Nitrogen-doped carbon nanotube/carbon composite oxygen reduction catalyst and preparation method thereof

A carbon nanotube, nitrogen-doped carbon technology, applied in structural parts, electrical components, battery electrodes, etc., can solve the problems of complex operation, harsh reaction conditions, unfavorable large-scale use, etc., achieving simple operation steps, flexible design, Structure and composition controllable effects

Inactive Publication Date: 2019-03-19
XIANGTAN UNIV
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  • Abstract
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  • Application Information

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Problems solved by technology

The methods for synthesizing nitrogen-doped carbon nanocomposites often include chemical vapor deposition (CVD), hydrothermal synthesis, solution self-assembly, and high-temperature post-treatment of nitrogen-containing organic precursors. The requirements are relatively high. The solution self-assembly method is a method of assembling and constructing structures without relying on manpower, and the controllability is poor.
Although the CVD method can well regulate the morphology of composite materials, the reaction conditions are relatively harsh and the operation is complicated, which is not conducive to large-scale production of this method; the method of high-temperature post-treatment of nitrogen-containing organic precursors is the simplest, and the obtained nitrogen-doped carbon nano The ORR activity of tube composites is also high, which is a good way to prepare high-efficiency ORR electrocatalysts.

Method used

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  • Nitrogen-doped carbon nanotube/carbon composite oxygen reduction catalyst and preparation method thereof
  • Nitrogen-doped carbon nanotube/carbon composite oxygen reduction catalyst and preparation method thereof
  • Nitrogen-doped carbon nanotube/carbon composite oxygen reduction catalyst and preparation method thereof

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preparation example Construction

[0080] According to the second embodiment provided by the present invention, a method for preparing a nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst is provided. The method includes the following steps:

[0081] 1) Preparation of carbon nanotube / melamine composite (CNT-MAM): put CNTs in an absolute ethanol environment, mix and disperse, then add melamine (MAM) for reflux stirring, after cooling, perform suction filtration and washing, Obtain carbon nanotube / melamine composite (CNT-MAM) after drying;

[0082] 2) Preparation of carbon nanotube / poly(melamine-aldehyde) composite: the obtained carbon nanotube / melamine composite (CNT-MAM) was dispersed in anhydrous dimethyl sulfoxide (DMSO) or DMSO aqueous solution, Then add it to the reaction kettle lined with polytetrafluoroethylene, add melamine (MAM) and aldehyde-containing compound in sequence under stirring, stir and react after heating, reheat, and crush, wash, and dry the obtained solid after cooli...

Embodiment 1

[0091] A preparation of nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst, comprising the steps of:

[0092] (1) Preparation of carbon nanotube / melamine composite (CNT-MAM): put 1000mg of CNTs and 200mL of absolute ethanol in a 500mL round-bottomed flask, and then ultrasonically disperse the CNTs for 30min, then add 2000mg of melamine (MAM), stirring at reflux for 24h. Cool to room temperature, filter with PTFE membrane, wash the product with 80°C hot water and ethanol three times, and finally dry in a vacuum oven for 8 hours.

[0093] (2) Preparation of carbon nanotube / poly(melamine-formaldehyde) composite: Disperse carbon nanotube / melamine (CNT-MAM) (2.5 g) prepared in step (1) in 33.6 mL of anhydrous DMSO, and then Add it into a reaction kettle lined with polytetrafluoroethylene, add MAM (3.78g, 30mmol) and formaldehyde (1.62g, 54mmol) sequentially under stirring, then place it in a 120°C oven at constant temperature for 1h, take it out and stir to ...

Embodiment 2

[0096] A preparation of nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst, comprising the steps of:

[0097] (1) Preparation of carbon nanotube / melamine composite (CNT-MAM): Weigh 1000mg of CNTs and 200mL of absolute ethanol in a 500mL round-bottomed flask, then ultrasonically sonicate for 30min to fully disperse the CNTs, then add 2000mg of melamine (MAM), stirring at reflux for 24h. Cool to room temperature, filter with PTFE membrane, wash the product with 80°C hot water and ethanol three times, and finally dry in a vacuum oven for 8 hours.

[0098] (2) Preparation of carbon nanotube / poly(melamine-benzaldehyde) composite: put CNT-MAM prepared in step (1) and melamine (6.3g, 50mmol), benzaldehyde (7.95g, 75mmol) in 500mL Add 200mL of anhydrous DMSO to the round bottom flask, and ultrasonically sonicate for 10min (40kHz) to fully disperse CNT-MAM in the reaction solvent. After sealing, blow argon to exhaust oxygen for 30min, and move it into a 170°C oi...

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Abstract

The invention provides a nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst and a preparation method thereof. The catalyst firstly adds melamine (MAM) into carbon nanotubes (CNTs), and prepares melamine through a non-covalent bond modification method. modified carbon nanotubes (CNT‑MAM), and then in situ polymerized them with melamine and aldehyde-containing compounds in dimethyl sulfoxide (DMSO) to synthesize carbon nanotubes / poly(melamine‑aldehyde) composites, and then A nitrogen-doped carbon nanotube / carbon composite catalyst is prepared by pyrolyzing the composite at high temperature. The nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst provided by the invention has high specific surface area and nitrogen content, excellent oxygen reduction catalytic activity, methanol resistance performance and stability.

Description

technical field [0001] The invention relates to a nitrogen-doped carbon nanotube / carbon composite oxygen reduction catalyst and a preparation method thereof, belonging to the field of fuel cell science and technology. Background technique [0002] Due to its unique structure and synergistic effect between different materials, nitrogen-doped carbon nanocomposites can further improve the catalytic activity of oxygen reduction reaction (ORR) compared with single nitrogen-doped carbon materials, and are ideal for fuel cell cathodes. Contains metal-free catalysts. CNTs themselves have excellent properties, and many researchers compound them with polymers to prepare CNTs / polymer composites with desired properties. CNTs have small diameter and large surface energy, and are easy to attract each other to form larger aggregates. In order to make CNTs uniformly dispersed in composite materials, it is necessary to modify CNTs before polymerization. The non-covalent modification will n...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): H01M4/90H01M4/88
CPCH01M4/88H01M4/90Y02E60/50
Inventor 阳梅罗岚陈红飙黎华明
Owner XIANGTAN UNIV
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