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A spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst and its preparation method and use

A carbon-supported cobalt-based, nitrogen-doped technology, applied in electrical components, battery electrodes, circuits, etc., can solve the problems of low methanol oxidation catalytic performance, high cost and low life of platinum-based catalysts, and achieve excellent stability and resistance The effect of methanol performance, good ORR catalytic activity, and high degree of graphitization

Active Publication Date: 2019-01-11
XIANGTAN UNIV
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Problems solved by technology

[0004] However, its short life, low efficiency and high cost limit its large-scale commercial application
The main reason is the high cost of platinum-based catalysts and their low catalytic performance for methanol oxidation

Method used

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  • A spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst and its preparation method and use
  • A spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst and its preparation method and use
  • A spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst and its preparation method and use

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Embodiment approach

[0046] According to the first embodiment provided by the present invention, a spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst is provided.

[0047] A spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst is prepared by the following preparation method: first synthesize 3,6-bis(3,5-dimethylpyrazole)-1,2 through guanidine nitrate, 4,5-tetrazine (BT), then add imidazole to 3,6-bis(3,5-dimethylpyrazole)-1,2,4,5-tetrazine (BT) to synthesize 3,6- Bis(imidazolyl)-1,2,4,5-tetrazine (DT) ligand, followed by 3,6-bis(imidazolyl)-1,2,4,5-tetrazine (DT) with transition metal Cobalt ions are coordinated to form a cobalt-based zeolite imidazolate framework coordination polymer (CoDT-ZIF), and then the spherical nitrogen-doped carbon-supported cobalt is prepared by high-temperature pyrolysis of the cobalt-based zeolite imidazolate framework coordination polymer (CoDT-ZIF) based (Co-N / C) oxygen reduction catalysts.

[0048] In the p...

Embodiment 1

[0070] A preparation method of a spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst, the method comprising the following steps:

[0071] (1) Preparation of 3,6-bis(3,5-dimethylpyrazole)-1,2,4,5-tetrazine (BT): 3,6-bis(3,5 -Dimethylpyrazole)-1,2,4,5-tetrazine (BT);

[0072] (2) Preparation of 3,6-bis(imidazolyl)-1,2,4,5-tetrazine (DT) ligand: 3,6-bis(3,5-dimethylpyrazole)-1 , 2,4,5-tetrazine (BT) is loaded into the reactor, imidazole is added, heated for a period of time, cooled, filtered, and dried to obtain 3,6-bis(imidazolyl)-1,2,4, 5-tetrazine (DT) ligand;

[0073] (3) Preparation of cobalt-based zeolite imidazolate framework coordination polymer (CoDT-ZIF): 3,6-di(imidazolyl)-1,2,4,5-tetrazine (DT) ligand was dissolved in organic Add cobalt nitrate hexahydrate to the solvent, heat and react for a period of time after dispersion, filter with suction after cooling, and wash to obtain a brown solid, which is the cobalt-based zeolite imidazolat...

Embodiment 2

[0076] Preparation of 3,6-bis(3,5-dimethylpyrazole)-1,2,4,5-tetrazine (BT):

[0077] Dissolve 6.11g of guanidine nitrate in 50ml of dioxane solution, add 6.26g of hydrazine hydrate, heat to 110°C, and reflux for 4h, filter to obtain a white solid, then dissolve the white solid in water, add 15.02g of Acetylacetone, heated to 70°C for 4 hours, filtered, washed with water and dried to obtain 3,6-bis(3,5-dimethylpyrazole)-1,2,4,5-tetrazine (BT) .

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Abstract

The invention provides a spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst, which is prepared by the following preparation methods: firstly, synthesizing 3, 6-dimethyl-3-nitroguanidine by guanidine nitrate; secondly, synthesizing 3, 6-dimethyl-3-nitroguanidine by guanidine nitrate; finally, synthesizing 3, 6-dimethyl-3-nitroguanidine by guanidine nitrate. Bis (3, 5-dimethylpyrazole)-1, 2, 4, 5-Tetrazine (BT), and 3, 6-Bis (3, 5-dimethylpyrazole)-1, 2, 4, 5-Imidazole is added into tetrazine (BT) to synthesize 3, 6-Bis (imidazolyl)-1, 2, 4, 5-Tetrazine (DT) ligand,and then 3, 6-Bis (imidazolyl)-1, 2, 4, 5-Tetrazine (DT) coordinated with transition metal cobalt ion to form cobalt-based zeolite imidazolium ester framework coordination polymer (CoDT ZIF), and then pyrolyzed cobalt-based zeolite imidazolium ester framework coordination polymer (CoDT ZIF) to prepare spherical nitrogen doped carbon supported cobalt (Co N / C) oxygen reduction catalyst. The preparation method of the catalyst is simple, the cost is low, and the catalyst has extremely rich active sites, which is conducive to promote the practical application of fuel cells.

Description

technical field [0001] The invention relates to an oxygen reduction catalyst, in particular to a spherical nitrogen-doped carbon-supported cobalt-based oxygen reduction catalyst and its preparation method and application, belonging to the field of fuel cell science and technology. Background technique [0002] The widespread use of fossil energy, such as oil, natural gas and coal, has promoted the rapid development of human society, but the non-renewability of fossil energy and the environmental problems caused by the use of fossil energy are two major problems facing human beings. The development of environmentally friendly and renewable new energy sources and new energy technologies has become the most important research hotspot in the world today. [0003] A fuel cell is a power generation device that directly converts the chemical energy in the fuel into electrical energy through the oxidation-reduction reaction between the fuel and the oxidant. It is a new generation of...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/90
CPCH01M4/9041H01M4/9083Y02E60/50
Inventor 陈红飙白亚峰杨端光阳梅黎华明
Owner XIANGTAN UNIV
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