Patent
US 9,162,894METHOD FOR PREPARING GRAPHENE
Zhaoping Liu
US
Copyright © 2026 Matter42. All rights reserved.
Patent
Atlas literature
Patent
US 9,162,894Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
(Cu rr ently Amended) A method for preparing graphene, characterized in that the method consists consisting of the following steps: (i) reacting graphite in an acid solution in which an oxidant is present, (ii) washing the product obtained in step (i) with water to neutral, and (ii) (iii) subjecting the product obtained in step (i) step (ii) to a step of stripping selected from mechanical grinding and/or ultrasonic treatment, thereby resulting in formation of a graphene, wherein the graphene has a ratio of carbon to oxygen atoms of greater than 10, and the ratio of graphite: acid: oxidant: solvent is 1:0.1-50:0.1-50:0.1-100 by mass.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 14.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the acid in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, and oxalic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the oxidant in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, and peroxides.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein solvent in the acid solution comprises one or more selected from the group consisting of ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, and acetic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out at a temperature of 0-90 0C.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out for 1 minute to 10 hours.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 16.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 20. UNT 0050 US 3 Serial No. 13/577,027
UNT 0050 US 2 Serial No. 13/577,027 canceled
9-11. canceled
canceled
canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
2 materials1 process step
Graphene prepared by reacting graphite in an acid solution with an oxidant present, followed by washing to neutral and stripping (mechanical grinding and/or ultrasonic treatment). Raman spectrum shown in Figure 1.
1 material
Graphene prepared by conventional oxidation-reduction preparation in the solution-phase. Raman spectrum shown in Figure 2 for comparison.
Materials described outside the worked examples.
acid (nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, oxalic acid)
oxidant (nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, peroxides)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Raman spectrum of graphene prepared in Example 1 (Figure 1)
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Carbon To Oxygen Ratio | ≥ 10 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 14 atomic ratio |
Patent
Atlas literature
Patent
US 9,162,894Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
(Cu rr ently Amended) A method for preparing graphene, characterized in that the method consists consisting of the following steps: (i) reacting graphite in an acid solution in which an oxidant is present, (ii) washing the product obtained in step (i) with water to neutral, and (ii) (iii) subjecting the product obtained in step (i) step (ii) to a step of stripping selected from mechanical grinding and/or ultrasonic treatment, thereby resulting in formation of a graphene, wherein the graphene has a ratio of carbon to oxygen atoms of greater than 10, and the ratio of graphite: acid: oxidant: solvent is 1:0.1-50:0.1-50:0.1-100 by mass.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 14.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the acid in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, and oxalic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the oxidant in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, and peroxides.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein solvent in the acid solution comprises one or more selected from the group consisting of ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, and acetic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out at a temperature of 0-90 0C.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out for 1 minute to 10 hours.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 16.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 20. UNT 0050 US 3 Serial No. 13/577,027
UNT 0050 US 2 Serial No. 13/577,027 canceled
9-11. canceled
canceled
canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
2 materials1 process step
Graphene prepared by reacting graphite in an acid solution with an oxidant present, followed by washing to neutral and stripping (mechanical grinding and/or ultrasonic treatment). Raman spectrum shown in Figure 1.
1 material
Graphene prepared by conventional oxidation-reduction preparation in the solution-phase. Raman spectrum shown in Figure 2 for comparison.
Materials described outside the worked examples.
acid (nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, oxalic acid)
oxidant (nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, peroxides)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Raman spectrum of graphene prepared in Example 1 (Figure 1)
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Carbon To Oxygen Ratio | ≥ 10 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 14 atomic ratio |
Patent
Atlas literature
Patent
US 9,162,894Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
(Cu rr ently Amended) A method for preparing graphene, characterized in that the method consists consisting of the following steps: (i) reacting graphite in an acid solution in which an oxidant is present, (ii) washing the product obtained in step (i) with water to neutral, and (ii) (iii) subjecting the product obtained in step (i) step (ii) to a step of stripping selected from mechanical grinding and/or ultrasonic treatment, thereby resulting in formation of a graphene, wherein the graphene has a ratio of carbon to oxygen atoms of greater than 10, and the ratio of graphite: acid: oxidant: solvent is 1:0.1-50:0.1-50:0.1-100 by mass.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 14.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the acid in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, and oxalic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the oxidant in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, and peroxides.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein solvent in the acid solution comprises one or more selected from the group consisting of ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, and acetic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out at a temperature of 0-90 0C.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out for 1 minute to 10 hours.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 16.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 20. UNT 0050 US 3 Serial No. 13/577,027
UNT 0050 US 2 Serial No. 13/577,027 canceled
9-11. canceled
canceled
canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
2 materials1 process step
Graphene prepared by reacting graphite in an acid solution with an oxidant present, followed by washing to neutral and stripping (mechanical grinding and/or ultrasonic treatment). Raman spectrum shown in Figure 1.
1 material
Graphene prepared by conventional oxidation-reduction preparation in the solution-phase. Raman spectrum shown in Figure 2 for comparison.
Materials described outside the worked examples.
acid (nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, oxalic acid)
oxidant (nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, peroxides)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Raman spectrum of graphene prepared in Example 1 (Figure 1)
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Carbon To Oxygen Ratio | ≥ 10 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 14 atomic ratio |
Patent
Atlas literature
Patent
US 9,162,894Claims define the patent's legal scope. Independent claims stand alone; dependent claims (nested) narrow them. Click a claim to expand its dependents.
(Cu rr ently Amended) A method for preparing graphene, characterized in that the method consists consisting of the following steps: (i) reacting graphite in an acid solution in which an oxidant is present, (ii) washing the product obtained in step (i) with water to neutral, and (ii) (iii) subjecting the product obtained in step (i) step (ii) to a step of stripping selected from mechanical grinding and/or ultrasonic treatment, thereby resulting in formation of a graphene, wherein the graphene has a ratio of carbon to oxygen atoms of greater than 10, and the ratio of graphite: acid: oxidant: solvent is 1:0.1-50:0.1-50:0.1-100 by mass.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 14.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the acid in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, and oxalic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the oxidant in the acid solution comprises one or more selected from the group consisting of nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, and peroxides.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein solvent in the acid solution comprises one or more selected from the group consisting of ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, and acetic acid.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out at a temperature of 0-90 0C.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the reaction of step (i) is carried out for 1 minute to 10 hours.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 16.
(Cu rr ently Amended) The method according to claim 1, characterized in that wherein the graphene has a ratio of carbon to oxygen atoms of greater than 20. UNT 0050 US 3 Serial No. 13/577,027
UNT 0050 US 2 Serial No. 13/577,027 canceled
9-11. canceled
canceled
canceled
Embodiments described in the patent, grouped by the materials and process steps they use.
2 materials1 process step
Graphene prepared by reacting graphite in an acid solution with an oxidant present, followed by washing to neutral and stripping (mechanical grinding and/or ultrasonic treatment). Raman spectrum shown in Figure 1.
1 material
Graphene prepared by conventional oxidation-reduction preparation in the solution-phase. Raman spectrum shown in Figure 2 for comparison.
Materials described outside the worked examples.
acid (nitric acid, sulfuric acid, perchloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, acetic acid, oxalic acid)
oxidant (nitric acid, sulfuric acid, perchloric acid, hydrochloric acid, hypochlorous acid, nitrous acid, chlorosulfonic acid, dichromates, perchlorates, chlorates, hypochlorites, persulfates, hydrogen peroxide, peroxides)
Additional fabrication and treatment steps described in the patent.
Measurements and analyses referenced in the patent, with their drawing references.
Raman spectrum of graphene prepared in Example 1 (Figure 1)
Performance values and ranges asserted in the specification or claims.
| Property | Value | Material |
|---|---|---|
Carbon To Oxygen Ratio | ≥ 10 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 14 atomic ratio |
solvent (ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, acetic acid)
Raman spectrum of graphene prepared in Comparative Example 1 (Figure 2)
Carbon To Oxygen Ratio | ≥ 16 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 20 atomic ratio | graphene |
Thickness | 1–50 µm | — |
Duration | 60–36000 s | — |
Duration | 600–32400 s | — |
Duration | 1800–18000 s | — |
Duration | 10–300 s | — |
Duration | 50–180 s | — |
Duration | 1800–72000 s | — |
Duration | 2–15 hours | — |
Duration | 10–14 hours | — |
Duration | 600–28800 s | — |
Duration | 1200–21600 s | — |
Duration | 2400–14400 s | — |
Thickness | 2–3 nm | — |
Duration | ≥ 10 seconds | — |
Duration | ≥ 10 minutes | — |
Duration | ≥ 15 minutes | — |
Duration | ≥ 20 minutes | — |
solvent (ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, acetic acid)
Raman spectrum of graphene prepared in Comparative Example 1 (Figure 2)
Carbon To Oxygen Ratio | ≥ 16 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 20 atomic ratio | graphene |
Thickness | 1–50 µm | — |
Duration | 60–36000 s | — |
Duration | 600–32400 s | — |
Duration | 1800–18000 s | — |
Duration | 10–300 s | — |
Duration | 50–180 s | — |
Duration | 1800–72000 s | — |
Duration | 2–15 hours | — |
Duration | 10–14 hours | — |
Duration | 600–28800 s | — |
Duration | 1200–21600 s | — |
Duration | 2400–14400 s | — |
Thickness | 2–3 nm | — |
Duration | ≥ 10 seconds | — |
Duration | ≥ 10 minutes | — |
Duration | ≥ 15 minutes | — |
Duration | ≥ 20 minutes | — |
solvent (ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, acetic acid)
Raman spectrum of graphene prepared in Comparative Example 1 (Figure 2)
Carbon To Oxygen Ratio | ≥ 16 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 20 atomic ratio | graphene |
Thickness | 1–50 µm | — |
Duration | 60–36000 s | — |
Duration | 600–32400 s | — |
Duration | 1800–18000 s | — |
Duration | 10–300 s | — |
Duration | 50–180 s | — |
Duration | 1800–72000 s | — |
Duration | 2–15 hours | — |
Duration | 10–14 hours | — |
Duration | 600–28800 s | — |
Duration | 1200–21600 s | — |
Duration | 2400–14400 s | — |
Thickness | 2–3 nm | — |
Duration | ≥ 10 seconds | — |
Duration | ≥ 10 minutes | — |
Duration | ≥ 15 minutes | — |
Duration | ≥ 20 minutes | — |
solvent (ethanol, carbon tetrachloride, benzene, water, methanol, acetone, formaldehyde, acetaldehyde, acetic acid)
Raman spectrum of graphene prepared in Comparative Example 1 (Figure 2)
Carbon To Oxygen Ratio | ≥ 16 atomic ratio | graphene |
Carbon To Oxygen Ratio | ≥ 20 atomic ratio | graphene |
Thickness | 1–50 µm | — |
Duration | 60–36000 s | — |
Duration | 600–32400 s | — |
Duration | 1800–18000 s | — |
Duration | 10–300 s | — |
Duration | 50–180 s | — |
Duration | 1800–72000 s | — |
Duration | 2–15 hours | — |
Duration | 10–14 hours | — |
Duration | 600–28800 s | — |
Duration | 1200–21600 s | — |
Duration | 2400–14400 s | — |
Thickness | 2–3 nm | — |
Duration | ≥ 10 seconds | — |
Duration | ≥ 10 minutes | — |
Duration | ≥ 15 minutes | — |
Duration | ≥ 20 minutes | — |