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Monatomic catalyst and application thereof

A catalyst and atom technology, applied in single-atom catalysts and their application fields, can solve the problems of low overall structural stability, loss, and small disorder of metal sites.

Pending Publication Date: 2021-01-01
SUZHOU ADVANCED MATERIALS CO LTD
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, these MOF-derived metal single-atom catalysts usually show a single metal site supported on the MOF-derived carbon-based support. Under certain harsh reaction conditions, the metal site may still be leached and lost, indicating that the structure of the system Stability needs to be further improved
From the perspective of the second law of thermodynamics, the chaos of the metal sites in the MOF-derived single metal site catalyst system is small, and the entropy value is not high, so the stability of the overall structure is not high.

Method used

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  • Monatomic catalyst and application thereof
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Examples

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preparation example Construction

[0053] The single-atom catalyst of the embodiment of the present invention is a type of crystalline porous material with a periodic network structure formed by connecting a transition metal salt and a nitrogen-containing organic ligand through self-assembly. The preparation method includes the following steps:

[0054] S1, dissolving nitrogen-containing organic ligands and transition metal salts in an organic solvent to form a solution;

[0055] Wherein, the nitrogen-containing organic ligand is selected from heterocyclic compounds whose heteroatoms are nitrogen atoms, and the transition metal salt is selected from the soluble compounds of at least 5 elements in chromium, manganese, iron (II), cobalt, nickel, copper, zinc, and cadmium. Salt;

[0056] S2. The solution is stirred, refluxed, centrifuged, washed and dried to obtain a solid powder, that is, a multi-component MOF precursor; preferably, the particle size of the multi-component MOF precursor is 100-500 nm, preferably ...

Embodiment 1

[0074] A single-atom catalyst is a nitrogen-doped carbon skeleton loaded with Zn, Cu, Ni, Co, Fe.

[0075] Concrete preparation method is:

[0076] 1. Mix 3.4g Zn(NO 3 ) 2 ·6H 2 O, 120mg Cu(NO 3 ) 2 ·3H 2 O, 145mg Ni(NO 3 ) 2 ·6H 2 O, 30mg Co(NO 3 ) 2 ·6H 2 O and 144mg Fe(NO 3 ) 2 ·6H 2 O was dissolved in 150mL methanol, stirred and mixed evenly;

[0077] 2. Dissolve 3.94g of dimethylimidazole in another portion of 150mL of methanol, stir and mix evenly;

[0078] 3. Mix the above two parts of methanol solution evenly, heat to reflux, and make it fully react; centrifuge, wash and dry the mixed solution to obtain a solid powder, which is the multi-element MOF precursor (referred to as ZnCuNiCoFe-ZIF);

[0079] 4. After heat-treating the above solid powder in an inert gas atmosphere, prepare a nitrogen-doped carbon material loaded with five single-atom sites such as ZnCuNiCoFe, (denoted as (Zn 1 Cu 1 Ni 1 co 1 Fe 1 ) / NC).

[0080] Zn will be prepared 1 Cu ...

Embodiment 2

[0090] A single-atom catalyst is a nitrogen-doped carbon skeleton loaded with Zn, Cu, Ni, Co, and Mn.

[0091] Concrete preparation method is:

[0092] 1. Mix 3.4g Zn(NO 3 ) 2 ·6H 2 O, 120mg Cu(NO 3 ) 2 ·3H 2 O, 145mg Ni(NO 3 ) 2 ·6H 2 O, 30mg Co(NO 3 ) 2 ·6H 2 O and 125mg Mn(NO 3 ) 2 4H 2 O was dissolved in 150mL methanol, stirred and mixed evenly;

[0093] 2. Dissolve 3.94g of dimethylimidazole in another portion of 150mL of methanol, stir and mix evenly;

[0094] 3. Mix the above two methanol solutions evenly, heat to reflux, and make them fully react; centrifuge, wash, and dry the mixed solution to obtain a solid powder that is the multi-element MOF precursor (referred to as ZnCuNiCoMn-ZIF);

[0095] 4. Prepare the nitrogen-doped carbon material (denoted as (Zn 1 Cu 1 Ni 1 co 1 mn 1 ) / NC).

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Abstract

The invention relates to the technical field of catalyst preparation, in particular to a monatomic catalyst and application thereof. The monatomic catalyst is a nitrogen-doped carbon skeleton loaded with metal atoms, wherein the metal atoms comprise at least five of chromium atoms, manganese atoms, iron atoms, cobalt atoms, nickel atoms, copper atoms, zinc atoms and cadmium atoms; a nitrogen-dopedcarbon skeleton is composed of carbon atoms and nitrogen atoms. The at least five monatomic sites are disorderly distributed on the MOF-derived nitrogen-doped carbon skeleton, so that the disorder degree of the system is increased, and the entropy of the system is increased From the perspective of thermodynamics, the high-entropy monatomic catalyst provided by the invention is more beneficial toimproving the overall structural stability of the system.

Description

technical field [0001] The invention relates to the technical field of catalyst preparation, in particular to a single-atom catalyst and its application. Background technique [0002] Metal single-atom catalysts refer to catalysts in which metals are uniformly dispersed on the support at the atomic level and have excellent catalytic performance. Due to the characteristics of high atom utilization, highly unsaturated metal site coordination, and strong interaction between the metal site and the support, metal single-atom catalysts usually exhibit ultra-high catalytic activity and selectivity, and have become the current scientific research. One of the important research hotspots in the world and industry. [0003] Metal-organic framework (MOF) materials provide a powerful synthetic platform for the preparation of metal single-atom catalysts due to their intrinsic physical and chemical properties such as the ordered distribution of metal nodes and the well-defined coordinatio...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J35/00B01J37/08C25B1/04
CPCB01J27/24B01J37/086C25B1/04B01J35/391B01J35/33Y02E60/36
Inventor 邢立文高鸿毅其他发明人请求不公开姓名
Owner SUZHOU ADVANCED MATERIALS CO LTD
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