# US 11,299,395 B2 · Porous one-dimensional polymeric graphitic carbon nitride-based nanosystems for catalytic conversion of carbon monoxide and carbon dioxide under ambient conditions

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

- Number: US 11,299,395 B2
- Document ID: US11299395B2
- Status: Granted
- Kind: B2
- Application number: 16/846,020
- Filed: 2020-04-10
- Published: 2020-07-30
- Granted: 2022-04-12
- Earliest claimed: 2020-01-14
- Assignees: Qatar University
- Applicants: Qatar University
- Inventors: Kamel Abdelmoniem Mohamed Eid; Aboubakr Moustafa Abdullah
- Web page: https://patentgrep.com/patent/US11299395B2

## CPC

- C01B 21/0605: {Binary compounds of nitrogen with carbon}
- B01D 53/04: with stationary adsorbents {(B01D53/025 takes precedence)}
- B01D 53/864: {Removing carbon monoxide or hydrocarbons}
- B01J 21/185: {Carbon nanotubes (carbon nanotubes per se C01B32/15)}
- B01J 23/42: Platinum
- B01J 23/44: Palladium
- B01J 23/52: Gold
- B01J 23/8926: {Copper and noble metals}
- B01J 27/24: Nitrogen compounds
- B01J 35/45: Nanoparticles
- B01J 35/615: {100-500 m2/g}
- B01J 35/633: {less than 0.5 ml/g}
- B01J 35/635: {0.5-1.0 ml/g}
- B01J 35/647: {2-50 nm}
- B01J 35/651: {50-500 nm}
- B01J 37/031: {Precipitation}
- B01J 37/033: {Using Hydrolysis}
- B01J 37/084: {Decomposition of carbon-containing compounds into carbon}
- B01J 37/088: {Decomposition of a metal salt}
- B01D 2255/1021: Platinum
- B01D 2255/1023: Palladium
- B01D 2255/106: Gold
- B01D 2255/20761: Copper
- B01D 2255/702: Carbon
- B01D 2255/9202: Linear dimensions
- B01D 2257/504: Carbon dioxide
- C01P 2002/01: depicted by a TEM-image
- C01P 2002/10: One-dimensional structures
- C01P 2002/52: containing elements as dopants
- C01P 2002/85: by XPS, EDX or EDAX data
- C01P 2004/03: obtained by SEM
- C01P 2004/04: obtained by TEM, STEM, STM or AFM
- C01P 2004/16: Nanowires or nanorods, i.e. solid nanofibres with two nearly equal dimensions between 1-100 nanometer
- C01P 2006/12: Surface area
- C01P 2006/16: Pore diameter
- Y02C 20/40: of CO2
- Y02P 20/151: Reduction of greenhouse gas [GHG] emissions, e.g. CO2
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- 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)
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02C: CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

In some aspects and embodiments, the present application provides a wide range of porous 1-D polymeric graphitic carbon-nitride materials that are atomically doped with binary metals in different morphologies. In some embodiments, the graphitic carbon-nitride materials can be prepared with high mass production from inexpensive and natural abundant precursors. In some embodiments, the materials were used successfully for the oxidation of CO to CO2 under ambient reaction temperature in addition to the reduction of CO2 into hydrocarbons. In some embodiments, the materials can be used for practical and large-scale gas conversion for household or industrial applications.

## Claims

### Claim 1

A graphitic-like carbon nitride nanostructure, wherein the nanostructure is doped atomically with one or more metal elements;
wherein the nanostructure comprises at least one of nanotubes, nanorods, or nanofibers; and
wherein the one or more metal elements comprise a metal element selected from the group consisting of gold (Au), palladium (Pd), copper (Cu), and platinum (Pt);
wherein the nanostructure is additionally characterized by at least one of the following features:
(i) wherein the nanostructure is doped with 1-1.2 wt. % Au/Pd, or 1-1.2 wt. % Pd/Cu, or 1-1.2 wt. % Pt/Pd;
(ii) wherein the nanostructure is selected from the group consisting of a carbon nitride nanotube doped with Au and Pd (Au/Pd/g C3N4NT); a carbon nitride nanofiber doped with Au and Pd (Au/Pd/gC3N4NF); a carbon nitride nanorod doped with Pt and Pd (Pt/Pd/CN nanorod); and a carbon nitride nanotube doped with Pd and Cu (Pd/Cu/gC3N4NF); or
(iii) wherein the nanostructure is porous, having surface area ranging from 300 m2g−1 to 350 m2 g−1, an average pore size/diameter ranging from 45 nm to 65 nm, and a pore volume ranging from 0.45 cc/g to 0.65 cc/g.

### Claim 2 (depends on 1)

The nanostructure of claim 1, wherein the one or more metal elements comprise Pd and at least a second metal element selected from the group consisting of Au and Pt.

### Claim 3 (depends on 1)

The nanostructure of claim 1, wherein the nanostructure is one-dimensional (1-D).

### Claim 4 (depends on 1)

The nanostructure of claim 1, wherein the nanostructure is functionalized with one or more metal-based nanoparticles, single atoms, metal oxide nanoparticles, or hybrid nanoparticles; and wherein the nanostructure is a catalyst for a CO oxidation reaction and/or a CO2 reduction reaction.

### Claim 5 (depends on 4)

The graphitic-like carbon nitride nanostructure of claim 4, wherein the one or more metal elements are in the form of dopants, single atoms, nanoparticles, ions, oxide, or any combination thereof.

### Claim 6 (depends on 1)

The graphitic-like carbon nitride nanostructure of claim 1, wherein the nanostructure is doped atomically with Pd.

### Claim 7 (depends on 6)

The graphitic-like carbon nitride nanostructure of claim 6, wherein the nanostructure is doped atomically at least a second metal element selected from the group consisting of Au, Cu, and Pt.

### Claim 8 (depends on 7)

The graphitic-like carbon nitride nanostructure of claim 7, wherein the nanostructure is doped with 1-1.2 wt. % Au/Pd, or 1-1.2 wt. % Pd/Cu, or 1-1.2 wt. % Pt/Pd.

### Claim 9 (depends on 1)

The graphitic-like carbon nitride nanostructure of claim 1, wherein the nanostructure is doped with 1-1.2 wt. % metal elements.

### Claim 10 (depends on 1)

The graphitic-like carbon nitride nanostructure of claim 1, wherein the nanostructure is selected from the group consisting of a carbon nitride nanotube doped with Au and Pd (Au/Pd/g C3N4NT); a carbon nitride nanofiber doped with Au and Pd (Au/Pd/gC3N4NF); a carbon nitride nanorod doped with Pt and Pd (Pt/Pd/CN nanorod); and a carbon nitride nanotube doped with Pd and Cu (Pd/Cu/gC3N4NF).

### Claim 11 (depends on 1)

The graphitic-like carbon nitride nanostructure of claim 1, wherein the nanostructure is porous, having surface area ranging from 300 m2g−1 to 350 m2 g−1, an average pore size/diameter ranging from 45 nm to 65 nm, and a pore volume ranging from 0.45 cc/g to 0.65 cc/g.

### Claim 12 (depends on 1)

The graphitic-like carbon nitride nanostructure of claim 1, wherein the nanostructure is a catalyst for oxidizing CO in a CO gas mixture and/or reducing CO2 in a CO2 gas mixture at a temperature ranging from room temperature to 300° C., wherein the CO gas mixture contains 1%-100% of CO, and wherein the CO2 gas mixture contains 1%-100% of CO2.

### Claim 13

A graphitic-like carbon nitride nanostructure, wherein the nanostructure is doped atomically with one or more metal elements;
wherein the nanostructure comprises at least one of nanotubes, nanorods, or nanofibers; and
wherein the one or more metal elements comprise a metal element selected from the group consisting of gold (Au), palladium (Pd), copper (Cu), and platinum (Pt);
wherein the nanostructure is a catalyst for oxidizing CO in a CO gas mixture and/or reducing CO2 in a CO2 gas mixture at a temperature ranging from room temperature to 300° C., wherein the CO gas mixture contains 1%-100% of CO, and wherein the CO2 gas mixture contains 1%-100% of CO2;
wherein the CO and CO2 conversion is enhanced using at least one other metal support selected from the group consisting of metal oxides, molecular sieves, carbon supports, ceramic-based materials, clay-based materials, and promoters,
wherein the metal oxides is at least one of TiO2, CeO2,Fe2O3, SiO2, or Fe3O4,
wherein the molecular sieves is a zeolite,
wherein the carbon supports is at least one of diamond, graphene, cellulose, lignin, and carbon nanotube,
wherein the ceramic-based materials comprises bioglass and hydroxyapatite,
wherein the clay-based materials comprises bentonite and halloysite, and
wherein the promotors comprises KOH, HCl, HNO3, and CH3COOH.