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Monatomic catalyst, preparation method and application thereof

A catalyst and atom technology, applied in the field of organic compound catalytic synthesis, can solve problems such as low dispersion, and achieve the effects of high selectivity, easy separation and high activity

Pending Publication Date: 2021-05-11
北京氦舶科技有限责任公司
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] Single-atom catalysts have high activity and high selectivity, and are expected to be used in the selective oxidation of ethylbenzene to acetophenone, but there is a problem of low dispersion

Method used

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  • Monatomic catalyst, preparation method and application thereof

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preparation example Construction

[0035] The preparation method of single atom catalyst of the present invention, comprises the steps:

[0036] (1) Add the MOFs material containing amino functional groups to an organic solvent, mix evenly, add an organic ligand and stir for reaction, the organic ligand contains carbon groups; the product after the reaction is washed and dried to obtain a mat-containing MOFs materials with alkali functional groups;

[0037] (2) Add the MOFs material containing the Schiff base functional group into the organic solvent, mix well, slowly add the transition metal precursor and continue to stir the reaction; wash and dry the reacted product, then pyrolyze at high temperature, pickle and dry , to obtain single-atom catalysts.

[0038] In the present invention, MOFs materials containing amino functional groups and organic ligands containing carbonyl and active nitrogen are used to form a mixed solution, and amino groups in MOFs materials are used to react with carbonyl groups in orga...

Embodiment 1

[0061] Take 1g of UiO66-NH2 and add it to 50mL of methanol, mix well, add 0.05g of pyridine-2-carboxaldehyde, stir and react at 20°C for 6h; wash the reacted product with deionized water, and dry at 50°C for 24h to obtain Schiff base-containing MOFs materials with functional groups; add MOFs materials containing Schiff base functional groups to 50mL methanol, mix well, slowly add 10mL 4g / L methanol solution of manganese acetate, stir and react at 20°C for 6h; wash the reacted product with deionized water After washing and drying at 50°C for 24 hours, it was pyrolyzed at 600°C for 1 hour, then washed with 0.5 mol / L sulfuric acid, and finally dried at 50°C for 24 hours to obtain a single-atom catalyst.

Embodiment 2

[0063] Take 1g of UiO66-NH2 and add it to 50mL of ethanol, mix well, add 0.1g of 2-dipyridyl ketone, stir and react at 30°C for 24h; wash the reacted product with deionized water and dry at 100°C for 12h to obtain the Schiff-containing MOFs materials with alkali functional groups; add MOFs materials containing Schiff base functional groups to 50mL ethanol, mix well, slowly add 10mL 100g / L ethanol solution of cobalt acetate, stir and react at 30°C for 24h; After washing with water and drying at 100°C for 12 hours, it was pyrolyzed at 800°C for 5 hours, then washed with 5 mol / L sulfuric acid, and finally dried at 100°C for 12 hours to obtain a single-atom catalyst.

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Abstract

The invention particularly relates to a monatomic catalyst, a preparation method and application thereof. The monatomic catalyst is prepared by the following steps of: (1) preparing an MOFs material containing a Schiff base functional group; and (2) combining the MOFs material containing the Schiff base functional group with a transition metal precursor through a coordinate bond, and then carrying out reduction to prepare the monatomic catalyst. According to the prepared catalyst, the transition metal is uniformly dispersed on the carrier in an atomic form, the catalyst is applied to direct oxidation of aromatic hydrocarbon and oxygen to generate arone, the catalyst has the characteristics of high selectivity and high activity, the catalytic activity of the catalyst is basically unchanged after repeated recycling, and the active metal is basically not lost along with the reaction and recycling.

Description

technical field [0001] The invention belongs to the technical field of catalytic synthesis of organic matter, and in particular relates to a single-atom catalyst and its preparation method and its application in the reaction of aromatic ketones produced by direct oxidation of aromatic hydrocarbons and oxygen. Background technique [0002] The reaction of the side chain methylene oxidation of ethylbenzene and its derivatives to prepare aromatic ketones has broad application prospects, and is of great importance to the development of petrochemical downstream products, the development of fine chemicals, and the theoretical research on the selective oxidation of saturated carbon-hydrogen bonds. meaning. Aromatic ketones are raw materials for the synthesis of fine chemicals such as dyes, spices and medicines, and are mainly produced through Friedel-Crafts acylation in industry. However, in the Friedel-Crafts reaction, the catalyst AlCl3 produces a large amount of acidic wastewat...

Claims

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Application Information

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IPC IPC(8): B01J23/34B01J23/75C07C45/36C07C49/78
CPCB01J23/34B01J23/75C07C45/36C07C49/78Y02P20/584
Inventor 郭文雅关超阳郎嘉良赵刚黄翟
Owner 北京氦舶科技有限责任公司
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