Patent
US 11,247,906Electrochemical Production of Graphene Sheets Directly from Graphite Mineral
Aruna Zhamu, Bor Z. Jang
US
Copyright © 2026 Matter42. All rights reserved.
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing an embodiment of the presently invented method of producing isolated graphene sheets. 25
FIG.2 Schematic drawing of an apparatus for electrochemical intercalation of graphite.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
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 supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein, wherein the intercalating agents comprise lithium perchlorate and at least one of sodium perchlorate and potassium perchlorate; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, sodium (ethylenediamine), hexamethylenetetramine, 1- pyrenamine, or a combination thereof; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
The method of claim 1, wherein multiple particles of said graphite mineral powder are dispersed in said liquid solution electrolyte, disposed in a working electrode compartment, and supported or confined by a current collector in electronic contact therewith, and wherein said working electrode compartment and said multiple particles supported thereon or confined therein are not in electronic contact with said counter electrode. Original
The method of claim 1, wherein said method is conducted intermittently or continuously and said supply of graphite mineral powder and said liquid solution electrolyte are provided into said reactor intermittently or continuously. Original
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 20% to 97% by weight. Previously presented
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 30% to 90% by weight. Previously presented
The method of claim 1, wherein said working electrode comprises no other graphite material than said graphite mineral powder as an electrode active material to be intercalated. Previously presented
The method of claim 1, wherein said mechanical shearing treatment comprises operating air milling, air jet milling, ball milling, rotating-blade mechanical shearing, or a combination thereof. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 0. 1 to 600 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 1 to 500 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 10 to 300 A/m 2. Original
The method of claim 1, wherein said thermal shock exposure comprises heating said intercalated graphite to a temperature in the range of 300-1,200 ° C for a period of 15 seconds to 2 minutes. Original
The method of claim 1, wherein said isolated graphene sheets comprise single-layer graphene. Previously presented
The method of claim 1, wherein said isolated graphene sheets comprise few-layer graphene having 2-10 graphene planes. Previously presented
The method of claim 1, wherein said electrochemical intercalation comprises intercalation of both said intercalating agents and said wetting agent into the interlayer spacing. Currently amended
The method of claim 1, wherein said intercalated graphite compound comprises Stage- 1, Stage-2, or a combination of Stage- 1 and Stage-2 graphite intercalation compounds. Previously presented
The method of claim 1, further comprising a step of re-intercalating said isolated graphene sheets using an electrochemical or chemical intercalation method to obtain intercalated graphene sheets followed by a step of further exfoliating and separating said intercalated graphene sheets to produce single-layer graphene sheets using ultrasonication, thermal shock exposure, exposure to water solution, mechanical shearing treatment, or a combination thereof. Previously presented
The method of claim 1, wherein said intercalating agents comprises a dichloroacetic acid (Cl 2 CH COO H); or an alkylsulfonic acid selected from the group consisting of methanesulfonic (MeS O 3 H), ethanesulfonic (EtS O 3 H), or 1-propanesulfonic (n-PrS O 3 H); and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises a metal halide. Currently amended
The method of claim 1, wherein said intercalating agents further comprises an alkali metal salt selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFS I), bis- trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, 4 -)- lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiBF 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), an ionic liquid lithium salt, and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises an organic solvent which is tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol) dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), or a combination thereof. Currently amended
Canceled
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising an intercalating agents dissolved therein, wherein said intercalating agents comprises mixed metal ions; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents into said interlayer spacing; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets Wherein during sub process a) said liquid solution consists essentially of 1,3-dioxolane (DOL), 1,2-dimethoxyethane (DME), tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol), dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), sulfone, sulfolane, ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), methylethyl carbonate (MEC), diethyl carbonate (DEC), ethyl propionate, methyl propionate, gamma-butyrolactone (y-BL), acetonitrile (AN), ethyl acetate (E A), propyl formate (PF), methyl formate (MF), toluene, xylene, methyl acetate (MA), fluoroethylene carbonate (FEC), vinylene carbonate (VC), allyl ethyl carbonate (AEC), hydrofloroether, or a combination thereof, wherein said intercalating agents comprise two or more alkali metal salts selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6 1 sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO ? 1 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO ? 1 2), a sodium ionic liquid salt, lithium perchlorate (LiC 10 4), lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiB F 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis- trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C₀ 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3 j 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt. Currently amended
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder without purification comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agent and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, ammonium sulfate, sodium (ethylenediamine), carbamide, hexamethylenetetramine, organic amine, 1-pyrenamine, or a combination thereof; and wherein said intercalating agents comprise two or more salts -i§ selected from the group consisting of potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, lithium hexafluoroarsenide (LiAsF 6), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt; (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
Materials described outside the worked examples.
graphite mineral powder
lithium perchlorate
LiClO₄
sodium perchlorate
NaClO₄
potassium perchlorate
KClO₄
graphene plane-wetting agent (melamine, sodium ethylenediamine, hexamethylenetetramine, or 1-pyrenamine)
intercalated graphite compound
single-layer graphene
few-layer graphene (2-10 graphene planes)
dichloroacetic acid or alkylsulfonic acid (methanesulfonic, ethanesulfonic, or 1-propanesulfonic acid)
metal halide
alkali metal salt intercalating agents (NaClO4, KClO4, NaPF6, KPF6, NaBF4, KBF4, NaCF₃SO3, KCF₃SO3, NaN(CF₃SO₂)2, NaTFSI, KN(CF₃SO₂)2, sodium ionic liquid salt, LiClO4, LiPF6, LiBF4, LiAsF6, LiCF₃SO3, LiN(CF₃SO₂)2, LiBOB, LiBF₂C₂O4, LiNO3, LiPF₃(CF₂CF₃)3, LiBETI, lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, LiTFSI, ionic liquid lithium salt)
organic solvent intercalating agent (TEGDME, PEGDME, DEGDBE, 2-ethoxyethyl ether)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 10–120 s | — |
Duration | 30–60 seconds | — |
Duration | 2–5 hours | — |
Thickness | 200–300 nm | — |
Thickness | 2.1–7.7 nm | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 3.4 nm | — |
Thickness | ≤ 2 nm | — |
Duration | 15–120 s | — |
Temperature | 300–1200 °C | — |
Related documents with shared materials, methods, properties, or citations.
GRAPHENE SHELL AND PROCESS OF PREPARING THE SAME
METHOD FOR PREPARING GRAPHENE BY USING HIGH SPEED HOMOGENIZATION PRETREATMENT AND HIGH PRESSURE HOMOGENATION
GRAPHENE BASE AND METHOD OF PREPARING THE SAME
METHOD OF MANUFACTURING GRAPHENE-COATED COMPOSITE POWDER
GRAPHENE COMPOSITE NANOFIBER AND PREPARATION METHOD THEREOF
Lithium super-battery with a functionalized nano graphene cathode
SPACER-MODIFIED NANO GRAPHENE ELECTRODES FOR SUPERCAPACITORS
MOLYBDENUM DISULFIDE/GRAPHENE/CARBON COMPOSITE MATERIAL AND USE THEREOF
HEAT DISSIPATION SHEET MANUFACTURED USING GRAPHENE/GRAPHITE NANOPLATE/CARBON NANOTUBE/NANO-METAL COMPLEX AND METHOD OF MANUFACTURING THE SAME
Spacer-modified graphene electrode for supercapacitor
Aluminum Secondary Battery Cathode Having Oriented Graphene
Continuous process for producing spacer-modified nano Graphene electrodes for supercapacitors
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing an embodiment of the presently invented method of producing isolated graphene sheets. 25
FIG.2 Schematic drawing of an apparatus for electrochemical intercalation of graphite.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
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 supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein, wherein the intercalating agents comprise lithium perchlorate and at least one of sodium perchlorate and potassium perchlorate; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, sodium (ethylenediamine), hexamethylenetetramine, 1- pyrenamine, or a combination thereof; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
The method of claim 1, wherein multiple particles of said graphite mineral powder are dispersed in said liquid solution electrolyte, disposed in a working electrode compartment, and supported or confined by a current collector in electronic contact therewith, and wherein said working electrode compartment and said multiple particles supported thereon or confined therein are not in electronic contact with said counter electrode. Original
The method of claim 1, wherein said method is conducted intermittently or continuously and said supply of graphite mineral powder and said liquid solution electrolyte are provided into said reactor intermittently or continuously. Original
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 20% to 97% by weight. Previously presented
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 30% to 90% by weight. Previously presented
The method of claim 1, wherein said working electrode comprises no other graphite material than said graphite mineral powder as an electrode active material to be intercalated. Previously presented
The method of claim 1, wherein said mechanical shearing treatment comprises operating air milling, air jet milling, ball milling, rotating-blade mechanical shearing, or a combination thereof. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 0. 1 to 600 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 1 to 500 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 10 to 300 A/m 2. Original
The method of claim 1, wherein said thermal shock exposure comprises heating said intercalated graphite to a temperature in the range of 300-1,200 ° C for a period of 15 seconds to 2 minutes. Original
The method of claim 1, wherein said isolated graphene sheets comprise single-layer graphene. Previously presented
The method of claim 1, wherein said isolated graphene sheets comprise few-layer graphene having 2-10 graphene planes. Previously presented
The method of claim 1, wherein said electrochemical intercalation comprises intercalation of both said intercalating agents and said wetting agent into the interlayer spacing. Currently amended
The method of claim 1, wherein said intercalated graphite compound comprises Stage- 1, Stage-2, or a combination of Stage- 1 and Stage-2 graphite intercalation compounds. Previously presented
The method of claim 1, further comprising a step of re-intercalating said isolated graphene sheets using an electrochemical or chemical intercalation method to obtain intercalated graphene sheets followed by a step of further exfoliating and separating said intercalated graphene sheets to produce single-layer graphene sheets using ultrasonication, thermal shock exposure, exposure to water solution, mechanical shearing treatment, or a combination thereof. Previously presented
The method of claim 1, wherein said intercalating agents comprises a dichloroacetic acid (Cl 2 CH COO H); or an alkylsulfonic acid selected from the group consisting of methanesulfonic (MeS O 3 H), ethanesulfonic (EtS O 3 H), or 1-propanesulfonic (n-PrS O 3 H); and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises a metal halide. Currently amended
The method of claim 1, wherein said intercalating agents further comprises an alkali metal salt selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFS I), bis- trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, 4 -)- lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiBF 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), an ionic liquid lithium salt, and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises an organic solvent which is tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol) dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), or a combination thereof. Currently amended
Canceled
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising an intercalating agents dissolved therein, wherein said intercalating agents comprises mixed metal ions; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents into said interlayer spacing; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets Wherein during sub process a) said liquid solution consists essentially of 1,3-dioxolane (DOL), 1,2-dimethoxyethane (DME), tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol), dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), sulfone, sulfolane, ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), methylethyl carbonate (MEC), diethyl carbonate (DEC), ethyl propionate, methyl propionate, gamma-butyrolactone (y-BL), acetonitrile (AN), ethyl acetate (E A), propyl formate (PF), methyl formate (MF), toluene, xylene, methyl acetate (MA), fluoroethylene carbonate (FEC), vinylene carbonate (VC), allyl ethyl carbonate (AEC), hydrofloroether, or a combination thereof, wherein said intercalating agents comprise two or more alkali metal salts selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6 1 sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO ? 1 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO ? 1 2), a sodium ionic liquid salt, lithium perchlorate (LiC 10 4), lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiB F 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis- trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C₀ 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3 j 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt. Currently amended
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder without purification comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agent and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, ammonium sulfate, sodium (ethylenediamine), carbamide, hexamethylenetetramine, organic amine, 1-pyrenamine, or a combination thereof; and wherein said intercalating agents comprise two or more salts -i§ selected from the group consisting of potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, lithium hexafluoroarsenide (LiAsF 6), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt; (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
Materials described outside the worked examples.
graphite mineral powder
lithium perchlorate
LiClO₄
sodium perchlorate
NaClO₄
potassium perchlorate
KClO₄
graphene plane-wetting agent (melamine, sodium ethylenediamine, hexamethylenetetramine, or 1-pyrenamine)
intercalated graphite compound
single-layer graphene
few-layer graphene (2-10 graphene planes)
dichloroacetic acid or alkylsulfonic acid (methanesulfonic, ethanesulfonic, or 1-propanesulfonic acid)
metal halide
alkali metal salt intercalating agents (NaClO4, KClO4, NaPF6, KPF6, NaBF4, KBF4, NaCF₃SO3, KCF₃SO3, NaN(CF₃SO₂)2, NaTFSI, KN(CF₃SO₂)2, sodium ionic liquid salt, LiClO4, LiPF6, LiBF4, LiAsF6, LiCF₃SO3, LiN(CF₃SO₂)2, LiBOB, LiBF₂C₂O4, LiNO3, LiPF₃(CF₂CF₃)3, LiBETI, lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, LiTFSI, ionic liquid lithium salt)
organic solvent intercalating agent (TEGDME, PEGDME, DEGDBE, 2-ethoxyethyl ether)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 10–120 s | — |
Duration | 30–60 seconds | — |
Duration | 2–5 hours | — |
Thickness | 200–300 nm | — |
Thickness | 2.1–7.7 nm | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 3.4 nm | — |
Thickness | ≤ 2 nm | — |
Duration | 15–120 s | — |
Temperature | 300–1200 °C | — |
Related documents with shared materials, methods, properties, or citations.
GRAPHENE SHELL AND PROCESS OF PREPARING THE SAME
METHOD FOR PREPARING GRAPHENE BY USING HIGH SPEED HOMOGENIZATION PRETREATMENT AND HIGH PRESSURE HOMOGENATION
GRAPHENE BASE AND METHOD OF PREPARING THE SAME
METHOD OF MANUFACTURING GRAPHENE-COATED COMPOSITE POWDER
GRAPHENE COMPOSITE NANOFIBER AND PREPARATION METHOD THEREOF
Lithium super-battery with a functionalized nano graphene cathode
SPACER-MODIFIED NANO GRAPHENE ELECTRODES FOR SUPERCAPACITORS
MOLYBDENUM DISULFIDE/GRAPHENE/CARBON COMPOSITE MATERIAL AND USE THEREOF
HEAT DISSIPATION SHEET MANUFACTURED USING GRAPHENE/GRAPHITE NANOPLATE/CARBON NANOTUBE/NANO-METAL COMPLEX AND METHOD OF MANUFACTURING THE SAME
Spacer-modified graphene electrode for supercapacitor
Aluminum Secondary Battery Cathode Having Oriented Graphene
Continuous process for producing spacer-modified nano Graphene electrodes for supercapacitors
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing an embodiment of the presently invented method of producing isolated graphene sheets. 25
FIG.2 Schematic drawing of an apparatus for electrochemical intercalation of graphite.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
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 supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein, wherein the intercalating agents comprise lithium perchlorate and at least one of sodium perchlorate and potassium perchlorate; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, sodium (ethylenediamine), hexamethylenetetramine, 1- pyrenamine, or a combination thereof; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
The method of claim 1, wherein multiple particles of said graphite mineral powder are dispersed in said liquid solution electrolyte, disposed in a working electrode compartment, and supported or confined by a current collector in electronic contact therewith, and wherein said working electrode compartment and said multiple particles supported thereon or confined therein are not in electronic contact with said counter electrode. Original
The method of claim 1, wherein said method is conducted intermittently or continuously and said supply of graphite mineral powder and said liquid solution electrolyte are provided into said reactor intermittently or continuously. Original
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 20% to 97% by weight. Previously presented
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 30% to 90% by weight. Previously presented
The method of claim 1, wherein said working electrode comprises no other graphite material than said graphite mineral powder as an electrode active material to be intercalated. Previously presented
The method of claim 1, wherein said mechanical shearing treatment comprises operating air milling, air jet milling, ball milling, rotating-blade mechanical shearing, or a combination thereof. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 0. 1 to 600 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 1 to 500 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 10 to 300 A/m 2. Original
The method of claim 1, wherein said thermal shock exposure comprises heating said intercalated graphite to a temperature in the range of 300-1,200 ° C for a period of 15 seconds to 2 minutes. Original
The method of claim 1, wherein said isolated graphene sheets comprise single-layer graphene. Previously presented
The method of claim 1, wherein said isolated graphene sheets comprise few-layer graphene having 2-10 graphene planes. Previously presented
The method of claim 1, wherein said electrochemical intercalation comprises intercalation of both said intercalating agents and said wetting agent into the interlayer spacing. Currently amended
The method of claim 1, wherein said intercalated graphite compound comprises Stage- 1, Stage-2, or a combination of Stage- 1 and Stage-2 graphite intercalation compounds. Previously presented
The method of claim 1, further comprising a step of re-intercalating said isolated graphene sheets using an electrochemical or chemical intercalation method to obtain intercalated graphene sheets followed by a step of further exfoliating and separating said intercalated graphene sheets to produce single-layer graphene sheets using ultrasonication, thermal shock exposure, exposure to water solution, mechanical shearing treatment, or a combination thereof. Previously presented
The method of claim 1, wherein said intercalating agents comprises a dichloroacetic acid (Cl 2 CH COO H); or an alkylsulfonic acid selected from the group consisting of methanesulfonic (MeS O 3 H), ethanesulfonic (EtS O 3 H), or 1-propanesulfonic (n-PrS O 3 H); and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises a metal halide. Currently amended
The method of claim 1, wherein said intercalating agents further comprises an alkali metal salt selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFS I), bis- trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, 4 -)- lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiBF 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), an ionic liquid lithium salt, and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises an organic solvent which is tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol) dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), or a combination thereof. Currently amended
Canceled
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising an intercalating agents dissolved therein, wherein said intercalating agents comprises mixed metal ions; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents into said interlayer spacing; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets Wherein during sub process a) said liquid solution consists essentially of 1,3-dioxolane (DOL), 1,2-dimethoxyethane (DME), tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol), dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), sulfone, sulfolane, ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), methylethyl carbonate (MEC), diethyl carbonate (DEC), ethyl propionate, methyl propionate, gamma-butyrolactone (y-BL), acetonitrile (AN), ethyl acetate (E A), propyl formate (PF), methyl formate (MF), toluene, xylene, methyl acetate (MA), fluoroethylene carbonate (FEC), vinylene carbonate (VC), allyl ethyl carbonate (AEC), hydrofloroether, or a combination thereof, wherein said intercalating agents comprise two or more alkali metal salts selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6 1 sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO ? 1 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO ? 1 2), a sodium ionic liquid salt, lithium perchlorate (LiC 10 4), lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiB F 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis- trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C₀ 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3 j 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt. Currently amended
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder without purification comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agent and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, ammonium sulfate, sodium (ethylenediamine), carbamide, hexamethylenetetramine, organic amine, 1-pyrenamine, or a combination thereof; and wherein said intercalating agents comprise two or more salts -i§ selected from the group consisting of potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, lithium hexafluoroarsenide (LiAsF 6), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt; (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
Materials described outside the worked examples.
graphite mineral powder
lithium perchlorate
LiClO₄
sodium perchlorate
NaClO₄
potassium perchlorate
KClO₄
graphene plane-wetting agent (melamine, sodium ethylenediamine, hexamethylenetetramine, or 1-pyrenamine)
intercalated graphite compound
single-layer graphene
few-layer graphene (2-10 graphene planes)
dichloroacetic acid or alkylsulfonic acid (methanesulfonic, ethanesulfonic, or 1-propanesulfonic acid)
metal halide
alkali metal salt intercalating agents (NaClO4, KClO4, NaPF6, KPF6, NaBF4, KBF4, NaCF₃SO3, KCF₃SO3, NaN(CF₃SO₂)2, NaTFSI, KN(CF₃SO₂)2, sodium ionic liquid salt, LiClO4, LiPF6, LiBF4, LiAsF6, LiCF₃SO3, LiN(CF₃SO₂)2, LiBOB, LiBF₂C₂O4, LiNO3, LiPF₃(CF₂CF₃)3, LiBETI, lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, LiTFSI, ionic liquid lithium salt)
organic solvent intercalating agent (TEGDME, PEGDME, DEGDBE, 2-ethoxyethyl ether)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 10–120 s | — |
Duration | 30–60 seconds | — |
Duration | 2–5 hours | — |
Thickness | 200–300 nm | — |
Thickness | 2.1–7.7 nm | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 3.4 nm | — |
Thickness | ≤ 2 nm | — |
Duration | 15–120 s | — |
Temperature | 300–1200 °C | — |
Related documents with shared materials, methods, properties, or citations.
GRAPHENE SHELL AND PROCESS OF PREPARING THE SAME
METHOD FOR PREPARING GRAPHENE BY USING HIGH SPEED HOMOGENIZATION PRETREATMENT AND HIGH PRESSURE HOMOGENATION
GRAPHENE BASE AND METHOD OF PREPARING THE SAME
METHOD OF MANUFACTURING GRAPHENE-COATED COMPOSITE POWDER
GRAPHENE COMPOSITE NANOFIBER AND PREPARATION METHOD THEREOF
Lithium super-battery with a functionalized nano graphene cathode
SPACER-MODIFIED NANO GRAPHENE ELECTRODES FOR SUPERCAPACITORS
MOLYBDENUM DISULFIDE/GRAPHENE/CARBON COMPOSITE MATERIAL AND USE THEREOF
HEAT DISSIPATION SHEET MANUFACTURED USING GRAPHENE/GRAPHITE NANOPLATE/CARBON NANOTUBE/NANO-METAL COMPLEX AND METHOD OF MANUFACTURING THE SAME
Spacer-modified graphene electrode for supercapacitor
Aluminum Secondary Battery Cathode Having Oriented Graphene
Continuous process for producing spacer-modified nano Graphene electrodes for supercapacitors
Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG.1 A flow chart showing an embodiment of the presently invented method of producing isolated graphene sheets. 25
FIG.2 Schematic drawing of an apparatus for electrochemical intercalation of graphite.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
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 supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein, wherein the intercalating agents comprise lithium perchlorate and at least one of sodium perchlorate and potassium perchlorate; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, sodium (ethylenediamine), hexamethylenetetramine, 1- pyrenamine, or a combination thereof; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
The method of claim 1, wherein multiple particles of said graphite mineral powder are dispersed in said liquid solution electrolyte, disposed in a working electrode compartment, and supported or confined by a current collector in electronic contact therewith, and wherein said working electrode compartment and said multiple particles supported thereon or confined therein are not in electronic contact with said counter electrode. Original
The method of claim 1, wherein said method is conducted intermittently or continuously and said supply of graphite mineral powder and said liquid solution electrolyte are provided into said reactor intermittently or continuously. Original
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 20% to 97% by weight. Previously presented
The method of claim 1, wherein said graphite mineral powder comprises a proportion of layered graphite material in the range from 30% to 90% by weight. Previously presented
The method of claim 1, wherein said working electrode comprises no other graphite material than said graphite mineral powder as an electrode active material to be intercalated. Previously presented
The method of claim 1, wherein said mechanical shearing treatment comprises operating air milling, air jet milling, ball milling, rotating-blade mechanical shearing, or a combination thereof. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 0. 1 to 600 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 1 to 500 A/m 2. Original
The method of claim 1, wherein the imposing current provides a current density in the range of 10 to 300 A/m 2. Original
The method of claim 1, wherein said thermal shock exposure comprises heating said intercalated graphite to a temperature in the range of 300-1,200 ° C for a period of 15 seconds to 2 minutes. Original
The method of claim 1, wherein said isolated graphene sheets comprise single-layer graphene. Previously presented
The method of claim 1, wherein said isolated graphene sheets comprise few-layer graphene having 2-10 graphene planes. Previously presented
The method of claim 1, wherein said electrochemical intercalation comprises intercalation of both said intercalating agents and said wetting agent into the interlayer spacing. Currently amended
The method of claim 1, wherein said intercalated graphite compound comprises Stage- 1, Stage-2, or a combination of Stage- 1 and Stage-2 graphite intercalation compounds. Previously presented
The method of claim 1, further comprising a step of re-intercalating said isolated graphene sheets using an electrochemical or chemical intercalation method to obtain intercalated graphene sheets followed by a step of further exfoliating and separating said intercalated graphene sheets to produce single-layer graphene sheets using ultrasonication, thermal shock exposure, exposure to water solution, mechanical shearing treatment, or a combination thereof. Previously presented
The method of claim 1, wherein said intercalating agents comprises a dichloroacetic acid (Cl 2 CH COO H); or an alkylsulfonic acid selected from the group consisting of methanesulfonic (MeS O 3 H), ethanesulfonic (EtS O 3 H), or 1-propanesulfonic (n-PrS O 3 H); and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises a metal halide. Currently amended
The method of claim 1, wherein said intercalating agents further comprises an alkali metal salt selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFS I), bis- trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, 4 -)- lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiBF 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), an ionic liquid lithium salt, and combinations thereof. Currently amended
The method of claim 1, wherein said intercalating agents comprises an organic solvent which is tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol) dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), or a combination thereof. Currently amended
Canceled
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising an intercalating agents dissolved therein, wherein said intercalating agents comprises mixed metal ions; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agents into said interlayer spacing; and (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets Wherein during sub process a) said liquid solution consists essentially of 1,3-dioxolane (DOL), 1,2-dimethoxyethane (DME), tetraethylene glycol dimethylether (TEGDME), poly(ethylene glycol), dimethyl ether (PEGDME), diethylene glycol dibutyl ether (DEGDBE), 2-ethoxyethyl ether (EE E), sulfone, sulfolane, ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), methylethyl carbonate (MEC), diethyl carbonate (DEC), ethyl propionate, methyl propionate, gamma-butyrolactone (y-BL), acetonitrile (AN), ethyl acetate (E A), propyl formate (PF), methyl formate (MF), toluene, xylene, methyl acetate (MA), fluoroethylene carbonate (FEC), vinylene carbonate (VC), allyl ethyl carbonate (AEC), hydrofloroether, or a combination thereof, wherein said intercalating agents comprise two or more alkali metal salts selected from the group consisting of sodium perchlorate (NaC lO 4), potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6 1 sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO ? 1 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO ? 1 2), a sodium ionic liquid salt, lithium perchlorate (LiC 10 4), lithium hexafluorophosphate (LiPF 6), lithium borofluoride (LiB F 4), lithium hexafluoroarsenide (LiAsF 6), lithium trifluoro-methanesulfonate (LiCF 3 SO 3), bis- trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO) 2), lithium bis(oxalato)borate (LiBOB), lithium oxalyldifluoroborate (LiBF 2 C₀ 4), lithium nitrate (LiNO 3), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3 j 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt. Currently amended
A method of producing isolated graphene sheets directly from a supply of graphite mineral powder without purification comprising therein graphene planes with an interlayer spacing, said method comprising: (a) forming an intercalated graphite compound by an electrochemical intercalation procedure which is conducted in an intercalation reactor, wherein said reactor comprises (i) a liquid solution electrolyte comprising intercalating agents and a graphene plane-wetting agent dissolved therein; (ii) a working electrode that comprises said graphite mineral powder as an active material in ionic contact with said liquid solution electrolyte; and (iii) a counter electrode in ionic contact with said liquid solution electrolyte, and wherein a current is imposed upon said working electrode and said counter electrode at a current density for a duration of time sufficient for effecting electrochemical intercalation of said intercalating agent and/or said wetting agent into said interlayer spacing, wherein said wetting agent is melamine, ammonium sulfate, sodium (ethylenediamine), carbamide, hexamethylenetetramine, organic amine, 1-pyrenamine, or a combination thereof; and wherein said intercalating agents comprise two or more salts -i§ selected from the group consisting of potassium perchlorate (KC 10 4), sodium hexafluorophosphate (NaPF 6), potassium hexafluorophosphate (KPF 6), sodium borofluoride (NaBF 4), potassium borofluoride (KBF 4), sodium hexafluoroarsenide, potassium hexafluoroarsenide, sodium trifluoro-methanesulfonate (NaCF 3 SO 3), potassium trifluoro-methanesulfonate (KCF 3 SO 3), bis-trifluoromethyl sulfonylimide sodium (NaN(CF 3 SO 2) 2), sodium trifluoromethanesulfonimide (NaTFSI), bis-trifluoromethyl sulfonylimide potassium (KN(CF 3 SO 2) 2), a sodium ionic liquid salt, lithium hexafluoroarsenide (LiAsF 6), bis-trifluoromethyl sulfonylimide lithium (LiN(CF 3 SO 2) 2), lithium oxalyldifluoroborate (LiBF 2 C 2 0 4), Li-fluoroalkyl-phosphates (LiPF 3 (CF 2 CF 3) 3), lithium bispe r fluoro-ethysulfonylimide (LiBETI), lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, lithium trifluoromethanesulfonimide (LiTFSI), and an ionic liquid lithium salt; (b) exfoliating and separating said graphene planes from said intercalated graphite compound using an ultrasonication, thermal shock exposure, mechanical shearing treatment, or a combination thereof to produce said isolated graphene sheets. Currently amended
Materials described outside the worked examples.
graphite mineral powder
lithium perchlorate
LiClO₄
sodium perchlorate
NaClO₄
potassium perchlorate
KClO₄
graphene plane-wetting agent (melamine, sodium ethylenediamine, hexamethylenetetramine, or 1-pyrenamine)
intercalated graphite compound
single-layer graphene
few-layer graphene (2-10 graphene planes)
dichloroacetic acid or alkylsulfonic acid (methanesulfonic, ethanesulfonic, or 1-propanesulfonic acid)
metal halide
alkali metal salt intercalating agents (NaClO4, KClO4, NaPF6, KPF6, NaBF4, KBF4, NaCF₃SO3, KCF₃SO3, NaN(CF₃SO₂)2, NaTFSI, KN(CF₃SO₂)2, sodium ionic liquid salt, LiClO4, LiPF6, LiBF4, LiAsF6, LiCF₃SO3, LiN(CF₃SO₂)2, LiBOB, LiBF₂C₂O4, LiNO3, LiPF₃(CF₂CF₃)3, LiBETI, lithium bis(trifluoromethanesulfonyl)imide, lithium bis(fluorosulfonyl)imide, LiTFSI, ionic liquid lithium salt)
organic solvent intercalating agent (TEGDME, PEGDME, DEGDBE, 2-ethoxyethyl ether)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
FIG.3(B) Transmission electron micrograph of graphene sheets produced by conventional chemical intercalation and oxidation of graphite using strong sulfuric …
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Duration | 10–120 s | — |
Duration | 30–60 seconds | — |
Duration | 2–5 hours | — |
Thickness | 200–300 nm | — |
Thickness | 2.1–7.7 nm | — |
Thickness | ≤ 10 nm | — |
Thickness | ≤ 3.4 nm | — |
Thickness | ≤ 2 nm | — |
Duration | 15–120 s | — |
Temperature | 300–1200 °C | — |
Related documents with shared materials, methods, properties, or citations.
GRAPHENE SHELL AND PROCESS OF PREPARING THE SAME
METHOD FOR PREPARING GRAPHENE BY USING HIGH SPEED HOMOGENIZATION PRETREATMENT AND HIGH PRESSURE HOMOGENATION
GRAPHENE BASE AND METHOD OF PREPARING THE SAME
METHOD OF MANUFACTURING GRAPHENE-COATED COMPOSITE POWDER
GRAPHENE COMPOSITE NANOFIBER AND PREPARATION METHOD THEREOF
Lithium super-battery with a functionalized nano graphene cathode
SPACER-MODIFIED NANO GRAPHENE ELECTRODES FOR SUPERCAPACITORS
MOLYBDENUM DISULFIDE/GRAPHENE/CARBON COMPOSITE MATERIAL AND USE THEREOF
HEAT DISSIPATION SHEET MANUFACTURED USING GRAPHENE/GRAPHITE NANOPLATE/CARBON NANOTUBE/NANO-METAL COMPLEX AND METHOD OF MANUFACTURING THE SAME
Spacer-modified graphene electrode for supercapacitor
Aluminum Secondary Battery Cathode Having Oriented Graphene
Continuous process for producing spacer-modified nano Graphene electrodes for supercapacitors