Porous one-dimensional polymeric graphitic carbon nitride-based nanosystems for catalytic conversion of carbon monoxide and carbon dioxide under ambient conditions
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 CO 2 under ambient reaction temperature in addition to the reduction of CO 2 into hydrocarbons. In some embodiments, the materials can be used for practical and large-scale gas conversion for household or industrial applications.
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 C 3 N 4 NT); a carbon nitride nanofiber doped with Au and Pd (Au/Pd/gC 3 N 4 NF); 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/gC 3 N 4 NF); or
(iii) wherein the nanostructure is porous, having surface area ranging from 300 m 2 g −1 to 350 m 2 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.
2. 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.
3. The nanostructure of claim 1 , wherein the nanostructure is one-dimensional (1-D).
4. 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 CO 2 reduction reaction.
5. 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.
6. The graphitic-like carbon nitride nanostructure of claim 1 , wherein the nanostructure is doped atomically with Pd.
7. 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.
8. 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.
9. The graphitic-like carbon nitride nanostructure of claim 1 , wherein the nanostructure is doped with 1-1.2 wt. % metal elements.
10. 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 C 3 N 4 NT); a carbon nitride nanofiber doped with Au and Pd (Au/Pd/gC 3 N 4 NF); 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/gC 3 N 4 NF).
11. The graphitic-like carbon nitride nanostructure of claim 1 , wherein the nanostructure is porous, having surface area ranging from 300 m 2 g −1 to 350 m 2 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.
12. 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 CO 2 in a CO 2 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 CO 2 gas mixture contains 1%-100% of CO 2 .
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 CO 2 in a CO 2 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 CO 2 gas mixture contains 1%-100% of CO 2 ;
wherein the CO and CO 2 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 TiO 2 , CeO 2 ,Fe 2 O 3 , SiO 2 , or Fe 3 O 4 ,
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, HNO 3 , and CH 3 COOH.