Patent
US 11,453,594ENVIRONMENTALLY BENIGN PRODUCTION OF GRAPHENE OXIDE
Aruna Zhamu, Bor Z. Jang
US
Copyright © 2026 Matter42. All rights reserved.
Patent
Atlas literature
Patent
US 11,453,594Patent 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 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 oxide sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material, 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 to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) sequentially or concurrently oxidizing and separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene oxide sheets, wherein said step (c) comprises exposing said graphene sheets to an oxidizing medium, before, during or after the graphene sheets are separated from said solid carrier material particle surfaces, wherein said oxidizing medium is selected from an oxidizing gas or vapor, an oxidizing plasma, or an oxidizing liquid, wherein said oxidizing liquid is selected from a liquid comprising an oxidizer selected from sodium permanganate, transition metal permanganate; wherein said step (a) includes adding an oxidizing liquid in said mixture so that said oxidizing liquid acts to partially oxidize said graphene sheets during step (b). Currently amended
The method of claim 1, wherein a plurality of impacting balls or media are added to the impacting chamber of said energy impacting apparatus. Original
The method of claim 1, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, glass, ceramic, or inorganic material. Original
The method of claim 1, wherein said solid carrier material is selected from the group consisting of plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires, metal oxide particles, ceramic particles, and combinations thereof. Original
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 sublimed away, or burned off, and said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, or burning off said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, burning off, or ultrasonicating said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) comprises oxidizing said graphene sheets on said solid carrier material particle surfaces in an oxidizing liquid medium while being submitted to ultrasonication. Original
The method of claim 1 wherein said graphitic material is selected from the group consisting of natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modified graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, mesocarbon microbead, and combinations thereof. Original
The method of claim 1, 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, ultrasonic homogenizer mill, or resonant acoustic mixer. Original
The method of claim 1, wherein said graphitic material contains a non- intercalated and nonoxidized graphitic material that has never been previously exposed to a chemical or oxidation treatment prior to said mixing step. Original
The method of claim 1 wherein said graphene oxide sheets contain single-layer graphene oxide sheets. Original
The method of claim 1 wherein said graphene oxide sheets contain at least 80% single-layer graphene oxide or at least 80% few-layer graphene oxide having no greater than 10 graphene planes. Original
The method of claim 1, further comprising a step of exposing said graphene oxide to a functionalizing agent to produce functionalized graphene oxide. Original
The method of claim 1, wherein said procedure of operating said ener g y impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. Original
Canceled
Canceled
Canceled
Materials described outside the worked examples.
graphitic material
graphene oxide sheets
Additional fabrication and treatment steps described in the patent.
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 | 1–20 mm | — |
Temperature | 30–1000 °C |
Patent
Atlas literature
Patent
US 11,453,594Patent 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 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 oxide sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material, 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 to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) sequentially or concurrently oxidizing and separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene oxide sheets, wherein said step (c) comprises exposing said graphene sheets to an oxidizing medium, before, during or after the graphene sheets are separated from said solid carrier material particle surfaces, wherein said oxidizing medium is selected from an oxidizing gas or vapor, an oxidizing plasma, or an oxidizing liquid, wherein said oxidizing liquid is selected from a liquid comprising an oxidizer selected from sodium permanganate, transition metal permanganate; wherein said step (a) includes adding an oxidizing liquid in said mixture so that said oxidizing liquid acts to partially oxidize said graphene sheets during step (b). Currently amended
The method of claim 1, wherein a plurality of impacting balls or media are added to the impacting chamber of said energy impacting apparatus. Original
The method of claim 1, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, glass, ceramic, or inorganic material. Original
The method of claim 1, wherein said solid carrier material is selected from the group consisting of plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires, metal oxide particles, ceramic particles, and combinations thereof. Original
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 sublimed away, or burned off, and said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, or burning off said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, burning off, or ultrasonicating said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) comprises oxidizing said graphene sheets on said solid carrier material particle surfaces in an oxidizing liquid medium while being submitted to ultrasonication. Original
The method of claim 1 wherein said graphitic material is selected from the group consisting of natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modified graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, mesocarbon microbead, and combinations thereof. Original
The method of claim 1, 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, ultrasonic homogenizer mill, or resonant acoustic mixer. Original
The method of claim 1, wherein said graphitic material contains a non- intercalated and nonoxidized graphitic material that has never been previously exposed to a chemical or oxidation treatment prior to said mixing step. Original
The method of claim 1 wherein said graphene oxide sheets contain single-layer graphene oxide sheets. Original
The method of claim 1 wherein said graphene oxide sheets contain at least 80% single-layer graphene oxide or at least 80% few-layer graphene oxide having no greater than 10 graphene planes. Original
The method of claim 1, further comprising a step of exposing said graphene oxide to a functionalizing agent to produce functionalized graphene oxide. Original
The method of claim 1, wherein said procedure of operating said ener g y impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. Original
Canceled
Canceled
Canceled
Materials described outside the worked examples.
graphitic material
graphene oxide sheets
Additional fabrication and treatment steps described in the patent.
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 | 1–20 mm | — |
Temperature | 30–1000 °C |
Patent
Atlas literature
Patent
US 11,453,594Patent 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 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 oxide sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material, 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 to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) sequentially or concurrently oxidizing and separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene oxide sheets, wherein said step (c) comprises exposing said graphene sheets to an oxidizing medium, before, during or after the graphene sheets are separated from said solid carrier material particle surfaces, wherein said oxidizing medium is selected from an oxidizing gas or vapor, an oxidizing plasma, or an oxidizing liquid, wherein said oxidizing liquid is selected from a liquid comprising an oxidizer selected from sodium permanganate, transition metal permanganate; wherein said step (a) includes adding an oxidizing liquid in said mixture so that said oxidizing liquid acts to partially oxidize said graphene sheets during step (b). Currently amended
The method of claim 1, wherein a plurality of impacting balls or media are added to the impacting chamber of said energy impacting apparatus. Original
The method of claim 1, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, glass, ceramic, or inorganic material. Original
The method of claim 1, wherein said solid carrier material is selected from the group consisting of plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires, metal oxide particles, ceramic particles, and combinations thereof. Original
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 sublimed away, or burned off, and said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, or burning off said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, burning off, or ultrasonicating said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) comprises oxidizing said graphene sheets on said solid carrier material particle surfaces in an oxidizing liquid medium while being submitted to ultrasonication. Original
The method of claim 1 wherein said graphitic material is selected from the group consisting of natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modified graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, mesocarbon microbead, and combinations thereof. Original
The method of claim 1, 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, ultrasonic homogenizer mill, or resonant acoustic mixer. Original
The method of claim 1, wherein said graphitic material contains a non- intercalated and nonoxidized graphitic material that has never been previously exposed to a chemical or oxidation treatment prior to said mixing step. Original
The method of claim 1 wherein said graphene oxide sheets contain single-layer graphene oxide sheets. Original
The method of claim 1 wherein said graphene oxide sheets contain at least 80% single-layer graphene oxide or at least 80% few-layer graphene oxide having no greater than 10 graphene planes. Original
The method of claim 1, further comprising a step of exposing said graphene oxide to a functionalizing agent to produce functionalized graphene oxide. Original
The method of claim 1, wherein said procedure of operating said ener g y impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. Original
Canceled
Canceled
Canceled
Materials described outside the worked examples.
graphitic material
graphene oxide sheets
Additional fabrication and treatment steps described in the patent.
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 | 1–20 mm | — |
Temperature | 30–1000 °C |
Patent
Atlas literature
Patent
US 11,453,594Patent 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 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 oxide sheets directly from a graphitic material, said method comprising: a) mixing multiple particles of a graphitic material, 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 to surfaces of said solid carrier material particles to produce graphene-coated solid carrier particles inside said impacting chamber; and c) sequentially or concurrently oxidizing and separating said graphene sheets from said surfaces of said solid carrier material particles to produce said isolated graphene oxide sheets, wherein said step (c) comprises exposing said graphene sheets to an oxidizing medium, before, during or after the graphene sheets are separated from said solid carrier material particle surfaces, wherein said oxidizing medium is selected from an oxidizing gas or vapor, an oxidizing plasma, or an oxidizing liquid, wherein said oxidizing liquid is selected from a liquid comprising an oxidizer selected from sodium permanganate, transition metal permanganate; wherein said step (a) includes adding an oxidizing liquid in said mixture so that said oxidizing liquid acts to partially oxidize said graphene sheets during step (b). Currently amended
The method of claim 1, wherein a plurality of impacting balls or media are added to the impacting chamber of said energy impacting apparatus. Original
The method of claim 1, wherein said solid carrier material is selected from solid particles of an organic, polymeric, metal, glass, ceramic, or inorganic material. Original
The method of claim 1, wherein said solid carrier material is selected from the group consisting of plastic beads, plastic pellets, wax pellets, polymer powder or polymer reactor spheres, glass beads or fibers, metal particles or wires, metal oxide particles, ceramic particles, and combinations thereof. Original
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 sublimed away, or burned off, and said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, or burning off said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) includes a procedure of dissolving, melting, etching, vaporizing, subliming, burning off, or ultrasonicating said solid carrier material for separating said graphene sheets. Original
The method of claim 1, wherein said step (c) comprises oxidizing said graphene sheets on said solid carrier material particle surfaces in an oxidizing liquid medium while being submitted to ultrasonication. Original
The method of claim 1 wherein said graphitic material is selected from the group consisting of natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite fluoride, oxidized graphite, chemically modified graphite, exfoliated graphite, recompressed exfoliated graphite, expanded graphite, mesocarbon microbead, and combinations thereof. Original
The method of claim 1, 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, ultrasonic homogenizer mill, or resonant acoustic mixer. Original
The method of claim 1, wherein said graphitic material contains a non- intercalated and nonoxidized graphitic material that has never been previously exposed to a chemical or oxidation treatment prior to said mixing step. Original
The method of claim 1 wherein said graphene oxide sheets contain single-layer graphene oxide sheets. Original
The method of claim 1 wherein said graphene oxide sheets contain at least 80% single-layer graphene oxide or at least 80% few-layer graphene oxide having no greater than 10 graphene planes. Original
The method of claim 1, further comprising a step of exposing said graphene oxide to a functionalizing agent to produce functionalized graphene oxide. Original
The method of claim 1, wherein said procedure of operating said ener g y impacting apparatus is conducted in a continuous manner using a continuous energy impacting device. Original
Canceled
Canceled
Canceled
Materials described outside the worked examples.
graphitic material
graphene oxide sheets
Additional fabrication and treatment steps described in the patent.
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 | 1–20 mm | — |
Temperature | 30–1000 °C |
solid carrier material
oxidizing liquid
functionalizing agent
sodium permanganate
NaMnO₄
natural graphite
synthetic graphite
highly oriented pyrolytic graphite
hydrogen peroxide
H₂O₂
potassium permanganate
KMnO₄
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer's route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 46–200 °C | — |
Duration | 900–7200 s | — |
Duration | 0.5–12 hours | — |
Duration | 1–4 hours | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | 0.5–2 hours | — |
Temperature | ≥ 600 °C | — |
solid carrier material
oxidizing liquid
functionalizing agent
sodium permanganate
NaMnO₄
natural graphite
synthetic graphite
highly oriented pyrolytic graphite
hydrogen peroxide
H₂O₂
potassium permanganate
KMnO₄
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer's route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 46–200 °C | — |
Duration | 900–7200 s | — |
Duration | 0.5–12 hours | — |
Duration | 1–4 hours | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | 0.5–2 hours | — |
Temperature | ≥ 600 °C | — |
solid carrier material
oxidizing liquid
functionalizing agent
sodium permanganate
NaMnO₄
natural graphite
synthetic graphite
highly oriented pyrolytic graphite
hydrogen peroxide
H₂O₂
potassium permanganate
KMnO₄
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer's route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 46–200 °C | — |
Duration | 900–7200 s | — |
Duration | 0.5–12 hours | — |
Duration | 1–4 hours | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | 0.5–2 hours | — |
Temperature | ≥ 600 °C | — |
solid carrier material
oxidizing liquid
functionalizing agent
sodium permanganate
NaMnO₄
natural graphite
synthetic graphite
highly oriented pyrolytic graphite
hydrogen peroxide
H₂O₂
potassium permanganate
KMnO₄
FIG. 4(A) Transmission electron micrograph of graphene sheets produced by conventional Hummer's route (much smaller graphene sheets, but comparable thickness).
| — |
Temperature | 46–200 °C | — |
Duration | 900–7200 s | — |
Duration | 0.5–12 hours | — |
Duration | 1–4 hours | — |
Duration | 5–120 hours | — |
Temperature | 800–1100 °C | — |
Temperature | 950–1050 °C | — |
Duration | 0.5–2 hours | — |
Temperature | ≥ 600 °C | — |