# US 10,864,498 B2 · Composite graphene-based material

> Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt

- Number: US 10,864,498 B2
- Document ID: US10864498B2
- Status: Granted
- Kind: B2
- Application number: 15/578,149
- Filed: 2016-05-27
- Published: 2018-05-17
- Granted: 2020-12-15
- Earliest claimed: 2015-05-29
- Assignees: Adelaide Research & Innovation Pty Ltd
- Applicants: Adelaide Research & Innovation Pty Ltd
- Inventors: Dusan Losic; Diana Tran; Shervin Kabiri
- Web page: https://patentgrep.com/patent/US10864498B2

## CPC

- B01J 20/28026: {Particles within, immobilised, dispersed, entrapped in or on a matrix, e.g. a resin}
- B01D 15/00: Separating processes involving the treatment of liquids with solid sorbents; Apparatus therefor
- B01D 15/08: Selective adsorption, e.g. chromatography
- B01D 53/02: by adsorption, e.g. preparative gas chromatography {(solid sorbent compositions B01J20/00, preparation of inorganic compounds or elements C01)}
- B01J 20/0229: {Compounds of Fe}
- B01J 20/0233: {Compounds of Cu, Ag, Au}
- B01J 20/06: comprising oxides or hydroxides of metals not provided for in group B01J20/04
- B01J 20/14: Diatomaceous earth
- B01J 20/20: comprising free carbon; comprising carbon obtained by carbonising processes
- B01J 20/205: {Carbon nanostructures, e.g. nanotubes, nanohorns, nanocones, nanoballs (carbon nanotubes per se C01B32/15)}
- B01J 20/28009: {Magnetic properties}
- B01J 20/28011: {Other properties, e.g. density, crush strength}
- B01J 20/305: {Addition of material, later completely removed, e.g. as result of heat treatment, leaching or washing, e.g. for forming pores}
- B01J 20/3085: {Chemical treatments not covered by groups B01J20/3007 - B01J20/3078}
- B01J 20/3242: {Layers with a functional group, e.g. an affinity material, a ligand, a reactant or a complexing group}
- B01J 20/3248: {the functional group or the linking, spacer or anchoring group as a whole comprising at least one type of heteroatom selected from a nitrogen, oxygen or sulfur, these atoms not being part of the carrier as such}
- B01J 20/3257: {the functional group or the linking, spacer or anchoring group as a whole comprising at least one of the heteroatoms nitrogen, oxygen or sulfur together with at least one silicon atom, these atoms not being part of the carrier as such}
- B01J 20/3274: {Proteins, nucleic acids, polysaccharides, antibodies or antigens}
- B01J 20/3289: {Coatings involving more than one layer of same or different nature}
- C01B 32/192: starting from graphitic oxides
- C02F 1/28: by sorption (using ion-exchange C02F1/42; sorbent compositions B01J)
- C02F 1/281: {using inorganic sorbents}
- C02F 1/288: {using composite sorbents, e.g. coated, impregnated, multi-layered}
- B01D 2253/102: Carbon
- B01D 2253/106: Silica or silicates
- B01D 2253/108: Zeolites
- B01D 2253/1124: Metal oxides
- B01D 2253/25: Coated, impregnated or composite adsorbents
- B01D 2253/304: Linear dimensions, e.g. particle shape, diameter
- B01D 2257/60: Heavy metals or heavy metal compounds
- B01D 2257/602: Mercury or mercury compounds
- B01D 2258/0283: Flue gases
- C02F 1/283: {using coal, charred products, or inorganic mixtures containing them}
- C02F 2101/20: Heavy metals or heavy metal compounds
- C02F 2101/32: Hydrocarbons, e.g. oil
- C02F 2305/08: Nanoparticles or nanotubes
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C02F: TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE (separation in general B01D; special arrangements on waterborne vessels of installations for treating water, waste water or sewage, e.g. for producing fresh water, B63J; adding materials to water to prevent corrosion C23F; treating radioactively-contaminated liquids G21F9/04; regeneration of reactants for recirculation into processes, see the relevant places for the processes)

## Abstract

The present invention provides composite material having a porous graphene-based foam matrix and comprising porous inorganic micro-particles and metal oxide nano-particles distributed throughout the foam matrix.

## Claims

### Claim 1

Composite material having (i) a porous graphene-based foam matrix comprising reduced graphene oxide and (ii) porous inorganic micro-particles and metal oxide nano-particles distributed throughout the foam matrix, wherein a surface of the composite material is functionalised with one or more of: sulfur-containing functional groups comprising a thiol group or a thio silane group, oxygen-containing functional groups comprising a hydroxyl group, phospho-containing functional groups, nitrogen-containing functional groups comprising an amine group, a quaternary ammonium group or an amino silane group, and a chelating agent selected from the group consisting of N-(trimethoxysilylpropyl) ethylenediamine triacetic acid (EDTA-silane) and N-(trimethoxysilylpropyl) diethylene triamine pentaacetic acid (DPTA-silane): wherein the ratio of graphene-based matrix to porous inorganic micro-particles ranges from about 6:1 to about 3:1 by weight.

### Claim 2 (depends on 1)

The composite material according to claim 1, wherein the porous graphene-based foam matrix is an aerogel or a xerogel.

### Claim 3 (depends on 1)

The composite material according to claim 1, wherein the porous inorganic micro-particles comprise or are made of diatomaceous earth, zeolites, silica, clays carbonates, magnetite, alumina, titania, ZnO, SnO2, ZrO2, MgO, CuO, Fe2O3, Fe3O4 or combinations thereof.

### Claim 4 (depends on 1)

The composite material according to claim 1, wherein the metal oxide nano-particles are selected from oxides of iron, manganese, aluminium, titanium, zinc, gold, silver, copper, lithium, manganese, magnesium, cerium and combinations thereof.

### Claim 5 (depends on 1)

The composite material according to claim 1 having a density ranging from about 0.01 mg/cm3 to about 0.1 mg/cm3.

### Claim 6 (depends on 1)

A method of removing a target species from a liquid or gas, the method comprising contacting at least the target species with the composite material according to claim 1.

### Claim 7 (depends on 6)

The method according to claim 6, wherein the target species are anions derived from one or more of P, CN, As, and Cr, or cations derived from one or more of Hg, Cd, Pb, Cr, Co, Ni, Cu, Zn, As, Se, Au, U, Po and Th.

### Claim 8 (depends on 6)

The method according to claim 6, wherein the liquid is an aqueous liquid and the gas is a flue, combustion or exhaust gas.

### Claim 9 (depends on 1)

The composite material according to claim 1, wherein the porous inorganic micro-particles and metal oxide nano-particles are distributed substantially uniformly throughout the foam matrix.

### Claim 10 (depends on 1)

The composite material according to claim 1, wherein the porous inorganic micro-particles and metal oxide nano-particles are adhered or bound to the surface of the foam matrix.

### Claim 11 (depends on 1)

The composite material according to claim 1, wherein the porous inorganic micro-particles are present in the composite material in an amount ranging from about 20% to about 80% by weight of the composite.

### Claim 12 (depends on 1)

The composite material according to claim 1, wherein the metal oxide nano-particles are present in the composite material in an amount ranging from about 5% to about 35% by weight of the composite.

### Claim 13

A method of preparing composite material having (a) a porous graphene-based foam matrix comprising reduced graphene oxide and (b) porous inorganic micro-particles and metal oxide nano-particles distributed throughout the foam matrix, the method comprising: (i) providing a liquid dispersion comprising dispersed graphene-based material, porous inorganic micro-particles, and metal oxide nano-particles: (ii) forming a gel from the liquid dispersion: (iii) forming the composite material by removing the liquid from the so formed gel; and (iv) reacting surface functional groups of the so formed composite material with one or more compounds to covalently attach to the composite material sulfur-containing functional groups comprising a thiol group or a thio silane group, oxygen-containing functional groups comprising a hydroxyl group, phospho-containing functional groups, nitrogen-containing functional groups comprising an amine group, a quaternary ammonium group or an amino silane group, a chelating agent selected from the group consisting of N-(trimethoxysilylpropyl) ethylenediamine triacetic acid (EDTA-silane) and N-(trimethoxysilylpropyl) diethylene triamine pentaacetic acid (DPTA-silane), or a combination thereof; wherein the ratio of graphene-based matrix to porous inorganic micro-particles ranges from about 6:1 to about 3:1 by weight.

### Claim 14 (depends on 13)

The method according to claim 13, wherein the graphene-based material comprises graphene oxide.

### Claim 15 (depends on 13)

The method according to claim 13, wherein the liquid dispersion is prepared by a process comprising contacting a liquid with a metal oxide nano-particle precursor, and wherein the metal oxide nano-particle precursor is converted in situ to form the metal oxide nano-particles.