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Preparation method of Co particle coated CNT (carbon nanotube) catalytic material and application of catalytic material in cyclohexane oxidation reaction

A technology of carbon nanotubes and catalytic materials, which is applied in the direction of hydrocarbon oxidation to prepare oxygen-containing compounds, oxidation reaction preparation, and carbon-based compound preparation. It can solve the problems of low conversion rate, increased separation energy consumption, and unsuitability for industrial production. Not easy to lose, improve catalytic activity, and improve yield

Inactive Publication Date: 2017-04-26
XIANGTAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] Yu Hao et al. (CN102040504A) invented a carbon nanotube filled with magnetic iron particles as a catalyst to catalyze the oxidation of cyclohexane. This invention uses the magnetism of the catalyst to simplify the separation of the catalyst, and the filling of Fe improves the catalytic performance of the carbon nanotube. Activity, but the use of organic solvents in the reaction increases the energy consumption of the separation, and a large amount of adipic acid is obtained
[0005] Xu Lixin et al. (CN105646153A) invented a method for catalytic oxidation of cyclohexane with a supported Au / C3N4@SBA-15 nanocatalyst, and Chen Lijuan et al. (CN105327717) invented a SiO 2 -Mesoporous TiO 2 Nano-gold cyclohexane oxidation catalyst encapsulated by hollow microspheres. This catalyst has high catalytic activity, but it uses Au precious metal, and the cost is high.
[0006] However, homogeneous catalysts are used in industrial applications, not only the conversion rate is low, but the catalysts are also difficult to recycle.
[0007] However, if a noble metal catalyst is used, although it can increase the conversion rate, it will consume a high cost, which is uneconomical and not suitable for industrial production; in addition, if the reaction process uses an organic solvent as a reaction solvent, it will cause a heavy separation load and also will significantly increase production costs

Method used

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  • Preparation method of Co particle coated CNT (carbon nanotube) catalytic material and application of catalytic material in cyclohexane oxidation reaction

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0038] Co@OCNTs for Catalyzing Cyclohexane Oxidation

[0039] (1) Take 2g of carbon nanotubes in a 250ml round bottom flask, add 100ml of concentrated nitric acid solution (mass fraction 65%~68%), and reflux at 100°C for 16h;

[0040] (2) After the reflux is completed, cool to room temperature, filter and wash with deionized water several times until neutral;

[0041] (3) drying the solid obtained in step (2) at 110° C. for 12 hours to obtain oxidized carbon nanotubes (OCNTs);

[0042] (4) Dissolve 1.3g of cobalt nitrate in 20ml of absolute ethanol to make 0.223mol / L ethanol solution of cobalt nitrate;

[0043] (5) Take 0.5g of OCNTs obtained in step (3) in a small beaker, place the small beaker in an ultrasonicator, and add 2ml of cobalt nitrate ethanol solution dropwise to the small beaker with a rubber dropper under ultrasonication and stirring , then add 1.5ml of deionized water dropwise under ultrasonic stirring;

[0044] (6) Ultrasound for 30 minutes, then stand still...

Embodiment 2

[0055] The difference from Example 1 is that the reaction temperature is 145° C. and the reaction pressure is 1.0 MPa.

[0056] The results showed that the conversion rate of cyclohexane was 7.06%, and the total selectivity of product alcohols and ketones was 54.93%.

Embodiment 3

[0058] The difference from Example 1 is that the reaction temperature is 155° C. and the reaction pressure is 0.8 MPa.

[0059] The results showed that the conversion rate of cyclohexane was 8.95%, and the total selectivity of product alcohols and ketones was 74.92%.

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Abstract

The invention discloses a preparation method of a Co particle coated CNT (carbon nanotube) catalytic material and an application of the catalytic material in a cyclohexane oxidation reaction. CNTs are coated with Co particles, obtained Co@OCNTs are used for preparation of KA oil through cyclohexane oxidation, and better cyclohexane conversion rate and KA selectivity are shown; size of the Co particles is controlled by sufficiently utilizing the confinement effect of CNTs, meanwhile, electronic structures of the CNTs are changed by Co, and relatively considerable cyclohexane conversion rate and KA oil selectivity are obtained through the interaction of the CNTs and the Co particles. The use of noble metal and organic solvents is avoided, so that the preparation method is more economical and more environment-friendly; due to limitation of the CNTs to Co, Co is not prone to losing and can be recycled, and thought for modified application of the CNTs is broadened.

Description

technical field [0001] The invention belongs to the field of material preparation, in particular to a method for preparing a carbon nanotube-coated cobalt particle catalytic material and its application in cyclohexane oxidation reaction. Background technique [0002] At present, the industrial production of cyclohexanol and cyclohexanone (KA oil) by oxidation of cyclohexane mainly includes cobalt salt method and boric acid method in non-catalytic oxidation method and catalytic oxidation method. Among them, no catalytic oxidation reaction product is easy to separate and purify, and the selectivity of KA oil is high, but the reaction temperature is high, the energy consumption is large, and the conversion rate of cyclohexane is low; 2 (1-2MPa), carried out at 160°C, the conversion rate of cyclohexane is about 4%, the selectivity of KA oil is about 80%, and the energy consumption is high and the efficiency is low; the boric acid catalytic oxidation method has high alcohol and k...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/75C07C29/50C07C35/08C07C45/33C07C49/403C07C27/12
CPCB01J21/185B01J23/75C07C29/50C07C45/33C07C35/08C07C49/403
Inventor 郝芳吕崔华刘平乐熊伟李翔熊绍锋
Owner XIANGTAN UNIV
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