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Monatomic iron nitrogen-doped porous carbon catalyst as well as preparation method and application thereof

A catalyst and porous carbon technology, applied in the field of monoatomic iron nitrogen-doped porous carbon catalyst and its preparation, can solve the problems of high catalyst cost, increased catalyst cost, unfavorable catalyst recovery, etc., achieve economical and environmental protection in the production process, and save post-processing costs , Excellent catalytic effect

Active Publication Date: 2017-11-24
CHINA UNIV OF PETROLEUM (BEIJING)
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0012] It can be seen that the catalysts used in the dehydrogenation and oxidation reactions of nitrogen-containing heterocyclic compounds are mostly limited to homogeneous noble metal catalysts such as iridium, palladium, etc., which are expensive and unfavorable for catalyst recovery; The efficiency is low, and it often depends on oxidizing agents such as hydrogen peroxide or tert-butanol peroxy, which is not ideal for the expansion of derivatives
[0013] For metal catalysts with high loads, only a very small number of metal active components play a catalytic role in the catalytic reaction process. In comparison, single-atom catalysis in which each metal atom acts as an active site is "one in ten" in terms of efficiency, while the traditional Metal utilization efficiencies of supported metal catalysts are far below ideal
Especially for noble metals, the use of large doses will undoubtedly increase the cost of the catalyst, which is not conducive to large-scale application in industrial production

Method used

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  • Monatomic iron nitrogen-doped porous carbon catalyst as well as preparation method and application thereof
  • Monatomic iron nitrogen-doped porous carbon catalyst as well as preparation method and application thereof
  • Monatomic iron nitrogen-doped porous carbon catalyst as well as preparation method and application thereof

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Effect test

Embodiment 1

[0064] This embodiment provides a method for preparing a monoatomic iron-nitrogen-doped porous carbon catalyst, which includes the following steps:

[0065] Preparation of porous sheet-like hexagonal magnesium oxide template:

[0066] Disperse magnesium oxide powder in deionized water, reflux and boil for 24 hours, dry overnight at 80°C, cool the dried product to room temperature, then heat up to 450°C at a rate of 10°C per minute and bake for 60 minutes to obtain a porous sheet-shaped hexagonal Shaped magnesium oxide template, its specific surface area is 200m 2 / g, the two-dimensional film size is about 300nm;

[0067] Preparation of monoatomic iron nitrogen doped porous carbon catalyst:

[0068] Stir and dissolve 300mg ferric chloride and 500mg 2,2'-bipyridine in ethanol at room temperature, then add 1g of the magnesium oxide template prepared above, stir for 12h, remove the solvent, and dry to obtain a precursor mixture (solid mixture) ;

[0069] The precursor mixture ...

Embodiment 2

[0072] This embodiment provides a method for preparing a monoatomic iron-nitrogen-doped porous carbon catalyst, which includes the following steps:

[0073] Preparation of porous sheet-like hexagonal magnesium oxide template:

[0074] Disperse magnesium oxide powder in deionized water, reflux and boil for 24 hours, dry overnight at 80°C, and then heat up to 450°C at a heating rate of 10°C per minute and bake for 60 minutes to obtain a porous sheet-shaped hexagonal magnesium oxide template. The specific surface area 200m 2 / g, the two-dimensional film size is about 300nm;

[0075] Preparation of monoatomic iron nitrogen doped porous carbon catalyst:

[0076] Stirring and dissolving 300 mg of ferric chloride and 500 mg of 2,2'-bipyridine in ethanol at room temperature, then adding 1 g of the magnesium oxide template prepared above, stirring for 12 h, removing the solvent, and drying to obtain a precursor mixture;

[0077] The precursor mixture was placed in a tube furnace and...

Embodiment 3

[0088] This embodiment provides a method for preparing a monoatomic iron-nitrogen-doped porous carbon catalyst, which includes the following steps:

[0089] Preparation of porous sheet-like hexagonal magnesium oxide template:

[0090] Disperse magnesium oxide powder in deionized water, reflux and boil for 24 hours, dry overnight at 80°C, and then heat up to 450°C at a heating rate of 10°C per minute and bake for 60 minutes to obtain a porous sheet-shaped hexagonal magnesium oxide template. The specific surface area 200m 2 / g, the two-dimensional film size is about 300nm;

[0091] Preparation of monoatomic iron nitrogen doped porous carbon catalyst:

[0092] Stirring and dissolving 300 mg of ferric chloride and 500 mg of 2,2'-bipyridine in ethanol at room temperature, then adding 1 g of the magnesium oxide template prepared above, stirring for 12 h, removing the solvent, and drying to obtain a precursor mixture;

[0093] The precursor mixture was placed in a tube furnace and...

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Abstract

The invention provides a monatomic iron nitrogen-doped porous carbon catalyst as well as a preparation method and application thereof. In the catalyst, monatomic iron is taken as an active component, a nitrogen-doped porous carbon material is taken as a carrier, and iron is dispersed on the surface and the interior of the nitrogen-doped porous carbon material in a monatomic form, wherein every 100 wt% of the monatomic iron nitrogen-doped porous carbon catalyst contains 1.0-3.0 wt% of iron and 4.0-9.0 wt% of nitrogen. The invention also provides a method for catalyzing a nitrogen heterocyclic compound with the monatomic iron nitrogen-doped porous carbon catalyst for a dehydrogenation oxidation reaction and application of the monatomic iron nitrogen-doped porous carbon catalyst for catalyzing the nitrogen heterocyclic compound for the dehydrogenation oxidation reaction. The catalyst has an excellent catalytic effect; a product is analyzed by GC-MS (gas chromatography-mass spectrometer) after a catalytic reaction is ended; and an analysis result indicates that no by-product is produced, and the activity of the catalyst is not obviously reduced after the catalyst is used for 5 times.

Description

technical field [0001] The invention relates to a single-atom iron-nitrogen-doped porous carbon catalyst and its preparation method and application, belonging to the technical field of single-atom catalysts. Background technique [0002] Nitrogen-containing heterocyclic compounds have a wide range of biological activities, and they also have the characteristics of low toxicity, high efficiency, environmental friendliness, and diverse structures; and the dehydrogenation and oxidation of nitrogen-containing heterocyclic compounds is one of the basic and important reaction types in the field of organic synthesis. First, this reaction can synthesize a variety of high value-added compounds; quinoline, as a typical representative of nitrogen-containing heterocyclic compounds, is a synthetic precursor for many biological and pharmaceutical molecules; and quinoline derivatives have multiple uses , such as 8-hydroxyquinoline can be used as a point-emitting material, 6-chloroquinoline...

Claims

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Application Information

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IPC IPC(8): B01J27/24C07D215/06C07D215/18C07D215/20C07D215/26C07D215/48C07D217/02
CPCB01J27/24C07D215/06C07D215/18C07D215/20C07D215/26C07D215/48C07D217/02
Inventor 杨帆邱天王敏键李永峰
Owner CHINA UNIV OF PETROLEUM (BEIJING)
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