PROCESS FOR PRODUCING INTEGRAL GRAPHENE FILMS FROM FUNCTIONALIZED GRAPHENE SHEETS | Matter42 Literature
Patent
Atlas literature
Patent
US 12,246,967 B2
PROCESS FOR PRODUCING INTEGRAL GRAPHENE FILMS FROM FUNCTIONALIZED GRAPHENE SHEETS
Aruna Zhamu, Bor Z. Jang
Global Graphene Group, Inc., Dayton, OH (US)·Mar. 11, 2025·US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
FIG. 1 Schematic drawing illustrating the processes for producing conventional paper, mat, film, and membrane of 40 simply aggregated graphite or graphene …
FIG. 2
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
FIG. 3
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
FIG. 4
FIG. 4(c) Schematic of yet another reverse roll-based graphene layer transfer apparatus for producing an integral graphene film composed of highly oriented …
FIG. 5
FIG. 5(c) An example to illustrate one mechanism with which neighboring chemically functionalized graphene sheets are chemically interconnected together.
FIG. 6
FIG. 6 Tensile strength and Young’s modulus of three graphene films: one derived from highly oriented chemically functionalized graphene sheets, one derived …
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
2 independent · 12 dependent
1
Independentchemically functionalized graphene sheetsintegral graphene film
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 gra-phene 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 proce-dure includes mechanical shear stress-induced align-ment of said chemically functionalized graphene sheets along a film planar direction, and partially or com-pletely 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 reac-tions 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 com-binations thereof; wherein said chemically functional-ized graphene sheets contain a chemical functional group selected from an oxygenated group consisting of hydroxyl, peroxide, ether, keto, aldehyde, and combi-nations thereof; or wherein said chemically function-alized 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.
2
Dependent← claim 1integral graphene film
The process of claim 1, wherein said inter-plane spacing d002 is from 0.4 nm to 1.2 nm, the non-carbon element content is from 1% to 20%, or physical density from 2.0 to 2.15 g/cm3.
3
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a thermal conductivity from 200 to 1,600 W/mK or an electrical conductivity from 600 to 15,000 S/cm.
4
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a Young’s modulus from 20 GPa to 200 GPa, or a tensile strength from 1.0 GPa to 3.5 G Pa.
5
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-phene sheets.
6
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means.
7
Independentchemically functionalized graphene sheetsun-functionalized graphene sheetsintegral graphene film
A process for producing an integral graphene film from graphene sheets, said process comprising: (a) preparing a graphene dispersion having un-function-alized graphene sheets dispersed in a liquid medium; (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 proce-dure includes mechanical shear stress-induced align-ment of said un-functionalized graphene sheets along a film planar direction, and partially or completely removing said liquid medium from said film to form a dried graphene film comprising aligned graphene sheets; (c) bringing said dried graphene film in contact with a chemical functionalizing agent so as to produce a film of chemically functionalized graphene sheets having chemical functional groups attached thereto and a noncarbon element content of 0.1% to 47% by weight; and (d) using high-energy radiation to induce chemical reac-tions or chemical bonding between chemical functional groups attached to adjacent chemically functionalized graphene sheets to form said integral graphene film, wherein said integral graphene film comprises chemi-cally functionalized graphene sheets that are chemi-cally 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 gra-phene film has a length from 1 cm to 10,000 m, a width from 1 cm to 5 m, a thickness from 10 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, quinoi-dal, fluorocarbon, derivatives thereof, and combina-tions 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 combi-nations thereof; or wherein said chemically function-alized 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.
8
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically functionalized graphene sheets further contain a chemical functional group selected from a derivative of an azide compound selected from the group consisting of 2-azido-ethanol, 3-azidopropan-1-amine, 4-(2-azidoethoxy)-4-27 28 oxobutanoic acid, 2-azidoethyl-2-bromo-2-methylpropano- 9. The process of claim 7, wherein said chemically ate, chlorocarbonate, azidocarbonate, dichlorocarbene, functionalized graphene sheets further contain a chemical carbene, aryne, nitrene, (R—)-oxycarbonyl nitrenes, where functional group selected from the group consisting of R=any one of the following groups, —SO₃H, —COOH, —NH2, —OH, —R'CHOH, —CHO, 5 —CN, —COCl, halide, —COSH, —SH, —COOR', —SR', —SiR'3, —Si(—OR'—)yR'3—y, —Si(—O—SiR'2—)OR', —R", Li, AlR'2, Hg—X, TlZ₂ and Mg—X; wherein y is an integer equal to or less than 3, R' is hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), R" is 10 fluoroalkyl, fluoroaryl, fluorocycloalkyl, fluoroaralkyl or cycloaryl, X is halide, and Z is carboxylate or trifluoroac-etate, derivatives thereof, and combinations thereof. O S
10
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically O 15 functionalized graphene sheets further contain a chemical O O O functional group selected from the group consisting of O O 2-3 amidoamines, polyamides, aliphatic amines, modified ali-phatic amines, cycloaliphatic amines, aromatic amines, O O anhydrides, ketimines, diethylenetriamine (DETA), triethyl-20 ene-tetramine (TETA), tetraethylene-pentamine (TEPA), polyethylene polyamine, polyamine epoxy adduct, phenolic O O hardener, non-brominated curing agent, non-amine cura-tives, derivatives thereof, and combinations thereof.
11
Dependent← claim 7integral graphene film
The process claim 7, wherein said chemically func-O O tionalized graphene sheets further contain a chemical func-tional group selected from OY, NHY, O~C—OY, P~C— O O NR'Y, O~C—SY, O~C—Y, —CR'1—OY, N'Y or C'Y, a O O derivative thereof, or a combination thereof, and Y is a 30 functional group of a protein, a peptide, an amino acid, an enzyme, an antibody, a nucleotide, an oligonucleotide, an O O antigen, or an enzyme substrate, enzyme inhibitor or the O O transition state analog of an enzyme substrate or is selected O O from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X, R'N+ O O 35 (R')3X", R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—) OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆O—)w O O O H, (—C₂H₄O)w—R', (C₃H₆O)w—R', R', and w is an integer O O greater than one and less than 200.
12
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a thermal conductivity from 350 to 1,600 W/mK or O O an electrical conductivity from 1,000 to 15,000 S/cm. O O O
13
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a Young’s modulus from 20 GPa to 130 GPa or a O O 45 tensile strength from 1.0 GPa to 3.0 GPa. O O
14
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-50 phene sheets.
15
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means. and combinations thereof. ∗ ∗ ∗ ∗ ∗
Materials
Materials described outside the worked examples.
chemically functionalized graphene sheets
Starting Material
integral graphene film
Product
Process steps
Additional fabrication and treatment steps described in the patent.
1
Film Deposition And Functionalization
Step 1
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation (electron beam, Gamma ray, or X-ray)
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
starting material:chemically functionalized graphene sheets dispersed in liquid medium
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
sem
SEM
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
PROCESS FOR PRODUCING INTEGRAL GRAPHENE FILMS FROM FUNCTIONALIZED GRAPHENE SHEETS
Aruna Zhamu, Bor Z. Jang
Global Graphene Group, Inc., Dayton, OH (US)·Mar. 11, 2025·US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
FIG. 1 Schematic drawing illustrating the processes for producing conventional paper, mat, film, and membrane of 40 simply aggregated graphite or graphene …
FIG. 2
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
FIG. 3
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
FIG. 4
FIG. 4(c) Schematic of yet another reverse roll-based graphene layer transfer apparatus for producing an integral graphene film composed of highly oriented …
FIG. 5
FIG. 5(c) An example to illustrate one mechanism with which neighboring chemically functionalized graphene sheets are chemically interconnected together.
FIG. 6
FIG. 6 Tensile strength and Young’s modulus of three graphene films: one derived from highly oriented chemically functionalized graphene sheets, one derived …
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
2 independent · 12 dependent
1
Independentchemically functionalized graphene sheetsintegral graphene film
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 gra-phene 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 proce-dure includes mechanical shear stress-induced align-ment of said chemically functionalized graphene sheets along a film planar direction, and partially or com-pletely 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 reac-tions 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 com-binations thereof; wherein said chemically functional-ized graphene sheets contain a chemical functional group selected from an oxygenated group consisting of hydroxyl, peroxide, ether, keto, aldehyde, and combi-nations thereof; or wherein said chemically function-alized 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.
2
Dependent← claim 1integral graphene film
The process of claim 1, wherein said inter-plane spacing d002 is from 0.4 nm to 1.2 nm, the non-carbon element content is from 1% to 20%, or physical density from 2.0 to 2.15 g/cm3.
3
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a thermal conductivity from 200 to 1,600 W/mK or an electrical conductivity from 600 to 15,000 S/cm.
4
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a Young’s modulus from 20 GPa to 200 GPa, or a tensile strength from 1.0 GPa to 3.5 G Pa.
5
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-phene sheets.
6
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means.
7
Independentchemically functionalized graphene sheetsun-functionalized graphene sheetsintegral graphene film
A process for producing an integral graphene film from graphene sheets, said process comprising: (a) preparing a graphene dispersion having un-function-alized graphene sheets dispersed in a liquid medium; (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 proce-dure includes mechanical shear stress-induced align-ment of said un-functionalized graphene sheets along a film planar direction, and partially or completely removing said liquid medium from said film to form a dried graphene film comprising aligned graphene sheets; (c) bringing said dried graphene film in contact with a chemical functionalizing agent so as to produce a film of chemically functionalized graphene sheets having chemical functional groups attached thereto and a noncarbon element content of 0.1% to 47% by weight; and (d) using high-energy radiation to induce chemical reac-tions or chemical bonding between chemical functional groups attached to adjacent chemically functionalized graphene sheets to form said integral graphene film, wherein said integral graphene film comprises chemi-cally functionalized graphene sheets that are chemi-cally 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 gra-phene film has a length from 1 cm to 10,000 m, a width from 1 cm to 5 m, a thickness from 10 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, quinoi-dal, fluorocarbon, derivatives thereof, and combina-tions 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 combi-nations thereof; or wherein said chemically function-alized 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.
8
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically functionalized graphene sheets further contain a chemical functional group selected from a derivative of an azide compound selected from the group consisting of 2-azido-ethanol, 3-azidopropan-1-amine, 4-(2-azidoethoxy)-4-27 28 oxobutanoic acid, 2-azidoethyl-2-bromo-2-methylpropano- 9. The process of claim 7, wherein said chemically ate, chlorocarbonate, azidocarbonate, dichlorocarbene, functionalized graphene sheets further contain a chemical carbene, aryne, nitrene, (R—)-oxycarbonyl nitrenes, where functional group selected from the group consisting of R=any one of the following groups, —SO₃H, —COOH, —NH2, —OH, —R'CHOH, —CHO, 5 —CN, —COCl, halide, —COSH, —SH, —COOR', —SR', —SiR'3, —Si(—OR'—)yR'3—y, —Si(—O—SiR'2—)OR', —R", Li, AlR'2, Hg—X, TlZ₂ and Mg—X; wherein y is an integer equal to or less than 3, R' is hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), R" is 10 fluoroalkyl, fluoroaryl, fluorocycloalkyl, fluoroaralkyl or cycloaryl, X is halide, and Z is carboxylate or trifluoroac-etate, derivatives thereof, and combinations thereof. O S
10
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically O 15 functionalized graphene sheets further contain a chemical O O O functional group selected from the group consisting of O O 2-3 amidoamines, polyamides, aliphatic amines, modified ali-phatic amines, cycloaliphatic amines, aromatic amines, O O anhydrides, ketimines, diethylenetriamine (DETA), triethyl-20 ene-tetramine (TETA), tetraethylene-pentamine (TEPA), polyethylene polyamine, polyamine epoxy adduct, phenolic O O hardener, non-brominated curing agent, non-amine cura-tives, derivatives thereof, and combinations thereof.
11
Dependent← claim 7integral graphene film
The process claim 7, wherein said chemically func-O O tionalized graphene sheets further contain a chemical func-tional group selected from OY, NHY, O~C—OY, P~C— O O NR'Y, O~C—SY, O~C—Y, —CR'1—OY, N'Y or C'Y, a O O derivative thereof, or a combination thereof, and Y is a 30 functional group of a protein, a peptide, an amino acid, an enzyme, an antibody, a nucleotide, an oligonucleotide, an O O antigen, or an enzyme substrate, enzyme inhibitor or the O O transition state analog of an enzyme substrate or is selected O O from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X, R'N+ O O 35 (R')3X", R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—) OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆O—)w O O O H, (—C₂H₄O)w—R', (C₃H₆O)w—R', R', and w is an integer O O greater than one and less than 200.
12
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a thermal conductivity from 350 to 1,600 W/mK or O O an electrical conductivity from 1,000 to 15,000 S/cm. O O O
13
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a Young’s modulus from 20 GPa to 130 GPa or a O O 45 tensile strength from 1.0 GPa to 3.0 GPa. O O
14
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-50 phene sheets.
15
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means. and combinations thereof. ∗ ∗ ∗ ∗ ∗
Materials
Materials described outside the worked examples.
chemically functionalized graphene sheets
Starting Material
integral graphene film
Product
Process steps
Additional fabrication and treatment steps described in the patent.
1
Film Deposition And Functionalization
Step 1
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation (electron beam, Gamma ray, or X-ray)
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
starting material:chemically functionalized graphene sheets dispersed in liquid medium
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
sem
SEM
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
PROCESS FOR PRODUCING INTEGRAL GRAPHENE FILMS FROM FUNCTIONALIZED GRAPHENE SHEETS
Aruna Zhamu, Bor Z. Jang
Global Graphene Group, Inc., Dayton, OH (US)·Mar. 11, 2025·US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
FIG. 1 Schematic drawing illustrating the processes for producing conventional paper, mat, film, and membrane of 40 simply aggregated graphite or graphene …
FIG. 2
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
FIG. 3
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
FIG. 4
FIG. 4(c) Schematic of yet another reverse roll-based graphene layer transfer apparatus for producing an integral graphene film composed of highly oriented …
FIG. 5
FIG. 5(c) An example to illustrate one mechanism with which neighboring chemically functionalized graphene sheets are chemically interconnected together.
FIG. 6
FIG. 6 Tensile strength and Young’s modulus of three graphene films: one derived from highly oriented chemically functionalized graphene sheets, one derived …
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
2 independent · 12 dependent
1
Independentchemically functionalized graphene sheetsintegral graphene film
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 gra-phene 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 proce-dure includes mechanical shear stress-induced align-ment of said chemically functionalized graphene sheets along a film planar direction, and partially or com-pletely 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 reac-tions 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 com-binations thereof; wherein said chemically functional-ized graphene sheets contain a chemical functional group selected from an oxygenated group consisting of hydroxyl, peroxide, ether, keto, aldehyde, and combi-nations thereof; or wherein said chemically function-alized 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.
2
Dependent← claim 1integral graphene film
The process of claim 1, wherein said inter-plane spacing d002 is from 0.4 nm to 1.2 nm, the non-carbon element content is from 1% to 20%, or physical density from 2.0 to 2.15 g/cm3.
3
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a thermal conductivity from 200 to 1,600 W/mK or an electrical conductivity from 600 to 15,000 S/cm.
4
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a Young’s modulus from 20 GPa to 200 GPa, or a tensile strength from 1.0 GPa to 3.5 G Pa.
5
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-phene sheets.
6
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means.
7
Independentchemically functionalized graphene sheetsun-functionalized graphene sheetsintegral graphene film
A process for producing an integral graphene film from graphene sheets, said process comprising: (a) preparing a graphene dispersion having un-function-alized graphene sheets dispersed in a liquid medium; (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 proce-dure includes mechanical shear stress-induced align-ment of said un-functionalized graphene sheets along a film planar direction, and partially or completely removing said liquid medium from said film to form a dried graphene film comprising aligned graphene sheets; (c) bringing said dried graphene film in contact with a chemical functionalizing agent so as to produce a film of chemically functionalized graphene sheets having chemical functional groups attached thereto and a noncarbon element content of 0.1% to 47% by weight; and (d) using high-energy radiation to induce chemical reac-tions or chemical bonding between chemical functional groups attached to adjacent chemically functionalized graphene sheets to form said integral graphene film, wherein said integral graphene film comprises chemi-cally functionalized graphene sheets that are chemi-cally 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 gra-phene film has a length from 1 cm to 10,000 m, a width from 1 cm to 5 m, a thickness from 10 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, quinoi-dal, fluorocarbon, derivatives thereof, and combina-tions 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 combi-nations thereof; or wherein said chemically function-alized 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.
8
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically functionalized graphene sheets further contain a chemical functional group selected from a derivative of an azide compound selected from the group consisting of 2-azido-ethanol, 3-azidopropan-1-amine, 4-(2-azidoethoxy)-4-27 28 oxobutanoic acid, 2-azidoethyl-2-bromo-2-methylpropano- 9. The process of claim 7, wherein said chemically ate, chlorocarbonate, azidocarbonate, dichlorocarbene, functionalized graphene sheets further contain a chemical carbene, aryne, nitrene, (R—)-oxycarbonyl nitrenes, where functional group selected from the group consisting of R=any one of the following groups, —SO₃H, —COOH, —NH2, —OH, —R'CHOH, —CHO, 5 —CN, —COCl, halide, —COSH, —SH, —COOR', —SR', —SiR'3, —Si(—OR'—)yR'3—y, —Si(—O—SiR'2—)OR', —R", Li, AlR'2, Hg—X, TlZ₂ and Mg—X; wherein y is an integer equal to or less than 3, R' is hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), R" is 10 fluoroalkyl, fluoroaryl, fluorocycloalkyl, fluoroaralkyl or cycloaryl, X is halide, and Z is carboxylate or trifluoroac-etate, derivatives thereof, and combinations thereof. O S
10
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically O 15 functionalized graphene sheets further contain a chemical O O O functional group selected from the group consisting of O O 2-3 amidoamines, polyamides, aliphatic amines, modified ali-phatic amines, cycloaliphatic amines, aromatic amines, O O anhydrides, ketimines, diethylenetriamine (DETA), triethyl-20 ene-tetramine (TETA), tetraethylene-pentamine (TEPA), polyethylene polyamine, polyamine epoxy adduct, phenolic O O hardener, non-brominated curing agent, non-amine cura-tives, derivatives thereof, and combinations thereof.
11
Dependent← claim 7integral graphene film
The process claim 7, wherein said chemically func-O O tionalized graphene sheets further contain a chemical func-tional group selected from OY, NHY, O~C—OY, P~C— O O NR'Y, O~C—SY, O~C—Y, —CR'1—OY, N'Y or C'Y, a O O derivative thereof, or a combination thereof, and Y is a 30 functional group of a protein, a peptide, an amino acid, an enzyme, an antibody, a nucleotide, an oligonucleotide, an O O antigen, or an enzyme substrate, enzyme inhibitor or the O O transition state analog of an enzyme substrate or is selected O O from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X, R'N+ O O 35 (R')3X", R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—) OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆O—)w O O O H, (—C₂H₄O)w—R', (C₃H₆O)w—R', R', and w is an integer O O greater than one and less than 200.
12
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a thermal conductivity from 350 to 1,600 W/mK or O O an electrical conductivity from 1,000 to 15,000 S/cm. O O O
13
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a Young’s modulus from 20 GPa to 130 GPa or a O O 45 tensile strength from 1.0 GPa to 3.0 GPa. O O
14
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-50 phene sheets.
15
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means. and combinations thereof. ∗ ∗ ∗ ∗ ∗
Materials
Materials described outside the worked examples.
chemically functionalized graphene sheets
Starting Material
integral graphene film
Product
Process steps
Additional fabrication and treatment steps described in the patent.
1
Film Deposition And Functionalization
Step 1
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation (electron beam, Gamma ray, or X-ray)
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
starting material:chemically functionalized graphene sheets dispersed in liquid medium
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
sem
SEM
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
PROCESS FOR PRODUCING INTEGRAL GRAPHENE FILMS FROM FUNCTIONALIZED GRAPHENE SHEETS
Aruna Zhamu, Bor Z. Jang
Global Graphene Group, Inc., Dayton, OH (US)·Mar. 11, 2025·US
Drawings
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1
FIG. 1 Schematic drawing illustrating the processes for producing conventional paper, mat, film, and membrane of 40 simply aggregated graphite or graphene …
FIG. 2
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
FIG. 3
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
FIG. 4
FIG. 4(c) Schematic of yet another reverse roll-based graphene layer transfer apparatus for producing an integral graphene film composed of highly oriented …
FIG. 5
FIG. 5(c) An example to illustrate one mechanism with which neighboring chemically functionalized graphene sheets are chemically interconnected together.
FIG. 6
FIG. 6 Tensile strength and Young’s modulus of three graphene films: one derived from highly oriented chemically functionalized graphene sheets, one derived …
Claims
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
2 independent · 12 dependent
1
Independentchemically functionalized graphene sheetsintegral graphene film
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 gra-phene 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 proce-dure includes mechanical shear stress-induced align-ment of said chemically functionalized graphene sheets along a film planar direction, and partially or com-pletely 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 reac-tions 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 com-binations thereof; wherein said chemically functional-ized graphene sheets contain a chemical functional group selected from an oxygenated group consisting of hydroxyl, peroxide, ether, keto, aldehyde, and combi-nations thereof; or wherein said chemically function-alized 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.
2
Dependent← claim 1integral graphene film
The process of claim 1, wherein said inter-plane spacing d002 is from 0.4 nm to 1.2 nm, the non-carbon element content is from 1% to 20%, or physical density from 2.0 to 2.15 g/cm3.
3
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a thermal conductivity from 200 to 1,600 W/mK or an electrical conductivity from 600 to 15,000 S/cm.
4
Dependent← claim 1integral graphene film
The process of claim 1, wherein said integral graphene film has a Young’s modulus from 20 GPa to 200 GPa, or a tensile strength from 1.0 GPa to 3.5 G Pa.
5
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-phene sheets.
6
Dependent← claim 1integral graphene film
The process of claim 1, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means.
7
Independentchemically functionalized graphene sheetsun-functionalized graphene sheetsintegral graphene film
A process for producing an integral graphene film from graphene sheets, said process comprising: (a) preparing a graphene dispersion having un-function-alized graphene sheets dispersed in a liquid medium; (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 proce-dure includes mechanical shear stress-induced align-ment of said un-functionalized graphene sheets along a film planar direction, and partially or completely removing said liquid medium from said film to form a dried graphene film comprising aligned graphene sheets; (c) bringing said dried graphene film in contact with a chemical functionalizing agent so as to produce a film of chemically functionalized graphene sheets having chemical functional groups attached thereto and a noncarbon element content of 0.1% to 47% by weight; and (d) using high-energy radiation to induce chemical reac-tions or chemical bonding between chemical functional groups attached to adjacent chemically functionalized graphene sheets to form said integral graphene film, wherein said integral graphene film comprises chemi-cally functionalized graphene sheets that are chemi-cally 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 gra-phene film has a length from 1 cm to 10,000 m, a width from 1 cm to 5 m, a thickness from 10 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, quinoi-dal, fluorocarbon, derivatives thereof, and combina-tions 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 combi-nations thereof; or wherein said chemically function-alized 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.
8
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically functionalized graphene sheets further contain a chemical functional group selected from a derivative of an azide compound selected from the group consisting of 2-azido-ethanol, 3-azidopropan-1-amine, 4-(2-azidoethoxy)-4-27 28 oxobutanoic acid, 2-azidoethyl-2-bromo-2-methylpropano- 9. The process of claim 7, wherein said chemically ate, chlorocarbonate, azidocarbonate, dichlorocarbene, functionalized graphene sheets further contain a chemical carbene, aryne, nitrene, (R—)-oxycarbonyl nitrenes, where functional group selected from the group consisting of R=any one of the following groups, —SO₃H, —COOH, —NH2, —OH, —R'CHOH, —CHO, 5 —CN, —COCl, halide, —COSH, —SH, —COOR', —SR', —SiR'3, —Si(—OR'—)yR'3—y, —Si(—O—SiR'2—)OR', —R", Li, AlR'2, Hg—X, TlZ₂ and Mg—X; wherein y is an integer equal to or less than 3, R' is hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), R" is 10 fluoroalkyl, fluoroaryl, fluorocycloalkyl, fluoroaralkyl or cycloaryl, X is halide, and Z is carboxylate or trifluoroac-etate, derivatives thereof, and combinations thereof. O S
10
Dependent← claim 7integral graphene film
The process of claim 7, wherein said chemically O 15 functionalized graphene sheets further contain a chemical O O O functional group selected from the group consisting of O O 2-3 amidoamines, polyamides, aliphatic amines, modified ali-phatic amines, cycloaliphatic amines, aromatic amines, O O anhydrides, ketimines, diethylenetriamine (DETA), triethyl-20 ene-tetramine (TETA), tetraethylene-pentamine (TEPA), polyethylene polyamine, polyamine epoxy adduct, phenolic O O hardener, non-brominated curing agent, non-amine cura-tives, derivatives thereof, and combinations thereof.
11
Dependent← claim 7integral graphene film
The process claim 7, wherein said chemically func-O O tionalized graphene sheets further contain a chemical func-tional group selected from OY, NHY, O~C—OY, P~C— O O NR'Y, O~C—SY, O~C—Y, —CR'1—OY, N'Y or C'Y, a O O derivative thereof, or a combination thereof, and Y is a 30 functional group of a protein, a peptide, an amino acid, an enzyme, an antibody, a nucleotide, an oligonucleotide, an O O antigen, or an enzyme substrate, enzyme inhibitor or the O O transition state analog of an enzyme substrate or is selected O O from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X, R'N+ O O 35 (R')3X", R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—) OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆O—)w O O O H, (—C₂H₄O)w—R', (C₃H₆O)w—R', R', and w is an integer O O greater than one and less than 200.
12
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a thermal conductivity from 350 to 1,600 W/mK or O O an electrical conductivity from 1,000 to 15,000 S/cm. O O O
13
Dependent← claim 7integral graphene film
The process of claim 7, wherein said integral graphene film has a Young’s modulus from 20 GPa to 130 GPa or a O O 45 tensile strength from 1.0 GPa to 3.0 GPa. O O
14
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of compressing said integral graphene film to increase a degree of graphene sheet orientation and physical density, and to improve contact between chemically functionalized gra-50 phene sheets.
15
Dependent← claim 7integral graphene film
The process of claim 7, further comprising a step of reducing said non-carbon content to less than 20% by weight using chemical, thermal, UV, or radiation means. and combinations thereof. ∗ ∗ ∗ ∗ ∗
Materials
Materials described outside the worked examples.
chemically functionalized graphene sheets
Starting Material
integral graphene film
Product
Process steps
Additional fabrication and treatment steps described in the patent.
1
Film Deposition And Functionalization
Step 1
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation (electron beam, Gamma ray, or X-ray)
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
starting material:chemically functionalized graphene sheets dispersed in liquid medium
Characterization
Measurements and analyses referenced in the patent, with their drawing references.
sem
SEM
FIG. 2(b) An SEM image of a cross-section of a flexible graphite foil, showing many graphite flakes with orienta- tions not parallel to the flexible graphite foil …
optional post step:compressing integral graphene film
non carbon element content:0.1% to 47% by weight
Materials:chemically functionalized graphene sheetsintegral graphene film
2
Film Deposition Functionalization And Bonding
Step 2
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
functionalization:contact with chemical functionalizing agent after drying
optional post step:compressing integral graphene film
non carbon element content after functionalization:0.1% to 47% by weight
Materials:un-functionalized graphene sheetsintegral graphene film
SEM
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
thermal conductivity of integral graphene film (claim 3, process from functionalized sheets)
200–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 3, process from functionalized sheets)
600–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 4, process from functionalized sheets)
20–200 GPa
integral graphene film
tensile strength of integral graphene film (claim 4, process from functionalized sheets)
1–3.5 GPa
integral graphene film
thermal conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
350–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
1000–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 13, process from un-functionalized sheets)
20–130 GPa
integral graphene film
tensile strength of integral graphene film (claim 13, process from un-functionalized sheets)
1–3 GPa
integral graphene film
—
200–1600 W
—
—
350–1500 W
—
Thickness
2–500000 nm
—
Thickness
10–200000 nm
—
Duration
900–7200 s
—
Duration
0.1–105 sec
—
Duration
102–104 sec
—
Duration
48–72 hours
—
Duration
4–120 hours
—
Temperature
20–25 °C
—
Thickness
100–300 µm
—
—
140–300 W
—
—
10–30 W
—
Temperature
200–400 °C
—
Temperature
150–250 °C
—
Thickness
2800–3000 cm
—
Temperature
200–700 °C
—
Duration
48–96 hours
—
Duration
10–100 minutes
—
Thickness
≥ 1 nm
—
Thickness
≥ 50 µm
—
—
≥ 350 W
—
—
≥ 600 W
—
—
≥ 1 W
—
—
≥ 1200 W
—
Thickness
10–500000 nm
—
—
350–1600 W
—
Thickness
4–50 cm
—
Thickness
1–50 µm
—
US 2010/0055025 A12010/0055025 A1 3/2010 Jang et al.
US 2011/0017587 A12011/0017587 A1 1/2011 Zhamu et al.
US 2011/0017955 A12011/0017955 A1 1/2011 Zhamu et al.
US 2011/0062422 A12011/0062422 A1 3/2011 Ryu et al.
US 2011/0127638 A12011/0127638 A1 * 6/2011 Brenner.............. H01L 29/1606examiner
US 2014/0147648 A12014/0147648 A1 5/2014 Zhamu et al.
US 2015/0218003 A12015/0218003 A1 * 8/2015 Zhamu.................. C01B 32/192examiner
US 2015/0239741 A12015/0239741 A1 * 8/2015 Burton................. C08G 65/321examiner
US 2015/0284253 A12015/0284253 A1 10/2015 Zhamu et al.
US 2016/0079001 A12016/0079001 A1 * 3/2016 Lin...................... H01G 4/1245examiner
US 2016/0304351 A12016/0304351 A1 * 10/2016 Zhamu..................... C09K 5/14examiner
US 2017/0021387 A12017/0021387 A1 * 1/2017 Lin.......................... B05D 1/28examiner
US 2017/0081193 A12017/0081193 A1 * 3/2017 Zhamu.................. C01B 32/194examiner
Cited non-patent literature · 7
KR-101489174-B1, Google Patent translation (Year: 2015).
Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers. Cong et al., “Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers” Scientific Report (2012) vol. 2, pp. 613-618.
Facile fabrication of light, flexible and multifunctional graphene fibers. Dong et al., “Facile fabrication of light, flexible and multifunctional graphene fibers” Ad. Mater. (2012) vol. 24, pp. 1856-1861.
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications. Georgakilas et al., “Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications” Chem. Rev. (2012) vol. 112, No. 11, pp. 6156-6214; DOI: 10.1021/cr3000412.10.1021/cr3000412
Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives. Karlicky et al., “Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives” ACS Nano (2013) vol. 7, No. 8, pp. 6434-6464.
Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity. Wan et al., “Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity” PNAS Latest Articles, 6 pages. www.pnas.org/cgi/doi/10.1073/pnas.1719111115.10.1073/pnas.1719111115
Graphene chiral liquid crystals and macroscopic assembled fibers. Xu et al., “Graphene chiral liquid crystals and macroscopic assembled fibers” Nature Communications (2011) vol. 2, p. 571-580.
optional post step:compressing integral graphene film
non carbon element content:0.1% to 47% by weight
Materials:chemically functionalized graphene sheetsintegral graphene film
2
Film Deposition Functionalization And Bonding
Step 2
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
functionalization:contact with chemical functionalizing agent after drying
optional post step:compressing integral graphene film
non carbon element content after functionalization:0.1% to 47% by weight
Materials:un-functionalized graphene sheetsintegral graphene film
SEM
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
thermal conductivity of integral graphene film (claim 3, process from functionalized sheets)
200–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 3, process from functionalized sheets)
600–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 4, process from functionalized sheets)
20–200 GPa
integral graphene film
tensile strength of integral graphene film (claim 4, process from functionalized sheets)
1–3.5 GPa
integral graphene film
thermal conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
350–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
1000–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 13, process from un-functionalized sheets)
20–130 GPa
integral graphene film
tensile strength of integral graphene film (claim 13, process from un-functionalized sheets)
1–3 GPa
integral graphene film
—
200–1600 W
—
—
350–1500 W
—
Thickness
2–500000 nm
—
Thickness
10–200000 nm
—
Duration
900–7200 s
—
Duration
0.1–105 sec
—
Duration
102–104 sec
—
Duration
48–72 hours
—
Duration
4–120 hours
—
Temperature
20–25 °C
—
Thickness
100–300 µm
—
—
140–300 W
—
—
10–30 W
—
Temperature
200–400 °C
—
Temperature
150–250 °C
—
Thickness
2800–3000 cm
—
Temperature
200–700 °C
—
Duration
48–96 hours
—
Duration
10–100 minutes
—
Thickness
≥ 1 nm
—
Thickness
≥ 50 µm
—
—
≥ 350 W
—
—
≥ 600 W
—
—
≥ 1 W
—
—
≥ 1200 W
—
Thickness
10–500000 nm
—
—
350–1600 W
—
Thickness
4–50 cm
—
Thickness
1–50 µm
—
US 2010/0055025 A12010/0055025 A1 3/2010 Jang et al.
US 2011/0017587 A12011/0017587 A1 1/2011 Zhamu et al.
US 2011/0017955 A12011/0017955 A1 1/2011 Zhamu et al.
US 2011/0062422 A12011/0062422 A1 3/2011 Ryu et al.
US 2011/0127638 A12011/0127638 A1 * 6/2011 Brenner.............. H01L 29/1606examiner
US 2014/0147648 A12014/0147648 A1 5/2014 Zhamu et al.
US 2015/0218003 A12015/0218003 A1 * 8/2015 Zhamu.................. C01B 32/192examiner
US 2015/0239741 A12015/0239741 A1 * 8/2015 Burton................. C08G 65/321examiner
US 2015/0284253 A12015/0284253 A1 10/2015 Zhamu et al.
US 2016/0079001 A12016/0079001 A1 * 3/2016 Lin...................... H01G 4/1245examiner
US 2016/0304351 A12016/0304351 A1 * 10/2016 Zhamu..................... C09K 5/14examiner
US 2017/0021387 A12017/0021387 A1 * 1/2017 Lin.......................... B05D 1/28examiner
US 2017/0081193 A12017/0081193 A1 * 3/2017 Zhamu.................. C01B 32/194examiner
Cited non-patent literature · 7
KR-101489174-B1, Google Patent translation (Year: 2015).
Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers. Cong et al., “Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers” Scientific Report (2012) vol. 2, pp. 613-618.
Facile fabrication of light, flexible and multifunctional graphene fibers. Dong et al., “Facile fabrication of light, flexible and multifunctional graphene fibers” Ad. Mater. (2012) vol. 24, pp. 1856-1861.
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications. Georgakilas et al., “Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications” Chem. Rev. (2012) vol. 112, No. 11, pp. 6156-6214; DOI: 10.1021/cr3000412.10.1021/cr3000412
Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives. Karlicky et al., “Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives” ACS Nano (2013) vol. 7, No. 8, pp. 6434-6464.
Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity. Wan et al., “Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity” PNAS Latest Articles, 6 pages. www.pnas.org/cgi/doi/10.1073/pnas.1719111115.10.1073/pnas.1719111115
Graphene chiral liquid crystals and macroscopic assembled fibers. Xu et al., “Graphene chiral liquid crystals and macroscopic assembled fibers” Nature Communications (2011) vol. 2, p. 571-580.
optional post step:compressing integral graphene film
non carbon element content:0.1% to 47% by weight
Materials:chemically functionalized graphene sheetsintegral graphene film
2
Film Deposition Functionalization And Bonding
Step 2
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
functionalization:contact with chemical functionalizing agent after drying
optional post step:compressing integral graphene film
non carbon element content after functionalization:0.1% to 47% by weight
Materials:un-functionalized graphene sheetsintegral graphene film
SEM
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
thermal conductivity of integral graphene film (claim 3, process from functionalized sheets)
200–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 3, process from functionalized sheets)
600–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 4, process from functionalized sheets)
20–200 GPa
integral graphene film
tensile strength of integral graphene film (claim 4, process from functionalized sheets)
1–3.5 GPa
integral graphene film
thermal conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
350–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
1000–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 13, process from un-functionalized sheets)
20–130 GPa
integral graphene film
tensile strength of integral graphene film (claim 13, process from un-functionalized sheets)
1–3 GPa
integral graphene film
—
200–1600 W
—
—
350–1500 W
—
Thickness
2–500000 nm
—
Thickness
10–200000 nm
—
Duration
900–7200 s
—
Duration
0.1–105 sec
—
Duration
102–104 sec
—
Duration
48–72 hours
—
Duration
4–120 hours
—
Temperature
20–25 °C
—
Thickness
100–300 µm
—
—
140–300 W
—
—
10–30 W
—
Temperature
200–400 °C
—
Temperature
150–250 °C
—
Thickness
2800–3000 cm
—
Temperature
200–700 °C
—
Duration
48–96 hours
—
Duration
10–100 minutes
—
Thickness
≥ 1 nm
—
Thickness
≥ 50 µm
—
—
≥ 350 W
—
—
≥ 600 W
—
—
≥ 1 W
—
—
≥ 1200 W
—
Thickness
10–500000 nm
—
—
350–1600 W
—
Thickness
4–50 cm
—
Thickness
1–50 µm
—
US 2010/0055025 A12010/0055025 A1 3/2010 Jang et al.
US 2011/0017587 A12011/0017587 A1 1/2011 Zhamu et al.
US 2011/0017955 A12011/0017955 A1 1/2011 Zhamu et al.
US 2011/0062422 A12011/0062422 A1 3/2011 Ryu et al.
US 2011/0127638 A12011/0127638 A1 * 6/2011 Brenner.............. H01L 29/1606examiner
US 2014/0147648 A12014/0147648 A1 5/2014 Zhamu et al.
US 2015/0218003 A12015/0218003 A1 * 8/2015 Zhamu.................. C01B 32/192examiner
US 2015/0239741 A12015/0239741 A1 * 8/2015 Burton................. C08G 65/321examiner
US 2015/0284253 A12015/0284253 A1 10/2015 Zhamu et al.
US 2016/0079001 A12016/0079001 A1 * 3/2016 Lin...................... H01G 4/1245examiner
US 2016/0304351 A12016/0304351 A1 * 10/2016 Zhamu..................... C09K 5/14examiner
US 2017/0021387 A12017/0021387 A1 * 1/2017 Lin.......................... B05D 1/28examiner
US 2017/0081193 A12017/0081193 A1 * 3/2017 Zhamu.................. C01B 32/194examiner
Cited non-patent literature · 7
KR-101489174-B1, Google Patent translation (Year: 2015).
Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers. Cong et al., “Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers” Scientific Report (2012) vol. 2, pp. 613-618.
Facile fabrication of light, flexible and multifunctional graphene fibers. Dong et al., “Facile fabrication of light, flexible and multifunctional graphene fibers” Ad. Mater. (2012) vol. 24, pp. 1856-1861.
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications. Georgakilas et al., “Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications” Chem. Rev. (2012) vol. 112, No. 11, pp. 6156-6214; DOI: 10.1021/cr3000412.10.1021/cr3000412
Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives. Karlicky et al., “Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives” ACS Nano (2013) vol. 7, No. 8, pp. 6434-6464.
Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity. Wan et al., “Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity” PNAS Latest Articles, 6 pages. www.pnas.org/cgi/doi/10.1073/pnas.1719111115.10.1073/pnas.1719111115
Graphene chiral liquid crystals and macroscopic assembled fibers. Xu et al., “Graphene chiral liquid crystals and macroscopic assembled fibers” Nature Communications (2011) vol. 2, p. 571-580.
optional post step:compressing integral graphene film
non carbon element content:0.1% to 47% by weight
Materials:chemically functionalized graphene sheetsintegral graphene film
2
Film Deposition Functionalization And Bonding
Step 2
Process details
alignment:mechanical shear stress-induced alignment along film planar direction
bonding method:high-energy radiation
deposition method:high-rate or high-intensity spraying, or extrusion plus high-rate wiping
functionalization:contact with chemical functionalizing agent after drying
optional post step:compressing integral graphene film
non carbon element content after functionalization:0.1% to 47% by weight
Materials:un-functionalized graphene sheetsintegral graphene film
SEM
FIG. 3(b) A SEM image of a cross-section of a conven- tional graphene paper prepared from discrete graphene sheets/platelets using a paper-making process (e.g. …
thermal conductivity of integral graphene film (claim 3, process from functionalized sheets)
200–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 3, process from functionalized sheets)
600–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 4, process from functionalized sheets)
20–200 GPa
integral graphene film
tensile strength of integral graphene film (claim 4, process from functionalized sheets)
1–3.5 GPa
integral graphene film
thermal conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
350–1600 W/mK
integral graphene film
electrical conductivity of integral graphene film (claim 12, process from un-functionalized sheets)
1000–15000 S/cm
integral graphene film
Young's modulus of integral graphene film (claim 13, process from un-functionalized sheets)
20–130 GPa
integral graphene film
tensile strength of integral graphene film (claim 13, process from un-functionalized sheets)
1–3 GPa
integral graphene film
—
200–1600 W
—
—
350–1500 W
—
Thickness
2–500000 nm
—
Thickness
10–200000 nm
—
Duration
900–7200 s
—
Duration
0.1–105 sec
—
Duration
102–104 sec
—
Duration
48–72 hours
—
Duration
4–120 hours
—
Temperature
20–25 °C
—
Thickness
100–300 µm
—
—
140–300 W
—
—
10–30 W
—
Temperature
200–400 °C
—
Temperature
150–250 °C
—
Thickness
2800–3000 cm
—
Temperature
200–700 °C
—
Duration
48–96 hours
—
Duration
10–100 minutes
—
Thickness
≥ 1 nm
—
Thickness
≥ 50 µm
—
—
≥ 350 W
—
—
≥ 600 W
—
—
≥ 1 W
—
—
≥ 1200 W
—
Thickness
10–500000 nm
—
—
350–1600 W
—
Thickness
4–50 cm
—
Thickness
1–50 µm
—
US 2010/0055025 A12010/0055025 A1 3/2010 Jang et al.
US 2011/0017587 A12011/0017587 A1 1/2011 Zhamu et al.
US 2011/0017955 A12011/0017955 A1 1/2011 Zhamu et al.
US 2011/0062422 A12011/0062422 A1 3/2011 Ryu et al.
US 2011/0127638 A12011/0127638 A1 * 6/2011 Brenner.............. H01L 29/1606examiner
US 2014/0147648 A12014/0147648 A1 5/2014 Zhamu et al.
US 2015/0218003 A12015/0218003 A1 * 8/2015 Zhamu.................. C01B 32/192examiner
US 2015/0239741 A12015/0239741 A1 * 8/2015 Burton................. C08G 65/321examiner
US 2015/0284253 A12015/0284253 A1 10/2015 Zhamu et al.
US 2016/0079001 A12016/0079001 A1 * 3/2016 Lin...................... H01G 4/1245examiner
US 2016/0304351 A12016/0304351 A1 * 10/2016 Zhamu..................... C09K 5/14examiner
US 2017/0021387 A12017/0021387 A1 * 1/2017 Lin.......................... B05D 1/28examiner
US 2017/0081193 A12017/0081193 A1 * 3/2017 Zhamu.................. C01B 32/194examiner
Cited non-patent literature · 7
KR-101489174-B1, Google Patent translation (Year: 2015).
Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers. Cong et al., “Wet-spinning assembly of continuous, neat, and macroscopic graphene fibers” Scientific Report (2012) vol. 2, pp. 613-618.
Facile fabrication of light, flexible and multifunctional graphene fibers. Dong et al., “Facile fabrication of light, flexible and multifunctional graphene fibers” Ad. Mater. (2012) vol. 24, pp. 1856-1861.
Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications. Georgakilas et al., “Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications” Chem. Rev. (2012) vol. 112, No. 11, pp. 6156-6214; DOI: 10.1021/cr3000412.10.1021/cr3000412
Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives. Karlicky et al., “Halogenated Graphenes: Rapidly Growing Family of Graphene Derivatives” ACS Nano (2013) vol. 7, No. 8, pp. 6434-6464.
Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity. Wan et al., “Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity” PNAS Latest Articles, 6 pages. www.pnas.org/cgi/doi/10.1073/pnas.1719111115.10.1073/pnas.1719111115
Graphene chiral liquid crystals and macroscopic assembled fibers. Xu et al., “Graphene chiral liquid crystals and macroscopic assembled fibers” Nature Communications (2011) vol. 2, p. 571-580.