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Tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and preparation method and application thereof

A nitrogen-doped carbon and catalyst technology, applied in electrical components, battery electrodes, circuits, etc., can solve problems such as low specific surface area and low ORR catalytic activity

Inactive Publication Date: 2018-11-06
XIANGTAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the catalyst prepared by this method has low ORR catalytic activity due to the low specific surface area, and the use of porous organic polymer (POP) as a single precursor to prepare N / C catalysts came into being.

Method used

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  • Tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and preparation method and application thereof
  • Tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and preparation method and application thereof
  • Tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and preparation method and application thereof

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Effect test

Embodiment 1

[0066] A nitrogen-doped carbon-oxygen reduction catalyst based on tetrazine ring polycarbazole, which is prepared by the following preparation method: first, 3,6-bis(3,5-dimethylpyrazole)-1,2 , 4,5-tetrazine prepared 3,6-bis(carbazolyl)-1,2,4,5-tetrazine (TCy) monomer by substitution reaction, and then 3,6-bis(carbazolyl) -1,2,4,5-Tetrazine (TCy) is obtained by Friedel-Crafts alkylation reaction to obtain tetrazine ring polycarbazole; then tetrazine ring polycarbazole is pyrolyzed to obtain tetrazine ring polycarbazole Nitrogen-doped carbon-oxygen reduction catalysts.

Embodiment 2

[0068]A nitrogen-doped carbon-oxygen reduction catalyst based on tetrazine ring polycarbazole, which is prepared by the following preparation method: first, 3,6-bis(3,5-dimethylpyrazole)-1,2 , 4,5-tetrazine prepared 3,6-bis(carbazolyl)-1,2,4,5-tetrazine (TCy) monomer by substitution reaction, and then 3,6-bis(carbazolyl) -1,2,4,5-tetrazine (TCy) can be obtained tetrazine ring polycarbazole through oxidative coupling reaction; then tetrazine ring polycarbazole is pyrolyzed to obtain tetrazine ring polycarbazole-based nitrogen-doped Heterocarbon oxygen reduction catalyst.

Embodiment 3

[0070] A method for preparing a nitrogen-doped carbon-oxygen reduction catalyst based on tetrazine ring polycarbazole, comprising the following steps:

[0071] (1) Preparation of 3,6-bis(carbazolyl)-1,2,4,5-tetrazine (TCy): add 10mmol 3,6-bis(3,5-dimethylpyrazole) -1,2,4,5-tetrazine suspension in acetonitrile was added to the flask with 22mmol carbazole salt (preparation method: carbazole was added KOH at 0°C, stirred for 5h), stirred at room temperature for one hour, refluxed for 8h; cooled to At room temperature, filter, wash with acetonitrile and dry, and finally pass through the column with petroleum ether / chloroform; figure 2 is the composite map of TCy, image 3 is the NMR map of TCy;

[0072] (2) Synthesis based on 1,2,4,5-tetrazine ring polycarbazole hypercrosslinked polymer network (PTCy-1): add 40mmol dimethoxymethane to the nitrobenzene solution system of 10mmolTCy, stir 30min, then 40mmol FeCl 3 Added to the reaction system, and reacted at 45°C for 5h, and rea...

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Abstract

The invention discloses a tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and a preparation method thereof. The method comprises the steps of firstly synthesizing 3,6-bis(carbazolyl)-1,2,4,5-tetrazine (TCy) through a simple method; synthesizing a novel super-crosslinked polymer tetrazine ring polycarbazole (PTCy-1 or PTCy-2) by taking TCy as a monomer through Friedel-Crafts alkylation reaction or oxidative coupling reaction; and obtaining the tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst (N / C) from the tetrazine ring polycarbazole through a direct pyrolysis method. The synthesized catalyst has excellent oxygen reduction (ORR) catalytic activity and electrochemical stability.

Description

technical field [0001] The invention relates to an oxygen reduction catalyst and a preparation method thereof, in particular to a tetrazine ring polycarbazole-based nitrogen-doped carbon-oxygen reduction catalyst and a preparation method thereof, belonging to the field of fuel cell science and technology. Background technique [0002] Environmental pollution and energy shortages brought about by the development of industrialization have prompted people to urgently look for new energy devices. Fuel cells are a kind of green energy that can directly convert chemical energy into electrical energy, and its process is not limited by the Caljo cycle. New energy devices have set off a research boom in recent years. However, Pt and Pt-based catalysts that catalyze the oxygen reduction reaction (ORR) at the cathode of fuel cells have seriously hindered the large-scale commercial production of fuel cells due to their high price, poor stability, and poor resistance to methanol. Theref...

Claims

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Application Information

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IPC IPC(8): H01M4/90
CPCH01M4/9091Y02E60/50
Inventor 陈红飙孙滔阳梅刘益江黎华明
Owner XIANGTAN UNIV
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