Graphene macro-assembly-fullerene composite for electrical energy storage

Patent metadata

Field	Value
Publication number	US-10633255-B2
Application number	US-201715805010-A
Country	US
Kind code	B2
Filing date	Nov 6, 2017
Priority date	Sep 8, 2016
Publication date	Apr 28, 2020
Grant date	Apr 28, 2020

Abstract

Disclosed here is a method for producing a graphene macro-assembly (GMA)-fullerene composite, comprising providing a GMA comprising a three-dimensional network of graphene sheets crosslinked by covalent carbon bonds, and incorporating at least 20 wt. % of at least one fullerene compound into the GMA based on the initial weight of the GMA to obtain a GMA-fullerene composite. Also described are a GMA-fullerene composite produced, an electrode comprising the GMA-fullerene composite, and a supercapacitor comprising the electrode and optionally an organic or ionic liquid electrolyte in contact with the electrode.

First claim

What is claimed is:

1. A composition comprising a graphene macro-assembly (GMA)-fullerene composite, wherein the GMA-fullerene composite comprises a GMA comprising a three-dimensional network of graphene sheets crosslinked by covalent carbon bonds, and at least 20 wt.% of at least one fullerene compound incorporated into the GMA based on the weight of the GMA.

2. The composition of claim 1 , wherein the fullerene compound is covalently bound to the graphene sheets.

3. The composition of claim 2 , wherein the fullerene compound is represented by: F*-(R 1 ) n , wherein:
F* comprises a fullerene having a surface comprising six-membered and five-membered rings,
R 1 comprises a conjugated linker covalently linking the fullerene to the graphene sheet, and
n is at least one.

4. The composition of claim 3 , wherein the conjugated linker comprises a conjugated C 1 -C 30 hydrocarbon chain optionally substituted with one or more heteroatoms.

5. The composition of claim 4 , wherein the conjugated linker comprises alternating single and multiple bonds, and optionally comprises at least one aromatic or heteroaromatic ring.

6. The composition of claim 4 , wherein n is 1 or 2, F* is C 60 or C 70 , and R 1 is

7. The composition of claim 1 , wherein the fullerene compound is noncovalently attached to the graphene sheets.

8. The composition of claim 7 , wherein the fullerene compound comprises at least one phenylamine functionlized fullerene.

9. The composition of claim 8 , wherein the phenylamine functionlized fullerene is represented by: F*-(R 2 ) n , wherein:
F* comprises a fullerene having a surface comprising six-membered and five-membered rings,
R 2 comprises a phenylamine group and a conjugated linker covalently connecting the phenylamine group to the fullerene, and
n is at least one.

10. The composition of claim 9 , wherein the conjugated linker comprises a conjugated C 1 -C 30 hydrocarbon chain optionally substituted with one or more heteroatoms.

11. The composition of claim 9 , wherein the conjugated linker comprises alternating single and multiple bonds, and optionally comprises at least one aromatic or heteroaromatic ring.

12. The composition of claim 9 , wherein n is 1 or 2, F* is C 60 or C 70 , and R 2 is

13. The composition of claim 1 , wherein the GMA-fullerene composite comprises at least 50 wt.% of the fullerene compound based on the weight of the GMA.

14. The composition of claim 1 , wherein the GMA-fullerene composite comprises at least 100 wt.% of the fullerene compound based on the weight of the GMA.

15. The composition of claim 1 , wherein the GMA-fullerene composite is a monolith having a thickness of at least 1 mm.

16. The composition of claim 1 , wherein the GMA-fullerene composite has an electrical conductivity of at least 10 S/m.

17. The composition of claim 1 , wherein the GMA-fullerene composite has a mesopore volume of at least 0.5 cm 3 /g.

18. The composition of claim 1 , wherein the GMA-fullerene composite has a BET surface area of at least 200 m 2 /g.

19. The composition of claim 1 , wherein the GMA-fullerene composite has a Young's modulus of at least 20 MPa.

20. A supercapacitor comprising an electrode comprising the GMA-fullerene composite of claim 1 , and further comprising an organic or ionic liquid electrolyte in contact with the electrode.

Assignees

• L Livermore Nat Security Llc

Inventors

• Campbell Patrick G
• Baumann Theodore F
• Biener Juergen
• Merrill Matthew
• Montalvo Elizabeth
• Worsley Marcus
• Biener Monika M
• Hernandez Maira Raquel Ceron

Classifications

• H01G11/86

  specially adapted for electrodes (carbonisation or activation of carbon for the manufacture of electrodes H01G11/34) · CPC title

• C01B32/156

  After-treatment · CPC title

• B82Y40/00

  Manufacture or treatment of nanostructures · CPC title

• C01B32/194 Primary

  After-treatment · CPC title

• H01M4/133

  Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx · CPC title