Preparation method of metal monatomic catalyst, metal monatomic catalyst and application

A catalyst and metal technology, applied in catalyst activation/preparation, preparation of organic compounds, preparation of amino compounds, etc., can solve the problems of metal single-atom catalysts, such as poor dispersion and high thermal stability, high preparation cost, and poor universality. Good application prospects, precise and controllable preparation, and the effect of improving stability

Active Publication Date: 2021-06-18
CHINA UNIV OF PETROLEUM (EAST CHINA)
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] The first object of the present invention is to provide a method for preparing a metal single-atom catalyst to alleviate the problems of poor universality, high preparation cost and poor dispersion and high thermal stability of the existing preparation method. technical problem;

Method used

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  • Preparation method of metal monatomic catalyst, metal monatomic catalyst and application
  • Preparation method of metal monatomic catalyst, metal monatomic catalyst and application
  • Preparation method of metal monatomic catalyst, metal monatomic catalyst and application

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preparation example Construction

[0054] According to a first aspect of the present invention, a method for preparing a metal single-atom catalyst is provided, comprising the following steps:

[0055] (a) providing a hydroxylation template;

[0056] Mixing the hydroxylated template, coupling agent and solvent A, reacting and separating to obtain the first template with surface functionalization;

[0057] (b) mixing and separating the first template, the metal precursor and the solvent B to obtain a second template with the metal precursor loaded on the surface;

[0058] (c) mixing the second template with a carbon source, calcining under a protective atmosphere, and detemplating the obtained calcined material to obtain a metal single-atom catalyst; wherein, the carbon source has a penetration of 30-160 / 0.1mm.

[0059] Specifically, in step (a), the hydroxylated template is modified with a coupling agent, and the coupling agent is grafted onto the hydroxylated template to form a surface-functionalized first te...

Embodiment approach

[0068] As an optional embodiment of the present invention, in step (a), the preparation method of the hydroxylated template comprises the following steps:

[0069] The template, basic reagent and solvent C are mixed and separated to obtain the hydroxylated template.

[0070] As a morphology regulator, the template can regulate the morphology of metal single-atom catalysts. The template can be removed by high-temperature pyrolysis or acid-base washing in the later stage.

[0071] Treating the surface of the template with an alkaline reagent can increase the hydroxyl density on the surface of the template, which is conducive to grafting more coupling agents, thereby effectively increasing the loading of metal single atoms (metal precursors). The hydroxyl content on the surface of the hydroxylated template can be flexibly adjusted by the amount of basic reagent used.

[0072] As an optional embodiment of the present invention, the template includes metal oxide and / or metal hydr...

Embodiment 1

[0117] This embodiment provides a method for preparing a Co-N-C metal single-atom catalyst, comprising the following steps:

[0118] (a) Provide hydroxylated template: Ultrasonic disperse 5.61g of alkaline reagent (sodium hydroxide) in 200mL of absolute ethanol, add 2g of template (flaky magnesium oxide), ultrasonically disperse for 1h, then stir at 25°C for 6h, The precipitate was filtered and washed with absolute ethanol, and freeze-dried at minus 55°C for 24 hours to obtain a hydroxylated template (hydroxylated magnesium oxide);

[0119] Disperse 1.0g of hydroxylated template in 200mL of solvent A (absolute ethanol), ultrasonically disperse for 1h, slowly add 0.5mL of coupling agent (3-aminopropyltriethoxysilane) dropwise, and vigorously stir the reaction at 60°C 6h, the precipitate was filtered and washed with absolute ethanol, and freeze-dried for 24h to obtain the surface functionalized first template (surface aminated magnesium oxide);

[0120] (b) Weigh 1.0 g of the f...

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Abstract

The invention provides a preparation method of a metal monatomic catalyst, the metal monatomic catalyst and application, which relate to the technical field of catalysts. The preparation method comprises the following steps of firstly, grafting a coupling agent onto a hydroxylation template to form a surface-functionalized first template, and anchoring a metal precursor on the surface of the first template in a monodisperse manner through interaction between functional groups carried by the coupling agent and metal atoms so as to form a second template of which the surface is loaded with the metal precursor, performing physical coating isolation on the metal precursor on the surface of the second template by using a carbon source, and then performing template removal to obtain a metal monatomic catalyst. The preparation method is based on a strategy of combining chemical confinement (dispersion anchoring) and physical confinement (coating isolation) effects, uniform spatial isolation and atomic-scale dispersion of a metal precursor are realized, migration and agglomeration of metal in a calcination (pyrolysis) process are effectively inhibited, and the purpose of precise and controllable preparation of a metal monatomic catalyst is achieved.

Description

technical field [0001] The invention relates to the technical field of catalysts, in particular to a preparation method of a metal single-atom catalyst, a metal single-atom catalyst and applications. Background technique [0002] Single-atom catalysts refer to catalysts with excellent catalytic performance formed by metals uniformly dispersed on the carrier in the form of single atoms. Compared with traditional supported catalysts, single-atom catalysts have the advantages of high activity and good selectivity. Since the metal active components are reduced to the atomic scale, the highest atom utilization can be achieved in the reaction. Therefore, single-atom catalysts have broad application prospects in oxidation reactions, hydrogenation reactions, water-gas shift, photocatalytic hydrogen production, and electrochemical catalysis. [0003] Due to the large specific surface energy of single atoms, it is easy to migrate and agglomerate, so it is difficult to prepare single-...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J27/043B01J27/14B01J37/03B01J37/32B01J37/34B01J37/00B01J37/08C07C209/32
CPCB01J27/24B01J27/043B01J27/14B01J37/031B01J37/32B01J37/343B01J37/0018C07C209/325
Inventor 赵青山曹风亮吴明铂倪万鑫李义文李忠涛宁汇
Owner CHINA UNIV OF PETROLEUM (EAST CHINA)
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