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US 11,767,221 B2Granted
Production of graphene sheets from highly aromatic molecules
AssigneeGlobal Graphene Group, Inc.
InventorsAruna Zhamu, Bor Z. Jang
Life of this patent
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Abstract
Provided is a method of producing isolated graphene sheets directly from a carbon/graphite precursor. The method comprises: (a) providing a mass of halogenated aromatic molecules selected from halogenated petroleum heavy oil or pitch, coal tar pitch, polynuclear hydrocarbon, or a combination thereof; (b) heat treating this mass at a first temperature of 25 to 300° C. in the presence of a catalyst and optionally at a second temperature of 300-3,200° C. to form graphene domains dispersed in a disordered matrix of carbon or hydrocarbon molecules, and (c) separating and isolating the planes of hexagonal carbon atoms or fused aromatic rings to recover graphene sheets from the disordered matrix.
Claims17
A method of producing isolated graphene sheets, said method comprising:
- a) providing a mass of halogenated aromatic molecules in a solid, or semi-solid state wherein said halogenated aromatic molecules are selected from halogenated variants of petroleum heavy oil or pitch, coal tar pitch, a polynuclear hydrocarbon, and combinations thereof, wherein said halogenated variants of polynuclear hydrocarbon are selected from halogenated variants of naphthalene, phenanthrene, chrysene, triphenylene, corannulene, benzo-perylene, coronene, ovalene, benzo-fluorene, a derivative thereof having a substituent on a ring structure thereof, a chemical derivative thereof, and combinations thereof;
- b) heat treating said mass of halogenated aromatic molecules at a first temperature selected from 25° C. to 3,000° C. so that said halogenated aromatic molecules are merged or fused into larger aromatic molecules and optionally heat-treating said larger molecules at a second temperature, higher than the first temperature, selected from 300° C. to 3,200° C., to form graphene domains dispersed in a disordered matrix of carbon or hydrocarbon molecules, wherein said graphene domains are each composed of from 1 to 30 planes of hexagonal carbon atoms or fused aromatic rings having a length or width from 5 nm to 35 μm and, in the situations wherein there are 2-30 planes in a graphene domain, having an inter-graphene space between two planes of hexagonal carbon atoms or fused aromatic rings no less than 0.34 nm;
- c) separating and isolating said planes of hexagonal carbon atoms or fused aromatic rings to recover graphene sheets from said disordered matrix;
- and
- d) conducting a chemical means to treat said halogenated aromatic molecules during or after said step (b), wherein said chemical means comprises adding a functionalizing agent into said mass of halogenated aromatic molecules and said halogenated aromatic molecules are chemically functionalized by said agent, wherein said functionalizing agent contains a functional group selected from the group consisting of amidoamines, polyamides, aliphatic amines, modified aliphatic amines, cycloaliphatic amines, aromatic amines, anhydrides, ketimines, diethylenetriamine (DETA), triethylene-tetramine (TETA), tetraethylene-pentamine (TEPA), polyethylene polyamine, polyamine epoxy adduct, phenolic hardener, non-brominated curing agent, non-amine curatives, an acrylonitrile chain, polyfurfuryl alcohol, phenolic resin, and combinations thereof;
- and/or said functionalizing agent contains a functional group selected from OY, NHY, O═C—OY, P═C—NR′Y, O═C—SY, O═C—Y, —CR′1-OY, N′Y or C′Y, and Y is a functional group of a protein, a peptide, an amino acid, an enzyme, an antibody, a nucleotide, an oligonucleotide, an antigen, or an enzyme substrate, enzyme inhibitor or the transition state analog of an enzyme substrate or is selected from R′—OH, R′—NR′2, R′SH, R′CHO, R′CN, R′X, R′N+(R′)3X−, R′SiR′3, R′Si(—OR′—)yR′3-y, R′Si(—O—SiR′2—)OR′, R′—R″, R′—N—CO, (C2H4O—)wH, (—C3H6O—)wH, (—C2H4O)w—R′, (C3H6O)w—R′, R′, and w is an integer greater than one and less than 200;
- wherein said graphene sheet production and said chemical functionalization are accomplished concurrently.
4 more elements
A method of producing isolated graphene sheets, said method comprising:
- a) providing a mass of halogenated aromatic molecules in a liquid, solid, or semi-solid state wherein said halogenated aromatic molecules are selected from halogenated variants of petroleum heavy oil or pitch, coal tar pitch, a polynuclear hydrocarbon, and combinations thereof;
- b) heat treating said mass of halogenated aromatic molecules at a first temperature selected from 25° C. to 3,000° C. so that said halogenated aromatic molecules are merged or fused into larger aromatic molecules and optionally heat-treating said larger molecules at a second temperature, higher than the first temperature, selected from 300° C. to 3,200° C., to form graphene domains dispersed in a disordered matrix of carbon or hydrocarbon molecules, wherein said graphene domains are each composed of from 1 to 30 planes of hexagonal carbon atoms or fused aromatic rings having a length or width from 5 nm to 35 μm and, in the situations wherein there are 2-30 planes in a graphene domain, having an inter-graphene space between two planes of hexagonal carbon atoms or fused aromatic rings no less than 0.34 nm, and further comprising conducting a mechanical means on said halogenated aromatic molecules or said larger aromatic molecules during step (b) wherein said mechanical means is selected from exposing said mass of halogenated aromatic molecules to a gaseous environment, flowing fluid, sonic waves, mechanical shearing, and combinations thereof;
- and
- c) separating and isolating said planes of hexagonal carbon atoms or fused aromatic rings to recover graphene sheets from said disordered matrix.
1 more element
A method of producing isolated graphene sheets, said method comprising:
- a) providing a mass of halogenated aromatic molecules in a liquid, solid, or semi-solid state wherein said halogenated aromatic molecules are selected from halogenated variants of petroleum heavy oil or pitch, coal tar pitch, a polynuclear hydrocarbon, and combinations thereof;
- b) heat treating said mass of halogenated aromatic molecules at a first temperature selected from 25° C. to 3,000° C. so that said halogenated aromatic molecules are merged or fused into larger aromatic molecules and optionally heat-treating said larger molecules at a second temperature, higher than the first temperature, selected from 300° C. to 3,200° C., to form graphene domains dispersed in a disordered matrix of carbon or hydrocarbon molecules, wherein said graphene domains are each composed of from 1 to 30 planes of hexagonal carbon atoms or fused aromatic rings having a length or width from 5 nm to 35 μm and, in the situations wherein there are 2-30 planes in a graphene domain, having an inter-graphene space between two planes of hexagonal carbon atoms or fused aromatic rings no less than 0.34 nm;
- and
- c) separating and isolating said planes of hexagonal carbon atoms or fused aromatic rings to recover graphene sheets from said disordered matrix, wherein said step of separating and isolating includes solvent extraction or supercritical fluid extraction of said planes of hexagonal carbon atoms or fused aromatic rings from said disordered matrix to form said graphene sheets.
1 more element
A method of producing isolated graphene sheets, said method comprising:
- a) providing a mass of halogenated aromatic molecules in a liquid, solid, or semi-solid state wherein said halogenated aromatic molecules are selected from halogenated variants of petroleum heavy oil or pitch, coal tar pitch, a polynuclear hydrocarbon, and combinations thereof;
- b) heat treating said mass of halogenated aromatic molecules at a first temperature selected from 25° C. to 3,000° C. so that said halogenated aromatic molecules are merged or fused into larger aromatic molecules and optionally heat-treating said larger molecules at a second temperature, higher than the first temperature, selected from 300° C. to 3,200° C., to form graphene domains dispersed in a disordered matrix of carbon or hydrocarbon molecules, wherein said graphene domains are each composed of from 1 to 30 planes of hexagonal carbon atoms or fused aromatic rings having a length or width from 5 nm to 35 μm and, in the situations wherein there are 2-30 planes in a graphene domain, having an inter-graphene space between two planes of hexagonal carbon atoms or fused aromatic rings no less than 0.34 nm;
- and
- c) separating and isolating said planes of hexagonal carbon atoms or fused aromatic rings to recover graphene sheets from said disordered matrix, wherein said step (c) includes a step of dissolving, melting, etching, vaporizing, subliming, burning off, or ultrasonicating said disordered matrix material for separating said graphene sheets.
1 more element
Dependencies are inferred from the claim text.