Preparation of Covalently Supported Biomimetic Multinuclear Copper Oxygen Reduction Electrocatalysts on Carbon Materials

An electrocatalyst and multi-core copper technology, applied in the direction of circuits, electrical components, battery electrodes, etc., can solve the problems of poor stability, long-distance targets, and inability to control catalyst reactivity, etc., to increase oxygen flux, improve activity, and catalyst structure. control effect

Active Publication Date: 2018-12-14
EAST CHINA UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, since the preparation of non-noble metal ORR catalysts mostly adopts a trial-and-error method, the preparation process often requires high-temperature treatment. This heat treatment process causes the cracking of the molecular structure of the precursor, making it impossible for researchers to adjust the reaction of the catalyst by changing the catalyst structure. active
In addition, most of the currently reported copper-containing ORR electrocatalysts have relatively low catalytic activity and poor stability in alkaline environments, and are still far from the goal of commercial application.

Method used

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  • Preparation of Covalently Supported Biomimetic Multinuclear Copper Oxygen Reduction Electrocatalysts on Carbon Materials
  • Preparation of Covalently Supported Biomimetic Multinuclear Copper Oxygen Reduction Electrocatalysts on Carbon Materials
  • Preparation of Covalently Supported Biomimetic Multinuclear Copper Oxygen Reduction Electrocatalysts on Carbon Materials

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0039] Example 1 Functional modification of triazole groups on the surface of graphene oxide

[0040] Dissolve purified graphene oxide (SP-1graphite, purchased from Bay Carbon Corporation) and triisopropylsilylpyridine in acetonitrile and disperse uniformly by ultrasonic, add a certain amount of isoamyl nitrite solution, heat to 80°C, Under the protection of nitrogen, the reaction was carried out for 24h. The resulting filter cake was filtered, washed with DMF until the filtrate was colorless, and then dispersed in DMF.

[0041] Take a certain amount of the dispersion obtained in the above steps, add tetrabutylammonium fluoride under an ice-water bath, and react for 4 hours at room temperature under a nitrogen atmosphere. Then, a certain amount of copper sulfate pentahydrate, sodium ascorbate and 2-azidopyridine were respectively added therein, and reacted at 50° C. for 36 h under a nitrogen atmosphere. Filter the obtained filter cake, wash with DMF, 50mmol / L EDTA aqueous so...

Embodiment 2

[0042] Example 2 Coordination loading of copper salt on the surface of reduced graphene oxide

[0043] Mix 10.0mg modified reduced graphene oxide with 20.0mg CuCl 2 2H 2 O was dispersed in 20.0 mL of acetonitrile and stirred at room temperature for 24 h. The complex was filtered, washed three times with a small amount of acetonitrile and water, dried in vacuum for 4 h, and the target compound obtained in the above steps was stored in a dark place under a nitrogen atmosphere.

Embodiment 3

[0044] Example 3 Preparation of rGO+TAPyCu

[0045] Preparation of TAPyCu

[0046] Dissolve a certain amount of 2-azidopyridine and 2-ethynylpyridine in DMF, add a certain amount of copper sulfate pentahydrate and sodium ascorbate, heat to 80°C, and react for 36 hours under nitrogen protection. After treatment, wash with a large amount of water to remove DMF, extract with dichloromethane to obtain an organic phase, and obtain the target product TAPy by column chromatography. A certain amount of TAPy and CuCl 2 2H 2 O was dispersed in acetonitrile, and after stirring at room temperature for 24 h, the post-treatment was washed with acetonitrile for several times until the filtrate was colorless, and the target product TAPyCu was obtained.

[0047] Preparation of rGO+TAPyCu

[0048] Take a certain amount of TAPyCu and rGO and disperse them in acetonitrile, stir at room temperature for 16 hours, filter and dry to obtain the target product rGO+TAPyCu.

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Abstract

The invention provides a method for preparing a bionic electrocatalyst by modifying covalent bonds to the surface of a carbon-based material through a multi-core copper catalytic active center of simulated laccase. The complex system prepared by the technology refers to a high-efficiency simulated laccase multi-core copper catalytic active center and can be used for catalyzing an oxygen molecule reduction reaction, and the catalyst serves as an oxygen molecule reduction electrocatalyst and is high in catalytic activity and high in stability. Under alkaline conditions, the stability of the prepared catalyst far exceeds that of a Pt / C catalyst, and the methanol crossover resistance is excellent. The research proves that a multi-core copper complex is modified onto the carbon-based material by utilizing the covalent bonds, the method is expected to become an effective method for preparing a high-efficiency base metal oxygen reduction electrocatalyst, and the electrocatalyst has huge potential application prospects and commercial values in the field of alkaline fuel cell electric automobiles and the like.

Description

technical field [0001] The invention relates to the field of non-precious metal catalysts for fuel cells. Specifically, the invention describes a preparation method of a multi-nuclear copper biomimetic electrocatalyst that simulates laccase multi-nuclear copper catalytic active centers and covalently supports the surface of carbon-based materials. Background technique [0002] A fuel cell is a high-efficiency continuous power generation device that directly converts the chemical energy of fuel and oxidant into electrical energy by electrochemical reaction without combustion. It is a renewable and environmentally friendly new energy source that can be used to replace coal, Traditional energy sources such as oil and natural gas. Therefore, when the fuel cell is in use, it is neither like a primary battery that consumes active materials and must be discarded, nor does it need to be regularly charged like a secondary battery. Theoretically speaking, as long as fuel is continuou...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): H01M4/88
CPCH01M4/88Y02E60/50
Inventor 刘劲刚奚月婷王茹春韦萍洁
Owner EAST CHINA UNIV OF SCI & TECH
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