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US 2018/0008968 A1Published application
Method for preparing highly nitrogen-doped mesoporous carbon composites
AssigneesUniversite De Strasbourg, Centre National de la Recherche Scientifique (CNRS), Consiglio Nazionale Delle Ricerche
InventorsCuong PHAM-HUU, Giuliano GIAMBASTIANI, Yuefeng LIU, Housseinou BA, Lam NGUYEN-DINH, Jean-Mario NHUT, Cuong DUONG-VIET
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Abstract
Some embodiments are directed to a new methodology aimed at preparing highly N-doped mesoporous carbon macroscopic composites, and their use as highly efficient heterogeneous metal-free catalysts in a number of industrially relevant catalytic transformations.
Claims17
A method of preparing macroscopic composites made of a macroscopic support coated with a thin layer of highly nitrogen-doped mesoporous carbon phase (active phase), said method comprising:
- (a) providing an aqueous solution of (i) (NH4)2CO3;
- (ii) a carbohydrate as carbon source, selected from aldose monosaccharides and glycosilated forms thereof, disaccharides and oligosaccharides or dextrine deriving from biomass conversion, and (iii) a carboxylic acid source selected from citric acid, and any other mono-, di-, tri-, and poly-carboxylic acid or their ammonium mono-, di-, tri- and poly-basic forms;
- (b) providing a macroscopic support made of carbon-, silicium- or aluminum-based material, or binary mixtures thereof;
- wherein the macroscopic support is a single object or an assembly of smaller objects, wherein the overall dimension of the support ranges from 0.1 μm to 100 cm in three orthogonal directions;
- optionally subjecting the maccroscopic support of step (b) to a passivation process comprising steps of:
- (a1) providing an aqueous solution of citric acid and a carbohydrate as carbon source, selected from aldose monosaccharides and glycosilated forms thereof, disaccharides and oligosaccharides;
- (c1) prior to step (c), immerging/soaking or impregnating the macroscopic support of step (b) in the aqueous solution of step (a1) for a suitable amount of time;
- (d1) optionally removing the immerged macroscopic support from the aqueous solution of step (a1) if an excess aqueous solution is used in step (c1);
- (e1′) optionally subjecting the resulting macroscopic support to a gentle thermal treatment (drying) under air at low temperatures from 45 to 55° C., preferably 50° C.±3° C.;
- (e1) subjecting the resulting macroscopic support to a first thermal treatment (drying) under air at moderate temperatures from 110-150° C.±5° C., preferably 130° C.±5° C.;
- and
- (f1) subjecting the thermally treated (dried) macroscopic support to a second thermal treatment under inert atmosphere at higher temperatures from 600-800° C.±10° C., preferably 600° C.±5° C.;
- thereby generating a macroscopic composite coated with a carbon layer;
- (c) immerging/soaking or impregnating the macroscopic support of step (b), or the passivated macroscopic support obtained in step (f1) when a passivation process is used, in the aqueous solution of step (a) for a suitable amount of time;
- (d) optionally removing the immerged macroscopic support from the aqueous solution of step (a) if an excess aqueous solution is used in step (c);
- (e′) optionally subjecting the resulting macroscopic support to a gentle thermal treatment (drying) under air at low temperatures from 45 to 55° C., preferably 50° C.±3° C.;
- (e) subjecting the resulting macroscopic support to a first thermal treatment (drying) under air at moderate temperatures from 110-150° C.±5° C., preferably 130° C.±5° C.;
- (f) optionally subjecting the thermally treated (dried) macroscopic support to a second thermal treatment under air at higher temperatures:
- from 400-500° C.±10° C., preferably 400° C.±5° C. for 1 to 2 hours, or
- at 300° C.±10° C. for 2 to 4 hours;
- thereby generating a macroscopic composite composed of a macroscopic support coated with a 20-200 nm thick layer of highly N-doped mesoporous carbonaceous material;
- wherein the N atom % in the mesoporous carbonaceous material is 25-40%;
- and
- (g) optionally subjecting the macroscopic composite obtained in step (f) to a third thermal treatment by heating it to a temperature ranging between 600 to 900° C.±10° C. under inert atmosphere, preferably 700 to 900° C.±10° C.;
- thereby generating a macroscopic composite composed of a macroscopic support coated with a 10-100 nm thick layer of highly N-doped mesoporous carbonaceous material;
- wherein the N atom % in the mesoporous carbonaceous material is 2-35%, preferably 5-30%, most preferably about 15% (12-18%);
- wherein the method comprises at least one of steps (f) or (g).
24 more elements
A macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm.
2 more elements
A method of performing a catalytic reaction, comprising:
- providing a macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material, wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm;
- and
- initiating the catalytic reaction with the macroscopic composite.
5 more elements
A method for performing a catalytic reaction, comprising:
- providing a macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material, wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm;
- and
- initiating the catalytic reaction with the macroscopic composite as catalytic support for metal(s) and oxide(s) in at least one of liquid-phase and gas-phase hydrogenation, oxidation of linear alkanes and volatil organic compounds (VOCs), hydrogenation of CO in the Fischer-Tropsch process, and methanization of synthesis gas mixture.
5 more elements
A method of manufacturing, comprising:
- providing a macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material, wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm;
- and
- manufacturing metal-free surface heater in inductive heating devices with the macroscopic composite.
5 more elements
A method of performing absorption, comprising:
- providing a macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material, wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm;
- and
- performing absorption with the macroscopic composite for volatil organic compounds.
5 more elements
A method of performing a catalytic reaction, comprising:
- providing a macroscopic composite coated with a layer of highly N-doped mesoporous carbonaceous material, wherein the N-doped carbonaceous material layer:
- has an N atom contents of 1-40%, preferably 5-40%, preferably 10-35%, preferably about 15% (e.g., 12-18%);
- has an average pore size of 2-50 nm, preferably 2-30 nm;
- most preferably 3-12 nm;
- and
- has a thickness of 5 to 200±5 nm, preferably 10 to 100±5 nm;
- and
- initiating the catalytic reaction with the macroscopic composite as a metal-free catalyst in the Advanced Oxidation Processes for water and wastewater treatment.
5 more elements
Dependencies are inferred from the claim text.