amount of layers or specific thickness · CPC title

• C01B32/22

  Intercalation · CPC title

• C01B2204/02

  Single layer graphene · CPC title

• C01B32/19

  by exfoliation · CPC title