Patent
US 11,772,975 B2CHEMICAL-FREE PRODUCTION OF GRAPHENE MATERIALS
Aruna Zhamu, Bor Z Jang
Global Graphene Group, Inc., Dayton, OH (US)·Oct. 3, 2023·US
Copyright © 2026 Matter42. All rights reserved.
Patent
Atlas literature
Patent
US 11,772,975 B2Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 A flow chart showing the most commonly used prior art process of producing highly oxidized NGPs that entails tedious chemical oxidation/intercalation, …
FIG. 2 A flow chart showing the presently invented two-step process for producing isolated graphitic materials
FIG. 3 A flow chart showing the presently invented process for producing isolated graphitic materials via a 35 continuous ball mill.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus; b) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, high energy mill, basket mill, agitator ball mill, con-tinuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, or vibratory sieve, wherein said separating includes a step of dissolving, melting, vaporizing, sublimat-ing, or burning off said solid carrier material to separate said graphene sheet, wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a func-tional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligonucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w —R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkyle-ther), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoroaralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than
The method of claim 1, wherein said solid carrier material includes micron- or nanometer-scaled particles that can be dissolved in a solvent, melted above a melting temperature, etched away using an etching agent, vaporized or sublimated away, or burned off, and said method includes a step of dissolving, melting, etching, vaporizing, sublimat-ing, or burning off said solid carrier material for separating said graphene sheets.
The method of claim 1 wherein said graphitic material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modi-fied graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, meso-carbon micro-bead, or a combination thereof.
The method of claim 1, wherein said graphitic material contains a non-intercalated and non-oxidized graphitic material that has never been previously exposed to a chemi-cal or oxidation treatment prior to said mixing step.
The method of claim 1 wherein said graphene sheets contain single-layer graphene sheets.
The method of claim 1 wherein said graphene sheets contain at least 80% single-layer graphene or at least 80% few-layer graphene having no greater than 10 graphene layers.
The method of claim 1 wherein said graphene sheets contain pristine graphene, oxidized graphene with less than 5% oxygen content by weight, graphene fluoride, graphene fluoride with less than 5% fluorine by weight, graphene with a carbon content no less than 95% by weight, or chemically modified graphene. 19
The method of claim 1, wherein operating said energy impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. ∗ ∗ ∗ ∗ ∗
15
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, or glass; b) operating said energy impacting apparatus with a fre-quency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein said sepa-rating includes a step of dissolving, melting, etching, vapor-izing, sublimating, or burning off said solid carrier material to separate said graphene sheets, wherein the energy impact-ing apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O—C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting B₂ apparatus, wherein said solid carrier material includes plas-tic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal par-ticles or wires, or a combination thereof; b) operating said energy impacting apparatus with a frequency and an inten-sity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer, wherein said separating includes a step of dissolving, melting, etching, vaporizing, sublimating, or burning off said solid carrier material to separate said graphene sheets wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R' SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
Materials described outside the worked examples.
graphitic material
solid carrier material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Thickness | 200–20000 nm | — |
Thickness |
Patents and literature cited by this patent (applicant and examiner references).
Cited patents · 67
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 11,772,975 B2Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 A flow chart showing the most commonly used prior art process of producing highly oxidized NGPs that entails tedious chemical oxidation/intercalation, …
FIG. 2 A flow chart showing the presently invented two-step process for producing isolated graphitic materials
FIG. 3 A flow chart showing the presently invented process for producing isolated graphitic materials via a 35 continuous ball mill.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus; b) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, high energy mill, basket mill, agitator ball mill, con-tinuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, or vibratory sieve, wherein said separating includes a step of dissolving, melting, vaporizing, sublimat-ing, or burning off said solid carrier material to separate said graphene sheet, wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a func-tional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligonucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w —R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkyle-ther), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoroaralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than
The method of claim 1, wherein said solid carrier material includes micron- or nanometer-scaled particles that can be dissolved in a solvent, melted above a melting temperature, etched away using an etching agent, vaporized or sublimated away, or burned off, and said method includes a step of dissolving, melting, etching, vaporizing, sublimat-ing, or burning off said solid carrier material for separating said graphene sheets.
The method of claim 1 wherein said graphitic material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modi-fied graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, meso-carbon micro-bead, or a combination thereof.
The method of claim 1, wherein said graphitic material contains a non-intercalated and non-oxidized graphitic material that has never been previously exposed to a chemi-cal or oxidation treatment prior to said mixing step.
The method of claim 1 wherein said graphene sheets contain single-layer graphene sheets.
The method of claim 1 wherein said graphene sheets contain at least 80% single-layer graphene or at least 80% few-layer graphene having no greater than 10 graphene layers.
The method of claim 1 wherein said graphene sheets contain pristine graphene, oxidized graphene with less than 5% oxygen content by weight, graphene fluoride, graphene fluoride with less than 5% fluorine by weight, graphene with a carbon content no less than 95% by weight, or chemically modified graphene. 19
The method of claim 1, wherein operating said energy impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. ∗ ∗ ∗ ∗ ∗
15
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, or glass; b) operating said energy impacting apparatus with a fre-quency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein said sepa-rating includes a step of dissolving, melting, etching, vapor-izing, sublimating, or burning off said solid carrier material to separate said graphene sheets, wherein the energy impact-ing apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O—C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting B₂ apparatus, wherein said solid carrier material includes plas-tic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal par-ticles or wires, or a combination thereof; b) operating said energy impacting apparatus with a frequency and an inten-sity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer, wherein said separating includes a step of dissolving, melting, etching, vaporizing, sublimating, or burning off said solid carrier material to separate said graphene sheets wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R' SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
Materials described outside the worked examples.
graphitic material
solid carrier material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Thickness | 200–20000 nm | — |
Thickness |
Patents and literature cited by this patent (applicant and examiner references).
Cited patents · 67
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 11,772,975 B2Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 A flow chart showing the most commonly used prior art process of producing highly oxidized NGPs that entails tedious chemical oxidation/intercalation, …
FIG. 2 A flow chart showing the presently invented two-step process for producing isolated graphitic materials
FIG. 3 A flow chart showing the presently invented process for producing isolated graphitic materials via a 35 continuous ball mill.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus; b) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, high energy mill, basket mill, agitator ball mill, con-tinuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, or vibratory sieve, wherein said separating includes a step of dissolving, melting, vaporizing, sublimat-ing, or burning off said solid carrier material to separate said graphene sheet, wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a func-tional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligonucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w —R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkyle-ther), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoroaralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than
The method of claim 1, wherein said solid carrier material includes micron- or nanometer-scaled particles that can be dissolved in a solvent, melted above a melting temperature, etched away using an etching agent, vaporized or sublimated away, or burned off, and said method includes a step of dissolving, melting, etching, vaporizing, sublimat-ing, or burning off said solid carrier material for separating said graphene sheets.
The method of claim 1 wherein said graphitic material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modi-fied graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, meso-carbon micro-bead, or a combination thereof.
The method of claim 1, wherein said graphitic material contains a non-intercalated and non-oxidized graphitic material that has never been previously exposed to a chemi-cal or oxidation treatment prior to said mixing step.
The method of claim 1 wherein said graphene sheets contain single-layer graphene sheets.
The method of claim 1 wherein said graphene sheets contain at least 80% single-layer graphene or at least 80% few-layer graphene having no greater than 10 graphene layers.
The method of claim 1 wherein said graphene sheets contain pristine graphene, oxidized graphene with less than 5% oxygen content by weight, graphene fluoride, graphene fluoride with less than 5% fluorine by weight, graphene with a carbon content no less than 95% by weight, or chemically modified graphene. 19
The method of claim 1, wherein operating said energy impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. ∗ ∗ ∗ ∗ ∗
15
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, or glass; b) operating said energy impacting apparatus with a fre-quency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein said sepa-rating includes a step of dissolving, melting, etching, vapor-izing, sublimating, or burning off said solid carrier material to separate said graphene sheets, wherein the energy impact-ing apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O—C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting B₂ apparatus, wherein said solid carrier material includes plas-tic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal par-ticles or wires, or a combination thereof; b) operating said energy impacting apparatus with a frequency and an inten-sity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer, wherein said separating includes a step of dissolving, melting, etching, vaporizing, sublimating, or burning off said solid carrier material to separate said graphene sheets wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R' SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
Materials described outside the worked examples.
graphitic material
solid carrier material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Thickness | 200–20000 nm | — |
Thickness |
Patents and literature cited by this patent (applicant and examiner references).
Cited patents · 67
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 11,772,975 B2Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 A flow chart showing the most commonly used prior art process of producing highly oxidized NGPs that entails tedious chemical oxidation/intercalation, …
FIG. 2 A flow chart showing the presently invented two-step process for producing isolated graphitic materials
FIG. 3 A flow chart showing the presently invented process for producing isolated graphitic materials via a 35 continuous ball mill.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus; b) operating said energy impacting apparatus with a frequency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, high energy mill, basket mill, agitator ball mill, con-tinuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, or vibratory sieve, wherein said separating includes a step of dissolving, melting, vaporizing, sublimat-ing, or burning off said solid carrier material to separate said graphene sheet, wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a func-tional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligonucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si(—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N—CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w —R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkyle-ther), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoroaralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than
The method of claim 1, wherein said solid carrier material includes micron- or nanometer-scaled particles that can be dissolved in a solvent, melted above a melting temperature, etched away using an etching agent, vaporized or sublimated away, or burned off, and said method includes a step of dissolving, melting, etching, vaporizing, sublimat-ing, or burning off said solid carrier material for separating said graphene sheets.
The method of claim 1 wherein said graphitic material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modi-fied graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, meso-carbon micro-bead, or a combination thereof.
The method of claim 1, wherein said graphitic material contains a non-intercalated and non-oxidized graphitic material that has never been previously exposed to a chemi-cal or oxidation treatment prior to said mixing step.
The method of claim 1 wherein said graphene sheets contain single-layer graphene sheets.
The method of claim 1 wherein said graphene sheets contain at least 80% single-layer graphene or at least 80% few-layer graphene having no greater than 10 graphene layers.
The method of claim 1 wherein said graphene sheets contain pristine graphene, oxidized graphene with less than 5% oxygen content by weight, graphene fluoride, graphene fluoride with less than 5% fluorine by weight, graphene with a carbon content no less than 95% by weight, or chemically modified graphene. 19
The method of claim 1, wherein operating said energy impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. ∗ ∗ ∗ ∗ ∗
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A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting apparatus, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, or glass; b) operating said energy impacting apparatus with a fre-quency and an intensity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein said sepa-rating includes a step of dissolving, melting, etching, vapor-izing, sublimating, or burning off said solid carrier material to separate said graphene sheets, wherein the energy impact-ing apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O—C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R'SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
A method of producing isolated graphene sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material having never been previously intercalated or chemically oxidized and multiple particles of a solid carrier material to form a mixture in an impacting chamber of an energy impacting B₂ apparatus, wherein said solid carrier material includes plas-tic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal par-ticles or wires, or a combination thereof; b) operating said energy impacting apparatus with a frequency and an inten-sity for a length of time sufficient for peeling off graphene sheets from said graphitic material and transferring said graphene sheets directly from said graphitic material to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene sheets, wherein the energy impacting apparatus is a vibratory ball mill, planetary ball mill, high energy mill, basket mill, agitator ball mill, continuous ball mill, stirred ball mill, pressurized ball mill, freezer mill, vibratory sieve, or resonant acoustic mixer, wherein said separating includes a step of dissolving, melting, etching, vaporizing, sublimating, or burning off said solid carrier material to separate said graphene sheets wherein said impacting chamber further contains a functionalizing agent and said graphene sheets contain chemically functionalized graphene wherein said functionalizing agent contains O~C—SY, and Y is a functional group of a protein, a peptide, an enzyme, an antibody, a nucleotide, an oligo-nucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R'—OH, R'—NR'2, R' SH, R'CHO, R'CN, R'X (a halide), R'N+(R')3X−, R'SiR'3, R'Si (—OR'—)yR'3-y, R'Si(—O—SiR'2—)OR', R'—R", R'—N— CO, (C₂H₄O—)wH, (—C₃H₆)—)wH, (—C₂H₄O)w—R', (C₃H₆O)w—R', wherein R' is selected from hydrogen, alkyl, aryl, cycloalkyl, or aralkyl, cycloaryl, or poly(alkylether), and R" is fluoroalkyl, fluoroaryl, fuorocycloalkyl, fluoro-aralkyl, or cycloaryl, and w is an integer greater than one and less than 200, wherein y is an integer of less than 3.
Materials described outside the worked examples.
graphitic material
solid carrier material
Measurements and analyses referenced in the patent, with their drawing references.
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Thickness | 200–20000 nm | — |
Thickness |
Patents and literature cited by this patent (applicant and examiner references).
Cited patents · 67
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FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
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Temperature | 30–1000 °C | — |
Temperature | 46–200 °C | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | ≤ 5 hours | — |
Temperature | ≥ 600 °C | — |
Duration | ≤ 4 hours | — |
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isolated graphene sheets
solid carrier material (organic, polymeric, metal, or glass particles)
solid carrier material (plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires)
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graphene fluoride
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synthetic graphite
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FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 30–1000 °C | — |
Temperature | 46–200 °C | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | ≤ 5 hours | — |
Temperature | ≥ 600 °C | — |
Duration | ≤ 4 hours | — |
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isolated graphene sheets
solid carrier material (organic, polymeric, metal, or glass particles)
solid carrier material (plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires)
pristine graphene
C
graphene fluoride
natural graphite
synthetic graphite
highly oriented pyrolytic graphite
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer’s route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 30–1000 °C | — |
Temperature | 46–200 °C | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | ≤ 5 hours | — |
Temperature | ≥ 600 °C | — |
Duration | ≤ 4 hours | — |
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