Patent
US 10,023,468HIGH QUALITY LARGE SCALE SINGLE AND MULTILAYER GRAPHENE PRODUCTION BY CHEMICAL VAPOR DEPOSITION
Ivan V. Vlassiouk
US
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Patent
Atlas literature
Patent
US 10,023,468Patent 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 of making a monolayer or multilayer of poly- crystalline and single crystalline graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a deposition region in fluid communication with each other at atmospheric pressure; providing a continuous copper substrate for movement through the chemical vapor deposition chamber; drawing the copper substrate through the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas to anneal the copper substrate; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region, the reaction gas mixture having a partial pressure of hydrogen gas at 10-20 Torr and a partial pressure of hydrocarbon gas at 0.00123-100 mTorr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400 to form a monolayer or multilayer of gra p hene including crystal hexagonal grains, wherein the hydrogen gas contributes to the Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:3 annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting the monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 1 wherein the hydrocarbon gas includes about 30 ppm methane gas at about 23 mTorr to about 100 mTorr.
The method according to claim 1 further including continuously extracting the copper substrate from the chemical vapor deposition chamber with a poly-crystalline or single-crystalline graphene.
The method according to claim 1 wherein the hexagonal grains have an average grain size of between about 3 p m and about 1000 pm.
The method according to claim 1 wherein the number of continuous multilayers of graphene is between 2 and 6.
The method according to claim 1 further including heating the copper substrate to approximately 1000 ° C using an infrared or plasma arc lamp.
The method according to claim 1 further including heating the copper substrate using inductive coils.
A method of synthesizing graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a dep osition region in fluid communication with each other at atmos p heric p ressure; Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:4 providing a continuous catalyst substrate for movement through the chemical vapor deposition chamber; annealing the catalyst substrate in hydrogen gas within the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas while passing the catalyst substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the catalyst substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the annealed catalyst substrate continuously reacts with the reaction gas mixture, the reaction gas mixture having a partial pressure of the hydrocarbon gas between about 4-9 23 mTorr and about 100 mTorr, and having a partial pressure of the hydrogen gas between about 10 Torr and about 20 Torr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the hydrogen gas contributes to the annealing of the catalyst substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the catalyst substrate from the chemical vapor deposition chamber, the extracted catalyst substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 8 wherein the hydrocarbon gas is selected from the group consisting of methane, ethane, propane, butane, pentane, hexane, heptane, octane, benzene, toluene and combinations thereof.
The method according to claim 8 wherein the catalyst substrate includes a copper foil.
The method according to claim 8 wherein annealing the catalyst substrate includes gradually heating the catalyst substrate to approximately 1000 °C.
The method according to claim 8 wherein the buffer gas includes helium to maintain atmospheric pressure within the chemical vapor deposition chamber.
The method according to claim 8 further including bonding the synthesized graphene to a polymeric or dielectric substrate.
canceled
(Current ly Amended) A method of synthesizing gra p hene: Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:6 providing a chemical vapor deposition chamber including a pre-deposition region and a laterally-extending deposition region in fluid communication with each other at atmospheric pressure; passing a continuous copper substrate through the predeposition region of the chemical vapor deposition chamber at atmospheric pressure; annealing the copper substrate within the pre-deposition region of the chemical vapor deposition chamber in H₂ gas while drawing the copper substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; passing the annealed copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region to form poly-crystalline or single-crystalline graphene on the annealed copper substrate, the hydrocarbon gas having a partial pressure between about 23 mTorr and about 100 mTorr, the H₂ gas having a partial pressure between about 10 Torr and about 20 Torr with a ratio of H₂ gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the H₂ gas contributes to the annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon s p ecies in the de p osition region; and Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:7 continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 17 further including continuously extracting the copper substrate with poly-crystalline or single-crystalline graphene from the chemical vapor deposition chamber.
The method according to claim 17 wherein annealing the copper substrate includes gradually heating the copper substrate to approximately 1000 °C.
The method according to claim 17 wherein the annealed copper substrate is exposed to hydrocarbon gas for at least 5 minutes before removal from the chemical vapor deposition chamber.
The method according to claim 17 wherein the hexagonal grains having an average grain size between about 3 p m and about 20 pm.
The method according to claim 17 wherein the hydrocarbon gas is selected from the grou p consisting of CH 4, C₂ H 6, C 3 H 8, and C 4 H 10.
canceled
Materials described outside the worked examples.
copper substrate
Cu
hydrocarbon gas (methane)
CH₄
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
hexagonal graphene grain size (claimed range, claim 4) | 3–1000 µm | C |
hexagonal graphene grain size (claimed range, claim 22) | 3–20 µm |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 10,023,468Patent 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 of making a monolayer or multilayer of poly- crystalline and single crystalline graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a deposition region in fluid communication with each other at atmospheric pressure; providing a continuous copper substrate for movement through the chemical vapor deposition chamber; drawing the copper substrate through the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas to anneal the copper substrate; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region, the reaction gas mixture having a partial pressure of hydrogen gas at 10-20 Torr and a partial pressure of hydrocarbon gas at 0.00123-100 mTorr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400 to form a monolayer or multilayer of gra p hene including crystal hexagonal grains, wherein the hydrogen gas contributes to the Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:3 annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting the monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 1 wherein the hydrocarbon gas includes about 30 ppm methane gas at about 23 mTorr to about 100 mTorr.
The method according to claim 1 further including continuously extracting the copper substrate from the chemical vapor deposition chamber with a poly-crystalline or single-crystalline graphene.
The method according to claim 1 wherein the hexagonal grains have an average grain size of between about 3 p m and about 1000 pm.
The method according to claim 1 wherein the number of continuous multilayers of graphene is between 2 and 6.
The method according to claim 1 further including heating the copper substrate to approximately 1000 ° C using an infrared or plasma arc lamp.
The method according to claim 1 further including heating the copper substrate using inductive coils.
A method of synthesizing graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a dep osition region in fluid communication with each other at atmos p heric p ressure; Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:4 providing a continuous catalyst substrate for movement through the chemical vapor deposition chamber; annealing the catalyst substrate in hydrogen gas within the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas while passing the catalyst substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the catalyst substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the annealed catalyst substrate continuously reacts with the reaction gas mixture, the reaction gas mixture having a partial pressure of the hydrocarbon gas between about 4-9 23 mTorr and about 100 mTorr, and having a partial pressure of the hydrogen gas between about 10 Torr and about 20 Torr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the hydrogen gas contributes to the annealing of the catalyst substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the catalyst substrate from the chemical vapor deposition chamber, the extracted catalyst substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 8 wherein the hydrocarbon gas is selected from the group consisting of methane, ethane, propane, butane, pentane, hexane, heptane, octane, benzene, toluene and combinations thereof.
The method according to claim 8 wherein the catalyst substrate includes a copper foil.
The method according to claim 8 wherein annealing the catalyst substrate includes gradually heating the catalyst substrate to approximately 1000 °C.
The method according to claim 8 wherein the buffer gas includes helium to maintain atmospheric pressure within the chemical vapor deposition chamber.
The method according to claim 8 further including bonding the synthesized graphene to a polymeric or dielectric substrate.
canceled
(Current ly Amended) A method of synthesizing gra p hene: Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:6 providing a chemical vapor deposition chamber including a pre-deposition region and a laterally-extending deposition region in fluid communication with each other at atmospheric pressure; passing a continuous copper substrate through the predeposition region of the chemical vapor deposition chamber at atmospheric pressure; annealing the copper substrate within the pre-deposition region of the chemical vapor deposition chamber in H₂ gas while drawing the copper substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; passing the annealed copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region to form poly-crystalline or single-crystalline graphene on the annealed copper substrate, the hydrocarbon gas having a partial pressure between about 23 mTorr and about 100 mTorr, the H₂ gas having a partial pressure between about 10 Torr and about 20 Torr with a ratio of H₂ gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the H₂ gas contributes to the annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon s p ecies in the de p osition region; and Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:7 continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 17 further including continuously extracting the copper substrate with poly-crystalline or single-crystalline graphene from the chemical vapor deposition chamber.
The method according to claim 17 wherein annealing the copper substrate includes gradually heating the copper substrate to approximately 1000 °C.
The method according to claim 17 wherein the annealed copper substrate is exposed to hydrocarbon gas for at least 5 minutes before removal from the chemical vapor deposition chamber.
The method according to claim 17 wherein the hexagonal grains having an average grain size between about 3 p m and about 20 pm.
The method according to claim 17 wherein the hydrocarbon gas is selected from the grou p consisting of CH 4, C₂ H 6, C 3 H 8, and C 4 H 10.
canceled
Materials described outside the worked examples.
copper substrate
Cu
hydrocarbon gas (methane)
CH₄
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
hexagonal graphene grain size (claimed range, claim 4) | 3–1000 µm | C |
hexagonal graphene grain size (claimed range, claim 22) | 3–20 µm |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 10,023,468Patent 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 of making a monolayer or multilayer of poly- crystalline and single crystalline graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a deposition region in fluid communication with each other at atmospheric pressure; providing a continuous copper substrate for movement through the chemical vapor deposition chamber; drawing the copper substrate through the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas to anneal the copper substrate; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region, the reaction gas mixture having a partial pressure of hydrogen gas at 10-20 Torr and a partial pressure of hydrocarbon gas at 0.00123-100 mTorr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400 to form a monolayer or multilayer of gra p hene including crystal hexagonal grains, wherein the hydrogen gas contributes to the Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:3 annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting the monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 1 wherein the hydrocarbon gas includes about 30 ppm methane gas at about 23 mTorr to about 100 mTorr.
The method according to claim 1 further including continuously extracting the copper substrate from the chemical vapor deposition chamber with a poly-crystalline or single-crystalline graphene.
The method according to claim 1 wherein the hexagonal grains have an average grain size of between about 3 p m and about 1000 pm.
The method according to claim 1 wherein the number of continuous multilayers of graphene is between 2 and 6.
The method according to claim 1 further including heating the copper substrate to approximately 1000 ° C using an infrared or plasma arc lamp.
The method according to claim 1 further including heating the copper substrate using inductive coils.
A method of synthesizing graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a dep osition region in fluid communication with each other at atmos p heric p ressure; Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:4 providing a continuous catalyst substrate for movement through the chemical vapor deposition chamber; annealing the catalyst substrate in hydrogen gas within the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas while passing the catalyst substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the catalyst substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the annealed catalyst substrate continuously reacts with the reaction gas mixture, the reaction gas mixture having a partial pressure of the hydrocarbon gas between about 4-9 23 mTorr and about 100 mTorr, and having a partial pressure of the hydrogen gas between about 10 Torr and about 20 Torr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the hydrogen gas contributes to the annealing of the catalyst substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the catalyst substrate from the chemical vapor deposition chamber, the extracted catalyst substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 8 wherein the hydrocarbon gas is selected from the group consisting of methane, ethane, propane, butane, pentane, hexane, heptane, octane, benzene, toluene and combinations thereof.
The method according to claim 8 wherein the catalyst substrate includes a copper foil.
The method according to claim 8 wherein annealing the catalyst substrate includes gradually heating the catalyst substrate to approximately 1000 °C.
The method according to claim 8 wherein the buffer gas includes helium to maintain atmospheric pressure within the chemical vapor deposition chamber.
The method according to claim 8 further including bonding the synthesized graphene to a polymeric or dielectric substrate.
canceled
(Current ly Amended) A method of synthesizing gra p hene: Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:6 providing a chemical vapor deposition chamber including a pre-deposition region and a laterally-extending deposition region in fluid communication with each other at atmospheric pressure; passing a continuous copper substrate through the predeposition region of the chemical vapor deposition chamber at atmospheric pressure; annealing the copper substrate within the pre-deposition region of the chemical vapor deposition chamber in H₂ gas while drawing the copper substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; passing the annealed copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region to form poly-crystalline or single-crystalline graphene on the annealed copper substrate, the hydrocarbon gas having a partial pressure between about 23 mTorr and about 100 mTorr, the H₂ gas having a partial pressure between about 10 Torr and about 20 Torr with a ratio of H₂ gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the H₂ gas contributes to the annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon s p ecies in the de p osition region; and Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:7 continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 17 further including continuously extracting the copper substrate with poly-crystalline or single-crystalline graphene from the chemical vapor deposition chamber.
The method according to claim 17 wherein annealing the copper substrate includes gradually heating the copper substrate to approximately 1000 °C.
The method according to claim 17 wherein the annealed copper substrate is exposed to hydrocarbon gas for at least 5 minutes before removal from the chemical vapor deposition chamber.
The method according to claim 17 wherein the hexagonal grains having an average grain size between about 3 p m and about 20 pm.
The method according to claim 17 wherein the hydrocarbon gas is selected from the grou p consisting of CH 4, C₂ H 6, C 3 H 8, and C 4 H 10.
canceled
Materials described outside the worked examples.
copper substrate
Cu
hydrocarbon gas (methane)
CH₄
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
hexagonal graphene grain size (claimed range, claim 4) | 3–1000 µm | C |
hexagonal graphene grain size (claimed range, claim 22) | 3–20 µm |
Related documents with shared materials, methods, properties, or citations.
Patent
Atlas literature
Patent
US 10,023,468Patent 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 of making a monolayer or multilayer of poly- crystalline and single crystalline graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a deposition region in fluid communication with each other at atmospheric pressure; providing a continuous copper substrate for movement through the chemical vapor deposition chamber; drawing the copper substrate through the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas to anneal the copper substrate; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region, the reaction gas mixture having a partial pressure of hydrogen gas at 10-20 Torr and a partial pressure of hydrocarbon gas at 0.00123-100 mTorr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400 to form a monolayer or multilayer of gra p hene including crystal hexagonal grains, wherein the hydrogen gas contributes to the Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:3 annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting the monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 1 wherein the hydrocarbon gas includes about 30 ppm methane gas at about 23 mTorr to about 100 mTorr.
The method according to claim 1 further including continuously extracting the copper substrate from the chemical vapor deposition chamber with a poly-crystalline or single-crystalline graphene.
The method according to claim 1 wherein the hexagonal grains have an average grain size of between about 3 p m and about 1000 pm.
The method according to claim 1 wherein the number of continuous multilayers of graphene is between 2 and 6.
The method according to claim 1 further including heating the copper substrate to approximately 1000 ° C using an infrared or plasma arc lamp.
The method according to claim 1 further including heating the copper substrate using inductive coils.
A method of synthesizing graphene comprising: providing a chemical vapor deposition chamber including a pre-deposition region and a dep osition region in fluid communication with each other at atmos p heric p ressure; Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:4 providing a continuous catalyst substrate for movement through the chemical vapor deposition chamber; annealing the catalyst substrate in hydrogen gas within the pre-deposition region of the chemical vapor deposition chamber at atmospheric pressure and in the presence of hydrogen gas while passing the catalyst substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; drawing the catalyst substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the annealed catalyst substrate continuously reacts with the reaction gas mixture, the reaction gas mixture having a partial pressure of the hydrocarbon gas between about 4-9 23 mTorr and about 100 mTorr, and having a partial pressure of the hydrogen gas between about 10 Torr and about 20 Torr with a ratio of hydrogen gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the hydrogen gas contributes to the annealing of the catalyst substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon species in the deposition region; and continuously extracting the catalyst substrate from the chemical vapor deposition chamber, the extracted catalyst substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 8 wherein the hydrocarbon gas is selected from the group consisting of methane, ethane, propane, butane, pentane, hexane, heptane, octane, benzene, toluene and combinations thereof.
The method according to claim 8 wherein the catalyst substrate includes a copper foil.
The method according to claim 8 wherein annealing the catalyst substrate includes gradually heating the catalyst substrate to approximately 1000 °C.
The method according to claim 8 wherein the buffer gas includes helium to maintain atmospheric pressure within the chemical vapor deposition chamber.
The method according to claim 8 further including bonding the synthesized graphene to a polymeric or dielectric substrate.
canceled
(Current ly Amended) A method of synthesizing gra p hene: Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:6 providing a chemical vapor deposition chamber including a pre-deposition region and a laterally-extending deposition region in fluid communication with each other at atmospheric pressure; passing a continuous copper substrate through the predeposition region of the chemical vapor deposition chamber at atmospheric pressure; annealing the copper substrate within the pre-deposition region of the chemical vapor deposition chamber in H₂ gas while drawing the copper substrate therethrough; introducing a hydrocarbon gas and a buffer gas at a nozzle opening coextensive with the deposition region of the chemical vapor deposition chamber to mix with hydrogen gas escaping from the pre-deposition region at the nozzle opening, thereby forming a reaction gas mixture in the deposition region, the reaction gas mixture being at atmospheric pressure; passing the annealed copper substrate through the deposition region of the chemical vapor deposition chamber while introducing the hydrocarbon gas at the nozzle opening so that the copper substrate continuously reacts with the reaction gas mixture in the deposition region to form poly-crystalline or single-crystalline graphene on the annealed copper substrate, the hydrocarbon gas having a partial pressure between about 23 mTorr and about 100 mTorr, the H₂ gas having a partial pressure between about 10 Torr and about 20 Torr with a ratio of H₂ gas partial pressure to hydrocarbon gas partial pressure of greater than 400, wherein the H₂ gas contributes to the annealing of the copper substrate in the pre-deposition region and contributes to the formation of active surface-bound carbon s p ecies in the de p osition region; and Inventors: Ivan V. V l assiouk et al App l. No.: 13/734,823 Page:7 continuously extracting the copper substrate from the chemical vapor deposition chamber, the extracted copper substrate supporting a monolayer or multilayer of graphene including crystal hexagonal grains.
The method according to claim 17 further including continuously extracting the copper substrate with poly-crystalline or single-crystalline graphene from the chemical vapor deposition chamber.
The method according to claim 17 wherein annealing the copper substrate includes gradually heating the copper substrate to approximately 1000 °C.
The method according to claim 17 wherein the annealed copper substrate is exposed to hydrocarbon gas for at least 5 minutes before removal from the chemical vapor deposition chamber.
The method according to claim 17 wherein the hexagonal grains having an average grain size between about 3 p m and about 20 pm.
The method according to claim 17 wherein the hydrocarbon gas is selected from the grou p consisting of CH 4, C₂ H 6, C 3 H 8, and C 4 H 10.
canceled
Materials described outside the worked examples.
copper substrate
Cu
hydrocarbon gas (methane)
CH₄
Additional fabrication and treatment steps described in the patent.
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
hexagonal graphene grain size (claimed range, claim 4) | 3–1000 µm | C |
hexagonal graphene grain size (claimed range, claim 22) | 3–20 µm |
Related documents with shared materials, methods, properties, or citations.
graphene
C
hydrogen gas
H₂
catalyst substrate (generic)
helium buffer gas
He
argon buffer gas
Ar
number of multilayers of graphene (claimed range, claim 5) | 2–6 layers | C |
Temperature | 800–1080 °C | — |
Pressure | 10–25 Torr | — |
Pressure | 10–20 Torr | — |
Pressure | 2–11 Torr | — |
Pressure | ≤ 2 Torr | — |
Pressure | ≤ 500 mTorr | — |
Pressure | ≥ 10 Torr | — |
Pressure | 23–100 mTorr | — |
Pressure | 0.00123–100 mTorr | — |
Duration | ≥ 5 minutes | — |
Pressure | 0–50 Torr | — |
Temperature | 700–1080 °C | — |
graphene
C
hydrogen gas
H₂
catalyst substrate (generic)
helium buffer gas
He
argon buffer gas
Ar
number of multilayers of graphene (claimed range, claim 5) | 2–6 layers | C |
Temperature | 800–1080 °C | — |
Pressure | 10–25 Torr | — |
Pressure | 10–20 Torr | — |
Pressure | 2–11 Torr | — |
Pressure | ≤ 2 Torr | — |
Pressure | ≤ 500 mTorr | — |
Pressure | ≥ 10 Torr | — |
Pressure | 23–100 mTorr | — |
Pressure | 0.00123–100 mTorr | — |
Duration | ≥ 5 minutes | — |
Pressure | 0–50 Torr | — |
Temperature | 700–1080 °C | — |
graphene
C
hydrogen gas
H₂
catalyst substrate (generic)
helium buffer gas
He
argon buffer gas
Ar
number of multilayers of graphene (claimed range, claim 5) | 2–6 layers | C |
Temperature | 800–1080 °C | — |
Pressure | 10–25 Torr | — |
Pressure | 10–20 Torr | — |
Pressure | 2–11 Torr | — |
Pressure | ≤ 2 Torr | — |
Pressure | ≤ 500 mTorr | — |
Pressure | ≥ 10 Torr | — |
Pressure | 23–100 mTorr | — |
Pressure | 0.00123–100 mTorr | — |
Duration | ≥ 5 minutes | — |
Pressure | 0–50 Torr | — |
Temperature | 700–1080 °C | — |
graphene
C
hydrogen gas
H₂
catalyst substrate (generic)
helium buffer gas
He
argon buffer gas
Ar
number of multilayers of graphene (claimed range, claim 5) | 2–6 layers | C |
Temperature | 800–1080 °C | — |
Pressure | 10–25 Torr | — |
Pressure | 10–20 Torr | — |
Pressure | 2–11 Torr | — |
Pressure | ≤ 2 Torr | — |
Pressure | ≤ 500 mTorr | — |
Pressure | ≥ 10 Torr | — |
Pressure | 23–100 mTorr | — |
Pressure | 0.00123–100 mTorr | — |
Duration | ≥ 5 minutes | — |
Pressure | 0–50 Torr | — |
Temperature | 700–1080 °C | — |