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A carbon nanotube and graphite flake hybrid material and its preparation method and application

A hybrid material and carbon nanotube technology, which is applied in the field of water treatment, can solve the problems of limited catalytic performance and difficult modification of original graphite sheets/carbon nanotubes, and achieve excellent activation effect, strong anti-interference ability and high catalytic activity. Effect

Active Publication Date: 2021-11-23
JIANGNAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Moreover, the electronic properties of carbon nanotubes depend largely on their size and chirality, and it is difficult to modify them.
Therefore, the improvement of the catalytic performance of pristine graphite flakes / CNTs is limited

Method used

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  • A carbon nanotube and graphite flake hybrid material and its preparation method and application
  • A carbon nanotube and graphite flake hybrid material and its preparation method and application
  • A carbon nanotube and graphite flake hybrid material and its preparation method and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0050] Example 1 Preparation of catalyst and performance test

[0051] (1) Preparation of catalyst

[0052] Catalyst 1 to 5: Weighing the mass of 10 g of ferric cyanide, placed under a nitrogen atmosphere, raised to 800 ° C under a nitrogen atmosphere, and thermally thermally insulated from 1H, 3H, 5H, respectively. 7H, 9H ° C, then washed, vacuum drying, and catalyst 1, 2, 3, 4, 5, respectively.

[0053] Catalyst 6 to 8: The catalyst 3 was washed at different times, weighed 100 mg of catalyst 3, and stirred in a 1 m sulfuric acid solution, stirred for 12 h, 24h, 36 h, then washed to neutral, centrifuge, 60 ° C drying, respectively Catalysts 6, 7, 8.

[0054] Catalysts 9 to 11: The catalyst 6-8 is annealed twice separately. A 100 mg catalyst 6-8 was weighed, and the temperature increase rate of 5 ° C / min in the tube furnace was raised to 700 ° C under a nitrogen atmosphere and was held for 1 h. After cooling to room temperature, the catalysts 9, 10, 11 were obtained.

[0055] (2...

Embodiment 2

[0060] Example 2 Detailed degradation experiments were performed in a TC model contaminant with a catalyst 10 as an optimal catalyst.

[0061] Catalytic activity was evaluated in a 150 ml reactor containing a concentration of catalyst, PMS and contaminated, and stirred at a water bath at 25 ° C. 10 mg of catalyst (catalyst 10, commercial nitrogen doped carbon nanotubes, commercial multilayer graphite, and mixed nitrogen doped carbon nanotubes) were added to 50 ml of TC (50 mg / l) solution for 20 minutes, The balance of adsorption-desorption is reached until it is reached. 10 mg of PMS was added to the above solution to initiate a reaction. Specific methods, see the performance test portion of Example 1, all experiments are carried out under pH = 7. Such as Figure 5 As shown, it can be seen that the degradation capability of a separate PMS is almost ignored, only 3.0%, indicating that the PMS is an oxidant, but its oxidation capacity is limited; the separate catalyst 10 has only a...

Embodiment 3

[0062] Example 3 Catalytic degradation mechanism before and after pickling

[0063] In order to confirm the active substances and degradation mechanisms generated during the PMS activation process, a series of free radical quas was carried out in the catalyst 10 and the catalyst 3. Methanol (MeOH), tert-butanol (TBA), and L-Histidine are used as the free radical cleavage agent, respectively, for hydroxy free radicals (· OH) and sulfate (SO4 · -) , Free radical (SO4 · -), single-line oxygen ( 1 O 2 Clear, the result is like Image 6 Indicated. The catalyst 10 / PMS system exhibits high tolerance to MeOH and TBA, indicating that · OH and SO4 · - not the primary active substance. Interestingly, the inhibition of the TBA on the degradation process is stronger than MeOH, which should be attributed to the hydrophobic interaction of the catalyst 10 and TBA. However, when the system is added at 1.55 g / L L-histidine, the degradation efficiency of the catalyst 10 is significantly reduced, ...

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Abstract

The invention discloses a carbon nanotube and graphite flake hybrid material, a preparation method and application thereof, and belongs to the field of advanced catalytic oxidation water treatment. A certain amount of salt whose central atom is an iron-based transition metal is pyrolyzed at a certain temperature in an inert nitrogen atmosphere, washed, etched, dried after cooling, and then annealed twice to obtain carbon nanotubes and graphite sheet hybrid material. The invention uses the hybrid material of carbon nanotubes and graphite flakes as a catalyst to activate PMS to degrade TC and OTC, and maintains a high TC removal rate even in high-salinity wastewater (with an anion content of 500mM). Compared with the traditional Fenton reaction, the catalyst has a wide range of pH tolerance. The degradation product of the present invention is CO 2 and H 2 O, no secondary pollution has the advantages of green, high efficiency, low cost and so on. The catalyst can be prepared on a large scale and has potential commercial value.

Description

Technical field [0001] The present invention relates to a carbon nanotube and a graphite hybrid material and a preparation method thereof, which belongs to a high-grade catalytic oxidation technology, which can be used in the field of water treatment. Background technique [0002] With the development of the economy, the improvement of people's living standards, more and more drugs, chemicals, etc. In our daily lives, they have brought convenience to our lives, and they also bring huge challenges to what we live. . Drugs are generally existent in the environment, closely related to people, such as aminol antibiotics, large cycloys, aminoglycoside antibiotics, tetracyclines, and the like. Among them, tetracycline (Tc) and oxytes (OTC) are typical residual contaminants. Tc, OTC is difficult to degrade after entering the environment, with a gather of food, and remains in the human body. Even with decomposition, the formed intermediate product is often more toxic. Therefore, it is ur...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J21/18B01J37/08B01J27/24B01J37/06C02F1/72C02F101/30C02F101/34C02F101/36C02F101/38
CPCB01J21/18B01J21/185B01J27/24B01J37/06B01J37/08B01J37/082C02F1/725C02F2101/30C02F2101/308C02F2101/34C02F2101/36C02F2101/38C02F2101/40
Inventor 宋启军付程王婵卫邦琪
Owner JIANGNAN UNIV