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Nitrogen-doped graphdiyne riveted transition metal monatomic catalyst as well as preparation method and application thereof

A transition metal and transition metal salt technology, applied in electrical components, battery electrodes, circuits, etc., can solve the problems of reduced catalyst activity, limited non-precious metal catalyst activity, and low atom utilization

Active Publication Date: 2020-07-07
NANJING NORMAL UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The study found that the nitrogen in the catalyst can coordinate with the transition metal atoms to form a TM-N structure, and these TM-N structures are the catalytic active sites of the TM-N-C catalyst. When the size of the metal particle is reduced to the atomic size, its specific surface area and surface The energy will be multiplied, and it is very easy to agglomerate to form large clusters in the process of preparation and reaction, resulting in low atom utilization, which leads to a decrease in catalyst activity and limits the activity of non-noble metal catalysts.

Method used

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  • Nitrogen-doped graphdiyne riveted transition metal monatomic catalyst as well as preparation method and application thereof
  • Nitrogen-doped graphdiyne riveted transition metal monatomic catalyst as well as preparation method and application thereof
  • Nitrogen-doped graphdiyne riveted transition metal monatomic catalyst as well as preparation method and application thereof

Examples

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Effect test

Embodiment 1

[0040]Dissolve 50 mg of hexa[trimethylsilyl]ethynyl]benzene in 15 mL of tetrahydrofuran, stir for 1 h under Ar gas purging, add 1 mL of tetrabutylammonium fluoride at 0°C for 15 min; add 20 mL of ethyl acetate to dilute, Then add 20 mL of saturated saline to wash three times, extract and separate the liquid to take the upper layer solution, add 20 mg of anhydrous magnesium sulfate to remove water and filter, and the mixture is rotary evaporated at 45 ° C to remove the solvent to obtain a yellow solid hexaethynylbenzene; 100 mL of acetone and 5 mL Pyridine, 1mL tetramethylethylenediamine, and 2*2cm*10 acid-washed copper foil were stirred at 50°C for 2h under the protection of Ar gas to obtain a mixture, and the hexaethynylbenzene obtained in the previous step was dissolved in 50mL of acetone, and the Slowly add the above mixture to react for 36h; centrifuge the reacted mixture at 10000r / min to get the black solid, and wash it with N,N,N,N-tetramethylethylenediamine, acetone, eth...

Embodiment 2

[0042] Mix 10 mg of graphyne synthesized in Example 1 with 50 mg of melamine in 30 mL of ethanol (AR), and stir thoroughly at room temperature 20° C. for 12 h; place the mixture in a vacuum oven at 70° C. and dry for 6 h to obtain mixture A; The dried mixture A was placed in a tube furnace, heated to 900°C for 2 hours under an Ar gas atmosphere, and pyrolyzed at a rate of 5°C / min, and cooled to room temperature to obtain a black solid B; all the black solid B was mixed with 0.1 Disperse mol of ferric chloride hexahydrate into 30mL water, stir magnetically under Ar atmosphere at 25°C for 12h to obtain mixture C, use a 200W power ultrasonic machine to sonicate for 10min, and centrifuge at 10000r / min for 10min to obtain solid precipitate D; all solid precipitate D Disperse in 30mL of water, dissolve 5mg of sodium borohydride in 10mL of water, add to the above dispersion under Ar atmosphere, stir with a magnetic stirrer at 20°C for 12h; wash the stirred mixed solution twice with wa...

Embodiment 3

[0045] The preparation method of embodiment 3 is the same as that of embodiment 2, except that ferric chloride hexahydrate is replaced by ferric nitrate nonahydrate.

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Abstract

The invention discloses a nitrogen-doped graphdiyne riveted transition metal monatomic catalyst as well as a preparation method and application thereof. According to the catalyst, nitrogen atoms are doped in a novel carbon material graphdiyne carrier, transition metal single atoms are riveted on the surface of nitrogen-doped graphdiyne through the covalent effect between the transition metal single atoms and N and C atoms, and thus transition metal is uniformly dispersed on the surface of the nitrogen-doped graphdiyne in a single atom form to form the catalyst. Transition metal atoms in the catalyst are uniformly dispersed on the surface of the nitrogen-graphdiyne-based catalyst in a single atom state, a large number of active sites are provided for oxidation-reduction reaction, graphdiyneis adopted as a carbon substrate and has excellent morphological characteristics, formation of catalytic active sites is facilitated, and catalytic advantages of single atoms are brought into play. The catalyst disclosed by the invention has high electrocatalytic activity on oxygen reduction under an alkaline condition, is simple and effective in preparation process, low in cost and easy to popularize and put into production, and has important significance in the field of fuel cell development and application.

Description

technical field [0001] The invention belongs to the technical field of material chemistry and electrocatalyst, and in particular relates to a preparation method of a fuel cell cathode catalyst, in particular to a nitrogen-doped graphyne riveted transition metal single-atom catalyst and its preparation method and application. Background technique [0002] Because of its superior performance and environmental friendliness, cleanliness and non-pollution, fuel cells have shown outstanding advantages in various types of batteries. It can directly convert chemical energy into electrical energy and has a very high fuel utilization rate. It has always been a hot spot in the field of energy research. hotspot. Oxygen reduction reaction (ORR) is the first reduction reaction of fuel cells and one of the important basic reactions in living organisms. However, due to its slow reaction kinetics and complicated reaction steps, it is necessary to select a suitable catalyst to improve its rea...

Claims

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Application Information

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IPC IPC(8): H01M4/90H01M4/88
CPCH01M4/9041H01M4/9083H01M4/8825H01M2004/8689Y02E60/50
Inventor 蔡称心周家兴胡耀娟蔡哲炜潘永慧吴萍
Owner NANJING NORMAL UNIVERSITY
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