IP Library Granted Patent US 10,633,255
Granted Patent B2
US 10,633,255 · App. 15/805,010 · Granted Apr 28, 2020

Graphene macro-assembly-fullerene composite for electrical energy storage

Inventors: Patrick G. Campbell (Oakland, CA); Theodore F. Baumann (Discovery Bay, CA); Juergen Biener (San Leandro, CA); Matthew Merrill (Dublin, CA); Elizabeth Montalvo (Oakland, CA); Marcus Worsley (Hayward, CA); Monika M. Biener (San Leandro, CA); Maira Raquel Ceron Hernandez (Livermore, CA)
Assignee: Lawrence Livermore National Security, LLC
C01B32/194B82Y30/00C01B32/156H01G11/32H01G11/36H01G11/38H01G11/86H01M4/133H01M4/1393H01M4/364H01M4/587B82Y40/00H01G11/68H01G11/70Y02E60/13Y10S977/738Y10S977/896Y10S977/948
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Quick Facts
Patent No.
US 10,633,255
App. No.
15/805,010
Granted
Apr 28, 2020
Kind
B2
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.

Claims (26)

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.

Assignments (2)
CONFIRMATORY LICENSE Recorded Jan 25, 2018
From: LAWRENCE LIVERMORE NATIONAL SECURITY, LLC
To: U.S. DEPARTMENT OF ENERGY
Reel/Frame 044724/0208 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 7, 2017
From: CAMPBELL, PATRICK G.; BAUMANN, THEODORE F.; BIENER, JUERGEN; MERRILL, MATTHEW; MONTALVO, ELIZABETH; WORSLEY, MARCUS; BIENER, MONIKA M.; CERON HERNANDEZ, MAIRA RAQUEL
To: LAWRENCE LIVERMORE NATIONAL SECURITY, LLC
Reel/Frame 044057/0267 →
Continuity (2)
Continuation In Part 15260197 · Sep 8, 2016
Related Publication 20180118574A1 · May 3, 2018