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A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst and a preparation method and use thereof

A nitrogen-doped carbon and catalyst technology, applied in electrical components, battery electrodes, circuits, etc., can solve the problems of slow electrode reaction rate, scarce reserves, expensive precious metal Pt, etc., and achieves short synthesis cycle, simple preparation method and cost. low cost effect

Active Publication Date: 2018-12-18
XIANGTAN UNIV
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Problems solved by technology

The low reaction temperature causes the reaction rate of the fuel cell electrode to be slow, so Pt nanoparticles with high catalytic activity must be used as the cathode and anode electrocatalysts, especially the cathode oxygen reduction reaction (Oxygen reduction reaction, ORR) rate is much lower than that of the anode fuel oxidation reaction. Therefore, a catalyst much higher than that of the anode is required to accelerate its oxygen reduction reaction process. The precious metal Pt is not only expensive, but also has scarce reserves in nature. The Pt / C catalyst used in the existing technology accounts for 55% of the entire battery cost.

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  • A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst and a preparation method and use thereof
  • A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst and a preparation method and use thereof
  • A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst and a preparation method and use thereof

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Embodiment approach

[0045] According to the first embodiment provided by the present invention, a nitrogen-doped carbon-supported iron-based oxygen reduction catalyst is provided.

[0046] A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst, which is prepared by the following preparation method: first synthesize 3,6-bis(3,5-dimethylpyrazole)-1,2,4 by guanidine nitrate ,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, and then 3,6-bis(imidazolyl)-1,2,4,5-tetrazine (DT) with transition metal iron Iron-based zeolite imidazolate framework coordination polymer (FeDT-ZIF) was formed by ion coordination, and nitrogen-doped carbon-supported iron-based (Fe- N / C) Oxygen reduction catalyst.

[0047] In the present invention, the transition metal iron ions are from metal iron salts.

[0048] Preferably, the metal iron salt is one or more of ferrous sulfate heptahydrate, ferrous ...

Embodiment 1

[0069] A method for preparing a nitrogen-doped carbon-supported iron-based oxygen reduction catalyst or a method for preparing a nitrogen-doped carbon-supported iron-based oxygen reduction catalyst described in the first embodiment, the method comprising the following steps:

[0070] (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);

[0071] (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;

[0072] (3) Preparation of iron-based zeolite imidazolate framework coordination polymer (FeDT-ZIF): 3,6-bis(imidazolyl)-1,2,4,5-tetrazine (DT) ligand was dissolved in organic Add ferrous sulfate heptahydrate to the solvent, heat and react for a period of time after disper...

Embodiment 2

[0075] Preparation of 3,6-bis(3,5-dimethylpyrazole)-1,2,4,5-tetrazine (BT):

[0076] 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

A nitrogen-doped carbon-supported iron-based oxygen reduction catalyst is prepared by synthesizing 3, 6-dichloroethane by guanidine nitrate, adding nitric acid to form 3, 6-dichloroethane, adding nitric acid to form 3, 6-dichloroethane, adding nitric acid to form 3, 6-dichloroethane, and adding nitric acid to form 3, 6-dichloroethane. Bis (3, 5-dimethylpyrazole)-1, 2, 4, 5-Tetrazine (BT), and 3, 6-Bis (3, 5-dimethylpyrazole)-1, 2, 4, 5-Imidazole was added into tetrazine (BT) to synthesize 3, 6-Bis (imidazolyl)-1, 2, 4, 5Tetrazine (DT) ligand, and then 3, 6-Bis (imidazolyl)-1, 2, 4, 5-Tetrazine(DT) coordinated with transition metal iron ions to form iron-based zeolite imidazolium ester framework coordination polymer (FeDT ZIF), and then pyrolyzed iron-based zeolite imidazolium ester framework coordination polymer (FeDT ZIF) to prepare nitrogen doped carbon supported iron (Fe 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 nitrogen-doped carbon-supported iron-based oxygen reduction catalyst and its preparation method and application, belonging to the field of fuel cell science and technology. Background technique [0002] Energy crisis and environmental pollution are two major problems that people must face at present. The application of fossil energy has played an important role in the development of human society for a long time. But along with the application of fossil energy, there are increasingly serious environmental pollution and energy shortage. Research and development of other renewable and clean energy sources has become an important task facing mankind. 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 power generati...

Claims

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Application Information

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IPC IPC(8): H01M4/90
CPCH01M4/9008H01M4/9083Y02E60/50
Inventor 杨端光白亚峰陈红飙阳梅黎华明
Owner XIANGTAN UNIV
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