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Nitrogen-doped hollow carbon polyhedron-carbon@nanotube-based monatomic cobalt catalyst capable of efficiently activating persulfate and preparation method thereof

A technology for activating persulfate and carbon polyhedron, applied in physical/chemical process catalysts, chemical instruments and methods, chemical/physical processes, etc., can solve the problem of low density of catalyst active sites, high reaction activation energy, easy loss of catalyst, etc. problems, achieve the effect of reducing the activation energy of the reaction, broad application prospects, and strengthening the surface adsorption

Active Publication Date: 2021-01-05
NANJING UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] Aiming at the deficiencies in the heterogeneous catalytic technology based on sulfate radicals, such as low density of catalyst active sites, high reaction activation energy, great influence of temperature, easy to be interfered by inorganic salts and natural organic matter in water, easy loss of catalyst, etc. Problem, the present invention provides a nitrogen-doped hollow carbon polyhedron@carbon nanotube-based single-atom cobalt catalyst and its preparation method for efficiently activating persulfate

Method used

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  • Nitrogen-doped hollow carbon polyhedron-carbon@nanotube-based monatomic cobalt catalyst capable of efficiently activating persulfate and preparation method thereof
  • Nitrogen-doped hollow carbon polyhedron-carbon@nanotube-based monatomic cobalt catalyst capable of efficiently activating persulfate and preparation method thereof
  • Nitrogen-doped hollow carbon polyhedron-carbon@nanotube-based monatomic cobalt catalyst capable of efficiently activating persulfate and preparation method thereof

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Experimental program
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Effect test

Embodiment 1

[0035] A nitrogen-doped hollow carbon polyhedron@carbon nanotube-based single-atom cobalt catalyst with high-efficiency activation of persulfate and a preparation method thereof, the specific steps of which are as follows:

[0036] a. Disperse 0.5g ZIF-8 in 2.47mol methanol, dissolve 6.16g 2-methylimidazole in 2.47mol methanol to form solution A, and dissolve 5.82g Co(NO 3 ) 2 ·6H 2 O was dissolved in 2.47mol methanol to form solution B. First, add solution A to the dispersion of ZIF-8, stir well and then add solution B. The mixed solution was stirred and reacted at room temperature for 24 hours, and the precipitated product was collected by centrifugation and washed with water. After vacuum drying, ZIF-8@ZIF-67 was obtained.

[0037] b. Place the ZIF-8@ZIF-67 obtained in step a in a crucible, put the lid on and transfer to a tube furnace, and under the protection of an argon inert atmosphere, heat up to 950°C for calcination at a rate of 2°C / min 3h. After the reaction, th...

Embodiment 2

[0043] With embodiment 1, difference is:

[0044] The soluble cobalt salt in step a was changed to CoSO 4 ·7H 2 O, its mass is 5.62g, the amount of 2-methylimidazole is 9.85g, after adding solution A and solution B, the amount of total methanol in the mixed solution is 10mol.

[0045] Under the same experimental conditions as in Example 1, the obtained catalyst had a degradation rate of 92.3% to bisphenol A within 4 minutes.

Embodiment 3

[0047] With embodiment 1, difference is:

[0048] The soluble cobalt salt in step a is changed to CoCl 2 ·6H 2 O, its mass is 4.76g, the amount of 2-methylimidazole is 4.93g, after adding solution A and solution B, the total amount of methanol in the mixed solution is 4mol.

[0049] Under the same experimental conditions as in Example 1, the obtained catalyst had a degradation rate of 91.8% to bisphenol A within 4 minutes.

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Abstract

The invention relates to the field of new environmental materials, in particular to a nitrogen-doped hollow carbon polyhedron-carbon@nanotube-based monatomic cobalt catalyst capable of efficiently activating persulfate and a preparation method thereof. According to the invention, ZIF-8 is used as a seed crystal, ZIF-67 grows on the surface of the ZIF-8 through an epitaxial growth method to obtainZIF-8@ZIF-67 with a core-shell structure, then the ZIF-8@ZIF-67 is calcined in an inert atmosphere to obtain carbonized ZIF-8@ZIF-67, exposed cobalt nanoparticles are removed through acid pickling, and the nitrogen-doped hollow carbon polyhedron@carbon nanotube-based monatomic cobalt catalyst is prepared. According to the catalyst, monatomic cobalt is anchored on a carbon matrix through coordination, the catalytic site density is high, the conductivity is good, the ferromagnetism is good, persulfate can be efficiently activated to degrade toxic and harmful organic pollutants in water, the useamount of the catalyst and persulfate is greatly reduced, and the cost is reduced. Moreover, multi-component comprehensive regulation and control of the hollow carbon polyhedron, the carbon nanotubesand the monatomic cobalt are realized for the first time, efficient and stable operation can be realized within a wide temperature range and under the interference of inorganic salt, natural organic matters and the like, and the application prospect is expanded.

Description

technical field [0001] The invention relates to the field of new environmental materials, in particular to a nitrogen-doped hollow carbon polyhedron@carbon nanotube-based single-atom cobalt catalyst for efficiently activating persulfate and a preparation method thereof. Background technique [0002] With the various production activities of human beings, a large amount of toxic organic pollutants enter the water body. They usually have "three-caused" effects and pose a serious threat to water ecological security. Such pollutants are difficult to biochemically degrade and transform efficiently, and new water treatment technologies are urgently needed. Compared with the generation of active oxygen species such as hydroxyl radicals and sulfate radicals to degrade pollutants, the reaction is bound to the surface of the catalyst, and the degradation of pollutants through electron transfer between oxidants and pollutants can effectively avoid inorganic salts in water. And the int...

Claims

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Application Information

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IPC IPC(8): B01J27/24B01J35/10C02F1/72C02F101/30C02F101/34C02F103/34
CPCB01J27/24C02F1/725C02F1/722C02F2101/30C02F2101/308C02F2101/345C02F2103/343B01J35/61
Inventor 刘福强范钟伟朱长青徐晓明李爱民
Owner NANJING UNIV
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