US 12,246,967 B2
Process for producing integral graphene films from functionalized graphene sheets
Aruna Zhamu, Springboro, OH (US); and Bor Z. Jang, Centerville, OH (US)
Assigned to Global Graphene Group, Inc., Dayton, OH (US)
Filed by Nanotek Instruments, Inc., Dayton, OH (US)
Filed on May 15, 2018, as Appl. No. 15/980,015.
Prior Publication US 2019/0352186 A1, Nov. 21, 2019
Int. Cl. H01M 4/00 (2006.01); C01B 32/194 (2017.01); C09K 5/14 (2006.01); H01B 1/24 (2006.01); H01B 5/00 (2006.01); B82Y 30/00 (2011.01); B82Y 40/00 (2011.01)
CPC C01B 32/194 (2017.08) [C09K 5/14 (2013.01); H01B 1/24 (2013.01); H01B 5/00 (2013.01); B82Y 30/00 (2013.01); B82Y 40/00 (2013.01); C01B 2204/04 (2013.01); C01B 2204/22 (2013.01); C01B 2204/24 (2013.01); C01B 2204/32 (2013.01); Y10S 977/734 (2013.01); Y10S 977/847 (2013.01)] 15 Claims
OG exemplary drawing
 
1. A process for producing an integral graphene film from chemically functionalized graphene sheets, said process comprising:
(a) preparing a graphene dispersion having chemically functionalized graphene sheets dispersed in a liquid medium wherein said chemically functionalized graphene sheets comprise chemical functional groups attached thereto and a non-carbon element content of 0.1% to 47% by weight;
(b) dispensing and depositing a wet film of said graphene dispersion onto a supporting substrate via high-rate or high-intensity spraying, or extrusion plus high-rate wiping, wherein said dispensing and depositing procedure includes mechanical shear stress-induced alignment of said chemically functionalized graphene sheets along a film planar direction, and partially or completely removing said liquid medium from said wet film to form a dried graphene film comprising aligned chemically functionalized graphene sheets; and
(c) using high-energy radiation to induce chemical reactions or chemical bonding between chemical functional groups attached to adjacent chemically functionalized graphene sheets in said dried graphene film to form said integral graphene film, wherein said integral graphene film comprises chemically functionalized graphene sheets that are chemically bonded or interconnected with one another having an inter-planar spacing d002 from 0.36 nm to 1.5 nm as determined by X-ray diffraction and a non-carbon element content of 0.1% to 47% by weight, wherein said functionalized graphene sheets are substantially parallel to one another and parallel to a planar direction of said integral graphene film and said integral graphene film has a length from 1 cm to 10,000 m, a width from 1 cm to 5 m, a thickness from 2 nm to 500 μm, and a physical density from 1.5 to 2.2 g/cm3, wherein said integral graphene film has a degree of graphene plane orientation from 87% to 99%,
wherein said chemically functionalized graphene sheets contain a chemical functional group selected from the group consisting of alkyl or aryl silane, alkyl or aralkyl group, hydroxyl group, carboxyl group, carboxylic group, amine group, sulfonate group, aldehydic group, quinoidal, fluorocarbon, derivatives thereof, and combinations thereof; wherein said chemically functionalized graphene sheets contain a chemical functional group selected from an oxygenated group consisting of hydroxyl, peroxide, ether, keto, aldehyde, and combinations thereof; or wherein said chemically functionalized graphene sheets contain a chemical functional group selected from the group consisting of 10,12-pentacosadiyn-1-ol, hydroiodic acid, 1-pyrenebutyric acid N-hydroxysuccinimide ester, 1-aminopyrene, derivatives thereof, and combinations thereof.