Patent
US 8,524,067ELECTROCHEMICAL METHOD OF PRODUCING NANO-SCALED GRAPHENE PLATELETS
Aruna Zhamu, Joan Jang, Bor Z. Jang
US
Copyright © 2026 Matter42. All rights reserved.
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US 8,524,067Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
FIG.2 Schematic of an apparatus for electrochemical intercalation of graphite.
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
FIG.5 of Ref. 10). Re-intercalation by liquid eutectic of sodium and potassium (NaK₂) and subsequent exfoliation yielded platelets with thicknesses of 2-150 nm …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116 Amendments to the Claims: This listing of claims will replace all prior versions, and listings, of claims in the application: (In the amended claims, the words with strik ettgh are to be deleted and the words underlined are to be inserted.) Listing of Claims: 1-12
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The method of claim 21 wherein said layered graphite material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite oxide, graphite fluoride, chemically modified graphite, or a combination thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from the group consisting of aromatic carboxylic acid, aliphatic or cycloaliphatic carboxylic acid, straight chain or branched chain carboxylic acid, saturated and unsaturated monocarboxylic acids, dicarboxylic acids, and polycarboxylic acids that have 1-10 carbon atoms, alkyl esters thereof, and combinations thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from saturated aliphatic carboxylic acids of the formula H(CH₂) nCOO H, wherein n is a number of from 0 to 5, anhydrides thereof, reactive carboxylic acid derivatives thereof, and a combination thereof.
The method of claim 21 wherein said mechanical shearing treatment comprises using air milling, air jet milling, ball milling, rotating-blade mechanical shearing, ultrasonication, or a combination thereof.
The method of claim 21 wherein the imposing current provides a current density in the range of 50 to 600 A/m2. 2 Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116
The method of claim 21 wherein the imposing current provides a current density in the range of 100 to 400 A/m2.
The method of claim 21 wherein said step (b) or (d) comprises heating said carboxylic acid-intercalated graphite compound or said further carboxylic acid- intercalated graphite compound to a temperature in the range of 300-800 ° C for a duration of 15 seconds to 2 minutes.
The method of claim 21 wherein said ultra-thin, nano-scaled graphene platelets comprise single graphene-sheet and/or double graphene-sheet platelets.
A method of producing ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets from a layered graphite material, said method comprising: a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction which uses a carboxylic acid or derivative as both an electrolyte and an intercalate source, said layered graphite material as an anode material, and a metal or graphite as a cathode material, and wherein a current is imposed upon said cathode and said anode at a current density for a duration of time sufficient for effecting said electrochemical reaction; b) rapidly heating said carboxylic acid-intercalated graphite compound to a desired temperature to produce exfoliated graphite; c) re-intercalating said exfoliated graphite by repeating step (a) using said exfoliated graphite as an anode material to form a further carboxylic acid-intercalated graphite compound; d) rapidly heating said further carboxylic-intercalated graphite compound; e) subjecting a graphite compound obtained in step (d) to a mechanical shearing treatment to produce said ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets; and f) recovering said graphene platelets with an average thickness smaller than 2 nm or graphene sheets. 3
Materials described outside the worked examples.
layered graphite material
carboxylic acid-intercalated graphite compound
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 30–60 seconds | — |
Duration |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 8,524,067Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
FIG.2 Schematic of an apparatus for electrochemical intercalation of graphite.
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
FIG.5 of Ref. 10). Re-intercalation by liquid eutectic of sodium and potassium (NaK₂) and subsequent exfoliation yielded platelets with thicknesses of 2-150 nm …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116 Amendments to the Claims: This listing of claims will replace all prior versions, and listings, of claims in the application: (In the amended claims, the words with strik ettgh are to be deleted and the words underlined are to be inserted.) Listing of Claims: 1-12
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
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The method of claim 21 wherein said layered graphite material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite oxide, graphite fluoride, chemically modified graphite, or a combination thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from the group consisting of aromatic carboxylic acid, aliphatic or cycloaliphatic carboxylic acid, straight chain or branched chain carboxylic acid, saturated and unsaturated monocarboxylic acids, dicarboxylic acids, and polycarboxylic acids that have 1-10 carbon atoms, alkyl esters thereof, and combinations thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from saturated aliphatic carboxylic acids of the formula H(CH₂) nCOO H, wherein n is a number of from 0 to 5, anhydrides thereof, reactive carboxylic acid derivatives thereof, and a combination thereof.
The method of claim 21 wherein said mechanical shearing treatment comprises using air milling, air jet milling, ball milling, rotating-blade mechanical shearing, ultrasonication, or a combination thereof.
The method of claim 21 wherein the imposing current provides a current density in the range of 50 to 600 A/m2. 2 Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116
The method of claim 21 wherein the imposing current provides a current density in the range of 100 to 400 A/m2.
The method of claim 21 wherein said step (b) or (d) comprises heating said carboxylic acid-intercalated graphite compound or said further carboxylic acid- intercalated graphite compound to a temperature in the range of 300-800 ° C for a duration of 15 seconds to 2 minutes.
The method of claim 21 wherein said ultra-thin, nano-scaled graphene platelets comprise single graphene-sheet and/or double graphene-sheet platelets.
A method of producing ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets from a layered graphite material, said method comprising: a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction which uses a carboxylic acid or derivative as both an electrolyte and an intercalate source, said layered graphite material as an anode material, and a metal or graphite as a cathode material, and wherein a current is imposed upon said cathode and said anode at a current density for a duration of time sufficient for effecting said electrochemical reaction; b) rapidly heating said carboxylic acid-intercalated graphite compound to a desired temperature to produce exfoliated graphite; c) re-intercalating said exfoliated graphite by repeating step (a) using said exfoliated graphite as an anode material to form a further carboxylic acid-intercalated graphite compound; d) rapidly heating said further carboxylic-intercalated graphite compound; e) subjecting a graphite compound obtained in step (d) to a mechanical shearing treatment to produce said ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets; and f) recovering said graphene platelets with an average thickness smaller than 2 nm or graphene sheets. 3
Materials described outside the worked examples.
layered graphite material
carboxylic acid-intercalated graphite compound
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 30–60 seconds | — |
Duration |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 8,524,067Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
FIG.2 Schematic of an apparatus for electrochemical intercalation of graphite.
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
FIG.5 of Ref. 10). Re-intercalation by liquid eutectic of sodium and potassium (NaK₂) and subsequent exfoliation yielded platelets with thicknesses of 2-150 nm …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116 Amendments to the Claims: This listing of claims will replace all prior versions, and listings, of claims in the application: (In the amended claims, the words with strik ettgh are to be deleted and the words underlined are to be inserted.) Listing of Claims: 1-12
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
The method of claim 21 wherein said layered graphite material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite oxide, graphite fluoride, chemically modified graphite, or a combination thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from the group consisting of aromatic carboxylic acid, aliphatic or cycloaliphatic carboxylic acid, straight chain or branched chain carboxylic acid, saturated and unsaturated monocarboxylic acids, dicarboxylic acids, and polycarboxylic acids that have 1-10 carbon atoms, alkyl esters thereof, and combinations thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from saturated aliphatic carboxylic acids of the formula H(CH₂) nCOO H, wherein n is a number of from 0 to 5, anhydrides thereof, reactive carboxylic acid derivatives thereof, and a combination thereof.
The method of claim 21 wherein said mechanical shearing treatment comprises using air milling, air jet milling, ball milling, rotating-blade mechanical shearing, ultrasonication, or a combination thereof.
The method of claim 21 wherein the imposing current provides a current density in the range of 50 to 600 A/m2. 2 Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116
The method of claim 21 wherein the imposing current provides a current density in the range of 100 to 400 A/m2.
The method of claim 21 wherein said step (b) or (d) comprises heating said carboxylic acid-intercalated graphite compound or said further carboxylic acid- intercalated graphite compound to a temperature in the range of 300-800 ° C for a duration of 15 seconds to 2 minutes.
The method of claim 21 wherein said ultra-thin, nano-scaled graphene platelets comprise single graphene-sheet and/or double graphene-sheet platelets.
A method of producing ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets from a layered graphite material, said method comprising: a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction which uses a carboxylic acid or derivative as both an electrolyte and an intercalate source, said layered graphite material as an anode material, and a metal or graphite as a cathode material, and wherein a current is imposed upon said cathode and said anode at a current density for a duration of time sufficient for effecting said electrochemical reaction; b) rapidly heating said carboxylic acid-intercalated graphite compound to a desired temperature to produce exfoliated graphite; c) re-intercalating said exfoliated graphite by repeating step (a) using said exfoliated graphite as an anode material to form a further carboxylic acid-intercalated graphite compound; d) rapidly heating said further carboxylic-intercalated graphite compound; e) subjecting a graphite compound obtained in step (d) to a mechanical shearing treatment to produce said ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets; and f) recovering said graphene platelets with an average thickness smaller than 2 nm or graphene sheets. 3
Materials described outside the worked examples.
layered graphite material
carboxylic acid-intercalated graphite compound
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 30–60 seconds | — |
Duration |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 8,524,067Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
FIG.2 Schematic of an apparatus for electrochemical intercalation of graphite.
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
FIG.5 of Ref. 10). Re-intercalation by liquid eutectic of sodium and potassium (NaK₂) and subsequent exfoliation yielded platelets with thicknesses of 2-150 nm …
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116 Amendments to the Claims: This listing of claims will replace all prior versions, and listings, of claims in the application: (In the amended claims, the words with strik ettgh are to be deleted and the words underlined are to be inserted.) Listing of Claims: 1-12
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
canceled
The method of claim 21 wherein said layered graphite material is selected from natural graphite, synthetic graphite, highly oriented pyrolytic graphite, graphite fiber, graphitic nanofiber, graphite oxide, graphite fluoride, chemically modified graphite, or a combination thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from the group consisting of aromatic carboxylic acid, aliphatic or cycloaliphatic carboxylic acid, straight chain or branched chain carboxylic acid, saturated and unsaturated monocarboxylic acids, dicarboxylic acids, and polycarboxylic acids that have 1-10 carbon atoms, alkyl esters thereof, and combinations thereof.
The method of claim 21 wherein said carboxylic acid or derivative is selected from saturated aliphatic carboxylic acids of the formula H(CH₂) nCOO H, wherein n is a number of from 0 to 5, anhydrides thereof, reactive carboxylic acid derivatives thereof, and a combination thereof.
The method of claim 21 wherein said mechanical shearing treatment comprises using air milling, air jet milling, ball milling, rotating-blade mechanical shearing, ultrasonication, or a combination thereof.
The method of claim 21 wherein the imposing current provides a current density in the range of 50 to 600 A/m2. 2 Serial No.: 11/881,388 Attorney Docket No. 075213-00049US SECOND AMENDMENT UNDER 37 C.F.R § 1.116
The method of claim 21 wherein the imposing current provides a current density in the range of 100 to 400 A/m2.
The method of claim 21 wherein said step (b) or (d) comprises heating said carboxylic acid-intercalated graphite compound or said further carboxylic acid- intercalated graphite compound to a temperature in the range of 300-800 ° C for a duration of 15 seconds to 2 minutes.
The method of claim 21 wherein said ultra-thin, nano-scaled graphene platelets comprise single graphene-sheet and/or double graphene-sheet platelets.
A method of producing ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets from a layered graphite material, said method comprising: a) forming a carboxylic acid-intercalated graphite compound by an electrochemical reaction which uses a carboxylic acid or derivative as both an electrolyte and an intercalate source, said layered graphite material as an anode material, and a metal or graphite as a cathode material, and wherein a current is imposed upon said cathode and said anode at a current density for a duration of time sufficient for effecting said electrochemical reaction; b) rapidly heating said carboxylic acid-intercalated graphite compound to a desired temperature to produce exfoliated graphite; c) re-intercalating said exfoliated graphite by repeating step (a) using said exfoliated graphite as an anode material to form a further carboxylic acid-intercalated graphite compound; d) rapidly heating said further carboxylic-intercalated graphite compound; e) subjecting a graphite compound obtained in step (d) to a mechanical shearing treatment to produce said ultra-thin, nano-scaled graphene platelets with an average thickness smaller than 2 nm or 5 graphene sheets; and f) recovering said graphene platelets with an average thickness smaller than 2 nm or graphene sheets. 3
Materials described outside the worked examples.
layered graphite material
carboxylic acid-intercalated graphite compound
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.1 A flow chart showing a two-stage process of producing ultra-thin graphite platelets (NGPs with an average thickness thinner than 2 nm or 5 layers). Both …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 30–60 seconds | — |
Duration |
Related documents with shared materials, methods, properties, or citations.
carboxylic acid or derivative
ultra-thin nano-scaled graphene platelets
formic acid
HCOOH
acetic acid
CH₃COOH
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
| 2–5 hours |
| — |
Thickness | ≤ 2 nm | — |
Thickness | ≤ 1 nm | — |
Thickness | ≥ 10 nm | — |
Duration | 15–120 s | — |
Temperature | 300–800 °C | — |
Duration | 10–120 s | — |
Thickness | 10–30 nm | — |
Thickness | 2–10 nm | — |
Thickness | 10–15 nm | — |
Thickness | 2–150 nm | — |
Thickness | ≥ 2 nm | — |
carboxylic acid or derivative
ultra-thin nano-scaled graphene platelets
formic acid
HCOOH
acetic acid
CH₃COOH
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
| 2–5 hours |
| — |
Thickness | ≤ 2 nm | — |
Thickness | ≤ 1 nm | — |
Thickness | ≥ 10 nm | — |
Duration | 15–120 s | — |
Temperature | 300–800 °C | — |
Duration | 10–120 s | — |
Thickness | 10–30 nm | — |
Thickness | 2–10 nm | — |
Thickness | 10–15 nm | — |
Thickness | 2–150 nm | — |
Thickness | ≥ 2 nm | — |
carboxylic acid or derivative
ultra-thin nano-scaled graphene platelets
formic acid
HCOOH
acetic acid
CH₃COOH
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
| 2–5 hours |
| — |
Thickness | ≤ 2 nm | — |
Thickness | ≤ 1 nm | — |
Thickness | ≥ 10 nm | — |
Duration | 15–120 s | — |
Temperature | 300–800 °C | — |
Duration | 10–120 s | — |
Thickness | 10–30 nm | — |
Thickness | 2–10 nm | — |
Thickness | 10–15 nm | — |
Thickness | 2–150 nm | — |
Thickness | ≥ 2 nm | — |
carboxylic acid or derivative
ultra-thin nano-scaled graphene platelets
formic acid
HCOOH
acetic acid
CH₃COOH
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.3 Transmission electron micrographs of NGPs: (A) NGP with an average thickness < 30 nm (at the end of Phase I); (B) ultra-thin NGPs (Phase II).
FIG.4 Platelet thickness distributions for NGPs prepared from prior art sulfuric-nitric acid- 5 intercalated graphite and formic-acid intercalated graphite.
| 2–5 hours |
| — |
Thickness | ≤ 2 nm | — |
Thickness | ≤ 1 nm | — |
Thickness | ≥ 10 nm | — |
Duration | 15–120 s | — |
Temperature | 300–800 °C | — |
Duration | 10–120 s | — |
Thickness | 10–30 nm | — |
Thickness | 2–10 nm | — |
Thickness | 10–15 nm | — |
Thickness | 2–150 nm | — |
Thickness | ≥ 2 nm | — |