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Atomic-scale iron active site catalyst as well as preparation method and application thereof

An active site, atomic-level technology, applied in the field of nanomaterials, can solve the problems of atomic agglomeration, reduce the catalytic activity of metal active sites, etc., to accelerate the mass transfer rate, improve the catalytic activity and cycle stability, and achieve high stability. Effect

Active Publication Date: 2020-08-25
NANTONG UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the extremely high surface free energy of metal single atoms can lead to atomic aggregation, which reduces the catalytic activity of metal active sites.

Method used

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  • Atomic-scale iron active site catalyst as well as preparation method and application thereof
  • Atomic-scale iron active site catalyst as well as preparation method and application thereof
  • Atomic-scale iron active site catalyst as well as preparation method and application thereof

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preparation example Construction

[0025] The present invention also provides a method for preparing the above-mentioned atomic-level iron active site catalyst, comprising the following steps:

[0026] 1) Add 1-butyl-2-methylimidazolium bromide to the dispersion of silver ferricyanide, add deionized water and centrifuge to separate the lower layer product and disperse it in deionized water to obtain ferricyanide dimethylimidazole ionic liquid;

[0027] 2) Disperse the polystyrene nanosphere suspension and the ferricyanide dimethylimidazolium ionic liquid obtained in step 1) into deionized water to obtain the first mixed solution, then add pyrrole monomer to obtain the second mixed solution, add Ammonium persulfate solution, react for 5-7 hours, and then wash and dry the product obtained from the reaction to obtain a core-shell structure precursor with evenly dispersed iron ions;

[0028] 3) In an ammonia atmosphere, heat the core-shell structure precursor obtained in step 2) to 750-850° C. for 1.5-2.5 hours of...

Embodiment 1

[0035] This embodiment provides an atomic-level iron active site catalyst, and the preparation method is as follows:

[0036] (1) Synthesis of iron-containing ionic liquid: 0.128g of 1-butyl-2-methylimidazolium bromide (28mmol) was slowly added to 50mL of silver ferricyanide (10mmol) dispersion with a concentration of 0.2mol / L under stirring , centrifuged 3 times with deionized water and got 0.5g of the lower layer product, redispersed into 10mL of deionized water; to obtain a concentration of 0.5g / mL ferricyanide dimethyl imidazolium ionic liquid (Fe-ILs);

[0037] (2) Constructing a core-shell structure precursor with uniformly dispersed iron ions: Fe-ILs (4mL, 0.5g mL -1 ) and polystyrene (PS) nanosphere suspension (2mL, 0.1g mL -1 ) was dispersed into 100mL deionized water under vigorous stirring, and the stirring was continued for 10 min to obtain the first mixed solution PS@Fe-ILs, 0.4 mL of pyrrole monomer (pyrrole) was added, and the stirring was continued for 10 min to...

Embodiment 2

[0041] This embodiment provides an atomic level iron active site catalyst (Fe-N x - the preparation method of HCS-18), according to step (1) in embodiment 1, prepare ferricyanogen dimethyl imidazolium ionic liquid (Fe-IL), then 0.4mL pyrrole monomer in embodiment 1 step (2) Change to 0.6mL pyrrole monomer, then prepare Fe-N according to embodiment 1 step (3) x - HCS-18 (the number 18 indicates that the hollow carbon nanospheres have an average carbon shell thickness of 18 nm).

[0042] The content of iron active sites in the catalyst of this example was measured by an inductively coupled plasma mass spectrometer to be 1.6%.

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Abstract

The invention belongs to the field of nano materials, and discloses an atomic-scale iron active site catalyst as well as a preparation method and application thereof. The preparation method provided by the invention comprises the following steps: 1) preparing ferricyanide dimethylimidazole ionic liquid; 2) constructing a core-shell structure precursor with uniformly dispersed iron ions; and 3) preparing the atomic-scale iron active site catalyst. The atomic-scale iron active site catalyst obtained by the preparation method disclosed by the invention is microporous nanospheres loaded with atomic-scale iron active sites comprising Fe-N4 ligands and Fe3 clusters. The catalyst is low in density, high in stability and resistant to acid and alkali corrosion; porous properties are also exhibited;the reaction activation energy can be greatly reduced, the electron / ion transfer and the mass transfer rate of an intermediate product are accelerated, and thus, the catalytic activity and the cycling stability of the catalyst are improved, and the maximum atom utilization rate (100%) is realized; and the catalyst is suitable for being used as a catalyst material for electrocatalytic oxygen reduction (ORR) and oxygen evolution (OER) reactions in fuel cells and metal-air cells.

Description

technical field [0001] The invention belongs to the field of nanometer materials, and in particular relates to an atomic-level iron active site catalyst and its preparation method and application. Background technique [0002] Fuel cells and metal-air batteries are based on the positive side O 2 Two important types of electrochemical energy storage and conversion devices that convert chemical energy into electrical energy are characterized by reduction reaction (ORR) and precipitation reaction (OER). The large-scale applications of fuel cells and metal-air batteries face great challenges due to the limitations of the positive-side ORR and OER hysteresis kinetics (high overpotential) and electrode polarization. Both ORR and OER belong to multiple electron transfer reactions, involving the breaking and rearrangement of chemical bonds, and the reactions are mostly carried out in corrosive or oxidizing environments. In order to promote the rapid progress of the electrode react...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/90H01M4/88
CPCH01M4/9041H01M4/9083H01M4/8825Y02E60/50
Inventor 李奇
Owner NANTONG UNIVERSITY
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