Patent
US 9,630,852GRAPHENE MATERIAL AND METHOD OF PREPARING THE SAME
Jianhong LIU
US
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Patent
Atlas literature
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US 9,630,852Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 is a flow diagram of a method of preparing a graphene material in accordance to one embodiment of the invention; [0024]
FIG. 2A is a Raman pattern of a graphene material prepared in Example 1; [0025]
FIG. 3A is a Raman pattern of a graphene material prepared in Example 2; [0027]
FIG. 4A is a Raman pattern of a graphene material prepared in Example 3; and [0029]
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1, wherein in (1), a dopant is added to and uniformly mixed with the cyclized LPAN solution.
The method of claim 2, wherein the dopant is a metallic dopant or a non-metallic dopant; the metallic dopant is a pure metal comprising tin, copper, silver, aluminum, chromium, iron, manganese, titanium, nickel, and cobalt, or a metal oxide, metal nitride, metal boride, metal fluoride, metal bromide, metal sulfide, or a mixture thereof; and the non-metallic dopant is silicon, phosphorus, boron, nitrogen, carbon, sulfur, or a compound thereof, or a mixture thereof. 2/6 Application Serial No. [4/848,274 Reply to Office Action of September 23, 20 [6 Atty Docket No. SZDX-00501-UUS
The method of claim 2, wherein a mixing m o de of the dopant comprises stirring, ultrasound, and b all milling.
The method of claim 1, wherein a solute of the LPAN s olu tion is a liquid acryl o nitrile oligo m er with a relative molecular weight of between 1 06 and 100000, a solvent of the LPAN is water, methanol, alcohol, or a m ixt u re thereof, and a mass concentration of the LPAN is between 0.0 1: 1 and 0.8: 1.
6. The method of claim 5, wherein the liquid acryl o nitrile oligo m er is a homopolym er of acryl o nitrile.
The method of claim 5, wherein the liquid acryl o nitrile o lig om er is a copolymer of acryl o nitrile and a vinyl monomer, and the vinyl monomer is selected from the group of s tyrene, methyl methacrylate, hydr o xyethyl methylacrylate, acrylic acid, and itac o nic acid.
The method of claim 1, wherein the inert gas in (4) and (5) is nitrogen or argon.
9. 3/6 canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 240°C for 60 hrs to yield cyclized PAN. Cyclized solution heated at 240°C for 3 hrs to yield OPAN. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined in ceramic boat under inert gas flow 100 mL/min for 8 hrs at 900°C, cooled, ground and sieved to yield low-temperature carbonized product. Carbonized product calcined again at 2500°C for 1 hr under inert gas flow 100 mL/min to yield multilayer graphene material. Raman and TEM characterization confirmed multilayer graphene structure.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 150°C for 70 hrs to yield cyclized PAN. Cyclized solution heated at 220°C for 5 hrs to yield OPAN with ladder structure. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined at 900°C for 8 hrs under inert gas flow 100 mL/min, cooled, ground, and sieved to yield low-temperature carbonized product. Carbonized product calcined at 2500°C for 2 hrs under inert gas flow 100 mL/min to yield graphene material with higher graphitization degree and fewer layers (approaching monolayer) compared to Example 1. Raman and TEM characterization confirmed results.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 120°C for 50 hrs to yield cyclized PAN. Cyclized solution heated at 260°C for 8 hrs to yield OPAN. Further processing (as per the general method) to yield graphene material.
Materials described outside the worked examples.
liquid polyacrylonitrile (LPAN)
dopant (generic)
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 |
|---|---|---|
Temperature | 80–300 °C | — |
Temperature |
Patent
Atlas literature
Patent
US 9,630,852Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 is a flow diagram of a method of preparing a graphene material in accordance to one embodiment of the invention; [0024]
FIG. 2A is a Raman pattern of a graphene material prepared in Example 1; [0025]
FIG. 3A is a Raman pattern of a graphene material prepared in Example 2; [0027]
FIG. 4A is a Raman pattern of a graphene material prepared in Example 3; and [0029]
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1, wherein in (1), a dopant is added to and uniformly mixed with the cyclized LPAN solution.
The method of claim 2, wherein the dopant is a metallic dopant or a non-metallic dopant; the metallic dopant is a pure metal comprising tin, copper, silver, aluminum, chromium, iron, manganese, titanium, nickel, and cobalt, or a metal oxide, metal nitride, metal boride, metal fluoride, metal bromide, metal sulfide, or a mixture thereof; and the non-metallic dopant is silicon, phosphorus, boron, nitrogen, carbon, sulfur, or a compound thereof, or a mixture thereof. 2/6 Application Serial No. [4/848,274 Reply to Office Action of September 23, 20 [6 Atty Docket No. SZDX-00501-UUS
The method of claim 2, wherein a mixing m o de of the dopant comprises stirring, ultrasound, and b all milling.
The method of claim 1, wherein a solute of the LPAN s olu tion is a liquid acryl o nitrile oligo m er with a relative molecular weight of between 1 06 and 100000, a solvent of the LPAN is water, methanol, alcohol, or a m ixt u re thereof, and a mass concentration of the LPAN is between 0.0 1: 1 and 0.8: 1.
6. The method of claim 5, wherein the liquid acryl o nitrile oligo m er is a homopolym er of acryl o nitrile.
The method of claim 5, wherein the liquid acryl o nitrile o lig om er is a copolymer of acryl o nitrile and a vinyl monomer, and the vinyl monomer is selected from the group of s tyrene, methyl methacrylate, hydr o xyethyl methylacrylate, acrylic acid, and itac o nic acid.
The method of claim 1, wherein the inert gas in (4) and (5) is nitrogen or argon.
9. 3/6 canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 240°C for 60 hrs to yield cyclized PAN. Cyclized solution heated at 240°C for 3 hrs to yield OPAN. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined in ceramic boat under inert gas flow 100 mL/min for 8 hrs at 900°C, cooled, ground and sieved to yield low-temperature carbonized product. Carbonized product calcined again at 2500°C for 1 hr under inert gas flow 100 mL/min to yield multilayer graphene material. Raman and TEM characterization confirmed multilayer graphene structure.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 150°C for 70 hrs to yield cyclized PAN. Cyclized solution heated at 220°C for 5 hrs to yield OPAN with ladder structure. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined at 900°C for 8 hrs under inert gas flow 100 mL/min, cooled, ground, and sieved to yield low-temperature carbonized product. Carbonized product calcined at 2500°C for 2 hrs under inert gas flow 100 mL/min to yield graphene material with higher graphitization degree and fewer layers (approaching monolayer) compared to Example 1. Raman and TEM characterization confirmed results.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 120°C for 50 hrs to yield cyclized PAN. Cyclized solution heated at 260°C for 8 hrs to yield OPAN. Further processing (as per the general method) to yield graphene material.
Materials described outside the worked examples.
liquid polyacrylonitrile (LPAN)
dopant (generic)
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 |
|---|---|---|
Temperature | 80–300 °C | — |
Temperature |
Patent
Atlas literature
Patent
US 9,630,852Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 is a flow diagram of a method of preparing a graphene material in accordance to one embodiment of the invention; [0024]
FIG. 2A is a Raman pattern of a graphene material prepared in Example 1; [0025]
FIG. 3A is a Raman pattern of a graphene material prepared in Example 2; [0027]
FIG. 4A is a Raman pattern of a graphene material prepared in Example 3; and [0029]
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1, wherein in (1), a dopant is added to and uniformly mixed with the cyclized LPAN solution.
The method of claim 2, wherein the dopant is a metallic dopant or a non-metallic dopant; the metallic dopant is a pure metal comprising tin, copper, silver, aluminum, chromium, iron, manganese, titanium, nickel, and cobalt, or a metal oxide, metal nitride, metal boride, metal fluoride, metal bromide, metal sulfide, or a mixture thereof; and the non-metallic dopant is silicon, phosphorus, boron, nitrogen, carbon, sulfur, or a compound thereof, or a mixture thereof. 2/6 Application Serial No. [4/848,274 Reply to Office Action of September 23, 20 [6 Atty Docket No. SZDX-00501-UUS
The method of claim 2, wherein a mixing m o de of the dopant comprises stirring, ultrasound, and b all milling.
The method of claim 1, wherein a solute of the LPAN s olu tion is a liquid acryl o nitrile oligo m er with a relative molecular weight of between 1 06 and 100000, a solvent of the LPAN is water, methanol, alcohol, or a m ixt u re thereof, and a mass concentration of the LPAN is between 0.0 1: 1 and 0.8: 1.
6. The method of claim 5, wherein the liquid acryl o nitrile oligo m er is a homopolym er of acryl o nitrile.
The method of claim 5, wherein the liquid acryl o nitrile o lig om er is a copolymer of acryl o nitrile and a vinyl monomer, and the vinyl monomer is selected from the group of s tyrene, methyl methacrylate, hydr o xyethyl methylacrylate, acrylic acid, and itac o nic acid.
The method of claim 1, wherein the inert gas in (4) and (5) is nitrogen or argon.
9. 3/6 canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 240°C for 60 hrs to yield cyclized PAN. Cyclized solution heated at 240°C for 3 hrs to yield OPAN. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined in ceramic boat under inert gas flow 100 mL/min for 8 hrs at 900°C, cooled, ground and sieved to yield low-temperature carbonized product. Carbonized product calcined again at 2500°C for 1 hr under inert gas flow 100 mL/min to yield multilayer graphene material. Raman and TEM characterization confirmed multilayer graphene structure.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 150°C for 70 hrs to yield cyclized PAN. Cyclized solution heated at 220°C for 5 hrs to yield OPAN with ladder structure. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined at 900°C for 8 hrs under inert gas flow 100 mL/min, cooled, ground, and sieved to yield low-temperature carbonized product. Carbonized product calcined at 2500°C for 2 hrs under inert gas flow 100 mL/min to yield graphene material with higher graphitization degree and fewer layers (approaching monolayer) compared to Example 1. Raman and TEM characterization confirmed results.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 120°C for 50 hrs to yield cyclized PAN. Cyclized solution heated at 260°C for 8 hrs to yield OPAN. Further processing (as per the general method) to yield graphene material.
Materials described outside the worked examples.
liquid polyacrylonitrile (LPAN)
dopant (generic)
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 |
|---|---|---|
Temperature | 80–300 °C | — |
Temperature |
Patent
Atlas literature
Patent
US 9,630,852Patent drawings and their descriptions. Click a drawing to enlarge it.
FIG. 1 is a flow diagram of a method of preparing a graphene material in accordance to one embodiment of the invention; [0024]
FIG. 2A is a Raman pattern of a graphene material prepared in Example 1; [0025]
FIG. 3A is a Raman pattern of a graphene material prepared in Example 2; [0027]
FIG. 4A is a Raman pattern of a graphene material prepared in Example 3; and [0029]
Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
The method of claim 1, wherein in (1), a dopant is added to and uniformly mixed with the cyclized LPAN solution.
The method of claim 2, wherein the dopant is a metallic dopant or a non-metallic dopant; the metallic dopant is a pure metal comprising tin, copper, silver, aluminum, chromium, iron, manganese, titanium, nickel, and cobalt, or a metal oxide, metal nitride, metal boride, metal fluoride, metal bromide, metal sulfide, or a mixture thereof; and the non-metallic dopant is silicon, phosphorus, boron, nitrogen, carbon, sulfur, or a compound thereof, or a mixture thereof. 2/6 Application Serial No. [4/848,274 Reply to Office Action of September 23, 20 [6 Atty Docket No. SZDX-00501-UUS
The method of claim 2, wherein a mixing m o de of the dopant comprises stirring, ultrasound, and b all milling.
The method of claim 1, wherein a solute of the LPAN s olu tion is a liquid acryl o nitrile oligo m er with a relative molecular weight of between 1 06 and 100000, a solvent of the LPAN is water, methanol, alcohol, or a m ixt u re thereof, and a mass concentration of the LPAN is between 0.0 1: 1 and 0.8: 1.
6. The method of claim 5, wherein the liquid acryl o nitrile oligo m er is a homopolym er of acryl o nitrile.
The method of claim 5, wherein the liquid acryl o nitrile o lig om er is a copolymer of acryl o nitrile and a vinyl monomer, and the vinyl monomer is selected from the group of s tyrene, methyl methacrylate, hydr o xyethyl methylacrylate, acrylic acid, and itac o nic acid.
The method of claim 1, wherein the inert gas in (4) and (5) is nitrogen or argon.
9. 3/6 canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 240°C for 60 hrs to yield cyclized PAN. Cyclized solution heated at 240°C for 3 hrs to yield OPAN. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined in ceramic boat under inert gas flow 100 mL/min for 8 hrs at 900°C, cooled, ground and sieved to yield low-temperature carbonized product. Carbonized product calcined again at 2500°C for 1 hr under inert gas flow 100 mL/min to yield multilayer graphene material. Raman and TEM characterization confirmed multilayer graphene structure.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 150°C for 70 hrs to yield cyclized PAN. Cyclized solution heated at 220°C for 5 hrs to yield OPAN with ladder structure. OPAN ball milled (planetary, 8 hrs, 400 rad/min, grinding media:material 15:1), sieved and dried to yield thermally-oxidized precursor. Precursor calcined at 900°C for 8 hrs under inert gas flow 100 mL/min, cooled, ground, and sieved to yield low-temperature carbonized product. Carbonized product calcined at 2500°C for 2 hrs under inert gas flow 100 mL/min to yield graphene material with higher graphitization degree and fewer layers (approaching monolayer) compared to Example 1. Raman and TEM characterization confirmed results.
3 materials1 process step
20 g of LPAN solution (MW 4000) stirred at 120°C for 50 hrs to yield cyclized PAN. Cyclized solution heated at 260°C for 8 hrs to yield OPAN. Further processing (as per the general method) to yield graphene material.
Materials described outside the worked examples.
liquid polyacrylonitrile (LPAN)
dopant (generic)
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 |
|---|---|---|
Temperature | 80–300 °C | — |
Temperature |
metallic dopant
non-metallic dopant
homopolymer of acrylonitrile
copolymer of acrylonitrile and vinyl monomer
graphene material
| — |
Temperature | 1000–3000 °C | — |
Temperature | 400–1000 °C | — |
metallic dopant
non-metallic dopant
homopolymer of acrylonitrile
copolymer of acrylonitrile and vinyl monomer
graphene material
| — |
Temperature | 1000–3000 °C | — |
Temperature | 400–1000 °C | — |
metallic dopant
non-metallic dopant
homopolymer of acrylonitrile
copolymer of acrylonitrile and vinyl monomer
graphene material
| — |
Temperature | 1000–3000 °C | — |
Temperature | 400–1000 °C | — |
metallic dopant
non-metallic dopant
homopolymer of acrylonitrile
copolymer of acrylonitrile and vinyl monomer
graphene material
| — |
Temperature | 1000–3000 °C | — |
Temperature | 400–1000 °C | — |