Patent
US 9,452,934Synthesis of Ultra-large Graphene Oxide Sheets
Jang Kyo KIM
US
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Patent
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Patent
US 9,452,934Patent drawings and their descriptions. Click a drawing to enlarge it.
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 for forming graphene thin films, the method comprising: pre-intercalating of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expanding of graphite intercalation compound powders at a high temperature; further oxidizing using intercalating agents to exfoliate G expanded graphite into monolayer graphene oxide sheets; sequential centrifuging of graphene oxide and using the sequential centrifuging to collect graphene oxide as monolayer graphene oxide sheets with a mean lateral size in the range of 50-200 pm; preparing of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and reducing and chemical doping, with -Cl or -SO Cl 2 groups, to form doped Langmuir- Blodgett thin films.
The method of claim 1 further characterized by: subsequent to pre-intercalating the graphite flake, washing the graphite to form the graphite intercalation compound powders.
The method of claim 1, comprising applying a temperature of 800 ° C to 1200 ° C to effect the expansion of the graphite intercalation compound powders. 2
The method of claim 1, wherein said further oxidizing comprises adding a mixture of sulfuric acid, followed by adding potassium permanganate, followed by transferring the mixture to a chilled water bath, followed by washing with an acid solution, and then followed by washing with water, and rendering graphene oxide sheets.
The method of claim 1, wherein the sequential centrifugation of the graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 m comprises sorting the graphene oxide solution with polydispersity into plural groups of uniform sizes via said centrifugation in combination with dispersing the graphene oxide with water, and with said centrifugation performed at gradually reduced speeds to cause the graphene oxide to dividing into supernatant and precipitate.
The method of claim 1, further comprising the preparation of the Langmuir-Blodgett thin films comprising: applying the graphene oxide dispersion onto a water surface; compressing the graphene oxide monolayer to increase surface pressure; transferring the graphene oxide monolayer to a treated substrate selected from the group consisting of silicon, glass, quartz, mica or flexible polyethylene terephithalate (PET); and 3
The method of claim 1, wherein the reduction and chemical doping of graphene oxide thin films comprising heating the films on the substrate in a vacuum environment, followed by recovering the films to obtain reduced graphene oxide thin film.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films prior to preparing of Langmuir-Blodgett thin films.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films subsequent to preparing of Langmuir-Blodgett thin films.
An optoelectronic thin film, comprising: a plurality of monolayer graphene oxide sheets reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82 % and a DC to optical conductivity ratio of at least 7.29, and formed according to the method of claim 1. 4
An optoelectronic graphene thin film, comprising: a plurality of monolayer graphene oxide sheets with a mean lateral size in the range of 5 0-200 p m and reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82%, and formed by reducing and chemical doping of Langmuir-Blodgett thin films formed by: pre-intercalation of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expansion of graphite intercalation compound powders at a high temperature; further oxidation using intercalating agents to exfoliate expanded graphite into monolayer graphene oxide sheets; sequential centrifugation of graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 pm; preparation of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and thermal reduction and chemical doping of the graphene oxide thin films with -Cl or -SO Cl 2 groups, to form doped Langmuir-Blodgett thin films.
The optoelectronic graphene thin film of claim 14, further comprising: the a plurality of layers of graphene oxide film comprising said plural monolayer graphene oxide sheets obtained by the preparation, reduction and chemical doping of the graphene oxide sheets reduced to form graphene Langmuir-Blodgett thin films.
Layer stacks claimed or described, ordered top of device to substrate.
optoelectronic Langmuir-Blodgett graphene thin film
Materials described outside the worked examples.
natural graphite flake
graphite intercalation compound powders
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Lateral Size Range | 50–200 µm | ultra-large graphene oxide (UL-GO) sheets |
Patent
Atlas literature
Patent
US 9,452,934Patent drawings and their descriptions. Click a drawing to enlarge it.
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 for forming graphene thin films, the method comprising: pre-intercalating of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expanding of graphite intercalation compound powders at a high temperature; further oxidizing using intercalating agents to exfoliate G expanded graphite into monolayer graphene oxide sheets; sequential centrifuging of graphene oxide and using the sequential centrifuging to collect graphene oxide as monolayer graphene oxide sheets with a mean lateral size in the range of 50-200 pm; preparing of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and reducing and chemical doping, with -Cl or -SO Cl 2 groups, to form doped Langmuir- Blodgett thin films.
The method of claim 1 further characterized by: subsequent to pre-intercalating the graphite flake, washing the graphite to form the graphite intercalation compound powders.
The method of claim 1, comprising applying a temperature of 800 ° C to 1200 ° C to effect the expansion of the graphite intercalation compound powders. 2
The method of claim 1, wherein said further oxidizing comprises adding a mixture of sulfuric acid, followed by adding potassium permanganate, followed by transferring the mixture to a chilled water bath, followed by washing with an acid solution, and then followed by washing with water, and rendering graphene oxide sheets.
The method of claim 1, wherein the sequential centrifugation of the graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 m comprises sorting the graphene oxide solution with polydispersity into plural groups of uniform sizes via said centrifugation in combination with dispersing the graphene oxide with water, and with said centrifugation performed at gradually reduced speeds to cause the graphene oxide to dividing into supernatant and precipitate.
The method of claim 1, further comprising the preparation of the Langmuir-Blodgett thin films comprising: applying the graphene oxide dispersion onto a water surface; compressing the graphene oxide monolayer to increase surface pressure; transferring the graphene oxide monolayer to a treated substrate selected from the group consisting of silicon, glass, quartz, mica or flexible polyethylene terephithalate (PET); and 3
The method of claim 1, wherein the reduction and chemical doping of graphene oxide thin films comprising heating the films on the substrate in a vacuum environment, followed by recovering the films to obtain reduced graphene oxide thin film.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films prior to preparing of Langmuir-Blodgett thin films.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films subsequent to preparing of Langmuir-Blodgett thin films.
An optoelectronic thin film, comprising: a plurality of monolayer graphene oxide sheets reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82 % and a DC to optical conductivity ratio of at least 7.29, and formed according to the method of claim 1. 4
An optoelectronic graphene thin film, comprising: a plurality of monolayer graphene oxide sheets with a mean lateral size in the range of 5 0-200 p m and reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82%, and formed by reducing and chemical doping of Langmuir-Blodgett thin films formed by: pre-intercalation of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expansion of graphite intercalation compound powders at a high temperature; further oxidation using intercalating agents to exfoliate expanded graphite into monolayer graphene oxide sheets; sequential centrifugation of graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 pm; preparation of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and thermal reduction and chemical doping of the graphene oxide thin films with -Cl or -SO Cl 2 groups, to form doped Langmuir-Blodgett thin films.
The optoelectronic graphene thin film of claim 14, further comprising: the a plurality of layers of graphene oxide film comprising said plural monolayer graphene oxide sheets obtained by the preparation, reduction and chemical doping of the graphene oxide sheets reduced to form graphene Langmuir-Blodgett thin films.
Layer stacks claimed or described, ordered top of device to substrate.
optoelectronic Langmuir-Blodgett graphene thin film
Materials described outside the worked examples.
natural graphite flake
graphite intercalation compound powders
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Lateral Size Range | 50–200 µm | ultra-large graphene oxide (UL-GO) sheets |
Patent
Atlas literature
Patent
US 9,452,934Patent drawings and their descriptions. Click a drawing to enlarge it.
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 for forming graphene thin films, the method comprising: pre-intercalating of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expanding of graphite intercalation compound powders at a high temperature; further oxidizing using intercalating agents to exfoliate G expanded graphite into monolayer graphene oxide sheets; sequential centrifuging of graphene oxide and using the sequential centrifuging to collect graphene oxide as monolayer graphene oxide sheets with a mean lateral size in the range of 50-200 pm; preparing of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and reducing and chemical doping, with -Cl or -SO Cl 2 groups, to form doped Langmuir- Blodgett thin films.
The method of claim 1 further characterized by: subsequent to pre-intercalating the graphite flake, washing the graphite to form the graphite intercalation compound powders.
The method of claim 1, comprising applying a temperature of 800 ° C to 1200 ° C to effect the expansion of the graphite intercalation compound powders. 2
The method of claim 1, wherein said further oxidizing comprises adding a mixture of sulfuric acid, followed by adding potassium permanganate, followed by transferring the mixture to a chilled water bath, followed by washing with an acid solution, and then followed by washing with water, and rendering graphene oxide sheets.
The method of claim 1, wherein the sequential centrifugation of the graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 m comprises sorting the graphene oxide solution with polydispersity into plural groups of uniform sizes via said centrifugation in combination with dispersing the graphene oxide with water, and with said centrifugation performed at gradually reduced speeds to cause the graphene oxide to dividing into supernatant and precipitate.
The method of claim 1, further comprising the preparation of the Langmuir-Blodgett thin films comprising: applying the graphene oxide dispersion onto a water surface; compressing the graphene oxide monolayer to increase surface pressure; transferring the graphene oxide monolayer to a treated substrate selected from the group consisting of silicon, glass, quartz, mica or flexible polyethylene terephithalate (PET); and 3
The method of claim 1, wherein the reduction and chemical doping of graphene oxide thin films comprising heating the films on the substrate in a vacuum environment, followed by recovering the films to obtain reduced graphene oxide thin film.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films prior to preparing of Langmuir-Blodgett thin films.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films subsequent to preparing of Langmuir-Blodgett thin films.
An optoelectronic thin film, comprising: a plurality of monolayer graphene oxide sheets reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82 % and a DC to optical conductivity ratio of at least 7.29, and formed according to the method of claim 1. 4
An optoelectronic graphene thin film, comprising: a plurality of monolayer graphene oxide sheets with a mean lateral size in the range of 5 0-200 p m and reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82%, and formed by reducing and chemical doping of Langmuir-Blodgett thin films formed by: pre-intercalation of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expansion of graphite intercalation compound powders at a high temperature; further oxidation using intercalating agents to exfoliate expanded graphite into monolayer graphene oxide sheets; sequential centrifugation of graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 pm; preparation of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and thermal reduction and chemical doping of the graphene oxide thin films with -Cl or -SO Cl 2 groups, to form doped Langmuir-Blodgett thin films.
The optoelectronic graphene thin film of claim 14, further comprising: the a plurality of layers of graphene oxide film comprising said plural monolayer graphene oxide sheets obtained by the preparation, reduction and chemical doping of the graphene oxide sheets reduced to form graphene Langmuir-Blodgett thin films.
Layer stacks claimed or described, ordered top of device to substrate.
optoelectronic Langmuir-Blodgett graphene thin film
Materials described outside the worked examples.
natural graphite flake
graphite intercalation compound powders
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Lateral Size Range | 50–200 µm | ultra-large graphene oxide (UL-GO) sheets |
Patent
Atlas literature
Patent
US 9,452,934Patent drawings and their descriptions. Click a drawing to enlarge it.
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 for forming graphene thin films, the method comprising: pre-intercalating of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expanding of graphite intercalation compound powders at a high temperature; further oxidizing using intercalating agents to exfoliate G expanded graphite into monolayer graphene oxide sheets; sequential centrifuging of graphene oxide and using the sequential centrifuging to collect graphene oxide as monolayer graphene oxide sheets with a mean lateral size in the range of 50-200 pm; preparing of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and reducing and chemical doping, with -Cl or -SO Cl 2 groups, to form doped Langmuir- Blodgett thin films.
The method of claim 1 further characterized by: subsequent to pre-intercalating the graphite flake, washing the graphite to form the graphite intercalation compound powders.
The method of claim 1, comprising applying a temperature of 800 ° C to 1200 ° C to effect the expansion of the graphite intercalation compound powders. 2
The method of claim 1, wherein said further oxidizing comprises adding a mixture of sulfuric acid, followed by adding potassium permanganate, followed by transferring the mixture to a chilled water bath, followed by washing with an acid solution, and then followed by washing with water, and rendering graphene oxide sheets.
The method of claim 1, wherein the sequential centrifugation of the graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 m comprises sorting the graphene oxide solution with polydispersity into plural groups of uniform sizes via said centrifugation in combination with dispersing the graphene oxide with water, and with said centrifugation performed at gradually reduced speeds to cause the graphene oxide to dividing into supernatant and precipitate.
The method of claim 1, further comprising the preparation of the Langmuir-Blodgett thin films comprising: applying the graphene oxide dispersion onto a water surface; compressing the graphene oxide monolayer to increase surface pressure; transferring the graphene oxide monolayer to a treated substrate selected from the group consisting of silicon, glass, quartz, mica or flexible polyethylene terephithalate (PET); and 3
The method of claim 1, wherein the reduction and chemical doping of graphene oxide thin films comprising heating the films on the substrate in a vacuum environment, followed by recovering the films to obtain reduced graphene oxide thin film.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films prior to preparing of Langmuir-Blodgett thin films.
The method of claim 1 further characterized by: reducing and chemical doping of the graphene oxide thin films subsequent to preparing of Langmuir-Blodgett thin films.
An optoelectronic thin film, comprising: a plurality of monolayer graphene oxide sheets reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82 % and a DC to optical conductivity ratio of at least 7.29, and formed according to the method of claim 1. 4
An optoelectronic graphene thin film, comprising: a plurality of monolayer graphene oxide sheets with a mean lateral size in the range of 5 0-200 p m and reduced to form a Langmuir-Blodgett thin film having a transmittance of at least 82%, and formed by reducing and chemical doping of Langmuir-Blodgett thin films formed by: pre-intercalation of sulfuric acid and nitric acid to interlayers of natural graphite flake to form graphite intercalation compound powders; expansion of graphite intercalation compound powders at a high temperature; further oxidation using intercalating agents to exfoliate expanded graphite into monolayer graphene oxide sheets; sequential centrifugation of graphene oxide and collection of graphene oxide sheets with lateral size in the range of 50-200 pm; preparation of Langmuir-Blodgett thin films comprised of plural monolayer graphene oxide sheets; and thermal reduction and chemical doping of the graphene oxide thin films with -Cl or -SO Cl 2 groups, to form doped Langmuir-Blodgett thin films.
The optoelectronic graphene thin film of claim 14, further comprising: the a plurality of layers of graphene oxide film comprising said plural monolayer graphene oxide sheets obtained by the preparation, reduction and chemical doping of the graphene oxide sheets reduced to form graphene Langmuir-Blodgett thin films.
Layer stacks claimed or described, ordered top of device to substrate.
optoelectronic Langmuir-Blodgett graphene thin film
Materials described outside the worked examples.
natural graphite flake
graphite intercalation compound powders
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Lateral Size Range | 50–200 µm | ultra-large graphene oxide (UL-GO) sheets |
monolayer graphene oxide sheets
reduced graphene oxide thin film
doped Langmuir-Blodgett thin film
sulfuric acid
H₂SO₄
potassium permanganate
KMnO₄
hydrogen peroxide
H₂O₂
hydrochloric acid solution
HCl
substrate
nitric acid
HNO₃
thionyl chloride
SOCl₂
ultra-large graphene oxide (UL-GO) sheets
Monolayer Thickness |
| 0.738 nm |
ultra-large graphene oxide (UL-GO) sheets |
Uv Vis Transmittance At Wavelength | 90 % | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 459 Ω/sq | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 1100 Ω/sq | doped Langmuir-Blodgett thin film |
Uv Vis Transmittance At Wavelength | 82 % | doped Langmuir-Blodgett thin film |
Dc To Optical Conductivity Ratio | 7.29 | doped Langmuir-Blodgett thin film |
Temperature | 800–1200 °C | — |
Duration | 10–20 seconds | — |
Temperature | 1050–1550 °C | — |
Temperature | 35–60 °C | — |
Thickness | 5–15 mm | — |
Thickness | 0.1–0.5 mm | — |
Pressure | 0.00001 Torr | — |
monolayer graphene oxide sheets
reduced graphene oxide thin film
doped Langmuir-Blodgett thin film
sulfuric acid
H₂SO₄
potassium permanganate
KMnO₄
hydrogen peroxide
H₂O₂
hydrochloric acid solution
HCl
substrate
nitric acid
HNO₃
thionyl chloride
SOCl₂
ultra-large graphene oxide (UL-GO) sheets
Monolayer Thickness |
| 0.738 nm |
ultra-large graphene oxide (UL-GO) sheets |
Uv Vis Transmittance At Wavelength | 90 % | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 459 Ω/sq | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 1100 Ω/sq | doped Langmuir-Blodgett thin film |
Uv Vis Transmittance At Wavelength | 82 % | doped Langmuir-Blodgett thin film |
Dc To Optical Conductivity Ratio | 7.29 | doped Langmuir-Blodgett thin film |
Temperature | 800–1200 °C | — |
Duration | 10–20 seconds | — |
Temperature | 1050–1550 °C | — |
Temperature | 35–60 °C | — |
Thickness | 5–15 mm | — |
Thickness | 0.1–0.5 mm | — |
Pressure | 0.00001 Torr | — |
monolayer graphene oxide sheets
reduced graphene oxide thin film
doped Langmuir-Blodgett thin film
sulfuric acid
H₂SO₄
potassium permanganate
KMnO₄
hydrogen peroxide
H₂O₂
hydrochloric acid solution
HCl
substrate
nitric acid
HNO₃
thionyl chloride
SOCl₂
ultra-large graphene oxide (UL-GO) sheets
Monolayer Thickness |
| 0.738 nm |
ultra-large graphene oxide (UL-GO) sheets |
Uv Vis Transmittance At Wavelength | 90 % | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 459 Ω/sq | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 1100 Ω/sq | doped Langmuir-Blodgett thin film |
Uv Vis Transmittance At Wavelength | 82 % | doped Langmuir-Blodgett thin film |
Dc To Optical Conductivity Ratio | 7.29 | doped Langmuir-Blodgett thin film |
Temperature | 800–1200 °C | — |
Duration | 10–20 seconds | — |
Temperature | 1050–1550 °C | — |
Temperature | 35–60 °C | — |
Thickness | 5–15 mm | — |
Thickness | 0.1–0.5 mm | — |
Pressure | 0.00001 Torr | — |
monolayer graphene oxide sheets
reduced graphene oxide thin film
doped Langmuir-Blodgett thin film
sulfuric acid
H₂SO₄
potassium permanganate
KMnO₄
hydrogen peroxide
H₂O₂
hydrochloric acid solution
HCl
substrate
nitric acid
HNO₃
thionyl chloride
SOCl₂
ultra-large graphene oxide (UL-GO) sheets
Monolayer Thickness |
| 0.738 nm |
ultra-large graphene oxide (UL-GO) sheets |
Uv Vis Transmittance At Wavelength | 90 % | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 459 Ω/sq | doped Langmuir-Blodgett thin film |
Fet Sheet Resistance | 1100 Ω/sq | doped Langmuir-Blodgett thin film |
Uv Vis Transmittance At Wavelength | 82 % | doped Langmuir-Blodgett thin film |
Dc To Optical Conductivity Ratio | 7.29 | doped Langmuir-Blodgett thin film |
Temperature | 800–1200 °C | — |
Duration | 10–20 seconds | — |
Temperature | 1050–1550 °C | — |
Temperature | 35–60 °C | — |
Thickness | 5–15 mm | — |
Thickness | 0.1–0.5 mm | — |
Pressure | 0.00001 Torr | — |